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      Structural Determination of a Photochemically Active Diplatinum Molecule by Time-Resolved EXAFS Spectroscopy

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          Most cited references 34

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          Theoretical approaches to x-ray absorption fine structure

           J. Rehr,  R. Albers (2000)
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            Luminescent and Redox-Active Polynuclear Transition Metal Complexes.

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              Femtosecond XANES study of the light-induced spin crossover dynamics in an iron(II) complex.

              X-ray absorption spectroscopy is a powerful probe of molecular structure, but it has previously been too slow to track the earliest dynamics after photoexcitation. We investigated the ultrafast formation of the lowest quintet state of aqueous iron(II) tris(bipyridine) upon excitation of the singlet metal-to-ligand-charge-transfer (1MLCT) state by femtosecond optical pump/x-ray probe techniques based on x-ray absorption near-edge structure (XANES). By recording the intensity of a characteristic XANES feature as a function of laser pump/x-ray probe time delay, we find that the quintet state is populated in about 150 femtoseconds. The quintet state is further evidenced by its full XANES spectrum recorded at a 300-femtosecond time delay. These results resolve a long-standing issue about the population mechanism of quintet states in iron(II)-based complexes, which we identify as a simple 1MLCT-->3MLCT-->5T cascade from the initially excited state. The time scale of the 3MLCT-->5T relaxation corresponds to the period of the iron-nitrogen stretch vibration.
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                Author and article information

                Journal
                Angewandte Chemie International Edition
                Angew. Chem. Int. Ed.
                Wiley
                14337851
                March 30 2009
                March 30 2009
                March 05 2009
                : 48
                : 15
                : 2711-2714
                Article
                10.1002/anie.200805946
                © 2009

                http://doi.wiley.com/10.1002/tdm_license_1.1

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