Ab initio time-dependent method to study the hydrogen molecule exposed to intense ultrashort laser pulses

An ab initio non-perturbative time dependent method to describe ionization of molecular systems by ultrashort (femtosecond) laser pulses has been developed. The method allows one to describe competing processes such as non dissociative ionization, dissociative ionization and dissociation into neutrals, including the possibility of autoionization. In this work we assess the validity of the method by applying it to different physical situations and by comparing with results previously obtained within stationary perturbation theory. In particular, it is shown that inclusion of the nuclear motion is essential to describe H-2 resonance enhanced multiphoton ionization and interferences mediated by H-2 autoionizing states. (c) 2007 Elsevier B.V. All rights reserved.