Dryad
Published May 4, 2023 | Version v1
Dataset Open

Monitoring the evolution of relative product populations at early times during a photochemical reaction

Creators

  • 1. University of Nebraska–Lincoln
  • 2. SLAC National Accelerator Laboratory
  • 3. Kansas State University
  • 4. European X-Ray Free-Electron Laser
  • 5. University of New South Wales
  • 6. University of Paris-Saclay
  • 7. Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy
  • 8. Brown University
  • 9. Deutsches Elektronen-Synchrotron DESY
  • 10. University College London
  • 11. University of Bristol
  • 12. Daresbury Laboratory

Description

Identifying multiple rival reaction products and transient species formed during ultrafast photochemical reactions and determining their time-evolving relative populations are key steps towards understanding and predicting photochemical outcomes. Yet, most contemporary ultrafast studies struggle with clearly identifying and quantifying competing molecular structures/species amongst the emerging reaction products. Here, we show that mega-electronvolt ultrafast electron diffraction in combination with ab initio molecular dynamics calculations offers a unique route to determine time-resolved populations of the various isomeric products formed after UV (266 nm) excitation of the five-membered heterocyclic molecule thiophenone. This strategy reveals an unexpectedly high (~50%) yield of an episulfide isomer containing a strained 3-membered ring within ~1 ps at early times and rapid interconversions between the rival photoproducts.   

Notes

Trajectory dataset: xyz files can be opened with a text editor or a molecular visualizer (VMD).

Funding provided by: National Science Foundation
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100000001
Award Number: PHYS1753324

Funding provided by: U.S. Department of Energy
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100000015
Award Number: DE-AC02-05-CH11231

Funding provided by: U.S. Department of Energy
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100000015
Award Number: DE-AC02-76SF00515

Funding provided by: U.S. Department of Energy
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100000015
Award Number: DE-FG02-86ER13491

Funding provided by: U.S. Department of Energy
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100000015
Award Number: DE-SC0019451

Funding provided by: U.S. Department of Energy
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100000015
Award Number: DE-SC0017995

Funding provided by: U.S. Department of Energy
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100000015
Award Number: DE-SC0020276

Funding provided by: Horizon 2020 Framework Programme
Crossref Funder Registry ID: http://dx.doi.org/10.13039/100010661
Award Number: 803718

Funding provided by: Engineering and Physical Sciences Research Council
Crossref Funder Registry ID: http://dx.doi.org/10.13039/501100000266
Award Number: EP/V026690/1

Funding provided by: Australian Research Council
Crossref Funder Registry ID: http://dx.doi.org/10.13039/501100000923
Award Number: DE200100549

Funding provided by: Engineering and Physical Sciences Research Council
Crossref Funder Registry ID: http://dx.doi.org/10.13039/501100000266
Award Number: EP/L005913/1

Funding provided by: Engineering and Physical Sciences Research Council
Crossref Funder Registry ID: http://dx.doi.org/10.13039/501100000266
Award Number: EP/R513039/1

Funding provided by: Agence Nationale de la Recherche
Crossref Funder Registry ID: http://dx.doi.org/10.13039/501100001665
Award Number: ANR-20-CE29-0014

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