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Spectroscopic Signature of Oxidized Oxygen States in Peroxides. | LitMetric
Recent debates on the oxygen redox behaviors in battery electrodes have triggered a pressing demand for the reliable detection and understanding of nondivalent oxygen states beyond conventional absorption spectroscopy. Here, enabled by high-efficiency mapping of resonant inelastic X-ray scattering (mRIXS) coupled with first-principles calculations, we report distinct mRIXS features of the oxygen states in LiO, LiCO, and especially, LiO, which are successfully reproduced and interpreted theoretically. mRIXS signals are dominated by valence-band decays in LiO and LiCO. However, the oxidized oxygen in LiO leads to partially unoccupied O-2p states that yield a specific intraband excitonic feature in mRIXS. Such a feature displays a specific emission energy in mRIXS, which disentangles the oxidized oxygen states from the dominating transition-metal/oxygen hybridization features in absorption spectroscopy, thus providing critical hints for both detecting and understanding the oxygen redox reactions in transition-metal oxide based battery materials.
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