Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule
Abstract
In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this work, we employ a pair of attosecond x-ray pulses from an x-ray free-electron laser to follow electron motion resulting from the sudden removal of an electron from a prototypical aromatic system, para-aminophenol. X-ray absorption enables tracking this motion with atomic-site specificity. Our measurements are compared with state-of-the-art computational modeling, reproducing the observed response across multiple timescales. Sub-femtosecond dynamics are assigned to states undergoing non-radiative decay, while few-femtosecond oscillatory motion is associated with electronic wavepacket motion in stable cation states, that will eventually couple to nuclear motion. Our work provides insight on the ultrafast charge motion preceding and initiating chemical transformations in moderately complex systems, and provides a powerful benchmark for computational models of ultrafast charge motion in matter.
Keywords
Cite
@article{arxiv.2411.01700,
title = {Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule},
author = {Taran Driver and Zhaoheng Guo and Erik Isele and Gilbert Grell and Marco Ruberti and Jordan T. ONeal and Oliver Alexander and Sandra Beauvarlet and David Cesar and Joseph Duris and Douglas Garratt and Kirk A. Larsen and Siqi Li and Přemysl Kolorenč and Gregory A. McCracken and Daniel Tuthill and Zifan Wang and Nora Berrah and Christoph Bostedt and Kurtis Borne and Xinxin Cheng and Louis F. DiMauro and Gilles Doumy and Paris L. Franz and Andrei Kamalov and Xiang Li and Ming-Fu Lin and Razib Obaid and Antonio Picón and River R. Robles and Daniel Rolles and Artem Rudenko and Moniruzzaman Shaikh and Daniel S. Slaughter and Nicholas S. Sudar and Emily Thierstein and Kiyoshi Ueda and Enliang Wang and Anna L. Wang and Thorsten Weber and Thomas J. A. Wolf and Linda Young and Zhen Zhang and Vitali Averbukh and Oliver Gessner and Philip H. Bucksbaum and Matthias F. Kling and Alicia Palacios and Fernando Martín and Jon P. Marangos and Peter Walter and Agostino Marinelli and James P. Cryan},
journal= {arXiv preprint arXiv:2411.01700},
year = {2024}
}