ABSTRACT
The optical floating zone crystal growth technique is a well-established method for obtaining large, high-purity single crystals. While the floating zone method has been constantly evolving for over six decades, the development of high-pressure (up to 1000 bar) growth systems has only recently been realized via the combination of laser-based heating sources with an all-metal chamber. While our inaugural high-pressure laser floating zone furnace design demonstrated the successful growth of new volatile and metastable phases, the furnace design faces several limitations with imaging quality, heating profile control, and chamber cooling power. Here, we present a second-generation design of the high-pressure laser floating zone furnace, "Laser Optical Kristallmacher II" (LOKII), and demonstrate that this redesign facilitates new advances in crystal growth by highlighting several exemplar materials: α-Fe2O3, ß-Ga2O3, and La2CuO4+δ. Notably, for La2CuO4+δ, we demonstrate the feasibility and long-term stability of traveling solvent floating zone growth under a record pressure of 700 bar.
ABSTRACT
In this study, we employ bulk electronic properties characterization and x-ray scattering/spectroscopy techniques to map the structural, magnetic and electronic properties of (Eu1-x Ca x )2Ir2O7 as a function of Ca-doping. As expected, the metal-insulator transition temperature, T MIT, decreases with Ca-doping until a metallic state is realized down to 2 K. In contrast, T AFM becomes decoupled from the MIT and (likely short-range) AFM order persists into the metallic regime. This decoupling is understood as a result of the onset of an electronically phase separated state, the occurrence of which seemingly depends on both synthesis method and rare earth site magnetism. PDF analysis suggests that electronic phase separation occurs without accompanying chemical phase segregation or changes in the short-range crystallographic symmetry while synchrotron x-ray diffraction confirms that there is no change in the long-range crystallographic symmetry. X-ray absorption measurements confirm the J eff = ½ character of (Eu1-x Ca x )2Ir2O7. Surprisingly these measurements also indicate a net electron doping, rather than the expected hole doping, indicating a compensatory mechanism. Lastly, XMCD measurements show a weak Ir magnetic polarization that is largely unaffected by Ca-doping. Keywords: term, term, term.
ABSTRACT
In this study, we employ bulk electronic properties characterization and x-ray scattering/spectroscopy techniques to map the structural, magnetic and electronic properties of (Eu1-xCax)2Ir2O7as a function of Ca-doping. As expected, the metal-insulator transition temperature, TMIT, decreases with Ca-doping until a metallic state is realized down to 2 K. In contrast, the onset of magnetic order at TAFMbecomes decoupled from TMITand (likely short-range) antiferromagnetism persists into the metallic regime. This decoupling is understood as a result of the onset of an electronically phase separated state, the occurrence of which seemingly depends on both synthesis method and rare earth site magnetism. PDF analysis suggests that electronic phase separation occurs without accompanying chemical phase segregation or changes in the short-range crystallographic symmetry while synchrotron x-ray diffraction confirms that there is no change in the long-range crystallographic symmetry. X-ray absorption measurements confirm the Jeff = ½ character of (Eu1-xCax)2Ir2O7. Surprisingly these measurements also indicate a net electron doping, rather than the expected hole doping, indicating a compensatory mechanism. Lastly, XMCD measurements show a weak Ir magnetic polarization that is largely unaffected by Ca-doping.
ABSTRACT
The floating zone technique is a well-established single crystal growth method in materials research, which is able to produce volumetrically large specimens with extremely high purities. However, traditional furnace designs have relied on heating from high-powered bulb sources in combination with parabolic mirrors and hence are constrained to transparent growth chambers with large solid angles of optical access. This results in a stark limitation on achievable processing gas pressures and in turn renders a range of compounds unsuitable for crystal growth by the floating zone technique, either due to excessive volatility or due to metastability. Here, we demonstrate a novel high-pressure laser-based floating zone system (HP-LFZ). The use of lasers for heating allows implementation of a high-strength metal growth chamber, permitting greatly enhanced processing pressures over conventional mirror-based designs, with the current design allowing for pressures up to 1000 bar. We demonstrate a series of example single crystal growths using this design in pressures up to 675 bar, a significant increase over processing pressures attainable in commercially available floating zone systems. The general utility of the HP-LFZ is also illustrated via growths of a range of complex oxides.
ABSTRACT
The breakdown of [Formula: see text] antiferromagnetism in the limit of strong disorder is studied in Sr3(Ir1-x Mn x )2O7. Upon Mn-substitution, antiferromagnetic ordering of the Ir cations becomes increasingly two-dimensional, resulting in the complete suppression of long-range Ir magnetic order above [Formula: see text]. Long-range antiferromagnetism however persists on the Mn sites to higher Mn concentrations (x > 0.25) and is necessarily mediated via a random network of majority Ir sites. Our data suggest a shift in the Mn valence from Mn4+ to Mn3+ at intermediate doping levels, which in turn generates nonmagnetic Ir5+ sites and suppresses long-range order within the Ir network. The collapse of long-range [Formula: see text] antiferromagnetism and the survival of percolating antiferromagnetic order on Mn-sites demonstrates a complex 3d-5d exchange process that surprisingly enables minority Mn spins to order far below the conventional percolation threshold for a bilayer square lattice.
ABSTRACT
Materials that exhibit both strong spin-orbit coupling and electron correlation effects are predicted to host numerous new electronic states. One prominent example is the Jeff = 1/2 Mott state in Sr2IrO4, where introducing carriers is predicted to manifest high temperature superconductivity analogous to the S = 1/2 Mott state of La2CuO4. While bulk superconductivity currently remains elusive, anomalous quasiparticle behaviors paralleling those in the cuprates such as pseudogap formation and the formation of a d-wave gap are observed upon electron-doping Sr2IrO4. Here we establish a magnetic parallel between electron-doped Sr2IrO4 and hole-doped La2CuO4 by unveiling a spin density wave state in electron-doped Sr2IrO4. Our magnetic resonant X-ray scattering data reveal the presence of an incommensurate magnetic state reminiscent of the diagonal spin density wave state observed in the monolayer cuprate (La1-xSr x )2CuO4. This link supports the conjecture that the quenched Mott phases in electron-doped Sr2IrO4 and hole-doped La2CuO4 support common competing electronic phases.
