Laser-induced Electron-Transfer in the Dissociative Multiple Ionization of Argon Dimers

TL;DR

This study combines experimental and theoretical approaches to investigate laser-induced electron transfer in argon dimers, revealing sub-cycle electron dynamics and phase shifts that enable control of molecular processes with intense laser pulses.

Contribution

It demonstrates for the first time that intense laser fields can induce and control electron transfer between distant atoms in a molecule, affecting fragmentation dynamics.

Findings

Identification of a phase-shift in electron emission asymmetry due to electron transfer.

Observation of sub-cycle electron-electron interaction dynamics.

Evidence of laser-driven control over molecular electronic processes.

Abstract

We report on an experimental and theoretical study of the ionization-fragmentation dynamics of argon dimers in intense few-cycle laser pulses with a tagged carrier-envelope phase. We find that a field-driven electron transfer process from one argon atom across the system boundary to the other argon atom triggers sub-cycle electron-electron interaction dynamics in the neighboring atom. This attosecond electron-transfer process between distant entities and its implications manifest themselves as a distinct phase-shift between the measured asymmetry of electron emission curves of the $\text{Ar}^{+}+\text{Ar}^{2+}$ and $\text{Ar}^{2+}+\text{Ar}^{2+}$ fragmentation channels. Our work discloses a strong-field route to controlling the dynamics in molecular compounds through the excitation of electronic dynamics on a distant molecule by driving inter-molecular electron-transfer processes.