H2double ionization with few-cycle laser pulses

Abstract

The temporal dynamics of double ionization of ${\text{H}}_{2}$ has been investigated both experimentally and theoretically with few-cycle laser pulses. The main observables are the proton spectra associated with the ${\text{H}}^{+}+{\text{H}}^{+}$ fragmentation channel. The model is based on the time-dependent Schr\odinger equation and treats the electronic and nuclear coordinates on the same level. Therefore it allows the ultrafast nuclear dynamics to be followed as a function of the laser pulse duration, carrier-envelope phase offset, and peak intensity. We mainly report results in the sequential double-ionization regime above $2\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}\text{W}\phantom{\rule{0.2em}{0ex}}{\text{cm}}^{\ensuremath{-}2}$. The proton spectra are shifted to higher energies as the pulse duration is reduced from 40 down to 10 fs. The good agreement between the model predictions and the experimental data at 10 fs permits a theoretical study with pulse durations down to a few femtoseconds. We demonstrate the very fast nuclear dynamics of the ${\text{H}}_{2}{}_{+}$ ion for a pulse duration as short as 1 fs between the two ionization events, giving $\text{H}_{2}{}^{+}$ from ${\text{H}}_{2}$ and ${\text{H}}^{+}+{\text{H}}^{+}$ from $\text{H}_{2}{}^{+}$. The carrier-envelope phase offset plays a significant role only for pulse durations shorter than 4 fs. At 10 fs, the laser intensity dependence of the proton spectra is fairly well reproduced by the model.