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Nature communications
05 01, 2020;11 (1): 2157.

Observation of the molecular response to light upon photoexcitation.

Haiwang Yong, Nikola Zotev, Jennifer M Ruddock, Brian Stankus, Mats Simmermacher, Andrés Moreno Carrascosa, Wenpeng Du, Nathan Goff, Yu Chang, Darren Bellshaw, Mengning Liang, Sergio Carbajo, Jason E Koglin, Joseph S Robinson, Sébastien Boutet, Michael P Minitti, Adam Kirrander, Peter M Weber
Author Information
  1. Haiwang Yong: Department of Chemistry, Brown University, Providence, RI, 02912, USA. ORCID
  2. Nikola Zotev: EaStCHEM School of Chemistry and Centre for Science at Extreme Conditions, University of Edinburgh, David Brewster Road, Edinburgh, EH9 3FJ, UK.
  3. Jennifer M Ruddock: Department of Chemistry, Brown University, Providence, RI, 02912, USA.
  4. Brian Stankus: Department of Chemistry, Brown University, Providence, RI, 02912, USA.
  5. Mats Simmermacher: EaStCHEM School of Chemistry and Centre for Science at Extreme Conditions, University of Edinburgh, David Brewster Road, Edinburgh, EH9 3FJ, UK.
  6. Andrés Moreno Carrascosa: EaStCHEM School of Chemistry and Centre for Science at Extreme Conditions, University of Edinburgh, David Brewster Road, Edinburgh, EH9 3FJ, UK.
  7. Wenpeng Du: Department of Chemistry, Brown University, Providence, RI, 02912, USA.
  8. Nathan Goff: Department of Chemistry, Brown University, Providence, RI, 02912, USA.
  9. Yu Chang: Department of Chemistry, Brown University, Providence, RI, 02912, USA.
  10. Darren Bellshaw: EaStCHEM School of Chemistry and Centre for Science at Extreme Conditions, University of Edinburgh, David Brewster Road, Edinburgh, EH9 3FJ, UK.
  11. Mengning Liang: SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  12. Sergio Carbajo: SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA. ORCID
  13. Jason E Koglin: SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA. ORCID
  14. Joseph S Robinson: SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA. ORCID
  15. Sébastien Boutet: SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  16. Michael P Minitti: SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA. ORCID
  17. Adam Kirrander: EaStCHEM School of Chemistry and Centre for Science at Extreme Conditions, University of Edinburgh, David Brewster Road, Edinburgh, EH9 3FJ, UK. adam.kirrander@ed.ac.uk. ORCID
  18. Peter M Weber: Department of Chemistry, Brown University, Providence, RI, 02912, USA. peter_weber@brown.edu. ORCID
PMID: 32358535 DOI: 10.1038/s41467-020-15680-4

Abstract

When a molecule interacts with light, its electrons can absorb energy from the electromagnetic field by rapidly rearranging their positions. This constitutes the first step of photochemical and photophysical processes that include primary events in human vision and photosynthesis. Here, we report the direct measurement of the initial redistribution of electron density when the molecule 1,3-cyclohexadiene (CHD) is optically excited. Our experiments exploit the intense, ultrashort hard x-ray pulses of the Linac Coherent Light Source (LCLS) to map the change in electron density using ultrafast x-ray scattering. The nature of the excited electronic state is identified with excellent spatial resolution and in good agreement with theoretical predictions. The excited state electron density distributions are thus amenable to direct experimental observation.

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Journal Article Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S.
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