Dissociative ionization of H$_2^+$: Few-cycle effect in the joint electron-ion energy spectrum

TL;DR

This paper investigates how few-cycle infrared laser pulses influence the dissociative ionization of H$_2^+$, revealing pulse-dependent modulation effects linked to transient excited state populations, using ab initio simulations and simplified models.

Contribution

It demonstrates that the modulation in ionization probability is due to transient excited states, not vibrational excitations, providing new insights into ultrafast molecular ionization dynamics.

Findings

Ionization probability shows strong pulse-dependent modulation.

Modulation is linked to transient population of excited electronic states.

Simplified models confirm the role of excited states in ionization dynamics.

Abstract

Joint electron-ion energy spectra for the dissociative ionization of a model H$_2^+$ in few-cycle, infrared laser pulses are calculated via the numerical ab initio solution of the time-dependent Schr\"odinger equation. A strong, pulse-dependent modulation of the ionization probability for certain values of the protons' kinetic energy (but almost independent of the electron's energy) is observed. With the help of models with frozen ions, this feature---which mistakenly might be attributed to vibrational excitations---is traced back to the transient population of electronically excited states, followed by ionization. This assertion is further corroborated employing a two-level model incorporating strong-field ionization from the excited state.