title: Electronic dynamics by ultrafast pump photoelectron detachment probed by ionization: a dynamical simulation of negative-neutral-positive in LiH(-).
abstract: The control of electronic dynamics in the neutral electronic states of LiH before the onset of significant nuclei motion is investigated using a negative-neutral-positive (NeNePo) ultrafast IR pump-attoescond pulse train (APT) probe scheme. Starting from the ground state of the anion (LiH(-)), multiphoton ultrafast electron detachment and subsequent excitation of the neutral by a few femtosecond intense IR pulse produces a non-equilibrium electronic density in neutral LiH. The coherent electronic wave packet is then probed by angularly resolved photoionization to the cation by an APT generated from a replica of the pump IR pulse at several time delays. Realistic parameters for the pump and the APT are used. Several NeNePo schemes are simulated using different IR carrier frequencies, showing that the delay between the successive attosecond pulses in the train can be used as a filter to probe the different pairs of states present in the coherent electronic wave packet produced by the pump pulse. The dynamical simulations include the pump and the probe pulses to all orders by solving the time-dependent Schrödinger equation using a coupled equation scheme for the manifolds of the anion, neutral, and cation subspaces. We show that an incomplete molecular orientation of the molecule in the laboratory frame does not prevent probing the electronic density localization by angularly resolved photoelectron maps.
authors.affiliation: Department of Chemistry, B6c, University of Liège , B4000 Liège, Belgium.
authors.forename: B
authors.initials: B
authors.lastname: Mignolet
authors.forename: R D
authors.initials: RD
authors.lastname: Levine
authors.forename: F
authors.initials: F
authors.lastname: Remacle