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Register a new userHigh pressure floating zone growth and structural properties of ferrimagnetic quantum paraelectric BaFe$_{12}$O$_{19}$
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High quality single crystals of BaFe$_{12}$O$_{19}$ were grown using the floating zone technique in flowing oxygen pressurized to 100 atm. Single crystal neutron diffraction was used to determine the nuclear and magnetic structure of BaFe$_{12}$O$_{19}$ at 4 K and 295 K. At both temperatures, there exist local electric dipoles formed by the off-mirror-plane displacements of magnetic Fe$^{3+}$ ions at the bipyramidal sites. The displacement at 4 K is about half of that at room temperature. The temperature dependence of the specific heat shows no anomaly associated with long range polar ordering in the temperature range from 1.90-300 K. The inverse dielectric permittivity, $1/varepsilon$, along the c-axis shows a $T^2$ temperature dependence between 10 K and 20 K, with a significantly reduced temperature dependence displayed below 10 K. Moreover, as the sample is cooled below 1.4 K there is an anomalous sharp upturn in $1/varepsilon$. These features resemble those of classic quantum paraelectrics such as SrTiO$_3$. The presence of the upturn in $1/varepsilon$ indicates that BaFe$_{12}$O$_{19}$ is a critical quantum paraelectric system with Fe$^{3+}$ ions involved in both magnetic and electric dipole formation.
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Single crystals of the metallic Ruddlesden-Popper trilayer nickelates R$_4$Ni$_3$O$_{10}$ (R=La, Pr) were successfully grown using an optical-image floating zone furnace under oxygen pressure (pO$_2$) of 20 bar for La$_4$Ni$_3$O$_{10}$ and 140 bar for Pr$_4$Ni$_3$O$_{10}$. A combination of synchrotron and laboratory x-ray single crystal diffraction, high-resolution synchrotron x-ray powder diffraction and measurements of physical properties revealed that R$_4$Ni$_3$O$_{10}$ (R=La, Pr) crystallizes in the monoclinic $P$2$_1$/$a$ (Z=2) space group at room temperature, and that a metastable orthorhombic phase ($Bmab$) can be trapped by post-growth rapid cooling. Both La$_4$Ni$_3$O$_{10}$ and Pr$_4$Ni$_3$O$_{10}$ crystals undergo a metal-to-metal transition (MMT) below room temperature. In the case of Pr$_4$Ni$_3$O$_{10}$, the MMT is found at ~157.6 K. For La$_4$Ni$_3$O$_{10}$, the MMT depends on the lattice symmetry: 147.5 K for $Bmab$ vs. 138.6 K for $P$2$_1$/$a$. Lattice anomalies were found at the MMT that, when considered together with the pronounced dependence of the transition temperature on subtle structural differences between $Bmab$ and $P$2$_1$/$a$ phases, demonstrates a not insignificant coupling between electronic and lattice degrees of freedom in these trilayer nickelates.
We report the growth of large single-crystals of Cu2MnAl, a ferromagnetic Heusler compound suitable for polarizing neutron monochromators, by means of optical floating zone under ultra-high vacuum compatible conditions. Unlike Bridgman or Czochralsky grown Cu2MnAl, our floating zone grown single-crystals show highly reproducible magnetic properties and an excellent crystal quality with a narrow and homogeneous mosaic spread as examined by neutron diffraction. An investigation of the polarizing properties in neutron scattering suggests a high polarization efficiency, limited by the relatively small sample dimensions studied. Our study identifies optical floating zone under ultra-high vacuum compatible conditions as a highly reproducible method to grow high-quality single-crystals of Cu2MnAl.
Single crystals of PrNiO3 were grown under an oxygen pressure of 295 bar using a unique high-pressure optical-image floating zone furnace. The crystals, with volume in excess of 1 mm3, were characterized structurally using single crystal and powder X-ray diffraction. Resistivity, specific heat, and magnetic susceptibility were measured, all of which evidenced an abrupt, first order metal-insulator transition (MIT) at ~130 K, in agreement with previous literature reports on polycrystalline specimens. Temperature-dependent single crystal diffraction was performed to investigate changes through the MIT. Our study demonstrates the opportunity space for high fugacity, reactive environments for single crystal growth specifically of perovskite nickelates but more generally to correlated electron oxides.
We have developed the laser-diode-heated floating zone (LDFZ) method, in order to improve the broad and inhomogeneous light focusing in the conventional lamp-heated floating zone method, which often causes difficulties in the crystal growth especially for the incongruently melting materials. We have simulated the light focusing properties of the LDFZ method to make irradiated light homogeneous and restricted mostly to the molten zone. We have designed and assembled an LDFZ furnace, and have demonstrated how it works through actual crystal growth. The method is applicable to various kinds of materials, and enables stable and reproducible crystal growth even for the incongruently melting materials. We have succeeded in the crystal growth of representative incongruently melting materials such as BiFeO3 and (La,Ba)2CuO4, which are difficult to grow by the conventional method. Tolerance to the decentering of the sample and highly efficient heating are also established in the LDFZ method.
The structural properties of Thallium (III) oxide (Tl2O3) have been studied both experimentally and theoretically under compression at room temperature. X-ray powder diffraction measurements up to 37.7 GPa have been complemented with ab initio total-energy calculations. The equation of state of Tl2O3 has been determined and compared to related compounds. It has been found experimentally that Tl2O3 remains in its initial cubic bixbyite-type structure up to 22.0 GPa. At this pressure, the onset of amorphization is observed, being the sample fully amorphous at 25.2 GPa. The sample retains the amorphous state after pressure release. To understand the pressure-induced amorphization process, we have studied theoretically the possible high-pressure phases of Tl2O3. Although a phase transition is predicted at 5.8 GPa to the orthorhombic Rh2O3-II-type structure and at 24.2 GPa to the orthorhombic a-Gd2S3-type structure, neither of these phases were observed experimentally, probably due to the hindrance of the pressure-driven phase transitions at room temperature. The theoretical study of the elastic behavior of the cubic bixbyite-type structure at high-pressure shows that amorphization above 22 GPa at room temperature might be caused by the mechanical instability of the cubic bixbyite-type structure which is theoretically predicted above 23.5 GPa.
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