Identifying Strong-Field Effects in Indirect Photofragmentation Reactions.

Exploring molecular breakup processes induced by light-matter interactions has both fundamental and practical implications. However, it remains a challenge to elucidate the underlying reaction mechanism in the strong field regime, where the potentials of the reactant are modified dramatically. Here we perform a theoretical analysis combined with a time-dependent wavepacket calculation to show how a strong ultrafast laser field affects the photofragment products. As an example, we examine the photochemical reaction of breaking up the molecule NaI into the neutral atoms Na and I, which due to inherent nonadiabatic couplings are indirectly formed in a stepwise fashion via the reaction intermediate NaI*. By analyzing the angular dependencies of fragment distributions, we are able to identify the reaction intermediate NaI* from the weak to the strong field-induced nonadiabatic regimes. Furthermore, the energy levels of NaI* can be extracted from the quantum interference patterns of the transient photofragment momentum distribution.