Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy
Abstract
We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet (XUV) probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time- and angle-resolved photoelectron spectra. We show how a Fourier analysis of time- and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.
Cite
@article{arxiv.1607.01322,
title = {Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy},
author = {Daria Popova-Gorelova and Jochen Küpper and Robin Santra},
journal= {arXiv preprint arXiv:1607.01322},
year = {2018}
}