Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering

  • Matthijs R. Panman
  • , Elisa Biasin
  • , Oskar Berntsson
  • , Markus Hermann
  • , Stephan Niebling
  • , Ashley J. Hughes
  • , Joachim Kübel
  • , Kalina Atkovska
  • , Emil Gustavsson
  • , Amke Nimmrich
  • , Asmus O. Dohn
  • , Mads Laursen
  • , Diana B. Zederkof
  • , Alireza Honarfar
  • , Kensuke Tono
  • , Tetsuo Katayama
  • , Shigeki Owada
  • , Tim B. Van Driel
  • , Kasper Kjaer
  • , Martin M. Nielsen
  • Jan Davidsson, Jens Uhlig, Kristoffer Haldrup, Jochen S. Hub, Sebastian Westenhoff

Research output: Contribution to journalArticlepeer-review

Abstract

Resolving the structural dynamics of the initial steps of chemical reactions is challenging. We report the femtosecond time-resolved wide-angle X-ray scattering of the photodissociation of diiodomethane in cyclohexane. The data reveal with structural detail how the molecule dissociates into radicals, how the radicals collide with the solvent, and how they form the photoisomer. We extract how translational and rotational kinetic energy is dispersed into the solvent. We also find that 85% of the primary radical pairs are confined to their original solvent cage and discuss how this influences the downstream recombination reactions.

Original languageEnglish
Article number226001
JournalPhysical Review Letters
Volume125
Issue number22
DOIs
Publication statusPublished - 24 Nov 2020

Bibliographical note

Funding Information: Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The experiments at SACLA were performed at BL3 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (Proposal No. 2016A8037). S. W. acknowledges the European Research Council for support (Grants No. 6581802 and No. 279944). The DTU-affiliated authors gratefully acknowledge DANSCATT for support of the beam time activities. E. B. and S. W. further acknowledge support from Interreg. M. H., K. A., and J. S. H. were supported by the Deutsche Forschungsgemeinschaft (Grant No. HU 1971-1/1, No. HU 1971-3/1, and No. HU 1971-4/1). Publisher Copyright: © 2020 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the "https://creativecommons.org/licenses/by/4.0/"Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Funded by "https://www.kb.se/samverkan-och-utveckling/oppen-tillgang-och-bibsamkonsortiet/bibsamkonsortiet.HTML"Bibsam.

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