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  Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2'-bipyridine)2(CN)2].

Kjaer, K. S., Zhang, W., Alonso-Mori, R., Bergmann, U., Chollet, M., Hadt, R. G., et al. (2017). Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2'-bipyridine)2(CN)2]. Structural Dynamics, 4(4): 044030. doi:10.1063/1.4985017.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-F300-1 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-2D48-D
Genre: Journal Article

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 Creators:
Kjaer, K. S., Author
Zhang, W., Author
Alonso-Mori, R., Author
Bergmann, U., Author
Chollet, M., Author
Hadt, R. G., Author
Hartsock, R. W., Author
Harlang, T., Author
Kroll, T., Author
Kubicek, K.1, Author              
Lemke, H. T., Author
Liang, H. W., Author
Liu, Y., Author
Nielsen, M. M., Author
Robinson, J. S., Author
Solomon, E. I., Author
Sokaras, D., Author
van Driel, T. B., Author
Weng, T. C., Author
Zhu, D., Author
Persson, P., AuthorWarnmark, K., AuthorSundström, V., 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: We have used femtosecond resolution UV-visible and Kβ x-ray emission spectroscopy to characterize the electronic excited state dynamics of [Fe(bpy)2(CN)2], where bpy=2,2′-bipyridine, initiated by metal-to-ligand charge transfer (MLCT) excitation. The excited-state absorption in the transient UV-visible spectra, associated with the 2,2′-bipyridine radical anion, provides a robust marker for the MLCT excited state, while the transient Kβ x-ray emission spectra provide a clear measure of intermediate and high spin metal-centered excited states. From these measurements, we conclude that the MLCT state of [Fe(bpy)2(CN)2] undergoes ultrafast spin crossover to a metal-centered quintet excited state through a short lived metal-centered triplet transient species. These measurements of [Fe(bpy)2(CN)2] complement prior measurement performed on [Fe(bpy)3]2+ and [Fe(bpy)(CN)4]2− in dimethylsulfoxide solution and help complete the chemical series [Fe(bpy)N(CN)6–2N]2N-4, where N = 1–3. The measurements confirm that simple ligand modifications can significantly change the relaxation pathways and excited state lifetimes and support the further investigation of light harvesting and photocatalytic applications of 3d transition metal complexes.

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Language(s): eng - English
 Dates: 2017-06-06
 Publication Status: Published online
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 Rev. Method: Peer
 Identifiers: DOI: 10.1063/1.4985017
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Title: Structural Dynamics
Source Genre: Journal
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Pages: 11 Volume / Issue: 4 (4) Sequence Number: 044030 Start / End Page: - Identifier: -