Enhanced selectivity and yield in multichannel photodissociation reactions: application to CH3I.

We develop a method to improve the population transfer and final-channel control of multichannel photodissociation reactions. The method is applied to the photodissociation of methyl iodide, CH3(v)+I*(2P1/2)<--CH3I-->CH3(v)+I(2P3/2). Our method is based on simultaneously exciting many two-photon pathways that lead to the same final outcome, each proceeding via a different intermediate bound state. The selectivity of the final product state(s) is a result of coherently controlled interference between the quantum pathways. The improvement in the population transfer yield from the ground state to the selected dissociative channel(s) is made possible by executing the process in an adiabatic fashion.