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

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

Published
Washington, D.C. : United States. Dept. of Energy, 2017.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description
Article numbers 044,030 : digital, PDF file
Additional Creators
SLAC National Accelerator Laboratory, United States. Department of Energy, and United States. Department of Energy. Office of Scientific and Technical Information
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Summary
Here, 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.
Report Numbers
E 1.99:1362282
Subject(s)
Note
Published through SciTech Connect.
07/06/2017.
Structural Dynamics 4 4 ISSN 2329-7778 AM
Kasper S. Kjaer; Wenkai Zhang; Roberto Alonso-Mori; Uwe Bergmann; Matthieu Chollet; Ryan G. Hadt; Robert W. Hartsock; Tobias Harlang; Thomas Kroll; Katharina Kubicek; Henrik T. Lemke; Huiyang W. Liang; Yizhu Liu; Martin M. Nielsen; Joseph S. Robinson; Edward I. Solomon; Dimosthenis Sokaras; Tim B. van Driel; Tsu -Chien Weng; Diling Zhu; Petter Persson; Kenneth Warnmark; Villy Sundstrom; Kelly J. Gaffney.
Funding Information
AC02-76SF00515
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