Two-pulse coherent control of electronic states in the photodissociation of IBr: Theory and proposed experiment

It is shown how the principles of coherent control can be applied to a pulsed experiment aimed at controlling curve-crossing processes. A realistic computational study (incorporating the ground, A, B, and Y electronic states of IBr) of control of atomic states produced in the photodissociation of IBr is presented. The suggested scheme, which consists of applying an excitation pulse followed by a dissociation pulse, is theoretically shown to yield essentially total control over the Br*/Br atomic branching ratio. It is shown that the only external parameters that need to be varied are the central frequency of the excitation pulse and the time delay between the two pulses. A brief description of a proposed experiment is provided.