Ultrafast electron diffraction and direct observation of transient structures in a chemical reaction

被引:70
作者
Cao, JM [1 ]
Ihee, H [1 ]
Zewail, AH [1 ]
机构
[1] CALTECH, Arthur Amos Noyes Lab Chem Phys, Pasadena, CA 91125 USA
关键词
D O I
10.1073/pnas.96.2.338
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Ultrafast electron diffraction is a unique method for the studies of structural changes of complex molecular systems. In this contribution, we report direct ultrafast electron diffraction study of the evolution of short-lived intermediates in the course of a chemical change. Specifically, we observe the transient intermediate in the elimination reaction of 1,2 diiodotetrafluoroethane (C2F4I2) to produce the corresponding ethylene derivative by the breakage of two carbon-iodine, C-I, bonds. The evolution of the ground-state intermediate (C2F4I radical) is directly revealed in the population change of a single chemical bond, namely the second C-I bond. The elimination of two iodine atoms was shown to be nonconcerted, with reaction time of the second C-I bond breakage being 17 +/- 2 ps. The structure of the short-lived C2F4I radical is more favorable to the classical radical structure than to the bridged radical structure. This leap in our ability to record structural changes on the ps and shorter time scales bodes well for many future applications in complex molecular systems.
引用
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页码:338 / 342
页数:5
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