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nuclear, elastic energy deposition. Ionising energy deposition. Energy deposition. Radiation-induced material modifications. Lattice. Electrons. Small linear regime. Frenkel-pair creation linear cascades. Classical radiolysis. Perturbation. Strong non -linear regime.
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nuclear, elastic energy deposition Ionising energy deposition Energy deposition Radiation-induced material modifications Lattice Electrons Small linear regime Frenkel-pair creation linear cascades Classical radiolysis Perturbation Strong non -linear regime High LET effects Tracks regime Non-linear cascades Synergy?
! Nuclear reactions The displacement spectrum Abromeit C. JNM 216 (1994) 78 Nuclear reactions elastic V. M Agramovich and V; V; Kirsanov Physics of rad effects in crystals R. A. Johnson and A; N Orlov Eds. N-H 1986
T > The cascades: the mean free path TRIM (Å) Averback R. S. JNM 216 (1994) 49
Sub-cascades One dense cascade Cascades sub-cascades Linear-non linear Linear All the atoms in movement collide with atoms at rest dpa makes sense Non-linear Atoms in movement collide together collective motion of atoms local melting shock-wave generation
Low T, high T1/2 z = “resistivity” defect/ “Kinchin and Pease”dpa Recombinations: one dpa is not a defect Low T, low T1/2 Exemple : Cu sd 140 barns n0 135 volumes atomiques sr 4000 barns High T Radiation-enhanced diffusion Transient and stationary regimes Influence of: permanent sinks flux Averback R. S. JNM 216 (1994) 49
0.3 ps 0.62 ps 3.2 ps 0.1 ps 5 ps 11.5 ps 0.5 ps 1 ps 2 ps 6 ps 17.7 ps 23 ps Recombinations: cascades NiAl Au PKA 10 keV Averback R. S. JNM 216 (1994) 49
What happens to the projectile Stopping power range stragglings What happens to the solid What happens to: the projectile : secondary particles: electrons recoils
proton on hydrogen proton on aluminium Projectile ion : the atomic processes
Corrections : • Relativistic • Density • Deep levels • Effective charge Projectile ion: the electronic stopping; high velocity Bethe
Projectile: Swift heavy ions Secondary particles: electrons Velocity effect
Projectile: photons electrons Secondary particles: electrons Compton photoelectric
The (dE/dx)e distributions Bragg peak of electrons (dE/dx)e of the projectile over a given thickness Fraction of the dose (dE/dx)e of the secondary electrons (dE/dx)e (keV/µm)
Projectile: low energy heavy ions Secondary particles: recoils The recoils makes the inelastic energy deposition Xe 100keV Projectile: (100 to 50) keV (dE/dx)n≈ 2.5 (dE/dx)e
Radiolysis Low LET Radiolysis is the creation of permanent defects due to the non-radiative recombination of an elementary excitation (a hole-electron pair) The radiolysis yield G Quantum yield This is the “Kinchin and Pease” for inelastic damage
The radiolysis yield G Typical, yields (could be zero) Organic: a few 10-7 mol/J alkali halides (10-8 to 10-9) mol/J 100 eV 1 – 10 keV The yield concept is never use for elastic damage If one dpa = one defect (z=1) For ions (7 10-8 to 1.5 10-7) mol/J
The low LET radiolysis conditions The available energy, Egap (in fact Ex < Egap) > the formation energy of the Frenkel pair. the radiolysis can only occurs in insulators or wide band-gap semiconductors. The excitation must be localised on one atomic (or molecular) site Non-radiative transitions, allowing an efficient kinetic energy transfer to an atom, must prevail over radiative transitions
Could work in alkali halides (anions and cations) alkaline-earth halides Difficult in oxides Frenkel cation Egap Ex Frenkel anion
Low LET radiolysis versus ballistic damage • Radiolysis is not universal, not easily predictable • 2) Is in essence temperature dependent • 3) Spans over a wide time scale • 4) Occurs generally on one sub-lattice (anions) • 5) Radiolysis occurs occasionally • when it occurs, it is with a good energetic efficiency. Elastic damage occurs every time • but with a relatively poor energetic efficiency.
STE: Se et chalcogenides STE: BeO-YAG MgO, Al2O3 Charge-carriers self-trapping Self trapping of charge carriers results from a competition between deformation and polarisation of the lattice
STE Self trapped holes AgCl AgCl KCl KCl CaF2 CaF2 c-SiO2
STE Luminescence STE have several luminescence states a strong Stokes shift very variable lifetime: ns to ms
Correlation - anticorrelation STE luminescence and defect creation Correlation conversion thermal STE triplet -> F +H small S/D
Temporal dynamics Elastic damage : 25 keV Cu cascade over at 10 ps only numerical simulations Radiolysis: fast processes (ps) charge-carrier trapping conversion from STE highly excited stated slow processes (µs to ms) from STE triplet states Also measurements!! metastable defects
Conversion STE-defects a-SiO2 Transient defects c-SiO2 Also in SrTiO3, MgO, Al2O3
Resistant and sensitive materials Resistant: Metals, semi-conductors. crystalline Oxides. c-SiO2 (flux) NaAlSi3O8 : metastables (SrTiO3, MgO, Al2O3, c-SiO2) Sensitive: Alkali halides Alkaline-earth halides CaF2, MgF2,SrF2 : Gmeta , Gstable very low KMgF3, BaF1.1B 0.9, AlF3 (flux?), LiYF4: may be Silver halides AgCl; AgBr Amorphous solids a-SiO2 , a-As2Se3, a-As2S3, a-Se, a-As Water and organic mater (bio matter)
nuclear, elastic energy deposition Ionising energy deposition Energy deposition Radiation-induced material modifications Lattice Electrons Small linear regime Frenkel-pair creation linear cascades Classical radiolysis Perturbation Strong non -linear regime High LET effects Tracks regime Non-linear cascades Synergy?
“Classical” track formation in insulators MICA YIG LET threshold Amorphisation fluctuations critical size induced stress S. Bouffard et al. Phil. Mag. A 81 (2001) 2841 M. Toulemonde, F. Studer Phil. Mag. A 58 (1988) 799 Etching of the amorphous core GSI image Nanotechonology (ITT) M. Toulemonde et al. J. Appl Phys. 68 (1990) 1545
ZrO2 Less common High LET effects Crystal to crystal transformations can exist monoclinic-> tetragonal Two process (incubation fluence)
Unexpected High LET effects Some metals are sensitive to high LET radiation High Tc superconductors are sensitive to high LET radiation (pinning of vortices)
Unexpected High LET effects Plastic instability of amorphous materials: the hammering effect Co75Si15B10 1.7 1013 Xe/cm2; 2.8 MeV/A; 50K Klaumünzer et al. Mat. Res. Proc. 93 (1987) 21 Ion-aligned nanoparticle elongation sample implanted at 1 · 1017 Co/cm2 at 873 K and irradiated at (a) 1013, (b) 3 · 1013, (c) 6 · 1013 and (d) 1014 I/cm2. D'Orleans-C; Stouter-JP; Estournes-C; Grab-JJ; Muller-D; Guille-JL; Richard-Plouet-M; Cerruti-C; Haas-FNIM B 216: 372-8 2004 PHYSICAL REVIEW B 67, 220101 (2003) Fragmentation and grain rotation in NiO single crystals (Klaumuenzer REI-2007) Polygonisation (UO2, CaF2)
Cargèse Bibliography Summer schools The French summer school “Materials Under Irradiation”, Giens 1991, Trans Tech Publications, 1992 (in English) The USA summer school “Fundamentals of Radiation Damage”, Urbana in 1993, J. Nucl. Mat., volume 216 (1994) The French summer schools Lalonde les Maures 1999 et 2000, 2007 (PAMIR) Not published, but printed material (in French)
Bibliography Classics Chr. Lehmann, Interaction of Radiation with Solids and Elementary Defect Production, Series on Defects in Crystalline solids, vol. 10. North-Holland, 1977 N. Nastasi, J. W. Mayer and J. K. Hirvonen, Ion-Solid Interaction, Fundamentals and Applications Cambridge Solid State Science Series, 1996 R. A. Johnson and A. N. Orlov Eds Physics of Radiation Effects in Crystals, North-Holland, 1986 Specific to radiolysis N. Itoh and A. M. Stoneham Material Modification by Electronic Excitation, Cambridge University Press, 2001
Projectile: electron capture Very very slow HCI H. Kurtz et al, Phys. Rev. A49 (1994) 4693 proton on hydrogen
Bibliography Never go to the beach without a good book More specific to radiolysis N. Itoh and A. M. Stoneham Material Modification by Electronic Excitation, Cambridge University Press, 2001 F. Agullo-Lopez, C. R. A. Catlow, P. D. Townsend Point defects in materials Academic Press 1988 N. Itoh ed Defects Processes induced by electronic excitation in insulators World Scientific 1989 K. S. Song, R. T. Williams Self-trapped excitons Springer-Verlag 1993 P. D. Townsend, P. J. Chandler, L. Zhang Optical effects of ion implantation Cambridge 1994
rF ~ 1 µW.cm / % defect Low T, low T1/2 Exemple : Cu sd 140 barns n0 135 volumes atomiques sr 4000 barns J. Dural et al, J. de Physique 38 (1977) 1007
The (dE/dx)e distributions Bragg peak of electrons (dE/dx)e of the projectile over a given thickness Fraction of the dose (dE/dx)e of the secondary electrons (dE/dx)e (keV/µm)
Low LET radiolysis: organics; water The primary species Fragmentation of H2O+ Fragmentation of H2O* Up to 60 reactions < 10-12 s 10-12 s < blobs and short tracks < 10-7 s in bulk >10-7 s Distances empirically
Low LET radiolysis: specific role; multi-ionisation Double ionisation and superoxide OOH° Ar C H Gervais-B; Beuve-M; Oliver-GH; Galassi-MERadiation-Physics-and-Chemistry. 2006; 75(4): 493-513
blobs spurs E de 100 à 500 eV E<100 eV Primary electron Annex track Short track E> 5000 eV E< 5000 eV Projectile: photons electrons Secondary particles: electrons