Diffractive imaging of dissociation and ground-state dynamics in a complex molecule

Kyle J. Wilkin, Robert M. Parrish, Jie Yang, Thomas J. A. Wolf, J. Pedro F. Nunes, Markus Guehr, Renkai Li, Xiaozhe Shen, Qiang Zheng, Xijie Wang, Todd J. Martinez, and Martin Centurion
Phys. Rev. A 100, 023402 – Published 2 August 2019
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Abstract

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 orbital to a mixed 5pσ hole and CF2 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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  • Received 2 April 2019
  • Revised 27 June 2019

DOI:https://doi.org/10.1103/PhysRevA.100.023402

©2019 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Kyle J. Wilkin1,*, Robert M. Parrish2,3,4,*, Jie Yang2,3,*, Thomas J. A. Wolf3, J. Pedro F. Nunes1,5, Markus Guehr3,6, Renkai Li2, Xiaozhe Shen2, Qiang Zheng2, Xijie Wang2, Todd J. Martinez3,4, and Martin Centurion1

  • 1Department of Physics and Astronomy, University of Nebraska – Lincoln, 855 N 16th St., Lincoln, Nebraska 68588, USA
  • 2SLAC National Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA
  • 3Stanford PULSE Institute, Menlo Park, California 94025, USA
  • 4Department of Chemistry, Stanford University, 333 Campus Drive, Menlo Park, California 94305, USA
  • 5Department of Chemistry, University of York, Heslington, York, YO10 5DD, United Kingdom
  • 6Institut für Physik und Astronomie, Universität Potsdam, Potsdam 14476, Germany

  • *These authors contributed equally to the work.

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Vol. 100, Iss. 2 — August 2019

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