Abstract
The theoretical formulation of a frequency response technique, based on surface temperature modulation, for the study of surface reaction dynamics is described in detail. The formalism is developed for analyzing adsorption, desorption, and both unimolecular and bimolecular surface reactions. The evaluation of the activation barriers for the elementary surface reactions is straightforward even in the presence of strong nonlinearities and requires no knowledge of the composition or configuration (i.e., structure) of the adlayer. This capability provides a distinct advantage over competitive techniques such as modulated molecular beam reactive scattering. Although the evaluation of the preexponential factors of the rate coefficients is complicated by the presence of nonlinear effects (e.g., coverage-dependent rate parameters or a bimolecular reaction), in many cases the preexponential factors may also be evaluated in a straightforward manner.
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