Quantitative theory-versus-experiment comparison for the intense laser dissociation of H-2(+)

A detailed theory-versus-experiment comparison is worked out for H-2(+) intense laser dissociation, based on angularly resolved photodissociation spectra recently recorded in Figger's group. As opposite to other experimental setups, it is an electric discharge (and not an optical excitation) that prepares the molecular ion, with the advantage for the theoretical approach, to neglect without loss of accuracy, the otherwise important ionization-dissociation competition. Abel transformation relates the dissociation probability starting from a single rovibrational state to the probability of observing a hydrogen atom at a given pixel of the detector plate. Some statistics on initial rovibrational distributions, together with a spatial averaging over laser focus area, lead to photofragments kinetic spectra, with well separated peaks attributed to single vibrational levels. An excellent theory-versus-experiment agreement is reached not only for the kinetic spectra, but also for the angular distributions of fragments originating from two different vibrational levels resulting into more or less alignment. Some characteristic features can be interpreted in terms of basic mechanisms such as bond softening or vibrational trapping.