Intertwined charge and spin instability of La${}_3$Ni${}_2$O${}_7$

Abstract

Research on nickel-based superconductors has progressed from infinite-layer LaNiO${}_2$ to finite-layer La${}_6$Ni${}_5$O${}_{12}$, and most recently to the Ruddlesden-Popper phase La${}_3$Ni${}_2$O${}_7$, which was found to exhibits onset of superconductivity at $\sim$80\,K under a pressure of $\sim$16\,GPa. Unlike the superconductivity mainly driven by the $d_{x^2-y^2}$ orbital in infinite-layer nickelates, the Ni-$d_{z^2}$ and O-2$p$ orbitals contribute significantly to the low energy states and potentially to the superconducting electron pairing mechanism of La${}_3$Ni${}_2$O${}_7$. Employing density functional calculations and multi-orbital multi-atom cluster exact diagonalization including local exchange and Coulomb interactions, here we analyze the pressure dependent low-energy electronic states of the Ni${}_2$O${}_9$ cluster, relevant for the bilayer phase of La${}_3$Ni${}_2$O${}_7$. The various possible spin states and the exchange and superexchange mechanisms of the Ni${}_2$O${}_9$ cluster are quantified via the involvement of the Ni-$3d_{3z^2-r^2}$ orbitals and the atomic Hund's rule exchange, the apical bridging O-$2p_z$ orbitals, and the orbitals involved in the formation of local Zhang-Rice singlet like states. We find that the leading configurations contributiong to the cluster ground-states both for nominal valence and also with local charge fluctuations, do not involve occupation of the apical oxygen, instead they favor formation of in-plane Zhang-Rice singlet like states between an O ligand hole and the Ni $3d_{z^2-y^2}$ orbital. We also highlight two possible charge and spin ordered states suggested by our cluster results, that are nearly degenerate at all relevant pressures within our modelling.

13 pages, 9 figures

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Cited by in corpus (5)

• Possible Liquid-Nitrogen-Temperature Superconductivity Driven by Perpendicular Electric Field in the Single-Bilayer Film of La${}_3$Ni${}_2$O${}_7$ at Ambient Pressure
• Charge distribution and magnetism in bilayer La${}_3$Ni${}_2$O${}_7$: a hybrid functional study
• Quantum phase transition driven by competing intralayer and interlayer hopping in bilayer nickelates
• Universal electronic structure of multi-layered nickelates via oxygen-centered planar orbitals
• Magnetically Mediated Cross-Layer Pairing in Pressurized Trilayer Nickelate La${}_4$Ni${}_3$O${}_{10}$