Floquet surface hopping: Laser-driven dissociation and ionization dynamics ofH2+

Abstract

A quantum-classical approach is developed to describe the strong-field molecular dynamics of ${{\mathrm{H}}_{2}}^{+}$, taking into account all degrees of freedom and simultaneously dissociation as well as ionization. The electron and nuclei are treated correlated, by propagating the nuclei stochastically on potential energy surfaces. It is demonstrated that Floquet surface hopping (FSH) is particularly well suited to describe the laser-driven dynamics. The method is tested against exact solutions of the time-dependent Schr\odinger equation, where available. In addition, the FSH results are in excellent agreement with recent experimental data of the dissociation and ionization dynamics of ${{\mathrm{H}}_{2}}^{+}$. As an additional issue of this work, the primary importance of the focal volume average is worked out for the understanding of experimental results. It determines the gross features of the experimental spectra and provides also a natural explanation of the puzzling saturation effect in the dissociation spectra, observed experimentally. Future applications and further extensions of the method are discussed.