Probing Vibronic Coherence in Charge Migration of Molecules Using Strong Field Sequential Double Ionization

TL;DR

This paper introduces a new method using strong field sequential double ionization to directly probe vibronic coherence during charge migration in molecules, demonstrated through simulations on N₂ and O₂.

Contribution

The study presents a novel experimental scheme and simulation framework for observing vibronic coherence in charge migration, advancing the capabilities of molecular dynamics analysis.

Findings

Vibronic coherence imprints on kinetic energy spectra and dissociation ratios.

Simulations confirm the feasibility of the proposed probing method.

The DM-SDI model effectively accounts for molecular orientations in the analysis.

Abstract

We propose a novel scheme for probing vibronic coherence in charge migration in molecules utilizing strong field sequential double ionization. To demonstrate the feasibility of this approach, we perform full simulations of a pump-probe scheme employing few-cycle intense infrared pulses for N$_2$ and O$_2$. We predict that the vibronic coherence between the pumped states will be directly imprinted in experimental observables such as kinetic energy release spectra and branching ratios of the dissociative dications. Our simulations are based on the recently developed DM-SDI model, which is capable of efficiently accounting for molecular orientations and enabling direct comparison with experimental results. Our findings strongly encourage the use of this probing scheme in future charge migration experiments.