Tuning Crystal Field Potential by Orbital Dilution in $d^4$ Oxides

TL;DR

This paper explores how orbital dilution via doping affects the crystal field potential and orbital order in layered $d^4$ oxides, revealing a mechanism for tuning electronic properties through impurity-induced orbital polarization.

Contribution

It introduces a detailed analysis of impurity effects on spin-orbital coupling and crystal field inversion in strongly correlated $d^4$ oxides, highlighting a novel doping strategy.

Findings

Orbital polarization points towards impurities and outside the impurity-host plane.

Impurity-induced lattice potential can invert the crystal field interaction.

Doping can effectively tune the orbital and electronic structure.

Abstract

We investigate the interplay between Coulomb driven orbital order and octahedral distortions in strongly correlated Mott insulators due to orbital dilution, i.e., doping by metal ions without an orbital degree of freedom. In particular, we focus on layered transition metal oxides and study the effective spin-orbital exchange due to $d^3$ substitution at $d^4$ sites. The structure of the $d^3-d^4$ spin-orbital coupling between the impurity and the host in the presence of octahedral rotations favors a distinct type of orbital polarization pointing towards the impurity and outside the impurity--host plane. This yields an effective lattice potential that generally competes with that associated with flat octahedra and, in turn, can drive an inversion of the crystal field interaction.