Quantum Dynamics of $H_2^+$ in Orthogonal Two-Color Fields

Abstract

We present full-dimensional quantum simulations of $H_2^+$ dissociative ionization driven by strong orthogonal laser fields. We consider equal-frequency orthogonal components, which generate elliptical or circular polarization depending on their relative phase and amplitude, as well as orthogonal $800$- and $400$-nm two-color fields. These two-dimensional fields strongly modify the fragmentation dynamics. Most notably, we identify a high-energy peak in the proton kinetic-energy-release (KER) spectrum at approximately $4-5$ eV that is absent from the corresponding single-color, linearly polarized calculations. The yield of this peak can be coherently controlled by varying the relative carrier-envelope phase of the perpendicular field component. The perpendicular field also disrupts the clear electron-proton energy-sharing pattern observed in the main $3-3.5$ eV dissociation channel, indicating more complex multichannel dynamics. Time-dependent state projections and calculations initiated from individual excited states attribute the additional peak to laser-induced vibrational excitation of $H_2^+$. Furthermore, the perpendicular field rotates the fragment angular distributions, causing the most probable proton and electron emission directions to deviate substantially from the principal $z$ axis. These findings demonstrate that the spatial and temporal geometry of orthogonal laser fields provides an additional degree of freedom for controlling ultrafast electron-nuclear dynamics.