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We have investigated the electronic structure of Sr2IrO4 using core levelresonant inelastic x-ray scattering. The experimental spectra can be wellreproduced using ab initio density functional theory based multiplet ligandfield theory calculations, thereby validating these calculations. We found thatthe low-energy, effective Ir t2g orbitals are practically degenerate in energy.We uncovered that covalency in Sr2IrO4, and generally in iridates, is verylarge with substantial oxygen ligand hole character in the Ir t2g Wannierorbitals. This has far reaching consequences, as not only the onsitecrystal-field energies are determined by the long range crystal-structure, but,more significantly, magnetic exchange interactions will have long rangedistance dependent anisotropies in the spin direction. These findings setconstraints and show pathways for the design of d^5 materials that can hostcompass-like magnetic interactions.

Long-range interactions in the effective low energy Hamiltonian of Sr2IrO4: a core level resonant inelastic x-ray scattering study