Orbital alignment and electron control in photodissociation products by two-color laser interference

Abstract

Time-dependent coupled equations are used to illustrate the laser control of the spatial orientation of diatomic photodissociation products and the concomitant orbital alignment of the electrons in the atomic fragments along the dissociation orientation. Such asymmetrical photodissociation and its control can be achieved by symmetry-breaking interference between two multiphoton pathways which produce isoenergy states of different symmetry. Conditions for this new laser control scenario are obtained for the simultaneous photodissociation of the 1 1Π u and 1 1Π g states of Cl 2 by a two-color laser multiphoton absorption with subpicosecond pulses.