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

Fuente: arXiv
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Autores principales: Jiang, Guiwen, Qin, Chenye, Foyevtsova, Kateryna, Si, Liang, Berciu, Mona, Sawatzky, George A., Jiang, Mi
Formato: Preprint
Publicado: 2024
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author Jiang, Guiwen
Qin, Chenye
Foyevtsova, Kateryna
Si, Liang
Berciu, Mona
Sawatzky, George A.
Jiang, Mi
author_facet Jiang, Guiwen
Qin, Chenye
Foyevtsova, Kateryna
Si, Liang
Berciu, Mona
Sawatzky, George A.
Jiang, Mi
contents 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.
format Preprint
id arxiv_https___arxiv_org_abs_2410_15649
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Intertwined charge and spin instability of La$_3$Ni$_2$O$_7$
Jiang, Guiwen
Qin, Chenye
Foyevtsova, Kateryna
Si, Liang
Berciu, Mona
Sawatzky, George A.
Jiang, Mi
Superconductivity
Strongly Correlated Electrons
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.
title Intertwined charge and spin instability of La$_3$Ni$_2$O$_7$
topic Superconductivity
Strongly Correlated Electrons
url https://arxiv.org/abs/2410.15649