Role of Oxygen States in the Low Valence Nickelate La${}_4$Ni${}_3$O${}_8$

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.

13 pages; to appear in PRX

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Cited by in corpus (17)

• Superconductivity in trilayer nickelate La4Ni3O10 under pressure
• Superconducting Instabilities in Strongly-Correlated Infinite-Layer Nickelates
• Exploring Quantum Materials with Resonant Inelastic X-Ray Scattering
• Synthesis and physical properties of LaNiO${}_2$ crystals
• Microscopic Theory of Superconducting Phase Diagram in Infinite-Layer Nickelates
• Many-body electronic structure of $d^{9-\delta }$ layered nickelates
• Charge ordering as the driving mechanism for superconductivity in rare-earth nickel oxides
• Electronic character of charge order in square planar low valence nickelates
• Orbital polarization, charge transfer, and fluorescence in reduced valence nickelates
• Softening of $dd$ excitation in the resonant inelastic x-ray scattering spectra as a signature of Hund's coupling in nickelates
• Absence of mixed valency for Pr in pristine and hole-doped PrNiO${}_2$
• Magnetic excitations in Nd${}_{n+1}$Ni${}_n$O${}_{3n+1}$ Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering
• Pressure effects on the electronic structure and magnetic properties of infinite-layer nickelates
• Numerical study of resonant inelastic X-ray scattering at the oxygen $K$-edge in insulating cuprates
• Superconducting phase diagram of multi-layer square-planar nickelates
• Observation of correlated plasmons in low-valence nickelates
• Resonant inelastic X-ray scattering in the topological semimetal FeSi