Stochastic wave packet approach to nonadiabatic scattering of diatomic molecules from metals.

Abstract

In this contribution, we present a quantum dynamical approach to study inelastic scattering of diatomic molecules from metal surfaces at normal incidence. The dissipative dynamics obeys a stochastic Schrödinger equation describing the time-evolution of the system as a piecewise deterministic process. Energy exchange between the molecular vibrational degrees of freedom and the metal electrons is represented using operators in tensor product form, which are coupled via anharmonic transition rates calculated from first-order perturbation theory. Full dimensional observables are obtained by averaging over simulations in 4D-including the internal stretch, the distance to the surface, and the orientation angles-at different surface sites. The method is applied to the state-resolved scattering of vibrationally excited NO from Au(111), revealing important channels for quantized energy relaxation.