Attosecond pump-probe transition-state spectroscopy of laser-induced molecular dissociative ionization: adiabatic versus nonadiabatic dressed-state dynamics

Abstract

We discuss how a recent pump-probe study [Kelkensberg et al., Phys. Rev. Lett. 103, 123005 (2009)] of the dissociative ionization of H2, under the combined effect of a single extreme ultraviolet attosecond pulse and an intense near- infrared pulse, actually represents a transition-state spectroscopy of the strong-field dissociation step, i.e., of the (probe-pulse-)dressed H2+ molecular ion. The way the dissociation dynamics is influenced by the duration of the near-infrared probe pulse, and by the time delay between the two pulses, is discussed in terms of adiabatic versus nonadiabatic preparation and transport of time-parametrized Floquet resonances associated with the dissociating molecular ion. Under a long probe pulse, the field-free vibrational states of the initial wave packet are transported, in a one-to-one manner, onto the Floquet resonances defined by the field intensity of the probe pulse and propagated adiabatically under the pulse. As the probe pulse duration shortens, nonadiabatic transitions between the Floquet resonances become important and manifest themselves in two respects: first, as a vibrational shake-up effect occurring near the peak of the short pulse, and second, through strong interference patterns in the fragment's kinetic energy spectrum, viewed as a function of the time delay between the pump and the probe pulses.