Tomov Ivan V, Rentzepis Peter M
Department of Chemistry, University of California, Irvine, CA 92697, USA.
Chemphyschem. 2004 Jan 23;5(1):27-35. doi: 10.1002/cphc.200300917.
Detection of ultrafast transient structures and the evolution of ultrafast structural intermediates during the course of reactions has been a long standing goal of chemists and biologists. This article will be restricted to nanosecond, picosecond and shorter time-resolved extended X-ray absorption fine structure (EXAFS) studies, its aim being to present the progress and problems encounter in measurements and understanding the structure of transients. The recent advances in source technology has stimulated a wide variety of novel experiments using both synchrotrons and smaller laboratory size systems. With more efficient X-ray lenses and detectors many of the previously difficult experiments to perform, because of the exposure time required and weak signals, will now be easily performed. The experimental system for the detection of ultrafast, time-resolved EXAFS spectra of molecules in liquids is described and the method for the analysis of EXAFS spectra to yield transient structures is given. We believe that utilizing our table-top ultrafast X-ray source and the polycapillary optics in conjunction with dispersive spectrometer and charge coupled devices (CCD) we will be able to determine the structure of many reaction intermediates and excited states of chemical and biological molecules in solid and liquid state.
检测超快瞬态结构以及反应过程中超快结构中间体的演变一直是化学家和生物学家长期以来的目标。本文将局限于纳秒、皮秒及更短时间分辨的扩展X射线吸收精细结构(EXAFS)研究,其目的是介绍在测量以及理解瞬态结构方面所取得的进展和遇到的问题。源技术的最新进展推动了使用同步加速器和小型实验室系统开展的各种新颖实验。借助更高效的X射线透镜和探测器,许多以前因所需曝光时间长和信号微弱而难以进行的实验现在将易于开展。描述了用于检测液体中分子超快、时间分辨EXAFS光谱的实验系统,并给出了用于分析EXAFS光谱以获得瞬态结构的方法。我们相信,利用我们的台式超快X射线源和多毛细管光学器件,结合色散光谱仪和电荷耦合器件(CCD),我们将能够确定固态和液态中许多化学和生物分子反应中间体及激发态的结构。