Simultaneous control of selectivity and yield of molecular dissociation Pulsed incoherent interference control Original Research Article

The theory of resonantly enhanced molecular dissociation induced by a two-pulse sequence to a continuum which is dressed by a third pulse is developed. Closed form expressions for the state preparation and evolution are derived within the adiabatic approximation. Non-approximate numerical calculations demonstrate that extensive branching ratio control and high dissociation yield (near 100 percent) are simultaneously achieved by varying the central frequencies of one pulse relative to another. The control characteristics are found to depend strongly on the ordering of the three-pulse sequence.