Testing the validity of the strong spin-orbit-coupling limit for octahedrally coordinated iridates in a model system Sr${}_3$CuIrO${}_6$

Abstract

The electronic structure of Sr${}_3$CuIrO${}_6$, a model system for the 5d Ir ion in an octahedral environment, is studied through a combination of resonant inelastic x-ray scattering (RIXS) and theoretical calculations. RIXS spectra at the Ir L${}_3$-edge reveal an Ir $t_{2g}$ manifold that is split into three levels, in contrast to the expectations of the strong spin-orbit-coupling limit. Effective Hamiltonian and $abinito$ quantum chemistry calculations find a strikingly large non-cubic crystal field splitting comparable to the spin-orbit coupling, which results in a strong mixing of the $j_{\mathsf{eff}}=1/2$ and $j_{\mathsf{eff}}=3/2$ states and modifies the isotropic wavefunctions on which many theoretical models are based.

to appear in phys. Rev. Lett

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Cited by in corpus (76)

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• Ab initio analysis of the tight-binding parameters and magnetic interactions in Na2IrO3
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• Slaving of the magnetic moment canting to the correlated oxygen rotation in Sr2IrO4 revealed by X-ray resonant scattering
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• Emergent excitation at the magnetic metal-insulator transition in the pyrochlore osmate Cd2Os2O7
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• Determination of Hund's coupling in 5d Oxides using Resonant Inelastic X-ray Scattering
• Orbital reconstruction in nonpolar tetravalent transition-metal oxide layers
• Topological states in pyrochlore iridates: long-range anisotropy strongly competing with spin-orbit interaction
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• Resonant X-ray scattering and the $j_{\mathrm{eff}}=1/2$ electronic ground state in iridate perovskites
• Magnetic state of pyrochlore Cd2Os2O7 emerging from strong competition of ligand distortions and longer-range crystalline anisotropy
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• X-ray scattering study of pyrochlore iridates: crystal structure, electronic and magnetic excitations
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• Spectroscopic evidence for polaronic behaviour of the strong spin-orbit insulator Sr${}_3$Ir${}_2$O${}_7$
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• Evolution of structure, magnetism and electronic transport in doped pyrochlore iridate Y${}_2$Ir${}_{2-x}$Ru${}_x$O${}_7$
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• Strong antiferromagnetic interaction owing to a large trigonal distortion in the spin-orbit-coupled honeycomb lattice iridate CdIrO${}_3$
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• Covalency-driven collapse of strong spin-orbit coupling in face-sharing iridium octahedra
• Density matrix renormalization group study of a three-orbital Hubbard model with spin-orbit coupling in one dimension
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