Electron control in photodissociation by two-color multiphoton processes Original Research Article

Numerical solutions of coupled time-dependent Schrödinger equations for multiphoton excitation of the Cl2 molecule are used to illustrate the principle of electron control in photodissociation. Thus using a symmetry breaking laser-induced interference between two multiphoton pathways which produce isoenergy states of different symmetry, we have shown that it is possible to separate atomic fragments with different electron configurations. Laser alignment by rotational pumping at high intensity enhances the separation of the products. Temperature effects are shown to destroy the asymmetry or anisotropies in the angular distributions which are essential to the separation of the distinct photofragments.