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.
KeywordsCoherence Carbon Monoxide Rosen
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