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

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.