Photodissociation and photodesorption line shapes

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Abstract
Photodissociation line shapes are derived based on two‐level‐plus‐decay models. The simplest model involves only dissociative decay of the upper level and applies to laser‐induced vibrational predissociation of van der Waals molecules. A more general model which includes quenching processes that compete with dissociation is presented in a form applicable to laser‐induced desorption. Both models yield insightful line shape expressions with explicit dependence on laser power and frequency, irradiation time, absorption strength, and phenomenological rate constants. Implications of the line shape formulas for several recent experiments as well as feasibility of studying more complex systems are discussed.