Energy redistribution and dissociation in molecule-surface collisions involving charge transfer/surface hopping

Abstract

In analogy with resonance electron scattering from molecules in which substantial high vibrational overtone losses are observed, beams of diatomic molecules scattered from solid surfaces could emerge highly vibrationally excited due to the formation of temporary negative molecular ions resulting from charge transfer between the solid and molecule on the inward and outward legs of the scattering trajectory. In the proesent work, the exact classical trajectories for the diatomic molecule, including internal vibrational motion, are calculated for motion over model diabatic potential surfaces in which surface hopping due to charge transfer/harpooning is accounted for. From these calculations, the probability for translational to vibrational energy transfer are obtained as a function of incident kinetic energy and system parameters. Contact is also established with the concept of vibrationally assisted sticking and dissociative adsorption.