Design of Femtosecond Pulse Sequences to Control Photochemical Products

Abstract

The methodology of Optimal Control Theory (OCT) is applied to the design of optical femtosecond pulse sequences. Two studies are reported, involving different but related objectives. The first study concerns the design of pulses or pulse sequences to optimize electronic population inversion in a system consisting of two Born-Oppenheimer states. The second study involves the design of pulse sequences to control chemical arrangement channels in photodissociation. This latter study is an extension of earlier work by Kosloff et al. [4], but the techniques used here are refined and the yields vastly improved. The second study can be considered, in some sense, as the doubled version of the first study: the first study maximizes the pump pulse while the second study maximizes the pump-dump sequence to obtain a particular chemical objective.