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Monitoring Ultrafast Spin Crossover Intermediates in an Iron(II) Complex by Broad Band Stimulated X-ray Raman Spectroscopy.

The photoinduced spin crossover dynamics of transition metal complexes is of fundamental scientific importance and is used for sensor device applications and solar energy harvesting. Current X-ray and optical spectroscopy experiments for [FeII(bpy)3], an archetypal earth-abundant metal complex, show conflicting spin dynamics. We have simulated the broad band transient X-ray absorption and hybrid (broad + narrow band) X-ray stimulated Raman signals at the N and Fe K-edges of the key excited state intermediates involved in the spin crossover process of this complex. We find that these signals are much more sensitive to electron and spin populations than transition absorption and may be useful in the design of photovoltaic and artificial photosynthetic systems.