Control of charge migration in molecules by ultrashort laser pulses

TL;DR

This paper demonstrates how ultrashort laser pulses can control charge migration in molecules, enabling localization of charge and influencing subsequent molecular reactivity through ab initio calculations.

Contribution

It introduces a scheme for controlling charge migration with a single ultrashort laser pulse, supported by ab initio simulations on complex molecules.

Findings

Simple laser pulses can halt charge-migration oscillations.

Charge can be localized on specific molecular sites.

Control influences subsequent nuclear rearrangements.

Abstract

Due to electronic many-body effects, the ionization of a molecule can trigger ultrafast electron dynamics appearing as a migration of the created hole charge throughout the system. Here we propose a scheme for control of the charge migration dynamics with a single ultrashort laser pulse. We demonstrate by fully ab initio calculations on a molecule containing a chromophore and an amine moieties that simple pulses can be used for stopping the charge-migration oscillations and localizing the charge on the desired site of the system. We argue that this control may be used to predetermine the follow-up nuclear rearrangement and thus the molecular reactivity.