Attosecond imaging of photo-induced dynamics in molecules using time-resolved photoelectron momentum microscopy

TL;DR

This paper demonstrates how attosecond extreme ultraviolet and x-ray pulses enable real-time imaging of electron dynamics in molecules, specifically mapping charge migration in pentacene via time-resolved photoelectron microscopy.

Contribution

The study provides a theoretical framework for using attosecond pulses to visualize charge migration in molecules with high temporal and spatial resolution.

Findings

Charge migration in pentacene can be tracked with photoelectron momentum maps.

Spectral broadening effects are significant in attosecond probe pulses.

Unique features in momentum maps correspond to excited-state dynamics.

Abstract

We explore the novel capabilities offered by attosecond extreme ultraviolet and x-ray pulses that can be now generated by free-electron lasers and high-harmonics generation sources for probing photon-induced electron dynamics in molecules. We theoretically analyze how spatial and temporal dependence of charge migration in a pentacene molecule can be followed by means of time-resolved photoelectron microscopy on the attosecond time scale. Performing the analysis, we accurately take into account that an attosecond probe pulse leads to considerable spectral broadening. We demonstrate that the excited-state dynamics of a neutral pentacene molecule in the real space map onto unique features of photoelectron momentum maps.