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通过皮秒X射线衍射观察溶液中的化学反应。

Visualizing chemical reactions in solution by picosecond x-ray diffraction.

作者信息

Plech Anton, Wulff Michael, Bratos Savo, Mirloup Fabien, Vuilleumier Rodolphe, Schotte Friedrich, Anfinrud Philip A

机构信息

Fachbereich Physik der Universitaet Konstanz, Universitaetsstrasse 10, D-78457 Konstanz, Germany.

出版信息

Phys Rev Lett. 2004 Mar 26;92(12):125505. doi: 10.1103/PhysRevLett.92.125505.

Abstract

We present a time-resolved x-ray diffraction study to monitor the recombination of laser-dissociated iodine molecules dissolved in CCl4. The change in structure of iodine is followed during the whole recombination process. The deexcitation of solute molecules produces a heating of the solvent and induces tiny changes in its structure. The variations in the distance between pairs of chlorine atoms in adjacent CCl4 molecules are probed on the mA length scale. However, the most striking outcome of the present work is the experimental determination of temporally varying atom-atom pair distribution functions. Variations of the mean density of the solution during thermal expansion are also followed in real time. One concludes that not only time-resolved optical spectroscopy but also time-resolved x-ray diffraction can be used to monitor atomic motions in liquids.

摘要

我们进行了一项时间分辨X射线衍射研究,以监测溶解在四氯化碳中的激光解离碘分子的重组过程。在整个重组过程中跟踪碘结构的变化。溶质分子的去激发会导致溶剂升温,并引起其结构的微小变化。在毫安长度尺度上探测相邻四氯化碳分子中氯原子对之间距离的变化。然而,本研究最显著的成果是对随时间变化的原子-原子对分布函数的实验测定。同时还实时跟踪了热膨胀过程中溶液平均密度的变化。由此得出结论,不仅时间分辨光谱学,而且时间分辨X射线衍射都可用于监测液体中的原子运动。

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