Strong-field molecular ionization beyond the single active electron approximation.

This work explores quantitative limits to the single-active electron approximation, often used to deal with strong-field ionization and subsequent attosecond dynamics. Using a time-dependent, multiconfiguration approach, specifically the time-dependent configuration interaction method, we solve the time-dependent Schrödinger equation for the two-electron dihydrogen molecule with the possibility of tuning at will the electron-electron interaction by an adiabatic switch-on/switch-off function. We focus on signals of the single ionization of H2 under a strong near-infrared, four-cycle, linearly polarized laser pulse of varying intensity and within a vibrationally frozen molecular model. The observables we address are post-pulse total ionization probability profiles as a function of the laser peak intensity. Three values of the internuclear distance R taken as a parameter are considered, R = Req = 1.4 a.u. for the equilibrium geometry of the molecule, R = 5.0 a.u. for an elongated molecule, and R = 10.2 a.u. for a dissociating molecule. The most striking observation is the non-monotonous behavior of the ionization probability profiles at intermediate elongation distances with an instance of enhanced ionization and one of partial ionization quenching. We give an interpretation of this in terms of a resonance-enhanced-multiphoton ionization mechanism with interfering overlapping resonances resulting from excited electronic states.

Molecular dissociative ionization and wave-packet dynamics studied using two-color XUV and IR pump-probe spectroscopy.

We present a combined theoretical and experimental study of ultrafast wave-packet dynamics in the dissociative ionization of H_{2} molecules as a result of irradiation with an extreme-ultraviolet (XUV) pulse followed by an infrared (IR) pulse. In experiments where the duration of both the XUV and IR pulses are shorter than the vibrational period of H_{2};{+}, dephasing and rephasing of the vibrational wave packet that is formed in H_{2};{+} upon ionization of the neutral molecule by the XUV pulse is observed. In experiments where the duration of the IR pulse exceeds the vibrational period of H_{2};{+} (15 fs), a pronounced dependence of the H;{+} kinetic energy distribution on XUV-IR delay is observed that can be explained in terms of the adiabatic propagation of the H_{2};{+} wave packet on field-dressed potential energy curves.