Date Published:

DEC 22

Abstract:

Quantum and mixed quantum/classical calculations of the photolysis of a HCl adsorbate on a MgO surface are reported. In the quantum calculation of the hydrogen dynamics (with rigid surface and chlorine atoms) a strong oscillatory structure is found in the angular distribution of the photofragmented hydrogen as well as in the absorption spectrum. These resonances are caused by temporary trapping of the hydrogen atom between the chlorine atom and the surface and reflect the initial perpendicular adsorption geometry. Corrugation of the surface potential leads to a significant modification of these interference patterns, which exist even for a flat surface. Within a mixed quantum/classical time-dependent self-consistent field (Q/C TDSCF) propagation the influence of surface degrees of freedom on the interference patterns is investigated. The thermal motion of the surface and inelastic collisions of the hydrogen atom with the surface and the chlorine atom washes out most of the oscillatory structure. In the fully angular and energy resolved spectra nevertheless clearly distinguishable peaks are seen. They can be used in practice to extract information about adsorption geometry and surface potential parameters. (C) 1996 American Institute of physics.