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

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 Haldrup, Kyung Hwan Kim, Hyotcherl Ihee, Jeongho Kim, Henrik Lemke, Zheng Sun, Villy Sundström, Wenkai Zhang, Diling Zhu, Klaus B. Møller (), Martin M. Nielsen () and Kelly J. Gaffney ()
Additional contact information
Tim B. van Driel: Molecular Movies, Technical University of Denmark
Kasper S. Kjær: Molecular Movies, Technical University of Denmark
Robert W. Hartsock: PULSE Institute, SLAC National Accelerator Laboratory, Stanford University
Asmus O. Dohn: Technical University of Denmark
Tobias Harlang: Molecular Movies, Technical University of Denmark
Matthieu Chollet: LCLS, SLAC National Accelerator Laboratory
Morten Christensen: Molecular Movies, Technical University of Denmark
Wojciech Gawelda: European XFEL GmbH
Niels E. Henriksen: Technical University of Denmark
Jong Goo Kim: KAIST
Kristoffer Haldrup: Molecular Movies, Technical University of Denmark
Kyung Hwan Kim: KAIST
Hyotcherl Ihee: KAIST
Jeongho Kim: Inha University
Henrik Lemke: LCLS, SLAC National Accelerator Laboratory
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
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

Nature Communications, 2016, vol. 7, issue 1, 1-7

Abstract: 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.

Date: 2016
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DOI: 10.1038/ncomms13678

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