Doppler-broadened positron annihilation studies in Y-Ba-Cu-O,Tl-Ca-Ba-Cu-O and Bi-Ca-Sr-Cu-O superconductors

Doppler-broadened annihilation radiation spectra have been measured as a function of temperature from 77 K to 300 K, for several high temperature oxide superconductors viz single-phase YBCO, single- and mixed-phase Tl-Ca-Ba-Cu-O and Bi-Ca-Sr-Cu-O compounds. The temperature-dependent parameters extracted respond to a change at the onset of superconducting transition. The observations point to involvement of oxygen valence electrons at the onset of superconducting transition. Also a possible structural change and/or increase in electron density at the oxygen vacancy/defect sites seem to accompany the transition. In addition, the parameters derived are seen to be sensitive to the presence of more than one superconducting phases in mixed phase samples.     

Synthesis of cubic zirconium and hafnium nitride having Th3P4 structure

High-pressure synthesis is a powerful method for the preparation of novel materials with high elastic moduli and hardness. Additionally, such materials may exhibit interesting thermal, optoelectronic, semiconductuing, magnetic or superconducting properties. Here, we report on the high-pressure synthesis of zirconium and hafnium nitrides with the stoichiometry M3N4, where M = Zr, Hf. Synthesis experiments were performed in a laser-heated diamond anvil cell at pressures up to 18 GPa and temperatures up to 3,000 K. We observed formation of cubic Zr3N4 and Hf3N4 (c-M3N4) with a Th3P4-structure, where M-cations are eightfold coordinated by N anions. The c-M3N4 phases are the first binary nitrides with such a high coordination number. Both compounds exhibit high bulk moduli around 250 GPa, which indicates high hardness. Moreover, the new nitrides, c-Zr3N4 and c-Hf3N4, may be the first members of a larger group of transition metal and/or lanthanide nitrides with interesting ferromagnetic or superconducting behaviour.     

Electromagnetic wave absorbing properties of TMCs (TM=Ti,Zr, Hf,Nb and Ta) and high entropy (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C

Electromagnetic wave (EMW) absorbing materials play a vital role in modern communication and information processing technologies to inhibit information leakage and prevent possible damages to environment and human bodies.Currently,most of EMW absorbing materials are either composites of two or more phases or in the form of nanosheets,nanowires or nanofibers in order to enhance the EMW absorption performance through dielectric loss,magnetic loss and dielectric/magnetic loss coupling.However,the combination of complex shapes/multi phases and nanosizes may compound the difficulties of materials processing,composition and interfaces control as well as performance maintenance during service.Thus,searching for single phase materials with good stability and superior EMW absorbing properties is appealing.To achieve this goal,the EMW absorbing properties of transition metal carbides TMCs (TM=Ti,Zr,Hf,Nb and Ta) and high entropy (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C which belong to ultrahigh temperature ceramics,were investigated in this work.Due to the good electrical conductivity and splitting ofd orbitals into lower energy t2g level and higher energy eg level in TMC6 octahedral arrangement,TMCs (TM=Ti,Zr,Hf,Nb and Ta) exhibit good EMW absorbing properties.Especially,HfC and TaC exhibit superior EMW absorbing properties.The minimum reflection loss (RLmin) value of HfC is -55.8 dB at 6.0 GHz with the thickness of 3.8 mm and the effective absorption bandwidth (EAB) is 6.0 GHz from 12.0 to 18.0 GHz at thickness of 1.9 mm;the RLmin value of TaC reaches-41.1 dB at 16.2 GHz with a thickness of 2.0 mm and the EAB is 6.1 GHz with a thickness of 2.2 mm.Intriguingly,the electromagnetic parameters,i.e.,complex permittivity and permeability are tunable by forming single phase solid solution or high entropy (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C.The RLmin value of high entropy (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C is -38.5 dB at 9.5 GHz with the thickness of 1.9 mm,and the EAB is 2.3 GHz (from 11.3 to 13.6 GHz) atthickness of 1.5 mm.The significance of this work is that it opens a new window to design single phase high performance EMW absorbing materials by dielectric/magnetic loss coupling through tuning the conductivity and crystal field splitting energy of d orbitals of transition metals in carbides,nitrides and possibly borides.     

Imprinting Ferromagnetism and Superconductivity in Single Atomic Layers of Molecular Superlattices

Ferromagnetism and superconductivity are two antagonistic phenomena since ferromagnetic exchange fields tend to destroy singlet Cooper pairs. Reconciliation of these two competing phases has been achieved in vertically stacked heterostructures where these two orders are confined in different layers. However, controllable integration of these two phases in one atomic layer is a longstanding challenge. Here, an interlayer-space-confined chemical design (ICCD) is reported for the synthesis of dilute single-atom-doped TaS₂ molecular superlattice, whereby ferromagnetism is observed in the superconducting TaS₂ layers. The intercalation of 2H-TaS₂ crystal with bulky organic ammonium molecule expands its van der Waals gap for single-atom doping via co-intercalated cobalt ions, resulting in the formation of quasi-monolayer Co-doped TaS₂ superlattices. Isolated Co atoms are decorated in the basal plane of the TaS₂ via substituting the Ta atom or anchoring at a hollow site, wherein the orbital-selected p–d hybridization between Co and neighboring Ta and S atoms induces local magnetic moments with strong ferromagnetic coupling. This ICCD approach can be applied to various metal ions, enabling the synthesis of a series of crystal-size TaS₂ molecular superlattices.     

Multifilamentary superconducting (NbTa)-Sn Composite wire by solid-liquid reaction for possible application above 20 tesla

Nb alloyed with Ta was employed in fabricating multifilamentary composite wires of (NbTa)-Sn using the liquid-infiltration process. The superconducting A15 phase was formed with subsequent heat treatments at 800–950°C by the solid-liquid reaction. High inductive T_c's of 18.2K with sharp transition width (<0.3K) and high overall J_c's of ～1.6 × 10⁴ A/cm² at 20T and 4.2K were obtained. It was found that 2 wt.% Ta in the Nb was sufficient in the enhancement of the overall J_c at the high fields and in increasing the H_c2 (4.2K) to 25T.     

Structure and superconductivity studies on ternary equiatomic silicides,MM′Si

A series of ternary equiatiomic transition metal silicidesMM′Si (M=Zr, Nb, Ta;M′=Ru, Re) and Zr_1/2 M _1/2 RuSi (M=Nb, Ta) have been synthesized and characterized. Guinier x-ray data clearly indicate that the compoundsMM′Si (M=Nb, Ta;M′=Ru, Re) crystallize with the orthorhombic TiFeSi-structure. This is contrary to one of the literature reports ascribing the hexagonal ZrRuSi structure toMReSi,M=Nb, Ta. ZrRuSi and Zr_1/2 M _1/2RuSi (M=Nb, Ta), however, crystallize with the ZrRuSi structure. All the compounds are metallic and exhibit small and negative Seebeck coefficients. Superconductivity has been discovered inMM′Si,M=Nb, Ta;M′=Ru, Re and the transition temperatures, as measured by the low frequency a.c. susceptibility technique, range from 2·7 to 5·1 K. Zr_1/2Nb_1/2RuSi is not superconducting above 2·2 K. The observed properties are explained in terms of the electronic charge transfer effects and crystal structures adopted by these metal excess ternary silicides. Dedicated to the memory of Prof. N S Satya Murthy.     

First-principles study of structural stabilities,elastic and electronic properties of transition metal monocarbides (TMCs) and mononitrides (TMNs)

The structural stabilities, elastic and electronic properties of 5d transition metal mononitrides (TMNs) XN with (X = Ir, Os, Re, W and Ta) and 5d transition metal monocarbides (TMCs) XC with (X = Ir, Os, Re and Ta) were investigated using the full-potential linear muffin-tin orbital (FP-LMTO) method, in the framework of the density functional theory (DFT) within the local density approximation (LDA) for the exchange correlation functional. The ground state quantities such as the lattice parameter, bulks modulus and its pressure derivatives for the six considered crystal structures, Rock-salt (B1), CsCl (B2), zinc-blend (B3), Wurtzite (B4), NiAs (B8₁) and the tungsten carbides (B_h) are calculated. The elastic constants of TMNs and TMCs compounds in its different stable phases are determined by using the total energy variation with strain technique. The elastic modulus for polycrystalline materials, shear modulus (G), Young's modulus (E), and Poisson's ratio (ν) are calculated. The Debye temperature (θ_D) and sound velocities (v_m) were also derived from the obtained elastic modulus. The analysis of the hardness of the herein studied compounds classifies OsN – (B4 et B8₁), ReN – (B8₁), WN – (B8₁) and OsC – (B8₁) as superhard materials. Our results for the band structure and densities of states (DOS), show that TMNs and TMCs compounds in theirs energetically and mechanically stable phase has metallic characteristic with strong covalent nature Metal–Nonmetal elements.     

Superconductivity of new ternary borides with the LuRuB2-type structure

A new group of superconducting ternary borides has been found with the general formula MTB₂, where M is Sc, Y or Lu and T is Ru or Os. The superconducting transition temperatures range from 1.3K for ScOsB₂ to 10.0K for LuRuB₂. Additionally, ismorphous compounds with M=Tb, Dy, Ho, Er or Tm order magnetically with critical temperatures in the range 2K to 46K. The occurrence of superconductivity and magnetism in this new ternary boride structure is discussed with respect to analogous data in MT₄B₄ systems.     

一种新的过渡金属层状材料Na4Cu3TaAs4的结构和物理性质(英文)

我们报道了一种新的过渡金属层状砷化物Na4Cu3TaAs4的合成、结构和物理性质.这种材料采用Ⅰ√2 m空间群,晶胞参数为a=5.9101(3)?,c=13.8867(12)?.这个材料的结构中包含两层Na,而Na夹在反氧化铅型(Cu/Ta)As层之间,类似于"111"型铁基超导体NaFeAs.过渡金属位由75%的Cu和25%的Ta占据,Ta形成了明确的√2超结构.Cu和Ta分别为+1和+5价.角分辨光电子能谱测得的Na4Cu3TaAs4能带结构能够和DFT计算结果良好地吻合.角分辨光电子能谱和输运测量均表明该材料表现为金属行为,具有p型载流子.磁化率测量表明该材料表现为几乎不依赖温度的抗磁性.这种新材料扩展了含有反氧化铅型层的材料系统,并为进一步研究该材料系统提供了一个很好的平台.     

Phase separation in superoxygenated La2-xSrxCuO4+y

The complex interplay between superconducting and magnetic phases remains poorly understood. Here, we report on the phase separation of doped holes into separate magnetic and superconducting regions in superoxygenated La(2-x)Sr(x)CuO(4+y), with various Sr contents. Irrespective of Sr-doping, excess oxygen raises the superconducting onset to 40 K with a coexisting magnetic spin-density wave that also orders near 40 K in each of our samples. The magnetic region is closely related to the anomalous, 1/8-hole-doped magnetic versions of La(2)CuO(4), whereas the superconducting region is optimally doped. The two phases are probably the only truly stable ground states in this region of the phase diagram. This simple two-component system is a candidate for electronic phase separation in cuprate superconductors, and a key to understanding seemingly conflicting experimental observations.     

Low-temperature phase diagram of the heavy-fermion superconductor UPt3

The transition to the superconducting state of UPt₃ has been studied in specific-heat experiments on polycrystalline and single-crystalline samples in dependence of heat treatment, purity of starting materials and deviations from stoichiometry, as well as on substituted compounds. The concepts behind the splitting of the transition in two anomalies that are 60 mK apart are critically reviewed. The superconducting phase diagram in the B-T plane has been studied with the use of a sensitive dilatometric technique. The three superconducting phases meet at a tetracritical point and all four phase lines are of second order. From the length anomalies at the phase boundaries the pressure derivatives of the phase lines have been determined and the most stable phase under uniaxial pressure along the c-axis has been identified.     

Nonlinear dielectric response of AgNb(1-x)Ta(x)O3 in the vicinity of diffuse phase transitions

Linear and nonlinear dielectric studies of AgNb(1-x)Ta(x)O(3) (ATN) ceramics (x ≤ 0.6) were carried out in the temperature range of 80 to 673K. The temperature dependences of third-order nonlinear electric susceptibility X3'(T) exhibit two distinct maxima: at the temperature of the weak ferroelectric phase appearance, M(1)-M(2) transition, and at the temperature of the Nb/Ta ion dynamics freezing, Tf. For AgNbO3, they appear at 325K and 448K, respectively. With increasing Ta concentration, both maxima shift toward lower temperature: 4K/%Ta (M(1)-M(2)) and 5.6K/%Ta (T(f)). The X3' (T) maxima indicate changes of the Nb/Ta ion dynamics and their contribution to electric susceptibility. At T(f), a partial freezing of the Nb/Ta ion displacements to the disordered antipolar, antiferroelectric array takes place. At the M(1)-M(2) transition, further freezing of Nb/Ta displacements to polar weak relaxor ferroelectric or dipolar glass transition occurs. This polar state coexists with the ground antiferroelectric state. Studies of the aging process showed that below T(f) the aging influence on electric susceptibility is substantial, whereas above Tf it may be neglected. This means that for ATN ceramics in the concentration range used for applications, there is no aging process in the room temperature region, which is an additional advantage of this system.     

The magnetic susceptibility of transition-metal A15-type phases

The temperature dependence of the paramagnetic susceptibility was measured for several binary A15-type compounds of transition elements. Measurements were made between room temperature and either 3° K or the superconducting transition temperature, whichever was higher. The susceptibilities were found to have, in most cases, a small linear temperature dependence. Molar susceptibilities x _M , superconducting transition temperaturesT _c, and electronic specific heat coefficients for these compounds, when plotted as a function of the valence-electron concentratione/a, reveal peaks at ane/a of about 6.5 for all three properties. Compounds containing the 4d-series transition-elements molybdenum or niobium have higherT _c and lower x _M values than compounds containing the 3d transition-element chromium or vanadium. It appears that an increased mixing of atoms on either of the two crystallographic sites in the A15-type structure can be associated with a significant decrease in the paramagnetic susceptibility of the compound.Work performed under the auspices of the U.S. Atomic Energy Commission.     

The effect of resolidification on preform optimized infiltration growth processed (Y,Nd, Sm,Gd)BCO,multi-grain bulk superconductor

Controlling the microstructure of superconductors by incorporating the flux pinning centers and reducing the macro-defects to improve high field performance is the topic of recent research. In continuation, the preform optimized infiltration growth (POIG) processed YBa₂Cu₃O_7−δ (YBCO) system, Y-site substituted with three mixed RE (Nd, Sm, Gd) elements is investigated. 20 wt.% of (Nd, Sm, Gd)₂BaCuO₅ were mixed with Y₂BaCuO₅ and POIG processed in reduced oxygen atmosphere to obtain YNSG superconductor. No seed is employed for crystal growth; hence the processed samples are multi-grained. Microstructural and compositional investigations on YNSG revealed the presence of different phases in the matrix as well as in precipitates which are of the order of submicron to 4 μm. A large fraction of macro-defects (∼6% of porosity) was observed in the YNSG sample. For reducing the unwanted macro-defects and refine the non-superconducting precipitates, processed YNSG sample is pressed and resolidified (by infiltrating the liquid phases once again) in an argon atmosphere and the structural, microstructural, elemental and superconducting properties are compared with YNSG and undoped samples. Due to spatial scatter in superconducting critical temperatures, caused by the distribution of different REBCO unit cells in YBCO, superconducting transition curve is sharp in YNSG, whereas the resolidified sample showed the broad transition due to solidified liquid phases.     

Crystallization-induced superconductivity in amorphous Ti-Ta-Si alloys

Amorphous alloys containing 0 to 40 at% Ta and 15 to 20 at% Si have been produced in the ternary Ti-Ta-Si system by rapidly quenching the melts using a melt-spinning technique. The amorphous alloys did not show any superconducting transition down to liquid helium temperature (4.2 K). However, a transition was detected above 4.2 K after inducing crystallization in these alloys by annealing at appropriate temperatures. The superconducting transition temperature, T _c, increased with increasing tantalum content and showed the highest value of 7.6 K for the Ti₄₅Ta₄₀Si₁₅ alloy annealed for 1 h at 1073 K. An upper critical magnetic field, H _c2 of 4.7×10⁶ Am^–1 at 4.2 K and a critical current density, J _c, of 1.5×10⁴ A cm^–2 at zero applied field and 4.2 K were recorded for this alloy. Detailed electron microscopic studies of the crystallization behaviour of the amorphous alloys established that a supersaturated solid solution of tantalum in -Ti with a bcc structure forms first, followed by the precipitation of the bc tetragonal Ta₃Si compound. Since Ta₃Si is not superconducting above 4.2 K, it has been concluded that superconductivity in the crystallized alloys is due to the precipitation of -Ti(Ta) solid solution.     

A Simple,General Synthetic Route toward Nanoscale Transition Metal Borides

Most nanomaterials, such as transition metal carbides, phosphides, nitrides, chalcogenides, etc., have been extensively studied for their various properties in recent years. The similarly attractive transition metal borides, on the contrary, have seen little interest from the materials science community, mainly because nanomaterials are notoriously difficult to synthesize. Herein, a simple, general synthetic method toward crystalline transition metal boride nanomaterials is proposed. This new method takes advantage of the redox chemistry of Sn/SnCl₂, the volatility and recrystallization of SnCl₂ at the synthesis conditions, as well as the immiscibility of tin with boron, to produce crystalline phases of 3d, 4d, and 5d transition metal nanoborides with different morphologies (nanorods, nanosheets, nanoprisms, nanoplates, nanoparticles, etc.). Importantly, this method allows flexibility in the choice of the transition metal, as well as the ability to target several compositions within the same binary phase diagram (e.g., Mo₂B, α‐MoB, MoB₂, Mo₂B₄). The simplicity and wide applicability of the method should enable the fulfillment of the great potential of this understudied class of materials, which show a variety of excellent chemical, electrochemical, and physical properties at the microscale.     

Oxide glass filaments and their superconducting phase by annealing

Bi₄Ca₃Sr₃Cu _x O _y (4334) oxide glasses with different concentrations of the transition metal copper have been prepared by rapid quenching technique from respective melts. These glasses have been characterized from electrical, magnetic, dielectric and other properties. The semiconducting glasses are not superconducting even down to 4·2 K. However, by properly annealing the glasses in air or in oxygen atmosphere they can be converted into the corresponding superconducting phases with superconducting transition temperatures between 70 and 110 K depending on the Cu ion concentrations. The dc conductivity of the glasses could be explained with small polaron adiabatic hopping mechanism. Analysis shows that the correlated barrier hopping (CBH) mechanism is the most appropriate model for explaining the a.c. conductivities of these glasses. Addition of a small amount (about 2 wt%) of B₂O₃ makes it possible to draw glass filaments which could also be converted into the superconducting phase withT _c values lower than those obtained from the respective pure glasses.     

Metastable Polymorphic Phases in Monolayer TaTe2

Polymorphic phases and collective phenomena—such as charge density waves (CDWs)—in transition metal dichalcogenides (TMDs) dictate the physical and electronic properties of the material. Most TMDs naturally occur in a single given phase, but the fine-tuning of growth conditions via methods such as molecular beam epitaxy (MBE) allows to unlock otherwise inaccessible polymorphic structures. Exploring and understanding the morphological and electronic properties of new phases of TMDs is an essential step to enable their exploitation in technological applications. Here, scanning tunneling microscopy (STM) is used to map MBE-grown monolayer (ML) TaTe₂. This work reports the first observation of the 1H polymorphic phase, coexisting with the 1T, and demonstrates that their relative coverage can be controlled by adjusting synthesis parameters. Several superperiodic structures, compatible with CDWs, are observed to coexist on the 1T phase. Finally, this work provides theoretical insight on the delicate balance between Te…Te and Ta–Ta interactions that dictates the stability of the different phases. The findings demonstrate that TaTe₂ is an ideal platform to investigate competing interactions, and indicate that accurate tuning of growth conditions is key to accessing metastable states in TMDs.     

Electric Properties of Contacts t o HTS Thin Films at Current Densities J > J c

The role of superconducting film contacts when transporting critical current density was investigated using d.c. and electric short pulses. It was found that both d.c. and pulse current exceeding critical current I _c dissipate at the film contacts, i.e. at the metal/superconductor planar interface containing an intermediate layer of degraded superconductor. Current I > I _c dissipation at the contacts initiates electric-thermal destruction of the superconducting film cathode. The resulting damage to the film is explained in terms of the formation of a (p/i/n) junction at the normal-metal(n)/mixed-state super-conductor(p) interface containing (i) layer of low electric conductivity.