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Solvent-Dependent Structural Dynamics in the Ultrafast Photodissociation Reaction of Triiodide Observed with Time-Resolved X-ray Solution Scattering.
Nimmrich, Amke; Panman, Matthijs R; Berntsson, Oskar; Biasin, Elisa; Niebling, Stephan; Petersson, Jonas; Hoernke, Maria; Björling, Alexander; Gustavsson, Emil; van Driel, Tim B; Dohn, Asmus O; Laursen, Mads; Zederkof, Diana B; Tono, Kensuke; Katayama, Tetsuo; Owada, Shigeki; Nielsen, Martin M; Davidsson, Jan; Uhlig, Jens; Hub, Jochen S; Haldrup, Kristoffer; Westenhoff, Sebastian.
Afiliación
  • Nimmrich A; Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden.
  • Panman MR; Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden.
  • Berntsson O; Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden.
  • Biasin E; Department of Physics, Technical University of Denmark, 2800 Lyngby, Denmark.
  • Niebling S; Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden.
  • Petersson J; Department of Chemistry, Ångström Laboratory, Uppsala University, Box 523, 75120 Uppsala, Sweden.
  • Hoernke M; Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden.
  • Björling A; Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden.
  • Gustavsson E; Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden.
  • van Driel TB; Department of Physics, Technical University of Denmark, 2800 Lyngby, Denmark.
  • Dohn AO; Department of Physics, Technical University of Denmark, 2800 Lyngby, Denmark.
  • Laursen M; Faculty of Physical Sciences, University of Iceland, VR-III, 107 Reykjavík, Iceland.
  • Zederkof DB; Department of Physics, Technical University of Denmark, 2800 Lyngby, Denmark.
  • Tono K; Department of Physics, Technical University of Denmark, 2800 Lyngby, Denmark.
  • Katayama T; Japan Synchrotron Radiation Research Institute, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
  • Owada S; Japan Synchrotron Radiation Research Institute, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
  • Nielsen MM; RIKEN SPring-8 Center, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5148, Japan.
  • Davidsson J; Department of Physics, Technical University of Denmark, 2800 Lyngby, Denmark.
  • Uhlig J; Department of Chemistry, Ångström Laboratory, Uppsala University, Box 523, 75120 Uppsala, Sweden.
  • Hub JS; Department of Chemical Physics, Lund University, Box 124, 22100 Lund, Sweden.
  • Haldrup K; Georg-August-Universität Göttingen, Institute for Microbiology and Genetics, Justus-von-Liebig-Weg 11, 37077 Göttingen, Germany.
  • Westenhoff S; Department of Physics, Technical University of Denmark, 2800 Lyngby, Denmark.
J Am Chem Soc ; 145(29): 15754-15765, 2023 Jul 26.
Article en En | MEDLINE | ID: mdl-37163700
ABSTRACT
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.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article País de afiliación: Suecia
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article País de afiliación: Suecia