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The ultrafast X-ray spectroscopic revolution in chemical dynamics
Nature Reviews Chemistry ( IF 36.3 ) Pub Date : 2018-05-29 , DOI: 10.1038/s41570-018-0008-8
Peter M. Kraus , Michael Zürch , Scott K. Cushing , Daniel M. Neumark , Stephen R. Leone

The past two decades have seen rapid developments in short-pulse X-ray sources, which have enabled the study of nuclear and electronic dynamics by ultrafast X-ray spectroscopies with unprecedented time resolution ranging from nanoseconds to attoseconds. In this Perspective, we discuss some of the major achievements in the study of nuclear and electronic dynamics with X-ray pulses produced by high-harmonic, free-electron-laser and synchrotron sources. The particular dynamic processes probed by X-ray radiation highlighted in this Perspective are electronic coherences on attosecond to femtosecond timescales, chemical reactions, such as dissociations, and pericyclic ring-openings, spin-crossover dynamics, ligand-exchange dynamics and structural deformations in excited states. X-ray spectroscopic probing of chemical dynamics holds great promise for the future owing to the ongoing developments of new spectroscopies, such as four-wave mixing, and the continuous improvements in emerging laboratory-based, high-harmonic sources and large-scale, facility-based, free-electron lasers.



中文翻译:

化学动力学中的超快X射线光谱革命

在过去的二十年中,短脉冲X射线源得到了飞速发展,这使超快X射线光谱学能够以毫微秒的时间分辨率(从纳秒到十亿分之一秒)来研究核和电子动力学。在本《观点》中,我们讨论了在由高谐波,自由电子激光和同步加速器源产生的X射线脉冲研究核和电子动力学方面的一些主要成就。本透视图中突出显示的由X射线辐射探测到的特定动力学过程是:在十亿分之一秒至飞秒时间尺度上的电子相干性,化学反应(例如解离和周环开环),自旋交叉动力学,配体交换动力学和激发时的结构变形状态。

更新日期:2018-05-29
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