Selecting two-photon sequential ionization pathways in H2 through harmonic filtering.

Recent experiments in gas-phase molecules have shown the versatility of using attosecond pulse trains combined with IR femtosecond pulses to track and control excitation and ionization yields on the attosecond timescale. The interplay between electron and nuclear motions drives the light-induced transitions favoring specific reaction paths, so that the time delay between the pulses can be used as the tracking parameter or as a control knob to manipulate the molecular dynamics. Here, we present ab initio simulations on the hydrogen molecule to demonstrate that by filtering the high harmonics in an attosecond pulse train one can quench or enhance specific quantum paths thus dictating the outcome of the reaction. It is then possible to discriminate the dominant sequential processes in two-photon ionization, as for example molecular excitation followed by ionization or the other way around. More interestingly, frequency filters can be employed to steer the one- and two-photon yields to favor electron emission in a specific direction.

Direct and Sequential Two-Photon Double Ionization of Two-Electron Quantum Dots.

In this work we study the double ionization yields and kinetic energy spectra of a two-electron spherical quantum dot (QD) exposed in laser fields. The theoretical description is based on an ab initio nonperturbative configuration interaction theory capable of describing the two-electron QD dynamics in THz and mid-IR ultrashort laser fields. The QD's confinement potential is approximated to have a Gaussian-like spatial dependence. We have found that significant variations of the two-electron kinetic energy patterns and two-photon double ionization yields occur as we vary the QD's size. For a given laser pulse, the double ionization yield increases by orders of magnitude when the dot size is reduced. The size of the QD determines the sequential or direct character of the two-photon double ionization process. Provided that it is energetically allowed, the sequential two-photon double ionization process, requiring minimal interelectronic correlations, becomes dominant over the direct one. In the sequential regime, the corresponding two-electron kinetic energy spectrum changes from a broadened single-peaked to a doubly peaked one. Moreover, we also have identified features in the spectrum that are distinctively different than those in its atomic counterpart.

Clocking ultrafast wave packet dynamics in molecules through UV-induced symmetry breaking.

We investigate the use of UV-pump-UV-probe schemes to trace the evolution of nuclear wave packets in excited molecular states by analyzing the asymmetry of the electron angular distributions resulting from dissociative ionization. The asymmetry results from the coherent superposition of gerade and ungerade states of the remaining molecular ion in the region where the nuclear wave packet launched by the pump pulse in the neutral molecule is located. Hence, the variation of this asymmetry with the time delay between the pump and the probe pulses parallels that of the moving wave packet and, consequently, can be used to clock its field-free evolution. The performance of this method is illustrated for the H(2) molecule.

Nuclear interference in the Coulomb explosion of H2+ in short vuv laser fields.

We report ab initio calculations of H2+ three-photon ionization by vuv/fs 10(12) W/cm(2) laser pulses including electronic and vibrational degrees of freedom in the Born-Oppenheimer approximation. The initial nuclear wave packet of H2+(1ssigma(g)) is assumed to be equal to the H2 vibrational ground state. For pulse durations longer than 10 fs, we find an unexpected modulation in the kinetic energy spectra of the correlated fragments (H++H+). It is shown that the structures in the spectra originate from the interference between a direct and a sequential dissociation channel. While the first channel is open even for relatively short pulses, the sequential one only opens for pulse durations longer than 10 fs. In the latter case we show that interference between the two components results in a modulated kinetic energy release spectrum in the dissociation channel 3dsigma(g), which is reflected in the ionization spectrum.