Imaging the ultrafast photoinduced ring opening of 1,3-cyclohexadiene with MeV ultrafast electron diffraction (Conference Presentation)

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

doi:10.1117/12.2322176

17 September 2018 Imaging the ultrafast photoinduced ring opening of 1,3-cyclohexadiene with MeV ultrafast electron diffraction (Conference Presentation)

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

Author Affiliations +

Proceedings Volume 10753, Ultrafast Nonlinear Imaging and Spectroscopy VI; 107530T (2018) https://doi.org/10.1117/12.2322176
Event: SPIE Optical Engineering + Applications, 2018, San Diego, California, United States

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.

Conference Presentation

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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, and Michael P. Minitti "Imaging the ultrafast photoinduced ring opening of 1,3-cyclohexadiene with MeV ultrafast electron diffraction (Conference Presentation)", Proc. SPIE 10753, Ultrafast Nonlinear Imaging and Spectroscopy VI, 107530T (17 September 2018); https://doi.org/10.1117/12.2322176

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