Capturing photochemical and photophysical transformations in iron complexes with ultrafast X-ray spectroscopy and scattering |
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Authors: | Kelly J Gaffney |
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Institution: | Stanford PULSE Institute, SLAC National Accelerator Laboratory, Stanford University, Menlo Park California 94025 USA, |
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Abstract: | Light-driven chemical transformations provide a compelling approach to understanding chemical reactivity with the potential to use this understanding to advance solar energy and catalysis applications. Capturing the non-equilibrium trajectories of electronic excited states with precision, particularly for transition metal complexes, would provide a foundation for advancing both of these objectives. Of particular importance for 3d metal compounds is characterizing the population dynamics of charge-transfer (CT) and metal-centered (MC) electronic excited states and understanding how the inner coordination sphere structural dynamics mediate the interaction between these states. Recent advances in ultrafast X-ray laser science has enabled the electronic excited state dynamics in 3d metal complexes to be followed with unprecedented detail. This review will focus on simultaneous X-ray emission spectroscopy (XES) and X-ray solution scattering (XSS) studies of iron coordination and organometallic complexes. These simultaneous XES-XSS studies have provided detailed insight into the mechanism of light-induced spin crossover in iron coordination compounds, the interaction of CT and MC excited states in iron carbene photosensitizers, and the mechanism of Fe–S bond dissociation in cytochrome c.Ultrafast X-ray scattering and spectroscopy captures photophysical and photochemical transformations of 3d transition metal complexes with atomistic detail. |
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