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用 X 射线激光解开超快电子和结构动力学之谜。

Disentangling Ultrafast Electronic and Structural Dynamics with X-Ray Lasers.

机构信息

Univ Rennes, CNRS, IPR (Institut de Physique de Rennes)-UMR 6251, 35000, Rennes, France.

出版信息

Chemistry. 2018 Oct 22;24(59):15696-15705. doi: 10.1002/chem.201802105. Epub 2018 Sep 24.

Abstract

Directing the functionality of molecules, materials and biophysical systems is challenging both from fundamental and applied standpoints. For example, understanding the elementary processes responsible for light-induced transformations require watching electronic and structural reorganizations on their intrinsic timescales. The X-ray free electron lasers (X-FEL) represent a new generation of incredibly short and ultra-bright X-ray source, which open new possibilities for developing the multidisciplinary field of ultrafast science. Experiments around X-FEL provide probes, sensitive to electronic and structural reorganizations, able to monitor transformations on the femtosecond timescale (1 fs=10  s). Recent years have seen terrific successes in providing a detailed view on light-induced processes, compared to what was understood from conventional optical pump-probe spectroscopy. This Concept article aims at illustrating, through recent studies mainly focussing on light-induced excited spin state trapping, how these X-FEL based techniques can help understanding light-activated functions, by monitoring elementary electronic and structural processes that may occur beyond the Born-Oppenheimer approximation.

摘要

从基础和应用的角度来看,控制分子、材料和生物物理系统的功能都极具挑战性。例如,要理解导致光诱导转变的基本过程,就需要在其固有时间尺度上观察电子和结构的重新排列。自由电子 X 射线激光(X-FEL)代表了新一代极其短和超亮的 X 射线源,为超快科学这一多学科领域的发展开辟了新的可能性。X-FEL 周围的实验提供了对电子和结构重新排列敏感的探针,能够在飞秒时间尺度(1 飞秒=10 秒)上监测转变。与传统的光泵浦探测光谱相比,近年来在提供对光诱导过程的详细了解方面取得了巨大的成功。本文主要通过聚焦于光致激发态捕获的最新研究,旨在说明这些基于 X-FEL 的技术如何通过监测可能超出 Born-Oppenheimer 近似的基本电子和结构过程,帮助理解光激活功能。

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