Abstract
A General method of controlling branching (direct and resonant) unimolecular reactions, using the coherence of lasers is presented. It is shown that pre-selected products may be obtained, in preference to others, as a result of interference between decay channels of a superposition of degenerate continuum states. It is shown that such states can be prepared by exciting a superposition of bound states using two coherent light sources with a well defined relative phase. Theoretical limits of coherent control, in direct and compound (statistical like) processes are derived. Enhanced (often 100%) yields of the (chemical) products of interest are obtained. Computational results on the I*/I branching ratios in the photodissociation of FI and CH3I, including the effects of initial conditions are presented. In addition, complete blocking-off of a single pre-selected quantum state of a given reaction product, resulting in population inversion with respect to all higher energetic levels, is shown to be attainable.
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