Journal of Chemical Physics, Vol.109, No.7, 2856-2864, 1998
Formation and dynamics of hot-precursor hydrogen atoms on metal surfaces : Trajectory simulations and stochastic models
The results of a theoretical study of H atoms colliding with a Cu(lll) surface are presented. The metal is treated as a five-layer slab of 150 atoms, and all dynamics are classical. The formation of trapped ''hot-precursor'' atoms on the surface is examined, as well as the nature of their motion on the surface and their energy and momentum dissipation. Connections are made with recent Eley-Rideal experiments, for which hot-atom precursors may play an important role. To facilitate future simulations of Eley-Rideal and hot-atom reactions on metals, simple stochastic models are developed to describe hot-atom energy dissipation. A Fokker-Planck equation is used to model the hot-atom energy distribution. Quasi-Langevin terms, which simulate fluctuation and dissipation consistent with this Fokker-Planck description, are developed for the hat-atom equations of motion. These quasi-langevin terms are different from the hydrodynamic forms used for Brownian-type motion.
Keywords:ELEY-RIDEAL MECHANISM;RECOMBINATIVE DESORPTION;GAS-PHASE;VIBRATIONAL-EXCITATION;H-ABSTRACTION;CU(111);MOLECULES;DEUTERIUM;INCIDENT;KINETICS