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

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 (C_2F_4I_2) to produce the corresponding ethylene derivative by the breakage of two carbon-iodine, C-I, bonds. The evolution of the ground-state intermediate (C_2F_4I radical) is directly re- vealed 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. Tbe structure of the short-lived C_2F_4I 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.