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.
Highlights
Real-time imaging of electron dynamics is one of the most important and challenging tasks for modern ultrafast science [1,2,3,4,5,6,7,8]
We review the theoretical framework based on the quantum electrodynamics (QED), which has been developed to describe the interaction of an ultrashort light pulse with a coherently evolving electronic system
For the sake of comparison, Dixit et al have shown scattering patterns calculated with Equation (18) within the QED framework, but restricting the calculation to the two electronic states involved in the dynamics [see Figure 1b]
Summary
Real-time imaging of electron dynamics is one of the most important and challenging tasks for modern ultrafast science [1,2,3,4,5,6,7,8]. To using photons for imaging electron dynamics with X-ray scattering, one can consider employing photoelectrons dislodged by ultrashort light pulses for this goal. Taking into account all transitions that can be induced by a broadband, ultrashort probe pulse, one can obtain correct time-resolved scattering patterns. Such an analysis can be accurately performed within the quantum electrodynamics (QED) framework. We review the theoretical framework based on the QED, which has been developed to describe the interaction of an ultrashort light pulse with a coherently evolving electronic system.
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