Tuning the metal-insulator transition in d^1 and d^2 perovskites by epitaxial strain: a first principles-based study

TL;DR

This study uses first-principles calculations to explore how epitaxial strain influences the Mott metal-insulator transition in d^1 and d^2 perovskites, revealing strain effects on electronic correlations and phase control.

Contribution

It provides a detailed analysis of strain effects on the Mott transition in perovskites, combining DFT and DMFT to isolate individual influences of crystal-field splitting and hopping parameters.

Findings

Strain-induced crystal-field splitting favors insulating states.

Hopping changes under strain can either promote metallic or insulating phases.

Epitaxial strain can effectively tune electronic correlations in TM oxides.

Abstract

We investigate the effect of epitaxial strain on the Mott metal-insulator transition (MIT) in perovskite systems with d^1 and d^2 electron configuration of the transition metal (TM) cation. We first discuss the general trends expected from the changes in the crystal-field splitting and in the hopping parameters that are induced by epitaxial strain. We argue that the strain-induced crystal-field splitting generally favors the Mott-insulating state, whereas the strain-induced changes in the hopping parameters favor the metallic state under compressive strain and the insulating state under tensile strain. Thus, the two effects can effectively cancel each other under compressive strain, while they usually cooperate under tensile strain, in this case favoring the insulating state. We then validate these general considerations by performing electronic structure calculations for several d^1 and d^2 perovskites, using a combination of density functional theory (DFT) and dynamical mean-field theory (DMFT). We isolate the individual effects of strain-induced changes in either hopping or crystal-field by performing DMFT calculations where we fix one type of parameter to the corresponding unstrained DFT values. These calculations confirm our general considerations for SrVO_3 (d^1) and LaVO_3 (d^2), whereas the case of LaTiO_3 (d^1) is distinctly different, due to the strong effect of the octahedral tilt distortion in the underlying perovskite crystal structure. Our results demonstrate the possibility to tune the electronic properties of correlated TM oxides by using epitaxial strain, which allows to control the strength of electronic correlations and the vicinity to the Mott MIT.