Chergui Majed
Ecole Polytechnique Fédérale de Lausanne, Laboratoire de Spectroscopie Ultrarapide, ISIC, Faculté des Sciences de Base, Station 6, CH-1015 Lausanne, Switzerland.
Acta Crystallogr A. 2010 Mar;66(Pt 2):229-39. doi: 10.1107/S010876730904968X. Epub 2010 Feb 9.
The need to visualize molecular structure in the course of a chemical reaction, a phase transformation or a biological function has been a dream of scientists for decades. The development of time-resolved X-ray and electron-based methods is making this true. X-ray absorption spectroscopy is ideal for the study of structural dynamics in liquids, because it can be implemented in amorphous media. Furthermore, it is chemically selective. Using X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) in laser pump/X-ray probe experiments allows the retrieval of the local geometric structure of the system under study, but also the underlying photoinduced electronic structure changes that drive the structural dynamics. Recent developments in picosecond and femtosecond X-ray absorption spectroscopy applied to molecular systems in solution are reviewed: examples on ultrafast photoinduced processes such as intramolecular electron transfer, low-to-high spin change, and bond formation are presented.
几十年来,在化学反应、相变或生物功能过程中可视化分子结构一直是科学家们的梦想。基于时间分辨X射线和电子的方法的发展正在使这一梦想成为现实。X射线吸收光谱法非常适合研究液体中的结构动力学,因为它可以在非晶态介质中实施。此外,它具有化学选择性。在激光泵浦/X射线探测实验中使用X射线吸收近边结构(XANES)和扩展X射线吸收精细结构(EXAFS),不仅可以获取所研究系统的局部几何结构,还可以了解驱动结构动力学的潜在光诱导电子结构变化。本文综述了皮秒和飞秒X射线吸收光谱法在溶液中分子系统的最新进展:给出了超快光诱导过程的例子,如分子内电子转移、低自旋到高自旋变化和键形成。