Correlation-Driven Charge Migration as Initial Step in the Dynamics in Correlation Bands

TL;DR

This paper investigates how electron correlation causes charge migration in ionized molecules, leading to increased stability and providing insights into ultrafast molecular relaxation relevant for attochemistry.

Contribution

It introduces a dynamics-based explanation for charge migration in correlation bands, connecting theoretical calculations with recent experimental findings.

Findings

Charge migration can stabilize ionized molecules.

Correlation-driven charge redistribution occurs rapidly.

Implications for ultrafast molecular relaxation and attochemistry.

Abstract

We present dynamics calculations showing how electron-correlation-driven charge migration occurring in the correlation band of ionized molecules can lead to a redistribution of the charge increasing the stability of the system. These calculations offer an interpretation of recent experimental results obtained for adenine. We discuss the implications of the mechanism for the development of attochemistry and how it can be understood in the context of the ultrafast, non-adiabatic relaxation taking place in highly-excited molecular cations.