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Epitaxial growth and antiferromagnetism of Sn-substituted perovskite iridate SrI r 0.8 S n 0.2 O 3

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Abstract

5d iridates have shown vast emergent phenomena due to a strong interplay among their lattice, charge, and spin degrees of freedom, because of which the potential in spintronic application of the thin-film form is highly leveraged. Here we have epitaxially stabilized perovskite SrIr0.8Sn0.2O3 on [001] SrTiO3 substrates through pulsed laser deposition and systematically characterized the structural, electronic, and magnetic properties. Physical property measurements unravel an insulating ground state with a weak ferromagnetism in the compressively strained epitaxial film. The octahedral rotation pattern is identified by synchrotron x-ray diffraction, resolving a mix of a+b−c− and a−b+c− domains. X-ray magnetic resonant scattering directly demonstrates a G-type antiferromagnetic structure of the magnetic order and the spin canting nature of the weak ferromagnetism.

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Effects of spin-orbit interactions in condensed matter are an important and rapidly evolving topic. Strong competition between spin-orbit, on-site Coulomb and crystalline electric field interactions in iridates drives exotic quantum states that are unique to this group of materials. In particular, the "Jeff = ½" Mott state served as an early signal that the combined effect of strong spin-orbit and Coulomb interactions in iridates has unique, intriguing consequences. In this Key Issues Review, we survey some current experimental studies of iridates. In essence, these materials tend to defy conventional wisdom: absence of conventional correlations between magnetic and insulating states, avoidance of metallization at high pressures, "S-shaped" I-V characteristic, emergence of an odd-parity hidden order, etc. It is particularly intriguing that there exist conspicuous discrepancies between current experimental results and theoretical proposals that address superconducting, topological and quantum spin liquid phases. This class of materials, in which the lattice degrees of freedom play a critical role seldom seen in other materials, evidently presents some profound intellectual challenges that call for more investigations both experimentally and theoretically. Physical properties unique to these materials may help unlock a world of possibilities for functional materials and devices. We emphasize that, given the rapidly developing nature of this field, this Key Issues Review is by no means an exhaustive report of the current state of experimental studies of iridates. &#13.
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We investigated magnetotransport properties and charge dynamics of strain-free perovskite SrIrO3. Both the longitudinal and transverse magnetoresistivity (MR) are significantly enhanced with decreasing temperature, in accord with the evolution of the Dirac semimetallic state. The electron correlation effect in the Dirac state shows up as a dramatic change in charge dynamics with temperature and as an enhanced paramagnetic susceptibility. We propose that the field-induced topological transition of the Dirac node coupled to the enhanced paramagnetism causes the unique MR of correlated Dirac electrons.
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A high-pressure metastable orthorhombic phase of SrIrO 3 perovskite has been epitaxially stabilized on several substrates (DyScO 3 , GdScO 3 , NdScO 3 and SrTiO 3 ) in the form of thin monocrystalline layers with (110) surface orientation. The unit-cell parameters of the pseudomorphic thin SrIrO 3 layers depend on the biaxial strain imposed by the various substrates due to the different lattice mismatches of the particular substrate and the bulk orthorhombic SrIrO 3 structure. Using X-ray diffractometry, it is shown that both compressive and tensile strain increase the lattice parameters a and b , while the angle γ scales with the applied strain, being smaller or larger than 90° for compressive or tensile strain, respectively, resulting in a small monoclinic distortion of the layer unit cell. Owing to the similarity of the substrate and layer lattices, the diffraction signals from the two structures overlap partially, which complicates structure determination by standard refinement methods using measured integrated intensities. The measured signal is composed of two interfering components corresponding to the waves diffracted by the substrate and by the layer, where the first component is calculated exactly using the known substrate structure, while the second one is determined by the unknown unit-cell parameters of the layer. The unit-cell parameters were refined in order to fit the experimental data with the simulation. The fractional coordinates of the atoms in the unit cell resulting from the fit are similar to those in the bulk structure.
Article
Measuring how the magnetic correlations throughout the Brillouin zone evolve in a Mott insulator as charges are introduced dramatically improved our understanding of the pseudogap, non-Fermi liquids and high TC superconductivity. Recently, photoexcitation has been used to induce similarly exotic states transiently. However, understanding how these states emerge has been limited because of a lack of available probes of magnetic correlations in the time domain, which hinders further investigation of how light can be used to control the properties of solids. Here we implement magnetic resonant inelastic X-ray scattering at a free electron laser, and directly determine the magnetization dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state ~2ps after the excitation has strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. The magnetism recovers its two-dimensional (2D) in-plane Neel correlations on a timescale of a few ps, while the three-dimensional (3D) long-range magnetic order restores over a far longer, fluence-dependent timescale of a few hundred ps. The dramatic difference in these two timescales, implies that characterizing the dimensionality of magnetic correlations will be vital in our efforts to understand ultrafast magnetic dynamics.
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By using a combination of heteroepitaxial growth, structure refinement based on synchrotron x-ray diffraction, and first-principles calculations, we show that the symmetry-protected Dirac line nodes in the topological semimetallic perovskite SrIrO3 can be lifted simply by applying epitaxial constraints. In particular, the Dirac gap opens without breaking the Pbnm mirror symmetry. In virtue of a symmetry-breaking analysis, we demonstrate that the original symmetry protection is related to the n-glide operation, which can be selectively broken by different heteroepitaxial structures. This symmetry protection renders the nodal line a nonsymmorphic Dirac semimetallic state. The results highlight the vital role of crystal symmetry in spin-orbit-coupled correlated oxides and provide a foundation for experimental realization of topological insulators in iridate-based heterostructures.
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The control of magnetism by electric fields is an important goal for the future development of low-power spintronics. Various approaches have been proposed on the basis of either single-phase multiferroic materials or hybrid structures in which a ferromagnet is influenced by the electric field applied to an adjacent insulator (usually having a ferroelectric, piezoelectric, or multiferroic character). The electric field effect on magnetism can be driven by purely electronic or electrostatic effects or can occur through strain coupling. Here we review progress in the electrical control of magnetic properties (anisotropy, spin order, ordering temperature, domain structure) and its application to prototype spintronic devices (spin valves, magnetic tunnel junctions). We tentatively identify the main outstanding difficulties and give perspectives for spintronics and other fields.
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The structure of the atmospheric pressure form of SrIrO3 is shown to be a monoclinic distortion of the hexagonal BaTiO3 structure (, , , β = 93.26°). The cell dimensions have been studied to 1000°C and the coefficients of thermal expansion given. The structure transforms at 40 kbar and 1000°C to an orthorhombic perovskite (, , ) with a 3% decrease in volume. This high pressure phase only retransforms slowly at atmospheric pressure and 1200°C and exhibits metallic conductivity and Pauli paramagnetism.
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The post-perovskite (pPv) is the high-pressure phase of some highly distorted perovskites. The pPv phase of MgSiO3 stabilized under 125 GPa and 2000 K cannot be quenched to ambient pressure. In contrast, the pPv CaIrO3 can be synthesized under a modest pressure or even at ambient pressure. However, the pPv CaIrO3 has not been fully characterized. We report here systematic structural studies, measurements of transport and magnetic properties including critical phenomena, specific heat, and thermal conductivity in a series of samples Ca1-xSrxIrO3 synthesized under high pressure. The Ca1-xSrxIrO3 samples exhibit an evolution from the pPv phase to the perovskite phase. We have also prepared the perovskite (Pv phase) CaIrO3 with the wet chemical method. Rietveld refinements of the pPv and Pv phase CaIrO3 have been made based on high-resolution synchrotron diffraction. In comparison with effects of the chemical substitution on the crystal structure and physical properties, we have studied the structure and magnetic properties of the pPv CaIrO3 under hydrostatic pressure. Results have been discussed in the context of orbital ordering biased on the intrinsic structural distortion and the strong spin-orbit coupling that is much enhanced in these 5d oxides with the pPv structure.
Article
We discuss phenomena arising from the combined influence of electron correlation and spin-orbit coupling, with an emphasis on emergent quantum phases and transitions in heavy transition metal compounds with 4d and 5d elements. A common theme is the influence of spin-orbital entanglement produced by spin-orbit coupling, which influences the electronic and magnetic structure. In the weak-to-intermediate correlation regime, we show how non-trivial band-like topology leads to a plethora of phases related to topological insulators. We expound these ideas using the example of pyrochlore iridates, showing how many novel phases such as the Weyl semi-metal, axion insulator, topological Mott insulator, and topological insulators may arise in this context. In the strong correlation regime, we argue that spin-orbital entanglement fully or partially removes orbital degeneracy, reducing or avoiding the normally ubiquitous Jahn-Teller effect. As we illustrate for the honeycomb lattice iridates and double perovskites, this leads to enhanced quantum fluctuations of the spin-orbital entangled states and the chance to promote exotic quantum spin liquid and multipolar ordered ground states. Connections to experiments, materials, and future directions are discussed.
Article
We report a single-crystal neutron diffraction study of the layered $\rm Sr_2IrO_4$. This work unambiguously determines the magnetic structure of the system and reveals that the spin orientation rigidly tracks the staggered rotation of the $\rm IrO_6$ octahedra in $\rm Sr_2IrO_4$. The long-range antiferromagnetic order has a canted spin configuration with an ordered moment of 0.208(3) $\mu_B$/Ir site within the basal plane; a detailed examination of the spin canting yields 0.202(3) and 0.049(2) $\mu_B$/site for the a axis and the b axis, respectively. It is intriguing that forbidden nuclear reflections of space group $I4_1/acd$ are also observed in a wide temperature range from 4 K to 600 K, which suggests a reduced crystal structure symmetry. This neutron-scattering work provides a direct, well-refined experimental characterization of the magnetic and crystal structures that are crucial to the understanding of the unconventional magnetism exhibited in this unusual magnetic insulator.
Article
Measurement of the quantum-mechanical phase in quantum matter provides the most direct manifestation of the underlying abstract physics. We used resonant x-ray scattering to probe the relative phases of constituent atomic orbitals in an electronic wave function, which uncovers the unconventional Mott insulating state induced by relativistic spin-orbit coupling in the layered 5d transition metal oxide Sr2IrO4. A selection rule based on intra-atomic interference effects establishes a complex spin-orbital state represented by an effective total angular momentum = 1/2 quantum number, the phase of which can lead to a quantum topological state of matter.
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We study the magnetic interactions in Mott-Hubbard systems with partially filled t_{2g} levels and with strong spin-orbit coupling. The latter entangles the spin and orbital spaces, and leads to a rich variety of the low energy Hamiltonians that extrapolate from the Heisenberg to a quantum compass model depending on the lattice geometry. This gives way to "engineer" in such Mott insulators an exactly solvable spin model by Kitaev relevant for quantum computation. We, finally, explain "weak" ferromagnetism, with an anomalously large ferromagnetic moment, in Sr2IrO4.