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• W2883134037 endingPage "9530" @default.
• W2883134037 startingPage "9515" @default.
• W2883134037 abstract "Understanding the detailed electronic structure of transition metal ions is essential in numerous areas of inorganic chemistry. In particular, the ability to map out the many particle d–d spectrum of a transition metal catalyst is key to understanding and predicting reactivity. However, from a practical perspective, there are often experimental limitations on the ability to determine the energetic ordering, and multiplicity of all the excited states. These limitations derive in part from parity and spin-selection rules, as well as from the limited energy range of many standard laboratory instruments. Herein, we demonstrate the ability of 2p3d resonant inelastic X-ray scattering (RIXS) to obtain detailed insights into the many particle spectrum of simple inorganic molecular iron complexes. The present study focuses on low-spin ferrous and ferric iron complexes, including [FeIII/II(tacn)2]3+/2+ and [FeIII/II(CN)6]3–/4–. This series thus allows us to assess the contribution of d-count and ligand donor type, by comparing the purely σ-donating tacn ligand to the π-accepting cyanide. In order to highlight the conceptual difference between RIXS and traditional optical spectroscopy, we compare first RIXS results with UV–vis and magnetic circular dichroism spectroscopy. We then highlight the ability of 2p3d RIXS to (1) separate d–d transitions from charge transfer transitions and (2) to determine the many particle d–d spectrum over a much wider energy range than is possible by optical spectroscopy. Our experimental results are correlated with semiempirical multiplet simulations and ab initio complete active space self-consistent field calculations in order to obtain detailed assignments of the excited states. These results show that ΔS = 1, and possibly ΔS = 2, transitions may be observed in 2p3d RIXS spectra. Hence, this methodology has great promise for future applications in all areas of transition metal inorganic chemistry." @default.
• W2883134037 created "2018-08-03" @default.
• W2883134037 creator A5017692206 @default.
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• W2883134037 date "2018-07-25" @default.
• W2883134037 modified "2023-10-16" @default.
• W2883134037 title "Probing the Valence Electronic Structure of Low-Spin Ferrous and Ferric Complexes Using 2p3d Resonant Inelastic X-ray Scattering (RIXS)" @default.
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