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

Abstract

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

References in corpus (29)

• Anyons in an exactly solved model and beyond
• Electronic Structure of Pyrochlore Iridates: From Topological Dirac Metal to Mott Insulator
• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• Novel Jeff = 1/2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr2IrO4
• Kitaev-Heisenberg Model on Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides $A_2$IrO${}_3$
• Mott physics and band topology in materials with strong spin-orbit interaction
• Relevance of the Heisenberg-Kitaev model for the honeycomb lattice iridates A_2IrO_3
• On the Origin of Zigzag Magnetic Order in Iridium Oxide Na2IrO3
• Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales
• Multiplet ligand-field theory using Wannier orbitals
• Direct evidence of a zigzag spin chain structure in the honeycomb lattice: A neutron and x-ray diffraction investigation on single crystal $\mathrm{N}{\mathrm{a}}_2\mathrm{Ir}{\mathrm{O}}_3$
• Hyper-honeycomb iridate $\beta$-Li2IrO3 as a platform for Kitaev magnetism
• A new spin-anisotropic harmonic honeycomb iridate
• Crystal field splitting and correlation effect on the electronic structure of A2IrO3
• First-Principles Study of the Honeycomb-Lattice Iridates Na2IrO3 in the Presence of Strong Spin-Orbit Interaction and Electron Correlations
• Efficient real frequency solver for dynamical mean field theory
• Ab initio analysis of the tight-binding parameters and magnetic interactions in Na2IrO3
• Na2IrO3 as a molecular orbital crystal
• Non-coplanar and counter-rotating incommensurate magnetic order stabilized by Kitaev interactions in $\gamma$-Li2IrO3
• Excitonic quasiparticles in a spin-orbit Mott insulator
• Magnetic versus crystal field linear dichroism in NiO thin films
• Weyl spin liquids
• Topological Quantum Phase Transition in 5$d$ Transition Metal Oxide Na${}_2$IrO${}_3$
• Topological states in pyrochlore iridates: long-range anisotropy strongly competing with spin-orbit interaction
• Orbital reconstruction in nonpolar tetravalent transition-metal oxide layers
• Orbital occupancies and the putative jeff = 1/2 groundstate in Ba2IrO4: a combined oxygen K edge XAS and RIXS study
• Crystal-field level inversion in lightly Mn-doped Sr3Ru2O7
• Two-Spinon and Orbital Excitations of the Spin-Peierls System TiOCl
• Unoccupied electronic structure of TiOCl studied by x-ray absorption near-edge spectroscopy

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• Probing the $J_{eff}=0$ ground state and the Van Vleck paramagnetism of the Ir${}^{5+}$ ions in the layered Sr${}_2$Co${}_{0.5}$Ir${}_{0.5}$O${}_4$
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• Possibility to realize spin-orbit-induced correlated physics in iridium fluorides
• Magnetization density distribution of Sr${}_2$IrO${}_4$: Deviation from a local $j_{\text{eff}}=1/2$ picture
• Charge transfer energy in iridates: a hard x-ray photoelectron spectroscopy study
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• Strain-induced superconductivity in Sr2IrO4
• High-resolution valence band RIXS at the actinide M${}_{4,5}$-edges
• Absence of localized $5d^1$ electrons in KTaO${}_3$ interface superconductors