Toward highlighting the ultrafast electron transfer dynamics at the optically 
dark sites of photocatalysts.

Canton, S. E.; Zhang, X.; Zhang, J.; vaan Driel, T. B.; Kjaer, K. S.; Haldrup, K.; Chabera, P.; Harlang, T.; Suarez-Alcantara, K.; Liu, Y.; Perez, J.; Bordage, A.; Papai, M.; Vanko, G.; Jennings, G.; Kurtz, C. A.; Rovezzi, M.; Glatzel, P.; Smolentsev, G.; Uhlig, J.; Dohn, A. O.; Christensen, M.; Galler, A.; Gawelda, W.; Bressler, C.; Lemke, H. T.; Moller, K. B.; Nielsen, M. M.; Lomoth, R.; Warnmark, K.; Sundstrom, V.

doi:10.1021/jz401016h

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Toward highlighting the ultrafast electron transfer dynamics at the optically dark sites of photocatalysts.

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Canton, S. E.
Research Group of Structural Dynamics of (Bio)Chemical Systems, MPI for Biophysical Chemistry, Max Planck Society;

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引用

Canton, S. E., Zhang, X., Zhang, J., vaan Driel, T. B., Kjaer, K. S., Haldrup, K., Chabera, P., Harlang, T., Suarez-Alcantara, K., Liu, Y., Perez, J., Bordage, A., Papai, M., Vanko, G., Jennings, G., Kurtz, C. A., Rovezzi, M., Glatzel, P., Smolentsev, G., Uhlig, J., Dohn, A. O., Christensen, M., Galler, A., Gawelda, W., Bressler, C., Lemke, H. T., Moller, K. B., Nielsen, M. M., Lomoth, R., Warnmark, K., & Sundstrom, V. (2013). Toward highlighting the ultrafast electron transfer dynamics at the optically dark sites of photocatalysts. Journal of Physical Chemistry Letters, 4(11), 1972-1976. doi:10.1021/jz401016h.

引用: https://hdl.handle.net/11858/00-001M-0000-002D-7F65-C

要旨

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.