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Jens Uhlig. Portrait.

Jens Uhlig

Senior lecturer

Jens Uhlig. Portrait.

Solvent-Dependent Structural Dynamics in the Ultrafast Photodissociation Reaction of Triiodide Observed with Time-Resolved X-ray Solution Scattering

Author

  • Amke Nimmrich
  • Matthijs R. Panman
  • Oskar Berntsson
  • Elisa Biasin
  • Stephan Niebling
  • Jonas Petersson
  • Maria Hoernke
  • Alexander Björling
  • Emil Gustavsson
  • Tim B. van Driel
  • Asmus O. Dohn
  • Mads Laursen
  • Diana B. Zederkof
  • Kensuke Tono
  • Tetsuo Katayama
  • Shigeki Owada
  • Martin M. Nielsen
  • Jan Davidsson
  • Jens Uhlig
  • Jochen S. Hub
  • Kristoffer Haldrup
  • Sebastian Westenhoff

Summary, in English

Resolving the structural dynamics of bond breaking, bond formation, and solvation is required for a deeper understanding of solution-phase chemical reactions. In this work, we investigate the photodissociation of triiodide in four solvents using femtosecond time-resolved X-ray solution scattering following 400 nm photoexcitation. Structural analysis of the scattering data resolves the solvent-dependent structural evolution during the bond cleavage, internal rearrangements, solvent-cage escape, and bond reformation in real time. The nature and structure of the reaction intermediates during the recombination are determined, elucidating the full mechanism of photodissociation and recombination on ultrafast time scales. We resolve the structure of the precursor state for recombination as a geminate pair. Further, we determine the size of the solvent cages from the refined structures of the radical pair. The observed structural dynamics present a comprehensive picture of the solvent influence on structure and dynamics of dissociation reactions.

Department/s

  • LU Profile Area: Light and Materials
  • LTH Profile Area: Photon Science and Technology
  • LTH Profile Area: Nanoscience and Semiconductor Technology
  • Chemical Physics
  • NanoLund: Centre for Nanoscience

Publishing year

2023-07-26

Language

English

Pages

15754-15765

Publication/Series

Journal of the American Chemical Society

Volume

145

Issue

29

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Physical Chemistry (including Surface- and Colloid Chemistry)
  • Atom and Molecular Physics and Optics
  • Theoretical Chemistry (including Computational Chemistry)

Status

Published

ISBN/ISSN/Other

  • ISSN: 0002-7863