Monitoring Nonadiabatic Electron-Nuclear Dynamics in Molecules by Attosecond Streaking of Photoelectrons

TL;DR

This paper extends attosecond streaking techniques to monitor real-time non-adiabatic electron-nuclear dynamics in molecules, enabling direct observation of electronic coherences during critical photochemical processes.

Contribution

It introduces a new formalism for streaking that includes coupled electron and nuclear motions, providing a novel tool for studying non-adiabatic molecular dynamics.

Findings

Demonstrates how streaking reveals electronic coherences.

Shows potential to monitor dynamics near conical intersections.

Enhances temporal resolution of molecular processes.

Abstract

Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an additional phase information, which can be retrieved by the streaking technique. In this contribution we extend the streaking formalism to include coupled electron and nuclear dynamics in molecules as well as initial coherences and demonstrate how it offers a novel tool to monitor non-adiabatic dynamics as it occurs in the vicinity of conical intersections and avoided crossings. Streaking can enhance the time resolution and provide direct signatures of electronic coherences, which affect many primary photochemical and biological events.