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 (5)

• 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
• Twisted Hubbard Model for Sr2IrO4: Magnetism and Possible High Temperature Superconductivity
• Microscopic study of spin-orbit-induced Mott insulator in Ir oxides
• Electronic structures of layered perovskite Sr2MO4 (M=Ru, Rh, and Ir)

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