Journal
PHYSICAL REVIEW A
Volume 100, Issue 2, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevA.100.023402
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Funding
- U.S. Department of Energy (DOE) Office of Basic Energy Sciences (BES) SUF Division Accelerator and Detector RD program
- LCLS Facility
- SLAC [DE-AC02-05-CH11231, DE-AC02-76SF00515]
- U.S. Department of Energy (DOE) Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, AMOS program [DE-SC0014170]
- U.S. Department of Energy (DOE) Office of Basic Energy Science AMOS program
- Lichtenberg professorship of the Volkswagen Foundation
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We have investigated the structural dynamics in photoexcited 1,2-diiodotetrafluoroethane molecules (C2F4I2) in the gas phase experimentally using ultrafast electron diffraction and theoretically using FOMO-CASCI excited-state dynamics simulations. The molecules are excited by an ultraviolet femtosecond laser pulse to a state characterized by a transition from the iodine 5p perpendicular to orbital to a mixed 5p parallel to sigma hole and CF2 center dot antibonding orbital, which results in the cleavage of one of the carbon-iodine bonds. We have observed, with sub-Angstrom resolution, the motion of the nuclear wave packet of the dissociating iodine atom followed by coherent vibrations in the electronic ground state of the C2F4I radical. The radical reaches a stable classical (nonbridged) structure in less than 200 fs.
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