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Register a new userComplex Orbital State Stabilized by Strong Spin-Orbit Coupling in a Metallic Iridium Oxide IrO$_{2}$
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Resonant x-ray diffraction experiments were performed for the metallic iridium oxide IrO$_{2}$. We observed anisotropic tensor of susceptibility (ATS) scattering, the spectrum of which shows a sharp contrast between the $L_{3}$ and $L_{2}$ edges. At the $L_{3}$ edge, resonance excitations were clearly observed from the core 2$p$ orbitals to both the 5$d$ $t_{2g}$ and $e_{g}$ orbitals. In contrast, the resonance mode associated with 5$d$ $t_{2g}$ orbitals was indiscernible at the $L_{2}$ edge. This contrasting behavior indicates that Ir 5$d$ $t_{2g}$ orbitals are fairly close to the $J_{rm eff}$ = 1/2 state due to the strong spin--orbit coupling in 5$d$ transition metal ions, as in the Mott insulator Sr$_{2}$IrO$_{4}$. Our results clearly demonstrate that ATS scattering is a useful probe for investigating complex orbital states in a metallic state. Such states induce novel phenomena such as the spin Hall effect.
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Single-crystalline thin film of an iridium dioxide polymorph Ir2O4 has been fabricated by the pulsed laser deposition of LixIr2O4 precursor and the subsequent Li-deintercalation using soft chemistry. Ir2O4 crystallizes in a spinel (AB2O4) without A cations in the tetrahedral site, which is isostructural to lambda-MnO2. Ir ions form a pyrochlore sublattice, which is known to give rise to a strong geometrical frustration. This Ir spinel was found to be a narrow gap insulator, in remarkable contrast to the metallic ground state of rutile-type IrO2. We argue that an interplay of strong spin-orbit coupling and a Coulomb repulsion gives rise to an insulating ground state as in a layered perovskite Sr2IrO4.
We study the effect of a magnetic field on the low energy description of Mott insulators with strong spin-orbit (SO) coupling. In contrast to the standard case of the Hubbard model without SO coupling, we show that Peierls phases can modulate the magnetic exchange at leading order in the interaction. Our mechanism crucially depends on the existence of distinct exchange paths between neighboring magnetic ions enclosing a well-defined area. Thus it will generically be present in any solid state realisation of the Kitaev model and its extensions. We explicitly calculate the variation of the exchange constants of the so-called $JKGamma$ model as a function of the magnetic flux. We discuss experimental implications of our findings for various settings of candidate Kitaev spin liquids.
We investigated electronic structure of 5d transition-metal oxide Sr2IrO4 using angle-resolved photoemission, optical conductivity, and x-ray absorption measurements and first-principles band calculations. The system was found to be well described by novel effective total angular momentum Jeff states, in which relativistic spin-orbit (SO) coupling is fully taken into account under a large crystal field. Despite of delocalized Ir 5d states, the Jeff-states form so narrow bands that even a small correlation energy leads to the Jeff = 1/2 Mott ground state with unique electronic and magnetic behaviors, suggesting a new class of the Jeff quantum spin driven correlated-electron phenomena.
In atomic physics, the Hund rule says that the largest spin and orbital state is realized due to the interplay of the spin-orbit coupling (SOC) and the Coulomb interactions. Here, we show that in ferromagnetic solids the effective SOC and the orbital magnetic moment can be dramatically enhanced by a factor of $1/[1-(2U^prime-U-J_H)rho_0]$, where $U$ and $U^prime$ are the on-site Coulomb interaction within the same oribtals and between different orbitals, respectively, $J_H$ is the Hund coupling, and $rho_0$ is the average density of states. This factor is obtained by using the two-orbital as well as five-orbital Hubbard models with SOC. We also find that the spin polarization is more favorable than the orbital polarization, being consistent with experimental observations. This present work provides a fundamental basis for understanding the enhancements of SOC and orbital moment by Coulomb interactions in ferromagnets, which would have wide applications in spintronics.
We construct and analyze a microscopic model for insulating rock salt ordered double perovskites, with the chemical formula A$_2$BBO$_6$, where the B atom has a 4d$^1$ or 5d$^1$ electronic configuration and forms a face centered cubic (fcc) lattice. The combination of the triply-degenerate $t_{2g}$ orbital and strong spin-orbit coupling forms local quadruplets with an effective spin moment $j=3/2$. Moreover, due to strongly orbital-dependent exchange, the effective spins have substantial biquadratic and bicubic interactions (fourth and sixth order in the spins, respectively). This leads, at the mean field level, to three main phases: an unusual antiferromagnet with dominant octupolar order, a ferromagnetic phase with magnetization along the $[110]$ direction, and a non-magnetic but quadrupolar ordered phase, which is stabilized by thermal fluctuations and intermediate temperatures. All these phases have a two sublattice structure described by the ordering wavevector ${boldsymbol Q} =2pi (001)$. We consider quantum fluctuations and argue that in the regime of dominant antiferromagnetic exchange, a non-magnetic valence bond solid or quantum spin liquid state may be favored instead. Candidate quantum spin liquid states and their basic properties are described. We also address the effect of single-site anisotropy driven by lattice distortions. Existing and possible future experiments are discussed in light of these results.
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