Metal-insulator transition in layered nickelates La$_3$Ni$_2$O$_{7-\delta}$ ($\delta$=0.0, 0.5, 1)

TL;DR

This study uses ab initio methods to analyze the electronic and magnetic properties of layered nickelates La$_3$Ni$_2$O$_{7-eta}$, revealing diverse insulating and metallic behaviors and their relation to structural and electronic factors.

Contribution

It provides a detailed theoretical analysis of the metal-insulator transition in layered nickelates, highlighting the role of quantum confinement and band structure in their electronic states.

Findings

The $eta=0.5$ compound is insulating with Ni in a high-spin S=1 state.

The $eta=1$ compound exhibits a correlated molecular insulating state despite being nominally metallic.

The metallic compound has a larger bandwidth of e$_g$ states supporting paramagnetic metallic behavior.

Abstract

Three low-valence layered nickelates with general formula La$_3$Ni$_2$O$_{7-\delta}$ ($\delta$=0.0, 0.5, 1) are studied by ab initio techniques. Both the insulating and metallic limits are analyzed, together with the compound at the Mott transition ($\delta$= 0.5; Ni$^{2+}$), that shows insulating behavior, with all Ni atoms in a S=1 high-spin state. The compound in the $\delta$= 1 limit (La$_3$Ni$_2$O$_6$), with mean formal valence Ni$^{1.5+}$ and hence nominally metallic, nevertheless shows a correlated {\it molecular} insulating state, produced by the quantum confinement of the NiO$_2$ bilayers and the presence of mainly d$_{z^2}$ bands (bonding-antibonding split) around the gap. The metallic compound shows a larger bandwidth of the e$_g$ states that can sustain the experimentally observed paramagnetic metallic properties. The evolution of the in-plane antiferromagnetic coupling with the oxygen content is discussed, and also the similarities of this series of compounds with the layered superconducting cuprates.