Laser control of photopredissociation angular distributions and photoionization in Cl2 by two color interference

A coupled equations approach based on a general artificial channel method is used to demonstrate two color laser coherent control of photopredissociation and photoionization in Cl2. Photopredissociation of the 1Πg states of Cl2 is suppressed by a two plus four photon interference process 2ω2=4ω4, whereas the photoionization is controlled by interference between a six photon transition and a four photon transition 6ω4=2ω2+2ω4 using the same 1Πg photopredissociation resonances as intermediates. Photopredissociation angular distributions illustrate the suppression of the corresponding transition in selective rotational states.