光致电离芳香分子中的阿秒相干电子运动
化学物理
2024-11-05 v1
摘要
在分子系统中，电子的超快运动启动了化学变化的过程。追踪分子间的这种电子运动需要将阿秒时间分辨率与原子尺度的空间灵敏度相结合。在本工作中，我们利用X射线自由电子激光产生的一对阿秒X射线脉冲，追踪从典型芳香体系对氨基苯酚中突然移除一个电子所引发的电子运动。X射线吸收能够以原子位点特异性追踪这种运动。我们的测量结果与最先进的计算模型进行了对比，在多个时间尺度上重现了观测到的响应。亚飞秒动力学归因于经历非辐射衰变的态，而几飞秒的振荡运动则与稳定阳离子态中的电子波包运动相关联，这些态最终将与核运动耦合。我们的工作为理解中等复杂系统中化学转化之前和引发化学转化的超快电荷运动提供了见解，并为物质中超快电荷运动的计算模型提供了强有力的基准。
引用
@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}
}