Heavy ion irradiation of solids : electron ejection,sputtering, and effects on astrophysical ices

Hermann Rothard (CNRS) (rothard@ganil.fr)

CIMAPCentre de Recherche sur les Ions, les Materiaux et la Photonique(CEA/CNRS/ENSICAEN/Université de Caen-Basse Normandie)

BP 5133, F-14070 Caen Cedex 05, France

UNIVERSITEENSICAEN

GANIL

CYCERON

CIMAP

CIMAP-CIRIL

HE - SME

IRRSUDARIBE

50 µm

µ-mesons

electron

Particle Tracks

(photographic Emulsion)

proton

α-particleHe (ZP=2) F (ZP=9)

Ti (ZP=22)

As (ZP=33)

Collisions ions-atomes, molécules, agrégats, goutelettes

Stabilité des Matériaux du Nucléaire

Interaction Ion-Matière

Nanostructuration

Radiobiologie

LARIA CIRIL

Etc. …(Archade ...)

Ion beam

Energy deposition

(energy loss)

Strong electronic excitation

Secondary particle emission → analysis

Neutrals (atoms, molecules, cluster…)Ions

Electrons

Photons

Sputtering

(particle ejection)

Surface Modification,

Bulk: quasi one-dimensionalnanostructure

Tracks

(bulk,

surface)

SuIM: Surfaces, Interfaces et Matrices

Gaetano Lanzanò è stato unfisico, un filosofo, un artista, unuomo di gusto, ha partecipato egoduto del mondo, ha tenutouna consapevole linea dicondotta morale e quindi hacontribuito a sostenere oppurea modificare le concezioni chesi hanno del mondo, cioè asuscitare nuovi modi dipensare.

con affetto

gli amici di sempre(Angelo Pagano)

Gaetano Lanzanò, physicist at INFN Sezione di Catania since 1977, passed away suddenly on June 12, 2008.

IN MEMORIAM

The first experiment without the deeply missed Tano at CS-LNS Catania on fast electron emission (performed in spring 2009) could not have been performed without the solidarity of all colleagues and the help before and during the beam time from

I. Lombardo, E. La Guidara, F. Amorini, N. Rizzo, G. Politi, E. Geraci, P. Russotto, G. Cardella

Thanks to all ... Enrico De Filippo (INFN Sez. di Catania), Siegbert Hagmann (GSI + J.W. Goethe Univ. Frankfurt /Main), Hermann Rothard (CIMAP-CIRIL/CNRS Caen).

Scattering chambers LNS Ciclope + Chimera GANIL Nautilus

Detectors “Phoswich” scintillators (BaF2 + Foil)forward wall + detector battery,large in-plane angular range

Method Measurement of electron velocity by Time-of-Flight (TOF) technique

Resolution ∆V/V ≤ 5% in forward direction

Lanzanò et al.,PRA 58 (1998) 3534,PRA 63 (2001) 032702.

ARGOS multidetector

Electron Transfer to low projectile Continuum states (unbound, near zero kinetic energy in the projectile frame)

ECC (Target-) Electron Capture to the ContinuumELC (Projectile-) Electron Loss to the Continuum

Short summary of results obtained with ARGOS in atomic collision physics: E. De Filippo, G. Lanzanò and H. Rothard, Nucl. Phys. News 17, No. 2 (2007) 24-27 (NPN " Impact and applications" section)

102

103

104

105

10 15 20 25

doub

ly dif

feren

tial e

lectro

n yiel

d

electron velocity (cm/ns)

58Ni 28+ (45 MeV/u) + Au-Foil (280 µg/cm2)

binary encounter electrons

convoy electrons

Fermi shuttle electrons

( 280 µg/cm2 )

Lanzano et al., PRL 83 (1999) 4518Rothard et al., NIM B230 (2005) 419

Rothard et al., J Phys B: At Mol Opt Phys 43 (2001) 3261De Filippo et al., Phys. Rev. A68 (2003) 024701

ve ≈ 2vp

ve ≈ vp

vP

2vP

E. De Filippo, G. Lanzanò and H. Rothard, Nucl. Phys. News 17, No. 2 (2007) 24-27

Inelastic Binary Encounter

Experiment at LNS-CS 2007:

ARGOS +Chimera Chamber

LMMLMM

Experiment at LNS-CS 2009:

ARGOS Multidetector + Ciclope Chamber

Enrico De Filippo, Gaetano Lanzanò, Hermann Rothard, Claude VolantThree-Electron Auger Process from Beam-Foil excited multiply charged IonsPhys. Rev. Lett. 100 (2008) 233202

first results on heavy ion induced charging up of insulators:G. Lanzanò, E. De Filippo, S. Hagmann, H. Rothard, C. VolantRad. Eff. and Defects in Solids 162 (2007) 303-318

charging phenomena important for ion beam focusing bynano-capillaries: A. Cassimi et al., “Multiply-charged ion nano beams”,Int’l Journal of Nanotechnology Vol. 5 (2008)

LNS 2009: Carbon beam (23 A MeV)

Insulator Targets: PP, Mylar

Sandwich-Targets:Au/InsulatorAu/Insulator/Au

XY-TOF-imaging technique in Ion-Surface Collisions

Collimator

ion position (XY)

Time Of Flight

Mass spectrum N(m/q)Velocity Vector (vx, vy, vz)Angular Distribution N(θ) Master Thesis

Jérôme LenoirHussein HijaziEnergy Distribution N(E)

Beam direction

Ca17+ (9.1 MeV/u) → LiF

UHV sytem:

TOF Detector Chamber+ Preparation Chamber+ Target Transfer

S. Akcöltekin, I. Alzaher, B. Ban d’Etat, T. Been, P. Boduch, A. Cassimi, H. Hijazi, H. Lebius, B. Manil, J.M. Ramillon, H. Rothard, M. Schleberger, E.F. da Silveira, AODO: Secondary Ion Emission and Surface ModificationNucl. Instrum. Meth. B267 (2009) 649-651

Experiment September - November 2009

GANIL-SME (Fe, Pb, Kr, Ca?)

Merci à F. Aumayr

Basic Processes in Ion Collisions

ionisation - exc itation

capture

énergie

HE

SMEIRRSUD

ARIBE

Elastic collisions (ion-atom)(”nuclear stopping”)

Inelastic collisions (ion-electron)(”electronic stopping”)

Kinetic energy Ekin

Multi-charged Ions:

Potential energy Epot

102

103

10-1 100 101 102

Li+ y

ield

(arb

itrar

y un

its)

Li+ energy E (eV)

Xe21+ (17 keV/q)

102

103

10-1 100 101 102

Li+ y

ield

(arb

itrar

y un

its)

Li+ energy E (eV)

Ca17+ (9 MeV/u)

102

103

10-1 100 101 102

Li+ y

ield

(arb

itrar

y un

its)

Li+ energy E (eV)

Maxwell-BoltzmannT≈ (12 ± 1) * 103 K

Energy distribution of 7Li+

Coulomb Explosion ?

Thermal Spike ?(cf. PDMS)

Excitonic mechanism:defect mediated sputtering ?

J. Lenoir, P. Boduch, H. Rothard, B.Ban-d’Etat, T. Been, A. Cassimi, T. Jalowy, H. Lebius, B. Manil, J.M. RamillonSputtering by highly charged ions: application of the XY-TOF technique to secondary ion ejection from LiFNucl. Instrum. Meth. B258 (2007) 178-182

Radiation effects in condensed gases (ices)

Satellites of the giant planets (Europa, Ganymed, …)

Dust grains

Comets

Solar wind, cosmic rays, planetary magnetic fields

Interstellar icy grain mantles

The grains are covered with an icy mantle formed from atoms and molecules.

Thermal processes

Irradiation with:- cosmic rays;- stellar (solar) wind;- UV radiation;- electrons

(high and low-energy).

Irradiation induced chemicalmodification within ice and also desorption of species from ice.

Heavy ions in space

Ions in solar wind

Mewaldt et al. Space Sci. Rev. (2007) 130 323

H/Fe~104

H/Ni~105 Ions in cosmic rays(in dense clouds)

Shen et al. A&A. (2004) 415 203

Experimental DeviceC.A.S.I.M.I.R. : Analysis Chamber by Infrared Spectroscopy of IRradiated MoleculesC.A.S.I.M.I.R. : Analysis Chamber by Infrared Spectroscopy of IRradiated Molecules

FTIR Infrared Spectrometer

Cryostat Head

Analysis Chamber

Experimental DeviceDeposition tube

Ion beam

Detector

IR beam

Experimental Device

IR beam

Deposition tube

Detector

Ion beam

CO2H2OCO2

CO2

H2O

H2O2

CO H2CO3

O3

136Xe23+ 0.76 MeV/u => H2O+CO2 (1:1)

Fluence = 8.6 x 1012 cm-2

Dose = 95.8 MGy

Flux Moyen = 5.0 x 107 cm-2 s-1

FTIR spectrum: 46 MeV 58Ni11+ → C18O2

After irradiation

Before irradiation

Wavenumber (cm-1)

C18O2 Column Density

Destruction:dN/dF = - σd NN = N0 e- σd F

σd = 2.2 x 10‒13 cm2

Col

umn

dens

ity

Column density of C18O2

Destruction plus sputtering:dN/dF = - σd N -Y

N = N0 e- σd F - (Y/ σd) (1 - e-σd F)σd = 1.7 10-13 cm2

Y = 4.0 × 104 molecules/impactCol

umn

dens

ityColumn density of C18O2

1st regime 2nd regime

N = N0 e- σs F

46 MeV 58Ni11+ → C18O2C

olum

n de

nsity

Specific Sputtering Flux (SSF) for CO2 ice

SSF=ion flux (corresponding) sputtering yield

Mewaldt et al. Space Sci. Rev. (2007) 130 323Shen et al. A&A. (2004) 415 203

Y~Se2

Brown et al. Nucl. Instr. Meth. (1982) 198 1

E. Seperuelo -Duarte, Ph. Boduch, H.Rothard, T. Been, E. Dartois, L.S.Farenzena, E.F. da SilveiraHeavy Ion Irradiation of Condensed CO2: Sputtering and Molecule Formation Astronomy & Astrophysics 502 (2009) 599

CO2 CO

N0 = 1,5 1018 molecules/cm2

l = 660 nmN0 = 1,5 1018 molecules/cm2

l = 860 nm

Se = 2,6 10-12 eV cm2 / moleculer ≈ 13.000 nmσd = 1,7 10-13 cm2

Y = 4,0 104 molecules/impact

Se = 1,7 10-12 eV cm2 / moleculer ≈ 29.000 nmσd = 1,4 10-13 cm2

Y = 9,0 104 molecules/impactCO, CO3, O3, and C3 CO2, O3, C3O2, C5O2, C2O, C3

C4O2 or C7O2

Interaction of 46 MeV 58Ni11+ with different ices

Emmanuel Dartois Institut d’Astrophysique Spatiale IAS / Orsay

Philippe Boduch CIMAP/Université Caen Basse Normandie

Emmanuel BalanzatHermann Rothard

CIMAP/CNRS

Eduardo Seperuelo DuarteAlicja Domaracka

CIMAP/PUC de Rio/Univ. Caen (co-tutelle)CIMAP (Postdoc ENSICAEN)

Enio F. da Silveira PUC Rio / Brazil

Lucio FarenzenaSergio Pilling

Univ. Federal, Florianopolis / BrazilIP&D, Univ. do Vale do Paraíba - UNIVAP

Irradiation effects in astrophysical ices: sputtering !

Appearance of new molecules

Complex organic molecules (pre-biotic? H2O-CO-NH3 ice)

Caen

LARIA CIRIL

DSM/DRECAM SPM ENSICAEN Université de Caen

Laboratoire d’accueil auprès du

0.01

1

100

104

10-1 101 103 105 107

dE/d

x (

keV

/nm

)

projectile kinetic energy Ekin

(keV)

"electronic"

"nuclear"

Xe on UO2

80 keV

Potential Energy

A R I B E

15 keVNUCLEAR vs. ELECTRONIC STOPPING: Xe → UO2