A classical trajectory surface hopping approach to non-adiabatic molecule-surface processes

Abstract

Scattering processes of diatomic molecules from solid surfaces in which the molecular affinity level crosses the surface Fermi level thus enabling charge transfer back and forth between the metal and molecule are considered here. The nuclei are assumed to move classically on a single model potential energy surface until a diabatic potential energy surface crossing is reached. At such points the trajectory is split into branches, each of which follows a different potential surface. The probability for hopping onto a new potential energy surface or remaining on the initial one is determined within the Landau-Zener-Tully-Preston picture. The phase averaged outgoing vibrational energy as well as the average residence time of the molecular ion resonances have been calculated as a function of the incident kinetic energy treating the off-diagonal matrix element within the Landau-Zener branching probabilities parametrically.