Enhanced dissociation of H2+ into highly excited states via laser-induced sequential resonant excitation

TL;DR

This paper investigates how uv laser pulses can enhance the dissociation of H$_2$$^+$ into highly excited states through a sequential resonant excitation mechanism, revealing critical photon energies that optimize this process.

Contribution

It introduces a detailed quantum dynamical study showing the role of sequential resonant excitation in controlling molecular dissociation into excited states.

Findings

Significant dissociation enhancement at specific photon energies.

Identification of a sequential excitation mechanism.

Correlation between photon energy and dissociation pathways.

Abstract

We study the dissociation of H$_2$$^+$ in uv laser pulses by solving the non-Born-Oppenheimer time-dependent Schr\"{o}dinger equation as a function of the photon energy $\omega$ of the pulse. Significant enhancements of the dissociation into highly excited electronic states are observed at critical $\omega$. This is found to be attributed to a sequential resonant excitation mechanism where the population is firstly transferred to the first excited state by absorbing one photon and sequentially to higher states by absorbing another one or more photons at the same internuclear distance. We have substantiated the underlying dynamics by separately calculating the nuclear kinetic energy spectra for individual dissociation pathways through different electronic states.