COHERENT RADIATIVE CONTROL OF MOLECULAR PHOTODISSOCIATION VIA RESONANT 2-PHOTON VERSUS 2-PHOTON INTERFERENCE

We show that resonant two-photon versus two-photon interference provides a means of controlling relative photodissociation cross sections even when the initial molecular system is in a mixed state, e.g. in thermal equilibrium. The resultant technique, which also allows cancellation of incoherences due to laser phase fluctuations and the reduction of uncontrolled background photodissociation contributions, is demonstrated computationally on Na2 photodissociation, where a wide range of control over branching into Na(3s) + Na(4s) versus Na(3s) + Na(3p) is achieved.