Conformer-specific photochemistry imaged in real space and time

Authors

E. G. Champenois, SLAC National Accelerator Laboratory
D. M. Sanchez, SLAC National Accelerator Laboratory
J. Yang, SLAC National Accelerator Laboratory
J. P. Figueira Nunes, University of Nebraska–Lincoln
A. Attar, SLAC National Accelerator Laboratory
Martin Centurion, University of Nebraska - LincolnFollow
R. Forbes, SLAC National Accelerator Laboratory
M. Gühr, Universität Potsdam
K. Hegazy, SLAC National Accelerator Laboratory
F. Ji, SLAC National Accelerator Laboratory
S. K. Saha, University of Nebraska–LincolnFollow
Y. Liu, Stony Brook University
M. F. Lin, SLAC National Accelerator Laboratory
D. Luo, SLAC National Accelerator Laboratory
B. Moore, University of Nebraska–Lincoln
X. Shen, SLAC National Accelerator Laboratory
M. R. Ware, SLAC National Accelerator Laboratory
Xijie Wang, SLAC National Accelerator Laboratory, Menlo Park, CAFollow
T. J. Martínez, SLAC National Accelerator LaboratoryFollow
Thomas J. A. Wolf, Stanford PULSE InstituteFollow

Document Type

Article

Date of this Version

10-8-2021

Citation

Published in Science 374, 178–182 (2021) 8 October 2021

DOI: 10.1126/science.abk3132

Cite as: arXiv:2107.03592 [physics.chem-ph] (or arXiv:2107.03592v1 [physics.chem-ph] for this version)

Comments

Copyright © 2021 by the authors

Abstract

Conformational isomers (conformers) of molecules play a decisive role in biology and organic chemistry. However, experimental methods for investigating chemical reaction dynamics are typically not conformersensitive. We report on a gas-phase megaelectronvolt ultrafast electron diffraction investigation of a-phellandrene undergoing an electrocyclic ring-opening reaction. We directly imaged the evolution of a specific set of a-phellandrene conformers into the product isomer predicted by the Woodward-Hoffmann rules in real space and time. Our experimental results are in quantitative agreement with nonadiabatic quantum molecular dynamics simulations, which provide considerable detail of how conformation influences the time scale and quantum efficiency of photoinduced ring-opening reactions.

Supplemental files attached.