Microscopic Model of Excitation of Swift Heavy Ion Tracks in Insulators

S.A.
1)

1 Gorbunov ,

N.A.
2)

2 Medvedev ,

R.A.

3 Rymzhanov ,
3)

P.N.

4 Terekhin ,

A.E.

1,3,4 Volkov*
4) NRC Kurchatov Institute, Moscow, Russia

LPI of the Russian Academy of Sciences, Moscow, Russia

CFEL at DESY, Hamburg, Germany

JINR, Dubna, Moscow Region, Russia

Swift Heavy Ions

dE/dx, keV/nm 5 4 3 2 1 100
Au in Olivine

Problems of the macroscopic models

Heat diffusion equation cannot describe heat transport in SHI track [1]:

Sn / Se < 0.01
Electronic Nuclear

Eion > 1-10 MeV/u Mion > 20 mp Se > 1-10 keV/nm

Ti = div( i Ti ) t
MD simulations

Temperature approach for the lattice excitation is questionable till 1 ps [1]: pi 2 H = + U ( {q i } ) i 2m

Electron-lattice coupling [2]: Cooling down time of electrons is much shorter than the atomic vibration time:

102

104 E, keV

106

108

Initial excitation Re < 0.5 nm Structure transformations Rd ~ 10 nm

Rd

Finite velocity (sound) of heat propagation

pi i 2m
U ( {q i } )

H < pk >= k BTkin pk

H < qk >= k BTconf qk
Temperatures

(R0e)2 -14 s << t = 10-13 s c < 10 t e = 4 os e

Two limit cases: t <<tos => Dynamically isolated atoms (k)~ k2 t>>tos
=> Phonons

Heat Front
L~ 100 m 10-17 s 10-16 s 10-15 s 10-14 s 10-13 s 10-9 s
> 10-9 s

Equilibrium
Wave equation or MD simulations must be used instead:
Cattaneo wave equation of heat propagation:

(k) ~ k, (k<</a)

1. Initial electronic excitations 2. Plasmon screening 3. Thermalization of electrons 4. Cooling down of electrons 5. Energy transfer to lattice 6. Track cooling down
Marek Skupinski (Uppsala)

H H < pk >=< qk >= k BT pk qk

Tkin T T = = conf
Atomic system cannot be described by equilibrium temperature on sub-picosecond scale [2]

Lattice dynamic can not be ascribed to phonons at such times [2].

7. Stress relaxation

T 1 T K 1 T + r =0 2 t t C r r r
2

Electronphonon coupling mechanism can not be applied

Multiscale microscopic model of excitation of swift heavy ion tracks

Three microscopic models are combined together to describe nonequilibrium kinetics of the both, electrons and the lattice in SHI tracks [3]. Dynamic Structure Factor Complex Dielectric Function formalisms takes into account collective responses of electron subsystem and of lattice. Coupling between the both subsystems is realised via DSF formalism [2-4], giving electron-lattice heating beyond electron-phonon approximation.

SHI and electrons

40

Lattice excitation
Molecular Dynamics (MD) tracing atomic of the trajectories Monte-Carlo (MC) simulations of the initial electronic kinetics [5]
2

Cross-sections and energy exchange

Inelastic SHI and electron scattering:

10-17 s 10-16 s 10-15 s

-40 -20 0 20

SHI passage Nonequilibrum electron kinetics, secondary ionizations, Auger decays Spatial spreading of electrons, energy exchange with lattice

nm
20 0 -20 -40

t = 10-15 s 10-11 s
Electron-lattice coupling is described via DSF [4]:

1 - accounts for plasmons el k 2 ~ V (k ) Im - valence band and deep shell scattering E n e (k , ) - is extracted from experiments
2

CDF [3,5,6]

nm 40

10-14 s 10-13 s 10-12 s

Molecular-kinetic tracing of electron spreading n(t,r), Te(t,r) [3]

ion 2 kf ~ V (k ) Sion (k , ) ki E N i ( kr t ) S (k , ) = dtdre G (r, t ) 2

2

Elastic electron scattering on the lattice:

ion 2 kf ~ V (k ) Sion (k , ) ki E
2
2

DSF [2-4]
- satisfies both limits: phonons and plasma - gives realistic descriptions

Pair Correlation Function [4] is calculated directly in MD :

Electron-lattice coupling:

, t) G ( r=

1 (r + Ri (0) R j (t )) N i , j =1
N

ki ion Q ~ fk i (1 fk f ) dk i dk f k f f E f

Electron-lattice coupling beyond electron-phonon approximation, valid even on fs-timescales! [2-4]

Application to olivine crystals

CDF formalism for olivine
Electron mean free path, (A)
300 250 200 150 100 50 0 10 100 1000 10000 Calculated NIST

Electrons and lattice kinetics

MC calculated (a) radial distributions of the electrons (b) energy density of free electrons

Electron energy (eV)

Calculated electron inelastic mean free path in olivine agrees well with NIST database [7]
5000 4000
SRIM 2011 CasP 5.0 Calculated

Temperature of electrons and the kinetic temperature of the lattice (1 nm < R < 1.5 nm )
Ionic Kinetic T emperature, ( K)

312,0 377,3

dE/dx (eV/A)

3000 2000

Electrons thermalize with the lattice within 100 fs Lattice heating up to 800 K by 2 GeV Au
0,000 862,5 1725 3450

800
700
600
500
400
300
2

442,5 507,8 573,0 638,3 703,5 768,8 834,0

50000

6900 1,380E+04

Electronic te mperature

1000 0 10

40000

2,070E+04 2,760E+04 3,450E+04 4,140E+04 4,830E+04 5,520E+04

100

1000

10000

20000
10000

Good cross-sections for MC

nm

75

100

Tim e, fs

Energy (MeV) Calculated SHI energy losses in olivine agree with SRIM [9] and CasP codes

Output of MC is used as initial conditions for further molecular-kinetic tracing of electrons

0 0

25

Rad ius,

50

Lattice termalization within 200fs Further cooling down of the lattice due to spatial heat dissipation

Conclusions
1) A multiscale microscopic model describing quantitatively all stages of excitation of an insulator (olivine) in a SHI track. 2) The Complex Dielectric Function formalism provides with reliable cross-sections, mean free paths, and energy losses of a SHI and electrons. 3) The Dynamic Structure Factor formalism describes electron-lattice coupling beyond the phononic approximation. A general model linking both, phonon and plasma limit cases is developed. 4) Estimations of lattice excitation in solid olivine indicates heating up to 800 K after 2 GeV Au ion impact.
* Corresponding author: a.e.volkov@list.ru

References
[1] V.P. Lipp, A.E. Volkov, M.V. Sorokin, B. Rethfeld, NIMB 269 (2011) 865 [2] A.E. Volkov, V.A. Borodin, NIMB 146 (1998) 137 [3] S.A. Gorbunov et al., Phys. Stat. Sol. C, 10 (2013) 697 [4] L. van Hove, Phys. Rev. 95 (1954) 249 [5] N. Medvedev, R. Rymzhanov A.E. Volkov, NIMB (2013 in press) [6] R.H. Ritchie, A. Howie, Philos. Mag. 36 (1977) 463 [7] C.J. Powell, A. Jablonski, NIST Database 1.2 (2010)

Au ion in Olivine

Rad ius,
4

30000

(nm )

Tim e, (ps )