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Träfflista för sökning "WFRF:(Hub J. S.) srt2:(2020-2023)"

Sökning: WFRF:(Hub J. S.) > (2020-2023)

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1.
  • Nimmrich, Amke, 1995, et al. (författare)
  • Solvent-Dependent Structural Dynamics in the Ultrafast Photodissociation Reaction of Triiodide Observed with Time-Resolved X-ray Solution Scattering
  • 2023
  • Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 145:29, s. 15754-15765
  • Tidskriftsartikel (refereegranskat)abstract
    • Resolving the structural dynamics of bond breaking, bond formation, and solvation is required for a deeper understanding of solutionphase 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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2.
  • Panman, Matthijs R, 1983, et al. (författare)
  • Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering
  • 2020
  • Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 125:22
  • Tidskriftsartikel (refereegranskat)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.
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