Czech Technical University in Pragueojs.ujf.cas.cz/~wagner/transmutace/diplomky/PHD_Svoboda.pdfIII Czech Technical University in Prague Faculty of Nuclear Sciences and Physical Engineering

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Czech Technical University in Prague

Dissertation Thesis

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III

Czech Technical University in Prague

Faculty of Nuclear Sciences and Physical Engineering

Department of Nuclear Reactors

Ing. Ondřej Svoboda

Experimental Study of Neutron Production and

Transport for ADTT

Dissertation Thesis

Prague, 2011

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V

Declaration

I declare that this dissertation thesis was done in the internal and combined form of

postgradual study at the Department of Nuclear Reactors at the Faculty of Nuclear

Sciences and Physical Engineering at the Czech Technical University in Prague. All

data, tables, figures and ideas stated in this work are results of my own work unless

otherwise stated and referred. This work has not been submitted for any other

qualification to this or any other university.

Aspirant: Ing. Ondřej Svoboda

Postgradual study program: Application of Natural Sciences

Study field: Nuclear Engineering

Supervisor: RNDr. Vladimír Wagner, CSc.

Affiliation: Department of Nuclear Spectroscopy

Nuclear Physics Institute

Academy of Sciences of the Czech Republic

public research institution

250 68 Řež near Prague

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VII

Acknowledgements

My thanks belong to:

RNDr. Vladimír Wagner CSc., my great supervisor. He was always ready

selflessly to help and guide me, with huge patience and with sense for showing

the problems in consequences.

the head of the department of Nuclear Spectroscopy at Nuclear Physics Institute

Řež, RNDr. Andrej Kugler CSc., for his support, understanding and valuable

suggestions and remarks.

my colleague Mgr. Antonín Krása PhD., for the support and care that he gave

me from my early beginnings in the Academy of Sciences up to now.

my colleague Mitja Majerle PhD. for his dedication during introducing me to

MCNPX simulations and helping me programming.

my colleague Ing. Marek Fikrle, for preparing of iodine samples, the help with

irradiations on LVR-15 reactor, and for valuable advice on the field of HPGe

detectors and activation analysis.

PhD students Ing. Jitka Vrzalová and Ing. Martin Suchopár and also to grammar

school students Pavel Motal, Ondřej Novák, and Ondřej Sláma, same as to our

foreign students Anne Larédo, Gail de Cargouet, Tazio Torrieri, and Havard

Farder for their kind cooperation and a lot of interesting questions that forced me

to think again about the physics I am dealing with and which lead me to better

understanding.

This work would not exist without the kind help of the people around the

accelerators in Dubna, Uppsala, and Řež; namely M. I. Krivopustov, A. Prokofiev,

P. Bém and theirs teams. I am also grateful to J. Frána, for enabling me to use his HPGe

gamma-detector during measurements in Řež and the program DEIMOS32 for

evaluating of measured gamma-spectra.

Last but not least I would like to express thanks to my parents Zdena and

František Svobodovi and to my girlfriend Kateřina Blažková for support,

encouragement and love they gave me.

This work was financially supported from the Grant Agency of the Czech

Republic (grant No. 202/03/H043), Internal Grant Competition (grant number

CTU0808214), Grant Agency of the Academy of Sciences of the Czech Republic (grant

No. K2067107), F4E program of the Nuclear Reaction Department of the Nuclear

Physics Institute (grant number F4E-2008-GRT-014), and from the EFNUDAT

(European Facilities for Nuclear Data Measurements).

VIII

Abstract

High energy neutron production in spallation reactions and their transport in the

system of massive lead target and uranium blanket were studied within the international

project Energy and Transmutation of Radioactive Waste. A setup called Energy plus

Transmutation placed in Dubna, Russia, was irradiated with 1.6 GeV up to 4 GeV

deuterons. Threshold reactions on activation detectors from Al, Au, Bi, Co, In, Ta, and

Y were used for neutron measurements. Activated foils were measured on HPGe

detectors. Spectroscopic corrections were applied during data analysis to find the yields

of produced isotopes. The experimental results were compared with MCNPX

calculations. These experiments are a continuation of previous research of the above

mentioned setup with relativistic protons. No serious disagreement in neutron

production to backward angles was observed for deuteron experiments on contrary to

the proton ones.

Cross-sections of used threshold reactions were measured on quasi-

monoenergetic neutron sources at Nuclear Physics Institute in Řež and at The Svedberg

Laboratory in Uppsala, Sweden. In total eleven irradiations were done in the energy

range 17 – 94 MeV. Threshold reactions were measured up to (n,10n), the results were

compared with the data from EXFOR, EAF, and with the calculated values from

TALYS code with good agreement. Cross-sections for reactions over 40 MeV and

(n,4n) are unique and were measured for the first time. A part of the data has already

been published and presented at international conferences.

Key words: spallation reaction, Energy plus Transmutation of Radioactive Waste,

neutron activation analysis, HPGe gamma-ray detector, gamma-spectroscopy, MCNPX

code, threshold reaction, cross-section.

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Abstrakt

Produkce vysokoenergetických neutronů ve spalačních reakcích a jejich

transport v systému masivního olověného terče a uranového blanketu byly studovány

v rámci mezinárodního projektu „Energy and Transmutation of Radioactive Waste“.

Sestava nazvaná „Energy plus Transmutation“ umístěná v Dubně, Rusko, byla ozářena

deuterony o energiích 1,6 GeV až 4 GeV. Pro měření neutronů byly použity prahové

reakce na aktivačních detektorech z Al, Au, Bi, Co, In, Ta a Y. Záření gama

aktivovaných fólií bylo měřeno pomocí polovodičových HPGe detektorů. Při analýze

získaných dat byla aplikována řada spektroskopických korekcí za účelem nalezení

výtěžku sledovaných isotopů. Experimentální data byla nakonec porovnána s výsledky

simulací sestavy provedených pomocí programu MCNPX. Tyto experimenty navázaly

na předchozí výzkum zmíněné sestavy pomocí relativistických protonů. Pro

deuteronové experimenty nebyla na rozdíl od protonových pozorována žádná výraznější

neshoda v produkci vysokoenergetických neutronů do zpětných úhlů.

Účinné průřezy užitých prahových reakcí byly změřeny pomocí quasi-

monoenergetických neutronových zdrojů v Ústavu jaderné fyziky, Řež, a ve

Svedbergově laboratoři, Uppsala, Švédsko. Bylo provedeno celkem 11 ozařování

v energetickém rozsahu 17 až 94 MeV. Prahové reakce byly změřeny až do (n,10n),

výsledky byly porovnány s daty z databází EXFOR, EAF a s hodnotami vypočtenými

pomocí programu TALYS. Byla pozorována dobrá shoda. Účinné průřezy pro reakce

nad 40 MeV a (n,4n) jsou unikátní a byly změřeny vůbec poprvé. Část naměřených dat

již byla publikována a prezentována na mezinárodních konferencích.

Klíčová slova: tříštivá reakce, Energy and Transmutation of Radioactive Waste,

neutronová aktivační analýza, HPGe detektor záření gama, spektroskopie gama záření,

program MCNPX, prahová reakce, účinný průřez.

X

List of abbreviations

ABC – Accelerator Based Conversion

ADEP – Accelerator Driven Energy Production

ADS – Accelerator Driven System

ADTT – Accelerator Driven Transmutation Technology

AFCI – Advanced Fuel Cycle Initiative

AGS – Alternating Gradient Synchrotron

AMAVET – Asociace pro mládež, vědu a techniku

ATW – Accelerator Transmutation of Waste

ASCR – Academy of Sciences of the Czech Republic

barn – unit of cross-section used in nuclear physics (1 barn = 10-28

m2)

CEA – Commissariat à l‟énergie atomique

CERN – Conseil Européen pour la Recherche Nucléaire (European Organization for

Nuclear Research)

CNGS – CERN Neutrinos to Gran Sasso project

CONFIRM – Collaboration on Nitride Fuel Irradiation and Modeling

CSMSR – Cascade Subcritical Molten Salt Reactor

CSNS – China Spallation Neutron Source

E+T – Energy plus Transmutation setup

E&T RAW – Energy and Transmutations of Radioactive Waste project

EAF – European Activation File

EFNUDAT – European Facilities for NUclear DATa measurements

ENDF – Evaluated Nuclear Data File

EPAC – European Particle Accelerator Conference

ESS – European Spallation Source

EUROTRANS – EUROpean Research Programme for the TRANSmutation

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EUROPART – EUROpean research programme for the PARTitioning of minor

actinides

eV – electron volt

EXFOR – Experimental Nuclear Reaction Data

FUS – FUsion aSsociation

GeV – gigaelectron volt

GWe – GigaWatt electrical

GWd/MTHM – GigaWatt days per Metric Ton of Heavy Metal

HINDAS – High and Intermediate energy Nuclear Data for Accelerator-driven System

HM – Heavy Metal

HPGe – High Purity Germanium detector

IAEA – International Atomic Energy Agency

IEEE – Institute of Electrical and Electronics Engineers

INDC – International Nuclear Data Committee

INR – Institute for Nuclear Research of the Russian Academy of Sciences

ISNS – India Spallation Neutron Source

JASNAPP – nuclear spectroscopy on proton beam (from Russian)

JINR – Joint Institute for Nuclear Research, Dubna, Russia

J-PARC – Japan Proton Accelerator Research Complex

keV – kiloelectron volt

kW – kilowatt

LAHET – Los Alamos High-Energy Transport code

LAMF – Los Alamos Meson Physics Facility

LANSCE – Los Alamos Neutron Science Center

LEDA – Low Energy Demonstration Accelerator

MCNP – Monte-Carlo N-Particle

MCNPX – Monte-Carlo N-Particle eXtended

XII

MEGAPIE – MEGAwatt spallation target PIlot Experiment

MeV – Megaelectron Volt

MLF – Material and Life science Facility of the J-PARC

MOX – Mixed Oxide Fuel

MTIHM – Metric Tons of Initial Heavy Metal

MW - megawatt

MYRRHA – Multi-purpose hybrid research reactor for high-tech applications

NPI – Nuclear Physics Institute of the Academy of Sciences of the Czech Republic

NuMI – Neutrinos at the Main Injector

NWB – Nuclear Waste Burner

OMEGA – Options Making Extra Gain from Actinides and fission products

PEFP – Proton Engineering Frontier Project

PSI – Paul Scherrer Institut

PSR – Proton Storage Ring of the LAMF

SINQ - Schweizer Institut fur Nuklearforschung Quelle

SNS – Spallation Neutron Source in Oak Ridge, USA

SSNTD – Solid State Nuclear Track Detectors

SÚRAO – Správa úložišť radioaktivních odpadů (RAWRA - Radioactive Waste

Repository Authority)

TEF – Transmutation Experimental Facility of the J-PARC

TEF-P – Transmutation Physics Experimental Facility in TEF of the J-PARC

TEF-T – ADS Target Test Facility in TEF of the J-PARC

TIARA – Takasaki Ion accelerators for Advanced Radiation Application

TRIUMF – Tri-University Meson Facility

TSL – The Svedberg Laboratory of the Uppsala University, Sweden

UKAEA – United Kingdom Atomic Energy Autohority

XADS – eXperimental Accelerator Driven System

XIII

Table of contents

Introduction ....................................................................................................................... 1

1. Accelerator Driven Systems ......................................................................................... 3

1.1. Motivation for transmutation studies ..................................................................... 3

1.2. Transmutation ........................................................................................................ 7

1.3. Spallation reaction ................................................................................................. 8

1.4. History of accelerator driven systems .................................................................. 10

1.5. Modern spallation neutron sources ...................................................................... 11

1.6. Concepts of accelerator driven transmutation technologies ................................ 13

1.7. Spallation neutron sources for ADTT research ................................................... 13

1.8. Experiments focused on nuclear data measurements .......................................... 15

1.9. Summary of ADS research goals ......................................................................... 17

2. Energy and Transmutation of Radioactive Waste project .......................................... 19

2.1. Introduction to the E&T RAW project ................................................................ 19

2.2. Gamma-2 ............................................................................................................. 19

2.3. E+T setup ............................................................................................................. 20

2.4. Gamma-3 ............................................................................................................. 22

2.5. Kvinta setup ......................................................................................................... 22

2.6. EZHIK ................................................................................................................. 23

2.7. Placement of the E&T RAW targets .................................................................... 24

3. Experimental background ........................................................................................... 27

3.1. Activation detectors ............................................................................................. 27

3.2. Correction on decay of the isotope between the end of irradiation and beginning

of the measurement ............................................................................................. 31

3.3. Correction on decay during irradiation ................................................................ 32

3.4. Correction on the intensity of the I transition ..................................................... 33

3.5. Correction on dead-time of the detector .............................................................. 33

3.6. Correction on real - cascade coincidence ......................................................... 34

3.7. Correction on changed detector efficiency due to sample dimensions ................ 37

3.8. Self-absorption correction .................................................................................... 38

3.9. Square-emitter correction (geometrical correction) ............................................. 39

3.10. Beam instability correction ................................................................................ 42

3.11. HPGe detectors .................................................................................................. 43

3.12. DEIMOS32 program .......................................................................................... 48

3.13. Yield evaluation ................................................................................................. 50

3.14. Sources of uncertainties ..................................................................................... 52

3.15. Background ........................................................................................................ 54

4. Beam diagnostics on Nuclotron accelerator ............................................................... 55

4.1. Nuclotron accelerator ........................................................................................... 55

4.2. Irradiation course ................................................................................................. 58

4.3. Beam position and shape ..................................................................................... 60

4.4. Beam intensity ..................................................................................................... 65

XIV

5. E+T results of deuteron irradiation ............................................................................. 71

5.1. Plain experimental results .................................................................................... 71

5.2. Ratios of yields for different thresholds ............................................................... 75

5.3. Spectral indexes .................................................................................................... 77

5.4. Comparisons between deuteron experiments ....................................................... 79

5.5. Total neutron production ...................................................................................... 81

6. MCNPX simulations of the Energy plus Transmutation setup ................................... 85

6.1. MCNPX code ....................................................................................................... 85

6.2. Limitations of MCNPX code ............................................................................... 85

6.3. Simulation of the E+T setup................................................................................. 86

6.4. Neutron fluxes in the E+T setup .......................................................................... 87

6.5. Calculation of the yields in used activation foils ................................................. 89

6.6. Normalized experiment/simulation ratios ............................................................ 93

6.7. Yields for different beam particles of the same total energy ............................... 95

6.8. Summary of the MCNPX simulations ................................................................. 96

7. Cross-section measurements of the (n,xn) threshold reactions ................................... 99

7.1. State-of-the-art of the neutron cross-section libraries .......................................... 99

7.2. Limitations on neutron source ............................................................................ 100

7.3. EFNUDAT project ............................................................................................. 101

7.4. Quasi-monoenergetic neutron source at The Svedberg laboratory .................... 102

7.5. Cross-section estimation and planning of the experiment ................................. 105

7.6. Neutron beams at TSL ........................................................................................ 105

7.7. Quasi-monoenergetic neutron source at Nuclear Physics Institute .................... 106

7.8. Studied materials ................................................................................................ 109

7.9. Evaluation procedure .......................................................................................... 109

7.10. Background subtraction .................................................................................... 110

7.11. Uncertainty analysis ......................................................................................... 114

7.12. Discussion of the cross-section results ............................................................. 116

8. TALYS ...................................................................................................................... 119

8.1. Introduction to TALYS ...................................................................................... 119

8.2. Comparison among various models ................................................................... 119

8.3. Comparison between TALYS 1.0 and TALYS 1.2 ........................................... 123

9. Conclusion ................................................................................................................. 125

Appendix A - Threshold and non-threshold reactions on activation samples ............... 127

Appendix B - Placement of the foils during Energy plus Transmutation deuteron

experiments ................................................................................................................... 133

Appendix C - List of spectra measured in E+T deuteron experiments ......................... 137

Appendix D - Correction factor on beam instability ..................................................... 145

Appendix E - Examples of correction factors on real coincidences ............................. 147

Appendix F - Yields of isotopes produced on activation foils during 1.6 and 2.52 GeV

deuteron experiments on “Energy plus Transmutation” setup ...................................... 149

Appendix G - Graphs with yields of isotopes produced on activation foils in E+T

deuteron experiments .................................................................................................... 157

G.1. Longitudinal yields at 3 cm over the target axis ............................................... 157

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G.2. Radial yields in the first gap ............................................................................. 163

G.3. Spectral indexes ................................................................................................ 168

G.4. Ratios of the yield in dependence on the threshold .......................................... 170

G.5. Comparison between experiments .................................................................... 171

G.6. Ratios of the yields for various deuteron experiments ...................................... 174

Appendix H - Example of MCNPX input file – Au in 4 GeV deuteron experiment .... 177

Appendix I - Results of MCNPX simulations .............................................................. 189

I.1. Deuteron and proton spectra ............................................................................... 189

I.2. Experiment/simulation ratios .............................................................................. 190

I.3. Normalized experiment/simulation ratios .......................................................... 192

Appendix J - Cross-sections of threshold reactions from EXFOR and TALYS compared

with my data .................................................................................................................. 195

Appendix K - Comparison between TALYS 1.0 and TALYS 1.2 ............................... 211

Appendix L - Measured cross-section values ............................................................... 215

Appendix M - Equations of detector calibration for Excel Addin ................................ 219

Bibliography ................................................................................................................. 223

List of tables .................................................................................................................. 237

List of figures ................................................................................................................ 239

XVI

1

Introduction

Spallation reaction as a perspective source of neutrons has been studied with an

increased interest in the last two decades. These studies are motivated by the need of

high neutron fluxes for material research, transmutation of nuclear waste or production

of nuclear fuel from thorium. New spallation sources are planned (European Spallation

Source) or already commissioned (American Spallation Neutron Source) to fulfill

scientist requirements. With advances in accelerator technology Accelerator Driven

Systems, thanks to their high safety and unique properties, seem to be a perspective

energy source for the future.

This work is a part of the international research program Energy and

Transmutation of Radioactive Waste. Within this project, groups from 15 countries

study various aspects of spallation reaction, neutron production, transport and its usage

for transmutation of nuclear waste. Six different setups of massive target surrounded

with blanket and neutron moderator are used to measure differential as well as global

data for ADS (chapter 2). Three of the setups are already acknowledged as IAEA

benchmark targets.

This thesis is experimentally oriented and discusses results of deuteron

irradiations of the Energy plus Transmutation setup. This setup consists of a massive

lead target surrounded with natural uranium blanket and polyethylene biological

shielding. High energy neutrons from spallation reactions were measured using

activation detectors from Al, Au, Bi, Co, In, Ta, and Y materials. A detailed description

of used activation foils, reactions, HPGe detectors, and spectroscopic corrections is

written in chapter 3. Aluminum and copper activation foils were also used to measure

beam intensities, positions and shapes of all deuteron irradiations, details are stated in

chapter 4.

The (n,xn), (n,), and (n,p) threshold reactions have been used to distinguish

neutrons with different energies. Non-threshold (n,) reactions with combination of

polyethylene shielding have been used to assess total number of produced neutrons.

Experimental results and comparisons are in chapter 5. This thesis carries on the work

of my colleagues Antonín Krása and Mitja Majerle, who studied in their PhD theses

properties of the Energy plus Transmutation setup irradiated with proton beams. The

main aim of this work is to study the high energy neutrons in already well known setup

irradiated with different (deuteron) beams. Various spectroscopic corrections are

studied and routinely applied for the first time in order to produce more precise results.

Experiments have been performed using the Nuclotron Accelerator at the

Veksler and Baldin Laboratory of High Energy Physics of the Joint Institute for Nuclear

Research (JINR) in Dubna, Russia. Energy plus Transmutation setup was irradiated

with deuterons of 1.6, 2.52, and 4 GeV. Irradiated foils were measured using HPGe

detectors at JINR and Nuclear Physics Institute (NPI) of the Academy of Sciences of

the Czech Republic (ASCR). MCNPX simulations of the experiments were done and

calculated data was compared with the experimental data in chapter 6.

2

After a long time of using threshold detectors at NPI there appeared a

opportunity to measure their cross-sections in the energy regions where no data had

existed so far. Up to now only calculated cross-sections were used for the reactions over

40 MeV or order of reaction higher than (n,4n). With the financial support from

European Facilities for Nuclear Data Measurements grant organization (EFNUDAT)

quasi-monoenergetic neutron source at The Svedberg Laboratory (TSL) at Uppsala,

Sweden, was used. Three irradiations with energies 22, 47, and 94 MeV were performed

in June 2008. They were supplemented with 17, 22, 30, and 35 MeV irradiations on

similar neutron source at NPI Řež. A detail description of used neutron sources,

evaluation procedure and neutron background subtraction as well as cross-section

results can be found in chapter 7.

The analysis of the deterministic code TALYS which was used for the neutron

background subtraction at cross-section measurements is presented in Chapter 8. Two

versions of TALYS (1.0 and 1.2) are compared, the same as different settings of the

TALYS code. Their influence on the amount of subtracted background and thus on

cross-sections is discussed.

The summary of the main goals of PhD thesis is following:

prepare, perform and evaluate 1.6 GeV and 2.52 GeV deuteron experiments on

the E+T setup,

study and apply spectroscopic corrections needed for the data evaluation,

measure the beam intensities, positions and shapes during 1.6 GeV and 2.52 GeV

deuteron experiments on the E+T setup, provide the results to the whole E&T

RAW collaboration,

compare experimental results within each experiment, between deuteron

experiments and with previous proton experiments performed on the E+T setup,

perform MCNPX simulation of deuteron experiments, make comparisons between

experimental and simulated data,

prepare, perform and evaluate cross-section measurements of (n,xn) threshold

reactions used for high energy neutron measurements in the E+T setup, namely

TSL experiments at 22, 47, and 94 MeV and NPI experiments at 17 and 22 MeV.

Beside these PhD goals I have voluntarily worked on some topics of the 4 GeV

deuteron experiment. I also show in my PhD thesis these data because they supplement

deuteron systematics on the Energy plus Transmutation setup.

This thesis was written with respect to its potential users from the Energy and

Transmutation community as well as to other students from Nuclear Physics Institute of

the ASCR, who are interested in this field of physics. In the work there are maybe more

detailed descriptions and examples than would be necessary for the PhD work, but I

tried to present a clear description of all the aspects of my work in order to enable easier

continuation in these studies. With the constituency of the readers is connected also the

choice of used language.

3

Chapter 1

Accelerator Driven Systems

1.1. Motivation for transmutation studies

First nuclear reactor was started on December 2nd

, 1942, almost 70 years ago.

Since that day, nuclear industry has undergone an amazing evolution. Nowadays, 437

energetic nuclear reactors produce 371 GWe (14% of electricity consumption) and

56 new reactors are under construction [1]. Rising demand on electricity and worldwide

efforts on decrease of carbon dioxide emissions, as well as the oncoming insufficiency

of crude oil will push nuclear industry forward in the next decades. After the gas crisis

in the Central Europe in 2009, politically independent energy sources start to have

a high importance in many countries. Nuclear energy can be completely independent at

least in the period of several years.

After the Chernobyl accident, a strong public opinion against the nuclear energy

developed all over the world. Some countries even closed their nuclear power plants

and become non-nuclear. Today, public meaning is slowly changing and nuclear energy

is acceptable for most people under fulfillment of the following rules:

- any serious accident with effects outside the power plant area must be reliably

excluded,

- proliferation of nuclear materials (enriched uranium in fresh fuel, plutonium in

spent fuel, fission products etc.) must be out of question due to combination of

technical and organizational rules,

- time of nuclear power plant construction should by adequate, price of nuclear

energy must be comparable to other energy sources,

- question of spent fuel and high level radioactive waste generally must be reliably

solved out.

The last demand has not been fully solved out up to now. The total amount of

spent fuel that has been discharged globally is approximately 320 000 tones of heavy

metal (HM). There are nowadays three possible ways how to handle spent fuel – store

it in geological repositories, reprocess it and store only currently unusable items or

involve transmutation after the reprocessing.

Geological repositories are one of the possibilities, which cannot be omitted in

any scenario of spent fuel handling. Geological repository is a final storage place build

deep under the earth surface in suitable rock formation. Special attention is paid to the

stability and compactness of the rock massive, same as on the presence of underground

water. Dense urban settlements nearby the location as well as the presence of valuable

resources in the rock limit the choice of the repository site.

Underground repository is based on the principle of multiple physical barriers

that should stop potential leak of stored radioactive materials without future human

1. ACCELERATOR DRIVEN SYSTEMS

4

assistance. Barriers should also ensure safety to future generations, they should

embarrass the manipulation with such dangerous materials. Life-time of the deep

underground repository is planned to be long enough to let most of the stored

radionuclide to decay and to decrease the activity below the natural background level.

Figure 1: Geological repository for nuclear waste [2].

Originally it was planned to store whole used fuel rods in the underground

repository. This approach poses the easiest and safest way of spent fuel removal, but its

massive usage is nowadays improbable because of its unthrift. Reactors can currently

use only 3 – 4 percents of the total energy contained in the fuel. These 3 – 4 percents of

the fuel represents “ash” after the nuclear “burning”, mainly high active fission products

(most important fission products are summarized in the Table 1 bellow). These

radioisotopes cannot be further used and must be separated from the biosphere for a

long time (or transmuted). Vitrified fission products are nowadays the most probable

content for underground repositories, when they will be opened in the second half of the

21st century.


5

Table 1: Annual production of the most important transuranides and fission fragments

in light water reactor of thermal power 3000 MW [3].

Transuranides Production Half-life Fission Production Half-life

kg/year [years] fragment kg/year [years] 238

Pu 4.52 88 79

Se 0.17 6.5·104

239Pu 166 2.4·10

4

85Kr 0.39 10.7

240Pu 76.7 6.6·10

3

90Sr 13.4 28.8

241Pu 25.4 14.4

93Zr 23 1.5·10

6

242Pu 15.5 3.8·10

5

99Tc 25 2.1·10

5

237Np 14.5 2.1·10

6

107Pd 7.3 10.5·10

6

241Am 16.6 423

126Sn 0.96 1.0·10

5

242Am 0.022 141

129I 5.8 1.6·10

7

243Am 2.99 7.4·10

3

135Cs 9.4 3·10

6

243Cm 0.011 28.5

137Cs 32 30

244Cm 0.58 18.1

151Sm 0.4 90

Another limitation for the final deposition of spent fuel in the geological

repository is a residual heat production. Energy released in the decay of radioactive

isotopes is finally converted into heat, which must be safely diverted. In the first years,

spent fuel must be cooled in water nearby the reactor, otherwise it would melt. Later it

can be stored under a gas atmosphere, but heat removal must be still ensured. In the

geological repository, containers with spent fuel (or vitrified fission products) are

planned to be buried in bentonite with rock around, so the heat production at that time

must be smaller than the possible heat removal by conduction in used materials. Main

heat sources in spent fuel are displayed in following Figure 2. Goal of the research is to

eliminate components of the nuclear waste stream that account for the majority of the

heat load and toxicity over the 300 to 10 000 year time frame.

Build-up and operation of geological repository is a long-distance run, it can

take up a century until the repository site will be fully closed. Most of the states that use

nuclear energy are in various stages of the repository build up. The Swedish Nuclear

Fuel and Waste Management Company (SKB) selected locality Östhammar as the site

for a final spent fuel geological repository, following a nearly 20 year process that

narrowed the list of applicant sites to two in 2002. Site investigations for repositories at

Olkiluoto in Finland and in the Bure region in France continued on the schedule with

operation targeted for 2020 and 2025, respectively. In the USA, the Government

decided to terminate its development of a permanent repository for high level waste at

Yucca Mountain. It plans to establish a commission to evaluate alternatives. In the UK,

a voluntary sitting process has been initiated, as well as in many other countries.

Czech Republic stacks in the process of repository site selection. Initial study of

six localities with similar geological underground as in Sweden or Finland was finished,


6

new locality is studied inside former military area Boletice. Start of the repository

construction is planned beyond the year 2050 and operation after 2065 [4].

Figure 2: Dominant decay heat contributors in spent PWR fuel irradiated to 50

GWd/MTIHM [5]. The isotopes circled in red are the major contributors to the decay

heat in 300 to 10 000 year time frame. If these isotopes are removed then the solid blue

line shows the decay heat of the remaining waste; the green dashed line shows the time

at which the surface temperature of the waste container is below the boiling point of

water; and the blue dashed line gives the time at which the waste radiotoxicity is below

Class C nuclear waste1.

About 97 percent of the spent fuel contains uranium and plutonium, which can

be reused after the reprocessing. Up to now, 95 000 t of HM spent fuel were already

reprocessed. Total global reprocessing capacity is about 5000 t of HM per year.

Uranium gained from the reprocessing can be again enriched and fabricated to the fuel.

Cumulated amount of plutonium possesses a safety risk, so there is a rising interest in

the use of MOX fuel (mixed oxide fuel with uranium-235 partially replaced by

plutonium-239). At the beginning of the year 2010 there was a 250 t HM MOX fuel

fabrication capacity and 31 thermal reactors licensed for MOX fuel use in the world.

1 USA definition of radioactive waste classification, Class C is similar to Czech definition of low level

waste


7

Higher actinides contained in the spent fuel cannot be effectively burned in

present types of reactors. Higher actinides can be most efficiently eliminated through

nuclear transmutation using high intensive fields of fast neutrons.

1.2. Transmutation Transmutation is, generally said, every reaction, in which the composition of the

atom nucleus is changed. Nuclei differ apart not only in the number of protons that

defines the element, but they differ also in the number of neutrons. Neutrons impress

besides other the stability of the nucleus. Adding or removing of a neutron can lead to a

dramatic change in the nucleus, a new (stable) element can be produced in the following

decay.

Transmutation reactions are quite common in the nature. Production of 14

C and

tritium production in the upper parts of atmosphere can be introduced as an example of

cosmic rays induced transmutation reactions.

HCnN 1

1

14

6

14

7 HCnN 3

1

12

6

14

7

In 1951 Sir John D. Cockroft and Ernst T. S. Walton obtained the Nobel Prize

for discovery of the transmutation of atom nucleus by accelerated particles.

Fission products in the burned-up fuel are mostly -radioactive with a short half-

life. Only a few of them are long-lived. To make these materials stable, multiple neutron

absorption and consequent nucleus decay or fission is needed. Typical example can be

the 99

Tc with the half-life 2.1 · 105 years.

Figure 3: Transmutation of 99

Tc [6].

Plutonium and higher actinides which cannot be easily fissioned in thermal

reactor can be also transmuted. A single neutron capture can change a non-fissile

nuclide to a fissile one, which can be consequently fissioned in proper neutron

spectrum.

Basic physical requirement for successful transmutation of long lived waste is

highly intensive field of neutrons. High transmutation rates can be achieved by

combination of high neutron intensity, proper neutron energy and reaction cross-section.


8

Main difficulty of the transmutation is thus in ensuring strong neutron field of proper

energy. Spallation reaction is an ideal source of such neutrons.

1.3. Spallation reaction Spallation reaction is a process, in which a relativistic light ion (proton, deuteron

or heavier nucleus) interacts with a massive heavy metal target, resulting in the breakup

of the heavy nucleus and in production of wide range of new particles. Substantial parts

of these particles are neutrons with relatively high energy. Number of these neutrons

depends on the energy and mass of the interacting ion and on the target material.

Spallation reaction can be divided into a few stages. Spallation starts with the

accelerated proton (for example) interacting with the target nucleus of heavy element

(e.g. Pb). The proton penetrates the target nucleus, and distributes its energy to a few

nucleons of the nucleus. This stage is called intra-nuclear cascade. Target nucleus is

afterwards in highly excited state and undergoes a pre-equilibrium emission of particles

and photons. Particles are at this stage of process emitted unisotropicaly, most of them

in the forward direction. After this emission, energy is in the nucleus uniformly

distributed, but the nucleus is still highly excited. Such a nucleus can than disintegrate

or massively evaporate particles and photons to lower its energy. Particle and photon

production is isotropic in this phase.

Neutrons occurring in the spallation reaction can have a wide range of energies

(see e.g. Figure 63 in chapter 6 section 4). Highest energy of the neutrons can reach up

to the energy of the particles in the incident beam. In the low energy part of the

spectrum number of neutrons is decreasing significantly below the energy one MeV. In

order to produce intense thermal neutron fluxes various moderators must be used.

Figure 4: Principal schema of the spallation reaction [7].

1.3. Spallation reaction

9

With growing energy of the primary particle, course of the reaction substantially

changes. In the energy interval 0.02 – 2 GeV all interactions are only on the level of

nucleons. Towards higher energies, other reaction channels are opening and new

particles are produced in the nucleon-nucleon interactions. In the region hundreds of

MeV first pions are produced, at 2 – 10 GeV heavier hadrons occur. Produced particles

can further interact with other nuclei and a hadron showers are developed.

First on the list of the accelerated particles used in the spallation sources are

protons. Their accelerating is efficiently managed and commonly used process. Most

effective energy of the protons used for spallation lies in the region 800 – 1000 MeV,

where the neutron production per MeV per particle has its maximum. A little better

situation is for deuterons; they have the same ionization losses (at the same energy per

nucleon), but bring twice the amount of energy into the target. On the other hand,

deuteron acceleration is more complicated process resulting in lower beam intensities.

Very important for the spallation neutron sources is target material selection.

Target material must fulfill a wide range of criteria, often contradictory. Suitable target

material must have at first good spallation properties - high atom number and density.

Moreover good thermal conductivity, low melting point for liquid targets or high

melting point for solid targets, generally high boiling point, low activation and only

short-lived activation products are required.

Target materials for high power ADS can be sorted into three groups:

a) liquid non-fissionable targets

Targets in the form of molten material – Hg, Bi, Pb or eutectics. Main advantage

of this conception represents the cooling of such a target, liquid metal can

circulate and outer cooling loops can be used. On the other hand, both heavy

metals (Bi and Pb) produce long lived products when being irradiated (205

Pb –

1.53(3)·107 years,

208Bi – 3.68(4)·10

5 years,

210Bi – 3,04(6)·10

6 years).

b) solid non-fissionable targets

Tantalum or wolfram metal formed to wafers. After the irradiation these

materials show low radioactivity and residual heat. Wolfram has one of the

biggest densities from considered materials – 19.3 g/cm3.

c) solid natural uranium or thorium

Targets from fissionable materials offer some fast neutron bonus through the

fission. Among disadvantages can be named high cross-section for neutron

absorption and production of long-lived radioisotopes (e.g. 236

U – 2.342(3)·107

years). In some scenarios the transmuted material is placed directly into the

target.


10

Table 2: Overview of the properties of the most convenient materials for the spallation

targets [8].

Isotope Z Relative

atomic mass

Density

[g/cm3]

Melting

point

[oC]

Boiling

point

[oC]

Heat

capacity

[Jg-1

K-1

]

Heat

conductivity

[Jcm-1

s-1

K-1

]

Ta 73 180.9479 16.654 3017 5458 0.142 0.578

W 74 183.84 19.3 3422 5555 0.134 1.88

Pb 82 207.2 11.35 327.46 1749 0.13 0.347

Bi 83 208.9804 9.747 271.4 1564 0.142 0.083

Th 90 232.0381 11.72 1750 4788 0.117 0.377

U 92 238.0298 18.95 1135 4131 0.117 0.268

Np 93 (237) 20.25 644 3902

Pu 94 (244) 19.84 640 3228

Am 95 (243) 13.67 1176

1.4. History of accelerator driven systems Accelerator driven systems - ADS (including also accelerator driven

transmutation technologies – ADTT) come out from following four main research

directions:

a) ATW (Accelerator Transmutation of Waste) proposed by C. D. Bowman [9] and

developed in Los Alamos, USA. Main aim of this project is to substantially shorten the

half-life of the isotopes in the spent fuel by means of transmutation.

b) ADEP (Accelerator Driven Energy Production) or Energy Amplifier (CERN

project) [10] – idea of C. Rubbia is based on the fission of 233

U. This isotope of uranium

would be produced from thorium in the following reactions:

eUPa

ePaTh

ThThn

d

m

233967,26233

2333,22233

233232

Thorium is the fortieth most frequent element in the Earth crust. Few states

headed by India and China have thorium resources, but lack of uranium or fossil fuels to

meet their energy needs. Problem in usage of thorium is in the need of neutron source at

the beginning of the 233

U production process, one needs something to start the breeding

reaction. Spallation source as a representative of a strong neutron sources can be one of

the solutions.

c) APT (Accelerator Production of Tritium) [11] – tritium was formerly used in

fusion bombs. Nowadays, there starts to be a strong demand from the fusion community

as the tritium is important fuel in fusion reactors.

1.4. History of accelerator driven systems

11

d) ABC (Accelerator Based Conversion) [11] – accelerator steered conversion of

plutonium was proposed to liquidate huge plutonium resources from the reprocessing

and nuclear weapon programs. Practical use of this research is nowadays less probable

thanks to MOX fuels and development of new reactor types, but in the past it was one

of the important branches of accelerator driven systems research.

1.5. Modern spallation neutron sources At the beginning of 2010, there were nine spallation neutron sources distributed

in five countries. Another 50 synchrotron light sources of neutrons are located in over

20 countries [1]. Most of these neutron sources are used for material science and in

related branches.

Neutron scattering is one of the most effective ways to obtain information on

both, the structure and the dynamics of condensed matter. A wide scope of problems,

ranging from fundamental to solid state physics and chemistry, and from materials

science to biology, medicine and environmental science, can be investigated with

neutrons. Aside from the scattering techniques, non-diffractive methods like imaging

techniques can also be applied with increasing relevance for industrial applications.

In last decade, new international workplaces with intense spallation neutron

sources are being built or planed, below is a list of the most important and strongest

ones.

European spallation source (ESS)

European spallation source is a project, which involve partners from 16

countries. Now it is in the pre-construction phase, in 2012 should start the build-up

phase. Spallation source should be commissioned in 2019 and fully operational in 2025

with total cost 1.48 billion Euro [12].

Spallation Neutron Source (SNS)

American spallation neutron source located in Oak Ridge National Laboratory is

nowadays the world‟s most advanced high flux neutron source for material science. It

was launched in 2006 and offers 18 beam lines to 25 different experiments [13]. Linear

accelerator provides 1 GeV H- beam of 1.4 MW to the mercury target (beam current is

1.4 mA, repetition rate 60 Hz). Facility holds Guinness World Record for the most

powerful pulsed spallation neutron source.

Japan Proton Accelerator Research Complex (J-PARC)

In Japan Proton Accelerator Research Complex a mercury target irradiated by 3

GeV H- beam is used to produce neutrons. Current in pulsed proton beam can be up to

0.333mA, but total power deposited in current type of target is only 0.12 MW. Neutrons

are guided to various experiments in Material & Life Science Experimental Facility

(MLF) [14].

Spallation neutron source SINQ

Spallation neutron source SINQ is situated in Paul Scherrer Institut (PSI),

Switzerland. Cascade of three accelerators deliver protons with energy 0.59 GeV at a


12

current up to 2.3 mA [15]. Target is an array of lead rods enclosed in zircaloy tubes and

cooled by heavy water. SINQ is designed as a neutron source mainly for research with

extracted beams of thermal and cold neutrons, but hosts also facilities for isotope

production and neutron activation analysis.

China Spallation Neutron Source (CSNS)

China started to build their own spallation neutron source in May 2010 and plan

to have first neutrons in 2015 [16]. It will be based on 1.6 GeV H- beam at 25 Hz

repetition rate and 0.125 MW power in the first stage (up to 0.5 MW in the third stage).

Total cost of the facility is about 293 million US dollars.

India Spallation Neutron Source (ISNS)

India plans also to build its own spallation neutron source in near future. It will

be based on the experiences gathered at existing high flux spallation neutron sources.

Proposed parameters are 1 GeV proton beam on lead target, average beam current

0.1 mA at 25 Hz [17].

There is a long row of less powerful and older, but still excellent spallation

neutron sources. For example, at Los Alamos National Laboratory - USA, meson

physics facility (LAMPF) is working since 1977. At Rutherford Appleton Laboratory in

Oxfordshire – UK, ISIS pulsed neutron and muon source is used since 1985 [18].

Overview of spallation neutron sources from the beam power point of view is on the

following Figure 5.

Figure 5: Current powerful proton accelerators, SP - short pulsed, CW – continuous

wave, LP – long pulsed [19]. Acronyms are described in the list of abbreviations.

1.6. Concepts of accelerator driven transmutation technologies

13

1.6. Concepts of accelerator driven transmutation technologies

ADTT (Accelerator Driven Transmutation Technology) can be a future solution

for the rising amount of high-level nuclear waste from the nuclear reactors, as well as a

new source of energy. It is a combination of a subcritical reactor with an accelerator.

The basic principle is in production of a large number of high energy neutrons in the

spallation process (relativistic ions + heavy metal target), and their multiplication in

sub-critical blanket. In dense field of high energy neutrons lot of actinides and/or fission

products can be burned or effectively transmuted to short lived products. This approach

can minimize demands on the geological repository. Dense neutron field can be also

used to produce fuel from 232

Th. The main advantage of this technology is its safety;

switch off of the accelerator means a switch off of the system (with proper design there

can hardly be a criticality accident).

Figure 6: Scheme of the typical ADS proposal [20].

1.7. Spallation neutron sources for ADTT research In last decade, three main experiments with spallation neutron sources were

started and they were focused on future transmutation use of the accelerator driven

systems. Megapie experiment described below studied the behavior of a target under

extreme thermal and radiation load. TEF experiment in J-PARC studies behavior of

subcritical ADS under various beam conditions. Planned project MYRRHA will

combine both directions.


14

Megawatt Spallation Target Pilot Experiment (Megapie)

Megawatt Spallation Target Pilot Experiment was the first project, where the

target had the full power load as it is considered for the future ADS systems.

Experiment was involved in the Fifth Framework program of the European Union.

Megapie was an experiment aiming to demonstrate the safe operation of a liquid

metal spallation target at a beam power level of 1 MW in the SINQ target station at the

Paul Scherrer Institut (PSI). It was running successfully for four months and

accumulated total charge 2.8 Ah [21]. Now the decommissioning of the target is

ongoing.

Transmutation Experimental Facility (TEF) in J-PARC

Transmutation Experimental Facility (TEF) is situated in Japan Proton

Accelerator Research Complex. It consists of two experiments: Transmutation Physics

Experimental Facility (TEF-P) and ADS Target Test Facility (TEF-T) [22]. TEF-P is

equipped with a critical assembly to investigate physical and dynamic properties of the

accelerator-driven system by using low power (10W) proton beam. Uranium, plutonium

and minor actinide fuels are planned to be loaded into the assembly. TEF-T is a facility

to examine the existence of ADS (Accelerator-driven System) by engineering

viewpoint. Liquid lead-bismuth spallation target is installed to the TEF-T and is

irradiated by 600 MeV-0.2 MW proton beam.

Multi-purpose hybrid research reactor for high-tech applications (MYRRHA)

SCK CEN, the Belgian Nuclear Research Centre in Mol is the home institute of

the MYRRHA project. It will be a multi-purpose hybrid research reactor for high-tech

applications. It should replace ageing BR2 reactor, a multi-functional material testing

reactor that is in operation since 1962.

MYRRHA will be a flexible fast spectrum research reactor (50-100 MWth), it is

conceived as an accelerator driven system (ADS), able to operate in sub-critical and

critical modes. It contains a proton accelerator of 600 MeV, a spallation target and a

multiplying core with MOX fuel, cooled by liquid lead-bismuth (Pb-Bi). Construction

of the facility is foreseen in the period 2015-2019, full operation by 2023 [23].

There can be stated a long row of ADS experiments and facilities with focus on

transmutation that were proposed and developed in the past, but never transformed into

real scientific facility. With the development of new Generation IV reactors and mainly

molten salt reactors there is an evident decrease in the interest in ADTT. This is

connected also with the funding, so only a few projects have survived. Examples can be

found in the Table 3.

1.7. Spallation neutron sources for ADTT research

15

Table 3: Parameters of different ADS projects [24]. Acronyms are explained in the list

of abbreviations.

Project / CountryAccelerator / blanket

power [MW]keff

Flux / spectrum

[n/cm2s]

Target Fuel References

ABC-ADTT-ATW

-AFCI (USA)

4.8 / 250

(800 MeV, 6 mA)0.95 Thermal Pb ThU

DOE/RW(1999), 0519.

Oct, OECD/IAEA (2005)

Status Report, 5421

OMEGA

(Japan 1997)

58 / 820

(1.5 GeV, 39 mA)0.9 4x10

15 Fast W Np/5Pu/30Zr

Nakamura et al. (1992),

Takizuka et al. (1997)

JAERI-ADS

(Japan 2004)

27 / 800

(1.5 GeV 18 mA)0.97 Fast Pb-Bi MA/Pu/ZrN

Ikegani et al.(2004),

Kikuchi et al. (2004)

HYPER

(Korea)

15 / 1000

(1 GeV, 10 - 16 mA)0.98 Fast Pb-Bi Ma/Pu Yoo (2004

XADS Design A

(Italy)

3.6 / 80

(600 MeV, 3 - 6 mA)0.95 - 0.97 10

15 Fast Pb-Bi U/Pu/MOX Abderrahim et al. (2004)

XADS Design B

(France)

3.6 / 80

(600 MeV, 3 - 6 mA)0.95 - 0.97 10

15 Fast Steel U/Pu/MOX Abderrahim et al. (2004)

XADS Design C

(Belgium)

1.75 / 50

(350 MeV, 5 mA)0.95 3x10

15 Fast

Pb-Bi

windowlessU/Pu/MOX Abderrahim et al. (2004)

INR

(Russia)

0.15 / 5

(500 MeV, 10 mA)0.95 - 0.97 Fast W MA/MOX Markov et al. (2003)

NWB

(Russia)

3 /100

(380 MeV, 10 mA)0.95 - 0.98 10

14 - 10

15 Fast Pb-Bi

UO2/UN

U/MA/ZrPavlopoulos et al. (2003)

CSMSR

(Russia)

10 / 800

(1 GeV, 10 mA)0.95

5x1014

IntermediatePb-Bi

Np/Pu/MA

molten salt

Degtyarev et al.

(2005, 2006)

From US projects mentioned in the Table 3 only the Spallation Neutron Source

(SNS) was finished up to now. ATW project was postponed due to its inutility. Japan

projects are further developed in the JAERI under the TEF facilities. HYPER project in

South Korea was closed in 2006. Italian and French XADS (eXperimental Accelerator

Driven System) stayed up to now only in the planning phase. Belgium XADS project

developed into European project called MYRRHA with start of construction in 2015.

All three Russian projects were stopped in the planning phase because of the lack of

money.

1.8. Experiments focused on nuclear data measurements Cross-sections of various reactions are of fundamental importance for future

ADS. Many construction materials, which are nowadays commonly used in nuclear

reactors, will be exposed to extreme neutron fluxes of high energies. At this region of

energies, only very few cross-sections are known. Precision of cross-section knowledge

is even more important for materials of transmutation interest. Bad knowledge of cross-

sections and properties of nuclear reactions in general can lead in production of even

longer-lived isotopes than is the transmuted one or at least to low transmutation rates.

On the other hand, with good knowledge of cross-sections and thus proper choice of

neutron energy and time of irradiation, negative effects can be minimized or eliminated.

A few international initiatives were established to gain nuclear data for future

ADS. Within the Fifth Framework Programme (FP5) of the European Union

following researches were done [25]:


16

Thorium Cycle project

Thorium cycle project coordinated by Nuclear Research and Consultancy Group

from Netherlands was focused on the measurement of key data for thorium fuel cycle in

reactors and ADS systems. Various mixtures of Th/Pu fuel were studied under high

burn-up in order to decrease its long-term radioactivity and thus demands on geological

repositories.

CONFIRM

CONFIRM project was collaboration on Nitride Fuel Irradiation and Modeling.

Research was oriented on the oxide and nitride ADS fuels without uranium. Special

design of fuel pellets was developed in order to reach extremely high burn–up. Special

attention was paid to safety parameters of the fuel, which must be fulfilled through

whole fuel irradiation. Coordinator of this project was Royal Institute of Technology

from Stockholm, Sweden.

HINDAS

High and intermediate energy nuclear data for accelerator-driven system

(HINDAS) was European project focused directly on nuclear data. Experimental data

were measured on various accelerators throughout Europe. Nuclear models were

improved according to experimental data. Energy scope of the HINDAS project was on

energies from 20 to 2000 MeV. Libraries of nuclear data were extended up to 200 MeV

(format ENDF was used).

n-TOF

The neutron time-of-flight facility (n-TOF) has been developed in the European

Organization for Nuclear Research (CERN) since 2001. Time-of-flight method with fly

path 200 meters is used to determine energy of the neutrons. The main goal of the

project is to produce, evaluate and disseminate high precision cross sections for the

majority of the isotopes relevant to the waste incineration and the ADS design.

The Sixth Framework Programme [26] followed in the support of various

research activities related to ADS and transmutation. Direct relation to the ADS has

following four sub-programmes:

EUROTRANS (EUROpean Research Programme for the TRANSmutation of High

Level Nuclear Waste in a Accelerator Driven System).

EUROPART (EUROpean Research Programme for the Partitioning of Minor

Actinides).

EFNUDAT (European Facilites for Nuclear Data Measurements). We used this

programme to get access to the quasi-monoenergetic neutron source in The Svedberg

laboratory in Uppsala, Sweden. More details about this programme are described in the

chapter 7 Section 3.

1.8. Experiments focused on nuclear data measurements

17

RED IMPACT (Impact of Partitioning, Transmutation and Waste Reduction

Technologies on the Final Waste Disposal Project).

1.9. Summary of ADS research goals Research of various ADS aspects continues nowadays both on simple setups and

experiments, and on more complicated assemblies. Simple setups are used to measure

the cross-sections of GeV down to MeV neutrons, and to study the spallation reaction

and high energy neutron transport in more detail. More complex systems verify neutron

multiplication, transmutation rates, heat production, long-term stability and overall

suitable concepts for future XADS. Special attention starts to be paid to the engineering

problems in construction of future ADS systems.

There is also increasing motivation towards improving the precision of

predictions of the codes used to simulate production and transport of high-energy

spallation products in material. More realistic simulations will help to design more

effective spallation neutron sources, subcritical blankets or better radiation shielding.

Good codes can also spare budget in all stages of ADS life. But for codes development

and improvements, a lot of real experimental data for comparisons and benchmark tests

is needed.

My research in the field of accelerator driven systems involves both the simple

and complex experiments. The simple experiments are represented by the neutron cross-

section measurements of the (n,xn) threshold reactions. Spallation experiments on the

Energy plus Transmutation (E+T) setup belong to the complex experiments. Series of

experiments of both types are described and compared with simulations in the following

chapters.


18

19

Chapter 2

Energy and Transmutation of Radioactive Waste project

2.1. Introduction to the E&T RAW project There is a long tradition of spallation and high energy neutron studies in the

Joint Institute for Nuclear Research (JINR Dubna, Russia). During the 1980s and 1990s,

wide range of spallation targets was irradiated and the neutron production was studied

with the respect to the target shape, dimensions, material and to the surrounding

volumes. This aim culminated at the end of 1990s in the Energy plus Transmutation

(E+T) project. The leader of this project was for almost last two decades M. I.

Krivopustov, who established a big international team with interest in transmutation

studies. Target systems Gamma-2, Energy plus Transmutation and Gamma-MD were

developed and irradiated with protons and deuterons from the Nuclotron accelerator.

Since 2009, M. Kadykov has been a new leader of the collaboration. The

collaboration was renamed to Energy and Transmutation of Radioactive Waste (E&T

RAW) and got a better position in the JINR structure, so a further development is

foreseen. Collaboration is still growing and has nowadays approximately 85 members

from 15 countries (Armenia, Australia, Bulgaria, Czech Republic, Poland, Germany,

Russian federation, Belarus, Ukraine, Mongolia, Serbia, Kazakhstan, Greece, India, and

Moldova). Two new target systems are developed, the first setup called Kvinta was

already tested in experiment, the second setup called Ezhik is in the phase of technical

design.

Focus of our group from Řež is on high energy neutron measurement and beam

diagnostics. We use so called reversed activation neutron detectors – we put foil of a

known isotope into unknown neutron field. Energy range of studied neutrons is from 5

up to about 80 MeV. Other groups from the collaboration use activation analysis on

different isotopes, solid state nuclear track detectors (SSNTD), He-3 counters and

nuclear emulsions to study other parts of the neutron spectrum.

E&T RAW targets will be described shortly in the following sections. Main

physical purpose of all targets is to study spallation reactions caused by GeV protons

and deuterons, transport of high energy neutrons and transmutation. Use of various

target and blanket materials, geometries and surrounding moderators enables to study

their influence on neutron field. Systems have a big advantage in possibility of

measuring integral data – transmutation rates of actinides in real spallation field.

GAMMA-2, E+T and GAMMA-3 setups were introduced into a Coordinated Research

Project of IAEA and these targets are now acknowledged as “IAEA benchmark targets”.

2.2. Gamma-2 Gamma-2 setup consists of a lead target 8 cm in diameter and 20 cm long. Later

the target was prolonged to 50 cm. It is surrounded with paraffin moderator of 6 cm

thickness. Gamma-2 setup was irradiated with protons in the energy range 0.5 –

2. ENERGY AND TRANSMUTATION OF RADIOACTIVE WASTE PROJECT

20

4.15 GeV [27], respectively 1 – 2 GeV at the prolonged version [28]. Main

experimental task of this setup was a study of spallation reactions and transport of high

energy neutrons. First measurements with radioactive samples and their transmutation

in the field of moderated neutrons were done. Scientific program on this target was

more or less closed, but the target will be still ready for new irradiations if there is a

need.

Figure 7: Gamma-2 setup consisting of lead target (discs) and paraffin moderator.

2.3. E+T setup Further step in the transmutation studies was a more complex target system

called “Energy plus Transmutation” setup (E+T setup). Setup was irradiated with 0.7, 1,

1.5, and 2 GeV protons, results of 1.6, 2.52, and partly 4 GeV deuteron irradiations are

the main topic of this PhD thesis, that is why I will describe the target in more detail.

The 0.7 GeV proton experiment was a subject of my diploma thesis [29], results of all

proton experiments were the main subject of successfully defended PhD thesis of

A. Krása [30]. Results concerning the proton experiments were also published as JINR

Preprints [31], [32], [33], [34]; and presented on many conferences and workshops.

The E+T setup consists of a cylindrical lead target (diameter 84 mm, total length

480 mm) and a surrounding subcritical uranium blanket (206.4 kg of natural uranium).

Target and blanket are divided into four sections. Between the sections there are 8 mm

gaps for user‟s samples, detectors and emulsions. Each section contains target cylinder

114 mm long and 30 identical natural uranium rods, which are secured in a hexagonal

steel container with a wall thickness of 4 mm. The front and back of each section are

covered with hexagonal aluminum plate 6 mm thick. The four target-blanket sections

are mounted along the target axis on a wooden plate of 68 mm thickness, which is

moreover covered with 4 mm thick steel sheet. Uranium rods are hermetically

encapsulated in aluminum coverage of thickness 1 mm, respectively 2 mm at the bases.

Each rod has an outside diameter of 36 mm, a length of 104 mm, and a weight of

1.72 kg. Density of the uranium is considered to be 19.05 g·cm-3

.

Around the blanket, there is a radiation shielding consisting of a wooden box,

cadmium plates and polyethylene ((CH2)n) in the box walls. Cadmium plates have

thickness of 1 mm and are mounted on the inner walls of the box. Polyethylene has a

2.3. E+T setup

21

density of 0.8 g·cm-3

and is granulated. On the floor inside the shielding box a 38 mm

thick textolite2 plate is placed. Shielding moderates and absorbs only a part of the high

energy neutrons emerging from the setup, so there is a dosimetry limit on the beam flux.

Figure 8: Cross-sectional side view (left) and front view (right) of the "Energy plus

Transmutation" setup. All dimensions are in millimeters.

Figure 9: Photo of the Energy plus Transmutation setup with the biological shielding

(left). Detail of the natural uranium blanket (right).

2 Textolite (Latin textus – a cloth, and Greek lithos – stone) is a material consisting of several layers of

fabric (filler); it is soaked by a synthetic resin.


22

More detailed information about the setup can be found for example in [31]. The

detailed analysis of the influence of different setup parts and uncertainties in their

geometrical and physical definitions on the neutron flux and possible sources of

systematic uncertainties of obtained experimental data are analyzed using MCNPX

simulation code in [31].

2.4. Gamma-3 Gamma-3 setup, sometimes also called Gamma M-D

3, is a setup consisting of

cylindrical lead target and big graphite moderator. Target has a diameter of 8 cm and

length of 60 cm. Graphite moderator consists of blocks 25x25x60 cm3 and

20x20x60 cm3 big; total volume is 110x110x60 cm

3. In the moderator there are four

cylinders, that can be pulled out and contain holes for sensors. Besides this, there are a

few small plain holes through the moderator. Whole setup is placed on rails in F3 hall

for easier manipulation.

Figure 10: Photo of Gamma-3 setup in F3 experimental hall (left) and graphite cylinder

with holes for samples.

Up to now there was only one experiment on Gamma-3 setup with 2.33 GeV

deuterons. Main experimental task was a study of radioactive sample transmutation; 129

I, 237

Np, 238

Pu, 239

Pu, and 241

Am were used. Next experiments are planned in the first

half of the year 2011.

2.5. Kvinta setup A new “ready to use” target has been available for the E&T RAW collaboration

since the end of the year 2009. It is a setup of massive uranium target and lead

shielding. Target has three sections of the same shape as E+T blanket – a hexagon, but

filled completely with uranium rods (weight 315 kg). Target is surrounded with massive

3 Minsk – Dubna are names of the cities with the main institutes involved in the target construction

2.5. Kvinta setup

23

lead shielding of total weight 1780 kg. Target is permanently placed in the shielding and

the inner volume of the target is accessible only through four thin slots. Plastic holders

are used to place samples inside the target [35]. There were two pilot measurements

done during the 2009 winter run of the Nuclotron, setup was shortly irradiated with

deuterons of 1 and 4 GeV energy.

d

Figure 11: Schema of Kvinta target. On the left there is a cut-view on the uranium target

with supporting structures and plastics used for sample placement, on the right there is a

view on the lead shielding enfolding the target [35].

2.6. EZHIK Completely new target complex called EZHIK is nowadays projected and it

should be ready to use by the end of 2012. Then it will be the main experimental device

of the E&T RAW collaboration, although all previous targets will still exist and will be

available for users.

Name EZHIK means hedgehog in Russian, the parallel with hedgehog is

because of the vertical channels sticking from the target. The target complex EZHIK

is a quasi-infinite target from metallic uranium with wide range of measurement

channels and positions. Basic scheme can be seen in Figure 12. The original technical

solution of asymmetric beam input into a quasi-infinite target (first applied in [36]) is

implemented in somewhat modified form. It provides results equivalent to those that

could be obtained with 8 t uranium target in the case of conventional axial beam input

into a cylindrical symmetric target, but with just about 3 t of target material from natural

uranium [37].

Scientific program of the target EZHIK will be developed in three main fields.

First direction will be focused on gathering of integral data, mainly in the direction of

fission rates and transmutation cross-sections of actinide fission fragments. For this,

wide range of support data will be measured – particle fluxes, energy and heat

distribution, isotopes equilibrium, neutron multiplication and dosimetry quantities.

Second direction will be devoted to simulations. It is expected that all differences

between the models and experiments, which were observed in the past, will be more


24

pronounced at quasi-infinite target and thus it will be easier to find the reason and

correct it. Third direction will be focused on structural and fuel materials irradiated with

large doses of relativistic beams and high energy neutrons. Radiation damage and gas

production will be studied.

Uranium

Graphite

Lead

Measurement channels

Figure 12: Scheme of the new target EZHIK [35].

Besides the basic version with uranium marked EZHIK-U will be developed also

a version EZHIK-Pb, which will be geometrically identical, but whole inner volume

will be filled by natural lead. EZHIK-Pb will be used for verification and adjustment of

basic measurement systems and methods as well as background measurements with

proton and deuteron beams in the projected energy range before main experiments with

uranium target EZHIK-U will be made.

2.7. Placement of the E&T RAW targets For the E&T RAW collaboration is now allocated whole F3 experimental hall at

the Nuclotron accelerator, see Figure 13. Targets stand in the hall on rails, so they can

be quickly moved in/out of the beam. There is a crane in the hall to manipulate with

heavier parts of the targets and equipment.

2.7. Placement of the E&T RAW targets

25

0 1m 5m 10m

Scale:

Beam

Room for E&T RAO personal

A

B

C

D

Нейтронная защита

1 2 3

4

4

5

6

7 8 9 10

Experimental setups

A – «Energy+Тransmutation»;

B – «Еzhik»;C – «Gamma-3»;D – «Кvinta».

Hall diagnostic system:

1 – Ionization chamber

2 – Activation foils3 - Profile meter4 – Scintillator telescope

5 – Pneumatic transport system6 - B F3 detector

7 – Neutron spectrometer8 – Stilben detector;9 - Detector «Isомеr»(3He);

10 - Detector LaBr3(Ce).

Figure 13: Placement of E&T RAW targets inside the F3 experimental hall [35].


26

27

Chapter 3

Experimental background

My work is focused on the studies of high energy neutrons produced in

spallation reactions and their transport in the setup. High energy neutrons are in this

case neutrons with energies from approximately 5 MeV up to 100 MeV. These neutrons

can be measured by multiple methods (time of flight, nuclear emulsions, proton recoil

detectors etc.) but specific conditions in the E+T setup makes these methods hard to use

or unsuitable.

Main limitations of high energy neutron measurements are the following:

- lack of space – a need to measure the neutrons inside the setup,

- neutron field is changing on centimeter scale,

- presence of thermal, epithermal and resonance neutrons,

- presence of protons, deuterons and heavier charged particles,

- huge gamma background,

- specific conditions in JINR Dubna - problems with transport of electronics and

with its operation due to highly intensive short bunches from the accelerator.

Method of neutron activation detectors solves most of these problems. Samples

can be small, thin, are insensitive to gamma and they do not need any power or

maintenance during irradiation. Unirradiated samples can be easily transported, are

simple to handle and relatively cheap (compared to electronic equipment). Last but not

least there is a long tradition in using neutron activation detectors for high energy

neutrons measurement at NPI.

Following chapter will discuss the equipment, methods, and corrections used in

experiments. My PhD work is focused mainly on the experimental part of the E+T

experiment, so this description will go into detail on some places. I was the first one in

our group who routinely applied some of the corrections into the experimental data and

studied their effect. Results of these studies are also presented.

3.1. Activation detectors Neutron activation analysis method is mostly used for detecting the small

amount of some isotope in compound. It is a very sensible method with sensitivity level

up to 10-13

gram per gram [38]. It can measure qualitative as well as quantitative content

of tens of isotopes in one measurement. It uses known fields of neutrons or a system of

standards (reference materials with known content of studied isotopes). We used it

reversed - we placed a known amount of some elements into unknown high energy

neutron field in order to measure the neutron spectrum and flux.

Activation samples were made from pure aluminum, gold, tantalum, indium,

cobalt and bismuth, see Figure 14. In the evaluation of the experiments are shown also

3. EXPERIMENTAL BACKGROUND

28

results for yttrium, which was used by polish group, but was measured on our detectors

and evaluated independently by us. Chemical purity of the materials was better than

99.99 % 4.

Figure 14: Activation materials used in the E+T for the study of high energy neutron

field.

Above mentioned elements were chosen, because they are mostly naturally

mono-isotopic or one of the isotopes is dominant. They are also cheap, nontoxic and

have good physical properties (melting point, ductile, no long-live isotopes). Further

dominant criteria for choosing these elements were the decay times of the isotopes, that

were produced in observed (n,xn) threshold reactions. Isotopes with half lives shorter

than ~30 minutes or longer than ~year are not acceptable for us (we are not able to

measure them with current equipment). For more details of used reactions see Table 4

or Appendix A.

Table 4: Threshold reactions on aluminum activation samples.

Reaction Threshold energy

[MeV]

Half-life5 Used -line

[keV]

Intensity of used

-line [%] 27

Al (n,p) 27

Mg 1.9 9.5 min - -

27Al (n,)

24Na 3.2 14.959 h

1368.6 100

2754.1 99.9 27

Al (n,+2n) 22

Na 23.4 2.6 y 1274.5 10.5

4 Materials were bought mostly from Goodfellow with the support from various grants, I personally had a

grant from Czech Technical University from Internal grant competition (CTU 0808214) and bought of it

bismuth and gold foils. Bought foils had to be cut into smaller pieces suitable for us (we bought price

convenient but bigger pieces).

5 Half-life of isotopes and gamma line energies were taken from [39]. Threshold energies were taken from

[40]. Isotopes without listed gamma-line and intensity have not been detected.

3.1. Activation detectors

29

0

10

20

30

40

50

60

70

80

90

100

110

n,2n n,3n n,4n n,5n n,6n n,7n n,8n n,9n n,10n

Thre

shold

energ

y [

MeV

]

Order of threshold reaction [-]

89Y(n,xn)

115In(n,xn)

181Ta(n,xn)

197Au(n,xn)

209Bi(n,xn)

Figure 15: The threshold energies of (n,xn) reactions in Au, Bi, In, Ta, and Y detectors.

Activation detectors were placed in the setup in two main directions –

longitudinal and radial, see Figure 16. List of all detectors is in Table 5 or in

Appendix B. The foils had dimensions mostly 20x20x1-0.05 mm3 and were twice

wrapped up in the paper. Outer paper layer stopped most of the radioisotopes coming

from the setup and was removed before the measurement. Inner paper layer stopped

radioisotopes coming out from the foil and was present during all measurements [41].

Activation foils with the paper package were sticked on a plastic plane with

holders and put into the slots in the setup (totally 5 planes, ~ 100 detectors/one

experiment). After the irradiation and one to two hours cooling time (for decrease of the

setup radioactivity) the foils could be removed.

Figure 16: Placement of the gold and aluminum activation foils. Others were placed in

the same way, only in another direction (e.g. bismuth in the right-down direction from

the target axis).


30

Figure 17: Plastic plane with sticked samples (left) and the plane holders (right).

Figure 18: Energy plus Transmutation setup with inserted plane holders, top view – left,

and side view – right.

Table 5: Placement of the activation samples in 1.6 GeV deuteron experiment.

Distance from the

target axis [cm] Foil labels in 1.6 GeV deuteron experiment

6

1. pla

ne

0 Y_5

3 Al1 Au1 Ta01 Bi1 In1 Y_8

6 Al2 Au2 Ta02 Y_13

8.5 Al3 Au3 Ta03 Y_15

10.5 Y_22

10.7 Al4 Au4 Ta04

13.5 Y_9

up Y_19

down Y_21

left Y_38

right Y_20

6 Samples printed in normal letters were placed in the upward direction from the target axis (on the

vertical axis). Samples printed in bold letters were placed in the right-down direction 30° from the

horizontal axis. Samples printed in cursive were placed in the up-left direction 30° from the vertical axis.

3.1. Activation detectors

31

2. pla

ne

0 Y_10



8.5 Al7 Au7 Ta07 Bi4 In4 Y_7

10.5 Y_32

10.7 Al8 Au8 Ta08

11.5 Bi5 In5

13.5 Y_2

3. pla

ne

0 Y_4


6 Al10 Au10 Ta10 Y_36

8.5 Al11 Au11 Ta11 Y_18

10.5 Y_33

10.7 Al12 Au12 Ta12

13.5 Y_27

4. pla

ne

0 Y_41

3 Al13 Au13 Ta13 Bi7 In7 Y_25

6 Al14 Au14 Ta14 Y_34

8.5 Al15 Au15 Ta15 Y_37

10.5 Y_40

10.7 Al16 Au16 Ta16

13.5 Y_16

5. pla

ne

0 Y_17

3 Al17 Au17 Ta17 Bi8 In8 Y_11

6 Al18 Au18 Ta18 Y_29

8.5 Al19 Au19 Ta19 Y_3

10.5 Y_39

10.7 Al20 Au20 Ta20

13.5 Y_12

List of all spectra measured on the samples is shown in Appendix C.

Following paragraphs will contain description of various spectroscopic

corrections that I have used and applied to evaluate right yield of the isotopes. These

equations of corrections are the same for detector calibration, beam intensity and

position measurement as well as for experimental data analysis.

3.2. Correction on decay of the isotope between the end of irradiation

and beginning of the measurement Decay of all radioactive materials obeys the decay law:

teNtN 0)( (3.1)

In this equation decay constant) is the most important quantity, which says us

how quickly is the nuclide decaying.

Decay constant can be expressed by using half-live of the nuclide as follows:


32

21

2ln

T (3.2)

When we define the time t0 as the time between the end of irradiation and the

beginning of measurement, and the measurement lasted for a period treal, then the

number of nuclei at the end of irradiation can be expressed like a product of the peak

area and a factor

realt

t

e

e

1

0

(3.3)

This relation can be derived using following arithmetic process. If N(t) is a

number of nuclei in time t, than the decay law has the form

teNtN 0)( (3.4)

In our case is N0 the number of nuclei of studied isotope at the end of irradiation.

Number of registered decays during the measurement can be marked like N. N is

equal to the difference between the number of nuclei at the beginning and at the end of

measurement

)()( 00 realttNtNN (3.5)

When we introduce into this equation from the decay law than will be N equal to

)(

0000 realttt

eNeNN

(3.6)

From this we can express the ratio between the number of nuclei at the end of

irradiation and number of registered nuclei during the measurement time treal:

realt

t

e

e

N

N

1

0

0 (3.7)

3.3. Correction on decay during irradiation Studied radioactive isotopes decay already during irradiation. Let us assume that

tirr is a time of irradiation and that at the beginning of the irradiation there are no nuclei

of studied isotope in the sample. At the end of irradiation there is No of nuclei in the

foil. Next presumption is the rate of production – studied nuclei are produced in the foil

with stable rate P per unit of time.

Number of radioactive nuclei N of studied material in irradiated sample follows

differential equation:

NPdt

dN

(3.8)

This equation can be solved by the method of separation of variables:

3.3. Correction on decay during irradiation

33

0

00

Nt

NP

dNdt

irr

(3.9)

With the substitution NPx the equation becomes:

0NP

P

irrx

dxt

(3.10)

When we integrate the equation within the limits, we will get the term:

P

Nptirr

)0(ln

(3.11)

From this we can derive the rate of production of radioactive isotope, the quantity P:

irrte

NP

1

)0(

(3.12)

This equation can be transformed into the form, from which can be easily seen

how many times more nuclei of studied material were produced during the whole time

of irradiation tirr than it has remained in the sample at the end of its irradiation.

irrt

irrirr

e

t

N

tP

1)0( (3.13)

The right side of this equation is the searched correction on decay of studied

isotope during irradiation.

3.4. Correction on the intensity of the I transition

Gamma decay of the excited state of the daughter‟s nuclei can pass over various

energy levels. Intensity of the gamma transition I is defined as the probability, that a

gamma photon of energy E will be emitted during the decay of the nucleus (it is usually

given in percentage and its value is from almost zero to 100 %).

3.5. Correction on dead-time of the detector Dead time of the detector (and attached electronics) is the time, in which the

detector collects and process previous impulse and during this time the detector is not

able to handle next impulse. If a new impulse comes during this (dead) time, it is not

recorded. Theoretically, there can be three main dead time types: cumulative,

uncumulative and zero [42].


34

If the dead time is increasing with rising number of incoming gamma photons, it

is called a cumulative dead time7. At uncumulative dead time the detector has a fixed

maximal signal rate, which it can handle. From some intensity of the gamma source the

detector registers and processes one gamma photon and all others are ignored during

this time, but the dead time is not prolonged. When the signal is processed, the detector

“opens” for new gamma photons. The new photon is immediately registered and the

detector is again closed and works on processing of newly registered photon. Output

from the detector will display a constant activity of the source, although the real source

activity can rise further. Some detectors can have a zero dead time, this is valid for

example for gas-filled detectors working in current regime.

Our HPGe detectors have a cumulative dead time. Measurement runs over the

time treal, but the detector was able to accept new impulses/gamma photons during the

time tlive. Correction on dead time follows the equationlive

real

deadt

tC . In the Dubna

measurements, there was a limit on dead time given by the electronics and wiring of the

detectors to common ADC, more details are in chapter 3 section 11.

3.6. Correction on real - cascade coincidence

Most of the nuclei have complicated decay schemes and various energy levels

are fed. This leads to a complicated set of gamma and x-ray photons, which are emitted

during deexcitation of daughter‟s nucleus. In such cases, a correction on real - cascade

coincidence has to be used [43].

As an example for demonstration of the - cascade coincidence effect I will

assume general decay scheme, where the studied isotope has basically two possibilities

how to get from the excited state to the ground state. Process of emission of the photon

(A) competes with the process of photon emission (B), whose emission brings the

nucleus in other excited state with lower energy. From this excited state the nucleus can

emit a photon (C) and comes to its ground state.

Figure 19: General decay scheme.

7 gamma quantum incoming to the detector during processing of signal /dead time/ caused by previous

gamma-photon leads to prolongation of this dead time


35

In the first approximation we can say, that the emission directions of both

photons (B) and (C) coming from the same decay are independent. Then, with a certain

probability, both two photons will interact inside the detector. This probability is

growing with the decreasing distance between sample and the detector. Except some

cases the life time of the energetic level between transitions (B) and (C) is negligible

compared to the time that is needed for the signal collection after the absorption of the

photon (B). That is why the detector registers both photons at the “same” time and

summarizes the signals from photon (B) and (C). Energy of the summarized signal is

naturally the same as of the photon (A), and the peak respective to the photon (A) is

falsely increased. This effect is called - cascade coincidence.

Ratio between the area of the summing peak (B)+(C) and area of the peak

accordant to the -transition (A), which represents the coefficient of enlargement of the

area of the peak (A), is determined by the following relation:

)(

)(

)(

)()(

A

Cca

AI

BICBAS

p

p

CC

(3.14)

where I is absolute intensity of the gamma line, a is the branching ratio, )1/(1 tc ,

where t is total conversion coefficient and p is the peak efficiency of the detector.

Coefficient representing a decrease of the area of the peak B is equal to

)()( CcaCBL tCc , where aC is the probability that the transition (B) will be

followed by the transition (C), cC is the probability that a photon (C) will be emitted and

t(C) is a probability that photon (C) will interact in the detector leaving there at least

some part of its energy C, which will be bigger than the energy resolution of the

detector. Than the signal of energy (B) + C is registered outside the full absorption

peak of the transition B.

In the same way can be derived also the coefficient, which relates to the

reduction of the peak area connected with transition C, which follows after the

transition B:

)()(

)()( Bca

CI

BICBL tCC

(3.15)

These equations can be derived analogically in the case of multiple cascades.

When we make corrections corresponding to the coincidence summation S(A) and to

coincidence losses L(A), it is possible to formulate the number of measured impulses

Ndet(A) in the peak of full absorption of the gamma transition A like:

)()()()()()()()()(det ANASALANALASANANAN (3.16)

With the coincidence factor defined as ))(1))((1( ASALCOI the right

number of pulses N(A) coming from the transition (A) can be the expressed by the

equation:


36

COI

ANAN

)()( det (3.17)

Except the real cascade coincidences, a stochastic coincidence can also

occur. During stochastic coincidence, two photons from two different decays hit the

detector at the same time and they are summarized. Because of low activities of our

samples and small efficiency of used HPGe detectors this effect is negligibly small in

our case.

On the beginning of my PhD work I calculated the correction on real

coincidences with hand-made equations made by my colleague A. Krása [44].

Equations were made up according to the k-0 standardization method [43]. With the

rising number of studied isotopes, it was not further possible to set up the equations. Set

up of the COI equations is sometimes extremely time-consuming due to high number of

emitted gamma lines. With the number of gamma lines also the possibility of errors in

the equations is quickly growing. My second colleague M. Majerle developed a

program in Excel (Excel Addin in Visual Basic, see example in Appendix M) for

“automatic” calculation of real coincidences. The Addin needs as an input a table of

gamma lines, energy levels of the nucleus, gamma intensities and branching ratios; all

this converted to a special table. In the code, it is necessary to change the number of

valid rows in the table. With another Addin for the detector efficiencies, the COI can be

calculated. Using different detectors and geometries, COI must be calculated for all

these combinations used in each experiment.

I have compared both approaches of COI calculation with satisfactory results.

Table with an example of the coincidence correction for various isotopes is in the

Appendix E.

For the calculation of real coincidence correction both peak and total detector

efficiencies are needed. Peak efficiency of the detector appears also in the final equation

for calculation of the yield, so in the following two paragraphs I will make a short

description of peak (p) and total (t) efficiencies. Practical approach for their

measurement is stated in the section dealing with the detector calibration.

Peak efficiency of the detector

Peak efficiency of the detector in dependence on energy of registered photon is

defined as:

0N

Sp (3.18)

Peak efficiency is a ratio between the number of gamma photons from a level

transition in a calibration source registered into the peak of full absorption (per unit of

time) divided by the activity of the calibration source, recalculated to the day of

measurement. Peak efficiency depends on the photon energy, on the distance between

emitter and detector (solid angle) and on the detector type and quality.


37

Total detector efficiency t

Total detector efficiency t is a summary of efficiencies of all partial processes,

which leads to any deposition of the energy of emitted gamma-photon in the detector

resulting in an output signal. Main three processes are Compton scattering, photoeffect

and production of electron-positron pairs. Total efficiency t depends again on photon

energy, distance between emitter and detector and on type and quality of detector.

Knowledge about the total detector efficiency is necessary for calculation of the

correction on real coincidences. Total efficiency is determined during the calibration of

each detector, results for ORTEC(new2) detector can be seen in Figure 27.

3.7. Correction on changed detector efficiency due to sample

dimensions Correction on changed detector efficiency was used at thick foils (typically beam

monitor foil – 3 mm thick). During the measurement on the detector, calibration sources

same as studied foils were mounted on the same plane. Most of the foils have thickness

smaller than 1 mm (50 – 100 m), so the center of mass is approximately at the same

place like the calibration sample was. In the case of foils thicker than 1 mm this is not

true, so I had to recalculate the efficiency of the detector taking into account that center

of the foil is closer to the detector.

1.020

1.025

1.030

1.035

1.040

1.045

1.050

1.055

0 2 4 6 8 10 12

Corr

ecti

on facto

r [-

]

Distance from sample to detector [cm]

1368 keV 2754 keV

Figure 20: Correction on the change in detector efficiency in the case of 3 mm thick Al

foil measured on Ortec(new2) detector.

I used efficiencies of the detector measured for a certain energy at different

distances and fitted them with a second order polynomial. Then I used this fit to


38

calculate the efficiency for the closer position. Ratio between the recalculated and old

efficiency is the searched correction. In the Figure 20 the specimen values are used in

the 4 GeV deuteron run for 3 mm thick Al foil measured on Ortec(new2) detector.

Uncertainty of this correction is negligibly small compared to other uncertainties.

3.8. Self-absorption correction I have calculated the self absorption correction for each isotope and used foil

thickness. I used a formula (3.19), which can be derived as a ratio between gamma

fluxes from the foil with and without self-absorption. Quantity cm-1 used in the

equation is the total mass attenuation coefficient T [cm2/g] divided by density [g/cm

3].

Values of comes from Handbook of Nuclear Data for Neutron Activation Analysis

[45] and were verified in web database Mass attenuation coefficients [46]. Quantity I0 is

unattenuated intensity of the gamma photons produced in the foil and D is foil

thickness. I used a smooth curve between tabular values and calculated correction

values for all used gamma energies and materials. In the following Figure 21 there is an

example of self-absorption correction factor for 1 mm thick Bi foil (at this foil the

correction was most important because of the big thickness of the foil, dense and heavy

material, and low energies of used gamma lines).

DD

x

D

abse

D

dxeD

I

dxD

I

C

1

0

0

0

0

(3.19)

0.8

1

1.2

1.4

1.6

1.8

2

2.2

0 200 400 600 800 1000 1200 1400 1600 1800 2000

Self

-abso

rpti

on c

orr

erc

tion facto

r [

-]

Photon energy [MeV]

Tabular value Used gamma-energies

Bi - 1 mm thickness

Figure 21: Self-absorption correction factors for 1 mm thick Bi foil.

3.8. Self-absorption correction

39

Only gamma-rays going parallel with the detector axis were taken into account

in the self-absorption analysis stated above. Effective thickness of the sample can be

bigger than the real one for close sample to detector distances (gamma-ray going

sideways in the sample can be also detected), but this effect was assessed to be

negligibly small in our case.

3.9. Square-emitter correction (geometrical correction) I had to calibrate all detectors that I used. I exploited standard laboratory point-

like calibration sources, see chapter 3 section 11. The biggest activation samples had

dimensions 2.5x2.5 cm2 with more or less equally distributed activity. It was clear that

the detector efficiency was in close distances not the same for point and non-point like

emitter (so the efficiency calibration is not precise enough). To assess somehow this

effect, M. Majerle made a MCNPX calculation and studied the response of the detector

for point-like and nonpoint-like emitter (correction is defined according to the relation

(3.20)). Main problem of these simulations was missing knowledge about the detectors

geometry – size and shape of the crystal, thickness of dead layer and aluminum coating.

More details about the MCNPX simulations can be found in M. Majerle‟s PhD thesis

[41].

int)(

)(

po

foilc

p

p

g

(3.20)

To verify M. Majerle‟s MCNPX calculations a long row of experiments was

done. These experiments were done originally by M. Majerle, later by me and also by

our young student from Czech grammar school (O. Sláma, he was involved in the

project Open science) and foreign student S. Peeterman. Gold foils were irradiated in

LVR-15 reactor and cyclotron in Řež for these experiments. We used standard 2x2 cm2

foil and small – approximately 1x1 mm2 - piece of Al with admixture of gold. Yields of

198Au isotope were normalized to the measurement done in the biggest detector to

sample distance, where the difference between point and nonpoint-like emitter can be

neglected. Within the uncertainty bars, results of all measurements are comparable

among themselves and also with M. Majerle‟s MCNPX calculations, example can be

seen in following Figure 22.

One can object why not to buy a square-emitter calibration source.

Unfortunately, this was not a usable solution for us. The economic and administrative

obstacles were one of the main reasons. With this is connected also the number of

needed calibration sources – at least five various dimensions from 1.5x1.5 cm2 to

3x3 cm2 would be necessary to measure for covering the main dimensions of our

samples. Another question is the package type of these square-emitter samples, if they

would be closed emitters in the term of law. We would need these calibration sources at

three different places – Řež, Uppsala in Sweden and Dubna in Russia. Cross-border

transport of radioactive materials is a difficult task, which cost a lot of money and

manpower (and both we do not have in sufficient amount).


40

0.88

0.90

0.92

0.94

0.96

0.98

1.00

1.02

0 2 4 6 8 10 12 14 16 18 20

Sq

uare

-em

itte

r co

rrecti

on

[-]


MCNPX calculation

Sláma - measurement 1

Sláma - measurement 2

Peeterman measurement

Figure 22: Comparison between measured and simulated square-emitter correction for

2x2 cm2 foil and detector in Řež. Lines are only to guide reader‟s eyes. Sláma‟s data

come from [47], Peeterman‟s data are from [48].

0.88

0.90

0.92

0.94

0.96

0.98

1.00

0 2 4 6 8 10 12 14 16 18 20

Square

-em

itte

r corr

ecti

on [

-]


1.25x1.25 cm

2x2 cm

2.5x2.5 cm

3x3 cm

iodine 3cm round

Figure 23: Square-emitter correction for the detector in Řež calculated in MCNPX for

all sizes of measured samples. Distances correspond with used geometries (15 mm,

23 mm, 33 mm, 53 mm, 70 mm, 93 mm, and 178 mm).

3.9. Square-emitter correction (geometrical correction)

41

I calculated square-emitter correction in MCNPX and brought it to routine use.

I used the input file developed by M. Majerle and modified it to calculate the correction

for all sizes of foils, detector types and geometries used in Energy plus Transmutation

experiments and for cross-section measurements. Example of calculated correction can

be seen in Figure 23.

Up to now I have considered thin foils, where I can neglect the thickness of the

foil. In the case of Al beam monitor foils, this is not true. Aluminum foil for beam

intensity measurement is 10x10 cm2 big, as described in Chapter 4, section 3. For

gamma measurement, the foil was bended to half, and again and again, so it finally had

dimensions of 2.5x2.5 cm2 and thickness 3 mm. Due to the small beam spot and

bending procedure, the activity is not distributed in the foil homogenously. Thus, there

can be some uncertainty in measurement of such a foil. To assess the effect of various

placement of activity in the thick foil, I modified the MCNPX simulation and used

volume source instead of surface one. Schematic plot of the geometrical situation is in

following Figure 24, it is a visualization of the MCNPX input file made in VISED code

[49]. I put 80 % of activity in 20 % of the foil volume and opposite. The distance

between the foil and detector was changed according to experimentally used

geometries.

Figure 24: Detector with inhomogeneous volume source representing Al foil that is used

for beam intensity measurements.


42

0.00

0.01

0.02

0.03

0.04

0.05

0.06

4 5 6 7 8 9 10 11

Eff

icie

ncy [-]


Ep - activity up

Ep - activity down

Et - activity up

Et - activity down

Figure 25: Peak and total efficiencies of the ORTEC(new1) detector calculated for

inhomogeneous 25x25x3 mm3 volume source – hypothetic case of activity distribution

in Al monitor foil. Efficiencies are calculated for positions p3, p4, and p5 used in

the experiment. Uncertainties of the calculation are below 0.1% (high statistics).

I calculated peak and total efficiency of the detector for the case when the main

activity is on top or opposite. The results for the 4 GeV deuteron experiment are in

Figure 25. From the figure we can see, that the differences are small (mean value of the

p-up/p-down ratios is 0.972) in comparison with the uncertainties related with the

spectra evaluation in DEIMOS32, detector calibration etc.

3.10. Beam instability correction Irradiations on the Nuclotron accelerator were unfortunately not too much

stabile, see Figure 35 - Figure 37. To correct the beam instabilities I used an easy

program developed in Dubna, which counts production and decay of each isotope for

each bunch. The input to the program consists of two files describing the beam structure

and half-lives of the isotopes, for which the correction should be calculated. The

program works according to the equation (3.21), [50]. Isotope production and decay are

calculated for each beam bunch.

Less accurate correction factor can be obtained by a manual calculation

according to the equation (3.21) when the irradiation process is divided into sections

with the same beam intensity. By this manual procedure I checked the function of the

program getting almost the same correction factor values (differing at the third decimal

place). More details can be found in my Diploma thesis [29].

3.10. Beam instability correction

43

N

i

itit

p

irr

t

a

pe

irr

eeiWit

t

eB

)1()()(

1

1

)()(

(3.21)

where:

tirr – total irradiation time

te (i) – time from the end of the irradiation interval till the end of whole irradiation

tp (i) – time of calculated irradiation interval

W (i) – ratio between the number of protons in the interval and in the whole irradiation

N – total number of intervals

– decay constant

Beam correction factor is in most cases very close to the one, but it strongly

depends on the decay time of the isotope and on the irradiation structure. For small

decay times or more complicated beam it would naturally differ more from the one, but

as we cannot measure isotopes with decay time shorter than one hour, the biggest beam

correction is in my case equal to the factor of 0.8. Complete list of beam instability

correction factors for all observed isotopes in deuteron experiments is in

the Appendix D.

3.11. HPGe detectors For the measurement of all activated samples (beam monitors as well as threshold

detectors) we used High Purity Germanium (HPGe) detectors. Detectors are placed in

the JASNAPP laboratory in JINR, Dubna. In this laboratory there are four HPGe

detectors for gamma-measurements and one planar detector for X-ray measurements

[51]. We used detectors marked like Ortec new1 and Ortec new2. Their parameters are

in following Table 6. These detectors were connected together with the planar detector

to common ADC, so they had a collective dead time (high dead time caused by one

detector was added to the dead times of the others – all three detectors had the same

dead time value). Both used detectors were equipped with small Dewar flask, so I had to

refill the nitrogen every two days (to be sure there is always enough liquid nitrogen –

there are no scales). Detectors are during the year operated by J. Adam and his group

from RChL (Radiochemical Laboratory department of JINR).

Detectors were placed in lead shielding with the back and front wall partially

opened, see Figure 26. Shielding was built up of various types of lead bricks, minimal

thickness was 5 cm Pb, maximal 8 cm. This shielding suppressed the background

approximately ten times; moreover it shielded personnel from measured radioactive

samples (in the same room 3 detectors were operated at the same time and many people

were all the time present). During the upgrade of the shielding in summer 2009 I helped

to bring one tone of lead bricks from a very old beam dump. These bricks seemed to be

without any radioactivity, but after the building of the shielding gamma lines of 207

Bi

occurred (half-live 31.55 years). Intensity of this isotope was approximately five times


44

stronger than that of 40

K and the spectra from 4 GeV deuteron experiment are

contaminated. There was built new shielding made of unactivated lead recently.

Table 6: Parameters of used HPGe detectors, partly overtaken from [51].

Dubna detectors Řež detector

Manufacturer/Name ORTEC(new1) ORTEC(new2) Intertechnique

/IAA

Type GMX-20190 GMX-30 EGNC20

Resolution [keV]

(E=1332 keV) 1.80 keV 1.80 keV 1.80 keV

Relative efficiency [%]

(E=1332 keV ) 28.3 32.9 22.1

Coating [mm] 0.50 - Be 1.27 - Al 0.5 - Al

Dead Ge layer [m] 0.3 0.3 0.5

Detector bias supply ORTEC 659 ORTEC 660 ND360

Spectroscopy preamplifier Canberra 2024 Canberra 2026 Canberra 9615

ADC Multichannel buffer - ORTEC 919 Canberra 9635

Bias voltage [V] - 4800 - 4000 - 4000

Shaping time [s] 4 3 4

Figure 26: HPGe detector Ortec(new) with lead shielding (left) and the bank with

sample holder (right).

Inside the shielding there was a bank for exact placement of plastic holders with

samples. From one side it had a special hole, which fits firmly together with detector.

The bank was situated on a plate with adjustable height. It was manufactured from

acrylic glass, so it was light and easy to handle. Inside the bank there were eight

P8 P7 P6 P5 P4 P3 P2 P1

3.11. HPGe detectors

45

positions for holders at distances of 12 mm, 24 mm, 41 mm, 65 mm, 99 mm, 147 mm,

216 mm, and 311 mm from the front of the detector8.

I calibrated detectors with a standard set of calibration etalons9:

54Mn,

22Na,

57Co,

60Co,

65Zn,

88Y,

109Cd,

113Sn,

133Ba,

137Cs,

139Ce,

152Eu,

228Th,

226Ra, and

241Am

(all isotopes were not available during all calibration measurements). After the end of

measurements of samples from experiment I checked the calibration once more to

control the calibration stability (temperature and voltage changes during days and nights

were demonstrably changing energy calibration). I had to repeat the calibration before

each experiment because of changes in geometry (manipulation with the detector and

shielding during the year), changes in electronic settings and generally long time

between experiments. Calibration was performed for the positions P2 up to P5.

Measured activities of the calibration etalons were corrected on decay between

manufacture and current date of measurement; experimental efficiencies for each used

gamma line were calculated. Total number of used gamma lines was between 30 and 50

depending on the geometry and available time for measurement. Peak efficiency of the

detector was calculated according to the equation (3.22), where Speak is the area of the

peak related with the calibration isotope and A0 [Bq] is the activity of the calibration

etalon at the date of manufacture.

live

real

t

COI

t

peak

pt

t

eCIA

eS

real )1(0

0

(3.22)

CCOI is a correction on real coincidences, it was necessary for following

isotopes: 133

Ba, 60

Co, 152

Eu, 228

Th, and 88

Y. For these isotopes an iteration loop was

necessary – change in measured activities invoked change in efficiencies and

consequently in the fit of the points, which invoked change in fitted efficiency and in

real coincidences correction, which back invoked change in measured activities of

calibration samples. Iteration was repeated so far the efficiencies were not changing in

reasonable number of digits (mostly 8 decimal places).

Values of the experimental efficiency were taken into logarithm and fitted with

one or two curves so that the differences between the experimental values and the fit

would be minimal (3.23). I have omitted several experimental points that were too far

from the curve, probably because of the coincidence with natural background or

because of the complicated evaluation in DEIMOS32.

))ln()ln()ln(( 23 dEcEbEa

p e respectively ))ln()ln(( 2 cEbEa

p e (3. 23)

8 For the newest detector ORTEC(new2) I bought the material from MK Plexi s.r.o. I paid it from my

grant CTU0808214 and I transported it after the assemblage in NPI to JINR Dubna.

9 Half-lifes of the isotopes were taken from the etalon certificates. Intensities of used gamma-lines were

taken from [39].


46

Total uncertainty of the peak efficiency calibration is assessed to be at least 1%.

It comes from the uncertainty of the calibrations etalons (1% - 2% uncertainty in the

knowledge of activity) and from the fit of the experimental points.

In the case of total efficiency, only a few isotopes, which have one or two

gamma lines, could be used (57

Co, 139

Ce, 113

Sn, 137

Cs, 54

Mn, 60

Co – up to energy

1253 keV). In the DEIMOS32 code [52] I have summarized number of counts from the

beginning of the spectra up to the end of the peak (Stotal), activity of the etalon at the

date of manufacture is A0.

live

real

t

t

total

tt

t

eIA

eS

real )1(0

0

(3.24)

I have interlayed logarithmic values of experimental points with third order

polynomial, see equation (3.25).

))ln()ln()ln(( 23 dEcEbEa

t e (3.25)

Finally, I put calibration curves into the Excel as an Addin, so they can be easily

used as a function (function ep for peak efficiency and function et for total efficiency),

see Appendix M. Example of peak and total efficiencies for the ORTEC(new2) detector

in the 4 GeV experiment are in following Figure 27. In Figure 27 three geometries (p3,

p4, and p5 are shown, distances between sample and detector are according to the

Figure 26. Exp means experimental points from the calibration sample measurements,

fit indicates mathematical fit of experimental points.

0

0.01

0.02

0.03

0.04

0.05

0.06

0.07

0.08

0.09

0 500 1000 1500 2000 2500 3000

Eff

icie

ncy

[-]

Energy [MeV]

Ep-p3-exp Ep-p4-exp Ep-p5-exp

Ep-p3-fit Ep-p4-fit Ep-p5-fit

Et-p3-fit Et-p4-fit Et-p5-fit

Et-p3-exp Et-p4-exp Et-p5-exp

Figure 27: Example of peak and total efficiencies for the ORTEC(new2) detector in the

4 GeV experiment.

3.11. HPGe detectors

47

I have also studied homogeneity of the detector in X and Y axis, because foils

in our experiments are not irradiated homogenously10

. There can be a difference

in the activity of the foil on its sides. I have measured the difference in the response

of the detector on the same gamma source placed on different sides from the centre

of the crystal to assess a possible uncertainty coming from the detector in-homogeneity

in combination with un-homogenously irradiated foils.

I used a point-like laboratory etalon and displaced it in X and Y axis in a grid of

3 mm or more. Detector in JINR Dubna is homogenous within 2 percent, what is the

uncertainty of this type of measurement (uncertainty comes from the peak evaluation in

DEIMOS32). HPGe detector in Řež is not homogenous because it was accidentally

irradiated by neutrons in the past. After this irradiation, the crystal had to be newly

surfaced. Results of one of these measurements are in following Figure 28, it is a

comparison of the detector response to point-like 137

Cs source placed in the centre of the

detector and displaced to the left and to the right (in left – right direction is the biggest

difference). Conclusion is that we have to be careful when measuring big foils in close

distances, but under normal conditions no special precautions have to be done (there is

only a difference of 2.6 % between left and right side 27 mm from the centre, measured

at 15 mm distance from the detector cap).

0.60

0.65

0.70

0.75

0.80

0.85

0.90

0.95

1.00

1.05

0 0.5 1 1.5 2 2.5 3

Dis

pla

ced

to

cen

tre r

ati

o [

-]

Distance from the centre of detector [cm]

right side

left side

Figure 28: Homogeneity of Řež HPGe detector in X-axis. On Y-axis of the graph there

is a ratio between the responses of the detector to 137

Cs point-like source placed in the

centre and displaced to left and right. Homogeneity measured at the distance 15 mm

from the detector cap.

10

Change of the neutron field in the E+T setup is not negligible on the distance comparable with the

dimension of the foils [31], [53].


48

3.12. DEIMOS32 program

I used DEIMOS32 code to evaluate measured -spectra. This program was

developed at the Nuclear spectroscopy department by J. Frána [52]. Simplified principle

of the gamma spectra analysis is a fit of selected gamma peaks with Gauss curve.

DEIMOS32 code has a lot of functions, settings and possible ways of use; it was one of

the main tools I have used, so more detailed description of the code follows.

Basic function of the DEIMOS32 is a spectrum display. One can see whole

spectrum (with already evaluated regions if this function is used) or one can work

directly with a chosen part of the spectrum. Three modes of the Y-axis depiction can be

used: linear, square root, and logarithmic. Position of the mouse pointer is displayed

above as a function of energy (number of channel) and number of counts at this energy.

Evaluation of the spectra is possible in automatic or manual mode; both regimes can be

switched anytime. I have used only manual evaluation, because it enables the best

control over the peak fit procedure.

Peak fit procedure is based on the non-linear least squares method. In each

evaluated part of the spectrum positions, heights, common widths of the peaks, and

parabolic or linear background are fitted. Widths of the peaks can be pre-calibrated and

held fixed, or maintained in preset range. Regions for evaluation can be chosen

manually or found by automatic searching procedure. Peak distance can be also fixed.

I used a manual process of energy calibration, by which I evaluated a spectrum

with known peaks/energies and then modified the calibration file. Two-point energy

calibration was used. Program can work with the following list of spectra: DAT

(AccuSpec, Silena), .MCA (S100), .CHN a .SPC (Ortec), .SPE (Sampo), .CNF (Genie).

Reading of ASCII files is also possible. At some types of these spectra only some parts

of the file header are red. This caused to me a lot of problems, because I processed a lot

of CNF files, where the headers could not been displayed, so I had to store the times and

dates of the measurements separately.

DEIMOS32 solves also the staircase increase of the background on the low-

energy part of the peak. This jump in the background is small for energies over 300 keV

and can be considered stable for all energies (in our case of detectors with relative

efficiency ~ 20 % it is approximately 1 % of the peak height). In the region of energies

lower than 300 keV I have used preset values already involved in the code, that were

successfully tested on the same type of the detectors like I have used.

3.12. DEIMOS32 program

49

Figure 29: Graphical interface of the DEIMOS32 code [52].

Peak area can be established by two different procedures. A simple one is a

summary of the number of counts in each channel involved in the region that is

evaluated. This I have used during measurement of the total detector efficiency. More

sophisticated is the fit procedure with non-linear least squares fit. The code enables to

run the procedure step by step and change the parameters of the fit (background

description, region of fit, number of peaks in the fit, fixed FWHM etc.) between each

step. I have widely used this feature and I have evaluated thanks to it also very

complicated spectra. The disadvantage is an extreme time consumption of this

procedure.

It can be chosen many types of output files and data written in it, I used only a

simple one with the extension PRN. PRN file is a text file, which contains basic

information about the spectra (red from the file header if possible), peak position in

channels and energy, peak area and its uncertainty and several statistical parameters

related to the Gauss-fit.

Most of the peaks that I evaluated in DEIMOS32 were small ones on a

background of much bigger peaks from the isotopes produced in non-threshold (n,)

reactions (intensities of studied peaks are comparable with the peaks from unshielded

background). Precision of the DEIMOS32 evaluation was crucial for the experiment, so

I have tested differences between results of evaluation of the same spectra in

DEIMOS32 and Genie, as a representative of automatic commercial software for

spectra analysis [54].


50

I used spectra with a lot of peaks coming from threshold reactions, namely Al,

Au, and Bi. I chose the most and the less active sample of each isotope. I came to

following conclusions.

In the case of huge peaks on clear background (Al), the differences between the

programs are smaller than 0.1 %. When the background is more complicated and a lot

of peaks is nearby the main peak (e.g. Al with small activity and long time of

measurement = bigger background), differences between the fits are 3% on average.

When the size of the studied peak is comparable with the peaks from background,

studied peak lies on a complicated background or is nearby a strong peak, differences

between the two programs are up to tens of percent in some cases, on average 7%.

There is no clear trend in the differences, values of the differences between the

programs go equally to plus and minus. Differences between these two programs are in

any case smaller than the uncertainty of the peak fit in each program.

DEIMOS32 code is for my purpose of use much more convenient than the

automatic codes. It is much more complicated and time consuming to use, but I have

full control over the whole fitting process. I can focus on studied peak and do much

more for its analysis than any automatic code can ever do.

3.13. Yield evaluation Finally, yield of observed isotopes (products of the (n,xn) reactions) was

calculated with respect to the various spectroscopic corrections according to the

equation (3.26). Weight normalization is involved in the yield. Weight-normalized

yields from various foils (of the same material) can be compared within one experiment.

To be able to compare the yields among all E+T experiments, I have finally divided the

yields also by the total number of beam particles Nd (is discussed in following chapter).

Beam

correction

Weight

normalization

Square-emitter

correction

Correction for

coincidences

Peak area Dead time

correction

Self-absorption

correction

Decay during cooling and

measurement

Decay during

irradiation

)()(

)(

11

1

)(

)( 0

irrreal t

irr

t

t

foillive

real

areagP

aabsp

yielde

t

e

e

mt

t

CCoiCEI

BECSN

line –intensity

per decay Detector

efficiency Correction for

efficiency

change

(3.26)

Following notation is used in the equation:

treal – measurement time on the detector

tlive – live time of the detector

tirr – irradiation time

3.13. Yield evaluation

51

t0 – time between end of irradiation and beginning of measurement

– decay constant

Weighted average (X) according to the equation (3.27) was used for the isotopes

with more detected lines or in the case of multiple measurements. It is a standard

weighted least-square average over n values (xi) and their uncertainties (Δxi). I have

used the equations according to the publication Review of Particle Physics 2000

Edition [55].

n

i i

n

i i

i

x

x

x

X

12

12

1 (3.27)

I have determined the uncertainty of the weighted average (ΔXi) using the

equation (3.28):

n

i i

i

x

X

12

1

1 (3.28)

I have also calculated χ2 and compared it with (n-1), which is the expected value

of χ2 if the measurements are from a Gaussian distribution.

11

12

2

2

n

x

Xx

n

n

i i

i

(3.29)

If 1/2 n is less than or equal to one, I accepted the weighted average. If

1/2 n was slightly bigger than one, I increased the uncertainty of weighted average

by multiplying it with 1/2 n .

My reasoning for this is following: value of 1/2 n bigger than one means

that at least one of the partial values is too far from the Gaussian distribution and has

too small uncertainty (to be connected with the rest of the data). Not knowing which

uncertainty of which value is underestimated, I assumed they are all underestimated by

the same factor 1/2 n . If I scaled up all the input uncertainties by this factor, the

χ2 become equal to (n-1) and also the output uncertainty of the weighted average scales

up by the same factor 1/2 n .

If the 1/2 n was very large, I searched in the data for the values that were

far from the weighted average. I have reanalyzed these values in order to find possible


52

source of discrepancy11

. When the reanalysis did not helped I have excluded these

values from further analysis. This approach was not usable in all cases, because the

spread of all values was big at some isotopes and it was not possible to decide which

value should be excluded.

Yields of the most important isotopes produced in various reactions and samples

during 1.6 GeV and 2.52 GeV experiment are in the Appendix F.

3.14. Sources of uncertainties In the following Figure 30 there are shown basic sources of uncertainties

(measured quantities, corrections, given data), their partial steps and partial

uncertainties, that come out in each step (display idea comes from [56]). Dashed lines

represent most important relations between the quantities from the uncertainty point of

view. Red marked uncertainties I have already involved into the analysis, blue marked

uncertainties are exactly known, but are negligibly small or have practically no

influence on the result. Rest of uncertainties (marked black) is not exactly known but

they are negligible compared to the red ones.

Beam intensity determination was always the biggest source of uncertainties in

the E+T experiments. Besides the uncertainty coming from the spectroscopic evaluation

of the foils that are used for intensity measurement there is an uncertainty from the

cross-section and uncertainty from the shift of the cross-section to the used beam energy

(hard to assess). Anyway, uncertainty of the beam intensity is the same for all samples

and reactions in one experiment, so it has no influence on the shape of the relative

yields of the isotopes in radial or longitudinal direction. This is also the reason for

stating this uncertainty separately.

Other uncertainties in experiment come from the peak fit in DEIMOS32, these

vary from units of percents up to tens of percents. Detector calibration is known with at

least 1 % uncertainty, another 1 % uncertainty is contained in spectroscopic corrections.

Uncertainty coming from the foil placement can be up to 20 % at 5 mm foil

displacement [41].

Within the Energy and Transmutation RAW collaboration there has not been a

clear statement how to handle all these uncertainties (if involve them into data or put

them separately) up to now. Some of the uncertainties have changed in the time –

deuteron experiments were the first ones where I have involved some corrections (e.g.

on self-absorption) or modified older ones (COI correction). That is why I state my

experimental data only with the DEIMOS32 uncertainty, other uncertainties can be

modified and involved by the users when needed.

11

This was done in various ways – by repeated DEIMOS32 evaluation, searching in the background for

possible sources of interference, comparisons among the yields on all foils of the same type, comparison

between multiple measurements, looking for decay products of the isotope, comparison with the MCNPX

simulation etc.

3.14. Sources of uncertainties

53

Figure 30: Schema of the uncertainties.

Yie

ld

No

n-p

oin

t lik

e

emit

terNo

n-p

oin

t lik

e

emit

ter

corr

ecti

on

No

n-p

oin

t lik

e

emit

ter

corr

ecti

on

un

cert

ain

ty

Ga

mm

a li

ne

inte

nsi

ty

Ga

mm

a-l

ine

inte

nsi

ty

corr

ecti

on

Inte

nsi

ty

un

cert

ain

tyB

eam

corr

ecti

on

Bea

m

corr

ecti

on

un

cert

ain

ty

Bea

m s

tab

ility

Tim

e

mea

sure

men

t

Rea

l tim

eu

nce

rta

inty

Liv

e ti

me

un

cert

ain

ty

Sta

rt o

f

mea

sure

men

t

un

cert

ain

ty

Sta

rt o

f

irra

dia

tio

n

un

cert

ain

ty

En

d o

f

irra

dia

tio

n

un

cert

ain

ty

Det

ecto

r dea

d

tim

e

Det

ecto

r

dea

d ti

me

corr

ecti

on

Dea

d ti

me

un

cert

ain

ty

Rea

l co

inci

den

ces C

OI

corr

ecti

on

Det

ecto

r

effi

cien

cy

un

cert

ain

ty

CO

I

corr

ecti

on

un

cert

ain

ty

Fo

il m

ate

ria

l

Siz

eu

nce

rta

intyTh

ick

nes

su

nce

rta

inty

Pu

rity

un

cert

ain

ty

Den

sity

un

cert

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ty

Sel

f a

bso

rpti

on

Sel

f

ab

sorp

tion

corr

ecti

on

Att

enu

ati

on

coef

fici

ent

un

cert

ain

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Det

ecto

r eff

icie

ncy S

pec

tra

eva

lua

tio

n

DE

IMO

S

un

cert

ain

ty

Ga

mm

a li

ne

iden

tifi

cati

onC

alib

rati

on

sam

ple

s

Po

siti

on

un

cert

ain

ty

Act

ivit

y

un

cert

ain

ty

Fit

of

the

po

ints

Fit

un

cert

ain

ty

Bea

m in

ten

sity

Mo

nit

or

pla

cem

ent

Po

siti

on

un

cert

ain

ty

Mo

nit

or

mea

sure

men

t

Det

ecto

r

effi

cien

cy

un

cert

ain

ty

Sp

ectr

a

eva

lua

tio

n

DE

IMO

S

un

cert

ain

ty

Ga

mm

a li

ne

iden

tifi

cati

on

Cro

ss -

sect

ion

Cro

ss-s

ecti

on

un

cert

ain

ty

Wei

ght

of

the

foils

Wei

ght

mea

sure

men

t

Wei

ght

mea

sure

men

t

un

cert

ain

ty


54

3.15. Background

Natural background played a significant role in all my spectroscopic

measurements. Due to small cross-sections as well as low high energy neutron

intensities I worked with small activities, so some detector shielding was necessary.

HPGe detectors that I used in JINR Dubna had lead shielding described more in the

chapter 3 section 11, see e.g. Figure 26.

I measured the background before each experiment at JINR Dubna and also

afterwards I measured last sample. I supposed the background was not changing during

the sample measurements, although it had to be not necessarily true (laboratory with

detectors is in the building neighbouring with the Phasotron accelerator. During the

Phasotron operation the background was up to one order of magnitude higher than

usually. Nevertheless, after the fire of the power supply of beam line guiding magnets,

Phasotron is working rarely.). Spectroscopic laboratory at JINR Dubna is placed in the

first floor of the building, so radon and its daughter products are not a problem. There

are two more floors with massive concrete ceilings over it, so the cosmics is also

partially suppressed. After the long time of the laboratory usage there can be seen

artificial isotopes in the background spectra (152

Eu and 137

Cs).

I had to subtract the background at some isotopes where the energy of studied

gamma line was close or even the same like the energy of some gamma-line in

background (typically 207

Bi – all gamma lines or 192

Au – 295.96 keV gamma line).

55

Chapter 4

Beam diagnostics on Nuclotron accelerator

4.1. Nuclotron accelerator Irradiation of the E+T setup was carried out in the Laboratory of High Energies

by 1.6 GeV, 2.52 GeV and 4 GeV deuteron beam extracted from the Nuclotron

accelerator. These deuteron irradiations were a continuance of previous protons

experiments, in which the Energy plus Transmutation setup was irradiated by 0.7, 1, 1.5

and 2 GeV protons.

Table 7: Irradiation parameters of three deuteron experiments on the E+T setup.

Deuteron beam energy

[GeV] 1.6 2.52 4

Beam start 17.12.2006

23:55:33

30.11.2005

7:01:11

25.11.2009

23:59:20

Beam end 18.12.2006

6:42:18

30.11.2005

15:00:48

26.11.2009

17:47:37

Time of irradiation [h] 6.7 8 17.8

Beam intensity

measured by operators

[1013

]

5.8 4.7 2.47

The Nuclotron ring is installed in the tunnel around the synchrophasotron, see

Figure 31 and 33. This tunnel was originally built for cable communications and the

equipment of the synchrophasotron vacuum system. The Nuclotron median plane is at

3.7 m below the synchrophasotron one.

The Nuclotron lattice is typical for strong-focusing synchrotrons with separated

functions. It contains 8 super periods and 8 straight sections, one of which is "warm".

General view of the Nuclotron dipole and quadrupole magnet is presented on Figure 32.

The magnets are fastened to a vacuum shell of the cryostat 540 mm by 8 suspension

parts of stainless steel. A nitrogen shield 490 mm covered with 20 layers of super

insulation is placed in the vacuum space between the magnet and the vacuum shell. The

dipole magnet has a window-frame type iron yoke with the sizes of window of

110x55 mm2. The quadrupole lens has the iron yoke with hyperbolic poles. The SC-

cable was manufactured of a 5 mm in diameter copper-nickel tube with a wall thickness

of 0.5 mm and 31 in parallel connected multifilament strands of 0.5 mm in diameter

covering an outer surface of the tube. The strand consist of 1045 NbTi filaments 10 m

in diameter stabilized by copper [57].

The design parameters of the dipoles are: B=2.2 T and dB/dt = 2 4 T/s.

Nominal current amplitudes are: up to 6.3 kA and 6 kA for the dipoles and quadrupoles

respectively. There are 96 dipoles, 64 quadrupole, and 32 correcting SC-magnets in the

4. BEAM DIAGNOSTICS ON NUCLOTRON ACCELERATOR

56

Nuclotron ring with circumference of 251.5 m. Averaged specific weight of the

magnetic system is only 0.32 t/m.

Figure 31: Nuclotron site scheme. Energy plus Transmutation setup is placed in Hall B

[57].

Figure 32: One section of the

Nuclotron accelerator (inside beam

tube surrounded with superconducting

magnet, He and LN2-cooling pipes,

isolation and steel shell) [57].

Figure 33: Nuclotron accelerator ring in the

Synchrophasotron cable tunnel (own

photo). Underlying is the beam outlet.

4.1. Nuclotron accelerator

57

Table 8: Selected parameters of Nuclotron accelerator compared to the older

Synchrophasotron accelerator [58].

Parameter Synchrophasotron Nuclotron

Maximal kinetic energy - protons [GeV] 9 12.8

Maximal kinetic energy - Z/A=1/2 [GeV/A] 4 6

Repetition time (p.p.s.) 0.1 0.5 - 1.0

Extraction time [s] 0.5 10

Vacuum [torr] 10-6

- 10-7

10-10

- 10-11

Maximal magnetic field in magnets [T] 1.1 2.2

Circumference [m] 207.3 251.5

Accelerator consumption [MW] 8.5 0.7note 12

Figure 34: General scheme of the Nuclotron cryogenics. 1 - vacuum shell; 2 - heat

shield; 3 - supply header; 4 - return header; 5 - dipole magnet; 6 - quadrupole magnet; 7

- subcooler; 8 - separator; 9 - helium flow from the refrigerator; 10 - return helium flow

to the refrigerator, [59].

General scheme of the Nuclotron cryogenics is presented in Figure 34. All the

magnets are connected in parallel with supply and return helium headers. The internal

diameters of the headers are 36 mm and 52 mm respectively. The cooling of the

magnets is performed by two-phase helium flow. The liquid-vapor content varies from 0

12

0.7 MW is the consumption of the accelerator. Total consumption of the accelerator complex is ~8 MW

(cooling, vacuum etc.). Consumption of the beam guide to user area is another 8 – 13 MW according to

the place, energy and guided particles [60].


58

at the inlet of the magnet to 0.9 at its outlet. The temperature sensors are placed at the

helium inlet and outlet of the winding and also at the helium outlet of the iron yoke of

each magnet. Totally, the temperature measuring system includes about 600 points. The

Nuclotron operational temperature is 4.5-4.7 K. The cryogenic supply system is based

on three industrial helium refrigerator/liquefiers with a total capacity of 4.8 kW at

4.5 K.

Helium cooling of the accelerator is nowadays the biggest limitation for our

experiments. High price of helium in coincidence with leaking compressors enable to

accelerate particles only a few weeks in the year. For every accelerator run, operators

receive much more beam requests than they can accommodate. Moreover, cooling

system is a source of frequent failures, which canceled or postponed our irradiation in

the past. In the year 2011, a new system of cryogenic cooling should be installed and

thus annual year load should increase significantly.

4.2. Irradiation course The runs of the accelerator were unfortunately not too much stable during our

experiments, below are the figures from the irradiation process.

0:00 1:00 2:00 3:00 4:00 5:00 6:00 7:00

Beam

in

ten

sity

[d

eu

tero

n/b

un

ch

]

Time

3.0·1010

2.5·1010

2.0·1010

1.5·1010

1.0·1010

5.0·109

0

Figure 35: Beam intensity during 1.6 GeV deuteron irradiation of the E+T setup.

4.2. Irradiation course

59

6:00 7:00 8:00 9:00 10:00 11:00 12:00 13:00 14:00 15:00 16:00

Beam

inte

nsi

ty [

deute

ron/b

unch]

Time

3.5·1010

3 ·1010

2.5·1010

2 ·1010

1.5·1010

5 ·109

1 ·1010

0

Figure 36: Beam intensity during 2.52 GeV deuteron irradiation of the E+T setup.

0:00 2:00 4:00 6:00 8:00 10:00 12:00 14:00 16:00

Beam

inte

nsi

ty[d

eute

ron/b

unch]

Time

1.5·1010

5·109

7.5·109

1.0·1010

1.25·1010

0

2.5·109

Figure 37: Beam intensity during 4 GeV deuteron irradiation of the E+T setup.

Irradiation instabilities had to be corrected; so-called beam instability correction

is described in chapter 3, section 10.


60

4.3. Beam position and shape

Knowledge of the beam position and shape is crucial for the experiment

evaluation. Significant influence of the beam position on experimental results was

observed in the activation detectors placed close to the target axis, MCNPX simulations

were done to assess this effect [31]. In MCNPX simulations, experimentally measured

beam position and shape parameters are used in order to calculate comparable data. In

the following paragraphs a description of the beam measurement procedure and

examples of its application on deuteron experiments will be shown.

The geometrical adjustment of the experimental setup with respect to the

deuteron beam was tuned before the irradiation by the means of sensitive Polaroid

films. Only one low intensity bunch was necessary to get a visible trace on the Polariod

film. Films were placed directly in front of the target to see the position and profile at

the point, where the beam entered the target. Another Polaroid film was placed behind

the target to check the direction of the beam in the target. When the beam was not in the

target centre, whole setup was moved on the rails and lifted by screws and the Polaroid

procedure was repeated, until the target axis was reached. Examples of the irradiated

Polaroid films are on the Figure 38. A new method of beam alignment has to be

developed for future, because the Polaroid films are not produced anymore and the rest

of the reserves has already expired.

Figure 38: Polaroid films for pre-irradiation beam alignment (2.52 GeV deuteron

experiment).

Beam parameters during the irradiation were determined independently from

solid state nuclear track detectors (Belarus group) and from a set of copper activation

foils. Gained results were compared and a common beam-report was always prepared,

e.g. [61]. I will further discuss my results and compare them with the results of other

E&T groups.

I used a set of copper foils, which I placed directly in front of the target and

behind it. The copper was chosen, because in interaction with deuteron a lot of

radioactive isotopes are produced, but none of them are produced by neutrons13

. On the

13

Aluminum cannot be used at this position because of a significant production of the same isotope 24

Na

by the neutrons.


61

other hand, no experimental cross-sections are known for interaction of relativistic

deuteron and copper. I could make only relative comparison between the foils.

For measurement of the beam position in front of the target, 60x60 mm2 copper

foil was used in 1.6 and 2.52 GeV experiment. To cover bigger area of the beam

monitoring, I have enlarged the size of monitoring foil to 80x80 mm2 in the case of

4 GeV experiment, see Figure 39. Thickness of the foil was 100 m, respectively 70 m

in the case of 4 GeV deuteron experiment. I cut the foil after the irradiation into

20x20 mm2 pieces (totally 9 pieces, respectively 16 pieces in the case of 4 GeV

experiment), and I measured these pieces separately. Following isotopes were observed: 24

Na, 43

K, 47

Sc, 48

Sc, 44m

Sc, 44

Sc, 48

V, 48

Cr, 52

Mn, 58

Co, 56

Co, 55

Co, 57

Ni, and 61

Cu.

Totally 19 lines were used for the final evaluation. I have observed above mentioned

isotopes only in the most active foils, in other foils they were not detected or were on

the level of detection limit (this represents relative production between 1 % and 6 % in

non-hit foils). None of these isotopes was visible in all foils and with similar activities;

this lead me to the presumption that all the isotopes I used were produced by the

deuterons from the beam and not by back-scattered neutrons from the target. Yields of

each isotope were normalized to the most active foil and a weighted average over all

reactions and used gamma lines was made.

Figure 39: Photo of the copper foil used for front beam monitor (left) and its paper

envelope (right).

I will discuss 4 GeV experiment as a representative of the beam position

measurement (this beam analysis was done most detailed because of the large beam

shift). Relevant weighted averages are in the Table 9 and Figure 40.


62

0.06

0.78

0.37

0.02

0.02

1.00

0.51

0.03

0.04 0.020.010.01

0.02 0.040.030.02

Beam profile in front of the target - big monitors

left rightcentre

centre

top

down

1 2 3 4

5 6 7 8

9 10 11 12

13 14 15 16

Target

Figure 40: Weighted average over relative yields of 19 different gamma-lines in the

forward Cu beam monitor during 4 GeV experiment (left). Schema of the foil-cut and

target projection (right).

Even during gamma spectra measurement I could see (according to the activities

in the foils), where the beam passed through the uncut foil. In the case of 4 GeV

experiment I saw that the highest activity was in the right-up foils on the edge (and at

that moment I did not know if some or how much deuterons went out of the foil).

I decided to cut the most active foils 3, 4, 7, and 8 onto smaller pieces 1x1x0.007 cm3

and I measured each of them once again. I did the same procedure as in the previous

case and got results presented in Figure 41. I did these measurements two days later and

some of the isotopes were already decayed, but final weighted average is still over 11

gamma-lines. Values with their uncertainties are summarized in the Table 9.

0.04

0.08

0.06

0.03

0.28

0.77

0.37

0.09

0.31

1.00

0.54

0.10

0.04

0.12

0.08

0.03

Beam profile from small monitors

left

right

centre

centre

top

down

3-1 3-2 4-1 4-2

3-3 3-4 4-3 4-4

7-1 7-2 8-1 8-2

7-3 7-4 8-3 8-4

16151413

9 10 11 12

1 2

5 6

Target


double cut Cu beam monitor irradiated in 4 GeV deuteron experiment (left). Schema of

the foil-cut and target projection is on the right.


63

Table 9: Weighted average over relative yields in forward Cu monitor during 4 GeV

deuteron experiment.

Number of foil Relative yield

(uncertainty)

Number of foil Relative yield

(uncertainty)

1 0.055(11) 3-1 0.033(5)

2 0.0187(24) 3-2 0.060(5)

3 0.368(4) 3-3 0.077(5)

4 0.775(6) 3-4 0.042(5)

5 0.0160(22) 4-1 0.092(5)

6 0.0256(18) 4-2 0.372(9)

7 0.513(5) 4-3 0.771(13)

8 1.000(7) 4-4 0.277(7)

9 0.038(12) 7-1 0.104(6)

10 0.0076(21) 7-2 0.536(8)

11 0.0139(19) 7-3 1.000(11)

12 0.0161(18) 7-4 0.311(6)

13 0.018(8) 8-1 0.0283(22)

14 0.018(5) 8-2 0.083(5)

15 0.032(14) 8-3 0.118(4)

16 0.037(18) 8-4 0.0440(27)

A Gaussian beam profile in X and Y axis was assumed. Measured data were

fitted in the PAW program [62]. The final shift of the beam was during deuteron

irradiations in order of millimeters up to units of centimeters and is summarized in

following Table 10.

In 1.6 GeV experiment I also used two copper foils placed in front of the target

to measure exactly how many deuterons went out of the target. I used circles 84 mm in

diameter (same as target) and 120 mm in diameter. For the gamma measurement I

bended the foils to a smaller pieces approximately 25x25x3 mm3 big. Further analysis

procedure was the same as at forward beam monitor. Results can be seen on Figure 42.

In 2.52 GeV and 4 GeV experiment it was unfortunately not possible to place these foils

in the setup, so I can assess number of the out-of-target deuterons only from the fit.


64

Table 10: Beam position, shape and intensity during deuteron experiments, comparison

of data from various groups.

Deuteron beam energy [GeV] 1.6 2.52 4

Me I. Zhuk Me I. Zhuk Me I. Zhuk

X-axis shift [cm] -0.85 -0.64 1 1.5 2.35 2.1

Y-axis shift [cm] -0.6 -0.39 -0.4 -0.3 1.9 1.8

FWHM in x [cm] 3.45 2.87 1.7 1.63 1.53 2.4

FWHM in y [cm] 2.8 1.92 2.3 1.56 1.77 1.7

Measured beam intensity

[1013

] - Me 2.4±0.2

14 0.642 ±0.017 1.985 ± 0.019

Measured beam intensity

[1013

] - W. Westmeier 2.45 ± 0.1 0.650 ±0.021 1.40 ± 0.15

Final beam intensity [1013

] 2.45 ± 0.1 0.645 ±0.013 up to now

unknown

Deuterons out of the target -

Me 6 % - < 8 %


W. Westmeier 21.3 % 1 % 43.7 %


I. Zhuk 0.3 % 3 % 8.2 %

Final number of deuterons

out of the target 0.3 % 3 %

up to now

unknown

8.4 cm

12 cm

1.00

0.0600 ± 0.0004

Figure 42: Relative number of deuterons that did not hit the target during 2.52 GeV


I placed copper foil also behind the target to check the beam direction in the

target (if the beam goes parallel with the target axis). I used foil with dimensions

90x90x0.12 mm3 and made of the same copper as the front foil. After the irradiation I

14

Value determined only from 22

Na and 7Be reactions using method proposed by J. Blocki [63].


65

cut it onto 9 pieces 30x30x0.12 mm3 big and I measured each part separately. I detected

the same isotopes as in the forward foil and I was able to do the weighted average over

19 lines. From the results (Figure 43) we can see that the beam was during the 4 GeV

deuteron run more or less parallel with the target axis (the same I observed also in other

deuteron experiments).

0.07 0.11 0.15

0.11

0.39

0.64

0.12

0.49

1.00

Behind target

centre

top

down

left rightcentre

Z-1 Z-2 Z-3

Z-4 Z-5 Z-6

Z-7 Z-8 Z-9

Target

Figure 43: Weighted average over relative yields of 19 different gamma-lines in the Cu

beam monitor placed behind the target during 4 GeV deuteron experiment (left).

Schema of the foil-cut and target dimension (right).

4.4. Beam intensity Beam intensity was measured using aluminum foils. W. Westmeier used

concentric rings placed few meters in front of the setup, I used a square foil

100x100x0.2 mm3 placed close to W. Westmeier‟s ones. Number of neutrons coming

from the target is negligible at this distance; it was proven by M. Majerle using

MCNPX [64].

Cross-section of the 27

Al(d,3p2n)24

Na reaction is the only one known cross-

section at the region of GeV energies of deuterons with suitable half-life and energies of

gammas. It was measured by J. Banaigs [65] at deuteron energy 2330 MeV

(15.25 ± 1.5 mbarn), see Figure 44. I made a fit of the data in order to assess the change

of the cross-section value within our energy region. The most suitable seemed to be a

function bxay , which described well the data both in low and high energy region.

Finally, I used the same value as W. Westmeier in his analysis in order to get

comparable data. His fitted values are close to my fit, changes come from the selection

of the beginning of fitted curve. Cross-section uncertainties are not involved in the

uncertainty of the beam intensity.


66

For the gamma measurement on the detector I middled the foil few times to get a

dimension approximately 25x25x3 mm3. I measured this packed foil on the detector a

several times in various geometries (and also on different detectors if possible) to

suppress the uncertainty coming from detector calibration. The foil was also rather

thick, so a correction on detector efficiency was necessary, see chapter 3 section 7.

Same corrections as described in the section related to the sample evaluation were used.

Example of the summary of the intensity measurement is in the Table 11 (in this case it

is concretely 4 GeV deuteron experiment).

0

0.01

0.02

0.03

0.04

0.05

0.06

0.07

0.08

1 10 100 1000 10000

Cro

ss-s

ecti

on

[b

arn

]

Deuteron energy [MeV]

27Al(d,3p2n)24Na

measured value - 2.33 GeV - 15.25 mbarn

1.6 GeV - 15.75 mbarn 2.52 GeV - 15.12 mbarn

4 GeV - 14.49 mbarn

Figure 44: Cross-section15

of the 27

Al(d,3p2n)24

Na reaction from EXFOR [66] and fit

between the values for used deuteron energies.

Beam intensity Nd was calculated according to the following equation (4.1), where Nyield

(of 24

Na) is calculated using the (3.26) equation.

A

Yield

dN

ASNN

(4.1)

where:

S – area of the foil

A – molar weight

NA – Avogadro number

- 27

Al(d,3p2n)24

Na reaction cross-section

15

1 barn = 10-28

m2

4.4. Beam intensity

67

Table 11: Summary of the beam intensity measurements done in 4 GeV deuteron

experiment.

Spectrum16

wA

lbig

p51

wA

lbig

p54

wA

lbig

p46

wA

lbig

p5O

rt3

wA

lbig

p4O

rt2

wA

lbig

p3O

rt5

Yie

lds

of

24N

a fr

om

sep

arat

e

gam

ma-

lines

17

1368

keV

3.42E+08 3.35E+08 3.45E+08 3.45E+08 3.56E+08 3.62E+08

unce

rt

6.50E+06 5.35E+06 9.99E+06 6.56E+06 5.69E+06 4.70E+06

2754

keV

3.26E+08 3.44E+08 3.40E+08 3.14E+08 3.33E+08 3.38E+08

unce

rt

6.20E+06 6.53E+06 6.11E+06 4.71E+06 5.33E+06 4.73E+06

Eff

icie

ncy

of

det

ecto

r

1368

keV

0.00193 0.00193 0.00365 0.00207 0.00420 0.00859

2754

keV

0.00098 0.00098 0.00185 0.00118 0.00234 0.00476

Changed

efficiency

correction18

1.025 1.025 1.034 1.027 1.039 1.041

COI

1368

keV

0.9925 0.9925 0.9867 0.9939 0.9885 0.9771

27

54

keV

0.9925 0.9925 0.9884 0.9877 0.9768 0.9542

Non-point like

emitter

correction

0.9906 0.9906 0.9838 0.9906 0.9838 0.9709

16

Spectra label is constructed in following way, e.g. wAlbigp51 – w is from Wagner (our spectrum), Al –

material, big – label for beam monitor foil, p5 – position on the detector, 1 – number of measurement.

17 Grey marked numbers were omitted from the further evaluation because of their deviousness.

18 Changed efficiency correction means change of the detector peak efficiency due to the thickness of the

sample (3 mm) in comparison to standard one – centre of the thick sample is closer to the detector.


68

Beam

correction 0.9695

Sel

f-

abso

rpti

on

corr

ecti

on

1368

keV

1.0212

2754

keV

1.0145

Wei

ghte

d

aver

age

for

1368

keV

3.49E+08 uncert. 2.44E+06 χ2 3.51

2754

keV

3.31E+08 uncert. 2.23E+06 χ2 7.09

Total weighted

average (except

3.10E+08

value)

3.43E+08 uncert. 1.76E+06 χ2 3.48

Number of

deuterons 1.99E+13 uncert. 1.91E+11

In each experiment there was a difference between the beam intensity value

measured by me and by W. Westmeier, but till the 4 GeV deuteron experiment,

differences were always within the uncertainty bars. In 4 GeV deuteron experiment, a

new additional electronic system of beam monitoring was installed. Unfortunately,

beam intensity measured by this device is by 25 percent higher than my value, which is

of 30 percent higher than the value of W. Westmeier. Up to now, no clear reason for

such differences was found19

.

When searching for the source of uncertainties I tried to calculate the beam

intensity using also other reactions in the Al monitor and in the copper monitor of beam

shape and profile. There are no experimental data for cross-section of deuterons and

copper (or Al except those leading to 24

Na), but a lot of data exist for protons on copper

and aluminum. It is possible to recalculate the cross-sections from proton to deuteron

using following method (proposed by J. Blocki [63], used also by W. Westmeier to

analyze the yields of 22

Na and 7Be in his Al beam intensity monitor).

Cross-section recalculation is based on the presumption that there is a fixed ratio

between the inelastic cross-section for proton and deuteron (at relativistic energies two

nucleons in 2H behave as two separate items). Cross-section for protons and deuterons

seems to change slowly and run parallel at GeV energies. I have started from already

mentioned reaction 27

Al(d,3p2n)24

Na, where I know the cross-section for deuterons at

2330 MeV (J. Banaigs, [65]). I found cross-section for protons leading also to 24

Na

(reaction 27

Al(p,3pn)24

Na) at similar energy 1200 MeV: Dittrich B. 12 mbarn [67],

19

Data analysis of this experiment was not closed up to now and will be a subject of M. Suchopár‟s PhD

work.

4.4. Beam intensity

69

Michel R. 10.8 mbarn [68], and Titarenko 12.9 mbarn [69]. Mean cross-section value is

11.9 mbarn. Ratio between the deuteron and proton cross-section is thus 1.282 (this

should be the same for all reactions on Al). With this ratio I multiplied cross-sections of

proton induced reactions 27

Al(p,3p3n)22

Na and 27

Al(p,10p11n)7Be and calculated beam

intensity from the 22

Na and 7Be yields produced by deuteron beams. In the best case the

differences from the directly evaluated intensity were smaller than 4 % at the 22

Na and

2 % at 7Be (in the case of 1.6 GeV deuteron experiment). During 2.52 GeV deuteron

experiment no long-time measurements of Al beam monitors were done (because of

lack of time), so it was not possible to test this procedure. In the 4 GeV experiment, the

differences were much higher: beam intensity was 15 % higher in the case of 22

Na,

respectively 50 % higher in the case of 7Be (statistical uncertainty from DEIMOS32 is

six percent at 22

Na and 20 percent at 7Be).

The reason for the disagreement can be partially in bad statistics; long term

measurement for 22

Na and 7Be was done in the case of 4 GeV experiment half a year

after the irradiation and took place for a few weeks. The natural background played a

significant role in this case and had to be subtracted at 7Be. Another source

of disagreement can be in chosen cross-section of protons with Al or in the efficiency of

the detector.

Finally, I tried to calculate deuteron beam intensity from the copper foils. No

experimental cross-sections for suitable nat

Cu(d,x) reactions are known at used energy

region, so I had to calculate my own cross-sections. Above mentioned procedure was

not usable because of missing cross-sections, so I assumed the beam intensity in

2.52 GeV deuteron experiment is determined properly. With this beam intensity I have

calculated cross-sections of various reactions observed on copper during 2.52 GeV

deuteron experiment. These cross-sections I have to shift to 1.6 GeV and 4 GeV energy.

I have done the shift according three various reactions for protons, for which I have

found experimental cross-section at 1.6 GeV, 2.52 GeV and 4 GeV. I have determined

average ratio between the cross-sections (1.6 GeV / 2.52 GeV, respectively 4 GeV /

2.52 GeV). With this ratio I have shifted the cross-sections and calculated deuteron

beam intensity for 1.6 GeV and 4 GeV E+T experiment.

For some of the reactions the beam intensity values were close to the intensity

value determined by 24

Na, but some of them were one order of magnitude higher or

lower (no serious reason for the discrepancy was found). The final result (average over

10 reactions) is in the case of 1.6 GeV experiment (2.24 ± 0.08)·1013

deuterons in the

beam (value determined from the 24

Na is (2.45 ± 0.04)·1013

, so this procedure gives

rather good results, but is less reliable. In the case of 4 GeV experiment this analysis has

not been finished yet, but the preliminary value of the beam intensity determined by

using the data from copper foil is (2.5 ± 0.7)·1013

(intensity determined from 24

Na is

(1.985 ± 0.019)·1013

).


70

71

Chapter 5

E+T results of deuteron irradiation

5.1. Plain experimental results After the gamma-spectra evaluation and application of necessary spectroscopic

corrections, I have determined the yields of produced isotopes. These yields are

proportional to the neutron field in the place of the foil20

. The uncertainty bars in the

graphs bellow are only from the Gauss fit in the DEIMOS32 and are hardly visible in

the logarithmic scale (are only a few %). Lines in the graphs are only to guide reader‟s

eyes and have no real physical meaning.

-5 5 15 25 35 45

Yie

ld [1

/g*

deu

tero

n]

Position along the target [cm]

198Au 196Au 194Au 192Au 24Na

10-7

10-6

10-5

10-4

10-3

10-2

Figure 45: Yields of the isotopes produced in Au and Al activation detectors in

longitudinal direction, 3 cm over the target axis, 1.6 GeV deuteron experiment.

Products of the threshold reactions have their maxima near to the first gap

(~12 cm from the target beginning). This value does not differ for higher beam energies

very much, although the deuteron range in the lead is rising. The reason is in the

probability of the first collision (spallation), which takes place for most of the deuterons

in first ~20 cm. During the spallation reaction high energy neutrons are produced mostly

to the forward angles (intranuclear cascade), neutrons from high energy fission and

evaporation are produced isotropicaly. These isotropicaly emitted neutrons cause most

of the threshold reactions in the foils placed in front of the lead target.

20

The higher the yield of some (n,xn) reaction is, the more neutrons with the energy higher than the

relevant threshold had to be in that place.

5. ENERGY + TRANSMUTATION RESULTS OF DEUTERON IRRADIATION

72

-5 5 15 25 35 45

Yie

ld [1/g

*deute

ron]

Position along the target[cm]

198Au 196Au 194Au 192Au 24Na

10-7

10-6

10-5

10-4

10-3

10-2


longitudinal direction, 10.7 cm over the target axis, 1.6 GeV deuteron experiment.

Non-threshold 197

Au(n,)198

Au reaction is caused by the epithermal and

resonance neutrons coming from the biological shielding. High energy neutrons

escaping from the target and blanket are moderated in the polyethylene inside the

shielding and some of them are backscattered into the inner volume of the biological

shielding. Cadmium layer on the inner walls of the shielding absorbs only neutrons with

energies under the cadmium edge (0.5 eV). Neutrons with higher energies create inside

the biological shielding almost constant field, which is not so strong like the field of

high energy neutrons, see Figure 63. But, the yields of 198

Au or 182

Ta are by one to two

orders of magnitude higher than the yields of threshold reactions due to the high cross-

section values of the non-threshold reactions, see Figure 45 or Figure 46.

Field of epithermal and resonance neutrons inside the biological shielding is

disturbed only in the beginning and at the end of the setup due to the holes

in the shielding (used for manipulation and beam entrance). This can be documented in

the Figure 46, where the outer points of 198

Au yield are lower than the average between.

In radial direction the yields of threshold reactions are quickly (almost

exponentially) decreasing. This can be read out from the lines in Figure 47 and Figure

48. From the product of non-threshold 198

Au can be seen, that the epithermal and

resonance neutron field is really homogenous in radial direction. It is slightly disturbed

close to the target by difference in neutron absorption in uranium and lead (there are a

lot of resonances of neutron capture in 238

U, see Figure 64). Outside the blanket

(10.7 cm position) there is visible a small influence of the moderator/reflector.

5.1. Plain experimental results

73

2 4 6 8 10 12

Yie

ld [

1/g

*d

eute

ron

]

Radial distance from the target axis [cm]

198Au 196Au 194Au 192Au 24Na

10-7

10-6

10-5

10-4

10-3

10-2

Figure 47: Yields of the isotopes produced in Au and Al activation detectors in radial

direction, first gap of the E+T setup – 12.2 cm from the target beginning, 1.6 GeV


2 4 6 8 10 12

Yie

ld [1/g

*deute

ron]


198Au 196Au 194Au 192Au 24Na

10-7

10-6

10-5

10-4

10-3

10-2


direction, behind the E+T setup – 48.8 cm from the target beginning, 1.6 GeV deuteron

experiment.


74

More figures for reactions on Bi, In, Ta and Y from 1.6 GeV experiment as well

as from 2.52 GeV and 4 GeV deuteron experiment can be found in Appendix G.

-5 5 15 25 35 45

Yie

ld [1/g

*deu

tero

n]

Distance along the target [cm]

3 cm

6 cm

8.5 cm

10.7 cm

196Au

4·10-5

3·10-5

2·10-5

1·10-5

0

Figure 49: Yields of the

196Au isotope produced in Au activation detectors in

longitudinal direction, various distance from the target axis, 1.6 GeV deuteron

experiment.

2 4 6 8 10 12

Yie

ld [

1/g

*deu

tero

n]


in front of

1st gap

2nd gap

3rd gap

behind target

4·10-5

3·10-5

2·10-5

1·10-5

0

196Au

Figure 50: Yields of the 196

Au isotope produced in Au activation detectors in radial

direction, various distance from the target beginning, 1.6 GeV deuteron experiment.

5.1. Plain experimental results

75

Example of the comparison of the yields of threshold reaction 197

Au(n,2n)196

Au

(threshold 8.1 MeV) is shown on the Figure 49 and Figure 50. Normal scale is used for

the Y-axis (not a logarithmic one), thus the statistic uncertainties from Gauss fit in

DEIMOS32 are better visible. In the longitudinal direction it can be seen that

the highest production was close to the target centre (3 cm from the target axis). In the

radial direction the highest flux of the neutrons with E > 8 MeV was in the first gap

(12.2 cm from the beginning of the target), than in the second gap and the lowest flux

was behind the target.

Most of the data were already published on national conferences (6. Mikulášské

setkání sekce mladých při České nukleární společnosti [70]) and international

conferences (Baldin conference [71], ND2007 [72], NEMEA-4 [73]). General overview

can be found in article in revised journal Nuclear Instruments and Methods in Physics

Research [74].

5.2. Ratios of yields for different thresholds In Figure 51 are plotted ratios of the yields of various threshold reactions in front

of and behind the target in dependence on their threshold (longitudinal direction 3 cm

over the target axis). Neither in 1.6 GeV deuteron experiment nor in 2.52 GeV deuteron

experiment (see Appendix G, section 4) a clear dependence is visible like it was during

proton experiments (see e.g. [30] or [32]). There is some trend that shows a decrease of

the ratio with rising threshold energy, that means the difference in neutron flux in front

of and behind the target is smaller for neutron energies higher than ~20 MeV.

The difference comes from the probability of the first interaction, respectively

spallation reaction. Neutron field inside the setup is a complicated mixture of spallation,

fission, moderated and back-scattered neutrons. Neutron field has its maximum around

12 cm from the target beginning, see e.g. Figure 45. Neutrons with higher energies

come from the intranuclear phase of the spallation reaction and are emitted more

forward, in contradiction to neutrons below 20 MeV, which come from evaporation and

fission phase of the spallation reaction and are emitted isotropicaly. Epithermal

and resonance neutrons come from the biological shielding. Combination of the

spallation probability and various sources of neutrons in spallation reaction causes

observed difference in front/end yield ratio for threshold energy approximately 20 MeV.

In radial direction the ratios are calculated from the yields at 3 cm and 10.7 cm

from the target axis. Ratios are made of the foils placed in the first gap of the setup

(place with maximal neutron flux). The ratios oscillate around the value 6.5 up to the

neutron energy 35 MeV in the case of 1.6 GeV experiment, see Figure 52. Above

35 MeV there is a steep increase. The situation is very similar in the case of 2.52 GeV

deuteron experiment, see Figure 126 in the Appendix G. This difference originates from

the course of spallation reaction – neutrons with higher energies are produced mainly in

intranuclear cascade and move to forward angels, so they can hardly get far from the

target in radial direction.


76

0

1

2

3

4

5

0 10 20 30 40 50 60

Rati

o in f

ront of

/ beh

ind targ

et [-

]

Threshold energy [MeV]

Al Au Y Bi In

Figure 51: Ratio in front of and behind the target for various threshold reactions,

1.6 GeV deuteron experiment.

0

2

4

6

8

10

12

14

16

18

0 10 20 30 40 50 60

Rati

o 3

/10

.5 c

m [

-]


Al Au Y Bi In

Figure 52: Ratio in 3cm and 10.7 cm (11.5 cm) in the first gap of the target for various

threshold reactions, 1.6 GeV deuteron experiment.

Yields of various threshold reactions can be theoretically used for deconvolution

and acquiring of the neutron spectrum in certain point. Problem can be in the knowledge

of cross-section data, there are except Bi no experimental cross-section data for

reactions higher than (n,4n) or energies over 40 MeV. Spectrum calculated with the use

5.2. Ratios of yields for different thresholds

77

of simulated/calculated cross-sections would be no more experimental. This is one of

the reasons for my cross-section measurements described in chapter 7.

Polish E+T group tried neutron spectra deconvolution from their yttrium

samples [75]. They used simulated cross-sections from the TALYS code [76], where the

experimental ones were missing. They divided the spectrum to three parts according to

various thresholds of three used (n,xn) reactions. They got three Fredholm equations

for the yields of different threshold reactions. Then they assumed that the yield is a

continuous function of threshold energy. Using further mathematical presumptions they

converted Fredholm equations to the Volterra‟s equation of the first kind and solved

them. Calculated neutron spectrum is in MeV energy region close to the simulated one,

but its maximum shifted to higher energies. Usage of this method for the deconvolution

of the yields of threshold reactions has to be further studied; authors admit problems

caused by used presumptions (final function describing the neutron spectra is concave

instead of convex function observed in MCNPX simulations). Authors also use

presumption about the shape of neutron spectrum below the threshold of the first

reaction, although they do not have any experimental sign for it.

5.3. Spectral indexes When I compared yields of reactions with different threshold (e.g.

196Au and

192Au) I have observed a spectrum hardening at the end of the target (see Figure 53 or

Figure 54).

Figure 53 or Figure 54 are in principal similar to previous Figure 51 and Figure

52. Threshold energy is here hidden in the ratio of two reactions with different

threshold. Observed spectrum hardening is specific for the spallation reaction; high

energy neutrons are produced more into the forward direction. In comparison between

experiments it can be seen that the differences in spectral indexes in front of and behind

the target are decreasing with rising beam energy. More spectral indexes can be found

in Appendix G.3.


78

10.7 cm

8.5 cm

6 cm

3 cm

0.0

0.1

0.2

0.3

0.4

012

2436

48

Sp

ectr

al in

dex

192A

u/1

96A

u [

-]

Figure 53: Neutron spectra hardening along the target in 1.6 GeV deuteron experiment

(ratio between 192

Au and 196

Au).

10.7 cm

6 cm 0.0

0.1

0.2

0.3

012

2436

48

Spectr

al in

dex 1

92A

u/1

96A

u [

-]

Figure 54: Neutron spectra hardening along the target in 4 GeV deuteron experiment

(ratio between 192

Au and 196

Au).

5.4. Comparison between deuteron experiments

79

5.4. Comparisons between deuteron experiments

It is well-known from the experiments21

that the most effective energy of the

proton beam for spallation neutron production is around 800 MeV - 1 GeV. In this

interval is the biggest neutron production per MeV per proton on heavy target. The

usage of deuterons brings another bonus in neutron production, but complicates

accelerating. This leads to lower intensity of the beam.

Experimental results (non-threshold and threshold yields per 1 gram of foil

material and one beam particle) are in following Figure 55 and Figure 56. Data are

normalized to the second foil to see the difference in the shape. More figures with

comparison of experiments (normalized and unnormalized) are in Appendix G.5.

Except the 4 GeV deuteron experiment there can be seen an increase in the

neutron flux behind the first gap (maximum) with rising beam energy. Differences in

the shape of the yields of 4 GeV deuteron experiment can be caused by the beam

placement – beam was displaced to the right and up, almost to the corner of the target

close to the Au samples (see Table 10). Some spallation in uranium was thus possible

and it is probably the reason of much higher neutron yield due to additional fission in

irradiated uranium. Yield normalization led to difference in the shape of the yields of

4 GeV deuteron experiment.

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

-5 5 15 25 35 45

Yie

ld [

-]


4 GeV d 2.52 GeV d 1.6 GeV d 0.7 GeV p

198Au

Figure 55: Comparison of non-threshold 198

Au yields in longitudinal direction at 3 cm

from the target axis, deuterons and 0.7 GeV proton experiment on E+T setup. Values

are normalized to the second foil. Results of the 4 GeV experiment are preliminary.

21

Example of multiplicity experiments can be found for example in the summary article of A.V.

Dementyev [77].


80

Comparison of unnormalized yields from various experiments shows problems

with the beam position, results of threshold 197

Au(n,2n)196

Au reaction are close together

or even disordered in front of the target and in the first gap (=maximum), where the

beam position influence is the most significant, see Figure 130 and Figure 132 in

Appendix G.5. The yields of 4 GeV deuteron experiment are much higher than the rest,

probably because of the uranium spallation and additional fission22

.

I have calculated a ratio of the 198

Au, 196

Au and 194

Au yields for 2.52 GeV /

1.6 GeV and 4 GeV / 1.6 GeV deuteron experiments. There is a clearly visible trend for 198

Au, with rising beam energy the ratio is increasing in the radial direction (groups of

foils 1-4, 5-8 etc). That means the number of epithermal and resonance neutrons is

rising more rapidly with rising beam energy. This is valid up to approximately the half

of the setup, then the trend is changing and behind the target the epithermal and

resonance neutron flux is decreasing more rapidly when moving out from the target axis

(valid for increase in beam energy). For more details see following Figure 57 and Figure

133 in Appendix G.5.

In the case of 196

Au and 194

Au threshold reactions there is no visible trend in the

yield ratios for 2.52 GeV / 1.6 GeV and 4 GeV / 1.6 GeV deuteron experiments. For

more details see Figure 134 and Figure 135 in the Appendix G.6.

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

-5 5 15 25 35 45

Yie

ld [ -

]



196Au

Figure 56: Comparison of threshold 196

Au yields in longitudinal direction, deuterons

and 0.7 GeV proton experiment on E+T setup. Values are normalized to the second foil.

Results of the 4 GeV experiment are preliminary.

22

Higher neutron fluxes due to probable spallation of uranium were observed also by other E&T RAW

groups, but their results are still preliminary.

5.4. Comparison between deuteron experiments

81

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

0 5 10 15 20

Rati

o 2

.52G

eV

/ 1

.6 G

eV

[-]

Number of foil [-]

198Au

Figure 57: Ratio of the 198

Au yields for 2.52 GeV and 1.6 GeV deuteron experiments in

all twenty Au foils, which were used.

5.5. Total neutron production The so-called water-bath/activation foil method [78] is often used for the

determination of the integral numbers of neutrons produced in thick targets.

The conventional variant of this method uses two basic premises: neutrons from the

source are predominantly contained within the moderator volume; and it is possible to

integrate the measured thermal flux distribution over the water volume with adequate

precision. As the latter requires the usage of a large-scale grid of activation foils, I have

used a new form of this method [79], which replaces the flux integration by relating a

small-scale set of foil activities to the integral quantity – the integral number of neutrons

produced per one beam particle (so-called neutron multiplicity) sim

totaln obtained by

simulation.

Polyethylene in the biological shielding of the E+T setup worked as a water bath

– it moderated outgoing neutrons. I neglected front and back openings of the biological

shielding. I did multiplicity simulations in MCNPX 2.7.a using INCL4 + ABLA

models23

. For calculation of the neutron multiplicity, I determined the ratios between

experimental and simulated yields of 198

Au in all gold samples. I tried to use also

tantalum samples for the first time, because tantalum has similar cross-section for (n,)

reaction like the gold has (see Figure 58), and tantalum samples were placed close (or

even at the same place) like the gold samples. I calculated weighted average over these

23

neutron multiplicity does not depend significantly on the combination of the models available in

MCNPX in this energy region, proven by A. Krása in his PhD work [30]


82

ratios and I multiplied it with the simulated neutron multiplicity – see following

equation 5.1:

sim

Yield

Yieldsim

totaltotalN

Nnn

exp

exp (5.1)

The advantage of this procedure is that the experimental value of neutron

multiplicity exp

totaln is highly insensitive to the simulated value sim

totaln and its uncertainty.

Assuming that the MCNPX describes well the spatial distribution of the neutrons as

well as the shape of low energy part of neutron spectrum and its approximate

magnitude; the product of the two terms in equation (5.1) effectively cancels

out the dependence on sim

totaln . Neutron multiplicity results for deuteron experiments are

summarized in Table 12, Figure 59 and Figure 60. Results from gold and

tantalum samples are comparable within the uncertainties. Multiplicity determined by

tantalum seems to be closer to the simulated multiplicity of the E+T setup.

Figure 58: Cross-section of the (n,) reaction on Au and Ta, overtaken from ENDF/B-

VII. [85].

5.5. Total neutron production

83

Table 12: Experimental neutron multiplicities for deuteron experiments24

.

Beam

energy

[GeV] per GeV per GeV

1.6 1.89 ± 0.20 100 ± 11 53.3 63 ± 7 33.3

2.52 1.41 ± 0.15 112 ± 12 79.7 44 ± 5 31.6

4 1.68 ± 0.18 189 ± 20 112.5 47 ± 5 28.1

1.6 1.85 ± 0.19 99 ± 18 53.3 62 ± 11 33.3

2.52 1.16 ± 0.12 93 ± 10 79.7 38 ± 4 31.6

4 1.35 ± 0.14 152 ± 16 112.5 38 ± 4 28.1

198Au

182Ta

exp

to ta lnexp

totalnsim

Yield

Yield

N

Nexp

sim

totaln

sim

totaln

0

50

100

150

200

250

0 1 2 3 4

Neutr

on

s per

beam

part

icle

[-]

Beam energy [GeV]

protons -exp

deuterons - exp - Au

deuterons - exp - Ta

sim-p

sim-d

Figure 59: Neutron multiplicities for E+T setup (proton experimental points overtaken

from the PhD thesis of A. Krása, [30]).

24 Data for the

182Ta in 4 GeV deuteron experiment were evaluated by our grammar school student

Ondřej Novák.


84

0

10

20

30

40

50

60

70

80

0 1 2 3 4

Neu

tro

ns

per

beam

part

icle

per

GeV

[-]

Beam energy [GeV]

protons - exp

deuterons - exp - Au

deuterons - exp - Ta

protons - sim

deuterons - sim

Figure 60: Neutron multiplicities for E+T setup normalized per GeV (proton

experimental points overtaken from the PhD thesis of A. Krása, [30]).

85

Chapter 6

MCNPX simulations of the Energy plus Transmutation

setup

6.1. MCNPX code MCNPX is a general purpose Monte Carlo radiation transport code designed to

track many particle types over broad ranges of energies [80]. MCNPX means Monte

Carlo N-Particle transport code – eXtended. It is the next generation in the series of

Monte Carlo transport codes that began at Los Alamos National Laboratory nearly sixty

years ago. The MCNPX program began in 1994 as an extension of MCNP4B and

LAHET 2.8 in support of the Accelerator Production of Tritium project (APT) [81]. The

work envisioned a formal extension of MCNP to 34 particle types and up to

teraelectronvolt energy range; improvement of physics simulation models; extension of

neutron, proton, and photonuclear libraries to 150 MeV; and the formulation of new

variance-reduction and data-analysis techniques. The APT project also included cross-

section measurements, benchmark experiments, deterministic code development, and

improvements in transmutation code and library tools.

Our group from Řež is a member of the MCNPX beta tester team, so for a long

time we have had access to the newest versions of MCNPX. In this PhD thesis, all

simulations were done in the version 2.7.a, which is the newest version we are allowed

to use. Beta tester mailing list is another helpful tool we use. Through this we can get

help and advice from the people from MCNPX community almost immediately.

6.2. Limitations of MCNPX code MCNPX code has specific restrictions coming out from its Monte-Carlo

approach. Correctness and accuracy of the MCNPX calculation is limited by used cross-

section data libraries, physical models and intrinsic imprecision. Spectra of different

particles are weakly dependant on the choice of used library (proven in M. Majerle‟s

PhD thesis, [41]). In my calculations I used LA150 library for proton and neutron

transport (it seems to give the best results). Energy range of the library is limited to

150 MeV, cross-section models are used for higher energies. For (n,xn) reactions, cross-

section combined from TALYS [82] and MCNPX - CEM were used to get the most

reliable results.

Correctness of the MCNPX is also determined by the description of physical

processes. In the case of MCNPX descriptions are based both on empirical fits of

experimental data and on mathematical idealizations of predicted theories. In my case

a description of the spallation reaction and transport of high energy particles is the most

crucial point. MCNPX offers a following set of intranuclear cascade models (BERTINI,

ISABEL, INCL4) and evaporation models (DRESNER, ABLA), which can be

combined, or all in one model (CEM03). Results of the MCNPX calculations with

different combinations were one of the topics studied by A. Krása. In his PhD thesis he

6. MCNPX SIMULATIONS OF THE E+T SETUP

86

used all available combinations of models for protons and studied the changes in the

yields of threshold and non-threshold reactions in our samples.

Up to the MCNPX version 2.6.e only the combination of INCL/ABLA was able

to handle the deuterons with energy higher than 2 GeV. From MCNPX 2.6.e all models

can be used also for higher deuteron beam energies. I used INCL4/ABLA combination

because it was available in all previous versions and thus it has been better tested.

Another reason is that INCL4/ABLA was used by A. Krása and M. Majerle in their

proton calculations prepared for comparison with deuterons (e.g. multiplicity).

Unfortunately, INCL4 model is very slow and the simulation takes ~10 times more

computer time than the other models. PC cluster of 64 processors was installed at

Nuclear Spectroscopy Department of the NPI in Řež and it is used for calculations, so

one E+T calculation with 107 source particles takes approximately one day.

Under intrinsic imprecision are meant rounding errors, interpretation of

numbers, inaccuracies in numerical solving of equations etc. These imprecision cannot

be usually influenced and changed by the user.

Another limitation of the code is due to the random nature of generated events.

Large number of single events is necessary to collect enough statistics in our small

volumes representing activation foils. Typical example can be in the case of 196

Au and 198

Au isotopes. In the spallation reaction mostly high energy neutrons are produced, so

enough neutrons above the reaction threshold can be collected in the foil for e.g. 106

source particles. 198

Au is produced mostly by the resonance neutrons, whose number is

at 106 source particles much smaller and hence determined with worse accuracy.

Number of source particles (statistics) had to be thus enlarged in some cases.

High statistics is connected with the problem of computer time, as mentioned

above. Precision of the calculation depends inversely on the square-root of the number

of processed events, so there is not too much place for a radical decrease of the

statistical uncertainties in simulations.

6.3. Simulation of the E+T setup For every E+T experiment we made a set of MCNPX simulations, e.g. [32].

After a few years of improving the setup description in the code, we have a detailed

model of the experimental setup now (see Appendix H). Two-dimensional visualization

can be seen in Figure 61-right, three dimensional visualization of some setup parts can

be seen on Figure 61-left and Figure 62.

Development and improvements of the MCNPX input file and calculation

procedure was one of the main tasks of my colleague M. Majerle and it is described in

his PhD thesis [41]. M. Majerle also studied various details of the E+T setup using

MCNPX. He tested the influence of the proton beam shape and position, foil placement

and thickness, setup composition etc. Results of these studies are also described in his

PhD work and in publications (e.g. [31] or [53]).

6.3. Simulation of the E+T setup

87

Figure 61: Visualization of the Energy plus Transmutation setup as defined in MCNPX

input file. On the left is SABRINA [83] plot provided by Jaroslav Šolc.

Figure 62: Model of the parts of E+T setup in MCNPX, rendered in Povray25

code [84],

author M. Majerle.

6.4. Neutron fluxes in the E+T setup Advantage of the MCNPX simulation is a possibility of easy calculation of

practically immeasurable things. In the calculation I can change material composition,

density and add or except parts of the setup like shielding, structural materials, uranium

etc. I repeated calculations of the neutron, proton and deuteron fluxes in the four target

cylinders that I formerly performed for 0.7 GeV proton experiment [29]. This time I

used deuterons with energy 2.52 GeV. In the Figure 63 we can see dependence between

the presence of various parts of the setup and produced neutron fluxes.

25

The Persistence of Vision Raytracer (POVRAY) is a high-quality, totally free tool for creating

stunning three-dimensional graphics [84]. It is available in official versions for Windows, Mac OS/Mac

OS X and i86 Linux.

http://www.povray.org/download/

http://hof.povray.org/







88

Neu

tro

n f

lux

·E[d

eu

tero

n-1

.cm

-2.M

eV

-1]

Neutron energy [MeV]

Pb Pb+const Pb+U+const without Cd whole E+T

10-2 100 102 10410-410-610-8

100

10-2

10-4

10-6

10-8

Figure 63: Neutron flux (multiplied by energy because of binning) in the first target

cylinder irradiated with 2.52 GeV deuterons, log-log scale, various parts of the setup are

omitted. Uncertainties are on the level of 1 percent.

Figure 64: Cross-section of the (n,) reaction on 238

U in ENDF database [85].

6.4. Neutron fluxes in the E+T setup

89

Difference between bare Pb target and target with all constructions (Al and Fe

support structures, U-rod cover from Al etc.) is almost negligible, support structures add

some more high energy neutrons due to the spallation induced on them by scattered

neutrons. Addition of natural uranium causes more neutrons in the region between

1 keV and 1 MeV due to the high energy fission. Biological shielding adds further

neutrons to the low energy region bellow 10 keV and also a second maximum of the

neutron spectrum around 0.025 eV. Addition of the cadmium layer on the inner walls of

the biological shielding suppresses this thermal energy peak. In all cases, a small peak

can be seen close to the highest neutron energies. These neutrons come from the

deuteron disintegration.

Absorptions on the resonances in 238

U are also visible in the Figure 63. First

depression on the low energy part of the neutron spectrum corresponds with the first

important resonance in 238

U(n,)239

U reaction at 6.67 eV (is visible directly from the

Figure 63 and Figure 64 comparison).

Several conclusions can be drawn from Figure 63. First of all, most high energy

neutrons are produced in the lead target and they are not notably moderated by the

target/blanket setup. Support structures have no influence on this part of the spectrum,

what is positive for the spallation spectrum studies. Addition of natural uranium causes

addition of neutrons with energies lower than 10 MeV, but this addition is not a

fundamental one. Biological shielding is fully responsible for the thermal, epithermal

and resonance neutrons, but it is not changing number and spectrum of neutrons with

energy higher than 8 MeV (differences are smaller than calculation uncertainty, which

is below one percent at this energy region). Cadmium layer is an effective absorber of

neutrons below 0.5 eV.

I have made the same flux calculations also for protons and deuterons to see the

production of these particles inside the target. Results can be seen in the Figure 136 and

Figure 137 in Appendix I Section 1. Deuterons are in the target mainly slowed down

and dismissed due to spallation (high energy peak), small amount of low energy

deuterons is produced in the spallation reaction (low energy part of the spectrum in

Figure 136 with four orders of magnitude lower intensity). Protons come from the

deuteron disintegration (high energy peak in Figure 137) and from spallation reaction

(low energy peak with three times lower intensity). No differences were observed in the

proton and deuteron spectra within the simulation uncertainties, when various parts of

the E+T setup were removed.

6.5. Calculation of the yields in used activation foils Due to the bad knowledge of experimental cross-sections of used reactions, our

experimental evaluation ended always at the yields of isotopes. To get the same value

from the simulation can be more complicated than the calculation of neutron spectra but

is still possible with a good accuracy.

Non-threshold reactions can be calculated directly using f4+fm tally. For

threshold reactions the situation is more complicated because of the missing cross-

sections. Products of some (n,xn) reactions can be also calculated with f4+fm tally, but


90

the MCNPX handles with cross-sections not ideally. It uses libraries up to their highest

energy, than when it has no model, it takes the last value in library and use it for the

convolution with the rest of the neutron spectrum. In reality, (n,xn) cross-sections

decrease slightly after their peak (see figures in Appendix J), so this approach is not

suitable. We solved this problem in the following way.

We add small volumes to the E+T model correspondent to the specific detector

positions during each irradiation and we calculate the neutron, proton, deuteron and

charged pion fluxes in these volumes using MCNPX. We calculate cross-sections of the

(n,xn), (p,pxn), (d,dxn), and (,xn) reactions in TALYS and MCNPX and we connect

them together. We make manual folding of the fluxes and cross-sections in Excel,

according to the following equation (6.1):

beamE

ddpipippnn

ur

Yield dEEEEEEEEEmA

N0

)()()()()()()()(1

(6.1)

where Ar is the specific atomic mass of a chemical element from which the foil was

made and mu is the unified atomic mass unit. Final outputs from the simulation part are

directly the yields of isotopes. Contributions of various particles to the total isotope

production in gold during 2.52 GeV deuteron experiment are displayed in the following

Table 13 (result of MCNPX spectra simulation and manual folding). Most important is

the contribution of neutrons, protons can create also a substantial part of the yield.

Contribution of deuterons and pions is under the level of neutron spectra uncertainty

and could be thus negligible. Nevertheless deuterons and charged pions are always

included.

Table 13: Contribution of various particles to the total yield, result of MCNPX

simulation and manual folding. Positions in the first gap and behind the target, radial

distance 3 cm and 10.7 cm, 2.52 GeV deuteron experiment.

first gap of the setup

196Au

194Au

192Au

3 cm 10.7 cm 3 cm 10.7 cm 3 cm 10.7 cm

neutrons 98.8% 99.7% 94.6% 98.7% 92.8% 98.2%

protons 1.1% 0.26% 5.06% 1.14% 6.63% 1.53%

deuterons 0.03% 0.05% 0.07% 0.08% 0.11% 0.07%

charged pions 0.08% 0.02% 0.24% 0.08% 0.45% 0.16%

behind the setup

196Au

194Au

192Au

3 cm 10.7 cm 3 cm 10.7 cm 3 cm 10.7 cm

neutrons 97.9% 99.2% 92.7% 97.3% 91.3% 96.6%

protons 1.96% 0.70% 6.99% 2.51% 8.14% 3.05%

deuterons 0.06% 0.02% 0.15% 0.06% 0.28% 0.12%

charged pions 0.08% 0.05% 0.18% 0.12% 0.31% 0.21%

6.5. Calculation of the yields in used activation foils

91

Manual folding of simulated spectra and cross-sections is a time consuming

procedure, but it gives better results and a contribution of various types of particles to

the total yield can be easily controlled. Dependence of the yield on neutron spectrum

changes (or cross-section changes) can be also directly studied. Examples of the

experiment to simulation ratios for 2.52 GeV deuteron experiment are in following

Figure 65 and Figure 66. More experiment/simulation ratios are in the Appendix I.

Uncertainty bars contain only statistical uncertainty from the DEIMOS32 and MCNPX,

because the main purpose of this comparison is to see the relative differences between

various isotopes and different measurement points (some uncertainties are the same for

all points – e.g. beam intensity uncertainty, and their involvement would be misleading

in this case).

If there would be an interest to compare absolute values of the exp/sim ratios to

the one, other uncertainties must be also involved. Beside the statistical uncertainty

from the DEIMOS32, three percent uncertainty from the HPGe detector calibration and

spectroscopic corrections must be included in the experimental yield uncertainty, the

same way as the additional uncertainty (at least ten percent) from the beam intensity

determination. Uncertainties are believed to be independent and thus they should be

summarized according to the equation ...2

3

2

2

2

1 yyyXX , where X is the

final experimental yield and ya is partial relative uncertainty (can be calculated as

1

11

x

xy

).

0.0

0.5

1.0

1.5

2.0

2.5

-5 5 15 25 35 45

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 192Au 24Na

Figure 65: Ratio between experiment and simulation in longitudinal direction for 2.52

GeV deuteron experiment, Au and Al samples at 3 cm from the target axis.


92

0.0

0.5

1.0

1.5

2.0

2.5

2 4 6 8 10 12

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 192Au 24Na

Figure 66: Ratio between experiment and simulation in radial direction for 2.52 GeV

deuteron experiment, Au and Al samples in the first gap.

Absolute values of the experiment/simulation ratio are strongly dependant on the

beam intensity determination. From the multiplicity calculation (Figure 60) can be seen,

that the beam intensity determination is probably not too correct in the case of deuteron

experiments. However, also in proton experiments the experimental neutron multiplicity

was slightly higher than the simulated one. Beam overestimation confirms also average

value of the exp/sim ratios, which is higher than one, especially in the case of 1.6 GeV

experiment (Figure 138 and Figure 139 in Appendix I, Section 2).

There is a clearly visible trend in the 198

Au exp/sim ratios in all three deuteron

experiments. In Figure 67 there are exp/sim ratios for the 198

Au yields on foils placed in

the first gap at distance 3, 6, 8.5, and 10.7 cm (1-4), the same in the second gap (5-8)

etc. I have observed the same behavior at 182

Ta, product of non-threshold (n,) reaction

in 181

Ta. The MCNPX simulation over-predicts number of epithermal and resonance

neutrons inside the setup, with rising distance from the axis the ratio is decreasing.

I have performed a few simulations with different uranium enrichment and density in

order to clear up this effect, but without a satisfactory result. No such a behavior was

observed at threshold reactions.

6.5. Calculation of the yields in used activation foils

93

0.0

0.5

1.0

1.5

2.0

2.5

0 5 10 15 20

Exp. yie

ld / s

im. yie

ld [

-]

Number of the foil [-]

198Au 1.6 GeV 198Au 2.52 GeV 198Au 4 GeV d

Figure 67: Ratio between experiment and simulation for all three deuteron experiments

and 198

Au isotope.

6.6. Normalized experiment/simulation ratios To see clearly the shape of the exp/sim ratio, I normalized the values to the first

foil in radial distance, respectively to the second foil in longitudinal distance (foils with

maximal yields). This normalization cancels out also the influence of the absolute value

of the cross-sections and of some correction uncertainties that are the same for each

isotope (possible differences in the shape of the cross-section in MCNPX and reality are

preserved). Only DEIMOS32 uncertainties are involved in these comparisons.

Most of the normalized exp/sim ratios are close to the one (see Figure 68 and

Figure 69, more figures can be found in Appendix I, Section 3). Discrepancies can have

multiple sources; starting from beam position and shape during whole irradiation

(uncertainty is hard to assess), ongoing with the cross-section shapes (can lead up to ten

percent uncertainty) and closing with discrepancies coming from the foil placement in

the experiment (imprecision of 5 mm can change the yield up to 20 percent – proven by

M. Majerle, see his PhD [41]). Exp/sim ratio is after including all of these uncertainties

equal to one (within the uncertainty bars).

No serious disagreements in the exp/sim ratios were found, so the INCL4/ABLA

models seem to be generally precise in the case of deuteron beams. This can be

confirmed also by the comparison between the figures with experimental yields, where

a maximum both in longitudinal and radial direction can be seen, and in the figures of

exp/sim ratios, where these maxima are missing (the simulation describes well the shape

of yield curves).


94

0.5

0.75

1

1.25

1.5

1.75

-5 5 15 25 35 45

Exp. y

ield

/ s

im. yie

ld [

-]


198Au 196Au 194Au 192Au 24Na

Figure 68: Ratio between experiment and simulation in longitudinal direction for

2.52 GeV deuteron experiment, Au and Al samples at 3 cm from the target axis. Ratios

are normalized to the second foil.

0.5

0.75

1

1.25

1.5

1.75

2 4 6 8 10 12

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 192Au 24Na


deuteron experiment, Au and Al samples in the first gap. Ratios are normalized to the

first foil.

6.7. Yields for different beam particles of the same total energy

95

6.7. Yields for different beam particles of the same total energy

I tried to compare yields of Au isotopes for different beam particles of the same

total energy. I used deuteron, proton, and proton plus neutron (50:50, 1.26 GeV) beam

of 2.52 GeV. I calculated neutron, proton, charged pion and deuteron spectra in the foil

volume and made a folding with calculated cross-sections. Yields were calculated at

3 cm over the target axis in longitudinal direction and in the first gap of the setup in

radial direction (places with highest neutron flux and thus also with highest yields).

Examples of the results of beam particle comparison are in the following Figure 70 and

Figure 71.

Deuteron beam is the most efficient for neutron production. At same total energy

it has lower ionization loses in the target than the proton beam, and so more energy can

be used for spallation. In comparison with hypothetic mixed beam of protons and

neutrons of the same total energy, deuterons generate slightly more neutrons (but still

within calculation uncertainty). Difference between the deuteron and mixed beam is

most probably caused by the difference in the MCNPX calculation of protons, neutrons

and deuterons (description of their behavior in the model).

0

0.002

0.004

0.006

0.008

0.01

0.012

0.014

0.016

-5 5 15 25 35 45

Sim

ula

ted

yie

ld [1

/g*

beam

part

icle

]


196Au

p+n 1260 MeV

d 2520 MeV

p 2520 MeV

Figure 70: Comparison of simulated longitudinal 196

Au yields for various beams of the

same total energy, samples placed at 3 cm from the target axis.


96

0

0.002

0.004

0.006

0.008

0.01

0.012

0.014

0.016

2 4 6 8 10 12

Sim

ula

ted y

ield

[1/g

*beam

part

icle

]


196Au

p+n 1260 MeV

d 2520 MeV

p 2520 MeV

Figure 71: Comparison of simulated radial 196

Au yields for various beams of the same

total energy, samples placed in the first gap of the setup.

6.8. Summary of the MCNPX simulations By summarizing MCNPX results from previous proton experiments, we

observed an increasing difference in the radial direction between experiment and

simulation for proton energies higher than 1.5 GeV, see Figure 72. For deuteron

experiments there is a good agreement for all three measured energies (from 1.6 GeV up

to 4 GeV), see Figure 73. This result prefers the hypothesis that in proton experiments

the problem is rather in the experimental part than in the simulations. 1.5 GeV and

2 GeV proton experiments were first experiments on the E+T setup. At that time the

influence of a lot of aspects was unknown (importance of proper beam position, foil

placement etc.). When the proton beams will be again available on the Nuclotron, we

will propose to perform an experiment at the beam energy equal or higher than 1.5 GeV

to confirm this conclusion.

6.8. Summary of the MCNPX simulations

97

0.0

0.5

1.0

1.5

2.0

2.5

2 4 6 8 10 12 14

exp. yie

ld /

sim

. yie

ld[-

]


2.0 GeV 1.5 GeV 1.0 GeV 0.7 GeV

194Au

Figure 72: Ratio between experiment and simulation for different proton beam energies

and 194

Au (overtaken from A. Krása [44]). Samples were placed in radial direction in

the first gap of the setup.

0.0

0.5

1.0

1.5

2.0

2.5

2 4 6 8 10 12

Ex

p. y

ield

/ s

im.

yie

ld [

-]


1.6 GeV 2.52 GeV 4 GeV

194Au

Figure 73: Ratio between experiment and simulation for different deuteron beam

energies and 194

Au. Samples were placed in radial direction in the first gap of the setup.


98

99

Chapter 7

Cross-section measurements of the (n,xn) threshold

reactions

My motivation for the cross-section measurements comes from the "Energy plus

Transmutation" project discussed in the previous chapters. Au, Al, Bi, Co, In, Ta, and Y

foils were used as activation neutron detectors, but unfortunately almost no

experimental cross-section data for most of the observed threshold (n,xn), (n,p), and

(n,) reactions are available for higher neutron energies.

7.1. State-of-the-art of the neutron cross-section libraries

The present status of knowledge of cross-sections for the (n,xn) reactions is

poor. Figure 74 shows measured (from EXFOR [66]) and evaluated (from ENDF [85])

cross-sections for (n,xn) reactions in Au and Bi.

0.0

0.5

1.0

1.5

2.0

2.5

3.0

0 10 20 30 40

Cro

ss-s

ecti

on [

bar

n]


197Au(n,2n)196Au

EXFOR

ENDF

0.0

0.5

1.0

1.5

2.0

0 10 20 30 40

Cro

ss-s

ecti

on [

barn

]


197Au(n,4n)194Au

EXFOR

ENDF

0.0

0.5

1.0

1.5

2.0

0 50 100 150

Cro

ss-s

ecti

on [

barn

]


209Bi(n,xn)

(n,4n)206Bi(n,5n)205Bi

0.01

0.1

1

10

0 25 50 75 100 125 150

Cro

ss-s

ecti

on [

barn

]


209Bi(n,xn)

(n,6n)204Bi (n,7n)203Bi

(n,8n)202Bi (n,9n)201Bi

(n,10n)200Bi (n,11n)199Bi

Figure 74: Neutron cross-sections for the Au and Bi (n,xn) threshold reactions. Data are

taken from the EXFOR [66] and ENDF [85].

In the case of gold, only (n,2n) reaction was measured in detail and by more

authors (Figure 74 – left up), but only up to less than 40 MeV. (n,4n) reaction on natural

Au was measured also only up to 40 MeV (Figure 74 - right up). Higher (n,xn) reactions

on Au have not been studied yet.

7. CROSS-SECTION MEASUREMENTS OF THE (N,XN) REACTIONS

100

In the case of bismuth, reactions from (n,4n) up to (n,12n) were already

measured (Figure 74 - down), highest neutron energy is 150 MeV. Unfortunately, all

these values are from one experiment only [86], so these values should be

independently verified. There are also huge distances between separate energies, so the

cross-section peak is not well described. There are no evaluated data available so far.

The situation for Al, Co, In, Ta, and Y is similar to Au. Low threshold reactions

(n,2n and 3n) were studied in detail up to 30 MeV, but no experimental data exist for

higher energies or (n,xn) reactions. More graphs with the data from EXFOR for various

reactions are further in the text in the section with cross-section results and in

Appendix J. One can there easily make his opinion on the situation in cross-section

libraries of (n,xn) reactions. It is really necessary to perform new cross-section

measurements to fill in the gaps in the libraries and estimate possible systematic errors

in already measured values. Not only for the high energy neutron measurements by the

means of activation foils, but also for the authors of the codes handling with cross-

sections and last but not least also for the designers of new spallation devices like ESS

[87] etc.

For the (n,xn) cross-section measurements we decided to use the same method as

we are familiar with from the Dubna activation measurements – neutron activation and

gamma spectra measurement. Usage of activation analysis brought us a lot of

difficulties, which we had to solve and fight with (e.g. background subtraction). On the

other hand, we had a good knowledge on working procedure and various spectroscopic

corrections.

It has to be mentioned, that the cross-sections of the threshold reactions can be

measured also by other methods, e.g. by the time of flight method for the neutron beam

and by on-line and X-Ray measurements of the samples. But, these methods require

more complicated equipment and longer time for preparation at the irradiation place,

which were both unavailable for us. One of this type of cross-section measurement is

described in the first chapter.

7.2. Limitations on neutron source First difficulty was a selection of proper neutron source. Spallation neutron

sources in Dubna mentioned in Chapter 2 are white neutron sources with unknown

neutron spectrum (neutron spectrum was up to now only calculated). These sources

cannot be used for this type of cross-section measurements, see Figure 75. In the world

there is a lot of quasi-monoenergetic neutron sources with more or less known spectrum

([88], [89], [90]), but only a few of them have sufficiently high beam intensity for

activation measurements ((n,xn) cross-section are in order of ~1 barn or lower). Most of

the neutron sources are also limited with the maximal neutron energy they can deliver,

usually 30 - 40 MeV (this is the reason for quite a good cross-section data in libraries

for lower energies, but no data for higher energies).

Other limitations were presence of spectroscopic laboratory – we needed at least

one detector with good resolution and efficiency for two weeks of continuous

measurement. Irradiation place had to be easily accessible for quick manipulation with

7.2. Limitations on neutron source

101

the samples, a low radiation around the irradiation place was also important (shortest

half-lives are in order of few minutes, so immediate access to the irradiation place was

needed). Last but not least was the question of experiment funding; we needed to find

money on transport, accommodation, diets for three people, beam-time and additional

experimental costs (liquid nitrogen for cooling the detector etc.).

Neu

tro

n f

lux

den

sity

[1

/(cm

2.s

)]


spallation source at JINR

quasi-monoenergetic source at TSL

102

104

108

106

0

10-7 10-310-5 10-1 101 103

Figure 75: Comparison of the spallation neutron spectrum in Dubna and quasi-

monoenergetic neutron spectrum in TSL.

7.3. EFNUDAT project We decided to use the EFNUDAT project (European Facilities for Nuclear Data

Measurements) to get access to one of the supported facilities – The Svedberg

laboratory of the Uppsala University, Sweden. The EFNUDAT project is an Integrated

Infrastructure Initiative (I3) funded under the 6th framework program (FP6) of the

European Commission. The main objective of EFNUDAT is to promote the coherent

use and integration of infrastructure related services via networking, transnational

access to the participating facilities for nuclear data measurements and joint research

activities [91].

Figure 76: Logo of the EFNUDAT project [91].

http://www.efnudat.eu/objective.html

http://www.efnudat.eu/network.html

http://www.efnudat.eu/access.html

http://www.efnudat.eu/access.html

http://www.efnudat.eu/facilities.html

http://www.efnudat.eu/joint.html

http://www.efnudat.eu/joint.html


102

Figure 77: Countries and institutes involved in EFNUDAT [91].

In 2007 we started discussions with The Svedberg laboratory about

the possibilities of the (n,xn) cross-section measurements on their quasi-monoenergetic

neutron source. I have prepared with my colleague A. Krása a proposal for

the experiment, which was accepted in October 2007. In June 2008 we have performed

three irradiations with neutron energies 22, 47, and 94 MeV, details are discussed

in following text. With the preliminary, but successful results we decided to exploit

the EFNUDAT once again to fill in the gap between 47 and 94 MeV. I have prepared

new proposal for further six energies, which was accepted in September 2009 and

the irradiation took place in February 2010.

7.4. Quasi-monoenergetic neutron source at The Svedberg laboratory Main experimental equipment of The Svedberg laboratory (TSL) is a Gustav

Werner cyclotron, which can deliver beams with the energies up to 180 MeV for

protons or 45 MeV per nucleon for heavier ions up to Xe. The main activity of TSL is

based on an agreement between Uppsala Academic Hospital and Uppsala University on

proton therapy. Tens of patients are routinely irradiated every week. Beamtime not used

for proton therapy is devoted to commercial neutron and proton irradiation projects,

mainly tests of radiation endurance of the electronics. The beam can be for this purposes

collimated to a very small shielded “pencil”, which can irradiate separate microchips on

the printed circuits. But, there is still some time for basic (academic) research, but one

must apply for long time in advance.

7.4. Quasi-monoenergetic neutron source at The Svedberg Laboratory

103

Figure 78: Photo of the Gustav Werner cyclotron (author‟s photo).

In this laboratory quasi-monoenergetic 11 - 175 MeV neutron source based on

the 7Li(p,n)

7Be reaction was developed [92]. High energy protons from the cyclotron at

TSL are directed to a thin, lithium target, neutron flux density can be up to 5.105 cm

-2s

-1

at standard user position (373 cm from the target). Neutron flux density is limited only

with available heat removal from the target. The half of intensity is in the peak with

FWHM = 1 MeV (corresponds to the ground state and first excited state at 0.43 MeV in 7Be) and half of intensity is in a continuum in lower energies (corresponds to higher

excited states, multiple-particle emission etc.). Proton energy loss in the target amounts

to 2-6 MeV depending on the incident beam energy and target thickness. Downstream

the target, the proton beam is deflected by a magnet and guided into a graphite beam

dump. The whole proton beam line, target, bending magnet and most active devices are

hidden in concrete corridor, so the hall is accessible immediately after the shutdown of

the beam.

The neutron beam is formed by an iron collimator (50 cm in diameter and

100 cm long) with a hole of variable size and shape. Behind the collimator there is a

large cave (so called Blue hall) with the neutron beam dump at the end, more than

15 meters of free space are ready for the users. Multiple system of laser surveying can

be used for exact sample allocation.

Beam can be handled directly by the users via a User control interface. After the

operators set up the beam and make intensity and calibration checks, they give the beam

control to the user. User can then remotely switch off or on the beam without any

contact to the accelerator operators. One can also open the Blue hall to restricted or free

access mode for manipulations. This appeared to be a very useful procedure, which we

used for short interruptions during the irradiation and taking out some of the samples.


104

Figure 79: Blue hall with the quasi-monoenergetic target and shielding [92].

Figure 80: User control interface for beam handling in TSL.

7.5. Cross-section estimation and planning of the experiment

105

7.5. Cross-section estimation and planning of the experiment

During planning of the irradiation it was necessary to have at least some

knowledge about the possible cross-section course and values. I have used the

knowledge about the reaction thresholds calculated for the E+T experiment – see

Chapter 3. For calculation of cross-section courses I have also used the TALYS 1.0

code [82].

For most of the isotopes it was possible to make a convolution of calculated

cross-sections and neutron spectra at irradiation points. I have roughly calculated yields

of the isotopes and with the knowledge about the detector efficiency I have planned the

weights and dimensions of the foils in order to get enough activated nuclei. Then I

could also calculate when and how long we had to measure the sample in order to catch

enough counts in the detector of the observed isotope (the activity of the foils was very

low, a few hours of measurements were necessary for each foil).

Table 14: Example of the number of predicted counts in the strongest line of gold

isotopes. I calculated the numbers for 89 MeV neutron beam in Uppsala, detector

position p2, weight of the foil 1.2 g.

Measurement time after

the beam end Number of counts in the strongest line of the isotope [-]

from [min] to[min] 196

Au 194

Au 193

Au 192

Au 191

Au 190

Au 189

Au 188

Au 187

Au

3 23 19 55 23 200 34 222 134 30 0

23 45 21 61 25 209 35 174 89 7 0

45 165 115 323 128 971 149 348 119 1 0

165 400 222 600 224 1267 156 57 7 0 0

400 700 277 706 240 872 77 1 0 0 0

700 1000 271 645 198 432 26 0 0 0 0

1020 1260 212 472 131 174 7 0 0 0 0

1260 1440 156 332 85 80 2 0 0 0 0

7.6. Neutron beams at TSL For every irradiation we received from the TSL staff report on the irradiation,

where all necessary data were summarized. To the report belonged also the file with the

course of irradiation (it contained the beam intensity during each burst). With this I

could calculate the correction on irradiation, see further.

I prepared samples and was present at all irradiations and gamma measurements.

I have completely analysed results from the first three irradiations. Data from the

second campaign in TSL from February 2010 will be the main subject of the PhD work

of J. Vrzalová, but I have already analysed a few parts of it and I act as a consultant of

Vrzalová‟s work.


106

Table 15: Neutron beam parameters at TSL Uppsala for used energies.

June 2008 February 2010

Proton beam energy

[MeV]

24.68

± 0.04

49.5

± 0.2

97.9

± 0.3

61.8

± 0.2

69.1

± 0.2

75.4

± 0.2

95.5

± 0.3

Li-target thickness26

[mm] 2 4 8.5 4 4 4 8.5

Proton beam current [A] 10 10 5 7.5 10 10 10

Average energy of peak

neutrons [MeV] 21.8 46.5 94.7 59 66.4 72.8 89.3

Fraction of neutrons in the

peak [%] 50 39 41 38 39 40 39

Peak neutron flux density

[105 cm

-2 s

-1]

0.5 1.3 1.4 1.0 1.8 2.2 2.7

Total peak neutron flux

[109 cm

-2]

1.52 3.74 4.15 2.98 5.32 6.37 7.69

7.7. Quasi-monoenergetic neutron source at Nuclear Physics Institute Second neutron source that we used is in the Nuclear Physics Institute (NPI) of

the Academy of Sciences of the Czech Republic in Řež. Protons from the isochronous

cyclotron U120-M are directed to the 7Li target and quasi-monoenergetic neutrons in

the range 20 – 37 MeV can be produced [93].

Figure 81: Isochronous cyclotron U-120M in NPI Řež (left - own photo, right photo

from [94]).

26

target thickness is connected with the FWHM of the high energy neutron peak. For used thicknesses of

the Li target, ~ 98% of the proton beam passed without producing a neutron, protons only lost energy

[95]. Thermal charge on the target is the main limiting factor for the neutron intensity (at TSL it is solved

by defocusation of the proton beam in front of the target and thus by hitting large area).

7.7. Quasi-monoenergetic neutron source at Nuclear Physics Institute

107

Cyclotron U120-M was designed and completed in JINR Dubna in 1972. In the

following years the cyclotron was gradually modernized, after the devastating floods in

2002 new systems of cooling, vacuum and power supplies were build.

This quasi-monoenergetic neutron source (placed at the point NG-2) is based on

the same reaction 7Li(p,n)

7Be like the TSL one, but the construction layout of the target

is completely different. Behind the foil with enriched lithium there is no bending

magnet, but a graphite beam dump, which stops the rest of the beam. Behind this is a

holder with the samples, so no collimators or shielding are applied. Whole setup

of target and graphite stopper is cooled by alcohol to 5 degrees of Celsius, 600 Watts

of heat are reliably dispatched. Target and its cooling are not fixed, but are movable,

because they possess the same beam-line like the targets for the production

of radiofarmacs27

.

Table 16: Neutron beam parameters at NPI Řež for used energies.

I prepared and was present at all four irradiations at NPI Řež. I have analyzed

first two experiments completely, the second two experiments were a subject of the

Diploma thesis of J. Vrzalová [96]. I was a consultant of this work and I helped

J. Vrzalová to understand all experimental details of these cross-section measurements.

This Diploma thesis was successfully defended in June 2010.

I have also tested possible attenuation of the neutron beam in the foils. In NPI

we have used spare positions behind the samples of P. Bém, so there were some thin

foils in front of us (usually 50 m thick). Neutron beam was partially collimated by the

holders to approximately 40 mm, so I could not place all our foils side-by-side. I used 4

to 6 holders and sticked few foils upon itself. The result was that there were multiple

foils in common beam. At studied neutron energies (17-34 MeV) cross-sections are

around one barn or smaller, so the attenuation should be negligibly small.

27

This quasi-monoenergetic source could be operated only during weekends or special occasions up to

now, because the beam-line is occupied most of the time with the radiofarmacs.

Proton beam energy [MeV] 19.838 25.126 32.5 37.4

Start of irradiation 8.8.2008

13:22

17.5.2008

15:26

17.4.2009

13:34

29.5.2009

14:47

End of irradiation 9.8.2008

9:17

18.5.2008

8:02

18.4.2009

10:00

30.5.2009

11:00

Time of irradiation 19h 55min 16h 36min 20h 26min 20h 13min

Average energy of peak

neutrons [MeV] 17.5 21.88 30.375 35.875

Total peak neutron flux

[1012

cm-2

] 2.31 2.95 4.38 4.25


108

Figure 82: Quasi-monoenergetic source in NPI Řež based on the design of Uwamino

[97]; scheme (left) [93] and a real outlook (right).

To assess this I made a simple MCNPX simulation. I put all foils in one row, set

maximal used thickness (the worst case that never happened in reality) and added

double paper wrap, for illustration see Figure 83. I put a pencil beam from one side of

this packet and calculated number of neutrons in the cells between the foils. Cells had

the same dimensions like the foils, but bigger thickness (1 cm). I also used 30 energy

bins for each cell to see, how the neutrons are decelerated.

Figure 83: The sequence of the foils in the MCNPX simulation of neutron beam

attenuation. First two Au-Cu sets are samples of P. Bém, rest are ours.

Attenuation of the neutron beam in simulation was for most of the foils

negligible, difference between the total number of neutrons in front of the first foil and

behind the last one was 4 %. More serious problem was the energy spread of the

originally monoenergetic beam, number of the neutrons in the energetic group 29 –

30 MeV decreased to 85 % of the original value. The simulation was done for the worst

case, in real measurement some foils were side by side, had smaller thickness or were

left out, so the total amount of mass in the beam was much lower. I have not involved

these results into the cross-section data from Řež, as I think this problem needs to be

further studied. It will be one of the topics of PhD thesis of J. Vrzalová.

Beam line

Samples

Graphite

stopper

Li-target

7.8. Studied materials

109

7.8. Studied materials

In all irradiations I studied Au, Al, Bi, In, and Ta materials, the same we use in

the Energy plus Transmutation experiments for high energy neutron measurements.

Other group from the E&T RAW collaboration studies transmutation of radioactive and

stable iodine in the field of spallation neutrons, so we involved tablets of natural iodine

to our cross-section studies. In the second irradiation campaign at TSL Uppsala we

measured samples of Y for the Polish E&T group. Neutron source at NPI is due to

closer distance between target and samples (10-15 cm) much more intensive (2 orders

of magnitude), so the samples were after the irradiation more active. Higher activity

shortened time of measurement on the detector and we could study more materials. We

decided to test beside the above mentioned also the foils from Zn, Mg, Fe, Cu, and Ni,

practically all suitable materials for (n,xn) measurements of high energy neutrons.

Materials were except the iodine in form of foils with dimensions of

20x20x0.05-1 mm3, weights of the foils varied from 0.2 up to 7 grams depending on the

foil type and beam energy. Foils were wrapped in two layers of paper; outer coating was

removed before gamma measurements. Iodine samples were in the form of solid KIO4

tablet. These tablets were manufactured on a pressing machine in NPI and packed

hermetically in plastic coating, its weight was between one and three grams and

dimension of the pills were 15x3 mm3.

7.9. Evaluation procedure Typical irradiation time was 8 hours at TSL Uppsala, respectively 15 hours at

NPI Řež. Transport from the irradiation hall to the spectrometer took approximately two

minutes in Uppsala, ten minutes in Řež. Principles of measurement of irradiated foils, -

spectra processing in DEIMOS32 and evaluation of the yields was the same as for the

Energy plus Transmutation experiments. I have calculated all necessary spectroscopic

corrections and I have included the important ones in the data (eg. beam instability

correction was negligible for TSL measurements due to high stability of the beam).

Theoretical background of the corrections was the same as described in E+T evaluation

section, only the numbers differed. Final yield of studied isotopes was calculated

according to the equation (3.26). I have used following equation (7.1) for determination

of reaction cross-sections .

An

yield

NN

ASN

(7.1)

where:

Nyield – yield of studied isotope

S – area of the foil

A – molar weight

Nn – number of neutrons in the peak

NA – Avogadro number


110

7.10. Background subtraction

Every source of high energy neutrons is more or less quasi-monoenergetic and

neutron spectrum contains beside the main neutron peak also lower continuum

stretching up to the thermal energies. This spectrum is different at every irradiating

facility because of different construction of the target and surrounding equipment, and

also because of the method of spectrum determination (experiment / experiment+

calculation / calculation). Neutron spectra for TSL are in Figure 84, for NPI in Figure

85.

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

0 10 20 30 40 50 60 70 80 90 100

Neu

tro

n f

lux

[1

/MeV

(p

eak

are

a=

1)]


24.7 MeV p-beam, 2 mm Li-target 49.5 MeV p-beam, 4 mm Li-target

61.8 MeV p-beam, 4 mm Li-target 69.1 MeV p-beam, 4 mm Li-target

75.4 MeV p-beam, 4 mm Li-target 92.5 MeV p-beam, 8.5 mm Li-target

97.6 MeV p-beam, 8 mm Li-target

Figure 84: Quasi-monoenergetic neutron spectrum from 7Li(p,n)

7Be at the TSL. Data

have been overtaken from the facility staff – A. Prokofiev.

Proper measurement of the high energy neutron spectrum (e.g. by the means of

the time-of-flight method) is not possible at all accelerators because of the beam

structure, small space, electromagnetic disturbance, etc. In TSL, the conditions for

neutron spectrum measurement were good and the neutron spectrum is nowadays

known with the uncertainty below 10% (from personal discussion with A. Prokofiev,

TSL). In NPI, neutron spectrum from the quasi-monoenergetic source was never exactly

measured because of long beam pulse and insufficient space in the cyclotron crypt. The

source was manufactured according to the source designed and operated in Japan by Y.

Uwamino, so the neutron spectrum is believed to be the same or very similar. More

about the neutron spectra can be found in [97].

Neutron spectrum at NPI is more complicated compared to TSL because of the

carbon beam stopper. Reaction nat

C(p,xn)X is not negligible in low energy region, see

Figure 86.


111

0 5 10 15 20 25 30 35 40

Nu

mb

er

of

neu

tro

ns

[1/s

r.M

eV

.C]


20 MeV 25 MeV 30 MeV 35 MeV 40 MeV

0

2·1014

6·1014

1·1015

1.4·1015

4·1014

8·1014

1.2·1015


7Be at cyclotron Řež –

data overtaken from the facility staff – M. Honusek.

Figure 86: Neutron spectrum produced in reaction with 7Li target and

natC beam stopper

in the case of NPI target station, overtaken from M. Honusek [98].

Because of the large amount of background neutrons, production of the isotope

by these neutrons was not negligible for most of the isotopes. Only reactions with the

threshold few MeV lower than the neutron peak could be used to direct cross-section

evaluation (Figure 87 – left). Number of these isotopes is not high, usually one or none

per one beam energy and material. Originally it was planned not to evaluate other


Neu

tro

n f

lux

[n

/MeV

/sr/

C]


112

isotopes than these backgroundless. I have developed a procedure how to subtract the

background in the case like in Figure 87 – right.

0 10 20 30 40 50Neutron energy [MeV]

neutron spectrum

simulated cross-

section

0 10 20 30 40 50

Arb

itra

ry u

nit

s [-

]Neutron energy [MeV]

neutron spectrum

simulated cross-

section

Figure 87: Example of folding of the quasi-monoenergetic neutron spectrum and

simulated cross-section.

I used TALYS to calculate cross-section of every reaction in the same energy

bins like is in the neutron spectrum in TSL and NPI. Then, I made a folding of the

neutron spectra and TALYS cross-section. I calculated isotope production in neutron

peak and by the whole neutron spectrum. Finally I made a ratio of these two values; this

ratio stands for the relative production of the isotope in the peak. I multiplied

the experimental yield of the isotope by this number, what resulted in the subtraction

of the amount of isotope produced by background neutrons. Peak to whole spectrum

ratio varies from 10 to 100 percent.

This background subtraction procedure is a potential source of unknown

uncertainty. It is insensitive to the absolute value of the cross-section (I use the same

cross-section both in numerator and denominator), but a modification in the cross-

section shape or in the neutron spectrum shape can change it. Calculation of the cross-

section in TALYS is also a weak point of this procedure. TALYS enables for example

five basic settings of nuclear level densities. Cross-sections have slightly different shape

for each of it (see Figure 95), so there is a space for variations and changes in

background subtraction procedure. At the end of the year 2009 a new version of

TALYS appeared, concretely version 1.2. I calculated the cross-sections of Au in this

new version and got different results compared to those from TALYS 1.0, see e.g.

Figure 99 - Figure 100. So, there is again a place for changes in background subtraction.

However, most of the changes remain within 10 %. Direct uncertainty assessment of

calculated cross-section is not involved in the TALYS up to now, but there are signs it

will be possible in a new version. At ND2010 conference, one of the TALYS authors –

S. Hillaire – showed his current work – repeated calculations with automatically varied

inner TALYS parameters. He got some region, where most of the calculated cross-

section lies. This region can be connected with the uncertainty of calculated cross-

section. More details about the TALYS calculations of cross-sections are discussed in

following Chapter 8.


113

I studied also other possibilities for background subtraction. M. Honusek from

NPI uses routinely step-by-step method [99], [100]. He plans the irradiations so, that he

has every 2 – 3 MeV one measurement. He starts with the cross-section value close to

the threshold, which is not affected by the neutron background. With this cross-section

value he moves step-by-step to higher energies and subtracts the background. Compared

to our procedure this approach is safer in using real cross-sections, not calculated ones.

We started cross-section measurements with three energies - 22, 47, and 94 MeV – so

this was no usable for us. But in the future, when we will have better coverage of the

energy interval, it is planned to try also this process of neutron background subtraction.

At some quasi-monoenergetic neutron sources the neutron background is

independent within some angle, but the neutron peak disappears when moving from the

beam axis. Then it is possible to irradiate the same samples in the direct beam and under

certain angle from the beam axis and then subtract the yields [101]. In the case of TSL

this is not possible because of the 1m thick iron collimator. In NPI I tried to place Au

samples under the angle 30° and 60° from the beam axis during 32.5 MeV irradiation,

see Figure 88. Comparison of the neutron spectra under selected angles are in Figure 89

(overtaken from Y. Uwamino [97]). From this figure it can be seen that in the case of

NPI the neutron peak does not disappear completely and also that the background

changes a bit.

Figure 88: Placement of the Au and Al samples under the 30° and 60° from the beam

axis.

The results of this experiment (relative ratios of the production by background

neutrons) were too far from values I got from TALYS/spectra convolution and most

probably also from the reality. Results completely confirmed my presumption that this

background subtraction procedure is not usable for us. Reasons can be found already in

the neutron spectra shown in Figure 89 - they do not agree completely with the

statements presented in the work of S. Sekimoto [101]. Second reason can be in the

construction of NPI neutron source. Neutron spectra are overtaken from Y. Uwamino,

who measured them on a neutron source similar to the NPI one only within the beam

axis. Under non-zero angle there is much more material around the target in NPI than it

was in Y. Uwamino‟s case, see Figure 90. This leads to probably higher differences


114

between the real neutron spectra in non-zero angles at NPI and those presented in Y.

Uwamino‟s work.

Figure 89: Neutron spectra under 0° and 60° angle from the beam axis, overtaken from

Y. Uwamino [97].

30 degrees

60 degrees

Figure 90: Comparison between the neutron source construction of Y. Uwamino [97]

and at NPI Řež [93]. Used angles are drawn in the right part of the figure.

7.11. Uncertainty analysisMain uncertainties in my cross-section measurements come from the neutron

spectrum knowledge (10%), beam intensity (10%), gamma-detector calibration (3%),

and from the Gauss-fit of the gamma peaks in DEIMOS32 (at least 2%). At this

moment I consider that all these uncertainties are independent, so the final cross-section

7.11. Uncertainty analysis

115

uncertainty is a sum calculated according to the following equation:

...2

3

2

2

2

1 yyyXX , where X is final cross section value and ya is partial

relative uncertainty (can be calculated as 1

11

x

xy

or is given – e.g. beam intensity

uncertainty).

Background subtraction procedure is a source of up to now not clearly resolved

uncertainty, which has to be studied. It is not independent, because it uses the

knowledge of neutron spectrum. It varies according to the amount of subtracted

background yield (is different for every reaction and energy). Main uncertainty in the

background subtraction procedure comes from the TALYS; it could not be clearly

calculated up to now. There are also differences between various versions and basic

settings of the TALYS. Based on some TALYS calculations I assess the uncertainty of

background subtraction procedure to be within 10 %, for more details see chapter 7.

This uncertainty is not included in the data, because it will be most likely changed and

specified in future.

Yield Cross-section

Background subtraction

Neutron

spectrum

Neutron

spectrum

uncertainty

TALYS

TALYS

uncertainty TALYS

version

TALYS

setings

TALYS

uncertainty

Beam intensity

Intensity

measurement

Beam dump

measurement

TFBC

measurement

TFBC

measurement

uncertainty

uncertainty

uncertainty

Neutron

spectrum

Neutron

spectrum

uncertainty

Figure 91: Uncertainty structure in cross-section processing from the yield.


116

Total uncertainty is quite conservative, because all included partial uncertainties

are the highest possible. With further experiments our knowledge of uncertainties will

improve and the total uncertainty value will probably decrease.

To have a better imagination of the mutual relations between separate

uncertainties I made a diagram, sometimes called also fishbone. For processing of the

isotope yield, the diagram is the same as in Figure 30, except the beam intensity part.

Uncertainties involved in cross-section processing from the yield are displayed in

Figure 91. Red marked uncertainties were involved in the cross-section data. In the

Figure 92 there are plotted relative values of the uncertainties for comparison.

From this it is clear that the uncertainty situation is very complicated and should

be studied further to evaluate clearly all uncertainties. This, I think, should be one of the

main tasks for J. Vrzalová in her PhD thesis dealing with cross-section measurements.

0 5 10 15 20 25 30

beam intensity

neutron spectra

detector calibration

min Deimos

max Deimos

uncertainty [%]

Řež

Uppsala

Figure 92: Comparison of partial uncertainty values for cross-section measurements at

Řež and Uppsala.

7.12. Discussion of the cross-section results

I used well-known (E) for low threshold reactions to check if I got appropriate

results. I made a comparison between the data from EXFOR, TALYS and results from

the measurements from Řež and Uppsala (data for 30.375 and 35.875 MeV were

produced by J. Vrzalová). Examples of the results can be seen in following two graphs

Figure 93 and Figure 94, more graphs and values are in the Appendix J and L. List of all

measured reactions is bellow.

7.12. Discussion of the cross-section results

117

0

0.5

1

1.5

2

2.5

3

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


197Au(n,2n)196Au

EXFOR

NPI experiments

TSL experiments

TALYS 1.0

Figure 93: Cross-section values of the 197

Au(n,2n)196

Au reaction, comparison among

EXFOR, TALYS 1.0 and my values. Last 10 EXFOR entries are [114] - [123].

0

0.03

0.06

0.09

0.12

0.15

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


EXFOR

NPI experiments

TSL experiments

TALYS 1.0

27Al(n,)24Na


Al(n,)24

Na reaction, comparison among

EXFOR, TALYS 1.0 and my values. Last 10 EXFOR entries are [114], [115], [117],

and [124] - [130].

For most of the isotopes I observe good agreement with TALYS and EXFOR.

For energies higher than 40 MeV and reactions higher than (n,4n) no data are available


118

in EXFOR (except bismuth). My cross-section data are in this sense unique and

I presented them on national conferences (16. konference českých a slovenských fyziků

[103]) and international conferences (Baldin conference [104], NEMEA-5 [105],

ND2010 [106], EFNUDAT meetings [107], [108], AER meetings…) with positive

response. But, for some reactions the cross-sections are differing from the TALYS and

I have measured only one or two values, what is from my opinion not enough to say

what is wrong. Evaluation of the last experiment in Uppsala has unfortunately not been

finished yet, but I believe that new four data points in the region 50 – 100 MeV will

bring answers to many of these differences.

List of all studied reactions (with at least one measured cross-section value):

27Al(n,)

24Na

27Al(n,p)

27Mg

197Au(n,2n)

196Au

197Au(n,4n)

194Au

197Au(n,5n)

193Au

197Au(n,6n)

192Au

197Au(n,7n)

191Au

197Au(n,8n)

190Au

209Bi(n,3n)

207Bi

209Bi(n,4n)

206Bi

209Bi(n,5n)

205Bi

209Bi(n,6n)

204Bi

209Bi(n,7n)

203Bi

209Bi(n,8n)

202Bi

209Bi(n,10n)

200Bi

181Ta(n,2n)

180Ta

181Ta(n,4n)

178mTa

181Ta(n,5n)

177Ta

181Ta(n,6n)

176Ta

natIn(n,xn)

114mIn

115In(n,2n)

114mIn

natIn(n,xn)

113mIn

natIn(n,xn)

112mIn

natIn(n,xn)

111In

natIn(n,xn)

110In

natIn(n,xn)

109In

natIn(n,xn)

108In

127I(n,2n)

126I

127I(n,4n)

124I

127I(n,7n)

121I

127I(n,8n)

120I

127I(n,9n)

119I

64Zn(n,2n)

63Zn

119

Chapter 8

TALYS

8.1. Introduction to TALYS TALYS is a nuclear reaction program created at NRG Petten, the Netherlands and CEA

Bruyères-le-Châtel, France [82]. Objective of the TALYS code is to provide a complete

and accurate simulation of nuclear reactions in the 1 keV-200 MeV energy range,

through an optimal combination of reliable nuclear models, flexibility and user-

friendliness. Incident particles can be neutrons, photons, protons, deuterons, tritons, 3He- and alpha-particles. Target nuclides are accepted of mass 12 and heavier.

The development of TALYS used to follow the “first completeness, then quality”

principle, in other words authors do not spend several years to the theoretical research

and absolutely perfect implementation of one particular reaction channel but aim to

enhance the quality of TALYS equally over the whole reaction range. TALYS falls in

the category of GNU General Public License software; it can be freely downloaded

from the web page http://www.talys.eu/, used, distributed and modified (within the

GNU license). On December 21, 2007 the first official version of the code, TALYS-1.0,

was released. Second (and up to now latest) version is TALYS 1.2, released on

December 22, 2009.

TALYS input file consists basically of four rows, where type of projectile (e.g.

n), target material (e.g. Au), nucleon number (197), and energy (100 (MeV)) have to be

defined. All other parameters are hidden in the code and preset to values that work for

most of the reactions and energies.

8.2. Comparison among various models Basic settings of TALYS can be modified by more than 250 key-words.

Practically all parameters can be changed within preset values (change of models,

libraries, procedures) or modified directly step by step by numbers.

My next logical step in the use of TALYS was to assess, how changes in

TALYS settings will influence calculated cross-section values and thus background

subtraction procedure and measured cross-section values. I resolved to change level

densities as an important ingredient for calculation of threshold reaction cross-sections.

There are 5 preset options of level densities in TALYS - 3 phenomenological level

density models and 2 options for microscopic level densities (page 180 and further in

[76]). One can switch among them using key-word “ldmodel” and number.

ldmodel 1: Constant temperature + Fermi gas model

ldmodel 2: Back-shifted Fermi gas model

ldmodel 3: Generalised superfluid model

8. TALYS

120

ldmodel 4: Microscopic level densities from Goriely's table

ldmodel 5: Microscopic level densities from Hilaire's table

These preset models work quite well for our heavy isotopes; differences among

various models are mostly within 20 % for energies up to ~ 30 MeV and decrease

quickly with rising energy (see Figure 95 and Figure 96). Big differences at the

beginning of the cross-section are caused by various threshold energy of the reaction in

each model and by steep increase of the cross-section. All models are in agreement with

experimental data from EXFOR.

0

0.5

1

1.5

2

2.5

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


ld1

ld2

ld3

ld4

ld5

196Au in TALYS 1.2

Figure 95: Cross-section of

197Au(n,2n)

196Au reaction calculated in TALYS 1.0 using

five different models (ld1 – Constant temperature + Fermi gas model, ld2 – back

shifted Fermi gas model, ld3 – generalized superfluid model, ld4 – microscopic level

densities from Goriely‟s table, ld5 – microscopic level densities from Hilaire‟s table).

At mid-weight isotopes calculations start to recede from experimental data in

EXFOR (I have observed it during cross-section calculations of Tc, Mo, and Nb).

Anyway there is a plan to change the level densities manually and try to find the values,

for which the calculation of cross-section will fit best to EXFOR data of my isotopes.

8.2. Comparison among various models

121

0.6

0.8

1

1.2

1.4

1.6

1.8

2

2.2

2.4

0 10 20 30 40 50 60 70 80 90 100

Lev

el d

en

sity

rati

o[-

]


ld1/ld2

ld1/ld3

ld1/ld4

ld1/ld5

Figure 96: Ratios among cross-sections calculated with different level density models in

TALYS 1.0 for 197

Au(n,2n)196

Au reaction.

0.75

0.8

0.85

0.9

0.95

1

1.05

1.1

196Au 194Au 193Au 192Au

Cro

ss-s

ecti

on r

ati

o[-

]

Isotope

ld1/ld2

ld1/ld3

ld1/ld4

ld1/ld5

ld1/TALYS 1.0 ld1

Neutron energy 47 MeV, TALYS 1.2

Figure 97: Ratios among cross-sections of various threshold reactions on gold for

neutron energy 47 MeV (like in TSL Uppsala).

I studied the same effect also in the new TALYS 1.2 version. Cross-section

ratios for different level density models changed; see Figure 97. Differences seem to be

8. TALYS

122

random and in the 10% range for most of the isotopes. Finally, I recalculated the

background subtraction for each model of level density in TALYS 1.2 and evaluated

experimentally measured cross-sections with these background values. Results are in

Figure 98. Final uncertainty caused by background subtraction was on account of these

studies estimated to 10 % and was added to total cross-section uncertainty. More

detailed studies of these effects are a subject of the PhD thesis of J. Vrzalová.

0.00

0.05

0.10

0.15

0.20

0.25

196Au 194Au 193Au 192Au 191Au 190Au 188Au

Cro

ss-s

ecti

on

[b

arn

]

Isotope

TALYS 1.2 - ld1

TALYS 1.2 - ld2

TALYS 1.2 - ld3

TALYS 1.2 - ld4

TALYS 1.2 - ld5

TALYS 1.0 - ld1

94 MeV - TSL data

Figure 98: Experimental cross-section of

197Au(n,xn) reactions measured at Uppsala for

energy 94 MeV.

During the work with TALYS 1.0 I have by chance discovered a serious error

in the code. Basic input file enables to calculate the cross-sections only at one energy

in one run. It is possible to create a file “energy” which can contain list of energies, for

which the TALYS should calculate when energy file is called in the input file. From

some reason number of the energies in this file is limited and was not sufficient for my

convolution purposes. I calculated the cross-sections with a simple script, which started

the simulation again and again and changed the energy in some preset steps. Number of

such steps is limited only by the available computing time. Results of these two

approaches should be the same – in both I only repeatedly start the calculation at some

energy. In my experience they differ, divergences are in the range of the changes

between different level density models or TALYS versions. At EFNUDAT meeting in

Paris (2010) I asked one of the TALYS authors S. Hilaire about the possible source of

these differences. He explained to me that there is some fixation of the TALYS inner

parameters when using the “energy” file, TALYS 1.0 looks at the highest energy and

preset the parameters. Then it runs from the lowest energy, but with already preset

parameters. In new TALYS 1.2 this problem is already fixed.

8.3. Comparison between TALYS 1.0 and TALYS 1.2

123

8.3. Comparison between TALYS 1.0 and TALYS 1.2 In December 2009, new version of TALYS code was released. New version of

the code contained changes on all levels of cross-section calculation, but no specific

change valid only for n,xn reactions was listed in the list of changes. I made cross-

section calculations for Au isotopes with the basic settings of the new version and made

a comparison with the older one. Differences between the two versions are small for

low threshold reactions (see Figure 99), with rising threshold energy the differences

start to be significant (Figure 100). I added to the graphs also the data from EXFOR and

from European Activation File (EAF) [102]. More figures with comparisons can be

found in Appendix K.

Clearly visible differences between the TALYS 1.0 and 1.2 represent no serious

problem, because at high energy threshold reactions (e.g 197

Au(n,8n)190

Au) background

subtraction is small and thus their influence on final cross-section value is also small,

see Figure 98.

0.0

0.5

1.0

1.5

2.0

2.5

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


EXFOR

Talys1.2

Talys 1.0

EAF

197Au(n,2n)196Au

Figure 99: Comparison of cross-section results for 197

Au(n,2n)196

Au in TALYS 1.0 and

TALYS 1.2 (both in basic setting). EXFOR data and data from European Activation

File (EAF) were also added for better understanding.

8. TALYS

124

0.0

0.1

0.2

0.3

0.4

0.5

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


Talys 1.2

Talys 1.0

197Au(n,8n)190Au


Au(n,8n)190

Au in TALYS 1.0 and

TALYS 1.2 (both in basic setting). No EXFOR and EAF data are available.

125

Chapter 9

Conclusion

As a member of the international project Energy and Transmutation

of Radioactive Waste I have studied production and transport of high energy neutrons

in the setup called Energy plus Transmutation. This setup consists of a thick, lead target

surrounded with a natural uranium blanket and a polyethylene biological shielding. The

setup was irradiated with 1.6 GeV, 2.52 GeV, and 4 GeV deuterons. I prepared foils for

all three irradiations; I was present during the irradiation and I measured irradiated foils

at JASNAPP laboratory of the Joint Institute for Nuclear Research, Dubna, Russia.

I have completely by myself evaluated the first two experiments.

I used neutron activation detectors from Al, Au, Bi, Co In, Ta, and Y in the form

of thin foils to measure spatial distribution of the neutrons inside the setup. I have

observed threshold (n,xn), (n,p), and (n,) reactions in the samples in order to

distinguish energies of the neutrons. The maximum order of these reactions was (n,11n),

that means a threshold of ~ 80 MeV. Maximum of neutron flux was detected in the first

gap of the setup that means 12 cm from the target beginning in longitudinal direction.

In radial direction the maximum was in the centre of the target and then it decreased

almost exponentially. Spectral indexes showed a hardening of the neutron spectra

in longitudinal direction. Comparison among deuteron experiments and also with the

previous 0.7 GeV experiment with protons resulted in clear dependence between beam

type or energy and intensity of the neutron flux inside the setup.

Polyethylene biological shielding in combination with non-threshold reactions

enabled me to calculate the total number of produced neutrons. In the case of deuteron

experiments neutron multiplicity was up to 152 ± 16 neutrons per one deuteron

at 4 GeV irradiation.

I have measured deuteron beam properties in detail. I have used Al foil for beam

intensity measurement and Cu foils for beam position, profile and direction

determination. The results of my beam analysis are used by the whole Energy and

Transmutation collaboration.

I made MCNPX simulations of deuteron experiments and I compared them with

experimental data. MCNPX describes relatively well the shape of the neutron

distribution in radial and longitudinal directions, however the absolute exp/sim

differences are much bigger than they should be at future ADS systems, so a further

MCNPX development and benchmark tests are needed. I have not observed any serious

discrepancies in the number of neutrons emitted to backward angles as it was observed

in previous proton experiments.

Further, I obtained unique data about cross-sections of used threshold reactions

for neutron energies above 40 MeV. With the support from EFNUDAT I used quasi-

monoenergetic 7Li(p,n)

7Be neutron source at TSL Uppsala, Sweden. In 2008,

9. CONCLUSION

126

I performed three irradiations with neutron energies 22, 47, and 94 MeV. These

measurements were supplemented with measurements at NPI Řež with neutron energies

17, 22, 30, and 35 MeV. In the meantime I prepared a proposal on the second cross-

section measurement in Uppsala and in 2010 I participated on irradiations at neutron

energies 59, 66, 73, and 89 MeV. I was involved in all experiments and I analyzed the

data completely by myself except the 30 and 35 MeV irradiations at NPI and the second

TSL experiment. I have developed a procedure how to subtract the neutron background,

which was applied at most of measured cross-sections. Using the two different neutron

sources and various spectroscopic equipment I got the same results within the

uncertainties. Therefore all the important sources of uncertainties seem to be under

control. I have compared measured cross-sections with the data from EXFOR where

possible, but the cross-sections over 40 MeV and x in the (n,xn) reaction higher than

four were measured for the first time. I used deterministic code TALYS to calculate

neutron cross-sections of all reactions and I compared cross-sections with measured

data.

I have already presented the data discussed in this work on 15 national and

international workshops and conferences (16. konference českých a slovenských fyziků

[103], Baldin conference [104], NEMEA-5 [105], ND2010 [106], EFNUDAT meetings

[107], [108], AER meetings,…). I am co-author of four articles in peer reviewed

journals ([74], [109], [110] and [111]). I am the first author of 11 proceedings (three of

them are peer reviewed), one internal report [34] and co-author of another five

proceedings (e.g. [37] or [112]) and four internal reports (e.g. [61] or [113]).

127

Appendix A

Threshold and non-threshold reactions on activation samples

Table 17: Threshold and non-threshold reactions on gold activation samples.

Reaction Threshold

energy [MeV]

Half-life Used -line

[keV]

Intensity of used -line

[%]

197Au (n,)

198Au 0 64.7 h

411.8 96

675.9 0.8

1087.7 0.2

197Au (n,2n)

196Au 8.1 6.2 d

426.0 7

333.0 22.9

355.7 87

197Au (n,3n)

195Au 14.8 186.1 d

98.9 10.9

129.7 0.8 197

Au (n,4n) 194

Au 23.2 38 h 328.5 61

197Au (n,5n)

193Au 30.2 17.7 h

173.5 2.9

186.2 10.1

255.6 6.7

268.4 3.9

197Au (n,6n)

192Au 38.9 4.9 h

296.0 22.3

316.5 58 197

Au (n,7n) 191

Au 46.0 3.2 h - - 197

Au (n,8n) 190

Au 55.0 42.8 min - - 197

Au (n,9n) 189

Au 62.5 28.7 min - - 197

Au (n,10n) 188

Au 71.8 8.8 min - -

Half-life of isotopes and gamma line energies were taken from [39]. Threshold energies

were taken from [40]. Isotopes without listed gamma-line and intensity have not been

detected in E+T experiments.

APPENDIX A. THRESHOLD AND NON-THRESHOLD REACTIONS ON ACTIVATION

SAMPLES

128

Table 18: Threshold reactions on bismuth activation samples.

Reaction Threshold

energy [MeV]


[keV]


[%] 209

Bi (n,2n) 208

Bi 7.5 3.68·105 y - -

209Bi (n,3n)

207Bi 14.4 31.6 y

569.7 97.7

1063.7 74.5

209Bi (n,4n)

206Bi 22.6 6.24 d

184.0 15.8

343.5 23.4

497.1 15.3

516.2 40.7

537.5 30.5

803.1 99

881.0 66.2

895.1 15.7

1718.7 31.8

209Bi (n,5n)

205Bi 29.6 15.31 d

579.7 5.4

703.4 31

987.6 16.1

1043.7 7.51

1764.4 32.5

1861.7 6.2

209Bi (n,6n)

204Bi 38.1 11.22 h

899.2 98

984.0 59

209Bi (n,7n)

203Bi 45.4 11.76 h

820.3 30

825.2 14.6

209Bi (n,8n)

202Bi 54.3 1.72 h

422.2 83.7

657.5 60.6

960.7 99.7 209

Bi (n,9n) 201

Bi 61.7 1.8 h 629.1 24 209

Bi (n,10n) 200

Bi 70.9 36.4 min - -


SAMPLES

129

Table 19: Threshold and non-threshold reactions on nat

In activation samples.

Reaction Threshold

energy [MeV]


[keV]


[%]

115In (n,)

116mIn 0 54.3 min

138.3 3.3

416.9 27.7

818.7 11.5

1097.3 56.2

1293.6 84.4

1507.7 10

2112.3 15.5 115

In (n,n') 115m

In 0.34 4.5 h 336.2 45.8 115

In (n,2n) 114

In 9.1 71.9 s - -

115In (n,2n)

114mIn 9.3 49.5 d

190.3 15.4

558.4 3.24

725.2 3.24 115

In (n,3n) 113

In 16.5 stable - - 115

In (n,3n) 113m

In 16.9 1.7 h 391.7 64.2 115

In (n,4n) 112

In 26.0 14.97 min - -

115In (n,5n)

111In 33.7 2.8 d

171.3 90

245.4 94

115In (n,6n)

110In 43.8 4.9 h

641.7 25.9

657.8 98.3

707.4 29.5

884.7 92.9

937.5 68.4

997.3 10.5 115

In (n,7n) 109

In 51.9 4.2 h 203.5 74 115

In (n,8n) 108

In 62.5 58 min - - 115

In (n,9n) 107

In 71.2 32.4 min - - 115

In (n,10n) 106

In 82.3 6.2 min - -

Reactions on 113

In were neglected because of its low abundance in natural indium

mixture (4.3 %).


SAMPLES

130

Table 20: Threshold and non-threshold reactions on tantalum activation samples.

Reaction Threshold

energy [MeV]


[keV]


[%]

181Ta (n,)

182Ta 0 114.5 d

100.0 14.1

152.4 6.9

179.4 3.1

222.1 7.5

229.3 3.6

264.1 3.6

1121.3 34.9

1189.1 16.2

1221.4 27.0

1231.0 11.4

181Ta (n,2n)

180Ta 7.6 8.152 h

93.3 4.5

103.6 0.8 181

Ta (n,3n) 179

Ta 14.3 1.82 y - - 181

Ta (n,4n) 178

Ta 22.3 9.31 min - -

181Ta (n,4n)

178mTa ~ 22.7 2.36 h

213.4 81.4

325.6 94.1

426.4 97 181

Ta (n,5n) 177

Ta 29.2 56.56 h 113.0 7.2

181Ta (n,6n)

176Ta 37.6 8.09 h

201.8 6

710.5 5

1159.3 25

1190.2 4.5

1224.9 6

1584.0 5

1696.6 4.6

1823.7 4.5

2832 4.3

181Ta (n,7n)

175Ta 44.7 10.5 h

207.4 14

266.9 10.8

348.5 12

1793.1 4.6

181Ta (n,8n)

174Ta 53.5 1.05 h

206.5 58

1205.9 4.9

181Ta (n,9n)

173Ta 61.0 3.14 h

172.2 18

160.4 4.9 181

Ta (n,10n) 172

Ta 70.1 36.8 min - -


SAMPLES

131

Table 21: Threshold and non-threshold reactions on yttrium activation samples.

Reaction Threshold

energy [MeV]


[keV]


[%]

89Y (n,)

90mY 0 3.19 h

202.5 97.3

479.2 90.7

89Y (n,2n)

88Y 11.6 106.65 d

898.0 93.7

1836.1 99.2

89Y (n,3n)

87Y 21.1 79.8 h

388.5 82

484.8 89.7

89Y (n,4n)

86Y 33.0 14.74 h

627.7 32.6

703.3 15.4

777.4 22.4

1076.6 82

1153.0 30.5

1854.4 17.2

1920.7 20.8

89Y (n,5n)

85Y 42.6 2.68 h

231.7 84

504.5 60

913.9 9 89

Y (n,6n) 84

Y 54.5 39.5 min - - 89

Y (n,7n) 83

Y 64.5 7.08 min - - 89

Y (n,8n) 82

Y 76.9 9.5 s - - 89

Y (n,9n) 81

Y 87.2 70.4 s - - 89

Y (n,10n) 80

Y 100.3 35 s - -


SAMPLES

132

133

Appendix B

Placement of the foils during Energy plus Transmutation

deuteron experiments Table 22: Placement of the activation samples in 2.52 GeV deuteron experiment.

Distance from the

target axis [cm] Foil label in the 2.52 GeV deuteron experiment

1. pla

ne

0 Y_32

3 Al31 Au1 Ta01 Bi1 In1 Y_34

6 Al32 Au2 Ta02 Y_15

8.5 Al33 Au3 Ta03 Y_16

10.5 Y_6

10.7 Al34 Au4 Ta04

13.5 Y_7

2. pla

ne

0 Y_9

3 Al35 Au5 Ta05 Bi2 In2 Y_12

6 Al36 Au6 Ta06 Bi3 In3 Y_31

8.5 Al37 Au7 Ta07 Bi4 In4 Y_14

10.5 Y_19

10.7 Al38 Au8 Ta08

11.5 Bi5 In5

13.5 Y_33

3. pla

ne

0 Y_23

3 Al39 Au9 Ta09 Bi6 In6 Y_35

6 Al40 Au10 Ta10 Y_24

8.5 Al11 Au11 Ta11 Y_29

10.5 Y_1

10.7 Al12 Au12 Ta12

13.5 Y_3

4. pla

ne

0 Y_25

3 Al13 Au13 Ta13 Bi7 Y_36

6 Al14 Au14 Ta14 Y_22

8.5 Al15 Au15 Ta15 Y_8

10.5 Y_18

10.7 Al16 Au16 Ta16

13.5 Y_5

5. pla

ne

0 Y_17

3 Al17 Au17 Ta17 Bi8 Y_26

6 Al18 Au18 Ta18 Y_20

8.5 Al19 Au19 Ta19 Y_11

10.5 Y_21

10.7 Al20 Au20 Ta20

13.5 Y_13

APPENDIX B. PLACEMENT OF THE FOILS DURING ENERGY PLUS

TRANSMUTATION DEUTERON EXPERIMENTS

134

Table 23: Placement of the activation samples in 4 GeV deuteron experiment.

Distance from

the target axis

[cm]

Foil label in the 4 GeV deuteron experiment

1. pla

ne

0

Y32

3 Al1 Au1 Ta01 Bi1 Co1 In1 Y61

6 Al2 Au2 Ta02

Y15

8.5 Al3 Au3 Ta03

Y16

10.5

Y6

10.7 Al4 Au4 Ta04

13.5

Y7

2. pla

ne

0

Y9


6

Al6,

Al1new,

Al2new,

Al3new

Au6,

Au1new,

Au2new,

Au3new

Ta06 Bi3 Co3 In3 Y31

8.5 Al7 Au7 Ta07 Bi4 Co4 In4 Y14

10.5

Y19

10.7 Al8 Au8 Ta08

11.5

Bi5 Co5 In5

13.5

Y33

3. pla

ne

0

Y58


6 Al10 Au10 Ta10

Y57

8.5 Al11 Au11 Ta11

Y56

10.5

Y54

10.7 Al12 Au12 Ta12

13.5

Y52

4. pla

ne

0

Y25


6 Al14 Au14 Ta14

Y22

8.5 Al15 Au15 Ta15

Y8

10.5

Y18

10.7 Al16 Au16 Ta16

13.5

Y5

5. pla

ne

0

Y17


6 Al18 Au18 Ta18

Y20

8.5 Al19 Au19 Ta19

Y11

10.5

Y21

10.7 Al20 Au20 Ta20

13.5

Y13

Samples printed in normal letters were placed in the upward direction from the target

axis (on the vertical axis, blue color in Figure 101). Samples printed in bold letters were



135

placed in the right-down direction 30° from the horizontal axis (red color in Figure

101). Samples printed in cursive were placed in the up-left direction 30° from the

vertical axis.

detector plate - 1

Pb target

this side to the beam

30°

3060107 3085

Dimensions in mm

detector plate - 2

Pb target


30°

3060107 3060

115

85

85

Dimensions in mm

60

detector plate - 3

Pb target


30°

3060107 3085

Dimensions in mm

detector plate - 4

Pb target


30°

3060107 3085

Dimensions in mm

detector plate - 5

Pb target


30°

3060107 3085

Dimensions in mm

Figure 101: Schematic drawings of detector placement in 4 GeV deuteron experiment

on E+T setup (blue color – Al, Au, Ta; red color Bi, In, Co; green color – Au).



136

137

Appendix C

List of spectra measured in E+T deuteron experiments

Table 24: Spectra measured in 1.6 GeV deuteron experiment.

Distance

from the

target axis

[cm]

Measured spectra

1. pla

ne

0

cY5p2,

cY5p2b

3 cAl01p2 cAu01p2,

cAu01p2b cTa01p3

cBi01p5,

cBi01p3b cIn01p4

cY8p2,

cY8p2b

6 cAl02p2 cAu02p2 cTa02p2

cY13p2

8.5 cAl03p2 cAu03p2 cTa03p2

cY15p2

10.5

cY22p2


13.5

cY9p2

up

cY19p2

down

cY21p2

left

cY38p2

right

cY20p2

2.

pla

ne

0

cY10p2,

cY10p2b

3 cAl05p2 cAu05p2,

cAu05p2b cTa05p3

cBi02p5,

cBi02p2b cIn02p5

cY1p2,

cY1p2b

6 cAl06p2 cAu06p2,

cAu06p2b cTa06p2

cBi03p3,

cBi03p3b cIn03p4 cY6p2

8.5 cAl07p2 cAu07p2,

cAu07p2b cTa07p2

cBi04p2,

cBi04p2b cY7p2

8.7

cIn04p4 cY32p2,

cY32p2b

10.7 cAl08p2 cAu08p2 cTa08p2 cBi05p2,

cBi5p2b

11.5

cIn05p4

13.5

cY2p2,

cY2p2b

3. pla

ne

0

cY4p2,

cY4p2b

3 cAl09p2 cAu09p2,

cAu09p2b cTa09p3

cBi06p5,

cBi06p3b cIn06p4

cY35p2,

cy35p2b

6 cAl10p2 cAu10p2,

cAu10p2b cTa10p2

cY36p2

APPENDIX C. LIST OF SPECTRA MEASURED IN E+T DEUTERON EXPERIMENTS

138

8.5 cAl11p2 cAu11p2,

cAu11p2b cTa11p2

cY18p2

10.5

cY33p2

10.7 cAl12p2 cAu12p2,

cAu12p2b cTa12p2

13.5

cY27p2

4. pla

ne

0

cY41p2,

cY41p2b

3 cAl13p2 cAu13p2,

cAu13p2b cTa13p3

cBi07p5,

cBi07p3b cIn07p2

cY25p2,

cY25p2b


cY34p2,

cY34p2b


cY37p2,

cY37p2b

10.5

cY40p2,

cY40p2b


13.5

cY16p2,

cY16p2b

5. pla

ne

0

cY17p2,

cY17p2b

3 cAl17p2 cAu17p2,

cAu17p2b cTa17p2

cBi08p4,

cBi08p2b cIn08p3

cY11p2,

cY11p2b


cY29p2,

cY29p2b


cY3p2,

cY3p2b

10.5

cY39p2,

cY39p2b


13.5

cY12p2,

cY12p2b


139

Table 25: Spectra measured in 2.52 GeV deuteron experiment.

Distance

from the

target axis

[cm]

Measured spectra

1. pla

ne

0

dy32p2

3 dal01p2 dau01p2,

dau01p2b

dta01p2,

dTa01p2b

dbi1p4,

dbi1p2b

din1p2,

din1p2b

dy34p2,

dy34p2b

6 dal02p5 dau02p2,

dau02p2b

dTa02p2,

dTa02p2b dy15p2

8.5 dal03p2 dau03p2,

dau03p2b

dTa03p2,

dTa03p2b dy16p2

10.5

dy6p2

10.7 dal04p2 dau04p2,

dau04p2b

dTa04p2,

dTa04p2b

13.5

dy7p2

2. pla

ne

0

dy9p2,

dy9p2b

3

dal05p2,

dal05p2x,

dal05p3x,

dal05p4x,

dal05p5x,

dal05p6x

dau05p2,

dau05p2b

dau05p2c

dTa05p2,

dTa05p2b

dbi2p6,

dbi2p2b

din2p2,

din2p2b

dy12p2,

dy12p2b

6 dal06p2 dau06p2,

dau06p2b

dTa06p2,

dTa06p2b

dbi3p3,

dbi3p2b

din3p2,

din3p2b

dy31p2,

dy31p2b


dau07p2b

dTa07p2,

dTa07p2b

dbi4p2,

dbi4p2b

din4p2,

din4p2b dy14p2

10.5

dy19p2,

dy19p2b

10.7 dal08p2 dau08p2,

dau08p2b

dTa08p2,

dTa08p2b

dbi5p2,

dbi5p2b

11.5

din5p2,

din5p2b

13.5

dy33p2,

dy33p2b

3. pla

ne

0

dy23p2

3 dal09p2 dau09p2,

dau09p2b

dTa09p2,

dTa09p2b

dbi6p4,

dbi6p2b

din6p2,

din6p2b

dy35p2,

dy35p2b

6 dal10p2 dau10p2,

dau10p2b

dTa10p2,

dTa10p2b dy24p2


dau11p2b

dTa11p2,

dTa11p2b dy29p2

10.5

dy1p2


140

10.7 dal12p2 dau12p2,

dau12p2b

dTa12p2,

dTa12p2b

13.5

dy3p2

4. pla

ne

0

dy25p2

3 dal13p2 dau13p2,

dau13p2b

dTa13p2,

dTa13p2b dbi7p3,

dy36p2,

dy36p2b

6 dal14p2 dau14p2,

dau14p2b

dTa14p2,

dTa14p2b dy22p2


dau15p2b

dTa15p2,

dTa15p2b dy8p2

10.5

dy18p2

10.7 dal16p2 dau16p2,

dau16p2b

dTa16p2,

dTa16p2b

13.5

dy5p2

5. pla

ne

0

dy17p2

3 dal17p2 dau17p2,

dau17p2b

dTa17p2,

dT17p2b,

dTa17p2c

dbi8p2

dy26p2,

dy26p2b

6 dal18p2 dau18p2,

dau18p2b

dTa18p2,

dTa18p2b dy20p2


dau19p2b

dTa19p2,

dTa19p2b dy11p2

10.5

dy21p2

10.7 dal20p2 dau20p2,

dau20p2b

dTa20p2,

dTa20p2b

13.5

dy13p2


141

Table 26: Spectra measured in 4 GeV deuteron experiment on Al, Au, Ta, and Bi foils.

Distance

from the

target axis

[cm]

Measured spectra

1. pla

ne

3 w-Al01-p2-1 w-Au01-p2-1,

w-Au01-p2-2

w-Ta01-p2-1,

w-Ta01-p2-2

w-Bi1-p3-1,

w-Bi1-p3-2,

w-Bi1-p2-3

6 w-Al02-p5-1 w-Au02-p2-1,

w-Au02-p2-2

w-Ta02-p2-1,

w-Ta02-p2-2

8.5 w-Al03-p2-1 w-Au03-p2-1,

w-Au03-p2-2

w-Ta03-p2-1,

w-Ta03-p2-2

10.7 w-Al04-p2-1 w-Au04-p2-1,

w-Au04-p2-2

w-Ta04-p2-1,

w-Ta04-p2-2

2. pla

ne

3 w-Al05-p2-1 w-Au05-p3-1,

w-Au05-p2-2

w-Ta05-p3-1,

w-Ta05-p2-2

w-Bi2-p5-1,

w-Bi2-p3-2,

w-Bi3-p2-3

6

w-Al06-p2-1,

w-Al1new-p2-

1, Al2new-p2-

1, Al3new-p2-1

w-Au06-p2-1,

w-Au06-p2-2,

w-Au1new-p2-1,

w-Au1new-p2-2,

w-Au2new-p2-1,

w-Au2new-p2-2,

w-Au3new-p2-1,

w-Au3new-p2-2

w-Ta06-p2-1,

w-Ta06-p2-2

w-Bi3-p3-1,

w-Bi3-p3-2,

w-Bi3-p2-3

8.5 w-Al07-p2-1 w-Au07-p2-1,

w-Au07-p2-2

w-Ta07-p2-1,

w-Ta07-p2-2

w-Bi4-p3-1,

w-Bi4-p3-2,

w-Bi4-p2-3

10.7 w-al08-p2-1 w-Au08-p2-1,

w-Au08-p2-2

w-Ta08-p2-1,

w-Ta08-p2-2

11.5

w-Bi5-p3-1,

w-Bi5-p3-2,

w-Bi5-p2-3

3. pla

ne

3 w-Al09-p2-1 w-Au09-p2-1,

w-Au09-p2-2

w-Ta09-p2-1,

w-Ta09-p2-2

w-Bi6-p4-1,

w-Bi6-p3-2,

w-Bi6-p2-3

6 w-Al10-p2-1 w-Au10-p2-1,

w-Au10-p2-2

w-Ta10-p2-1,

w-Ta10-p2-2

8.5 w-Al11-p2-1 w-Au11-p2-1,

w-Au11-p2-2

w-Ta11-p2-1,

w-Ta11-p2-2

10.7 w-Al12-p2-1 w-Au12-p2-2,

w-Au12-p2-2

w-Ta12-p2-1,

w-Ta12-p2-2


142

4. pla

ne

3 w-Al13-p2-1 w-Au13-p2-1,

w-Au13-p2-2

w-Ta13-p2-1,

w-Ta13-p2-2

w-Bi7-p3-1,

w-Bi7-p3-2,

w-Bi7-p2-3

6 w-Al14-p2-1 w-Au14-p2-1,

w-Au14-p2-2

w-Ta14-p2-1,

w-Ta14-p2-2

8.5 w-Al15-p2-1 w-Au15-p2-1,

w-Au15-p2-2

w-Ta15-p2-1,

w-Ta15-p2-2

10.7 w-Al16-p2-1 w-Au16-p2-1,

w-Au16-p2-2

w-Ta16-p2-1,

w-Ta16-p2-2

5. pla

ne

3 w-Al17-p2-1 w-Au17-p2-1,

w-Au17-p2-2

w-Ta17-p2-1,

w-Ta17-p2-2

w-Bi8-p3-1,

w-Bi8-p3-2,

w-Bi8-p2-3

6 w-Al18-p2-1 w-Au18-p2-1,

w-Au18-p2-2

w-Ta18-p2-1,

w-Ta18-p2-2

8.5 w-Al19-p2-1 w-Au19-p2-1,

w-Au19-p2-2

w-Ta19-p2-1,

w-Ta19-p2-2

10.7 w-Al20-p2-1 w-Au20-p2,

w-Au20-p2-2

w-Ta20-p2-1,

w-Ta20-p2-2


143

Table 27: Spectra measured in 4 GeV deuteron experiment on Co, In, and Y foils.

Distance

from the

target axis

[cm]

Measured spectra

1. p

lan

e

0

p-Y32-p2-1, p-Y32-p2-2

3 w-In1-p5-1, w-In1-p2-2 w-Co1-p2-1, w-Co1-p2-2 p-Y61-p2-1, p-Y61-p2-2

6

p-Y15-p2-1, p-Y15-p2-2

8.5

p-Y16-p2-1, p-Y16-p2-2

11

p-Y06-p2-1, p-Y06-p2-2

14

p-Y07-p2-1, p-Y07-p2-2

2. p

lan

e

0

p-Y09-p2-1, p-Y09-p2-2



8.5 w-In4-p5-1, w-In4-p2-2 w-Co4-p2-1, w-Co4-p2-2 p-Y14-p2-1, p-Y14-p2-2

11

p-Y19-p2-1, p-Y19-p2-2

11.5 w-In5-p5-1, w-In5-p2-2 w-Co5-p2-1, w-Co5-p2-2

14

p-Y33-p2-1, p-Y33-p2-2

3. p

lan

e

0

p-Y58-p2-1, p-Y58-p2-2


6

p-Y57-p2-1, p-Y57-p2-2

8.5

p-Y56-p2-1, p-Y56-p2-2

11

p-Y54-p2-1, p-Y54-p2-2

14

p-Y52-p2-1, p-Y52-p2-2

4. p

lan

e

0

p-Y25-p2-1, p-Y25-p2-2


6

p-Y22-p2-1, p-Y22-p2-2

8.5

p-Y08-p2-1, p-Y08-p2-2

11

p-Y18-p2-1, p-Y18-p2-2

14

p-Y05-p2-1, p-Y05-p2-2

5. p

lan

e

0

p-Y17-p2-1, p-Y17-p2-2


6

p-Y20-p2-1, p-Y20-p2-2

8.5

p-Y11-p2-1, p-Y11-p2-2

11

p-Y21-p2-1, p-Y21-p2-2

14

p-Y13-p2-1, p-Y13-p2-2


144

145

Appendix D

Correction factor on beam instability

Table 28: Correction factor on beam instability for all three deuteron experiments on

E+T setup

Isotope Half-life

[h]

Correction factor on beam instability

1.6 GeV 2.52 GeV 4 GeV 198

Au 64.7 0.9984 0.9904 0.9917 196

Au 148.4 0.9993 0.9958 0.9963 195

Au 4466.2 1.0000 0.9999 0.9999 194

Au 38.0 0.9972 0.9839 0.9863 193

Au 17.7 0.9941 0.9665 0.9733 192

Au 4.9 0.9793 0.8993 0.9377 191

Au 3.2 - - 0.9216 24

Na 15.0 0.9930 0.9610 0.9695 210

Po 3321.0 1.0000 0.9998 0.9998 207

Bi 276378.0 1.0000 1.0000 1.0000 206

Bi 149.8 0.9993 0.9958 0.9963 205

Bi 367.4 0.9997 0.9983 0.9985 204

Bi 11.2 0.9907 0.9493 0.9621 203

Bi 11.8 0.9912 0.9514 0.9634 202

Bi 1.7 0.9428 0.8166 0.8733 201

Bi 1.8 0.9452 0.8193 0.8786 201

Pb 9.3 0.9889 0.9403 0.9569 201

Tl 72.9 0.9986 0.9915 0.9926 200

Pb 21.5 0.9951 0.9722 0.9773 200

Tl 26.1 0.9960 0.9769 0.9808 199

Pb 1.5 0.9349 0.8099 0.8556 199

Tl 7.4 0.9861 0.9274 0.9502 198

Pb 2.4 0.9584 0.8399 0.9053 198

Tl 5.3 0.9807 0.9046 0.9400 197

Tl 1.8 0.9463 0.8206 0.8811 116m

In 54.3 0.9981 0.9886 0.9902 115m

In 4.5 0.9773 0.8918 0.9347 114m

In 1188.0 0.9999 0.9995 0.9995 113m

In 1.7 0.9407 0.8146 0.8688 111

In 67.3 0.9984 0.9908 0.9920 110

In 4.9 0.9792 0.8987 0.9375 110m

In 1.2 0.9170 0.8038 0.8154 109

In 4.2 0.9758 0.8866 0.9325 108

In 1.0 0.9029 0.8058 0.7843

APPENDIX D. CORRECTION FACTOR ON BEAM INSTABILITY

146

108mIn 0.7 0.8718 0.8260 0.7129

180Ta 8.2 0.9873 0.9329 0.9530

178Ta 2.4 0.9577 0.8385 0.9041

177Ta 56.6 0.9981 0.9891 0.9905

176Ta 8.1 0.9872 0.9325 0.9528

175Ta 10.5 0.9901 0.9462 0.9603

174Ta 1.1 0.9100 0.8042 0.7999

173Ta 3.1 0.9679 0.8622 0.9211

173Hf 23.6 0.9956 0.9746 0.9790

172Er 49.3 0.9979 0.9875 0.9892

171Er 7.5 0.9863 0.9282 0.9506

90mY 3.2 0.9684 0.8636 0.9218

88Y 2559.6 1.0000 0.9998 0.9998

87Y 79.8 0.9987 0.9922 0.9932

87mY 13.4 0.9922 0.9568 0.9667

86Y 14.7 0.9929 0.9605 0.9691

85Y 2.7 0.9626 0.8489 0.9127

85mY 4.9 0.9790 0.8981 0.9372

82mRb 6.5 0.9841 0.9186 0.9461

83Sr 32.4 0.9968 0.9812 0.9842

81Rb 4.6 0.9777 0.8934 0.9353

77Br 57.0 0.9982 0.9892 0.9906

73Se 7.2 0.9856 0.9251 0.9491

147

Appendix E

Examples of correction factors on real coincidences

Table 29: Correction factor on real coincidences of gold isotopes produced in 1.6 GeV

deuteron experiment on E+T, ORTEC(new1) detector, p2 position.

Isotope Energy of the gamma line [keV] Real coincidence correction [-]

198Au

411.8 0.9992

675.9 0.8850

1087.7 1.2610

196Au

333.0 0.8814

355.7 0.9676

426.0 1.0000

196m2Au

147.8 0.9368

188.3 0.9301

168.4 0.9301

285.5 1.0004

316.2 1.0107

137.7 0.9301

195Au

98.9 0.9998

129.7 1.0003

194Au

293.5 0.7948

328.5 0.9335

193Au

173.5 0.9882

186.2 0.9893

255.6 0.9986

268.2 1.0027

192Au

316.5 0.8953

296.0 0.8169

308.5 0.7785

582.6 0.7459

612.5 1.3465

191Au

277.9 0.9945

283.9 0.9397 188

Au 265.6 0.9169

189Pt

94.3 0.9415

243.4 0.6121

544.9 0.8389

568.9 0.4837

607.6 0.9903

721.4 1.0548

APPENDIX E. EXAMPLES OF CORRECTION FACTORS ON REAL COINCIDENCES

148

149

Appendix F

Yields of isotopes produced on activation foils during 1.6 and

2.52 GeV deuteron experiments on “Energy plus Transmutation”

setup

Table 30: Yields of main isotopes observed on aluminum and gold foils irradiated in

1.6 GeV experiment.

Foil 27

Al 197

Au

Reaction (n,) (n,) (n,2n) (n,4n) (n,5n) (n,6n)

Product 24

Na 198

Au 196

Au 194

Au 193

Au 192

Au

Ethresh [MeV] 3.2 0 8.1 23.2 30.2 38.9

T1/2 [h] 15 65 148 38 18 5

X [cm] Longitudinal yields for R = 3.0 cm [10-6

.g-1

.deuteron-1

]

0.0 11.38(16) 296(5) 15.1(18) 3.15(14) 1.78(25) 1.30(5)

11.8 26.2(3) 400(3) 33.7(12) 10.5(5) 9.5(5) 6.05(13)

24.0 15.58(19) 366.9(29) 20.3(7) 6.6(3) 5.5(5) 3.99(16)

36.2 7.56(12) 273(6) 10.2(4) 3.66(19) 4.0(3) 2.14(7)

48.4 2.80(13) 157.6(13) 3.71(24) 1.66(9) 1.72(18) 1.05(7)


.g-1

.deuteron-1

]

0.0 5.27(9) 264(3) 7.68(11) 1.61(4) 0.84(13) 0.81(5)

11.8 10.49(15) 343(6) 14.9(17) 4.43(17) 3.1(4) 2.46(9)

24.0 7.44(11) 327.4(20) 10.8(4) 3.48(15) 2.13(29) 1.84(7)

36.2 3.72(7) 256(6) 5.86(12) 1.93(6) 1.50(28) 1.16(8)

48.4 1.68(3) 146.6(24) 2.33(9) 0.89(6) 0.46(12) 0.75(11)


.g-1

.deuteron-1

]

0.0 3.23(6) 277(4) 4.67(13) 1.01(5) 0.82(21) 0.46(9)

11.8 6.4(6) 359.6(25) 8.8(5) 2.54(15) 1.53(22) 1.25(7)

24.0 4.64(9) 335.6(28) 6.11(29) 1.99(12) 1.53(25) 1.09(6)

36.2 2.40(5) 290.8(22) 3.50(11) 1.27(5) 0.66(15) 0.73(10)

48.4 1.04(3) 176.5(11) 1.46(8) 0.61(4) 0.56(16) 0.56(22)


.g-1

.deuteron-1

]

0.0 1.94(4) 302.2(28) 2.94(9) 0.76(4) 0.57(13) 0.29(7)

11.8 3.75(7) 398.2(28) 5.7(3) 1.90(11) 1.3(3) 0.86(5)

24.0 2.90(6) 349(11) 4.3(3) 1.34(13) 0.9(4) 0.69(5)

36.2 1.55(4) 352(3) 2.53(9) 0.93(4) 0.55(16) 0.46(10)

48.4 0.725(20) 210(3) 1.12(10) 0.39(5) 0.36(12) 0.34(12)

APPENDIX F. YIELDS OF ISOTOPES PRODUCED IN „E+T“ DEUTERON

EXPERIMENTS

150

Table 31: Yields of main isotopes observed on bismuth foils irradiated in 1.6 GeV

experiment.

Foil 209

Bi

Reaction (n,4n) (n,5n) (n,6n) (n,7n) (n,8n) (n,9n)

Product 206

Bi 205

Bi 204

Bi 203

Bi 202

Bi 201

Bi

Ethresh [MeV] 22.6 29.6 38.1 45.4 54.3 61.7

T1/2 [h] 150 367 11 12 2 2


.g-1

.deuteron-1

]

0.0 4.7(3) 5.3(29) 2.07(6) 1.23(19) 1.79(22) 1.7(3)

11.8 14.6(12) 17(14) 7.0(15) 6.3(12) 6.06(18) 3.4(4)

24.0 7.7(4) 11(5) 4.2(4) 3.41(13) 3.68(15) 2.7(3)

36.2 4.5(3) 4.9(24) 2.5(3) 2.01(19) 2.42(15) 1.81(17)

48.4 1.66(17) 2.1(19) 1.01(3) 0.93(5) 0.99(13) 0.55(6)

R [cm] Radial yields for X = 11.8 cm [10-6

.g-1

.deuteron-1

]

3.0 14.6(12) 17(14) 7.0(15) 6.3(12) 6.06(18) 3.4(4)

6.0 4.87(20) 4.8(10) 2.17(5) 1.77(22) 1.54(8) 0.95(9)

8.5 2.41(14) 2.03(22) 0.937(25) 0.76(7) 0.67(4) 0.34(4)

10.7 1.36(10) 1.36(15) 0.539(16) 0.49(13) 0.350(20) 0.196(27)

Table 32: Yields of main isotopes observed on indium foils irradiated in 1.6 GeV

experiment.

Foil 115

In

Reaction (n,) (n,n') (n,2n) (n,3n) (n,5n) (n,6n) (n,7n)

Product 116m

In 115m

In 114m

In 113m

In 111

In 110

In 109

In

Ethresh [MeV] 0 0.34 9.3 16.9 33.7 43.8 51.9

T1/2 [h] 1 4.5 1188 1.7 2.8 4.9 4.2


.g-1

.deuteron-1

]

0.0 440(16) 54.2(7) 419(44) 2.86(17) 3.5(18) 1.10(21) 0.70(7)

11.8 741(5) 152.9(17) 296(62) 9.2(4) 15.0(9) 4.6(3) 3.52(24)

24.0 715(4) 83.4(12) 147(41) 4.36(21) 9.9(6) 2.14(23) 2.13(14)

36.2 446.8(25) 49.8(7) 96(23) 2.47(14) 6.7(4) 1.06(16) 1.12(7)

48.4 222.7(17) 11.91(29) 31(12) - 1.80(16) 0.62(9) 0.55(6)


.g-1

.deuteron-1

]

3.0 741(5) 152.9(17) 296(62) 9.2(4) 15.0(9) 4.6(3) 3.52(24)

6.0 747(4) 67.4(9) 594(521) 3.8(2) 5.9(5) 1.88(21) 0.75(11)

8.5 751(4) 44.1(7) - 1.90(14) 2.2(15) 1.54(26) 0.56(14)

11.5 959(5) 24.6(6) 51(61) 1.05(16) 2.3(5) 0.62(24) -


EXPERIMENTS

151

Table 33: Yields of main isotopes observed on tantalum foils irradiated in 1.6 GeV

experiment.

Foil 181

Ta

Reaction (n,) (n,2n) (n,4n) (n,5n) (n,6n) (n,7n)

Product 182

Ta 180

Ta 178m

Ta 177

Ta 176

Ta 175

Ta

Ethresh [MeV] 0 7.6 22.7 29.2 37.6 44.7

T1/2 [h] 2746 8 2 57 8 11


.g-1

.deuteron-1

]

0.0 162(32) 12.8(15) 1.9(7) 0.24(3) 1.2(5) 0.88(20)

11.8 517(234) 46(12) 4.7(4) 1.38(14) 5.84(25) 5.43(22)

24.0 263(62) 17.2(9) 1.92(23) 0.49(6) 2.56(12) 2.5(5)

36.2 151(27) 7.8(10) 0.98(19) 0.28(3) 1.23(7) 1.07(10)

48.4 78(21) 3.23(27) 0.51(14) 0.144(18) 0.64(4) 0.61(7)


.g-1

.deuteron-1

]

0.0 309(14) 10.2(6) - 0.121(19) 0.87(15) 0.70(6)

11.8 215(14) 9.8(5) 1.001(18) 0.309(26) 1.36(6) 1.11(13)

24.0 149(10) 36.1(16) - 0.196(14) 6.01(20) 2.93(19)

36.2 259(9) 2.7(3) - 0.207(19) 0.89(13) 0.76(28)

48.4 84.7(17) 1.09(24) - 0.053(8) 0.40(7) 0.4(4)


.g-1

.deuteron-1

]

0.0 337(7) 7.2(19) - 0.298(18) 1.15(13) 0.42(5)

11.8 444(24) 13.8(8) 1.51(3) 0.36(5) 1.95(8) 1.37(23)

24.0 144(7) 23.7(10) - 0.118(13) 3.79(13) 1.93(15)

36.2 185(7) 1.12(20) - 0.149(11) 0.28(10) 0.277(25)

48.4 85(3) 0.7(6) - 0.066(6) 0.28(6) 0.22(5)


.g-1

.deuteron-1

]

0.0 282(6) 3.6(5) - 0.215(16) - -

11.8 461(12) 9.0(4) 1.136(25) 0.27(3) 1.03(5) 0.85(27)

24.0 264(8) 29.0(17) - 0.097(27) 4.07(19) 2.11(35)

36.2 268(8) 1.29(20) - 0.163(11) - 0.21(3)

48.4 97(3) 0.64(18) - 0.073(6) - 0.095(14)


EXPERIMENTS

152

Table 34: Yields of main isotopes observed on yttrium samples irradiated in 1.6 GeV

experiment.

Foil 89

Y

Reaction (n,) (n,2n) (n,3n) (n,4n) (n,5n)

Product 90m

Y 88

Y 87

Y 86

Y 85

Y

Ethresh [MeV] 0 11.6 21.1 33 42.6

T1/2 [h] 3 2568 80 15 3


.g-1

.deuteron-1

]

0.0 0.29(4) 77.7(12) 54.2(5) 22.8(22) 7.3(11)

11.8 0.79(5) 145.3(17) 103.0(22) 40(3) 11.8(13)

24.0 0.480(23) 67.6(11) 50.2(6) 18.1(15) 5.8(8)

36.2 0.238(25) 27.5(6) 20.95(29) 8.2(5) 2.06(5)

48.4 0.070(5) 9.1(3) 7.08(15) 2.64(8) 0.80(13)


.g-1

.deuteron-1

]

0.0 0.196(9) 19.8(6) 8.84(20) 2.21(5) 0.500(19)

11.8 0.514(14) 47.7(8) 30.1(5) 9.35(21) 2.5(4)

24.0 0.347(10) 26.6(8) 18.04(20) 5.80(16) 1.2(3)

36.2 0.193(7) 13.9(4) 9.61(15) 3.27(12) 0.48(6)

48.4 0.051(4) 4.78(22) 4.01(5) 1.44(11) 0.196(15)


.g-1

.deuteron-1

]

0.0 5.4(13) - 3.60(5) 0.983(26) -

11.8 0.311(12) - 5.8(3) 3.01(6) 0.651(24)

24.0 0.28(7) - 5.32(12) 2.64(8) 0.75(5)

36.2 41(5) 7.64(12) 4.9(3) 1.6(3) -

48.4 110(17) 3.40(8) 2.49(8) 0.92(5) 130(99)


.g-1

.deuteron-1

]

0.0 6.4(13) - 2.39(7) 0.62(6) -

11.8 0.242(26) - 3.68(25) 1.82(5) 0.431(23)

24.0 0.23(6) - 3.29(9) 1.51(4) 0.42(3)

36.2 56(7) 4.66(12) 2.97(15) 0.94(3) -

48.4 196(21) 2.00(5) 1.38(4) 0.480(21) -


.g-1

.deuteron-1

]

0.0 10.6(8) - 1.612(25) 0.442(18) -

11.8 0.17(3) 7.39(28) 2.36(21) 1.14(9) 0.241(13)

24.0 0.19(7) - 2.17(6) 1.056(28) 0.301(22)

36.2 82(8) 3.27(9) 2.03(9) 0.610(24) -

48.4 287(28) 1.52(4) 2.49(8) 0.342(24) -


EXPERIMENTS

153

Table 34: Part II


.g-1

.deuteron-1

]

0.0 14.9(12) - 1.00(3) 0.270(16) -

11.8 0.099(21) 4.36(24) 2.1(6) 0.66(5) 0.139(9)

24.0 0.10(6) - 1.19(4) 0.601(18) 0.165(21)

36.2 170(11) 1.80(9) 1.23(4) 0.358(17) -

48.4 614(48) 0.96(5) 0.65(4) 0.20(3) -


2.52 GeV experiment.

Foil 27

Al 197

Au

Reaction (n,) (n,) (n,2n) (n,4n) (n,5n) (n,6n)

Product 24

Na 198

Au 196

Au 194

Au 193

Au 192

Au

Ethresh [MeV] 3.2 0 8.1 23.2 30.2 38.9

T1/2 [h] 15 65 148 38 18 5


.g-1

.deuteron-1

]

0.0 11.63(21) 284(8) 22.3(4) 4.87(16) 2.3(4) 2.18(14)

11.8 20.8(29) 382(4) 35(4) 10.65(18) 8(1) 5.25(23)

24.0 15.08(28) 412.5(28) 20(5) 6.4(9) 6.8(8) 4.47(28)

36.2 8.94(15) 316(117) 14.9(3) 4.77(19) 5.6(5) 2.54(12)

48.4 3.46(8) 157(22) 5.59(11) 2.12(14) 2.11(29) 1.20(12)


.g-1

.deuteron-1

]

0.0 5.14(28) 266.5(23) 9.84(28) 2(1) 2.3(7) -

11.8 10.21(24) 343.8(18) 17.21(20) 5.16(24) 3.8(5) 2.39(17)

24.0 7.63(15) 342.5(18) 12.84(15) 4.2(26) 2.5(5) 3.0(4)

36.2 6.02(14) 269(13) 7.48(17) 2(3) 1.5(5) -

48.4 1.9(3) 157.87(15) 3.26(17) 1.2(17) 0.82(27) -


.g-1

.deuteron-1

]

0.0 3.9(14) 265(8) 6.7(7) 1.4(11) - -

11.8 6.13(14) 368.7(12) 10.45(19) 3.33(14) 2.3(6) 1.48(12)

24.0 4.54(12) 350.7(23) 7.76(18) 2.4(19) 1.1(5) 1.3(4)

36.2 2.94(9) 291(7) 5.14(28) 1.6(10) 1.8(5) -

48.4 1.23(6) 171.0(18) 2.08(14) 0.85(11) - -


.g-1

.deuteron-1

]

0.0 2.09(8) 303.0(21) 3.82(22) 1.2(14) - -

11.8 3.56(17) 382(6) 6.43(18) 1.90(26) - 0.80(12)

24.0 2.7(38) 382(56) 5.06(21) 1.8(10) - -

36.2 1.98(5) 340(6) 3.39(16) 1.0(6) - -

48.4 0.88(3) 209.4(15) 1.25(10) 0.64(28) - -


EXPERIMENTS

154


experiment.

Foil 209

Bi

Reaction (n,4n) (n,5n) (n,6n) (n,7n) (n,8n) (n,9n)

Product 206

Bi 205

Bi 204

Bi 203

Bi 202

Bi 201

Bi

Ethresh [MeV] 22.6 29.6 38.1 45.4 54.3 61.7

T1/2 [h] 150 367 11 12 2 2


.g-1

.deuteron-1

]

0.0 11.7(13) 9.5(11) 5.4(4) 4.28(28) 7.99(29) 3.9(8)

11.8 30(4) 27.6(21) 17(24) 16.5(13) 13.0(4) 8.9(9)

24.0 12.1(10) 10.8(13) 6.2(7) 5.4(5) 5.66(25) 2.6(3)

36.2 5.1(4) 6(6) 2.7(7) 2.4(7) 2.68(11) 1.75(24)

48.4 2.3(4) 4(3) 1.29(27) 1.6(6) 1.49(21) 0.58(14)


.g-1

.deuteron-1

]

3.0 30(4) 27.6(21) 17(24) 16.5(13) 13.0(4) 8.9(9)

6.0 8.6(5) 7.6(13) 4.1(17) 3.11(16) 2.73(20) 1.35(20)

8.5 4.07(21) 4(4) 2.05(24) 1.51(6) 1.098(22) 0.70(7)

10.7 2.30(6) 1.99(29) 0.9(3) 0.81(17) 0.57(6) 0.30(4)


experiment.

Foil 115

In

Reaction (n,) (n,n') (n,2n) (n,3n) (n,5n) (n,6n) (n,7n)

Product 116m

In 115m

In 114m

In 113m

In 111

In 110

In 109

In

Ethresh [MeV] 0 0.34 9.3 16.9 33.7 43.8 51.9

T1/2 [h] 1 4.5 1188 1.7 2.8 4.9 4.2


.g-1

.deuteron-1

]

0.0 580(30) 107.7(13) 69.5(29) 5.3(5) 7.7(5) 1.88(14) 1.80(12)

11.8 950(30) 234.9(28) 140(40) 13.0(5) 22.1(14) 6(3) 6.48(21)

24.0 953(28) 119.6(13) 74.9(16) 6.5(5) 9.3(4) 2.49(19) 2.65(18)


.g-1

.deuteron-1

]

3.0 950(30) 234.9(28) 140(40) 13.0(5) 22.1(14) 6(3) 6.48(21)

6.0 920(40) 117.0(14) 56(4) 5.8(5) 6.06(22) 2.1(6) 1.81(18)

8.5 910(40) 63.7(10) 46.1(25) 3.3(3) 2.90(9) 0.6(4) 0.45(8)

11.5 1110(40) 38.0(8) 39(14) 1.8(3) 1.43(8) - 0.35(8)


EXPERIMENTS

155


experiment.

Foil 181

Ta

Reaction (n,) (n,2n) (n,4n) (n,5n) (n,6n) (n,7n)

Product 182

Ta 180

Ta 178m

Ta 177

Ta 176

Ta 175

Ta

Ethresh [MeV] 0 7.6 22.7 29.2 37.6 44.7

T1/2 [h] 2746 8 2 57 8 11


.g-1

.deuteron-1

]

0.0 190(7) 32.2(22) 2.52(8) 8.9(12) 3.2(4) 1.53(23)

11.8 319(5) 46(3) 4.31(7) 11.4(8) 5.5(5) 3.5(4)

24.0 321(15) 29.7(14) 3.10(14) 21.3(11) 4.0(4) 2.69(23)

36.2 236(13) 16.8(11) 1.87(28) 15.2(12) 2.5(3) 1.82(25)

48.4 108(3) 6.4(6) 0.89(16) 11(3) 0.90(20) 1.0(9)


.g-1

.deuteron-1

]

0.0 164.5(28) 10.1(25) - 318(35) - 0.45(15)

11.8 247(12) 16.8(10) 2.06(7) 22.9(22) 2.3(4) 1.7(4)

24.0 284(6) 9.9(20) - 74.2(28) 2.3(5) 1.3(4)

36.2 224(4) 5.2(19) - 141(6) 1.0(4) 0.83(13)

48.4 100(3) 4.5(12) - 178(29) - 0.42(10)


.g-1

.deuteron-1

]

0.0 175(5) 10.2(20) - - - -

11.8 260(8) 11.1(5) 1.30(4) 21.9(16) 1.50(29) 0.87(8)

24.0 275(6) - - 96(25) 1.14(29) 0.99(13)

36.2 217(5) 4.8(11) - 598(25) 1.0(4) 0.55(20)

48.4 102(3) 4.4(15) - 180(21) 0.59(23) -


.g-1

.deuteron-1

]

0.0 180(4) 6.5(18) - 256(16) - -

11.8 308(81) 9.8(19) 0.91(5) 24.3(11) 1.21(18) 0.80(15)

24.0 274(8) - - 129(5) - 0.44(20)

36.2 231(7) 3.0(10) - 213(9) - 0.46(8)

48.4 149(13) - - 176(13) - -


EXPERIMENTS

156


experiment.

Foil 89

Y

Reaction (n,) (n,2n) (n,3n) (n,4n) (n,5n)

Product 90m

Y 88

Y 87

Y 86

Y 85

Y

Ethresh [MeV] 0 11.6 21.1 33 42.6

T1/2 [h] 3 2568 80 15 3


.g-1

.deuteron-1

]

0.0 0.196(18) 16.7(13) 6.01(13) 2.14(18) 0.44(12)

11.8 0.56(6) 36.8(24) 21.47(12) 6.7(6) 1.6(5)

24.0 0.43(4) 33.4(18) 16.95(27) 6.27(18) 2(2)

36.2 0.213(22) 19.0(20) 10.24(16) 3.99(27) 1.08(9)

48.4 - 6.6(8) 4.69(10) 2.20(18) 0.5(3)


.g-1

.deuteron-1

]

3.0 0.56(6) 36.8(24) 21.47(29) 6.7(6) 1.6(5)

6.0 0.360(24) 21.0(15) 10.91(18) 3.01(27) 0.7(7)

8.5 0.256(21) 12.0(10) 6.36(12) 1.8(3) 0.38(18)

10.7 0.182(23) 8(1) 3.30(9) 1.14(10) 0.196(29)

Note: Data evaluation for the 4 GeV deuteron experiment on E+T setup has not been

finished so far. These data are not a subject of these PhD theses.

157

Appendix G

Graphs with yields of isotopes produced on activation foils in E+T

deuteron experiments

G.1. Longitudinal yields at 3 cm over the target axis

-5 5 15 25 35 45

Yie

ld [

1/(

g*

deu

tero

n)]


198Au 196Au 194Au 192Au 24Na

10-5

10-4

10-3

10-6

10-2


longitudinal direction, 3 cm over the target axis, 2.52 GeV deuteron experiment.

APPENDIX G. GRAPHS WITH YIELDS OF ISOTOPES PRODUCED ON ACTIVATION

FOILS IN „E+T“ DEUTERON EXPERIMENTS

158

-5 5 15 25 35 45

Yie

ld [

1/g

*d

eu

tero

n]


198Au 196Au 194Au 192Au 24Na

10-3

10-4

10-5

10-6

10-2

Preliminary!!


longitudinal direction, 3 cm over the target axis, 4 GeV deuteron experiment, author

D. Wagner.


159

-5 5 15 25 35 45

Yie

ld [1/g

*deute

ron

]


182Ta 180Ta 178mTa 177Ta

176Ta 175Ta 174Ta 173Ta

10-5

10-4

10-3

10-6

10-2

10-7

Figure 104: Yields of the isotopes produced in Ta activation detectors in longitudinal

direction, 3 cm over the target axis, 1.6 GeV deuteron experiment.

-5 5 15 25 35 45

Yie

ld [1/g

*deute

ron]

Position along the the target [cm]

182Ta 180Ta 178mTa 177Ta 176Ta 175Ta 174Ta

10-5

10-4

10-3

10-6

10-2

10-7





160

-5 5 15 25 35 45

Yie

ld [1/g

*deute

ron]


206Bi 205Bi 204Bi 203Bi 202Bi

10-7

10-6

10-5

10-4

Figure 106: Yields of the isotopes produced in Bi activation detectors in longitudinal


-5 5 15 25 35 45

Yie

ld [

1/g

*d

eu

tero

n]


206Bi 205Bi 204Bi 203Bi 202Bi

10-6

10-5

10-4




161

-5 5 15 25 35 45

Yie

ld [

1/g

*deute

ron]


116mIn 115mIn 113mIn 111In 110In 109In

10-7

10-6

10-5

10-4

10-3

10-2

Figure 108: Yields of the isotopes produced in In activation detectors in longitudinal


-5 5 15 25 35 45

Yie

ld [

1/g

*d

eu

tero

n]


115mIn 114mIn 111In 109In

10-6

10-5

10-4

10-3





162

-5 5 15 25 35 45

Yie

ld [1

/g*

deu

tero

n]


90mY 87Y 86Y 85Y

10-7

10-6

10-5

10-4

10-8

Figure 110: Yields of the isotopes produced in Y activation detectors in longitudinal


-5 5 15 25 35 45

Yie

ld [1/g

*deute

ron

]


Y88 Y87 Y86 Y85

10-7

10-6

10-5

10-4



G.2. Radial yields in the first gap

163


2 4 6 8 10 12

Yie

ld [

1/g

*d

eu

tero

n]


198Au 196Au 194Au 193Au 192Au 24Na

10-5

10-4

10-3

10-6

10-2

10-7


direction, first gap of the E+T setup, 2.52 GeV deuteron experiment.

2 4 6 8 10 12

Yie

ld [

1/g

*d

eute

ron

]


198Au 196Au 194Au 192Au 24Na

Preliminary!!

10-3

10-4

10-5

10-6

10-2


direction, first gap of the E+T setup, 4 GeV deuteron experiment, author D. Wagner.



164

2 4 6 8 10 12

Yie

ld [

1/g

*d

eu

tero

n]


182Ta 180Ta 178mTa 177Ta

176Ta 175Ta 174Ta 173Ta

10-5

10-4

10-3

10-6

10-2

10-7

10-8

Figure 114: Yields of the isotopes produced in Ta activation detectors in radial


2 4 6 8 10 12

Yie

ld [1/g

*deute

ron]


182Ta 180Ta 178mTa 177Ta 176Ta 175Ta 173Ta

10-5

10-4

10-3

10-6

10-2

10-7




165

2 4 6 8 10 12

Yie

ld [

1/g

*d

eu

tero

n]


206Bi 205Bi 204Bi 203Bi 202Bi

10-7

10-6

10-5

10-4

Figure 116: Yields of the isotopes produced in Bi activation detectors in radial


2 4 6 8 10 12

Yie

ld [1/g

*deute

ron]


206Bi 205Bi 204Bi 203Bi 202Bi

10-7

10-6

10-5

10-4





166

2 4 6 8 10 12

Yie

ld [

1/g

*d

eu

tero

n]


116mIn 115mIn 113mIn 111In 110In 109In

10-7

10-6

10-2

10-3

10-4

10-5

Figure 118: Yields of the isotopes produced in In activation detectors in radial direction,

first gap of the E+T setup, 1.6 GeV deuteron experiment.

2 4 6 8 10 12

Yie

ld [1/g

*deute

ron]


116mIn 115mIn 114mIn 111In 109In

10-7

10-6

10-5

10-4

10-3

10-2




167

2 4 6 8 10 12

Yie

ld [1/g

*deute

ron]


90mY 87Y 86Y 85Y

10-7

10-6

10-5

10-4

Figure 120: Yields of the isotopes produced in Y activation detectors in radial direction,


2 4 6 8 10 12

Yie

ld [1/g

*deute

ron]


Y88 Y87 Y86 Y85

10-7

10-6

10-5

10-4





168

G.3. Spectral indexes

10.7 cm

8.5 cm

6 cm

3 cm

0.00

0.10

0.20

0.30

0.40

0.50

012

2436

48

Spectr

al in

dex

19

4A

u/1

96A

u[-

]


(ratio between 194

Au and 196

Au).

10.7 cm

8.5 cm

6 cm

3 cm

0

0.1

0.2

0.3

0.4

0.5

0.6

012

2436

48

Sp

ectr

al in

dex

19

4A

u/1

96A

u [

-]

Figure 123: Neutron spectra hardening along the target in 2.52 GeV deuteron

experiment (ratio between 194

Au and 196

Au).

G.3. Spectral indexes

169

10.7 cm

8.5 cm

6 cm

3 cm

0.00

0.10

0.20

0.30

0.40

0.50

0.60

012

2436

48

Sp

ectr

al in

dex

194A

u/1

96A

u [

-]


(ratio between 194

Au and 196

Au).



170

G.4. Ratios of the yield in dependence on the threshold

0

1

2

3

4

5

6

7

0 10 20 30 40 50 60 70

Rati

o in

fro

nt o

f /

beh

ind

targ

et [

-]


Al Au Y Bi In Ta


2.52 GeV deuteron experiment.

0

5

10

15

20

25

30

0 10 20 30 40 50 60

Rati

o 3

/ 1

0.5

cm

[-]


Al

Au

Y

In

Bi

Ta

Figure 126: Ratio in 3cm and 10.7 cm (11.5cm) in the first gap of the target for various

threshold reactions, 2.52 GeV deuteron experiment.

G.5. Comparison between experiments

171


0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

2 4 6 8 10 12

Yie

ld [ -

]



198Au


Au yields in longitudinal direction,

deuterons and 0.7 GeV proton experiment on E+T setup. Data are normalized to the

first foil. Results of the 4 GeV deuteron experiment are preliminary.

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

2 4 6 8 10 12

Yie

ld [

-]



196Au

Figure 128: Comparison of threshold

196Au yields in longitudinal direction, deuterons

and 0.7 GeV proton experiment on E+T setup. Data are normalized to the first foil.

Results of the 4 GeV deuteron experiment are preliminary.



172

-5 5 15 25 35 45 55

Yie

ld [

1/g

*d

(2p

)]


4 GeV 2.52GeV 1.6 GeV 0.7 GeV p

2.10-4

4.10-4

6.10-4

8.10-4

1.10-3

0

198Au

Figure 129: Comparison of non-threshold

198Au yields in longitudinal direction,

deuterons and 0.7 GeV proton experiment on E+T setup, unnormalized values. Results

of the 4 GeV deuteron experiment are preliminary.

-5 5 15 25 35 45 55

Yie

ld [1/g

*d(2

p)]


4 GeV 2.52 GeV d 1.6 GeV d 0.7 GeV p

196Au1·10-4

8·10-5

6·10-5

4·10-5

2·10-5

0

1.2·10-4

1.4·10-4


196Au yields in longitudinal direction, deuterons

and 0.7 GeV proton experiment on E+T setup, unnormalized values. Results of the

4 GeV deuteron experiment are preliminary.


173

2 4 6 8 10 12

Yie

ld [1

/g*

d(2

p)]



198Au

1·10-4

8·10-5

6·10-5

4·10-5

2·10-5

0

Figure 131: Comparison of non-threshold

198Au yields in radial direction, deuterons and

0.7 GeV proton experiment on E+T setup, unnormalized values. Results of the 4 GeV

deuteron experiment are preliminary.

2 4 6 8 10 12

Yie

ld [1/g

*d(2

p)]



196Au

1·10-4

8·10-5

6·10-5

4·10-5

2·10-5

1.2·10-4

0

1.4·10-4


196Au yields in radial direction, deuterons and


deuteron experiment are preliminary.



174

G.6. Ratios of the yields for various deuteron experiments

1.2

1.4

1.6

1.8

2.0

2.2

2.4

2.6

2.8

0 5 10 15 20

Rati

o 4

GeV

/ 1

.6 G

eV

[-]

Number of foil [-]

198Au

Preliminary!!!


Au yields for 4 GeV and 1.6 GeV deuteron experiments in

all twenty Au foils, which were used.

0.8

1.0

1.2

1.4

1.6

1.8

0 5 10 15 20

Rati

o 2

.52

GeV

/ 1

.6 G

eV

[-]

Number of foil [-]

196Au 194Au


Au and 194

Au yields for 2.52 GeV and 1.6 GeV deuteron

experiments in all twenty Au foils, which were used.

G.6. Ratios of the yields for various deuteron experiments

175

2.5

3.0

3.5

4.0

4.5

5.0

5.5

6.0

6.5

0 5 10 15 20

Rati

o 4

GeV

/ 1

.6 G

eV

[-]

Number of foil [-]

196Au 194Au

Preliminary!!!


Au and 194

Au yields for 4 GeV and 1.6 GeV deuteron

experiments in all twenty Au foils, which were used.



176

177

Appendix H

Example of MCNPX input file – Au in 4 GeV deuteron experiment

c CELL CARD for sample problem

c cell number, material number, density, surface numbers

1 1 -11.340 -1 50 -51 $ lead target

2 8 -7.874 2 -3 -4 $ iron - out of the beam tube

c U-rods place 50 0 358 70 -71 105 -100 103 -101 102 -104 fill=1

c lattice with U rods 51 0 203 -202 205 -204 -201 200 lat=2 u=1 trcl=(0 0 0.5) fill=-4:4 -4:4 0:0

3 3 3 3 3 3 3 3 3

3 3 3 3 2 2 2 2 3

3 3 3 2 2 2 2 2 3

3 3 2 2 3 3 2 2 3

3 2 2 3 3 3 2 2 3

3 2 2 3 3 2 2 3 3

3 2 2 2 2 2 3 3 3

3 2 2 2 2 3 3 3 3

3 3 3 3 3 3 3 3 3

100 2 -19.050 -250 252 -253 u=2 $ U rod definition

c aluminum envelope around uranium rods 101 3 -2.7 (250 -251 252 -253):(-251 50 -252):(-251 253 -254)

u=2

102 4 -0.00129 251 u=2 $ the air 103 4 -0.00129 -500 u=3

c vertical iron plate surrounding each blanket section 110 8 -7.874 (350 -351 352 -353 358 70 -354 -401 402 403 -404

(-105:100:-103:101:-102:104)):

(350 -351 352 -353 355 358 -71 -401 402 403 -404

(-105:100:-103:101:-102:104))

c vertical aluminum plate in front and behind the hexagon 120 3 -2.7 (358 -70 50 405 -400 403 -401 402 -404):

(358 -51 71 405 -400 403 -401 402 -404)

c aluminum shielding for lead target 130 3 -2.7 1 -358 50 -51

c iron shielding around uranium rods 140 8 -7.874 (-100 72 101 -451 354 -355):

(-72 105 -102 452 354 -355):

(-105 455 452 453 354 -355):

(-72 105 -103 453 354 -355):

(-100 72 104 -454 354 -355)

c upper iron shielding part around uranium rods 141 8 -7.874 100 -450 -451 -454 354 -355

c air inside target 145 4 -0.00129 (100:-103:101:-102:104:-105)

405 -400 403 -401 402 -404

70 -71 (#110) (#140) (#141)

(#152) (#155) (#202) (#205)

APPENDIX H. EXAMPLE OF MCNPX INPUT FILE

178

(#252) (#255) (#256) (#999)

c next three sections of the target transformed 150 like 1 but trcl=(0 0 12.2)

151 like 50 but trcl=(0 0 12.2)

152 like 110 but trcl=(0 0 12.2)

153 like 120 but trcl=(0 0 12.2)

154 like 130 but trcl=(0 0 12.2)

155 like 140 but trcl=(0 0 12.2)

156 like 145 but trcl=(0 0 12.2)

200 like 1 but trcl=(0 0 24.4)

201 like 50 but trcl=(0 0 24.4)

202 like 110 but trcl=(0 0 24.4)

203 like 120 but trcl=(0 0 24.4)

204 like 130 but trcl=(0 0 24.4)

205 like 140 but trcl=(0 0 24.4)

206 like 145 but trcl=(0 0 24.4)

250 like 1 but trcl=(0 0 36.6)

251 like 50 but trcl=(0 0 36.6)

252 like 110 but trcl=(0 0 36.6)

253 like 120 but trcl=(0 0 36.6)

254 like 130 but trcl=(0 0 36.6)

255 like 140 but trcl=(0 0 36.6)

256 like 141 but trcl=(0 0 36.6)

257 like 145 but trcl=(0 0 36.6)

c cadmium layer 350 6 -8.65 (304:-302:-308:310) (303 -305 309 -311 300 -

301)

c polyethylene shielding box 360 5 -0.802 (300 -301 303 -305 311 -313):

(300 -301 303 -305 312 -309):

(300 -301 305 -307 317 -318):

(300 -301 306 -303 312 -313):

(300 -301 314 -315 -306 316)

361 8 -7.874 58 -59 320 -321 -405 322 $ iron plate

c wooden plate under the blanket 362 9 -0.5 58 -59 320 -321 -322 323

363 9 -0.5 300 -301 308 -310 302 -323 $ textolite plate

c the air everywhere inside the shielding 370 4 -0.00129 300 -301 302 -304 308 -310

(400:401:-402:-403:404:-405:-58:59)

(#361) (#362) (#363)

c the air outside the setup 380 4 -0.00129 (-306:307:-300:301:-312:313) (#2) (#360) -

500

c Al detector part 301 3 -2.7 -90

302 like 301 but trcl=(0 3 0)

303 like 301 but trcl=(0 5.5 0)

304 like 301 but trcl=(0 7.7 0)

305 like 301 but trcl=(0 0 12.2)

306 like 301 but trcl=(0 3 12.2)

307 like 301 but trcl=(0 5.5 12.2)

308 like 301 but trcl=(0 7.7 12.2)


179

309 like 301 but trcl=(0 0 24.4)

310 like 301 but trcl=(0 3 24.4)

311 like 301 but trcl=(0 5.5 24.4)

312 like 301 but trcl=(0 7.7 24.4)

313 like 301 but trcl=(0 0 36.6)

314 like 301 but trcl=(0 3 36.6)

315 like 301 but trcl=(0 5.5 36.6)

316 like 301 but trcl=(0 7.7 36.6)

317 like 301 but trcl=(0 0 48.8)

318 like 301 but trcl=(0 3 48.8)

319 like 301 but trcl=(0 5.5 48.8)

320 like 301 but trcl=(0 7.7 48.8)

c Au detector part 401 10 -19.3 -80

402 like 401 but trcl=(0 3 0)

403 like 401 but trcl=(0 5.5 0)

404 like 401 but trcl=(0 7.7 0)

405 like 401 but trcl=(0 0 12.2)

406 like 401 but trcl=(0 3 12.2)

407 like 401 but trcl=(0 5.5 12.2)

408 like 401 but trcl=(0 7.7 12.2)

409 like 401 but trcl=(0 0 24.4)

410 like 401 but trcl=(0 3 24.4)

411 like 401 but trcl=(0 5.5 24.4)

412 like 401 but trcl=(0 7.7 24.4)

413 like 401 but trcl=(0 0 36.6)

414 like 401 but trcl=(0 3 36.6)

415 like 401 but trcl=(0 5.5 36.6)

416 like 401 but trcl=(0 7.7 36.6)

417 like 401 but trcl=(0 0 48.8)

418 like 401 but trcl=(0 3 48.8)

419 like 401 but trcl=(0 5.5 48.8)

420 like 401 but trcl=(0 7.7 48.8)

c detectors of tantal 501 11 -16.65 -81

502 like 501 but trcl=(0 3 0)

503 like 501 but trcl=(0 5.5 0)

504 like 501 but trcl=(0 7.7 0)

505 like 501 but trcl=(0 0 12.2)

506 like 501 but trcl=(0 3 12.2)

507 like 501 but trcl=(0 5.5 12.2)

508 like 501 but trcl=(0 7.7 12.2)

509 like 501 but trcl=(0 0 24.4)

510 like 501 but trcl=(0 3 24.4)

511 like 501 but trcl=(0 5.5 24.4)

512 like 501 but trcl=(0 7.7 24.4)

513 like 501 but trcl=(0 0 36.6)

514 like 501 but trcl=(0 3 36.6)

515 like 501 but trcl=(0 5.5 36.6)

516 like 501 but trcl=(0 7.7 36.6)

517 like 501 but trcl=(0 0 48.8)

518 like 501 but trcl=(0 3 48.8)

519 like 501 but trcl=(0 5.5 48.8)

520 like 501 but trcl=(0 7.7 48.8)


180

c detectors of bismuth 601 12 -9.78 -82

602 like 601 but trcl=(0 0 12.2)

603 like 601 but trcl=(2.5981 -1.5 12.2)

604 like 601 but trcl=(4.8064 -2.775 12.2)

605 like 601 but trcl=(7.3612 -4.25 12.2)

606 like 601 but trcl=(0 0 24.4)

607 like 601 but trcl=(0 0 36.6)

608 like 601 but trcl=(0 0 48.8)

c detectors of indium 701 13 -7.31 -83

702 like 701 but trcl=(0 0 12.2)

703 like 701 but trcl=(2.5981 -1.5 12.2)

704 like 701 but trcl=(4.8064 -2.775 12.2)

705 like 701 but trcl=(7.3612 -4.25 12.2)

706 like 701 but trcl=(0 0 24.4)

707 like 701 but trcl=(0 0 36.6)

708 like 701 but trcl=(0 0 48.8)

c yttrium detectors - Poland 801 14 -4.472 -84

802 like 801 but trcl=(-1.5 2.5981 0)

803 like 801 but trcl=(-3 5.19615 0)

804 like 801 but trcl=(-4.25 7.36122 0)

805 like 801 but trcl=(-5.25 9.09327 0)

806 like 801 but trcl=(-6.75 11.6913 0)

807 like 801 but trcl=(0 0 12.2)

808 like 801 but trcl=(-1.5 2.5981 12.2)

809 like 801 but trcl=(-3 5.19615 12.2)

810 like 801 but trcl=(-4.25 7.36122 12.2)

811 like 801 but trcl=(-5.25 9.09327 12.2)

812 like 801 but trcl=(-6.75 11.6913 12.2)

813 like 801 but trcl=(0 0 24.4)

814 like 801 but trcl=(-1.5 2.5981 24.4)

815 like 801 but trcl=(-3 5.19615 24.4)

816 like 801 but trcl=(-4.25 7.36122 24.4)

817 like 801 but trcl=(-5.25 9.09327 24.4)

818 like 801 but trcl=(-6.75 11.6913 24.4)

819 like 801 but trcl=(0 0 36.6)

820 like 801 but trcl=(-1.5 2.5981 36.6)

821 like 801 but trcl=(-3 5.19615 36.6)

822 like 801 but trcl=(-4.25 7.36122 36.6)

823 like 801 but trcl=(-5.25 9.09327 36.6)

824 like 801 but trcl=(-6.75 11.6913 36.6)

825 like 801 but trcl=(0 0 48.8)

826 like 801 but trcl=(-1.5 2.5981 48.8)

827 like 801 but trcl=(-3 5.19615 48.8)

828 like 801 but trcl=(-4.25 7.36122 48.8)

829 like 801 but trcl=(-5.25 9.09327 48.8)

830 like 801 but trcl=(-6.75 11.6913 48.8)

c detectors of cobalt 901 18 -8.8 -91

902 like 901 but trcl=(0 0 12.2)

903 like 901 but trcl=(2.5981 -1.5 12.2)

904 like 901 but trcl=(4.8064 -2.775 12.2)


181

905 like 901 but trcl=(7.3612 -4.25 12.2)

906 like 901 but trcl=(0 0 24.4)

907 like 901 but trcl=(0 0 36.6)

908 like 901 but trcl=(0 0 48.8)

c gaps between the target-blanket sections 5000 4 -0.00129 -400 -401 402 403 -404 405 58 -50

#301 #302 #303 #304 #401 #402 #403 #404

#501 #502 #503 #504 #601 #701 #801 #802

#803 #804 #805 #806 #901

5001 4 -0.00129 -400 -401 402 403 -404 405 51 -52

#305 #306 #307 #308 #405 #406 #407 #408

#505 #506 #507 #508 #602 #603 #604 #605

#702 #703 #704 #705 #807 #808 #809 #810

#811 #812 #902 #903 #904 #905

5002 4 -0.00129 -400 -401 402 403 -404 405 53 -54

#309 #310 #311 #312 #409 #410 #411 #412

#509 #510 #511 #512 #606 #706 #813 #814

#815 #816 #817 #818 #906

5003 4 -0.00129 -400 -401 402 403 -404 405 55 -56

#313 #314 #315 #316 #413 #414 #415 #416

#513 #514 #515 #516 #607 #707 #819 #820

#821 #822 #823 #824 #907

5004 4 -0.00129 -400 -401 402 403 -404 405 57 -59

#317 #318 #319 #320 #417 #418 #419 #420

#517 #518 #519 #520 #608 #708 #825 #826

#827 #828 #829 #830 #908

c nothing in the surrounding of the whole setup 10000 0 500

c SURFACE CARD

1 cz 4.2 $ target cylinder with diameter 4.2 cm

2 pz -100.5 $ planes for iron at the out of the beam tube 3 pz -100

4 cz 15

50 pz 0 $ z planes, for target and detectors 51 pz 11.4

52 pz 12.2

53 pz 23.6

54 pz 24.4

55 pz 35.8

56 pz 36.6

57 pz 48

58 pz -1.25

59 pz 49.25

70 pz 0.5

71 pz 10.9

72 py 0

79 pz 11.8

80 rpp -1 1 2 4 -0.4 -0.395 $ detectors - Au

81 rpp -1 1 2 4 -0.395 -0.385 $ detectors - Ta 82 box 0.8905 -1.9575 -0.4 2.165 -1.25 0 1.25 2.165 0 0 0 0.1

83 box 1.5736 -1.7745 -0.3 1.299 -0.75 0 0.75 1.299 0 0 0 0.05

84 rcc 0 0 -0.7 0 0 0.1 0.5


182

85 rpp -7.2 7.2 11.6 13.1 16.1 19.7

86 px -3.6

87 px 0

88 px 3.6

89 rcc 0 0 -0.6 0 0 0.1 0.5

90 rpp -1 1 2 4 -0.5 -0.4 $ detectors - Al 91 box 1.5736 -1.7745 -0.2 1.299 -0.75 0 0.75 1.299 0 0 0

0.1

100 py 11.20 $ big hexagon for fill with lattice 101 p 1 0.57735 0 12.93265

102 p -1 0.57735 0 -12.93265

103 p 1 0.57735 0 -12.93265

104 p -1 0.57735 0 12.93265

105 py -11.2

200 px -1.807573351 $ small hexagon, for the lattice definition 201 px 1.807573351

202 p 0.577350269 -1 0 2.087205922

203 p 0.577350269 -1 0 -2.087205922

204 p -0.577350269 -1 0 2.087205922

205 p -0.577350269 -1 0 -2.087205922

250 cz 1.6881 $ definition of U rod inside the lattice 251 cz 1.8

252 pz 0.1119

253 pz 10.2881

254 pz 10.4

300 pz -30 $ polyethylene box, Cd layer 301 pz 76

302 py -25

303 py -25.1

304 py 25

305 py 25.1

306 py -41.5

307 py 47.1

308 px -19.9

309 px -20

310 px 19.9

311 px 20

312 px -50

313 px 50

314 px -37.8 $ further polyethylene box, detail bottom, top 315 px 37.8

316 py -63.1

317 px -55

318 px 55

320 px -18.1 $ wooden and iron plate under the target 321 px 18.1

322 py -14.4

323 py -21.2

350 px -13 $ details on setup iron plates 351 px 13

352 py -13

353 py 13

354 pz 0.9


183

355 pz 10.5

358 cz 4.4

400 py 14 $ hexagon in front of the target 401 p 1 0.57735 0 16.16581

402 p -1 0.57735 0 -16.16581

403 p 1 0.57735 0 -16.16581

404 p -1 0.57735 0 16.16581

405 py -14

450 py 11.6 $ planes for iron hexagon around U rods 451 p 1 0.57735 0 13.39453

452 p -1 0.57735 0 -13.39453

453 p 1 0.57735 0 -13.39453

454 p -1 0.57735 0 13.39453

455 py -11.6

500 so 130

c DATA CARD

mode n h p / d $ neutrons, protons, photons, charged pions, deuterons

imp:n,h,p,/,d 1 162r 0 $particles are important in all cells

c material definition – number of material, isotope - composition

m1 82204 1.4 82206 24.1 82207 22.1 82208 52.4 & $ lead hlib=24h nlib=24c cond=1

m2 92238 99.2745 92235 0.72 92234 0.005 cond=1 $ uranium

m3 13027 1 hlib=24h nlib=24c cond=1

m4 7000 -0.755 & $ air 8000 -0.232 &

18000 -0.013 &

hlib=24h nlib=24c plib=02p cond=0

m5 6012 1 1001 2 nlib=60c cond=0 $ polyethylene mt5 poly.01t

m6 48000 1 cond=1 $ cadmium

m8 26058 0.282 26057 2.119 26056 91.754 26054 5.845 nlib=24c

hlib=24h cond=1 $ aluminum

m9 1001 0.513066 1002 0.000080 6000 0.230081 8016 0.256773 &

nlib=60c plib=02p cond=0

m10 79197 1 $ gold

m11 73181 1 $ tantalum

m12 83209 1 $ bismuth

m13 49115.00c 1 $ indium

m14 39089 1 $ yttrium

m18 27059 1 $ cobalt

c physics options – maximal energy and usage of library or model phys:n 4000 3j -1

phys:h 4000 j -1

phys:p 4000

phys:/ 4000

phys:d 4000

c calculation of yield of the 197

Au(n,gamma)198

Au reaction f4:n 401

fm4 0.0030574 10 102

f14:n 402

fm14 0.0030574 10 102


184

f24:n 403

fm24 0.0030574 10 102

f34:n 404

fm34 0.0030574 10 102

f44:n 405

fm44 0.0030574 10 102

f54:n 406

fm54 0.0030574 10 102

f64:n 407

fm64 0.0030574 10 102

f74:n 408

fm74 0.0030574 10 102

f84:n 409

fm84 0.0030574 10 102

f94:n 410

fm94 0.0030574 10 102

f104:n 411

fm104 0.0030574 10 102

f114:n 412

fm114 0.0030574 10 102

f124:n 413

fm124 0.0030574 10 102

f134:n 414

fm134 0.0030574 10 102

f144:n 415

fm144 0.0030574 10 102

f154:n 416

fm154 0.0030574 10 102

f164:n 417

fm164 0.0030574 10 102

f174:n 418

fm174 0.0030574 10 102

f184:n 419

fm184 0.0030574 10 102

f194:n 420

fm194 0.0030574 10 102

c spectra calculation for convolution

c neutron spectra in gold f1204:n 401

e1204 1 148i 150 175 200 75i 4000

f1214:n 402

e1214 1 148i 150 175 200 75i 4000

f1224:n 403

e1224 1 148i 150 175 200 75i 4000

f1234:n 404

e1234 1 148i 150 175 200 75i 4000

f1244:n 405

e1244 1 148i 150 175 200 75i 4000

f1254:n 406

e1254 1 148i 150 175 200 75i 4000

f1264:n 407

e1264 1 148i 150 175 200 75i 4000

f1274:n 408

e1274 1 148i 150 175 200 75i 4000


185

f1284:n 409

e1284 1 148i 150 175 200 75i 4000

f1294:n 410

e1294 1 148i 150 175 200 75i 4000

f1304:n 411

e1304 1 148i 150 175 200 75i 4000

f1314:n 412

e1314 1 148i 150 175 200 75i 4000

f1324:n 413

e1324 1 148i 150 175 200 75i 4000

f1334:n 414

e1334 1 148i 150 175 200 75i 4000

f1344:n 415

e1344 1 148i 150 175 200 75i 4000

f1354:n 416

e1354 1 148i 150 175 200 75i 4000

f1364:n 417

e1364 1 148i 150 175 200 75i 4000

f1374:n 418

e1374 1 148i 150 175 200 75i 4000

f1384:n 419

e1384 1 148i 150 175 200 75i 4000

f1394:n 420

e1394 1 148i 150 175 200 75i 4000

c proton spectra in gold f2334:h 401

e2334 1 148i 150 175 200 75i 4000

f2344:h 402

e2344 1 148i 150 175 200 75i 4000

f2354:h 403

e2354 1 148i 150 175 200 75i 4000

f2364:h 404

e2364 1 148i 150 175 200 75i 4000

f2374:h 405

e2374 1 148i 150 175 200 75i 4000

f2384:h 406

e2384 1 148i 150 175 200 75i 4000

f2394:h 407

e2394 1 148i 150 175 200 75i 4000

f2404:h 408

e2404 1 148i 150 175 200 75i 4000

f2414:h 409

e2414 1 148i 150 175 200 75i 4000

f2424:h 410

e2424 1 148i 150 175 200 75i 4000

f2434:h 411

e2434 1 148i 150 175 200 75i 4000

f2444:h 412

e2444 1 148i 150 175 200 75i 4000

f2454:h 413

e2454 1 148i 150 175 200 75i 4000

f2464:h 414

e2464 1 148i 150 175 200 75i 4000

f2474:h 415


186

e2474 1 148i 150 175 200 75i 4000

f2484:h 416

e2484 1 148i 150 175 200 75i 4000

f2494:h 417

e2494 1 148i 150 175 200 75i 4000

f2504:h 418

e2504 1 148i 150 175 200 75i 4000

f2514:h 419

e2514 1 148i 150 175 200 75i 4000

f2524:h 420

e2524 1 148i 150 175 200 75i 4000

c pion spectra in gold f3484:/ 401

e3484 1 148i 150 175 200 75i 4000

f3494:/ 402

e3494 1 148i 150 175 200 75i 4000

f3504:/ 403

e3504 1 148i 150 175 200 75i 4000

f3514:/ 404

e3514 1 148i 150 175 200 75i 4000

f3524:/ 405

e3524 1 148i 150 175 200 75i 4000

f3534:/ 406

e3534 1 148i 150 175 200 75i 4000

f3544:/ 407

e3544 1 148i 150 175 200 75i 4000

f3554:/ 408

e3554 1 148i 150 175 200 75i 4000

f3564:/ 409

e3564 1 148i 150 175 200 75i 4000

f3574:/ 410

e3574 1 148i 150 175 200 75i 4000

f3584:/ 411

e3584 1 148i 150 175 200 75i 4000

f3594:/ 412

e3594 1 148i 150 175 200 75i 4000

f3604:/ 413

e3604 1 148i 150 175 200 75i 4000

f3614:/ 414

e3614 1 148i 150 175 200 75i 4000

f3624:/ 415

e3624 1 148i 150 175 200 75i 4000

f3634:/ 416

e3634 1 148i 150 175 200 75i 4000

f3644:/ 417

e3644 1 148i 150 175 200 75i 4000

f3654:/ 418

e3654 1 148i 150 175 200 75i 4000

f3664:/ 419

e3664 1 148i 150 175 200 75i 4000

f3674:/ 420

e3674 1 148i 150 175 200 75i 4000

c deuteron spectra in gold f4714:d 401


187

e4714 1 148i 150 175 200 75i 4000

f4724:d 402

e4724 1 148i 150 175 200 75i 4000

f4734:d 403

e4734 1 148i 150 175 200 75i 4000

f4744:d 404

e4744 1 148i 150 175 200 75i 4000

f4754:d 405

e4754 1 148i 150 175 200 75i 4000

f4764:d 406

e4764 1 148i 150 175 200 75i 4000

f4774:d 407

e4774 1 148i 150 175 200 75i 4000

f4784:d 408

e4784 1 148i 150 175 200 75i 4000

f4794:d 409

e4794 1 148i 150 175 200 75i 4000

f4804:d 410

e4804 1 148i 150 175 200 75i 4000

f4814:d 411

e4814 1 148i 150 175 200 75i 4000

f4824:d 412

e4824 1 148i 150 175 200 75i 4000

f4834:d 413

e4834 1 148i 150 175 200 75i 4000

f4844:d 414

e4844 1 148i 150 175 200 75i 4000

f4854:d 415

e4854 1 148i 150 175 200 75i 4000

f4864:d 416

e4864 1 148i 150 175 200 75i 4000

f4874:d 417

e4874 1 148i 150 175 200 75i 4000

f4884:d 418

e4884 1 148i 150 175 200 75i 4000

f4894:d 419

e4894 1 148i 150 175 200 75i 4000

f4904:d 420

e4904 1 148i 150 175 200 75i 4000

lca 6j 1 j 2 $ INCL4 model with npdik=1 (pion decay)

lea 6j 2 $ ABLA model

stop nps 1e7 $ number of calculated events

prdmp -1440 -360 0 j 1e5 $ setting of the data written in output file

c source definition – 4 GeV deuteron beam parallel with the z-axis, preset profile sdef erg 4000. dir 1 vec 0. 0. 1. x=d1 y=d2 z=-100.5 par=d

si1 a -0.65 -0.15 0.35 0.85 1.35 1.85 2.35 2.85 3.35 3.85 4.35

4.85 5.35

si2 a -1.6 -1.1 -0.6 -0.1 0.4 0.9 1.4 1.9 2.4 2.9 3.4 3.9 4.4

4.9 5.4

sp1 0 7 105 826 3593 8682 11650 8682 3593 826 105 7 0

sp2 0 4 44 330 1592 4895 9602 12020 9602 4895 1592 330 44 4 0


188

189

Appendix I

Results of MCNPX simulations

I.1. Deuteron and proton spectra

Deu

tero

nfl

ux·E

[deu

tero

n-1

.cm

-2.M

eV-1

]

Deuteron energy [MeV]

1 10 102 103 104

10-2

10-4

10-6

10-8

10-10

Figure 136: Deuteron flux (multiplied by energy because of binning) in the first target

cylinder of whole E+T setup, log-log scale, beam energy 2.52 GeV. Zero points cannot

be depicted in logarithmic scale. Uncertainties are on the level of one percent for most

of the points.

Pro

ton

flux·E

[deu

tero

n-1

.cm

-2.M

eV-1

]

Proton energy [MeV]

101 102 103 1041

2.10-4

4.10-4

6.10-4

8.10-4

1.10-3

0

Figure 137: Proton flux (multiplied by energy because of binning) in the first target

cylinder of whole E+T setup. Deuteron beam energy is 2.52 GeV.

APPENDIX I. RESULTS OF MCNPX SIMULATIONS

190

I.2. Experiment/simulation ratios

0.0

0.5

1.0

1.5

2.0

2.5

-5 5 15 25 35 45

Exp. yie

ld / s

im. yie

ld [

-]


198Au 196Au 194Au 192Au 24Na


1.6 GeV deuteron experiment, Au and Al samples at 3 cm from the target axis.

0.0

0.5

1.0

1.5

2.0

2.5

2 4 6 8 10 12

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 192Au 24Na


deuteron experiment, Au and Al samples in the first gap of the setup.

I.2. Experiment/simulation ratios

191

0.0

0.5

1.0

1.5

2.0

2.5

-5 5 15 25 35 45 55

Ex

p. yie

ld /

sim

. yie

ld [

-]


198Au 196Au 194Au 192Au 24Na


4 GeV deuteron experiment, Au and Al samples at 3 cm from the target axis.

0.0

0.5

1.0

1.5

2.0

2.5

2 4 6 8 10 12

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 192Au 24Na

Figure 141: Ratio between experiment and simulation in radial direction for 4 GeV

deuteron experiment, Au and Al samples in the first gap of the setup.


192

I.3. Normalized experiment/simulation ratios

0.5

0.75

1

1.25

1.5

1.75

-5 5 15 25 35 45

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 192Au 24Na



are normalized to the second foil.

0.5

0.75

1

1.25

1.5

1.75

2 4 6 8 10 12

Ex

p. y

ield

/ s

im y

ield

[-]


198Au 196Au 194Au 192Au 24Na


deuteron experiment, Au and Al samples in the first gap of the setup. Ratios are

normalized to the first foil.

I.3. Normalized experiment/simulation ratios

193

0.5

0.75

1

1.25

1.5

1.75

-5 5 15 25 35 45

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 24Na

Figure 144: Ratio between experiment and simulation in longitudinal direction 10.7 cm

from the target axis, 2.52 GeV deuteron experiment, Au and Al samples at 3 cm from

the target axis. Ratios are normalized to the second foil.

0.5

0.75

1

1.25

1.5

1.75

2 4 6 8 10 12

Ex

p. y

ield

/ s

im.y

ield

[-]


198Au 196Au 194Au 24Na

Figure 145: Ratio between experiment and simulation in radial direction behind the

target, 2.52 GeV deuteron experiment, Au and Al samples in the first gap of the setup.

Ratios are normalized to the second foil.


194

0.5

0.75

1

1.25

1.5

1.75

-5 5 15 25 35 45

Ex

p. y

ield

/ s

im.

yie

ld [

-]


198Au 196Au 194Au 192Au 24Na

Preliminary!!


4 GeV deuteron experiment, Au and Al samples at 3 cm from the target axis. Ratios are

normalized to the second foil.

0.5

0.75

1

1.25

1.5

1.75

2 4 6 8 10 12

Exp. yie

ld /

sim

. yie

ld [-

]


198Au 196Au 194Au 192Au 24Na

Preliminary!!



normalized to the first foil.

195

Appendix J

Cross-sections of threshold reactions from EXFOR and TALYS

compared with my data

0.00

0.02

0.04

0.06

0.08

0.10

0.12

0.14

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


EXFOR

NPI experiments

TSL experiments

TALYS 1.0

27Al(n,p)27Mg

Figure 148: Cross-section values of the

27Al(n,p)

27Mg reaction, comparison among


and [131] - [137].

0

0.2

0.4

0.6

0.8

1

1.2

1.4

1.6

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


197Au(n,4n)194Au

EXFOR

NPI experiments

TSL experiments

TALYS 1.0


Au(n,4n)194


EXFOR, TALYS 1.0 and my values. EXFOR entries are [117], [138], and [139].

APPENDIX J. CROSS-SECTIONS OF THRESHOLD REACTIONS FROM EXFOR AND

TALYS COMPARED TO MY DATA

196

0.0

0.2

0.4

0.6

0.8

1.0

1.2

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


NPI experiment

TSL experiment

TALYS 1.0

197Au(n,5n)193Au


Au(n,5n)193

Au reaction, comparison between

TALYS 1.0 and my values (no EXFOR values exist).

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TALYS

TSL experiment

197Au(n,6n)192Au


Au(n,6n)192





197

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiments

TALYS 1.0

197Au(n,7n)191Au


Au(n,7n)191



0.0

0.1

0.2

0.3

0.4

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiments

TALYS 1.0

197Au(n,8n)190Au


Au(n,8n)190





198

0

0.3

0.6

0.9

1.2

1.5

1.8

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


209Bi(n,3n)207Bi

EXFOR

NPI experiments

TALYS 1.0


Bi(n,3n)207

Bi reaction, comparison among

EXFOR, TALYS 1.0 and my values. EXFOR entries are [86], [115], and [140] - [143].

0

0.3

0.6

0.9

1.2

1.5

1.8

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


209Bi(n,4n)206Bi

EXFOR

NPI experiments

TSL experiments

TALYS 1.0


Bi(n,4n)206


EXFOR, TALYS 1.0 and my values. EXFOR entry is [86].



199

0

0.2

0.4

0.6

0.8

1

1.2

1.4

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


209Bi(n,5n)205Bi

EXFOR

NPI experiments

TSL experiments

TALYS 1.0


Bi(n,5n)205



0

0.2

0.4

0.6

0.8

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


209Bi(n,6n)204Bi

EXFOR

TSL experiments

TALYS 1.0


Bi(n,6n)204





200

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


EXFOR

TSL experiments

TALYS 1.0

209Bi(n,7n)203Bi


209Bi(n,7n)

203Bi reaction, comparison among


0.0

0.1

0.2

0.3

0.4

0.5

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


EXFOR

TSL experiments

TALYS 1.0

209Bi(n,8n)202Bi


Bi(n,8n)202





201

0.00

0.05

0.10

0.15

0.20

0.25

0.30

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


EXFOR

TSL experiment

TALYS 1.0

209Bi(n,10n)200Bi


Bi(n,10n)200



0

0.5

1

1.5

2

2.5

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


181Ta(n,2n)180Ta

EXFOR

NPI experiments

TSL experiments

TALYS 1.0


Ta(n,2n)180

Ta reaction, comparison among

EXFOR, TALYS 1.0 and my values. EXFOR entries are [126] and [143] - [147].



202

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


NPI experiments

TSL experiments

181Ta(n,4n)178mTa


Ta(n,4n)178m

Ta reaction (no EXFOR values

exist, TALYS 1.0 cannot calculate this isomer).

0.0

0.2

0.4

0.6

0.8

1.0

1.2

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


NPI experiments

TSL experiments

TALYS 1.0

181Ta(n,5n)177Ta


Ta(n,5n)177

Ta reaction, comparison between




203

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiments

TALYS 1.0

181Ta(n,6n)176Ta


Ta(n,6n)176



0.00

0.25

0.50

0.75

1.00

1.25

1.50

1.75

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


NPI experiments

TSL experiments

TALYS 1.0

natIn(n,xn)114mIn

Figure 165: Cross-section values of the nat

In(n,xn)114m

In reaction, comparison between

TALYS 1.0 and my values.



204

0.00

0.25

0.50

0.75

1.00

1.25

1.50

1.75

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


EXFOR

NPI experiments

TSL experiments

TALYS 1.0

115In(n,2n)114mIn


In(n,xn)114m

In reaction, comparison among

EXFOR, TALYS 1.0 and my values. Last 10 EXFOR entries are [115] and [148] -

[156].

0.00

0.02

0.04

0.06

0.08

0.10

0.12

0.14

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


NPI experiments

TSL experiments

TALYS 1.0

natIn(n,xn)113mIn


In(n,xn)113m





205

0.00

0.10

0.20

0.30

0.40

0.50

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


NPI experiments

TSL experiments

TALYS 1.0

natIn(n,xn)112mIn


In(n,xn)112m



0.00

0.05

0.10

0.15

0.20

0.25

0.30

0.35

0.40

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


NPI experiments

TSL experiments

TALYS 1.0

natIn(n,xn)111In


In(n,xn)111





206

0.00

0.02

0.04

0.06

0.08

0.10

0.12

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


NPI experiments

TSL experiments

TALYS 1.0

natIn(n,xn)110In


In(n,xn)110



0.00

0.01

0.02

0.03

0.04

0.05

0.06

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiments

TALYS 1.0

natIn(n,xn)109In


In(n,xn)109





207

0.000

0.004

0.008

0.012

0.016

0.020

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiments

TALYS 1.0

natIn(n,xn)108In


In(n,xn)108



0

0.4

0.8

1.2

1.6

2

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


127I(n,2n)126I

EXFOR

NPI experiments

TSL experiments

TALYS 1.0


I(n,2n)126

I reaction, comparison among

EXFOR, TALYS 1.0 and my values. Last 10 EXFOR entries are [157] - [166].



208

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiment

NPI experiments

TALYS 1.0

127I(n,4n)124I


I(n,4n)124

I reaction, comparison between


0.00

0.04

0.08

0.12

0.16

0.20

0.24

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiment

TALYS 1.0

127I(n,7n)121I


I(n,7n)121





209

0.00

0.02

0.04

0.06

0.08

0.10

0.12

0.14

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


TSL experiments

TALYS 1.0

127I(n,8n)120I


I(n,8n)120



0.000

0.005

0.010

0.015

0.020

0.025

0.030

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


TSL experiment

TALYS 1.0

127I(n,9n)119I


I(n,9n)119





210

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


64Zn(n,2n)63Zn

EXFOR

NPI experiments

TALYS


64Zn(n,2n)

63Zn reaction, comparison among


and [167] - [172].

211

Appendix K

Comparison between TALYS 1.0 and TALYS 1.2

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

1.6

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


Talys 1.0

Talys 1.2

EXFOR

EAF

197Au(n,4n)194Au

Figure 179: Comparison of cross-section of

197Au(n,4n)

194Au reaction calculated in

TALYS 1.0 and TALYS 1.2 (both in basic setting). EXFOR and EAF data are included.

0.0

0.2

0.4

0.6

0.8

1.0

1.2

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

bar

n]


Talys 1.0

Talys 1.2

EAF

197Au(n,5n)193Au

Figure 180: Comparison of cross-section of

197Au(n,5n)

193Au reaction calculated in

TALYS 1.0 and TALYS 1.2 (both in basic setting). EAF is included, no EXFOR data

are available.

APPENDIX K. COMPARISON BETWEEN TALYS 1.0 AND TALYS 1.2

212

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


Talys 1.0

Talys 1.2

EAF

197Au(n,6n)192Au

Figure 181: Comparison of cross-section of 197

Au(n,6n)192

Au reaction calculated in


are available.

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on [

barn

]


Talys 1.2

Talys 1.0

197Au(n,7n)191Au


Au(n,7n)191


TALYS 1.0 and TALYS 1.2 (both in basic setting). No EXFOR and EAF data are

available.


213

0.0

0.1

0.1

0.2

0.2

0.3

0 10 20 30 40 50 60 70 80 90 100

Cro

ss-s

ecti

on

[b

arn

]


Talys 1.2

Talys 1.0

197Au(n,10n)188Au


Au(n,10n)188



available.


214

215

Appendix L

Measured cross-section values Table 40 – part one: Cross-section values already published at ND2010 conference.

Uncertainties are total (include all known partial uncertainties)

Energy Cross-section Cross-section uncertainty Energy uncertainty

[MeV] [barn] [barn] [MeV] 197

Au(n,2n)196

Au

17.5 1.64 0.18 0.75

21.88 0.67 0.08 0.75

22 0.56 0.08 0.5

30.375 0.33 0.04 0.75

35.875 0.28 0.03 0.8

47 0.24 0.03 0.55

94 0.124 0.018 0.65 197

Au(n,4n)194

Au

21.88 0.00133 0.00018 1.5

30.375 1.04 0.13 0.75

35.875 1.44 0.16 0.8

94 0.165 0.026 0.65 197

Au(n,5n)193

Au

35.875 0.0085 0.0022 0.8

47 0.7 0.4 0.55

94 0.158 0.027 0.65 197

Au(n,6n)192

Au

47 0.114 0.017 0.55

94 0.168 0.024 0.65 127

I(n,4n)124

I

30.375 0.053 0.006 0.75

35.875 0.37 0.05 0.8

47 1.09 0.16 0.55

94 0.21 0.03 0.65 181

Ta(n,2n)180

Ta

17.5 0.76 0.09 0.75

21.88 0.35 0.04 0.75

22 0.33 0.07 0.5

47 0.19 0.05 0.55

94 0.27 0.12 0.65

APPENDIX L. MEASURED CROSS-SECTION VALUES

216

Table 40 – part two:



Al(n,)24

Na

17.5 0.066 0.007 0.75

21.88 0.0197 0.0022 0.75

30.375 0.0112 0.0013 0.75

35.875 0.0086 0.001 0.8

47 0.0129 0.0019 0.55

94 0.019 0.003 0.65 27

Al(n,p)27

Mg

17.5 0.0261 0.0029 0.75

21.88 0.0142 0.0017 0.75

22 0.0123 0.0024 0.5

30.375 0.0125 0.0014 0.75

35.875 0.0083 0.0009 0.8

47 0.0033 0.0005 0.55

94 0.0009 0.00022 0.65 209

Bi(n,3n)207

Bi

17.5 0.26 0.029 0.75

30.375 0.79 0.1547 0.75

35.875 0.49 0.108 0.8 209

Bi(n,4n)206

Bi

21.88 0.000064 0.000012 1.5

30.375 0.98 0.11 0.75

35.875 1.16 0.13 0.8

47 0.35 0.05 0.55

94 0.148 0.021 0.65 209

Bi(n,5n)205

Bi

35.875 0.036 0.005 0.8

47 1.13 0.16 0.55

94 0.21 0.03 0.65 209

Bi(n,6n)204

Bi

47 0.171 0.025 0.55

94 0.127 0.019 0.65 209

Bi(n,7n)203

Bi

94 0.148 0.021 0.65 209

Bi(n,8n)202

Bi

94 0.147 0.023 0.65 209

Bi(n,10n)200

Bi

94 0.055 0.009 0.65


217

Table 40 – part three:


[MeV] [barn] [barn] [MeV] nat

In(n,xn)114m

In

17.5 1.09 0.15 0.75

30.375 0.38 0.07 0.75

35.875 0.31 0.04 0.8

94 0.14 0.05 0.65

Table 41 – part 1: Up to now unpublished cross-section values shown in figures in

Appendix J



Al(n,)24

Na

22 0.0135 0.0028 0.5 197

Au(n,7n)191

Au

94 0.142 0.029 0.65 197

Au(n,8n)190

Au

94 0.085 0.014 0.65 209

Bi(n,4n)206

Bi

22 0.17 0.07 0.5 181

Ta(n,4n)178m

Ta

21.88 0.0003 0.00004 1.5

35.875 0.69 0.08 0.8

47 0.155 0.023 0.55

94 0.060 0.009 0.65 181

Ta(n,5n)177

Ta

35.875 0.108 0.013 0.8

47 0.86 0.22 0.55 181

Ta(n,6n)176

Ta

47 0.21 0.04 0.55

94 0.143 0.024 0.65 115

In(n,2n)114m

In

17.5 1.14 0.17 0.75

30.375 0.4 0.07 0.75

35.875 0.32 0.05 0.8

94 0.15 0.05 0.65 64

Zn(n,2n)63

Zn

17.5 0.251 0.029 0.75

30.375 0.177 0.021 0.75

35.875 0.144 0.017 0.8


218

Table 41 – part two:


[MeV] [barn] [barn] [MeV] nat

In(n,xn)113m

In

17.5 0.023 0.003 0.75

22 0.0080 0.0013 0.5

30.375 0.125 0.018 0.75

35.875 0.076 0.011 0.8

47 0.020 0.004 0.55

94 0.0174 0.0029 0.65 nat

In(n,xn)112m

In

17.5 0.043 0.007 0.75

22 0.12 0.12 0.5

30.375 0.172 0.025 0.75

35.875 0.077 0.011 0.8

47 0.39 0.09 0.55 nat

In(n,xn)111

In

30.375 0.049 0.007 0.75

35.875 0.034 0.005 0.8

47 0.32 0.05 0.55

94 0.101 0.017 0.65 nat

In(n,xn)110

In

35.875 0.0081 0.0012 0.8

94 0.042 0.006 0.65 nat

In(n,xn)109

In

94 0.049 0.007 0.65 nat

In(n,xn)108

In

94 0.016 0.003 0.65 127

I(n,2n)126

I

17.5 0.68 0.08 0.75

30.375 0.187 0.022 0.75

35.875 0.47 0.06 0.8

47 0.59 0.09 0.55

94 0.149 0.026 0.65 127

I(n,7n)121

I

94 0.185 0.027 0.65 127

I(n,8n)120

I

94 0.10 0.03 0.65 127

I(n,9n)119

I

94 0.024 0.007 0.65

219

Appendix M

Equations of detector calibration for Excel Addin

ORTEC(new1) in 1.6 GeV deuteron experiment has the same calibration equations

as in 2.52 GeV deuteron experiment (changes in the calibration were smaller than

statistical uncertainties)

ORTEC(new1) in 2.52 GeV deuteron experiment:

Function ep(g As String, e As Double) As Double

Select Case g

Case "p2"

If e < 910 Then

ep = Exp((-24.6978) + (12.7394) * Log(e) + (-2.29594) * Log(e) ^ 2 + (0.127757) * Log(e) ^ 3)

Else

ep = Exp((2.4902868) + (-0.963331) * Log(e))

End If

Case "p2_1"


Case "p3"

If e < 830 Then


Else

ep = Exp((1.8054174) + (-0.9484711) * Log(e))

End If

Case "p4"

If e < 660 Then


Else

ep = Exp((1.0675032) + (-0.9346622) * Log(e))

End If

Case "p5"

If e < 970 Then


Else

ep = Exp((0.3201731) + (-0.9160703) * Log(e))

End If

Case "p6"

If e < 1085 Then


Else

ep = Exp((-0.356219) + (-0.911472) * Log(e))

End If

Case "p7"

If e < 1085 Then

APPENDIX M. EQUATIONS OF DETECTOR CALIBRATION FOR EXCEL ADDIN

220


Else

ep = Exp((-1.89081) + (-0.797354) * Log(e))

End If

Case "p8"

If e < 1085 Then


Else

ep = Exp((-2.089) + (-0.859659) * Log(e))

End If

End Select

End Function

Function et(g As String, e As Double) As Double

Select Case g

Case "p2"

et = 0.164889 * Exp(-0.00076896 * e)

Case "p3"

et = 0.0960947 * Exp(-0.000810623 * e)

Case "p4"

et = 0.0665387 * Exp(-0.00102779 * e)

Case "p5"

et = 0.045487 * Exp(-0.00121456 * e)

Case "p6"

et = 0.0347284 * Exp(-0.00147366 * e)

Case "p7"

et = 0.0280721 * Exp(-0.00177061 * e)

Case "p8"

et = 0.00621469 * Exp(-0.000738892 * e)

End Select

End Function

ORTEC(new1) in 4 GeV deuteron experiment:

Function ep(g As String, e As Double) As Double

Select Case g

Case "p2"

If e < 340 Then

ep = Exp(0.2684012 * Log(e) ^ 3 - 4.4072431 * Log(e) ^ 2 + 23.1514703 * Log(e) -

41.4958416)

Else

ep = Exp(-0.041615 * Log(e) ^ 2 - 0.378324) * Log(e) + 0.488166)

End If

Case "p3"

If e < 240 Then

ep = Exp(0.301079 * Log(e) ^ 3 - 4.993606) * Log(e) ^ 2 + 26.597239 * Log(e) -

48.738794)

Else

ep = Exp((0.0141) * Log(e) ^ 2 + (-1.0764) * Log(e) + (2.071))


221

End If

Case "p4"

If e < 340 Then

ep = Exp(0.2506255 * Log(e) ^ 3 - 4.1815457 * Log(e) ^ 2 + 22.3389667 * Log(e) -

42.1385929)

Else

ep = Exp(-0.0127 * Log(e) ^ 2 - 0.7338 * Log(e) + 0.3431)

End If

Case "p5"

If e < 380 Then

ep = Exp(0.1794 * Log(e) ^ 3 - 3.07591 * Log(e) ^ 2 + 16.70719 * Log(e) - 33.42541)

Else

ep = Exp(-0.017 * Log(e) ^ 3 + 0.3202 * Log(e) ^ 2 - 2.8876) * Log(e) + 4.3052)

End If

End Select

End Function

Function et(g As String, e As Double) As Double

Select Case g

Case "p2"

If e < 700 Then

et = Exp(0.24632 * Log(e) ^ 3 - 4.62675 * Log(e) ^ 2 + 28.10639 * Log(e) - 57.03302)

Else

et = Exp(-0.7751 * Log(e) + 2.8486)

End If

Case "p3"

If e < 700 Then

et = Exp(0.13367 * Log(e) ^ 3 - 2.88019 * Log(e) ^ 2 + 19.22776 * Log(e) - 42.80905)

Else

et = Exp(-0.6621 * Log(e) + 1.4881)

End If

Case "p4"

If e < 700 Then

et = Exp(-0.08946 * Log(e) ^ 3 + 0.63912 * Log(e) ^ 2 + 1.00152 * Log(e) - 12.37033)

Else

et = Exp(-0.6359 * Log(e) + 0.7133)

End If

Case "p5"

If e < 700 Then

et = Exp(-0.31652 * Log(e) ^ 3 + 4.15564 * Log(e) ^ 2 - 16.80285 * Log(e) + 16.53732)

Else

et = Exp(-0.6205 * Log(e) + 0.0278)

End If

End Select

End Function


222

223

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237

List of tables

Table 1: Annual production of the most important transuranides and fission fragments

in light water reactor of thermal power 3000 MW [3]. ...................................... 5

Table 2: Overview of the properties of the most convenient materials for the spallation

targets [8]. ......................................................................................................... 10

Table 3: Parameters of different ADS projects [24]. ...................................................... 15

Table 4: Threshold reactions on aluminum activation samples. ..................................... 28

Table 5: Placement of the activation samples in 1.6 GeV deuteron experiment. ........... 30

Table 6: Parameters of used HPGe detectors, party overtaken from [52]. ..................... 44

Table 7: Irradiation parameters of three deuteron experiments on the E+T setup. ........ 55

Table 8: Selected parameters of Nuclotron accelerator compared to the older

Synchrophasotron accelerator [58]. .................................................................. 57

Table 9: Weighted average over relative yields in forward Cu monitor during 4 GeV

deuteron experiment. ........................................................................................ 63

Table 10: Beam position, shape and intensity during deuteron experiments, comparison

of data from various groups. ............................................................................. 64

Table 11: Summary from the beam intensity measurements done in 4 GeV deuteron

experiment. ....................................................................................................... 67

Table 12: Experimental neutron multiplicities for deuteron experiments. ..................... 83

Table 13: Contribution of various particles to the total yield, result of MCNPX

simulation and manual folding. ........................................................................ 90

Table 14: Example of the number of predicted counts in the strongest line of gold

isotopes. .......................................................................................................... 105

Table 15: Neutron beam parameters at TSL Uppsala for used energies. ..................... 106

Table 16: Neutron beam parameters at NPI Řež for used energies. ............................. 107

Table 17: Threshold and non-threshold reactions on gold activation samples. ............ 127

Table 18: Threshold reactions on bismuth activation samples. .................................... 128

Table 19: Threshold and non-threshold reactions on 115

In activation samples. ............ 129

Table 20: Threshold and non-threshold reactions on tantalum activation samples. ..... 130

Table 21: Threshold and non-threshold reactions on yttrium activation samples. ....... 131

Table 22: Placement of the activation samples in 2.52 GeV deuteron experiment. ..... 133

Table 23: Placement of the activation samples in 4 GeV deuteron experiment. .......... 134

Table 24: Spectra measured in 1.6 GeV deuteron experiment. .................................... 137

Table 25: Spectra measured in 2.52 GeV deuteron experiment. .................................. 139

Table 26: Spectra measured in 4 GeV deuteron experiment on Al, Au, Ta, and Bi foils.

...................................................................................................................................... 141

Table 27: Spectra measured in 4 GeV deuteron experiment on Co, In, and Y foils. ... 143

Table 28: Correction factor on beam instability for all three deuteron experiments on

E+T setup ........................................................................................................ 145

Table 29: Correction factor on real coincidences of gold isotopes produced in 1.6 GeV

deuteron experiment on E+T. ......................................................................... 147

LIST OF TABLES

238


1.6 GeV experiment. ..................................................................................... 149


experiment. ................................................................................................... 150


experiment. ................................................................................................... 150


experiment. ................................................................................................... 151


experiment. ................................................................................................... 152


2.52 GeV experiment. ................................................................................... 153


experiment. ................................................................................................... 154


experiment. ................................................................................................... 154


experiment. ................................................................................................... 155


experiment. ................................................................................................... 156

Table 40: Cross-section values already published at ND2010 conference. .................. 215

Table 41: Up to now unpublished cross-section values shown in figures in Appendix J

....................................................................................................................................... 217

239

List of figures

Figure 1: Geological repository for nuclear waste [2]. ..................................................... 4

Figure 2: Dominant decay heat contributors in spent PWR fuel irradiated to 50

GWd/MTHM [5]. .............................................................................................................. 6

Figure 3: Transmutation of 99

Tc [6]. ................................................................................. 7

Figure 4: Principal schema of the spallation reaction [7]. ................................................ 8

Figure 5: Current powerful proton accelerators [19]. ..................................................... 12

Figure 6: Scheme of the typical ADS proposal [20]. ...................................................... 13

Figure 7: Gamma-2 setup consisting of lead target (discs) and paraffin moderator. ...... 20

Figure 8: Cross-sectional side view (left) and front view (right) of the "Energy plus

Transmutation" setup. ..................................................................................................... 21

Figure 9: Photo of the Energy plus Transmutation setup with the biological shielding

(left). Detail of the natural uranium blanket (right). ....................................................... 21

Figure 10: Photo of Gamma-3 setup in F3 experimental hall (left) and graphite cylinder

with holes for samples. ................................................................................................... 22

Figure 11: Schema of Kvinta target [35]. ....................................................................... 23

Figure 12: Scheme of the new target EZHIK [35]. ......................................................... 24

Figure 13: Placement of E&T RAW targets inside the F3 experimental hall [35]. ........ 25

Figure 14: Activation materials used in the E+T for the study of high energy neutron

field. ................................................................................................................................ 28

Figure 15: The threshold energies of (n,xn) reactions in Au, Bi, In, Ta, and Y detectors.

........................................................................................................................................ 29

Figure 16: Placement of the gold and aluminum activation foils. .................................. 29

Figure 17: Plastic plane with sticked samples (left) and the plane holders (right). ........ 30

Figure 18: Energy plus Transmutation setup with inserted plane holders. ..................... 30

Figure 19: General decay scheme. .................................................................................. 34

Figure 20: Correction on the change in detector efficiency in the case of 3 mm thick Al

foil measured on Ortec(new2) detector. ......................................................................... 37

Figure 21: Self-absorption correction factors for 1 mm thick Bi foil. ............................ 38

Figure 22: Comparison between measured and simulated square-emitter correction for

2x2 cm2 foil and detector in Řež. .................................................................................... 40

Figure 23: Square-emitter correction for the detector in Řež calculated in MCNPX for

all sizes of measured samples. ........................................................................................ 40

Figure 24: Detector with inhomogeneous volume source representing Al foil that is used

for beam intensity measurements. .................................................................................. 41

Figure 25: Peak and total efficiencies of the ORTEC(new1) detector calculated for

inhomogeneous 25x25x3 mm3 volume source. .............................................................. 42

Figure 26: HPGe detector Ortec(new) with lead shielding (left) and the bank with

sample holder (right). ...................................................................................................... 44

LIST OF FIGURES

240

Figure 27: Example of peak and total efficiencies for the ORTEC(new2) detector in the

4 GeV experiment. .......................................................................................................... 46

Figure 28: Homogeneity of Řež HPGe detector in X-axis. ............................................. 47

Figure 29: Graphical interface of the DEIMOS32 code [53] .......................................... 49

Figure 30: Schema of the uncertainties. .......................................................................... 53

Figure 31: Nuclotron site scheme [58]. ........................................................................... 56

Figure 32: One section of the Nuclotron accelerator [58]. .............................................. 56

Figure 33: Nuclotron accelerator ring in the Synchrophasotron cable tunnel ................. 56

Figure 34: General scheme of the Nuclotron cryogenics [60]. ....................................... 57

Figure 35: Beam intensity during 1.6 GeV deuteron irradiation of the E+T setup. ........ 58

Figure 36: Beam intensity during 2.52 GeV deuteron irradiation of the E+T setup. ...... 59

Figure 37: Beam intensity during 4 GeV deuteron irradiation of the E+T setup. ........... 59

Figure 38: Polaroid films for pre-irradiation beam alignment (2.52 GeV deuteron

experiment). ..................................................................................................................... 60

Figure 39: Photo of the copper foil used for front beam monitor (left) and its paper

envelope (right). .............................................................................................................. 61


forward Cu beam monitor during 4 GeV experiment (left). Schema of the foil-cut and

target projection (right). .................................................................................................. 62


double cut Cu beam monitor irradiated in 4 GeV deuteron experiment (left). Schema of

the foil-cut and target projection is on the right. ............................................................. 62

Figure 42: Relative number of deuterons that did not hit the target during 2.52 GeV

deuteron experiment. ....................................................................................................... 64

Figure 43: Weighted average over relative yields of 19 different gamma-lines in the Cu

beam monitor placed behind the target during 4 GeV deuteron experiment (left).

Schema of the foil-cut and target dimension (right). ...................................................... 65

Figure 44: Cross-section of the 27

Al(d,3p2n)24

Na reaction from EXFOR [67] and fit

between the values for used deuteron energies. .............................................................. 66


longitudinal direction, 3 cm over the target axis, 1.6 GeV deuteron experiment. .......... 71


longitudinal direction, 10.7 cm over the target axis, 1.6 GeV deuteron experiment. ..... 72


direction, first gap of the E+T setup – 12.2 cm from the target beginning, 1.6 GeV

deuteron experiment. ....................................................................................................... 73


direction, behind the E+T setup – 48.8 cm from the target beginning, 1.6 GeV deuteron

experiment. ...................................................................................................................... 73


Au isotope produced in Au activation detectors in

longitudinal direction, various distance from the target axis, 1.6 GeV deuteron

experiment. ...................................................................................................................... 74

LIST OF FIGURES

241


Au isotope produced in Au activation detectors in radial

direction, various distance from the target beginning, 1.6 GeV deuteron experiment. .. 74


1.6 GeV deuteron experiment. ........................................................................................ 76


threshold reactions, 1.6 GeV deuteron experiment. ........................................................ 76


(ratio between 192

Au and 196

Au). ..................................................................................... 78


(ratio between 192

Au and 196

Au). ..................................................................................... 78


Au yields in longitudinal direction at 3 cm

from the target axis, deuterons and 0.7 GeV proton experiment on E+T setup. Values

are normalized to the second foil. ................................................................................... 79



and 0.7 GeV proton experiment on E+T setup. Values are normalized to the second foil.

........................................................................................................................................ 80


Au yields for 2.52 GeV and 1.6 GeV deuteron experiments in

all twenty Au foils, which were used. ............................................................................. 81

Figure 58: Cross-section of the (n,) reaction on Au and Ta, overtaken from ENDF/B-

VII. [84]. ......................................................................................................................... 82

Figure 59: Neutron multiplicities for E+T setup. ........................................................... 83

Figure 60: Neutron multiplicities for E+T setup normalized per GeV. .......................... 84

Figure 61: Visualization of the Energy plus Transmutation setup as defined in MCNPX

input file. On the left is SABRINA [82] plot provided by Jaroslav Šolc. ...................... 87

Figure 62: Model of the parts of E+T setup in MCNPX, rendered in Povray code [83],

author M. Majerle. .......................................................................................................... 87

Figure 63: Spectrum of the neutrons in the first target cylinder irradiated with 2.52 GeV

protons, log-log scale, various parts of the setup are omitted. ........................................ 88

Figure 64: Cross-section of the (n,) reaction on 238

U in ENDF database [84]. ............. 88

Figure 65: Ratio between experiment and simulation in longitudinal direction for 2.52

GeV deuteron experiment, Au and Al samples at 3 cm from the target axis. ................ 91


deuteron experiment, Au and Al samples in the first gap. .............................................. 92

Figure 67: Ratio between experiment and simulation for all three deuteron experiments

and 198

Au isotope. ........................................................................................................... 93



are normalized to the second foil. ................................................................................... 94


deuteron experiment, Au and Al samples in the first gap. Ratios are normalized to the

first foil. .......................................................................................................................... 94

Figure 70: Comparison of simulated longitudinal 196

Au yields for various beams of the

same total energy, samples placed at 3 cm from the target axis. .................................... 95

LIST OF FIGURES

242

Figure 71: Comparison of simulated radial 196

Au yields for various beams of the same

total energy, samples placed in the first gap of the setup. ............................................... 96

Figure 72: Ratio between experiment and simulation for different proton beam energies

and 194

Au (overtaken from A. Krása [45]). Samples were placed in radial direction in

the first gap of the setup. ................................................................................................. 97

Figure 73: Ratio between experiment and simulation for different deuteron beam

energies and 194

Au. Samples were placed in radial direction in the first gap of the setup.

......................................................................................................................................... 97

Figure 74: Neutron cross-sections for the Au and Bi (n,xn) threshold reactions. Data are

taken from the EXFOR [67] and ENDF [84]. ................................................................. 99

Figure 75: Comparison of the spallation neutron spectrum in Dubna and quasi-

monoenergetic neutron spectrum in TSL. ..................................................................... 101

Figure 76: Logo of the EFNUDAT project [90]. .......................................................... 101

Figure 77: Countries and institutes involved in EFNUDAT [90]. ................................ 102

Figure 78: Photo of the Gustav Werner cyclotron ........................................................ 103

Figure 79: Blue hall with the quasi-monoenergetic target and shielding [91]. ............. 104

Figure 80: User control interface for beam handling in TSL. ....................................... 104

Figure 81: Isochronous cyclotron U-120M in NPI Řež (left - own photo, right photo

from [98]). ..................................................................................................................... 106

Figure 82: Quasi-monoenergetic source in NPI Řež based on the design of Uwamino

[95]; scheme (left) [96] and a real outlook (right). ....................................................... 108

Figure 83: The sequence of the foils in the MCNPX simulation of neutron beam

attenuation. First two Au-Cu sets are samples of P. Bém, rest are ours. ...................... 108


7Be at the TSL. ....... 110


7Be at cyclotron Řež.

....................................................................................................................................... 111

Figure 86: Neutron spectrum produced in reaction with 7Li target and

natC beam stopper

in the case of NPI target station. ................................................................................... 111

Figure 87: Example of folding of the quasi-monoenergetic neutron spectrum and

simulated cross-section. ................................................................................................ 112

Figure 88: Placement of the Au and Al samples under the 30° and 60° from the beam

axis. ............................................................................................................................... 113

Figure 89: Neutron spectra under 0° and 60° angle from the beam axis [95]. .............. 114

Figure 90: Comparison between the neutron source construction of Y. Uwamino [95]

and at NPI Řež [96]. Used angles are drawn in the right part of the figure. ................. 114

Figure 91: Uncertainty structure in cross-section processing from the yield. ............... 115

Figure 92: Comparison of partial uncertainty values for cross-section measurements at

Řež and Uppsala ............................................................................................................ 116


Au(n,2n)196


EXFOR, TALYS 1.0 and my values. Last 10 EXFOR entries are [107] - [116]. ......... 117


Al(n,)24

Na reaction, comparison among


and [117] - [123]. .......................................................................................................... 117

LIST OF FIGURES

243

Figure 95: Cross-section of 197

Au(n,2n)196

Au reaction calculated in TALYS 1.0 using

five different models (ld1 – Constant temperature + Fermi gas model, ld2 – back

shifted Fermi gas model, ld3 – generalized superfluid model, ld4 – microscopic level

densities from Goriely‟s table, ld5 – microscopic level densities from Hilaire‟s table)

...................................................................................................................................... 120

Figure 96: Ratios among cross-sections calculated with different level density models in

TALYS 1.0 for 197

Au(n,2n)196

Au reaction. ................................................................... 121

Figure 97: Ratios among cross-sections of various threshold reactions on gold for

neutron energy 47 MeV (like in TSL Uppsala). ........................................................... 121

Figure 98: Experimental cross-section of 197

Au(n,xn) reactions measured at Uppsala for

energy 94 MeV. ............................................................................................................ 122


Au(n,2n)196

Au in TALYS 1.0 and

TALYS 1.2 (both in basic setting). EXFOR data and data from European Activation

File (EAF) were also added for better understanding. .................................................. 123


Au(n,8n)190

Au in TALYS 1.0 and

TALYS 1.2 (both in basic setting). No EXFOR and EAF data are available. ............. 124

Figure 101: Schematic drawings of detector placement in 4 GeV deuteron experiment

on E+T setup (blue color – Al, Au, Ta; red color Bi, In, Co; green color – Au). ......... 135


longitudinal direction, 3 cm over the target axis, 2.52 GeV deuteron experiment. ...... 157


longitudinal direction, 3 cm over the target axis, 4 GeV deuteron experiment, author

D. Wagner. .................................................................................................................... 158


direction, 3 cm over the target axis, 1.6 GeV deuteron experiment. ............................ 159


direction, 3 cm over the target axis, 2.52 GeV deuteron experiment. .......................... 159














direction, first gap of the E+T setup, 2.52 GeV deuteron experiment. ......................... 163


direction, first gap of the E+T setup, 4 GeV deuteron experiment, author D. Wagner. 163

LIST OF FIGURES

244


direction, first gap of the E+T setup, 1.6 GeV deuteron experiment. ........................... 164




direction, first gap of the E+T setup, 1.6 GeV deuteron experiment. ........................... 165




first gap of the E+T setup, 1.6 GeV deuteron experiment. ........................................... 166


first gap of the E+T setup, 2.52 GeV deuteron experiment. ......................................... 166


first gap of the E+T setup, 1.6 GeV deuteron experiment. ........................................... 167


first gap of the E+T setup, 2.52 GeV deuteron experiment. ......................................... 167


(ratio between 194

Au and 196

Au). ................................................................................... 168

Figure 123: Neutron spectra hardening along the target in 2.52 GeV deuteron

experiment (ratio between 194

Au and 196

Au). ................................................................ 168


(ratio between 194

Au and 196

Au). ................................................................................... 169

Figure 125: Ratio in front of and behind the target for various threshold reactions, 2.52

GeV deuteron experiment. ............................................................................................ 170


threshold reactions, 2.52 GeV deuteron experiment. .................................................... 170



deuterons and 0.7 GeV proton experiment on E+T setup. Data are normalized to the

first foil. Results of the 4 GeV deuteron experiment are preliminary. .......................... 171



and 0.7 GeV proton experiment on E+T setup. Data are normalized to the first foil.

Results of the 4 GeV deuteron experiment are preliminary. ......................................... 171



deuterons and 0.7 GeV proton experiment on E+T setup, unnormalized values. Results

of the 4 GeV deuteron experiment are preliminary. ...................................................... 172



and 0.7 GeV proton experiment on E+T setup, unnormalized values. Results of the

4 GeV deuteron experiment are preliminary. ................................................................ 172


Au yields in radial direction, deuterons and


deuteron experiment are preliminary. ........................................................................... 173

LIST OF FIGURES

245


Au yields in radial direction, deuterons and 0.7

GeV proton experiment on E+T setup, unnormalized values. Results of the 4 GeV

deuteron experiment are preliminary. ........................................................................... 173


Au yields for 4 GeV and 1.6 GeV deuteron experiments in

all twenty Au foils, which were used. ........................................................................... 174


Au and 194

Au yields for 2.52 GeV and 1.6 GeV deuteron

experiments in all twenty Au foils, which were used. .................................................. 174


Au and 194

Au yields for 4 GeV and 1.6 GeV deuteron

experiments in all twenty Au foils, which were used. .................................................. 175

Figure 136: Spectrum of the deuterons in the first target cylinder, log-log scale, whole

setup. Beam energy is 2.52 GeV, zero points cannot be depicted in logarithmic scale.

Uncertainties are on the level of one percent for most of the points. ........................... 189

Figure 137: Spectrum of the protons in the first target cylinder, various parts of the

setup are omitted to see their (zero) influence. Beam energy is 2.52 GeV. ................. 189


1.6 GeV deuteron experiment, Au and Al samples at 3 cm from the target axis. ........ 190


deuteron experiment, Au and Al samples in the first gap of the setup. ........................ 190


4 GeV deuteron experiment, Au and Al samples at 3 cm from the target axis. ........... 191


deuteron experiment, Au and Al samples in the first gap of the setup. ........................ 191



are normalized to the second foil. ................................................................................. 192



normalized to the first foil. ........................................................................................... 192

Figure 144: Ratio between experiment and simulation in longitudinal direction 10.7 cm

from the target axis, 2.52 GeV deuteron experiment, Au and Al samples at 3 cm from

the target axis. Ratios are normalized to the second foil. ............................................. 193

Figure 145: Ratio between experiment and simulation in radial direction behind the

target, 2.52 GeV deuteron experiment, Au and Al samples in the first gap of the setup.

Ratios are normalized to the second foil. ...................................................................... 193


4 GeV deuteron experiment, Au and Al samples at 3 cm from the target axis. Ratios are

normalized to the second foil. ....................................................................................... 194



normalized to the first foil. ........................................................................................... 194


Al(n,p)27

Mg reaction, comparison among

EXFOR, TALYS 1.0 and my values. ........................................................................... 195

LIST OF FIGURES

246


Au(n,4n)194


EXFOR, TALYS 1.0 and my values. ............................................................................ 195


Au(n,5n)193


TALYS 1.0 and my values (no EXFOR values exist). ................................................. 196


Au(n,6n)192




Au(n,7n)191




Au(n,8n)190




Bi(n,3n)207




Bi(n,4n)206




Bi(n,5n)205




Bi(n,6n)204




Bi(n,7n)203




Bi(n,8n)202




Bi(n,10n)200




Ta(n,2n)180

Ta reaction, comparison among



Ta(n,4n)178m

Ta reaction (no EXFOR values

exist, TALYS 1.0 cannot calculate this isomer). ........................................................... 202


Ta(n,5n)177




Ta(n,6n)176




In(n,xn)114m


TALYS 1.0 and my values. ........................................................................................... 203


In(n,xn)114m

In reaction, comparison among



In(n,xn)113m




In(n,xn)112m




In(n,xn)111



LIST OF FIGURES

247


In(n,xn)110




In(n,xn)109




In(n,xn)108




I(n,2n)126

I reaction, comparison among



I(n,4n)124




I(n,7n)121




I(n,8n)120




I(n,9n)119




Zn(n,2n)63

Zn reaction, comparison among



Au(n,4n)194


TALYS 1.0 and TALYS 1.2 (both in basic setting). EXFOR and EAF data are included.

...................................................................................................................................... 211


Au(n,5n)193



are available. ................................................................................................................. 211


Au(n,6n)192



are available. ................................................................................................................. 212


Au(n,7n)191



available. ....................................................................................................................... 212


Au(n,10n)188



available. ....................................................................................................................... 213

Documents

Czech Technical University in Pragueojs.ujf.cas.cz/~wagner/transmutace/diplomky/PHD_Svoboda.pdfIII Czech Technical University in Prague Faculty of Nuclear Sciences and Physical Engineering