In the framework of a unified kinetic theory of particle–surface interactions, dependences of the relaxation, accommodation, and trapping of molecules on their angular momentum J are discussed. One of the basic parameters of the theory, the free flight time through the interaction region, is calculated using a simple model potential for which the classical equations of motion can be integrated analytically. With increasing J, an increase in molecular relaxation and accommodation is predicted at small J, and a decrease at larger J. These results constitute a microscopically founded interpretation of recent experiments on surface light-induced drift.
Articles you may be interested inEfficient vibrational and translational excitations of a solid metal surface: State-to-state time-of-flight measurements of HCl ( v = 2 , J = 1 ) scattering from Au (111) Rotational and vibrational wave packet motion during the infrared multiphoton excitation of HF State-to-state unimolecular reaction dynamics of HOCl near the dissociation threshold: The role of vibrations, rotations, and IVR probed by time-and eigenstate-resolved spectroscopy Experiments using surface light-induced drift are performed to yield information on the rotational (J) and vibrational (v) state dependence of molecule-surface interactions. Data are presented for the change in accommodation coefficient for tangential momentum transfer ␣ upon excitation of HF interacting with a polycrystalline LiF surface ͑on a Cu substrate͒ and a hydrophobic stearic-acid monolayer ͑on a stainless-steel substrate͒. We employed both P-and R-branch excitation of HF in the fundamental vibrational band (vϭ0→1) with Jϭ0 -4, using a continuously tunable color-center laser (Ϸ2.5 m). By combining the results for the P-and R-branch, we find that the influences of J and v upon the molecule-surface interaction can be considered independent to a good approximation. It is found that ␣ decreases upon vibrational excitation vϭ0→1, whereas it increases with increasing J. The J and v dependences of ␣ are discussed in the framework of a unified kinetic theory of molecule-surface interaction.
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