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Floating Zone Growth of Sr Substituted Han Purple: Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$

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 Added by Pascal Puphal
 Publication date 2019
  fields Physics
and research's language is English




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We present a route to grow single crystals of Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$ suitable for inelastic neutron studies via the floating zone technique. Neutron single crystal diffraction was utilized to check their bulk quality and orientation. Finally, the high quality of the grown crystals was proven by X-ray diffraction and magnetic susceptibility.

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We present a structural analysis of the substituted system (Ba$_{1-x}$Sr$_{x}$)CuSi$_{2}$O$_{6}$, which reveals a stable tetragonal crystal structure down to 1.5 K. We explore the structural details with lowtemperature neutron and synchrotron powder diffraction, room-temperature and cryogenic highresolution NMR, as well as magnetic- and specific-heat measurements and verify that a structural phase transition into the orthorhombic structure which occurs in the parent compound BaCuSi2O6, is absent for the x = 0.1 sample. Furthermore, synchrotron powder-diffraction patterns show a reduction of the unit cell for x = 0.1 and magnetic measurements prove that the Cu-dimers are preserved, yet with a slightly reduced intradimer coupling Jintra. Pulse-field magnetization measurements reveal the emergence of a field-induced ordered state, tantamount to Bose-Einsteincondensation (BEC) of triplons, within the tetragonal crystal structure of $I,4_{1}/acd$. This material offers the opportunity to study the critical properties of triplon condensation in a simple crystal structure.
Classical and quantum phase transitions (QPTs), with their accompanying concepts of criticality and universality, are a cornerstone of statistical thermodynamics. An exemplary controlled QPT is the field-induced magnetic ordering of a gapped quantum magnet. Although numerous quasi-one-dimensional coupled spin-chain and -ladder materials are known whose ordering transition is three-dimensional (3D), quasi-2D systems are special for several physical reasons. Motivated by the ancient pigment Han Purple (BaCuSi$_{2}$O$_{6}$), a quasi-2D material displaying anomalous critical properties, we present a complete analysis of Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$. We measure the zero-field magnetic excitations by neutron spectroscopy and deduce the magnetic Hamiltonian. We probe the field-induced transition by combining magnetization, specific-heat, torque and magnetocalorimetric measurements with low-temperature nuclear magnetic resonance studies near the QPT. By a Bayesian statistical analysis and large-scale Quantum Monte Carlo simulations, we demonstrate unambiguously that observable 3D quantum critical scaling is restored by the structural simplification arising from light Sr-substitution in Han Purple.
Neutron diffraction and magnetic susceptibility studies show that orthorhombic single-crystals of topological semimetals ${rm Sr(Mn_{0.9}Cu_{0.1})Sb_2}$ and ${rm Sr(Mn_{0.9}Zn_{0.1})Sb_2}$ undergo three dimensional C-type antiferromagnetic (AFM) ordering of the Mn$^{2+}$ moments at $T_N = 200pm10$ and $210pm12$ K, respectively, significantly lower than that of the parent SrMnSb$_2$ with $T_N=297 pm 3$ K. Magnetization versus applied magnetic field (perpendicular to MnSb planes) below $T_N$ exhibits slightly modified de Haas van Alphen oscillations for the Zn-doped crystal as compared to that of the parent compound. By contrast, the Cu-doped system does not show de Haas van Alphen magnetic oscillations, suggesting that either Cu substitution for Mn changes the electronic structure of the parent compound substantially, or that the Cu sites are strong scatterers of carriers that significantly shorten their mean free path thus diminishing the oscillations. Density functional theory (DFT) calculations including spin-orbit coupling predict the C-type AFM state for the parent, Cu-, and Zn-doped systems and identify the $a$-axis (i.e., perpendicular to the Mn layer) as the easy magnetization direction in the parent and 12.5% of Cu or Zn substitutions. In contrast, 25% of Cu content changes the easy magnetization to the $b$-axis (i.e., within the Mn layer). We find that the incorporation of Cu and Zn in SrMnSb$_2$ tunes electronic bands near the Fermi level resulting in different band topology and semi-metallicity. The parent and Zn-doped systems have coexistence of electron and hole pockets with opened Dirac cone around the Y-point whereas the Cu-doped system has dominant hole pockets around the Fermi level with a distorted Dirac cone. The tunable electronic structure may point out possibilities of rationalizing the experimentally observed de Haas van Alphen magnetic oscillations.
An emerging area in condensed matter physics is the use of multilayered heterostructures to enhance ferroelectricity in complex oxides. Here, we demonstrate that optically pumping carriers across the interface between thin films of a ferroelectric (FE) insulator and a ferromagnetic metal can significantly enhance the FE polarization. The photoinduced FE state remains stable at low temperatures for over one day. This occurs through screening of the internal electric field by the photoexcited carriers, leading to a larger, more stable polarization state that may be suitable for applications in areas such as data and energy storage.
Single crystals of iridates are usually grown by a flux method well above the boiling point of the SrCl2 solvent. This leads to non-equilibrium growth conditions and dramatically shortens the lifetime of expensive Pt crucibles. Here, we report the growth of Sr2IrO4, Sr3Ir2O7 and SrIrO3 single crystals in a reproducible way by using anhydrous SrCl2 flux well below its boiling point. We show that the yield of the different phases strongly depends on the nutrient/solvent ratio for fixed soak temperature and cooling rate. Using this low-temperature growth approach generally leads to a lower temperature-independent contribution to the magnetic susceptibility than previously reported. Crystals of SrIrO3 exhibit a paramagnetic behavior that can be remarkably well fitted with a Curie-Weiss law yielding physically reasonable parameters, in contrast to previous reports. Hence, reducing the soak temperature below the solvent boiling point not only provides more stable and controllable growth conditions in contrast to previously reported growth protocols, but also extends considerably the lifetime of expensive platinum crucibles and reduces the corrosion of heating and thermoelements of standard furnaces, thereby reducing growth costs.
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