Computer Simulation of DIET Processes: Molecular Dynamics with Electronic Transitions
We describe our progress towards developing self-consistent methods for incorporating the effects of electronic transitions in molecular dynamics simulations. We employ a “surface-hopping” technique to allow switches between potential energy hypersurfaces when localized electronic state changes such as charge transfer occur. To describe dynamics at metal surfaces, we introduce electronic frictions and fluctuating forces to account for energy dissipation and excitation via electron-hole pair transitions. We present preliminary new results for CO on Cu(100) and discuss implications of our results on the possible mechanisms of desorption induced via rapid heating of conduction electrons.
KeywordsElectronic Transition Friction Matrix Pair Transition Pair Excitation Potential Energy Hypersurface
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- 1.See, for example, N. H. Tolk, M. M. Traum, J. C. Tully and T. E. Madey, Eds., Desorption Induced by Electronic Transitions, DIET I, (Springer-Verlag, Berlin, 1983).Google Scholar
- See especially the chapters by J. W. Gadzuk, D. R. Jennison, J. C. Tully, R. Gomer, D. Menzel, P. J. Feibelman, D. E. Ramaker and W. Brenig. See also, J. W. Gadzuk, in Desorption Induced by Electronic Transitions, DIET IV, G. Betz and P. Varga, Eds., (Springer-Verlag, Berlin, 1990), p.2.Google Scholar
- J. C. Tully, in Dynamics of Molecular Collisions, Part B, edited by W. H. Miller (Plenum, New York, 1976), p. 217.Google Scholar
- 5.P. Nordlander, in Desorption Induced by Electronic Transitions, DIET V, edited by A. R. Burns, E. B. Stechel and D. R. Jennison, this volume; See also, P. Nordlander and J. C. Tully, Phys. Rev. Lett. 61, 990 (1988).Google Scholar
- 9.M. Head-Gordon and J. C. Tully, unpublished.Google Scholar
- M. HeadGordon and J. C. Tully, Phys. Rev. B in press.Google Scholar
- E. B. Stechel, D. R. Jennison and A. R. Burns, in Desorption Induced by Electronic Transitions, DIET III, R. H. Stulen and M. L. Knotek, Eds., (Springer-Verlag, Berlin, 1987), p. 136.Google Scholar
- 15.J. A. Misewich, T. R Heinz and D. M. Newns, unpublished.Google Scholar