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Title: Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction

Abstract

Simultaneous observation of nuclear and electronic motion is crucial for a complete understanding of molecular dynamics in excited electronic states. It is challenging for a single experiment to independently follow both electronic and nuclear dynamics at the same time. In this paper we show that ultrafast electron diffraction can be used to simultaneously record both electronic and nuclear dynamics in isolated pyridine molecules, naturally disentangling the two components. Electronic state changes (S1→S0 internal conversion) were reflected by a strong transient signal in small-angle inelastic scattering, and nuclear structural changes (ring puckering) were monitored by large-angle elastic diffraction. Supported by ab initio nonadiabatic molecular dynamics and diffraction simulations, our experiment provides a clear view of the interplay between electronic and nuclear dynamics of the photoexcited pyridine molecule.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4];  [2]; ORCiD logo [1]; ORCiD logo [3];  [5];  [6]; ORCiD logo [7]; ORCiD logo [3]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [6];  [7]; ORCiD logo [2]; ORCiD logo [6]
  1. SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
  2. SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Department of Chemistry, Stanford University, Stanford, CA, USA.
  3. Department of Physics and Astronomy, University of Nebraska–Lincoln, Lincoln, NE, USA.
  4. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Department of Chemistry, Stanford University, Stanford, CA, USA., Biophysics Program, Stanford University, Stanford, CA, USA.
  5. Institut für Physik und Astronomie, Universität Potsdam, Potsdam, Germany.
  6. SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
  7. Department of Physics and Astronomy, Stony Brook University, Stony Brook, NY, USA.
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Volkswagen Foundation
OSTI Identifier:
1630393
Alternate Identifier(s):
OSTI ID: 1617695
Grant/Contract Number:  
AC02-76SF00515; AC02-05CH11231; SC0014170; FG02-08ER15984
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 368 Journal Issue: 6493; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Citation Formats

Yang, Jie, Zhu, Xiaolei, F. Nunes, J. Pedro, Yu, Jimmy K., Parrish, Robert M., Wolf, Thomas J. A., Centurion, Martin, Gühr, Markus, Li, Renkai, Liu, Yusong, Moore, Bryan, Niebuhr, Mario, Park, Suji, Shen, Xiaozhe, Weathersby, Stephen, Weinacht, Thomas, Martinez, Todd J., and Wang, Xijie. Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction. United States: N. p., 2020. Web. doi:10.1126/science.abb2235.
Yang, Jie, Zhu, Xiaolei, F. Nunes, J. Pedro, Yu, Jimmy K., Parrish, Robert M., Wolf, Thomas J. A., Centurion, Martin, Gühr, Markus, Li, Renkai, Liu, Yusong, Moore, Bryan, Niebuhr, Mario, Park, Suji, Shen, Xiaozhe, Weathersby, Stephen, Weinacht, Thomas, Martinez, Todd J., & Wang, Xijie. Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction. United States. doi:https://doi.org/10.1126/science.abb2235
Yang, Jie, Zhu, Xiaolei, F. Nunes, J. Pedro, Yu, Jimmy K., Parrish, Robert M., Wolf, Thomas J. A., Centurion, Martin, Gühr, Markus, Li, Renkai, Liu, Yusong, Moore, Bryan, Niebuhr, Mario, Park, Suji, Shen, Xiaozhe, Weathersby, Stephen, Weinacht, Thomas, Martinez, Todd J., and Wang, Xijie. Fri . "Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction". United States. doi:https://doi.org/10.1126/science.abb2235.
@article{osti_1630393,
title = {Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction},
author = {Yang, Jie and Zhu, Xiaolei and F. Nunes, J. Pedro and Yu, Jimmy K. and Parrish, Robert M. and Wolf, Thomas J. A. and Centurion, Martin and Gühr, Markus and Li, Renkai and Liu, Yusong and Moore, Bryan and Niebuhr, Mario and Park, Suji and Shen, Xiaozhe and Weathersby, Stephen and Weinacht, Thomas and Martinez, Todd J. and Wang, Xijie},
abstractNote = {Simultaneous observation of nuclear and electronic motion is crucial for a complete understanding of molecular dynamics in excited electronic states. It is challenging for a single experiment to independently follow both electronic and nuclear dynamics at the same time. In this paper we show that ultrafast electron diffraction can be used to simultaneously record both electronic and nuclear dynamics in isolated pyridine molecules, naturally disentangling the two components. Electronic state changes (S1→S0 internal conversion) were reflected by a strong transient signal in small-angle inelastic scattering, and nuclear structural changes (ring puckering) were monitored by large-angle elastic diffraction. Supported by ab initio nonadiabatic molecular dynamics and diffraction simulations, our experiment provides a clear view of the interplay between electronic and nuclear dynamics of the photoexcited pyridine molecule.},
doi = {10.1126/science.abb2235},
journal = {Science},
number = 6493,
volume = 368,
place = {United States},
year = {2020},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
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DOI: https://doi.org/10.1126/science.abb2235

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