Role of Oxygen States in the Low Valence Nickelate La$_4$Ni$_3$O$_8$ (2110.08937v2)

Abstract: 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 La${4}$Ni${3}$O${8}$ and a prototypical cuprate La${2-x}$Sr${x}$CuO${4}$ ($x=0.35$). 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 $\Delta$. Nevertheless, the transition-metal-oxygen hopping is larger in La${4}$Ni${3}$O${8}$ than in La${2-x}$Sr${x}$CuO${4}$, leading to a significant superexchange interaction and an appreciable hole occupation of the ligand O orbitals in La${4}$Ni${3}$O$_{8}$ despite its larger $\Delta$. Our results clarify the essential characteristics of low valence nickelates and put strong constraints on theoretical interpretations of superconductivity in these materials.