Tuning Crystal Field Potential by Orbital Dilution in Strongly Correlated d4 Oxides

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 d3 substitution at d4 sites. The structure of the d3 − d4 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.