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Bulk single crystal growth of the theoretically predicted magnetic Weyl semimetals $R$AlGe ($R$ = Pr, Ce)

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




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We explore two methods for single crystal growth of the theoretically proposed magnetic Weyl semimetals $R$AlGe ($R$ = Pr,Ce), which prove that a floating zone technique, being both crucible- and flux-free, is crucial to obtain perfectly stoichiometric $R$AlGe crystals. In contrast, the crystals grown by a flux growth technique tend to be Al-rich. We further present both structural and elemental analysis, along with bulk magnetization and electrical resistivity data on the crystals prepared by the floating zone technique. Both systems with the intended 1:1:1 stoichiometry crystallize in the anticipated polar I4$_{1}$md (No. 109) space group, although neither displays the theoretically expected ferromagnetic ground state. Instead PrAlGe displays a spin-glass-like transition below 16 K with an easy-c-axis and CeAlGe has an easy-ab-plane antiferromagnetic order below 5 K. The grown crystals provide an ideal platform for microscopic studies of the magnetic field-tunable correlation physics involving magnetism and topological Weyl nodes.

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We investigate the macroscopic and microscopic physical properties of the solid solution of Ce$_{1-x}$Pr$_{x}$AlGe. The series tunes from CeAlGe with its multi-$vec{k}$ structure and a major Moment in the ab-plane, to PrAlGe with an easy-c-axis ferromagnetic ground state co-existing with a low density of nanoscale textured magnetic Domain walls. Using AC-, DC-susceptiblity, resistivity, specific heat, muon spin relaxation/rotation and neutron scattering we analyze the magnetic ground state of the series. We provide further evidence supporting our previous claim for spin-glass like properties in pure PrAlGe. With introduction of Pr to CeAlGe the finite magnetic field required to stabilize the topological multi-$vec{k}$ magnetic phase for $x=0$ becomes suppressed. The crossover between the two end-member ground states occurs in the vicinity of $x=0.3$, a region where we further anticipate the field-induced topological magnetic phase for $x < 0.3$ to become the zero field ground state.
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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.
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We report on structural and superconducting properties of La(3-x)R(x)Ni2B2N3 where La is substituted by the magnetic rare-earth elements Ce, Pr, Nd. The compounds Pr3Ni2B2N3 and Nd3Ni2B2N3 are characterized for the first time. Powder X-ray diffraction confirmed all samples R3Ni2B2N3 with R = La, Ce, Pr, Nd and their solid solutions to crystallize in the body centered tetragonal La3Ni2B2N3 structure type. Superconducting and magnetic properties of La(3-x)R(x)Ni2B2N3 were studied by resistivity, specific heat and susceptibility measurements. While La3Ni2B2N3 has a superconducting transition temperature Tc ~ 14 K, substitution of La by Ce, Pr, and Nd leads to magnetic pair breaking and, thus, to a gradual suppression of superconductivity. Pr3Ni2B2N3 exibits no long range magnetic order down to 2 K, Nd3Ni2B2N3 shows ferrimagnetic ordering below T_C = 17 K and a spin reorientation transition to a nearly antiferromagnetic state at 10 K.
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