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Analytical methods for the studies of nuclear materials
Andrzej Turos Institute of Electronic Materials Technology, Warsaw, Poland and National Centre for Nuclear Studies, Otwock, Poland
VINCO Technical Meeting, November 17, 2017
• The safe and economical operation of any nuclear power system relies to a great extent, on the success of the fuel and the materials of construction.
• During the lifetime of a nuclear power system which currently can be as long as 60 years, the materials are subject to high temperature, a corrosive environment, and damage from high-energy particles released during fission.
Nuclear materials
VINCO Technical Meeting, November 17, 2017
Nuclear Reactor 1600 MW+
3
Any solid substance inside the reactor dome is a
"nuclear material”
• The reactor vessel and many internal parts are steel, often highly alloyed with chromium and nickel.
• Some internal parts will be nickel-based superalloys,
• The fuel is often uranium oxide, sometimes doped with other elements like niobium or mixed with plutonium.
• The cladding and channels around the fuel will often be "zircaloy," lightly-alloyed zirconium base materials.
Nuclear materials
VINCO Technical Meeting, November 17, 2017
Research activities on nuclear meterials are focussed on understanding the performance
of these materials
when subjected to extreme environments.
Nuclear materials
VINCO Technical Meeting, November 17, 2017
• First, operating temperatures of the in-core materials might run above 300°C.
• Second, water itself can be a very corrosive environment.
• Third, irradiation has profound effects on materials properties and behavior over long times.
These three effects can often combine in ways that are difficult to foresee.
Enviroment in GIII reactors
VINCO Technical Meeting, November 17, 2017
• Operating temperatures of the in-core materials might run above 800°C up to 1000°C
• Cooling gas or liquid metal corrosion effects are hardly known.
• Radiation spectrum can be different from that in GIII reactors.
These three effects can often combine in ways that are difficult to foresee.
Enviroment in GIV reactors
VINCO Technical Meeting, November 17, 2017
Research scope
Establishing a relationship between atomic-scale structure and its function is an important topic in the
field of materials science.
Research scope
VINCO Technical Meeting, November 17, 2017
• Testing of real reactor materials – hot cells
• Modelling of physical processes
9
Fission
VINCO Technical Meeting, November 17, 2017
10
109 MeV
68 MeV
Fission
VINCO Technical Meeting, November 17, 2017
109 MeV Br in UO2 68 MeV Kr in UO2
VINCO Technical Meeting, November 17, 2017
• About 0.4% of fissions are ternary fissions, producing a third light nucleus such as
helium (90%) or tritium (7%).
• The fission products themselves are usually unstable and therefore radioactive
• This releases additional energy in the form of beta particles, antineutrinos, and gamma rays.
Fission
VINCO Technical Meeting, November 17, 2017
13 VINCO Technical Meeting, November 17, 2017
Fission
Prompt fission neutron energy spectrum Prompt fission neutron energy spectrum
VINCO Technical Meeting, November 17, 2017
Neutron energy spectra in reactor
VINCO Technical Meeting, November 17, 2017
VINCO Technical Meeting, November 17, 2017
Elastic scattering
M
m
Eo
Fe - M=55, n - m= 1 γ= 0,07 Threshold energy = 30 eV/0.07=428 eV
T(1MeV) = 1000 keV x 0.07 = 70 keV
Displaced host atoms – recoils
with energy ranging from 5 keV to 200 keV
are produced
Two-body collision
VINCO Technical Meeting, November 17, 2017
DISTRIBUTION OF ENERGY LOSS ALONG AN ION TRACK
18
Energy loss along the ion track
VINCO Technical Meeting, November 17, 2017
Collision cascade
VINCO Technical Meeting, November 17, 2017
PKA 10 keV
0.62 ps 8 ps
3 ps
5 ps
11.5 ps
23 ps
Averback R. S. JNM 216 (1994) 49
Molecular Dynamics simulations
VINCO Technical Meeting, November 17, 2017
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Effects of ion bombardment
VINCO Technical Meeting, November 17, 2017
a
a relv
reli VVc
Strain effects
Usually
cVi > 0 and cVv < 0
VINCO Technical Meeting, November 17, 2017
23
Dislocations
VINCO Technical Meeting, November 17, 2017
Nuclear reaction 58Ni(n,γ)59Ni
and subsequent 59Ni(n,α)56Fe reaction
are the main source of the He production in stainless steel, which leads to the damage of structural material.
VINCO Technical Meeting, November 17, 2017
4He production
Helium gas is produced by thermal neutron capture by nickel nuclei, and to a lesser extent by boron (both elements are present in the reactor vessel material)
Radiation effects in nuclear materials
Five phenomena occur in materials by neutron irradiation in a reactor environment: • irradiation hardening, • irradiation embrittlement, • irradiation creep – (creep is the time-dependent deformation
of a metal under constant load and at high temperature (T/Tm > 0.3). The metal responds by elongating. )
• irradiation growth – (dislocations present in the lattice preferentially absorb the defects, causing them to climb)
• void swelling – ( due to vacancy accumulaton)
VINCO Technical Meeting, November 17, 2017
Material synthesis
Irradiation
Testing
Structural properties
Functional properties
VINCO Technical Meeting, November 17, 2017
Modelling Roadmap
Polycrystals
VINCO Technical Meeting, November 17, 2017
28
The aim is to elucidate the damage buildup and defect
transformations in single crystals subjected to ion
bombardment.
It makes it possible to accumulate large dpa in a short time.
Molecular Dynamics simulations provide
close insight on these processes in the nanoscale.
Hence, the experimental validation of such computer
simulations is the key issue in defect studies.
Validating MD with direct imaging of radiation damage.
VINCO Technical Meeting, November 17, 2017
Materials structural analysis
Ion Beam Materials Laboratory (IBML)
Fundamental irradiation
studies performed at the
IBML
• Irradiations performed on
interfaces characterized to
the atomic scale
• Post irradiation analysis
will investigate the role of
interfaces on defect
formation and accumulation
• Aids in model development
and provides initial alloy
irradiation results.
Ion Beam Materials Laboratory (Los Alamos, NM)
VINCO Technical Meeting, November 17, 2017
RBS, RBS/C, NRA, ERDA, PIXE, PIXE/C, IL (on tandem and ion implanter) SEM/FIB/EDS/EBSD/CL, SEM TEM, HRTEM, EDS, EELS XRD, HRXRD Raman spectroscopy, ……
VINCO Technical Meeting, November 17, 2017
Materials structural analysis
31
Damage accumulation - single-step process
Fluence (1013
cm-2
)
0 2 4 6 8 10
Accu
mu
late
d d
am
ag
e
0.0
0.2
0.4
0.6
0.8
1.0 (a)
Fluence (1013
cm-2
)
0 5 10 150.0
0.1
0.2
0.3
0.4
(b)
Fluence (1013
cm-2
)
0 2 4 6 8 10
Accum
ula
ted d
am
age
0.0
0.2
0.4
0.6
0.8
1.0 (a)
Fluence (1013
cm-2
)
0 5 10 150.0
0.1
0.2
0.3
0.4
(b)
VINCO Technical Meeting, November 17, 2017
32 32
32
Damage accumulation in compound crystals
2 THETA [deg]
30.8 31.0 31.2 31.4 31.6
Inte
nsity
0.0
5.0e+6
1.0e+7
1.5e+7
2.0e+7
2.5e+7
3.0e+7
3.5e+7
1E14
5E14
1.2E15
fluence (x 1014
/cm2)
0.01 0.1 1 10 100 1000
dis
pla
ced
ato
ms (
at.
%)
0
20
40
60
80
100GaN
three-step accumulation model
stage I
VINCO Technical Meeting, November 17, 2017
33
Dislocations visualized by HRTEM
VINCO Technical Meeting, November 17, 2017
34
Dislocation tangle visualized by HRTEM magnification 620kx
stage II
VINCO Technical Meeting, November 17, 2017
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RBS/C
MC simulations Damage accumulation
description
Molecular Dynamics
XRD
IL, NI,
SPIS,…
TEM
NRA/C
Raman
VINCO Technical Meeting, November 17, 2017
Materials structural analysis
• Damage accumulation in nuclear materials can be studied using model single crystals subjected to ion bombardment.
• Damage buildup in compound crystals should be studied by the complementary use of appropriate techniques, typically HRTEM, HRXRD, and RBS/c.
• Molecular Dynamics simulations provides close look into collision processes on the atomic scale.
However, the validation of simulation results is indispensable.
Summary
36 VINCO Technical Meeting, November 17, 2017
Maybe someday we can enjoy such a view in our country
37
39
Rutherford Backscattering Spectrometry RBS/c
VINCO Technical Meeting, November 17, 2017
When the channeling ion
beam encounters a
defected region:
– probability of
scattering rises
– RBS data reveals
a damage peak
random (disoriented)
virgin (aligned)
irradiated (aligned)
RBS/c - Ion Channeling
40 VINCO Technical Meeting, November 17, 2017