Stability of the local electronic properties of La3Ni2O7 under pressure

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Abstract

Motivated by the recent discovery of superconductivity in bulk La3Ni2O7 under pressure, we investigated its local electronic structure—specifically the Ni oxidation state, 3d occupancy, spin configuration, and 3d − 2p hybridization—using Ni K-edge x-ray absorption spectroscopy (XAS) and Kβ x-ray emission spectroscopy (XES), complemented by density functional theory (DFT) and spectral simulations. Despite the average valence of ∼2.5+ indicated by XAS, analysis of the XES spectra revealed 3d8L electronic configuration with low-spin ground state. Under HP up to 30 GPa and low T down to 10 K, we find no evidence of changes in Ni valence, 3d occupancy, or spin state, effectively ruling out pressure-induced spin-state transitions proposed in some theoretical models. Additional La L3-edge XAS measurements show only subtle spectral modifications, inconsistent with significant 3d−5d charge transfer. These results suggest that the pressure-induced superconductivity in La3Ni2O7 is unlikely linked with substantial changes in the local electronic structure.

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