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Electron-Doped Sr2IrO4-delta (0 <= delta <= 0.04): Evolution of a Disordered Jeff = 1/2 Mott Insulator into an Exotic Metallic State

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 Added by Gang Cao
 Publication date 2010
  fields Physics
and research's language is English




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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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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.
290 - B. J. Kim , Hosub Jin , S. J. Moon 2008
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 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.
Heterointerfaces in complex oxide systems open new arenas in which to test models of strongly correlated material, explore the role of dimensionality in metal-insulator-transitions (MITs) and small polaron formation. Close to the quantum critical point Mott MITs depend on band filling controlled by random disordered substitutional doping. Delta-doped Mott insulators are potentially free of random disorder and introduce a new arena in which to explore the effect of electron correlations and dimensionality. Epitaxial films of the prototypical Mott insulator GdTiO3 are delta-doped by substituting a single (GdO)+1 plane with a monolayer of charge neutral SrO to produce a two-dimensional system with high planar doping density. Unlike metallic SrTiO3 quantum wells in GdTiO3 the single SrO delta-doped layer exhibits thermally activated DC and optical conductivity that agree in a quantitative manner with predictions of small polaron transport but with an extremely high two-dimensional density of polarons, ~ 7E14 cm-2
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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