Disentangle pathways in strong field molecular photoionization byangular distribution of dissociation fragments

TL;DR

This paper investigates how angular distributions of dissociation fragments can reveal population exchange pathways in strong field molecular photoionization, enabling detailed analysis of ion core dynamics through energy spectra.

Contribution

It introduces a method to disentangle and classify population redistribution mechanisms in molecular ionization using angle-resolved kinetic energy spectra.

Findings

Disentangled first and higher order population exchange processes.

Demonstrated the use of KER spectra to determine pathway branching ratios.

Showed pump intensity dependence reveals pathway dynamics.

Abstract

In strong field ionization, the pump pulse not only photoionizes the molecule, but also drives efficient population exchanges between its ionic ground and excited states.In this study, we investigated the population dynamics accompanying strong field molecular photoionization, using angular distribution of dissociative fragments after ionization.Our results reveal that the first and higher order processes of the post-ionization population redistribution mechanism (PPRM) in the ion core can be disentangled and classified by {its} angle-resolved kinetic energy release (KER) spectra.We demonstrate that the imprints of PPRM in the KER spectra can be used to determine the branching ratio of the population exchange pathways of different orders, by exploiting the pump intensity dependent variation of the spectra.