Cao, Jianming and Ihee, Hyotcherl and Zewail, Ahmed H. (1999) Ultrafast electron diffraction and direct observation of transient structures in a chemical reaction. Proceedings of the National Academy of Sciences of the United States of America, 96 (2). pp. 338-342. ISSN 0027-8424. PMCID PMC15137. http://resolver.caltech.edu/CaltechAUTHORS:CAOpnas99
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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.
|Additional Information:||© 1999, The National Academy of Sciences. Contributed by Ahmed H. Zewail, November 24, 1998. This research was supported by a grant from the Air Force Office of Scientific Research and the Office of Naval Research. We thank the two colleagues who carefully reviewed the manuscript and made valuable comments. The publication costs of this article were defrayed in part by page charge payment. This article must therefore be hereby marked "advertisement" in accordance with 18 U.S.C. §1734 solely to indicate this fact.|
|PubMed Central ID:||PMC15137|
|Official Citation:||Jianming Cao, Hyotcherl Ihee, and Ahmed H. Zewail Ultrafast electron diffraction and direct observation of transient structures in a chemical reaction PNAS 1999 96 (2) 338-342; doi:10.1073/pnas.96.2.338|
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|Deposited By:||Archive Administrator|
|Deposited On:||11 Jul 2005|
|Last Modified:||15 Aug 2016 18:35|
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