Journal
NATURE CHEMISTRY
Volume 11, Issue 6, Pages 504-509Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41557-019-0252-7
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Funding
- US Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
- DOE BES SUF Division Accelerator & Detector RD program
- Linac Coherent Light Source (LCLS) Facility
- SLAC [DE-AC02-05-CH11231, DE-AC02-76SF00515]
- Lichtenberg Professorship of the Volkswagen Foundation
- NSF
- Wild Overseas Scholars Fund of the Department of Chemistry, University of York
- US Department of Energy Office of Science, Basic Energy Sciences [DE-SC0014170]
- US Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0017995]
- Carnegie Trust for the Universities of Scotland [CRG050414]
- RSE/Scottish Government Sabbatical Research Grant [58507]
- U.S. Department of Energy (DOE) [DE-SC0017995] Funding Source: U.S. Department of Energy (DOE)
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The ultrafast photoinduced ring-opening of 1,3-cyclohexadiene constitutes a textbook example of electrocyclic reactions in organic chemistry and a model for photobiological reactions in vitamin D synthesis. Although the relaxation from the photoexcited electronic state during the ring-opening has been investigated in numerous studies, the accompanying changes in atomic distance have not been resolved. Here we present a direct and unambiguous observation of the ring-opening reaction path on the femtosecond timescale and subangstrom length scale using megaelectronvolt ultrafast electron diffraction. We followed the carbon-carbon bond dissociation and the structural opening of the 1,3-cyclohexadiene ring by the direct measurement of time-dependent changes in the distribution of interatomic distances. We observed a substantial acceleration of the ring-opening motion after internal conversion to the ground state due to a steepening of the electronic potential gradient towards the product minima. The ring-opening motion transforms into rotation of the terminal ethylene groups in the photoproduct 1,3,5-hexatriene on the subpicosecond timescale.
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