Low-Temperature Chiral Crystal Structure and Superconductivity in (Pt0.2Ir0.8)3Zr5.

We report the observation of superconductivity in (Pt0.2Ir0.8)3Zr5 with a chiral space group (P6122) at low temperatures. The bulk nature of the superconductivity at a transition temperature of 2.2 K was confirmed using specific heat measurements. We revealed that (Pt0.2Ir0.8)3Zr5 obeys the weak-coupling Bardeen-Cooper-Schrieffer model, and the dominant mechanism in the upper critical field is the orbital pair-breaking limit rather than the Pauli-Clogston limit. This indicates that the antisymmetric spin-orbit coupling caused by the chiral crystal structure does not significantly affect the superconductivity of (Pt0.2Ir0.8)3Zr5.

Observation of superconductivity and enhanced upper critical field of η-carbide-type oxide Zr4Pd2O.

We report the first observation of bulk superconductivity of a η-carbide-type oxide Zr4Pd2O. The crystal structure and the superconducting properties were studied through synchrotron X-ray diffraction, magnetization, electrical resistivity, and specific heat measurement. The superconducting transition was observed at Tc = 2.73 K. Our measurement revealed that the η-carbide-type oxide superconductor Zr4Pd2O shows an enhanced upper critical field µ0Hc2(0) = 6.72 T, which violates the Pauli-Clogston limit µ0HP = 5.29 T. On the other hand, we found that the enhanced upper critical field is absent in a Rh analogue Zr4Rh2O. The large µ0Hc2(0) of Zr4Pd2O would be raised from strong spin-orbit coupling with Pd-4d electrons. The discovery of new superconducting properties for Zr4Pd2O would shed light on the further development of η-carbide-type oxide superconductors.

Synthesis and Characterization of a Trigonal Layered Compound AgInS2.

Depending on thermal and pressure conditions, AgInS2 exhibits various crystal structures. In this study, we synthesized a high-purity polycrystalline sample of trigonal AgInS2, which is a layered compound, using a high-pressure synthesis technique. The crystal structure was investigated by synchrotron powder X-ray diffraction and the Rietveld refinement. On the basis of band calculation, X-ray photoelectron spectroscopy, and electrical resistance measurements, we found that the obtained trigonal AgInS2 is a semiconductor. Temperature dependencies of electrical resistance of AgInS2 were measured by a diamond anvil cell up to 31.2 GPa. Although semiconducting behavior was suppressed with pressure, metallic behavior was not observed within the pressure range investigated in this study.

Robustness of superconductivity to external pressure in high-entropy-alloy-type metal telluride AgInSnPbBiTe5.

High-entropy-alloy (HEA) superconductors are a new class of disordered superconductors. However, commonality of superconducting characteristics of HEA materials is unclear. Here, we have investigated the crystal and electronic structure, and the robustness of superconducting states in a HEA-type metal telluride (MTe; M = Ag, In, Sn, Pb, Bi) under high pressure, and the results were compared with the pressure effects for a middle-entropy system (AgPbBiTe3) and a reference system of PbTe. When the crystal structure is CsCl-type, all phases show superconductivity under high pressure but exhibit different pressure dependences of the transition temperature (Tc). For PbTe, its Tc decreases with pressure. In contrast, the Tc of HEA-type AgInSnPbBiTe5 is almost independent of pressure, for pressures ranging from 13.0 to 35.1 GPa. Those results suggest that the robustness of superconductivity to external pressure is linked to the configurational entropy of mixing at the M site in MTe. Since the trend is quite similar to previous work on a HEA (Ti-Zr-Hf-Nb-Ta), where the robustness of superconductivity was observed up to ~ 200 GPa, we propose that the robustness of superconductivity under high pressure would be a universal feature in HEA-type superconductors.

Improvement of critical current density of REBa2Cu3O7-δ by increase in configurational entropy of mixing.

REBa2Cu3O7- δ (RE123, RE: rare earth) is one of the high-temperature superconductors with a transition temperature (T c) exceeding 90 K. Because of its high-T c and large critical current density (J c) under magnetic fields, RE123 superconductors have been expected to play a key role in superconductivity application. To accelerate application researches on RE123-based devices, further improvements of J c characteristics have been desired. In this study, we investigated the effects of high-entropy alloying at the RE site on the superconducting properties, through the measurements of local (intra-grain) J c ( J c local ) by a remanent magnetization method. We found that J c local shows a trend to be improved when four or five RE elements are mixed at the RE site, which results in high configurational entropy of mixing (ΔS mix). All samples exhibited an order of few MA cm-2 which is a criterion for practical application and the highest J c local resulted in a value of around 7.0 MA cm-2 at T = 2.0 K. Because high-entropy alloying can improve J c local of RE123 superconductors, our entropy-engineering strategy introduced here would be useful for the development of RE123 superconducting materials available under high magnetic fields.

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.

High-pressure effects on superconducting properties and crystal structure of Bi-based layered superconductor La2O2Bi3Ag0.6Sn0.4S6.

The effects of pressure on the superconducting properties of a Bi-based layered superconductor La2O2Bi3Ag0.6Sn0.4S6, which possesses a four-layer-type conducting layer, have been studied through the electrical resistance and magnetic susceptibility measurements. The crystal structure under pressure was examined using synchrotron x-ray diffraction at SPring-8. In the low-pressure regime, bulk superconductivity with a transition temperatureTcof ∼4.5 K was induced by pressure, which was achieved by in-plane chemical pressure effect owing to the compression of the tetragonal structure. In the high-pressure regime above 6.4 GPa, a structural symmetry lowering was observed, and superconducting transitions with aTc∼ 8 K were observed. Our results suggest the possible commonality on the factor essential forTcin Bi-based superconductors with two-layer-type and four-layer-type conducting layers.

Possible pairing mechanism switching driven by structural symmetry breaking in BiS2-based layered superconductors.

Investigation of isotope effects on superconducting transition temperature (Tc) is one of the useful methods to examine whether electron-phonon interaction is essential for pairing mechanisms. The layered BiCh2-based (Ch: S, Se) superconductor family is a candidate for unconventional superconductors, because unconventional isotope effects have previously been observed in La(O,F)BiSSe and Bi4O4S3. In this study, we investigated the isotope effects of 32S and 34S in the high-pressure phase of (Sr,La)FBiS2, which has a monoclinic crystal structure and a higher Tc of ~ 10 K under high pressures, and observed conventional-type isotope shifts in Tc. The conventional-type isotope effects in the monoclinic phase of (Sr,La)FBiS2 are different from the unconventional isotope effects observed in La(O,F)BiSSe and Bi4O4S3, which have a tetragonal structure. The obtained results suggest that the pairing mechanisms of BiCh2-based superconductors could be switched by a structural-symmetry change in the superconducting layers induced by pressure effects.

Evolution of two bulk-superconducting phases in Sr0.5RE0.5FBiS2 (RE: La, Ce, Pr, Nd, Sm) by external hydrostatic pressure effect.

Polycrystalline samples of Sr0.5RE0.5FBiS2 (RE: La, Ce, Pr, Nd, and Sm) were synthesized via the solid-state reaction and characterized using synchrotron X-ray diffraction. Although all the Sr0.5RE0.5FBiS2 samples exhibited superconductivity at transition temperatures (Tc) within the range of 2.1-2.7 K under ambient pressure, the estimated superconducting volume fraction was small, which indicates non-bulk nature of superconductivity in those samples under ambient pressure. A dramatic increase in shielding fraction, which indicates the emergence of the bulk superconductivity was achieved by applying external hydrostatic pressures. We found that two phases, low-P phases with Tc = 2.5-2.8 K and high-P phases with Tc = 10.0-10.8 K, were induced by the pressure effect for samples with RE = La, Ce, Pr, and Nd. Pressure-Tc phase diagrams indicated that the critical pressure for the emergence of the high-P phase tends to increase with decreasing ionic radius of the doped RE ions, which was explained by the correlation between external and chemical pressure effects. According to the high-pressure X-ray diffraction measurements of Sr0.5La0.5FBiS2, a structural phase transition from tetragonal to monoclinic also occurred at approximately 1.1 GPa. Bulk superconducting phases in Sr0.5RE0.5FBiS2 induced by the external hydrostatic pressure effect are expected to be useful for understanding the effects of both external and chemical pressures to the emergence of bulk superconductivity and pairing mechanisms in BiCh2-based superconductors.

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.