Superconductivity in In-doped AgSnBiTe3 with possible band inversion.

We investigated the chemical pressure effects on structural and electronic properties of SnTe-based material using partial substitution of Sn by Ag0.5Bi0.5, which results in lattice shrinkage. For Sn1-2x(AgBi)xTe, single-phase polycrystalline samples were obtained with a wide range of x. On the basis of band calculations, we confirmed that the Sn1-2x(AgBi)xTe system is basically possessing band inversion and topologically preserved electronic states. To explore new superconducting phases related to the topological electronic states, we investigated the In-doping effects on structural and superconducting properties for x = 0.33 (AgSnBiTe3). For (AgSnBi)(1-y)/3InyTe, single-phase polycrystalline samples were obtained for y = 0-0.5 by high-pressure synthesis. Superconductivity was observed for y = 0.2-0.5. For y = 0.4, the transition temperature estimated from zero-resistivity state was 2.4 K, and the specific heat investigation confirmed the emergence of bulk superconductivity. Because the presence of band inversion was theoretically predicted, and the parameters obtained from specific heat analyses were comparable to In-doped SnTe, we expect that the (AgSnBi)(1-y)/3InyTe and other (Ag, In, Sn, Bi)Te phases are candidate systems for studying topological superconductivity.

An efficient way of increasing the total entropy of mixing in high-entropy-alloy compounds: a case of NaCl-type (Ag,In,Pb,Bi)Te1-xSex (x = 0.0, 0.25, 0.5) superconductors.

We propose an efficient way of increasing the entropy of mixing in high-entropy-alloy-type compounds, which can be achieved by multi-site alloying. As an example of this concept, we report the synthesis and observation of polycrystalline samples of new high-entropy-alloy-type metal chalcogenides (Ag,In,Pb,Bi)Te1-xSex (x = 0.0, 0.25, and 0.5) with a NaCl-type structure. The samples were synthesized using high pressure synthesis. Superconductivity with transition temperatures of 2.7, 2.5, and 2.0 K was observed with x = 0.0, 0.25, and 0.5, respectively. To investigate the multi-site alloying effect on the entropy of mixing (ΔSmix) for the examined samples, we calculated the total ΔSmix for two crystallographic sites. For the samples with x = 0.25 and 0.5, ΔSmix reaches 1.89R and 2.00R, respectively, which exceed the ΔSmix of 1.79R for a simple (single-site) high-entropy alloy containing six different elements.

Detection of Hole Pockets in the Candidate Type-II Weyl Semimetal MoTe_{2} from Shubnikov-de Haas Quantum Oscillations.

The bulk electronic structure of T_{d}-MoTe_{2} features large hole Fermi pockets at the Brillouin zone center (Γ) and two electron Fermi surfaces along the Γ-X direction. However, the large hole pockets, whose existence has important implications for the Weyl physics of T_{d}-MoTe_{2}, has never been conclusively detected in quantum oscillations. This raises doubt about the realizability of Majorana states in T_{d}-MoTe_{2}, because these exotic states rely on the existence of Weyl points, which originated from the same band structure predicted by density functional theory (DFT). Here, we report an unambiguous detection of these elusive hole pockets via Shubnikov-de Haas (SdH) quantum oscillations. At ambient pressure, the quantum oscillation frequencies for these pockets are 988 and 1513 T, when the magnetic field is applied along the c axis. The quasiparticle effective masses m^{*} associated with these frequencies are 1.50 and 2.77 m_{e}, respectively, indicating the importance of Coulomb interactions in this system. We further measure the SdH oscillations under pressure. At 13 kbar, we detected a peak at 1798 T with m^{*}=2.86m_{e}. Relative to the oscillation data at a lower pressure, the amplitude of this peak experienced an enhancement, which can be attributed to the reduced curvature of the hole pockets under pressure. Combining our experimental data with DFT+U calculations, where U is the Hubbard parameter, our results shed light on why these important hole pockets have not been detected until now.

Bulk superconductivity in a four-layer-type Bi-based compound La2O2Bi3Ag0.6Sn0.4S5.7Se0.3.

Recently, we reported the observation of superconductivity at ~0.5 K in a La2O2M4S6-type (M: metal) layered compound La2O2Bi3AgS6, which is a layered system related to the BiS2-based superconductor system but possesses a thicker Bi3AgS6-type conducting layer. In this study, we have developed the La2O2Bi3AgS6-type materials by element substitutions to increase the transition temperature (Tc) and to induce bulk nature of superconductivity. A resistivity anomaly observed at 180 K in La2O2Bi3AgS6 was systematically suppressed by Sn substitution for the Ag site. By the Sn substitution, Tc increased, and the shielding volume fraction estimated from magnetization measurements also increased. The highest Tc (=2.3 K) and the highest shielding volume fraction (~20%) was observed for La2O2Bi3Ag0.6Sn0.4S6. The superconducting properties were further improved by Se substitutions for the S site. By the combinational substitutions of Sn and Se, bulk-superconducting phase of La2O2Bi3Ag0.6Sn0.4S5.7Se0.3 with a Tc of 3.0 K (Tconset = 3.6 K) was obtained.

Magnetic, thermal, and neutron diffraction studies of a coordination polymer: bis(glycolato)cobalt(ii).

The two-dimensional quadratic lattice magnet, bis(glycolato)cobalt(ii) ([Co(HOCH2CO2)2]), showed antiferromagnetic ordering at 15.0 K and an abrupt increase in magnetisation at H = 22 600 Oe and 2 K, thereby acting as a metamagnet. Heat capacity measurements revealed that the associated entropy change ΔS around the transition temperature was evaluated to be 6.20 J K-1 mol-1 and that the Co(ii) ion had the total angular momentum of J = 1/2 at low temperatures. Neutron diffraction studies suggested that the magnetic moment vectors of the Co(ii) ions had an amplitude of 3.59µB and were not aligned in a fully antiparallel fashion to those of their neighbours, which caused canting between the magnetic moment vectors in the sheet. The canting angle was determined to be 7.1°. Canting induced net magnetisation in the sheet, but this magnetisation was cancelled between sheets. The magnetisations in the sheets were oriented parallel to the magnetic field at the critical magnetic field.

Na1-xSn2P2 as a new member of van der Waals-type layered tin pnictide superconductors.

Superconductors with a van der Waals (vdW) structure have attracted a considerable interest because of the possibility for truly two-dimensional (2D) superconducting systems. We recently reported NaSn2As2 as a novel vdW-type superconductor with transition temperature (Tc) of 1.3 K. Herein, we present the crystal structure and superconductivity of new material Na1-xSn2P2 with Tc = 2.0 K. Its crystal structure consists of two layers of a buckled honeycomb network of SnP, bound by the vdW forces and separated by Na ions, as similar to that of NaSn2As2. Amount of Na deficiency (x) was estimated to be 0.074(18) using synchrotron X-ray diffraction. Bulk nature of superconductivity was confirmed by the measurements of electrical resistivity, magnetic susceptibility, and specific heat. First-principles calculation using density functional theory shows that Na1-xSn2P2 and NaSn2As2 have comparable electronic structure, suggesting higher Tc of Na1-xSn2P2 resulted from increased density of states at the Fermi level due to Na deficiency. Because there are various structural analogues with tin-pnictide (SnPn) conducting layers, our results indicate that SnPn-based layered compounds can be categorized into a novel family of vdW-type superconductors, providing a new platform for studies on physics and chemistry of low-dimensional superconductors.

Crystal Structure and Superconductivity of Tetragonal and Monoclinic Ce1- xPr xOBiS2.

Ce1- xPr xOBiS2 powders and Ce0.5Pr0.5OBiS2 single crystals were synthesized and their structure and superconductive properties were examined by X-ray diffraction, X-ray absorption, electronic resistivity, and magnetization. While PrOBiS2 was found to be in a monoclinic phase with one-dimensional Bi-S zigzag chains showing no superconductive transition above 0.1 K, CeOBiS2 was in a tetragonal phase with two-dimensional Bi-S planes showing zero resistivity below 1.3 K. In the range x = 0.3-0.9 in Ce1- xPr xOBiS2, both monoclinic and tetragonal phases were formed together with zero resistivity up to a maximum temperature of 2.2 K. A Ce0.5Pr0.5OBiS2 single crystal, which showed both zero resistivity and a decrease in magnetization at ∼2.4 K, presented a tetragonal structure. Short Bi-S bonding in flat two-dimensional Bi-S planes and mixed Ce3+/Ce4+ were characteristic features of the Ce0.5Pr0.5OBiS2 single crystal, which presumably triggered its superconductivity.

Quadrupole effects in tetragonal crystals PrCu2Si2 and DyCu2Si2.

We have investigated quadrupole effects in tetragonal crystals of PrCu2Si2 and DyCu2Si2 by means of low-temperature ultrasonic measurements. The elastic constant C44 of PrCu2Si2 exhibits pronounced softening below 70 K down to a Néel temperature TN = 20 K, which is described in terms of a quadrupole susceptibility for a Γ5 doublet ground state and a Γ3 singlet first excited state located at 15.6 K in the crystalline electric field scheme. The C44 and C66 of DyCu2Si2 also show softening below 70 K down to TN1 = 9.7 K. A low-lying pseudo-sextet state consisting of three Kramers doublets of Γ6⊕2Γ7 brings about softening of C44 and C66 in DyCu2Si2.

Note: Improved sensitivity of magnetic measurements under high pressure in miniature ceramic anvil cell for a commercial SQUID magnetometer.

Two modifications have been made to a miniature ceramic anvil high pressure cell (mCAC) designed for magnetic measurements at pressures up to 12.6 GPa in a commercial superconducting quantum interference (SQUID) magnetometer [N. Tateiwa et al., Rev. Sci. Instrum. 82, 053906 (2011); ibid. 83, 053906 (2012)]. Replacing the Cu-Be piston in the former mCAC with a composite piston composed of the Cu-Be and ceramic cylinders reduces the background magnetization significantly smaller at low temperatures, enabling more precise magnetic measurements at low temperatures. A second modification to the mCAC is the utilization of a ceramic anvil with a hollow in the center of the culet surface. High pressures up to 5 GPa were generated with the "cupped ceramic anvil" with the culet size of 1.0 mm.

Magnetic measurements at pressures above 10 GPa in a miniature ceramic anvil cell for a superconducting quantum interference device magnetometer.

A miniature ceramic anvil high pressure cell (mCAC) was earlier designed by us for magnetic measurements at pressures up to 7.6 GPa in a commercial superconducting quantum interference magnetometer [N. Tateiwa et al., Rev. Sci. Instrum. 82, 053906 (2011)]. Here, we describe methods to generate pressures above 10 GPa in the mCAC. The efficiency of the pressure generation is sharply improved when the Cu-Be gasket is sufficiently preindented. The maximum pressure for the 0.6 mm culet anvils is 12.6 GPa when the Cu-Be gasket is preindented from the initial thickness of 300-60 µm. The 0.5 mm culet anvils were also tested with a rhenium gasket. The maximum pressure attainable in the mCAC is about 13 GPa. The present cell was used to study YbCu(2)Si(2) which shows a pressure induced transition from the non-magnetic to magnetic phases at 8 GPa. We confirm a ferromagnetic transition from the dc magnetization measurement at high pressure. The mCAC can detect the ferromagnetic ordered state whose spontaneous magnetic moment is smaller than 1 µ(B) per unit cell. The high sensitivity for magnetic measurements in the mCAC may result from the simplicity of cell structure. The present study shows the availability of the mCAC for precise magnetic measurements at pressures above 10 GPa.