Combinatorial synthesis and high-throughput characterization of copper-oxide superconductors

Fast synthesis and screening of materials are vital to the advance of materials science and are an essential component of the Materials Genome Initiative. Here we use copper-oxide superconductors as an example to demonstrate the power of integrating combinatorial molecular beam epitaxy synthesis with high-throughput electric transport measurements. Leveraging this method, we have generated a phase diagram with more than 800 compositions in order to unravel the doping dependence of interface superconductivity. In another application of the same method, we have studied the superconductorto-insulator quantum phase transition with unprecedented accuracy in tuning the chemical doping level.

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.

Prediction of novel layered indium halide superconductors

We design two new layered indium halide compounds LaOInF_(2)and LaOInCl_(2)by means of first-principles calculations and evolutionary crystal structure prediction.We find both compounds crystallize in a tetragonal structure with P4/nmm space group and have indirect band gaps of 2.58 eV and 3.21 eV,respectively.By substituting O with F,both of them become metallic and superconducting at low temperature.The F-doping leads to strong electron-phonon coupling in the low-energy acoustic phonon modes which is mainly responsible for the induced superconductivity.The total electron-phonon coupling strength are 1.86 and 1.48,while the superconducting transition temperature(T_(c))are about 7.2 K and 6.5 K with 10%and 5%F doping for LaOInF_(2)and LaOInCl_(2),respectively.

Topological superconductors with spin-triplet pairings and Majorana Fermi arcs

We construct a three-dimensional topological superconductor Bogoliubov–de Gennes(BdG)Hamiltonian with the normal state being a three-dimensional topological insulator.By introducing inter-orbital spin-triplet pairings term△3,there are topological Majorana nodes in the bulk and they are connected by Majorana Fermi arcs on the surface,similar to the case of Weyl semimetal.Furthermore,by adding an inversion-breaking term to the normal state,momentum-independent pairing terms with different parities can coexist in the Bd G Hamiltonian,which creates more Majorana modes similar to Andreev bound states and a richer phase diagram.

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).

Electronic Structure Investigation of 12442 Iron-Based Superconductors Based on Block-Layer Model

Superconducting transition temperature(Tc),as a crucial parameter,exploring its relationship with various macroscopic and microscopic factors helps to understand the mechanism of high-temperature superconductivity from multiple perspectives,aiding in a multidimensional comprehension of high-temperature superconductivity mechanisms.Drawing inspiration from the block-layer structure models of cuprate superconductors,we computationally investigated the interlayer interaction energies in the 12442-type iron-based superconducting materials AkCa_(2)Fe_(4)As_(4)F_(2)(Ak=K,Rb,Cs)systems based on the block-layer model and explored their relationship with Tc.We observed that an increase in interlayer combinative energy leads to a decrease in Tc,while conversely,a decrease in interlayer combination energy results in an increase in Tc.Further,we found that the contribution of the Fe 3d band structure,especially the 3dz2 orbital,to charge transfer is significant.

Crystal chemistry and structural design of iron-based superconductors

The second class of high-temperature superconductors （HTSCs）, iron-based pnictides and chalcogenides, necessarily contain Fe2X2 （＂X＂ refers to a pnictogen or a chalcogen element） layers, just like the first class of HTSCs which possess the essential CuO2 sheets. So far, dozens of iron-based HTSCs, classified into nine groups, have been discovered. In this article, the crystal-chemistry aspects of the known iron-based superconductors are reviewed and summarized by employing ＂hard and soft acids and bases （HSAB）＂ concept. Based on these understandings, we propose an alternative route to exploring new iron-based superconductors via rational structural design.

High-magnetic-field induced charge order in high-T_c cuprate superconductors

In the last few years, charge order and its entanglement with superconductivity are under hot debate in high-Tc community due to the new progress on charge order in high-Tc cuprate superconductors YBa2Cu3O6+x. Here, we will briefly introduce the experimental status of this field and mainly focus on the experimental progress of high-field nuclear magnetic resonance(NMR) study on charge order in YBa2Cu3O6+x. The pioneering high-field NMR work in YBa2Cu3O6+x sets a new stage for studying charge order which has become a ubiquitous phenomenon in high-Tc cuprate superconductors.

Angle-resolved photoemission spectroscopy study on iron-based superconductors

Angle-resolved photoemission spectroscopy （ARPES） has played an important role in determining the band structure and the superconducting gap structure of iron-based superconductors. In this paper, from the ARPES perspective, we briefly review the main results from our group in recent years on the iron-based superconductors and their parent compounds, and depict our current understanding on the antiferromagnetism and superconductivity in these materials.

Pressure-induced hydride superconductors above 200 K

Although it was proposedmany years ago that compressed hydrogen should be a high-temperature superconductor,the goal of room-temperature superconductivity has so far remained out of reach.However,the successful synthesis of the theoretically predicted hydrides H3S and LaH10 with high superconducting transition temperatures TC provides clear guidance for achieving this goal.The existence of these superconducting hydrides also confirms the utility of theoretical predictions in finding high-TC superconductors.To date,numerous hydrideshave been studied theoretically or experimentally,especially binary hydrides.Interestingly,some of them exhibit superconductivity above 200 K.To gain insight into these high-TC hydrides(>200 K)and facilitate further research,we summarize their crystal structures,bonding features,and electronic properties,as well as their superconductingmechanism.Based on hydrogen structuralmotifs,covalentH3Swith isolated hydrogen and several clathrate superhydrides(LaH10,YH9,and CaH6)are highlighted.Other predicted hydrides with various H-cages and two-dimensional H motifs are also discussed.Finally,we present a systematic discussion of the common features,current problems,and future challenges of these high-TC hydrides.

Theory-orientated discovery of high-temperature superconductors in superhydrides stabilized under high pressure

A dream long held by physicists has been to raise the critical temperature(Tc)—the temperature below which the material exhibits no electrical resistance—of a superconductor to room temperature.The most recent excitement in that regard has centered on rare-earth superhydrides,of which LaH10 at 190 GPa has a remarkably high Tc of 260 K.

The role of CALYPSO in the discovery of high-T_c hydrogen-rich superconductors

Hydrogen-rich compounds are promising candidates for high-Tc or even room-temperature superconductors. The search for high-Tc hydrides poses a major experimental challenge because there are many known hydrides and even more unknown hydrides with unusual stoichiometries under high pressure. The combination of crystal structure prediction and first-principles calculations has played an important role in the search for high-Tc hydrides, especially in guiding experimental synthesis. Crystal structure AnaLYsis by Particle Swarm Optimization(CALYPSO) is one of the most efficient methods for predicting stable or metastable structures from the chemical composition alone. This review summarizes the superconducting hydrides predicted using CALYPSO. We focus on two breakthroughs toward room-temperature superconductors initiated by CALYPSO: the prediction of high-Tc superconductivity in compressed hydrogen sulfide and lanthanum hydrides, both of which have been confirmed experimentally and have set new record Tc values. We also address the challenges and outlook in this field.

Electrochemical synthesis of alkali-intercalated iron selenide superconductors

Electrochemical method has been used to insert K/Na into FeSe lattice to prepare alkali-intercalated iron selenides at room temperature. Magnetization measurement reveals that KxFe2Se2 and NaxFe2Se2 are superconductive at 31 K and 46 K, respectively. This is the first successful report of obtaining metal-intercalated FeSe-based high-temperature superconductors using electrochemical method. It provides an effective route to synthesize metal-intercalated layered compounds for new superconductor exploration.

Electronic structure of transition metal dichalcogenides PdTe_2 and Cu_(0.05)PdTe_2 superconductors obtained by angle-resolved photoemission spectroscopy

The layered transition metal chalcogenides have been a fertile land in solid state physics for many decades. Various MX2-type transition metal dichalcogenides, such as WTe2, IrTe2, and MoS2, have triggered great attention recently, either for the discovery of novel phenomena or some extreme or exotic physical properties, or for their potential applications. PdTe2 is a superconductor in the class of transition metal dichalcogenides, and superconductivity is enhanced in its Cu- intercalated form, Cuo.05PdTe2. It is important to study the electronic structures of PdTe2 and its intercalated form in order to explore for new phenomena and physical properties and understand the related superconductivity enhancement mecha- nism. Here we report systematic high resolution angle-resolved photoemission （ARPES） studies on PdTe2 and Cuo.05PdTe2 single crystals, combined with the band structure calculations. We present in detail for the first time the complex multi-band Fermi surface topology and densely-arranged band structure of these compounds. By carefully examining the electronic structures of the two systems, we find that Cu-intercalation in PdTe2 results in electron-doping, which causes the band structure to shift downwards by nearly 16 meV in Cuo.05PdTe2. Our results lay a foundation for further exploration and investigation on PdTe2 and related superconductors.

Microstructure and structural phase transitions in iron-based superconductors

Crystal structures and microstructural features, such as structural phase transitions, defect structures, and chemical and structural inhomogeneities, are known to have profound effects on the physical properties of superconducting materials. Recently, many studies on the structural properties of Fe-based high-Tc superconductors have been published. This review article will mainly focus on the typical microstructural features in samples that have been well characterized by physical measurements. （i） Certain common structural features are discussed, in particular, the crystal structural features for different superconducting families, the local structural distortions in the Fe2Pn2 （Pn = P, As, Sb） or FeeCh2 （Ch = S, Se, Te） blocks, and the structural transformations in the 122 system. （ii） In FeTe（Se） （11 family）, the superconductivity, chemical and structural inhomogeneities are investigated and discussed in correlation with superconductivity. （iii） In the Ko.sFe1.6＋xSe2 system, we focus on the typical compounds with emphasis on the Fe-vacancy order and phase separations. The microstructural features in other superconducting materials are also briefly discussed.

Review of nuclear magnetic resonance studies on iron-based superconductors

The newly discovered iron-based superconductors have triggered renewed enormous research interest in the condensed matter physics community. Nuclear magnetic resonance （NMR） is a low-energy local probe for studying strongly correlated electrons, and particularly important for high-Tc superconductors. In this paper, we review NMR studies on the structural transition, antiferromagnetic order, spin fluctuations, and superconducting properties of several iron-based high-Tc superconductors, including LaFeAsOl_xFx, LaFeAsOl_x, BaFe2As2, Bal_xKxFe2As2, Cao.23Nao.67Fe2As2, BaFe2（Asl_xPx）2, Ba（Fel_xRux）2As2, Ba（Fel_xCox）2As2, Lil＋xFeAs, LiFel_xCoxAs, NaFeAs, NaFel_xCoxAs, KyFe2_xSe2, and （T1,Rb）yFe2_xSe2.

Fabrication and Properties of (Y,Gd)BCO Superconductors

The microstructures and superconducting properties of melt textured(Y_(1-x)Gd_x)BCO bulk samples were studied. It was found that the peritectic decomposition temperature(T_m)of(Y_(1-x)Gd_x)BCO samples increases with increasing x. Large single domain growth in air is readily obtained in all the composites. The results of X-ray distribution maps of x=0.4 composite indicate that the RE123 matrix is homogeneous and Y and Gd elements in the RE site forms a perfect solid solution. The onset T_c values exceeding 91 K with relatively broad transitions are obtained for almost all the samples. Magnetization measurements show no marked indication for the formation of a peak effect in the J_c-B curves, and the highest J_c measured is 3.08×10~4 A·cm^(-2) for x=0.4 sample at 77 K and self-field. The results clearly indicate that Y dominates the superconducting properties of x=0.2 and (0.4) composites.

Distinction between critical current effects and intrinsic anomalies in the point-contact Andreev reflection spectra of unconventional superconductors

In this work,we discuss the origin of several anomalies present in the point-contact Andreev reflection spectra of（Li1-xFex）OHFeSe,LiTi2O4,and La2-xCexCuO4.While these features are similar to those stemming from intrinsic superconducting properties,such as Andreev reflection,electron-boson coupling,multigap superconductivity,d-wave and p-wave pairing symmetry,they cannot be accounted for by the modified Blonder–Tinkham–Klapwijk（BTK） model,but require to consider critical current effects arising from the junction geometry.Our results point to the importance of tracking the evolution of the dips and peaks in the differential conductance as a function of the bias voltage,in order to correctly deduce the properties of the superconducting state.

Explanation of Pressure Effect for High Temperature Superconductors Using Pressure Dependent Schrodinger Equation and String Theory

A pressure dependent Schrodinger equation is used to find the conditions that lead to superconductivity. When no pressure is exerted, the superconductor resistance vanishes beyond a critical temperature related to the repulsive force potential of the electron gass, where one assuming the electron total energy to be thermal, where applying mechanical pressure destroys Sc when it exceeds a certain critical value. However when the electron total energy is an assumed to be that of the free electron model and that the pressure is thermal and mechanical, the situation is different. The quantum expression for resistance shows that the increase of mechanical pressure increases the critical temperature. Such phenomenon is observed in high temperature cupper group.