Abstract

Photodesorption may be initiated by resonant, laser-induced excitation of an internal vibrational mode of an adsorbed molecule. The desorption kinetics are predicted from a quantum-statistical theory based on a master equation describing phonon- and photon-assisted molecular transitions as well as elastic tunneling processes. The desorption rate frequently follows a power law rdIα as a function of laser intensity I that depends on the energetics of the adsorption system and on the efficiency of energy transfer from the vibrational mode to the surface bond and into the solid. The calculated line shape can differ markedly from the corresponding infrared absorption spectrum because of nonlinear intensity effects, vibrational anharmonicity, surface heterogeneity, vibrational (V–V) energy transfer, and multiquanta processes.

© 1987 Optical Society of America

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