Jm. Cao et al., Ultrafast electron diffraction and direct observation of transient structures in a chemical reaction, P NAS US, 96(2), 1999, pp. 338-342
Citations number
29
Categorie Soggetti
Multidisciplinary
Journal title
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Ultrafast electron diffraction is a unique method for the studies of struct
ural 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 diiodotetraf
luoroethane (C2F4I2) to produce the corresponding ethylene derivative by th
e breakage of two carbon-iodine, C-I, bonds. The evolution of the ground-st
ate intermediate (C2F4I radical) is directly revealed in the population cha
nge 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-liv
ed C2F4I radical is more favorable to the classical radical structure than
to the bridged radical structure. This leap in our ability to record struct
ural changes on the ps and shorter time scales bodes well for many future a
pplications in complex molecular systems.