Unraveling the Photochemical Ring-Opening Dynamics of 1,3-cyclohexadiene with Ultrafast Electron Diffraction and \textit{Ab initio} Multiple Spawning

ORAL

Abstract

While the photoinduced ring-opening of 1,3-cyclohexadiene (CHD) has been the topic of numerous experimental and theoretical studies, none have achieved the temporal and spatial resolution needed to unambiguously observe its ring-opening dynamics. Here, we directly observe the photoinduced ring-opening of CHD on the femtosecond and sub-{\AA}ngstr\"{o}m scales using MeV Ultrafast Electron Diffraction (UED) and Ab Initio Multiple Spawning (AIMS). We show that CHD experiences a substantial acceleration of the ring-opening motion upon relaxation to the ground state via a conical intersection, which is transformed into rotation of the terminal ethylene groups in 1,3,5-hexatriene (HT). Additionally, we observe a coherent oscillation between the cZc, tZc/cZt, and tZt rotamers of HT upon relaxation to the ground state.

*NSG GRFP and EDGE Diversity

Authors

  • David Sanchez

    • Stanford PULSE Inst and Stanford Univ
  • Thomas Wolf

    • Stanford PULSE Inst
  • Jie Yang

    • Stanford PULSE Inst and SLAC Natl Accelerator Lab
  • Robert Parrish

    • Stanford PULSE Inst and Stanford Univ
  • Joao Nunes

    • Univ of York and Univ of Nebraska Lincoln
  • Martin Centurion

    • Univof Nebraska Lincoln
  • Ryan Coffee

    • SLAC Natl Accelerator Lab
  • James Cryan

    • Stanford PULSE Inst
  • Markus Guhr

    • Stanford PULSE Inst and Univ Potsdam
  • Kareem Hegazy

    • Stanford PULSE Inst and Stanford Univ
  • Adam Kirrander

    • Univ of Edinburgh
  • Renkai Li

    • SLAC Natl Accelerator Lab
  • Jennifer Ruddock

    • Brown Univ
  • Xiaozhe Shen

    • SLAC Natl Accelerator Lab
  • Theodore Vecchione

    • SLAC Natl Accelerator Lab
  • Stephen Weathersby

    • SLAC Natl Accelerator Lab
  • Peter Weber

    • Brown Univ
  • Kyle Wilkin

    • Univ of Nebraska Lincoln
  • Hai-Wang Yong

    • Brown Univ
  • Qiang Zheng

    • SLAC Natl Accelerator Lab
  • Xijie Wang

    • SLAC Natl Accelerator Lab
  • Michael Minitti

    • SLAC Natl Accelerator Lab
  • Todd Martinez

    • Stanford PULSE Inst and Stanford Univ