In this review, we provide a survey of the application of advanced first-principle methods on the theoretical modeling and understanding of novel electronic, optical, and magnetic properties of the spin-orbit coupled Ruddlesden–Popper series of iridates Srn+1IrnO3n+1 (n = 1, 2, and ∞). After a brief description of the basic aspects of the adopted methods (noncollinear local spin density approximation plus an on-site Coulomb interaction (LSDA+U), constrained random phase approximation (cRPA), GW, and Bethe–Salpeter equation (BSE)), we present and discuss select results. We show that a detailed phase diagrams of the metal–insulator transition and magnetic phase transition can be constructed by inspecting the evolution of electronic and magnetic properties as a function of Hubbard U, spin–orbit coupling (SOC) strength, and dimensionality n, which provide clear evidence for the crucial role played by SOC and U in establishing a relativistic (Dirac) Mott–Hubbard insulating state in Sr2IrO4 and Sr3Ir2O7. To characterize the ground-state phases, we quantify the most relevant energy scales fully ab initio—crystal field energy, Hubbard U, and SOC constant of three compounds—and discuss the quasiparticle band structures in detail by comparing GW and LSDA+U data. We examine the different magnetic ground states of structurally similar n = 1 and n = 2 compounds and clarify that the origin of the in-plane canted antiferromagnetic (AFM) state of Sr2IrO4 arises from competition between isotropic exchange and Dzyaloshinskii–Moriya (DM) interactions whereas the collinear AFM state of Sr3Ir2O7 is due to strong interlayer magnetic coupling. Finally, we report the dimensionality controlled metal–insulator transition across the series by computing their optical transitions and conductivity spectra at the GW+BSE level from the the quasi two-dimensional insulating n = 1 and 2 phases to the three-dimensional metallic n=∞ phase.
Advanced First-Principle Modeling of Relativistic Ruddlesden—Popper Strontium Iridates