Theoretical investigation of the Freeman resonance in the dissociative ionization of $H_2+$

TL;DR

This paper uses full-dimensional quantum simulations to study how Freeman resonances influence the energy distribution in the dissociative ionization of $H_2^+$ under laser pulses, revealing deviations linked to ponderomotive energy.

Contribution

It provides a detailed theoretical analysis of Freeman resonances' role in $H_2^+$ ionization, highlighting their impact on energy sharing and deviations from classical energy relations.

Findings

Energy sharing in JES depends on pulse envelope shape.

Freeman resonances absorb ponderomotive energy U_p.

Deviations from expected energy relations are linked to Freeman resonances.

Abstract

The dissociative ionization of $H_2^+$ in linearly polarized, 400 nm laser pulses is simulated by solving a three-particle time-dependent Schr\"odinger equation in full dimensionality. The joint energy spectra (JES) are computed for $\cos^8$ and flat-top envelopes using the time-dependent surface flux (tSurff) methods. In JES, the energy sharing $n$ photon energies $\omega$ of nuclear kinetic energy release (KER) $E_N$ and electronic KER $E_e$ are well represented by $E_N+E_e=n\omega-U_p+E_0$ for $\cos^8$ pulses, but satisfy $E_N+E_e=n\omega+E_0$ for flat-top envelope, exposing a deviation of the ponderomotive energy $U_p$, which has been observed in experiments, where $E_0$ is the ground energy of $H_2^+$. The analysis of the wavefunction for electrons and protons after the pulse are presented, where we find $U_p$ is absorbed by the Freeman resonances between two excited ungerade states.