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  Tracking excited-state charge and spin dynamics in iron coordination complexes.

Zhang, W., Alonso-Mori, R., Bergmann, U., Bressler, C., Chollet, M., Galler, A., et al. (2014). Tracking excited-state charge and spin dynamics in iron coordination complexes. Nature, 509(7500), 345-348. doi:10.1038/nature13252.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0019-8C96-9 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-84C5-0
Genre: Journal Article

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 Creators:
Zhang, W., Author
Alonso-Mori, R., Author
Bergmann, U., Author
Bressler, C., Author
Chollet, M., Author
Galler, A., Author
Gawelda, W., Author
Hadt, R. G., Author
Hardsock, R. W., Author
Kroll, T., Author
Kjaer, K. S., Author
Kubicek, K.1, Author              
Lemke, H. T., Author
Liang, H. W., Author
Meyer, D. A., Author
Nielsen, M. M., Author
Purser, C., Author
Robinson, J. S., Author
Solomon, E. I., Author
Sun, Z., Author
Sokaras, D., Authorvan Driel, D. B., AuthorVanko, G., AuthorWeng, T. C., AuthorZhu, D., AuthorGaffney, K. J., Author more..
Affiliations:
1Research Group of Structural Dynamics of (Bio)chemical Systems, MPI for biophysical chemistry, Max Planck Society, ou_578564              

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 Abstract: Crucial to many light-driven processes in transition metal complexes is the absorption and dissipation of energy by 3d electrons1, 2, 3, 4. But a detailed understanding of such non-equilibrium excited-state dynamics and their interplay with structural changes is challenging: a multitude of excited states and possible transitions result in phenomena too complex to unravel when faced with the indirect sensitivity of optical spectroscopy to spin dynamics5 and the flux limitations of ultrafast X-ray sources6, 7. Such a situation exists for archetypal polypyridyl iron complexes, such as [Fe(2,2′-bipyridine)3]2+, where the excited-state charge and spin dynamics involved in the transition from a low- to a high-spin state (spin crossover) have long been a source of interest and controversy6, 7, 8, 9, 10, 11, 12, 13, 14, 15. Here we demonstrate that femtosecond resolution X-ray fluorescence spectroscopy, with its sensitivity to spin state, can elucidate the spin crossover dynamics of [Fe(2,2′-bipyridine)3]2+ on photoinduced metal-to-ligand charge transfer excitation. We are able to track the charge and spin dynamics, and establish the critical role of intermediate spin states in the crossover mechanism. We anticipate that these capabilities will make our method a valuable tool for mapping in unprecedented detail the fundamental electronic excited-state dynamics that underpin many useful light-triggered molecular phenomena involving 3d transition metal complexes.

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Language(s): eng - English
 Dates: 2014-05-072014-05-15
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1038/nature13252
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Title: Nature
Source Genre: Journal
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Pages: - Volume / Issue: 509 (7500) Sequence Number: - Start / End Page: 345 - 348 Identifier: -