Vacuum/volume44/numbers 3/4/pages 341 to 344/1993

Printed in Great Britain

0042-207X/9356.00+.00 1993 Pergamon PressLtd

A comparison of T R I M and molecular dynamics in calculating the backscattering yield of carbon incident on graphite
H Bergs&ker, and
F: Lama, BRAINK AG, Liechtenstein

Manne Siegbahn Institute of Physics, 104 05 Stockholm, Sweden

and R S m i t h , Department of Mathematical Sciences, University of Loughborough, Loughborough, Leicestershire LE11 3TU, UK 21nd R W e b b , Department of Electronic and Electrical Engineering, University of Surrey, Guildford GU2 5XH, UK

This report is an attempt to assess the validity of the binary collisions approximation by comparing TRIM and molecular dynamics in calculating the backscattering of carbon ions off a graphite surface. The TRIM calculations were performed for an amorphous target with smooth surface. In the molecular dynamics calculations, a recently available semi-empirical many body potential by Tersoff was used. The calculations were made for a perfect crystal at zero temperature, consisting of 1342 atoms in five layers. The probability of reflection was calculated as a function of energy and angle of incidence of the projectile. Compared with the binary collisions calculations, molecular dynamics predicts a significantly higher backscattering probability. For instance, at normal incidence TRIM shows less than one per cent reflection in the whole energy range up to 1 keV, whereas in molecular dynamics the reflection yield peaks around 20 eV with more than 40% reflection. The case of a head-on collision with a surface atom at normal incidence is discussed in detail.

1l. Introduction When an atom with energy in the eV, 10 eV or lower 100 eV range hits a surface, it may either be implanted and trapped, stick 1:o the surface or be kinematically reflected. Applications where it is essential to know the probability of reflection include the fuel recycling and impurity recycling in controlled fusion devices. ]In this context it is particularly essential to know in what circumstances the combination of backscattering and self-sputtering of relevant first wall materials leads to one or more than one atom being ejected per incoming atom, since this may entail an avalanche release of impurities into the plasma. Graphite is a favoured wall material in todays large Tokamak experiments, but 1:he plasma performance is partly degraded by so-called carbon blooms, when carbon flows into the plasma in an uncontrolled 'way ~. Not only the total yield, but also the angular and energy .distribution of reflected atoms is of interest in fusion plasma :research, since it determines how far into the plasma reflected atoms are able to penetrate before being ionized, and consequently restrained in their motion by the magnetic field. Moreover, collection of plasma ions, or of neutral atoms produced by charge exchange, on surfaces has been extensively used to study impurity fluxes at the plasma edge in fusion experi[ments2-8. The relevant energy range in fusion research is from l0 eV up to a few keV, and the ions or neutral atoms hit the surface with a wide distribution of angles of incidence.

Finally, collection of sputtered particles on solid surfaces has been used in sputtering yield measurements 9. The energies in this case are from ~ 1 eV to a few tens ofeV and the angle of incidence is usually near normal. In these measurements as in the collector probe measurements in plasma devices, it is often more or less implicitly assumed that the reflection of heavy atoms incident on the same or lower Z surfaces can be neglected. Few experimental data exist on backscattering in the 1 and 10 eV ranges. It has been shown that the sticking probability of metal ions incident on low Z substrates is close to unity ~ 0 except at energies below ~ 10 eV, where the reflection probability of uranium, Rh and Nb atoms at an AI20 3 surface can be 10o/ot t,~2. In an accurate relative measurement it was shown that the reflection probability of sputtered vanadium, nickel and stainless steel atoms (with energy around 1-20 eV) on Si, AI, Be or graphite surfaces is less than 4%, whereas it may exceed 10% for sputtered vanadium collected on a silver surface ~3. Recently the energy distributions have been measured of inert gas atoms scattered off metal surfaces with incident energies in the range 10-100 eV 14. Where solid collectors, usually graphite, have been used to collect carbon and boron ions in the edge plasma of Tokamaks, with energies mostly in the range 10-100 eV, there are indications that the probability of reflection may be 10-20% 7,~s. In these cases, the incident energy is likely to have been a distribution
341

H Bergs~4ker et al: TRIM and molecular dynamics comparison

from a few eV to a few tens of eV and the angles of incidence a fairly wide distribution but with few particles at very oblique angles. From a theoretical point of view, the backscattering probability of a heavy ion at surfaces of lower or similar atomic mass is expected to be low, since due to kinematics it cannot be backscattered in a single binary collision, and large angle scattering is generally suppressed. For backscattering to occur, it is necessary to have a sequence of small angle binary collisions without losing too much energy in the process, or that the energy is sufficiently low for multiple interactions to come into play. It is well known that binary collisions calculations, such as with TRIM ' 6 , 9, result in low reflection probability for ions incident on lower or like mass surfaces 17. At energies similar to the binding energy of the lattice atoms, the binary collision approximation is clearly not applicable, and it is necessary to include multiple interactions. In a molecular dynamics calculation, Shapiro and Tombrello investigated the case of copper atoms incident on a copper surface, and found no reflection at normal incidence 2. This was a calculation which was made for a zero temperature copper lattice and with a well-established pair potential. Pair potentials are suitable to simulate the properties of materials with metallic binding, but are inadequate for covalent materials. Recently, tractable empirical many body potentials have become available, which are suitable for materials like silicon and carb o n 21,22.

I15

~P

,03

90

91

79
o o o

tA P

Figure 1. A section of the graphite lattice in the molecular dynamics calculations. Only the surface layer atoms are shown. Also indicated is the regular grid of 300 impact points for incident atoms.

In spite of the expected shortcomings of the binary collisions approximation at lower energies, codes like TRIM have been widely applied in the modelling of plasma surface interactions in fusion plasma devices. This is because of their generality and speed of execution. Obviously it is then important to test the validity of the binary collisions approximation, in the first place by experiments. However, since experiments are difficult to perform in the 10-100 eV energy range, it is also interesting to compare TRIM predictions with calculations which include multiple interactions, and this is the purpose of the present report. We have chosen to compare TRIM and molecular dynamics in calculating the backscattering yield of carbon atoms at a graphite surface.
2. Calculations

For the binary collision calculations, a slightly modified version of TRIM85~6 has been used. The program uses the so-called universal interatomic potential ~6. The surface is modelled by a planar 7.4 eV surface potential. The target atoms are distributed randomly, and the projectile atom is subjected to binary collisions and to inelastic slowing down between collisions. In literature, attempts have been made to model surface roughness, e.g. by using a sawtooth shaped surface L s or a fractal surface 19in TRIM calculations. No such refinements are made here, a perfectly fiat surface is assumed. For the molecular dynamics calculations, we used a program which is a further development of the QDYN code 23. The program has been used previously for simulation of carbon selfsputtering 24"25. The 'two step A' integration method of ref 26 is used. A moving atom approximation is made, such that the equation of motion is integrated only for atoms which experience a force larger than 10-' N. The target is a lattice of 1342 atoms arranged in five layers, with the projectile atom incident on the (1000) surface. Figure 1 shows a section of the first atomic layer. In each simulation run, 300 projectile trajectories are calculated,
342

with impact point on the crystal surface distributed on a regular grid over the shaded area in Figure 1. Calculations have been performed for different angles of incidence 0 from the surface normal, different azimuthal angles ~p: 0 ~< q~ ~< 180 and different impact energies. As in the TRIM calculations, no account is taken of surface roughness, the target is a perfect crystal at zero temperature. For a number of selected sets of input parameters the moving atom approximation has been removed, the lattice has been heated to 2500 K or the target atoms have been randomly displaced according to a spherical gaussian distribution. neither of these tests has given significantly different results. The interatomic potential which has been used is a semi-empirical many body potential suggested by Tersoff 21'22. The form of the potential is chosen so as to reflect the fact that the bond strength between any two atoms decreases with increasing coordination of the two atoms to other neighbours. In all, the potential has 11 adjustable parameters, which were determined from the cohesive energies, elastic properties and defect energies in various carbon polytypes. The properties of diamond and the inplane properties of graphite have been shown to be well described by the potential 22, whereas the range is too short to model interplanar binding in graphite. The calculations have been performed on computers at the Manne Siegbahn Institute, mainly an Alliant FX/2824, a 31-100 VAX station and an Apollo 3500 work station. Typically a run with 300 trajectories takes 3-24 h on a single processor on the Alliant, twice longer on the VAX station and 10 times longer on the Apollo station.
3. Results

Figure 2 is a comparison of the backscattering yield from TRIM and molecular dynamics. The yield at normal incidence from TRIM is higher than that from Eckstein and Biersack by a factor two or so ' 7, whereas the yield at a 45 angle of incidence is similar, and the energy dependence is similar. For normal incidence the TRIM backscattering yield is everywhere less than 1% and drops steeply below 100 eV incident energy. The backscattering yield from molecular dynamics increases with decreasing energy from 50 eV, peaks around 20 eV with more than 40% backscattering and drops down below 10% at still lower energy. At a 45 angle of incidence the yield from molecular dynamics falls well below the TRIM prediction in the range 200-1000 eV, but peaks around 40 eV with unity yield. Figure 3 shows more in detail the backscattering yield from

t4 Bergs~ker et al. TRIM and molecular dynamics comparison

1.00 ~MolecuLor / " 0~-45~ dynomics ....~-,/1~_~

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.-

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0-45

I
I

I
I0

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Energy (eV)

I
I00

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[000

Figure 2. A comparison of the backscattering yield calculated with TRIM

and with molecular dynamics. The spline interpolation curves are to guide the eye. the plotted points for molecular dynamics with polar angle of incidence 0 = 45 are for azimuthal angle ~o = 0. The broken line represents calculations using MARLOWE 28 for these incident angles.

molecular dynamics as a function of incident energy and angle of incidence. The large majority of the calculated values are for azimuthal angle ~o = 0, in some cases they are an average o f many azimuthal angles. The dependence on the azimuthal angle appears to be weak. F o r instance, at 25 eV and with polar angle 0 = 30 , the yield varies between 0.25 and 0.32 for different azimuthal angles.
,1. D i s c u s s i o n

below 100 eV. The predicted backscattering yield in the molecular dynamics calculations is clearly large enough to be significant to impurity recycling in fusion devices, and to experiments where plasma ions or sputtered atoms are collected on surfaces. This is particularly true at non-normal incidence. It should be kept in mind that the angle of incidence of plasma ions is likely to be typically 30 , even if the magnetic field is normal to the surface 27. However, it is obvious that the case of a perfectly fiat surface does not correspond well to a real graphite surface. Since most of the reflection at grazing incidence occurs at specular angle it is likely to be much reduced for a rough surface. Note that in ref 15 the significant difference in collection efficiency was between rough graphite surfaces on the one hand, and polished graphite and other surfaces on the other hand. To understand the mechanism of backscattering in the model, it is necessary to study single events in more detail. As an illustrative example, consider the case where the projectile atom hits the target atom 91 (cf. Figure 1) in a head-on collision at normal incidence. Obviously, in the binary collision approximation there could be no backscattering in this case, since the projectile would transfer all its energy to the target atom. In the molecular dynamics calculations the system evolves as shown in Figures 4 and 5, where the normal velocities are plotted for the projectile (labelled 1), the target atom 91, its nearest neighbour 90 and the atom 358, which is situated in the second graphite plane, directly below

x IO s m/s

]For the present purpose the difference between the T R I M backscattering yield in this work and in ref 17 may be considered as minor, It may be due to the different interatomic potential or to different assumptions for surface binding energy and other details. The most striking result is that molecular dynamics predicts a high backscattering yield, even at normal incidence, at energies

E = leV f-~ 91

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Backscattering yield
-5

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-5

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o

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Time (femtoseconds) Figure 4. Normal velocities of the projectile (labelled I) and the target atoms 90, 91 and 358 in the case of the projectile hitting atom 91 in a head-on collision at normal incidence. Atom 90 is one of the nearest neighbours of atom 9 I. Atom 358 is situated in the second graphite plane directly below atom 91. 343

Figure 3. Backscattering yield from molecular dynamics. Calculations are

for every 5 eV and every 5 in angle of incidence, except in areas with zero or unity yield, where interpolation has been made. The yield at zero energy has been chosen as zero.

H Bergs~ker et al: T R I M and molecular dynamics comparison

x 103m/

5. Conclusions
_ I E = 58 eV

3o

.-~

91

>~

/ ~

358

~ to

It has been s h o w n h o w significant backscattering o f 10-50 eV c a r b o n a t o m s at n o r m a l incidence o n graphite surfaces is predicted from molecular dynamics calculations with m a n y body potential. This effect is n o t predicted in calculations based o n the binary collisions a p p r o x i m a t i o n , a n d if it occurs for real graphite surfaces it m a y be o f consequence to impurity recycling in fusion experiments, as well as to experiments where c a r b o n is collected o n surfaces for diagnostic purposes. Experimental tests are desirable.

Acknowledgements
J

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I
E " 6 0 eV

#--,

91

This work has been s u p p o r t e d by the British Science a n d Engineering Research Council (SERC) a n d by the Swedish N a t u r a l Science Research Council ( N F R ) . The a u t h o r s would also like to t h a n k the referee, D r I v a n C h a k a r o v , for the M A R L O W E calculations included in Figure 2.

References
N
N .

-IO

- -

I0

20

30

40

50

Time (femtoseconds)

Figure5. Normal velocities of the projectile (labelled 1) and the target

atoms 90, 91 and 958 in the case of the projectile hitting atom 91 in a head-on collision at normal incidence. Atom 90 is one of the nearest neighbours of atom 91. Atom 358 is situated in the second graphite plane directly below atom 91.

91. Positive velocities are directed into the crystal. A t low energy (Figure 4) a c o m p a r a t i v e l y large fraction o f the projectiles' forward m o m e n t u m is transferred to the nearest neighbours, note t h a t a t o m 90 is one o f three. A t 1 eV, however, a sufficient a m o u n t o f the projectile energy is dissipated for it to be t r a p p e d at the surface. A t 2 eV a n d above, the projectile is backscattered. As the projectile energy is increased, the collision with a t o m 91 becomes m o r e a n d m o r e like a binary collision, a n d at 58 eV a l m o s t all f o r w a r d m o m e n t u m is transferred to a t o m 91 (Figure 5), b u t the projectile is still backscattered, retaining very little energy. A b o v e 58 eV the projectile once again is n o t backscattered. This example shows t h a t the binary collision approxim a t i o n is i n a d e q u a t e below 60 eV for this particular system.

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