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Proceedings Paper

Imaging the ultrafast photoinduced ring opening of 1,3-cyclohexadiene with MeV ultrafast electron diffraction (Conference Presentation)
Author(s): Thomas Wolf; Jie Yang; David Sanchez; João P. F. Nunes; Robert M. Parrish; Xiaozhe Shen; Martin Centurion; Ryan Coffee; James P. Cryan; Markus Gühr; Kareem Hegazy; Adam Kirrander; Renkai K. Li; Jennifer Ruddock; Theodore Vecchione; Stephen P. Weathersby; Peter M. Weber; Kyle Wilkin; Haiwang Yong; Quiang Zheng; Todd J. Martinez; Xijie Wang; Michael P. Minitti
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Paper Abstract

The photoinduced ring opening of 1,3-cyclohexadiene is a prototypical photo-allowed, ultrafast reaction in agreement with the Woodward-Hoffmann rules. Furthermore, it is a model reaction for the biosynthesis of vitamin D. The reaction mechanism involves coupled dynamics of the electrons and nuclei of the molecule in the vicinity of a conical intersection between the excited state and the ground state. It has been intensively investigated by spectroscopic methods, which were primarily sensitive to transient changes in the electronic structure during internal conversion through a conical intersection between the excited state and the ground state. The corresponding structural dynamics have so far only been investigated by a ultrafast x-ray diffraction study. However, spatial resolution down to bond lengths has not been achieved so far. We have investigated the ring opening by gas phase MeV ultrafast electron diffraction with an unprecedented combination of femtosecond temporal and sub Angstrom spatial resolution. The obtained momentum transfer range allows us to follow transient bond length changes by real space transformation of the experimental dataset. Thus, the experimentally observed structural dynamics can be directly compared to quantum molecular dynamics simulations. We, furthermore, can follow the further structural relaxation of the molecule for several hundred femtoseconds beyond relaxation through the conical intersection with the ground state.

Paper Details

Date Published: 17 September 2018
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Proc. SPIE 10753, Ultrafast Nonlinear Imaging and Spectroscopy VI, 107530T (17 September 2018); doi: 10.1117/12.2322176
Show Author Affiliations
Thomas Wolf, SLAC National Accelerator Lab. (United States)
Jie Yang, SLAC National Accelerator Lab. (United States)
David Sanchez, SLAC National Accelerator Lab. (United States)
Stanford Univ. (United States)
João P. F. Nunes, Univ. of York (United Kingdom)
Robert M. Parrish, SLAC National Accelerator Lab. (United States)
Stanford Univ. (United States)
Xiaozhe Shen, SLAC National Accelerator Lab. (United States)
Martin Centurion, Univ. of Nebraska-Lincoln (United States)
Ryan Coffee, SLAC National Accelerator Lab. (United States)
James P. Cryan, SLAC National Accelerator Lab. (United States)
Markus Gühr, SLAC National Accelerator Lab. (United States)
Univ. Potsdam (Germany)
Kareem Hegazy, SLAC National Accelerator Lab. (United States)
Adam Kirrander, The Univ. of Edinburgh (United Kingdom)
Renkai K. Li, SLAC National Accelerator Lab. (United States)
Jennifer Ruddock, Brown Univ. (United States)
Theodore Vecchione, SLAC National Accelerator Lab. (United States)
Stephen P. Weathersby, SLAC National Accelerator Lab. (United States)
Peter M. Weber, Brown Univ. (United States)
Kyle Wilkin, Univ. of Nebraska-Lincoln (United States)
Haiwang Yong, Brown Univ. (United States)
Quiang Zheng, SLAC National Accelerator Lab. (United States)
Todd J. Martinez, SLAC National Accelerator Lab. (United States)
Stanford Univ. (United States)
Xijie Wang, SLAC National Accelerator Lab. (United States)
Michael P. Minitti, SLAC National Accelerator Lab. (United States)


Published in SPIE Proceedings Vol. 10753:
Ultrafast Nonlinear Imaging and Spectroscopy VI
Zhiwen Liu; Demetri Psaltis; Kebin Shi, Editor(s)

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