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Toward Highlighting the Ultrafast Electron Transfer Dynamics at the Optically Dark Sites of Photocatalysts

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Author

  • Sophie Canton
  • Xiaoyi Zhang
  • Jianxin Zhang
  • Tim B. van Driel
  • Kasper S. Kjaer
  • Kristoffer Haldrup
  • Pavel Chabera
  • Tobias Harlang
  • Karina Suarez Alcantara
  • Yizhu Liu
  • Jorge Perez Tuero
  • Amelie Bordage
  • Matyas Papai
  • Gyoergy Vanko
  • Guy Jennings
  • Charles A. Kurtz
  • Mauro Rovezzi
  • Pieter Glatzel
  • Grigory Smolentsev
  • Jens Uhlig
  • Asmus O. Dohn
  • Morten Christensen
  • Andreas Galler
  • Wojciech Gawelda
  • Christian Bressler
  • Henrik T. Lemke
  • Klaus B. Moller
  • Martin M. Nielsen
  • Reiner Lomoth
  • Kenneth Wärnmark
  • Villy Sundström
Show all

Summary, in English

Building a detailed understanding of the structure function relationship is a crucial step in the optimization of molecular photocatalysts employed in water splitting schemes. The optically dark nature of their active sites usually prevents a complete mapping of the photoinduced dynamics. In this work, transient X-ray absorption spectroscopy highlights the electronic and geometric changes that affect such a center in a bimetallic model complex. Upon selective excitation of the ruthenium chromophore, the cobalt moiety is reduced through intramolecular electron transfer and undergoes a spin flip accompanied by an average bond elongation of 0.20 +/- 0.03 angstrom. The analysis is supported by simulations based on density functional theory structures (B3LYP*/TZVP) and FEFF 9.0 multiple scattering calculations. More generally, these results exemplify the large potential of the technique for tracking elusive intermediates that impart unique functionalities in photochemical devices.

Publishing year

2013

Language

English

Pages

1972-1976

Publication/Series

The Journal of Physical Chemistry Letters

Volume

4

Issue

11

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Natural Sciences
  • Physical Sciences
  • Atom and Molecular Physics and Optics
  • Chemical Sciences

Status

Published

ISBN/ISSN/Other

  • ISSN: 1948-7185