Imaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective

TL;DR

This paper reviews the theoretical framework based on quantum electrodynamics for imaging electron dynamics in real time using ultrashort light pulses, highlighting the importance of accurate models for interpreting time-resolved measurements.

Contribution

It emphasizes the necessity of quantum electrodynamics for accurate ultrafast light-matter interaction modeling and compares different time-resolved techniques for electron dynamics imaging.

Findings

Quantum electrodynamics is essential for accurate ultrafast imaging.

Time-resolved signals encode different information than static measurements.

Various techniques provide complementary insights into electron dynamics.

Abstract

A wide range of ultrafast phenomena in various atomic, molecular and condense matter systems is governed by electron dynamics. Therefore, the ability to image electronic motion in real space and real time would provide a deeper understanding of such processes and guide developments of tools to control them. Ultrashort light pulses, which can provide unprecedented time resolution approaching subfemtosecond time scale, are perspective to achieve real-time imaging of electron dynamics. This task is challenging not only from an experimental view, but also from a theory perspective, since standard theories describing light-matter interaction in a stationary regime can provide erroneous results in an ultrafast case as demonstrated by several theoretical studies. We review the theoretical framework based on quantum electrodynamics, which has been shown to be necessary for an accurate description of time-resolved imaging of electron dynamics with ultrashort light pulses. We compare the results of theoretical studies of time-resolved nonresonant and resonant X-ray scattering, and time- and angle-resolved photoelectron spectroscopy and show that the corresponding time-resolved signals encode analogous information about electron dynamics. Thereby, the information about an electronic system provided by these time-resolved techniques is different from the information provided by their time-independent analogues.