Tuning of the flat band and its impact on superconductivity in Mo5Si3-xPx.

The superconductivity in systems containing dispersionless (flat) bands is seemingly paradoxical, as traditional Bardeen-Cooper-Schrieffer theory requires an infinite enhancement of the carrier masses. However, the combination of flat and steep (dispersive) bands within the multiple band scenario might boost superconducting responses, potentially explaining high-temperature superconductivity in cuprates and metal hydrides. Here, we report on the magnetic penetration depths, the upper critical field, and the specific heat measurements, together with the first-principles calculations for the Mo5Si3-xPx superconducting family. The band structure features a flat band that gradually approaches the Fermi level as a function of phosphorus doping x, reaching the Fermi level at x ≃ 1.3. This leads to an abrupt change in nearly all superconducting quantities. The superfluid density data placed on the 'Uemura plot' results in two separated branches, thus indicating that the emergence of a flat band enhances correlations between conducting electrons.

Superconductivity in a Layered Cobalt Oxychalcogenide Na2CoSe2O with a Triangular Lattice.

Unconventional superconductivity in bulk materials under ambient pressure is extremely rare among the 3d transition metal compounds outside the layered cuprates and iron-based family. It is predominantly linked to highly anisotropic electronic properties and quasi-two-dimensional (2D) Fermi surfaces. To date, the only known example of a Co-based exotic superconductor is the hydrated layered cobaltate, NaxCoO2·yH2O, and its superconductivity is realized in the vicinity of a spin-1/2 Mott state. However, the nature of the superconductivity in these materials is still a subject of intense debate, and therefore, finding a new class of superconductors will help unravel the mysteries of their unconventional superconductivity. Here, we report the discovery of superconductivity at ∼6.3 K in our newly synthesized layered compound Na2CoSe2O, in which the edge-shared CoSe6 octahedra form [CoSe2] layers with a perfect triangular lattice of Co ions. It is the first 3d transition metal oxychalcogenide superconductor with distinct structural and chemical characteristics. Despite its relatively low TC, this material exhibits very high superconducting upper critical fields, µ0HC2(0), which far exceeds the Pauli paramagnetic limit by a factor of 3-4. First-principles calculations show that Na2CoSe2O is a rare example of a negative charge transfer superconductor. This cobalt oxychalcogenide with a geometrical frustration among Co spins shows great potential as a highly appealing candidate for the realization of unconventional and/or high-TC superconductivity beyond the well-established Cu- and Fe-based superconductor families and opens a new field in the physics and chemistry of low-dimensional superconductors.

A quasi-one-dimensional bulk thermoelectrics with high performance near room temperature.

Pursuing efficient thermoelectricity from low-dimensional materials has been highly motivated since the seminal work of Hicks and Dresselhaus. In fact, many superior thermoelectric materials like Bi2Te3, Mg3Sb2/Mg3Bi2 and SnSe are quasi-two-dimensional (q2D), though the advantages of two-dimensionality appear to be diverse and sometimes controversial. Here, we report on a remarkably high thermoelectric performance in TlCu3Te2, which is quasi-one-dimensional (q1D) with a further reduced dimension. The thermoelectric figure of merit zT along its q1D axis amounts to 1.3 (1.5) at 300 (400) K, rivaling the best ever reported at these temperatures. The high thermoelectric performances benefit from, on one hand, large power factors derived from a center-hollowed, pancake-like Fermi pocket with q1D dispersion at the edge of a narrow band gap, and on the other hand, small lattice thermal conductivities caused by the large and anharmonic q1D lattice consisting of heavy, lone-pair-electron bearing (Tl+) and weakly-bonded (Cu+) ions. This compound represents the first bulk material with quasi-uniaxial thermoelectric transport of application level, offering a renewed opportunity to exploit reduced dimensionality for high-performance thermoelectricity.

Superconductivity in Mo4Ga20As with endohedral gallium clusters.

We report the discovery and detailed investigation of superconductivity in Mo4Ga20As. Mo4Ga20As crystallizes in a space group ofI4/m(No. 87), with the lattice parametersa= 12.86352 Å andc= 5.30031 Å. The resistivity, magnetization, and specific heat data reveal Mo4Ga20As to be a type-II superconductor withTc= 5.6 K. The upper and lower critical fields are estimated to be 2.78 T and 22.0 mT, respectively. In addition, electron-phonon coupling in Mo4Ga20As is possibly stronger than the BCS weak-coupling limit. First-principles calculations suggest the Fermi level being dominated by the Mo-4dand Ga-4porbitals.

Superconductivity Induced by Site-Selective Arsenic Doping in Mo5Si3.

Arsenic doping in silicides has been much less studied compared with phosphorus. In this study, superconductivity is successfully induced by As doping in Mo5Si3. The superconducting transition temperature (Tc) reaches 7.7 K, which is higher than those in previously known W5Si3-type superconductors. Mo5Si2As is a type-II BCS superconductor with upper and lower critical fields of 6.65 T and 22.4 mT, respectively. In addition, As atoms are found to selectively take the 8h sites in Mo5Si2As. The emergence of superconductivity is possibly due to the shift of Fermi level as a consequence of As doping, as revealed by the specific heat measurements and first-principles calculations. Our work provides not only another example of As doping but also a practical strategy to achieve superconductivity in silicides through Fermi level engineering.

Microstructure of quasi-one-dimensional superconductor KCr3As3prepared by K-ion deintercalation.

The microstructure of quasi-one-dimensional KCr3As3(133) superconductors, which were prepared by chemical cation deintercalation from their counterpart K2Cr3As3(233) compounds, are investigated using scanning transmission electron microscopy. The nominal KCr3As3crystals generally exhibit irregular nanoscale 133-phase domains accompanied by an amorphous As-deficient phase and cracks as a result of alkali cation deintercalation processes. Analysis of local defective structures reveals the existence of an intermediate state in the transformation from 233 to 133 phase and a possible K-deficient 233-type structure as a nanoscale cluster. Our microscopic investigations offer insight into the microstructure of KCr3As3and the alkali metal cation deintercalation processes.

Inelastic Electron Tunneling in 2H-Ta_{x}Nb_{1-x}Se_{2} Evidenced by Scanning Tunneling Spectroscopy.

We report a detailed study of tunneling spectra measured on 2H-Ta_{x}Nb_{1-x}Se_{2} (x=0∼0.1) single crystals using a low-temperature scanning tunneling microscope. The prominent gaplike feature, which has not been understood for a long time, was found to be accompanied by some "in-gap" fine structures. By investigating the second-derivative spectra and their temperature and magnetic field dependencies, we were able to prove that inelastic electron tunneling is the origin of these features and obtain the Eliashberg function of 2H-Ta_{x}Nb_{1-x}Se_{2} at an atomic scale, providing a potential way to study the local Eliashberg function and the phonon spectra of the related transition-metal dichalcogenides.

Interfacial Superconductivity on the Topological Semimetal Tungsten Carbide Induced by Metal Deposition.

Interfaces between materials with different electronic ground states have become powerful platforms for creating and controlling novel quantum states of matter, in which inversion symmetry breaking and other effects at the interface may introduce additional electronic states. Among the emergent phenomena, superconductivity is of particular interest. Here, by depositing metal films on a newly identified topological semimetal tungsten carbide (WC) single crystal, interfacial superconductivity is obtained, evidenced from soft point-contact spectroscopy. This very robust phenomenon is demonstrated for a wide range of metal/WC interfaces, involving both nonmagnetic and ferromagnetic films, and the superconducting transition temperatures are surprisingly insensitive to the magnetism of thin films. This method offers an opportunity to explore the long-sought topological superconductivity and has potential applications in topological-state-based spin devices.

Tuning the Distance to a Possible Ferromagnetic Quantum Critical Point in A_{2}Cr_{3}As_{3}.

Although superconductivity in the vicinity of an antiferromagnetic (AFM) instability has been extensively explored in the last three decades or so, superconductivity in compounds with a background of ferromagnetic (FM) spin fluctuations is still rare. We report ^{75}As nuclear quadrupole resonance measurements on the A_{2}Cr_{3}As_{3} family, which is the first group of Cr-based superconductors at ambient pressure, with A being alkali elements. From the temperature dependence of the spin-lattice relaxation rate (1/T_{1}), we find that by changing A in the order of A=Na, Na_{0.75}K_{0.25}, K, and Rb, the system is tuned to approach a possible FM quantum critical point (QCP). This may be ascribed to the Cr2-As2-Cr2 bond angle that decreases towards 90°, which enhances the FM interaction via the Cr2-As2-Cr2 path. Upon moving away from the QCP, the superconducting transition temperature T_{sc} increases progressively up to 8.0 K in Na_{2}Cr_{3}As_{3}, which is in sharp contrast to the AFM case where T_{sc} usually shows a maximum around a QCP. The 1/T_{1} decreases rapidly below T_{sc} with no Hebel-Slichter peak, and ubiquitously follows a T^{5} variation below a characteristic temperature T^{*}≈0.6 T_{sc}, which indicates the existence of point nodes in the superconducting gap function commonly in the family. These results suggest that the A_{2}Cr_{3}As_{3} family is a possible solid-state analog of superfluid ^{3}He.

Na-doping effects on structural evolution and superconductivity in (K1-x Na x )2Cr3As3 (x = 0-1).

In this report, we studied the effects of isovalent Na-doping on the recently discovered quasi-one-dimensional Cr-based unconventional superconductor K2Cr3As3. A series of polycrystalline samples with nominal component (K1-x Na x )2Cr3As3 (x = 0-1) were synthesized by the solid state reaction method. From crystal structure and chemical phase characterizations, we found two distinct chemical phases with the same hexagonal structure but distinguished by different site occupancy of Na+ ions at the two kinds of K-site in the K2Cr3As3 lattice structure. When x ⩽ 0.4, the doped samples form a continuous sosoloid phase of (K1-x Na x )2Cr3As3 with the Na+ ions randomly doping at the K-sites (denoted as α-phase); when x ⩾ 0.5, a novel individual phase of (K0.25Na0.75)2Cr3As3 emerges, in which the Na+ ions selectively occupy all the '3k' sites and the K+ ions occupy the '1c' sites (denoted as ß-phase). No chemical phase of Na2Cr3As3 was detected. Superconductivity in these samples was studied by electrical transport and magnetic susceptibility measurements, and it evolves in a much sophisticated manner. In the α-phase, the superconducting T c decreases quickly upon Na-doping. All these α-phase samples have surprisingly low superconducting volume fraction and relatively low T c compared with the undoped K2Cr3As3. However, the ß-phase has a clearly enhanced T c up to 7.6 K which locates between the values of K2Cr3As3 and Na2Cr3As3, and exhibits a full superconducting shielding signal.

Superconductivity in Bi3O2S2Cl with Bi-Cl Planar Layers.

A quaternary compound Bi3O2S2Cl, which consists of novel [BiS2Cl]2- layers, is reported. It adopts a layered structure of the space group I4/ mmm (No. 139) with lattice parameters: a = 3.927(1) Å, c = 21.720(5) Å. In this compound, bismuth and chlorine atoms form an infinite planar layer, which is unique among the bismuth halides. Superconductivity is observed in both polycrystals and single crystals, and is significantly enhanced in the samples prepared with less sulfur or at higher temperatures. By tuning the content of sulfur, Bi3O2S2Cl can be converted from a semiconductor into a superconductor. The superconducting critical temperature ranges from 2.6 to 3.5 K. Our discovery of the [BiS2Cl]2- layer opens another door in searching for the bismuth compounds with novel physical properties.

Superconductivity at 10.4 K in a novel quasi-one-dimensional ternary molybdenum pnictide K2Mo3As3.

Here we report the discovery of the first ternary molybdenum pnictide based superconductor K2Mo3As3. Polycrystalline samples were synthesized by the conventional solid state reaction method. X-ray diffraction analysis reveals a quasi-one-dimensional hexagonal crystal structure with (Mo3As3)2- linear chains separated by K+ ions, similar as previously reported K2Cr3As3, with the space group of P-6m2 (No. 187) and the refined lattice parameters a = 10.145(5) Šand c = 4.453(8) Å. Electrical resistivity, magnetic susceptibility, and heat capacity measurements exhibit bulk superconductivity with the onset Tc at 10.4 K in K2Mo3As3 which is higher than the isostructural Cr-based superconductors. Being the same group VIB transition elements and with similar structural motifs, these Cr and Mo based superconductors may share some common underlying origins for the occurrence of superconductivity and need more investigations to uncover the electron pairing within a quasi-one-dimensional chain structure.

Discovery of a novel 112-type iron-pnictide and La-doping induced superconductivity in Eu1-xLaxFeAs2 (x=0-0.15).

We report the discovery and characterization of a novel 112-type iron pnictide EuFeAs2, with La-doping induced superconductivity in a series of Eu1-xLaxFeAs2. The polycrystalline samples were synthesized through solid state reaction method only within a very narrow temperature window around 1073K. Small single crystals were also grown from a flux method with the size about 100µm. The crystal structure was identified by single crystal X-ray diffraction analysis as a monoclinic structure with space group of P21/m. From resistivity and magnetic susceptibility measurements, we found that the parent compound EuFeAs2 shows distinct anomalies probably due to the Fe2+ related antiferromagnetic/structural phase transition near 110K and the Eu2+ related antiferromagnetic phase transition near 40K. La-doping suppressed both phase transitions to lower temperatures and induced superconducting transitions with a Tc∼11K for Eu0.85La0.15FeAs2.

Atom-Thin SnS2-xSex with Adjustable Compositions by Direct Liquid Exfoliation from Single Crystals.

Two-dimensional (2D) chalcogenide materials are fundamentally and technologically fascinating for their suitable band gap energy and carrier type relevant to their adjustable composition, structure, and dimensionality. Here, we demonstrate the exfoliation of single-crystal SnS2-xSex (SSS) with S/Se vacancies into an atom-thin layer by simple sonication in ethanol without additive. The introduction of vacancies at the S/Se site, the conflicting atomic radius of sulfur in selenium layers, and easy incorporation with an ethanol molecule lead to high ion accessibility; therefore, atom-thin SSS flakes can be effectively prepared by exfoliating the single crystal via sonication. The in situ pyrolysis of such materials can further adjust their compositions, representing tunable activation energy, band gap, and also tunable response to analytes of such materials. As the most basic and crucial step of the 2D material field, the successful synthesis of an uncontaminated and atom-thin sample will further push ahead the large-scale applications of 2D materials, including, but not limited to, electronics, sensing, catalysis, and energy storage fields.

Unconventional superconductivity of NdFeAsO(0.82)F(0.18) indicated by the low temperature dependence of the lower critical field H(c1).

We measured the initial M-H curves for a sample of the newly discovered superconductor NdFeAsO(0.82)Fe(0.18), which had a critical temperature, T(c), of 51 K and was fabricated at the high pressure of 6 GPa. The lower critical field, H(c1), was extracted from the deviation point of the Meissner linearity in the M-H curves, which show linear temperature dependence in the low temperature region down to 5 K. The H(c1)(T) indicates no s-wave superconductivity, but rather an unconventional superconductivity with a nodal gap structure. Furthermore, the linearity of H(c1) at low temperature does not hold at high temperature, but shows other characteristics, indicating that this superconductor might have multi-gap features. Based on the low temperature nodal gap structure, we estimate that the maximum gap magnitude Δ(0) = (1.6 ± 0.2)  k(B)T(c).

Superconductivity in heavily boron-doped silicon carbide.

The discoveries of superconductivity in heavily boron-doped diamond in 2004 and silicon in 2006 have renewed the interest in the superconducting state of semiconductors. Charge-carrier doping of wide-gap semiconductors leads to a metallic phase from which upon further doping superconductivity can emerge. Recently, we discovered superconductivity in a closely related system: heavily boron-doped silicon carbide. The sample used for that study consisted of cubic and hexagonal SiC phase fractions and hence this led to the question which of them participated in the superconductivity. Here we studied a hexagonal SiC sample, free from cubic SiC phase by means of x-ray diffraction, resistivity, and ac susceptibility.