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Register a new userAnapole Correlations in Sr2IrO4 Defy the jeff = 1/2 Model
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Zeldovich (spin) anapole correlations in Sr2IrO4 unveiled by magnetic neutron diffraction contravene the spin-orbit coupled ground state used by the jeff = 1/2 (pseudo-spin) model. Specifically, spin and space know inextricable knots which bind each to the other in the iridate. The diffraction property studied in the Letter is enforced by strict requirements from quantum mechanics and magnetic symmetry. It has not been exploited in the past, whereas neutron diffraction by anapole moments is established. Entanglement of the electronic degrees of freedom is captured by binary correlations of the anapole and position operators, and hallmarked in the diffraction amplitude by axial atomic multipoles with an even rank.
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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.
We investigated the temperature-dependent evolution of the electronic structure of the Jeff,1/2 Mott insulator Sr2IrO4 using optical spectroscopy. The optical conductivity spectra $sigma(omega)$ of this compound has recently been found to exhibit two d-d transitions associated with the transition between the Jeff,1/2 and Jeff,3/2 bands due to the cooperation of the electron correlation and spin-orbit coupling. As the temperature increases, the two peaks show significant changes resulting in a decrease in the Mott gap. The experimental observations are compared with the results of first-principles calculation in consideration of increasing bandwidth. We discuss the effect of the temperature change on the electronic structure of Sr2IrO4 in terms of local lattice distortion, excitonic effect, electron-phonon coupling, and magnetic ordering.
The spin-orbit entangled (SOE) Jeff-state has been a fertile ground to study novel quantum phenomena. Contrary to the conventional weakly correlated Jeff=1/2 state of 4d and 5d transition metal compounds, the ground state of CuAl2O4 hosts a Jeff=1/2 state with a strong correlation of Coulomb U. Here, we report that surprisingly Cu2+ ions of CuAl2O4 overcome the otherwise usually strong Jahn-Teller distortion and instead stabilize the SOE state, although the cuprate has relatively small spin-orbit coupling. From the x-ray absorption spectroscopy and high-pressure x-ray diffraction studies, we obtained definite evidence of the Jeff=1/2 state with a cubic lattice at ambient pressure. We also found the pressure-induced structural transition to a compressed tetragonal lattice consisting of the spin-only S=1/2 state for pressure higher than Pc=8 GPa. This phase transition from the Mott insulating Jeff=1/2 to the S=1/2 states is a unique phenomenon and has not been reported before. Our study offers a rare example of the SOE Jeff-state under strong electron correlation and its pressure-induced transition to the S=1/2 state.
Ba3IrTi2O9 crystallizes in a hexagonal structure consisting of a layered triangular arrangement of Ir4+ (Jeff=1/2). Magnetic susceptibility and heat capacity data show no magnetic ordering down to 0.35K inspite of a strong magnetic coupling as evidenced by a large Curie-Weiss temperature=-130K. The magnetic heat capacity follows a power law at low temperature. Our measurements suggest that Ba3IrTi2O9 is a 5d, Ir-based (Jeff=1/2), quantum spin liquid on a 2D triangular lattice.
Stoichiometric Sr2IrO4 is a ferromagnetic Jeff = 1/2 Mott insulator driven by strong spin-orbit coupling. Introduction of very dilute oxygen vacancies into single-crystal Sr2IrO4-delta with delta < 0.04 leads to significant changes in lattice parameters and an insulator-to-metal transition at TMI = 105 K. The highly anisotropic electrical resistivity of the low-temperature metallic state for delta ~ 0.04 exhibits anomalous properties characterized by non-Ohmic behavior and an abrupt current-induced transition in the resistivity at T* = 52 K, which separates two regimes of resisitive switching in the nonlinear I-V characteristics. The novel behavior illustrates an exotic ground state and constitutes a new paradigm for devices structures in which electrical resistivity is manipulated via low-level current densities ~ 10 mA/cm2 (compared to higher spin-torque currents ~ 107-108 A/cm2) or magnetic inductions ~ 0.1-1.0 T.
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