Ab initio determination of excitation energies and magnetic couplings in correlated, quasi two-dimensional iridates

Abstract

To determine the strength of essential electronic and magnetic interactions in the iridates Sr${}_2$IrO${}_4$ and Ba${}_2$IrO${}_4$ - potential platforms for high-temperature superconductivity - we use many-body techniques from wavefunction-based electronic-structure theory. Multiplet physics, spin-orbit interactions, and Ir-O hybridization are all treated on equal footing, fully {\it ab initio}. Our calculations put the lowest d-d excitations of Sr${}_2$IrO${}_4$/Ba${}_2$IrO${}_4$ at 0.69/0.64 eV, substantially lower than in isostructural cuprates. Charge-transfer excitations start at 3.0/1.9 eV and the magnetic nearest-neighbor exchange coupling is 51/58 meV. Available experimental results are fully consistent with these values, which strongly constrains the parametrization of effective iridate Hamiltonians.

References in corpus (15)

• 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
• Isospin Dynamics in Sr2IrO4 : Forging Links to Cuprate Superconductivity
• Twisted Hubbard Model for Sr2IrO4: Magnetism and Possible High Temperature Superconductivity
• Topological insulators and metal-insulator transition in the pyrochlore iridates
• Finite-temperature phase diagram of the Heisenberg-Kitaev model
• Microscopic study of spin-orbit-induced Mott insulator in Ir oxides
• Reduced effective spin-orbital degeneracy and spin-orbital ordering in paramagnetic transition metal oxides: Sr2IrO4 vs. Sr2RhO4
• Kitaev-Heisenberg-J2-J3 model for the iridates A2IrO3
• Spin-Orbit Integrated Ground State and Magnetic Anisotropy in Sr${}_2$IrO${}_4$
• Electronic structures of layered perovskite Sr2MO4 (M=Ru, Rh, and Ir)
• Resonant Inelastic X-ray Scattering on Spin-Orbit Coupled Insulating Iridates

Cited by in corpus (46)

• On the Origin of Zigzag Magnetic Order in Iridium Oxide Na2IrO3
• Crystal field splitting and correlation effect on the electronic structure of A2IrO3
• Kitaev interactions between j=1/2 moments in honeycomb Na2IrO3 are large and ferromagnetic: insights from ab initio quantum chemistry calculations
• Excitonic quasiparticles in a spin-orbit Mott insulator
• Giant Magnon Gap in Bilayer Iridate Sr3Ir2O7: Enhanced Pseudo-dipolar Interactions Near the Mott Transition
• Robustness of basal-plane antiferromagnetic order and the $J_{eff}=1/2$ state in single-layer iridate spin-orbit Mott insulators
• Ba2YIrO6: A cubic double perovskite material with Ir5+ ions
• Square Lattice Iridates
• Magnetic couplings, optical spectra, and spin-orbit exciton in 5d electron Mott insulator Sr2IrO4
• Mixing of $t_{2g}$-$e_g$ orbitals in 4d and 5d transition metal oxides
• Anisotropic Magnetic Couplings and Structure-Driven Canted to Collinear Transitions in Spin-orbit Coupled Sr2IrO4
• Strongly frustrated triangular spin lattice emerging from triplet dimer formation in honeycomb Li2IrO3
• CaIrO3: a Spin-Orbit Mott Insulator Beyond the jeff = 1/2 Ground State
• Insights into the High Temperature Superconducting Cuprates from Resonant Inelastic X-ray Scattering
• Coulomb Correlations in 4d and 5d Oxides from First Principles - or How Spin-Orbit Materials choose their Effective Orbital Degeneracies
• Topological states in pyrochlore iridates: long-range anisotropy strongly competing with spin-orbit interaction
• Magnetic state of pyrochlore Cd2Os2O7 emerging from strong competition of ligand distortions and longer-range crystalline anisotropy
• Tuning Magnetic Coupling in Sr${}_2$IrO${}_4$ Thin Films with Epitaxial Strain
• Impact of spin-orbit coupling on the magnetism of Sr3MIrO6 (M = Ni, Co)
• Theoretical study of insulating mechanism in multi-orbital Hubbard models with a large spin-orbit coupling: Slater versus Mott scenario in Sr${}_2$IrO${}_4$
• CaIrO3 post-perovskite, a j = 1/2 quasi-one-dimensional antiferromagnet
• Interplay of many-body and single-particle interactions in iridates and rhodates
• Magnetic excitations and electronic interactions in Sr${}_2$CuTeO${}_6$: a spin-1/2 square lattice Heisenberg antiferromagnet
• The electronic structure of the high-symmetry perovskite iridate Ba2IrO4
• Mechanism of basal-plane antiferromagnetism in the spin-orbit driven iridate Ba2IrO4
• Electronic correlations and magnetic interactions in infinite-layer NdNiO${}_2$
• Pressure-Induced Confined Metal from the Mott Insulator Sr3Ir2O7
• Orbital occupancies and the putative jeff = 1/2 groundstate in Ba2IrO4: a combined oxygen K edge XAS and RIXS study
• Exchange Interactions Mediated by Non-Magnetic Cations in Double Perovskites
• First-order structural transition and pressure-induced lattice/phonon anomalies in Sr${}_2$IrO${}_4$
• Substrate-tuning of correlated spin-orbit oxides
• Correlation induced electron-hole asymmetry in quasi-2D iridates
• Anisotropic interactions opposing magnetocrystalline anisotropy in Sr${}_3$NiIrO${}_6$
• Magnetic properties of bilayer Sr${}_3$Ir${}_2$O${}_7$: role of epitaxial strain and oxygen vacancies
• Magnetic critical properties and basal-plane anisotropy of Sr${}_2$IrO${}_4$
• Analysis of resonant inelastic x-ray scattering from Sr${}_2$IrO${}_4$ in an itinerant-electron approach
• $J_1$-$J_2$ square lattice antiferromagnetism in the orbitally quenched insulator MoOPO${}_4$
• Multiband $d-p$ model and self-doping in the electronic structure of Ba${}_2$IrO${}_4$
• Influence of multiplet structure on photoemission spectra of spin-orbit driven Mott insulators: application to $\mathbf{S}{\mathbf{r}}_2\mathbf{Ir}{\mathbf{O}}_4$
• Precise control of $J_{\mathrm{eff}}=1/2$ magnetic properties in Sr${}_2$IrO${}_4$ epitaxial thin films by variation of strain and thin film thickness
• Charge ordering in Ir dimers in the ground state of Ba${}_5$AlIr${}_2$O${}_{11}$
• Possible superconductivity induced by a large spin-orbit coupling in carrier doped iridium oxide insulators: A weak coupling approach
• Collective excitations in Na${}_2$IrO${}_3$
• The rich phase diagram of the prototypical iridate Ba${}_2$IrO${}_4$: Effective low-energy models and metal-insulator transition
• Electronic excitations and spin interactions in chromium trihalides from embedded many-body wavefunctions
• Possibility of an unconventional spin state of Ir${}^{4+}$ in Ba${}_{21}$Ir${}_9$O${}_{43}$ single crystal