Femtosecond Soft X-ray Spectroscopy of Solvated Transition-Metal Complexes: Deciphering the Interplay of Electronic and Structural Dynamics

We present the first implementation of femtosecond soft X-ray spectroscopy as an ultrafast direct probe of the excited-state valence orbitals in solution-phase molecules. This method is applied to photoinduced spin crossover of [Fe(tren(py)3)]2+, where the ultrafast spin-state conversion of the meta...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2011-04, Vol.2 (8), p.880-884
Main Authors: Huse, Nils, Cho, Hana, Hong, Kiryong, Jamula, Lindsey, de Groot, Frank M. F, Kim, Tae Kyu, McCusker, James K, Schoenlein, Robert W
Format: Article
Language:English
Subjects:
Electron Transport, Optical and Electronic Devices, Hard Matter
femtosecond X-ray spectroscopy, transition-metal complex, spin-crossover
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Summary:We present the first implementation of femtosecond soft X-ray spectroscopy as an ultrafast direct probe of the excited-state valence orbitals in solution-phase molecules. This method is applied to photoinduced spin crossover of [Fe(tren(py)3)]2+, where the ultrafast spin-state conversion of the metal ion, initiated by metal-to-ligand charge-transfer excitation, is directly measured using the intrinsic spin-state selectivity of the soft X-ray L-edge transitions. Our results provide important experimental data concerning the mechanism of ultrafast spin-state conversion and subsequent electronic and structural dynamics, highlighting the potential of this technique to study ultrafast phenomena in the solution phase.
ISSN:1948-7185
1948-7185
DOI:10.1021/jz200168m