Probing transient molecular structures in photochemical processes using laser-initiated time-resolved X-ray absorption spectroscopy

被引:146
作者
Chen, LX [1 ]
机构
[1] Argonne Natl Lab, Div Chem, Argonne, IL 60439 USA
关键词
excited state structures; ultrafast X-ray studies; pump-probe technique;
D O I
10.1146/annurev.physchem.56.092503.141310
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Molecular structures' during chemical processes are crucial for predicting molecular reactivity and reaction mechanisms. Using a laser pulse as an internal clock for starting fundamental chemical processes, molecular structural dynamics can be characterized by coherent vibrational motions and by incoherent transitions between different intermediate states. Recent developments in pulsed X-ray facilities allow structural determination of discrete excited states and reaction intermediates using laser-initiated time-resolved X-ray absorption spectroscopy (LITR-XAS). Moreover, femtosecond X-ray sources have begun making significant contributions in monitoring coherent molecular motions. This review summarizes recent developments in the field, including technical and scientific challenges as well as several examples involving excited state. molecular structure and electronic configuration determinations. Future applications of this technique with high time resolution will enable visualization of fundamental chemical events in many systems and further our understanding in photochemistry.
引用
收藏
页码:221 / 254
页数:38
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