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Atomistic characterization of the active-site solvation dynamics of a model photocatalyst

Author

Listed:
  • Tim B. van Driel

    (Molecular Movies, Technical University of Denmark
    LCLS, SLAC National Accelerator Laboratory)

  • Kasper S. Kjær

    (Molecular Movies, Technical University of Denmark
    PULSE Institute, SLAC National Accelerator Laboratory, Stanford University
    PO Box 124, Lund University)

  • Robert W. Hartsock

    (PULSE Institute, SLAC National Accelerator Laboratory, Stanford University)

  • Asmus O. Dohn

    (Technical University of Denmark
    Present address: Science Institute of the University of Iceland, VR-III, 107 Reykjavik, Iceland)

  • Tobias Harlang

    (Molecular Movies, Technical University of Denmark
    PO Box 124, Lund University)

  • Matthieu Chollet

    (LCLS, SLAC National Accelerator Laboratory)

  • Morten Christensen

    (Molecular Movies, Technical University of Denmark)

  • Wojciech Gawelda

    (European XFEL GmbH
    Institute of Physics, Jan Kochanowski University)

  • Niels E. Henriksen

    (Technical University of Denmark)

  • Jong Goo Kim

    (KAIST
    Center for Nanomaterials and Chemical Reactions, Institute for Basic Science)

  • Kristoffer Haldrup

    (Molecular Movies, Technical University of Denmark)

  • Kyung Hwan Kim

    (KAIST
    Center for Nanomaterials and Chemical Reactions, Institute for Basic Science
    Present address: Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden)

  • Hyotcherl Ihee

    (KAIST
    Center for Nanomaterials and Chemical Reactions, Institute for Basic Science)

  • Jeongho Kim

    (Inha University)

  • Henrik Lemke

    (LCLS, SLAC National Accelerator Laboratory
    Present address: Paul Scherrer Institut, WSLA/207, 5232 Villigen PSI, Switzerland)

  • Zheng Sun

    (PULSE Institute, SLAC National Accelerator Laboratory, Stanford University)

  • Villy Sundström

    (PO Box 124, Lund University)

  • Wenkai Zhang

    (PULSE Institute, SLAC National Accelerator Laboratory, Stanford University
    Present address: Center for Advanced Quantum Studies, Department of Physics, Beijing Normal University, Beijing 100875, China)

  • Diling Zhu

    (LCLS, SLAC National Accelerator Laboratory)

  • Klaus B. Møller

    (Technical University of Denmark)

  • Martin M. Nielsen

    (Molecular Movies, Technical University of Denmark)

  • Kelly J. Gaffney

    (PULSE Institute, SLAC National Accelerator Laboratory, Stanford University)

Abstract

The interactions between the reactive excited state of molecular photocatalysts and surrounding solvent dictate reaction mechanisms and pathways, but are not readily accessible to conventional optical spectroscopic techniques. Here we report an investigation of the structural and solvation dynamics following excitation of a model photocatalytic molecular system [Ir2(dimen)4]2+, where dimen is para-diisocyanomenthane. The time-dependent structural changes in this model photocatalyst, as well as the changes in the solvation shell structure, have been measured with ultrafast diffuse X-ray scattering and simulated with Born-Oppenheimer Molecular Dynamics. Both methods provide direct access to the solute–solvent pair distribution function, enabling the solvation dynamics around the catalytically active iridium sites to be robustly characterized. Our results provide evidence for the coordination of the iridium atoms by the acetonitrile solvent and demonstrate the viability of using diffuse X-ray scattering at free-electron laser sources for studying the dynamics of photocatalysis.

Suggested Citation

  • Tim B. van Driel & Kasper S. Kjær & Robert W. Hartsock & Asmus O. Dohn & Tobias Harlang & Matthieu Chollet & Morten Christensen & Wojciech Gawelda & Niels E. Henriksen & Jong Goo Kim & Kristoffer Hald, 2016. "Atomistic characterization of the active-site solvation dynamics of a model photocatalyst," Nature Communications, Nature, vol. 7(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13678
    DOI: 10.1038/ncomms13678
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    Cited by:

    1. Marco Reinhard & Alessandro Gallo & Meiyuan Guo & Angel T. Garcia-Esparza & Elisa Biasin & Muhammad Qureshi & Alexander Britz & Kathryn Ledbetter & Kristjan Kunnus & Clemens Weninger & Tim Driel & Jos, 2023. "Ferricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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