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Register a new userCaIrO3: a Spin-Orbit Mott Insulator Beyond the jeff = 1/2 Ground State
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In CaIrO3 electronic correlation, spin-orbit coupling, and tetragonal crystal field splitting are predicted to be of comparable strength. However, the nature of its ground state is still object of debate, with contradictory experimental and theoretical results. We probe the ground state of CaIrO3 and assess the effective tetragonal crystal field splitting and spin-orbit coupling at play in this system by means of resonant inelastic x-ray scattering. We conclude that insulating CaIrO3 is not a jeff = 1/2 iridate and discuss the consequences of our finding to the interpretation of previous experiments. In particular, we clarify how the Mott insulating state in iridates can be readily extended beyond the jeff = 1/2 ground state.
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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 performed resonant x-ray diffraction experiments at the $L$ absorption edges for the post-perovskite-type compound CaIrO$_{3}$ with $(t_{2g})^5$ electronic configuration. By observing the magnetic signals, we could clearly see that the magnetic structure was a striped order with an antiferromagnetic moment along the c-axis and that the wavefunction of a $t_{2g}$ hole is strongly spin-orbit entangled, the $J_{rm eff} =1/2$ state. The observed spin arrangement is consistent with theoretical work predicting a unique superexchange interaction in the $J_{rm eff} =1/2$ state and points to the universal importance of the spin-orbit coupling in Ir oxides, irrespective of the local coordination and lattice topology. We also propose that the non-magnetic resonant scattering is a powerful tool for unraveling an orbital state even in a metallic iridate.
As a hallmark of electronic correlation, spin-charge interplay underlies many emergent phenomena in doped Mott insulators, such as high-temperature superconductivity, whereas the half-filled parent state is usually electronically frozen with an antiferromagnetic order that resists external control. We report on the observation of a new positive magnetoresistance that probes the staggered susceptibility of a pseudospin-half square-lattice Mott insulator built as an artificial SrIrO3/SrTiO3 superlattice. Its size is particularly large in the high-temperature insulating paramagnetic phase near the Neel transition. This novel magnetoresistance originates from a collective charge response to the large longitudinal spin fluctuations under a linear coupling between the external magnetic field and the staggered magnetization enabled by strong spin-orbit interaction. Our results demonstrate a magnetic control of the binding energy of the fluctuating particle-hole pairs in the Slater-Mott crossover regime analogous to the BCS-to-Bose-Einstein condensation crossover of ultracold-superfluids.
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.
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.
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