Papers › Role of Oxygen States in the Low Valence Nickelate La₄Ni₃O₈
Role of Oxygen States in the Low Valence Nickelate La₄Ni₃O₈
Y. Shen, J. Sears, G. Fabbris, J. Li, J. Pelliciari, I. Jarrige, Xi He, I. Bozovic, M. Mitrano, Junjie Zhang, J. F. Mitchell, A. S. Botana, V. Bisogni, M. R. Norman, S. Johnston, M. P. M. Dean
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The discovery of superconductivity in square-planar low valence nickelates has ignited a vigorous debate regarding their essential electronic properties: Do these materials have appreciable oxygen charge-transfer character akin to the cuprates, or are they in a distinct Mott-Hubbard regime where oxygen plays a minimal role? Here, we resolve this question using O K-edge resonant inelastic x-ray scattering (RIXS) measurements of the low valence nickelate La₄Ni₃O₈ and a prototypical cuprate La₂₋ₓSrₓCuO₄ (x=0.35). As expected, the cuprate lies deep in the charge-transfer regime of the Zaanen-Sawatzky-Allen scheme. The nickelate, however, is not well described by either limit of the ZSA scheme and is found to be of mixed charge-transfer/Mott-Hubbard character with the Coulomb repulsion U of similar size to the charge-transfer energy Δ. Nevertheless, the transition-metal-oxygen hopping is larger in La₄Ni₃O₈ than in La₂₋ₓSrₓCuO₄, leading to a significant superexchange interaction and an appreciable hole occupation of the ligand O orbitals in La₄Ni₃O₈ despite its larger Δ. Our results clarify the essential characteristics of low valence nickelates and put strong constraints on theoretical interpretations of superconductivity in these materials.
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