Stimulated emission processes and strong field effects in ultrashort pulse excitation of a predissociative molecule Original Research Article

We study the interaction of a diatomic molecule with two ultrashort and strong laser pulses. The first pulse prepares a wave packet in a dissociative electronic state which is coupled non-adiabatically to the bound electronic ground state. The conditions under which it is possible to stimulate parts of the wave packet back down to the ground state, a process which competes with excitation to a higher electronic state, are investigated. The results show to which extent it is possible to selectively transfer population between bound and dissociative states and thus influence the yield of a simple chemical reaction.