Engineering hollow core-shell hetero-structure box to induce interfacial charge modulation for promoting bidirectional sulfur conversion in lithium-sulfur batteries

Severe polysulfide shuttling and sluggish sulfur redox kinetics significantly decrease sulfur utilization and cycling stability in lithium-sulfur batteries(LSBs).Herein,we develop a hollow CoO/CoP-Box core-shell heterostructure as a model and multifunctional catalyst modified on separators to induce interfacial charge modulation and expose more active sites for promoting the adsorption and catalytic conversion ability of sulfur species.Theoretical and experimental findings verify that the in-situ formed core-shell hetero-interface induces the formation of P-Co-O binding and charge redistribution to activate surface O active sites for binding lithium polysulfides(LiPSs)via strong Li-O bonding,thus strongly adsorbing with Li PSs.Meanwhile,the strong Li-O bonding weakens the competing Li-S bonding in LiPSs or Li2S adsorbed on CoO/CoP-Box surface,plus the hollow heterostructure provides abundant active sites and fast electron/Li+transfer,so reducing Li2S nucleation/dissolution activation energy.As expected,LSBs with CoO/CoP-Box modified separator and traditional sulfur/carbon black cathode display a large initial capacity of 1240 mA h g^(-1)and a long cycling stability with 300 cycles(~60.1%capacity retention)at 0.5C.Impressively,the thick sulfur cathode(sulfur loading:5.2 mg cm^(-2))displays a high initial areal capacity of 6.9 mA h cm^(-2).This work verifies a deep mechanism understanding and an effective strategy to induce interfacial charge modulation and enhance active sites for designing efficient dual-directional Li-S catalysts via engineering hollow core-shell hetero-structure.

Strong Anisotropic Order Parameters at All-Nitride Ferromagnet/Superconductor Interfaces

Proximity effects between superconductors and ferromagnets(SC/FM)hold paramount importance in comprehending the spin competition transpiring at their interfaces.This competition arises from the interplay between Cooper pairs and ferromagnetic exchange interactions.The proximity effects between transition metal nitrides(TMNs)are scarcely investigated due to the formidable challenges of fabricating high-quality SC/FM interfaces.We fabricated heterostructures comprising SC titanium nitride(TiN)and FM iron nitride(Fe_(3)N)with precise chemical compositions and atomically well-defined interfaces.The magnetoresistance of Fe_(3)N/TiN heterostructures shows a distinct magnetic anisotropy and strongly depends on the external perturbations.Moreover,the superconducting transition temperatureT_(C) and critical field of TiN experience notable suppression when proximity to Fe_(3)N.We observe the intriguing competition of interfacial spin orientations near𝑇T_(C)(∼1.25 K).These findings not only add a new materials system for investigating the interplay between superconductor and ferromagnets,but also potentially provide a building block for future research endeavors and applications in the realms of superconducting spintronic devices.

Evolution of Superconducting-Transition Temperature with Superfluid Density and Conductivity in Pressurized Cuprate Superconductors

What factors fundamentally determine the value of superconducting transition temperature Tc in high temperature superconductors has been the subject of intense debate.Following the establishment of an empirical law known as Homes'law,there is a growing consensus in the community that the Tc value of the cuprate superconductors is closely linked to the superfluid density(ρ_(s))of its ground state and the conductivity(σ)of its normal state.However,all the data supporting this empirical law(ρ_(s)=AσT_(c))have been obtained from the ambientpressure superconductors.In this study,we present the first high-pressure results about the connection of the quantities of ρ_(s) and σ with T_(c),through the studies on the Bi_(1.74)Pb_(0.38)Sr_(1.88)CuO_(6+δ)and Bi_(2)Sr_(2)CaCu_(2)O_(8+δ),in which the value of their high-pressure resistivity(ρ=1/σ)is achieved by adopting our newly established method,while the quantity ofρs is extracted using Homes'law.We highlight that the Tc values are strongly linked to the joint response factors of magnetic field and electric field,i.e.,ρ_(s) and σ,respectively,implying that the physics determining T_(c) is governed by the intrinsic electromagnetic fields of the system.

Design of high-temperature superconductors at moderate pressures by alloying AlH3 or GaH3

Since the discovery of hydride superconductors,a significant challenge has been to reduce the pressure required for their stabilization.In this context,we propose that alloying could be an effective strategy to achieve this.We focus on a series of alloyed hydrides with the AMH_(6)composition,which can be made via alloying A15 AH_(3)(A=Al or Ga)with M(M=a group IIIB or IVB metal),and study their behavior under pressure.Seven of them are predicted to maintain the A15-type structure,similar to AH_(3)under pressure,providing a platform for studying the effects of alloying on the stability and superconductivity of AH_(3).Among these,the A15-type phases of AlZrH_(6)and AlHfH_(6)are found to be thermodynamically stable in the pressure ranges of 40–150 and 30–181 GPa,respectively.Furthermore,they remain dynamically stable at even lower pressures,as low as 13 GPa for AlZrH_(6)and 6 GPa for AlHfH_(6).These pressures are significantly lower than that required for stabilizing A15 AlH3.Additionally,the introduction of Zr or Hf increases the electronic density of states at the Fermi level compared with AlH3.This enhancement leads to higher critical temperatures(Tc)of 75 and 76 K for AlZrH_(6)and AlHfH_(6)at 20 and 10 GPa,respectively.In the case of GaMH_(6)alloys,where M represents Sc,Ti,Zr,or Hf,these metals reinforce the stability of the A15-type structure and reduce the lowest thermodynamically stable pressure for GaH_(3) from 160 GPa to 116,95,80,and 85 GPa,respectively.Particularly noteworthy are the A15-type GaMH_(6)alloys,which remain dynamically stable at low pressures of 97,28,5,and 6 GPa,simultaneously exhibiting high Tc of 88,39,70,and 49 K at 100,35,10,and 10 GPa,respectively.Overall,these findings enrich the family of A15-type superconductors and provide insights for the future exploration of high-temperature hydride superconductors that can be stabilized at lower pressures.

Two-fold symmetry of the in-plane resistance in kagome superconductor Cs(V_(1-x)Ta_(x))_(3)Sb_(5) with enhanced superconductivity

The kagome superconductor CsV_(3)Sb_(5) has attracted widespread attention due to its rich correlated electron states including superconductivity, charge density wave(CDW), nematicity, and pair density wave. Notably, the modulation of the intertwined electronic orders by the chemical doping is significant to illuminate the cooperation/competition between multiple phases in kagome superconductors. In this study, we have synthesized a series of tantalum-substituted Cs(V_(1-x)Ta_(x))_(3)Sb_(5) by a modified self-flux method. Electrical transport measurements reveal that CDW is suppressed gradually and becomes undetectable as the doping content of x is over 0.07. Concurrently, the superconductivity is enhanced monotonically from T_(c) ~ 2.8 K at x = 0 to 5.2 K at x = 0.12. Intriguingly, in the absence of CDW, Cs(V_(1-x)Ta_(x))_(3)Sb_(5)(x = 0.12) crystals exhibit a pronounced two-fold symmetry of the in-plane angular-dependent magnetoresistance(AMR) in the superconducting state, indicating the anisotropic superconducting properties in the Cs(V_(1-x)Ta_(x))_(3)Sb_(5). Our findings demonstrate that Cs(V_(1-x)Ta_(x))_(3)Sb_(5) with the non-trivial band topology is an excellent platform to explore the superconductivity mechanism and intertwined electronic orders in quantum materials.

An Overview of the Multi-Band and the Generalized BCS Equations-Based Approaches to Deal with Hetero-Structured Superconductors

We trace the conceptual basis of the Multi-Band Approach (MBA) and recall the reasons for its wide following for composite superconductors (SCs). Attention is then drawn to a feature that MBA ignores: the possibility that electrons in such an SC may also be bound via simultaneous exchanges of quanta with more than one ion-species—a lacuna which is addressed by the Generalized BCS Equations (GBCSEs). Based on several papers, we give a concise account of how this approach: 1) despite employing a single band, meets the criteria satisfied by MBA because a) GBCSEs are derived from a temperature-incorporated Bethe-Salpeter Equation the kernel of which is taken to be a “superpropagator” for a composite SC-each ion-species of which is distinguished by its own Debye temperature and interaction parameter and b) the band overlapping the Fermi surface is allowed to be of variable width. GBCSEs so-obtained reduce to the usual equations for the Tc and Δ of an elemental SC in the limit superpropagator → 1-phonon propagator;2) accommodates moving Cooper pairs and thereby extends the scope of the original BCS theory which restricts the Hamiltonian at the outset to terms that correspond to pairs having zero centre-of-mass momentum. One can now derive an equation for the critical current density (j0) of a composite SC at T = 0 in terms of the Debye temperatures of its ions and their interaction parameters— parameters that also determine its Tc and Δs;3) transforms the problem of optimizing j0 of a composite SC, and hence its Tc, into a problem of chemical engineering;4) provides a common canopy for most composite SCs, including those that are usually regarded as outside the purview of the BCS theory and have therefore been called “exceptional”, e.g., the heavy-fermion SCs;5) incorporates s±-wave superconductivity as an in-built feature and can therefore deal with the iron-based SCs, and 6) leads to presumably verifiable predictions for the values of some relevant parameters, e.g., the effective mass of electrons, for the SCs for which it has been employed.

Effect of the mixing of s-wave and chiral p-wave pairings on electrical shot noise properties of normal metal/superconductor tunnel junctions

We study theoretically the electrical shot noise properties of tunnel junctions between a normal metal and a superconductor with the mixture of singlet s-wave and chiral triplet p-wave pairing due to broken inversion symmetry. We investigate how the shot noise properties vary as the relative amplitude between the two parity components in the pairing potential is changed. It is demonstrated that some characteristics of the electrical shot noise properties of such tunnel junctions may depend sensitively on the relative amplitude between the two parity components in the pairing potential, and some significant changes may occur in the electrical shot noise properties when the relative amplitude between the two parity components is varied from the singlet s-wave pairing dominated regime to the chiral triplet p-wave pairing dominated regime. In the chiral triplet p-wave pairing dominated regime, the ratio of noise power to electric current is close to 2e both in the in-gap and in the out-gap region. In the singlet s-wave pairing dominated regime, the value of this ratio is close to 4e in the inner gap region but may reduce to about 2e in the outer gap region as the relative amplitude of the chiral triplet pairing component is increased. The variations of the differential shot noise with the bias voltage also exhibit some significantly different features in different regimes. Such different features can serve as useful diagnostic tools for the determination of the relative magnitude of the two parity components in the pairing potential.

High Harmonic Spectroscopy Retrieves Electronic Structure of High-pressure Superconductors

High pressure has revealed surprising physics and creates novel states in condensed matter.Exciting examples include near-roomtemperature superconductivity(T_(c)>200 K)in highlypressured hydrides such as H_(3)S and LaH_(10).

Thermoelectric-transport in metal/graphene/metal hetero-structure

We investigate the thermoelectric-transport properties of metal/graphene/metal hetero-structure. We use a single band tight-binding model to prcsent the two-dimensional electronic band structure of graphene. Using the LandauerButticker formula and taking the coupling between graphene and the two electrodes into account, we can calculate the thermoelectric potential and current versus temperature. It is found that in spite of metal electrodes, the carrier type of graphene determines the electron motion direction driven by the difference in temperature between the two electrodes, while for n type graphene, the electrons move along the thermal gradient, and for p type graphene, the electrons move against the thermal gradient.

Customizing topological phases in the twisted bilayer superconductors with even-parity pairings

We investigate the topological properties of twisted bilayer superconductors with different even-parity pairings in each layer.In the presence of spin-orbit coupling,the Hamiltonian is mapped into an effective odd-parity superconductor.Based on this,we deduce the topological properties by examining the relative configuration between Fermi surface and Dirac pairing node.We show that mixed Rashba and Dresselhaus spin-orbit coupling and anisotropic hopping terms,which break the C_(4)symmetry of the Fermi surface,can induce first-order topological superconductors with non-zero bulk Chern number.This provides a versatile way to control the topological phases of bilayer superconductors by adjusting the twisted angle and chemical potential.We demonstrate our results using a typical twisted angle of 53.13°,at which the translation symmetry is restored and the Chern number and edge state are calculated using the Moir′e momentum.

Gate-Tunable Negative Differential Conductance in Hybrid Semiconductor–Superconductor Devices

Negative differential conductance(NDC)serves as a crucial characteristic that reveals various underlying physics and transport process in hybrid superconducting devices.We report the observation of gate-tunable NDC outside the superconducting energy gap on two types of hybrid semiconductor–superconductor devices,i.e.,normal metal–superconducting nanowire–normal metal and normal metal–superconducting nanowire–superconductor devices.Specifically,we study the dependence of the NDCs on back-gate voltage and magnetic field.When the back-gate voltage decreases,these NDCs weaken and evolve into positive differential conductance dips;and meanwhile they move away from the superconducting gap towards high bias voltage,and disappear eventually.In addition,with the increase of magnetic field,the NDCs/dips follow the evolution of the superconducting gap,and disappear when the gap closes.We interpret these observations and reach a good agreement by combining the Blonder–Tinkham–Klapwijk(BTK)model and the critical supercurrent effect in the nanowire,which we call the BTK-supercurrent model.Our results provide an in-depth understanding of the tunneling transport in hybrid semiconductor–superconductor devices.

Abnormal magnetoresistance effect in the Nb/Si superconductor–semiconductor heterojunction

Ultrathin superconducting Nb films of about 8 nm thick have been deposited on heavily doped Si substrates through DC magnetron sputtering and then the high-quality Nb/Si superconductor–semiconductor heterojunctions have been fabricated by electron beam lithography and reactive ion etching.An abnormal magnetoresistance effect,which manifests itself as a zero field resistance peak under a magnetic field applied perpendicular to the interface,has been distinctly observed when the Nb film is in the superconductiing state.By considering the heterojunction interface being equivalent to the structure of superconductor–barrier layer–superconductor configuration,we could generally understand this unusual effect based on the Andreev reflection mechanism.Our results can be of help for the future development on compatibility and scalability of the silicon-based nanoscale superconducting devices for integrated circuits and superconducting quantum electronics.

Anisotropy of Electronic Spin Texture in the High-Temperature Cuprate Superconductor Bi_(2)Sr_(2)CaCu_(2)O_(8+δ)

Seeking new order parameters and the related broken symmetry and studying their relationship with phase transition have been important topics in condensed matter physics.Here,by using spin-and angle-resolved photoemission spectroscopy,we confirm the helical spin texture caused by spin-layer locking in the nodal region in the cuprate superconductor Bi_(2)Sr_(2)CaCu_(2)O_(8+δ)and discover the anisotropy of spin polarizations at nodes alongΓ–X andΓ–Y directions.The breaking of C_(4)rotational symmetry in electronic spin texture may give deeper insights into understanding the ground state of cuprate superconductors.

Majorana Corner Modes and Flat-Band Majorana Edge Modes in Superconductor/Topological-Insulator/Superconductor Junctions

Recently,superconductors with higher-order topology have stimulated extensive attention and research interest.Higher-order topological superconductors exhibit unconventional bulk-boundary correspondence,thus allow exotic lower-dimensional boundary modes,such as Majorana corner and hinge modes.However,higher-order topological superconductivity has yet to be found in naturally occurring materials.We investigate higher-order topology in a two-dimensional Josephson junction comprised of two s-wave superconductors separated by a topological insulator thin film.We find that zero-energy Majorana corner modes,a boundary fingerprint of higherorder topological superconductivity,can be achieved by applying magnetic field.When an in-plane Zeeman field is applied to the system,two corner modes appear in the superconducting junction.Furthermore,we also discover a two-dimensional nodal superconducting phase which supports flat-band Majorana edge modes connecting the bulk nodes.Importantly,we demonstrate that zero-energy Majorana corner modes are stable when increasing the thickness of topological insulator thin film.

Growth and Characterization of a New Superconductor GaBa2Ca3Cu4O11+δ

We successfully grow a new superconductor GaBa2Ca3Cu4O11+δ(Ga-1234) with a transition temperature of 113 K, using the Walker-type high-pressure synthesis apparatus. X-ray diffraction measurements on the powderized samples show a mixture of the Ga-1234 phase and the Ca0.85CuO2phase, and the former is dominant. Under the scanning electron microscope, plate-like crystals of the Ga-based 1234 phase with shiny surfaces can be seen.The obtained local chemical compositions revealed by energy dispersion x-ray spectroscopy are very close to the stoichiometric values. On some sub-millimeter crystal-like samples of the 1234 phase, we obtain a full Meissner shielding volume. From the temperature-dependent magnetizations, we determine the irreversibility fields and find that the system exhibits a highly anisotropic behavior.

Hole density dependent magnetic structure and anisotropy in Fe-pnictide superconductor

The competition between different magnetic structures in hole-doped Fe-pnicitides is explored based on an extended five-orbital Hubbard model including long-range Coulomb interactions.Our results show that the stabilized magnetic structure evolves with increasing hole doping level.Namely,the stripe antiferromagnetic phase dominates at zero doping,while magnetic structures with more antiferromagnetic linking numbers such as the staggered tetramer,staggered trimer,and staggered dimer phases become energetically favorable as the hole density increases.At a certain doping level,energy degeneracy of different magnetic structures appears,indicating strong magnetic frustration and magnetic fluctuations in the system.We suggest that the magnetic competition induced by the hole doping may explain the fast decrease of the Neel temperature TNand the moderately suppressed magnetic moment in the hole doped Fe-pnicitides.Moreover,our results show a sign reversal of the kinetic energy anisotropy as the magnetic ground state evolves,which may be the mechanism behind the puzzling sign reversal of the in-plane resistivity anisotropy in hole-doped Fe-pnicitides.

Ultralow-temperature heat transport study of noncentrosymmetric superconductor CaPtAs

The noncentrosymmetric superconductor CaPtAs with time-reversal symmetry breaking in its superconducting state was previously proposed to host nodal superconductivity.Here,by employing ultralow-temperature thermal conductivity measurement on CaPtAs single crystal,we study its superconducting gap structure.A negligible residual linear term of thermal conductivity(κ_(0)/T)in zero magnetic field and the field dependence ofκ_(0)/T indicate that CaPtAs has multiple superconducting gaps with a dominant s-wave component.This is consistent with recent nuclear quadrupole resonance measurements on CaPtAs.Our work puts a strong constraint on the theories to describe the superconducting pairing symmetry of CaPtAs.

Photoinduced valley-dependent equal-spin Andreev reflection in Ising superconductor junction

The Ising spin–orbit coupling could give rise to the spin-triplet Cooper pairs and equal-spin Andreev reflection(AR)in Ising superconductors.Here we theoretically study the valley-dependent equal-spin AR in a ferromagnet/Ising superconductor junction with a circularly polarized light applied to the ferromagnet.Because of the spin-triplet Cooper pairs and the optical irradiation,eight kinds of AR processes appear in the junction,including equal-spin AR and normal AR,the strengths and properties of which strongly depend on the valley degree of freedom.The AR probabilities for the incident electron from the two valleys exhibit certain symmetry with respect to the magnetization angle and the effective energy of light.The equal-spin AR and normal AR present different features and resonant behaviors near the superconducting gap edges.Due to equal-spin-triplet Cooper pairs,not only charge supercurrent but also spin supercurrent can transport in the Ising superconductors.The differential spin conductance for electron injecting from the two valleys can be controlled by the circularly polarized light.

Effect of thickness on magnetic properties of single domain GdBCO bulk superconductors

To study the influence of thickness on the magnetic properties of ReBCO(Re = Y, Gd, Sm, Nd, etc.) bulk superconductors, a single domain gadolinium barium copper oxide(GdBCO) bulk superconductor fabricated by the Re + 011 top seeded infiltration growth(Re + 011 TSIG) method was continuously sliced along the bottom to obtain samples of different thickness. The levitation force and attractive force of these samples were tested at 77 K in the zero-field-cooled(ZFC)state. It is found that as the sample thickness decreases, the levitation force decreases gradually whereas the attractive force increases. This is related to the varied ability to resist the penetration of magnetic field occasioned by varying sample thickness, which are deeply revealed by combining with the characteristics of the non-ideal type-II superconductor. Further,the levitation force exhibits a trend of slow initial change followed by rapid change, which may be attributed to the growth of the sample. Measurement of the trapped field shows that a similar distribution of trapped field at the top and bottom surfaces can be achieved by removing some materials from the bottom of the bulk. These results provide a reference for meeting the actual requirements of ReBCO bulks of different thicknesses and greatly contribute to practical designs and applications.

First-principles study of moderate phonon-mediated pairing in high-pressure monoclinic phase of BiS_(2)-based superconductors

Isotope effect on superconductive transition temperature(T_c)is an essential indicator to examine whether the mechanism of superconductors is conventional.Unconventional isotope effect of BiS_(2)-based superconductors has been previously reported in ambient-pressure tetragonal phase.However,to comprehensively ascertain the nature of superconductivity,the investigation of BiS_(2)-based system in high-pressure structure is highly desirable.In this work,we carried out the first-principles calculations of phonon spectra and superconductivity in high-pressure monoclinic phase of LaO_(0.5)F_(0.5)BiS_(2)with ^(32)S and ^(34)S,and observed that the corresponding isotope coefficient is 0.13≤α≤0.20.This value is much greater than that of BiS_(2)-based superconductors in ambient-pressure phase,but slightly smaller than that of conventional MgB_2.Taking into account the calculated T_(c) lower than experimental results,we finally conclude that the moderate phonon-mediated pairing plays a significant role in forming superconductivity of BiS_(2)-based system in high-pressure phase,moreover,the cooperative multiple paring interactions should also be considered.