Coulomb correlations in 4d and 5d oxides from first principles-or how spin-orbit materials choose their effective...

The interplay of spin-orbit coupling and Coulomb correlations has become a hot topic in condensed matter theory and is especially important in 4d and 5d transition metal oxides, like iridates or rhodates. Here, we review recent advances in dynamical mean-field theory (DMFT)-based electronic structure calculations for treating such compounds, introducing all necessary implementation details. We also discuss the evaluation of Hubbard interactions in spin-orbit materials. As an example, we perform DMFT calculations on insulating strontium iridate (Sr₂IrO₄) and its 4d metallic counterpart, strontium rhodate (Sr₂RhO₄). While a Mott-insulating state is obtained for Sr₂IrO₄ in its paramagnetic phase, the spectral properties and Fermi surfaces obtained for Sr₂RhO₄ show excellent agreement with available experimental data. Finally, we discuss the electronic structure of these two compounds by introducing the notion of effective spin-orbital degeneracy as the key quantity that determines the correlation strength. We stress that effective spin-orbital degeneracy introduces an additional axis into the conventional picture of a phase diagram based on filling and on the ratio of interactions to bandwidth, analogous to the degeneracy-controlled Mott transition in d¹ perovskites.