Layer- and Orbital-Selective Mott Physics Driving Dimensional Crossover in Nickelate Superlattices

Abstract

The design of quantum materials to manipulate dimensionality and electronic correlations is a central focus in the exploration of emergent phenomena. We propose a new correlated quantum material platform for realizing a layer- and orbital-selective Mott transition (LOSMT) in a nickelate heterostructure by combining bilayer and monolayer LaNiO$_3$ separated by a monolayer LaAlO$_3$ spacer under compressive strain from the LaAlO$_3$ substrate. The LOSMT emerges from the layer-dependent dimensional confinement of the apical Ni($d$)-$z^2$ orbital and strain-induced lifting of the orbital degeneracy. The monolayer LaNiO$_3$ exhibits an orbital-selective Mott insulating phase with a Mott gap in the Ni($d$)-$z^2$ orbital, whereas the bilayer LaNiO$_3$ exhibits a multi-orbital metallic phase, triggering the orbital-selective Mott transition upon cooling $via$ inter-layer hybridization of the Ni($d$)-$z^2$ orbitals. Calculations within the density functional theory plus dynamical mean-field theory (DFT+DMFT) framework reveal that the LOSMT drives a dimensional crossover by enabling out-of-plane electronic transport through the metallization of the localized apical Ni($d$)-$z^2$ orbital, while the planar Ni($d$)-$x^2-y^2$ orbital remains itinerant across the transition. The emergence of the LOSMT provides a new pathway for engineering correlated quantum materials toward unconventional superconductivity and Mott-transistor functionalities.