high-Tc Superconductors Research Articles

Designing multicomponent hydrides with potential high Tc superconductivity

While hydrogen-rich materials have been demonstrated to exhibit high Tc superconductivity at high pressures, there is an ongoing search for ternary, quaternary, and more chemically complex hydrides that achieve such high critical temperatures at much lower pressures. First-principles searches are impeded by the computational complexity of solving the Eliashberg equations for large, complex crystal structures. Here, we adopt a simplified approach using electronic indicators previously established to be correlated with superconductivity in hydrides. This is used to study complex hydride structures, which are predicted to exhibit promisingly high critical temperatures for superconductivity. In particular, we propose three classes of hydrides inspired by the Fm[Formula: see text]m RH[Formula: see text] structures that exhibit strong hydrogen network connectivity, as defined through the electron localization function. The first class [RH[Formula: see text]X[Formula: see text]Y] is based on a Pm[Formula: see text]m structure showing moderately high Tc, where the Tc estimate from electronic properties is compared with direct Eliashberg calculations and found to be surprisingly accurate. The second class of structures [(RH[Formula: see text])[Formula: see text]X[Formula: see text]YZ] improves on this with promisingly high density of states with dominant hydrogen character at the Fermi energy, typically enhancing Tc. The third class [(R[Formula: see text]H[Formula: see text])(R[Formula: see text]H[Formula: see text])X[Formula: see text]YZ] improves the strong hydrogen network connectivity by introducing anisotropy in the hydrogen network through a specific doping pattern. These design principles and associated model structures provide flexibility to optimize both Tc and the structural stability of complex hydrides.

Enhancing Superconductor Critical Temperature Prediction: A Novel Machine Learning Approach Integrating Dopant Recognition.

Doping plays a crucial role in determining the critical temperature (Tc) of superconductors, yet accurately predicting its effects remains a significant challenge. Here, we introduce a novel doping descriptor that captures the complex influence of dopants on superconductivity. By integrating the doping descriptor with elemental and physical features within a Mixture of Experts (MoE) model, we achieve a remarkable R2 of 0.962 for Tc prediction, surpassing all published prediction models. Our approach successfully identifies optimal doping levels in the Bi2-xPbxSr2Ca2-yCuyOz system, with predictions closely aligning with experimental results. Leveraging this model, we screen compounds from the Inorganic Crystal Structure Database and employ a generative approach to explore new doped superconductors. This process reveals 40 promising candidates for high Tc superconductivity among existing and hypothetical doped materials. By explicitly accounting for doping effects, our method offers a powerful tool for guiding the experimental discovery of new superconductors, potentially accelerating progress in high-temperature superconductivity research and opening new avenues for material design.

Chemically tuning stability and superconductivity of Pd–H compounds: A routine to high temperature superconductivity under modest pressures

Motivated by searching room-temperature superconductors that could be realized near ambient conditions, palladium hydrides were chosen as the research subject considering that they can stably exist under ambient conditions, and Li as an electron donor for its outstanding performance in chemically tuning stability. A novel cubic phase structure of Li2PdH6 with a remarkably high estimated Tc of ∼165 K at 90 GPa was found using particle swarm optimization algorithm calculations. The superconducting behavior persists down to 10 GPa with a high Tc of 106.382 K. Even though the parent binary Pd–H system is not a good superconductor, the introduction of extra electrons breaks up the H2 molecules, inducing the increase of atomic hydrogen compared with parent hydride, which is necessary for outstanding superconducting behavior. The existence of relatively soft phonons associated with the H atoms in phonon dispersion curves is responsible for its high-Tc. Our results indicated that the doping of Li to binary hydrides, especially to binary hydrides with low-Tc that exist under ambient pressure, can produce robust phonon-mediated superconductivity. This may be a strategy to design and optimize room-temperature superconductors that can be synthesized under modest pressure. The findings may pave the way for realizing new high-Tc superconductors in experiments under lower pressure than recently documented superconducting hydrides.

Possible Superconductivity for Layered Metal Boride Carbide Compounds MB2C2 (M = Alkali, Alkaline-Earth, or Rare-Earth Metals).

The possible emergence of superconductivity in layered metal boride carbide compounds MB2C2 (M = Sc, Y, Be, Ca) was investigated using density functional theory calculations upon the topology of a boron-carbon network and the nature of the metal. ScB2C2 and YB2C2 show metallic and superconductive properties with low critical temperatures (Tcs). The semiconducting BeB2C2 compound may show superconductivity upon carrier doping with a high Tc of 47.8 K by hole doping─comparable to the structurally related MgB2 superconductor─but with a low Tc by electron doping. In contrast, the semiconducting CaB2C2 compound is predicted to be a superconductor by hole and electron doping but with low Tcs. These differences arise from the spatial distribution of electrons at the Fermi level. For compounds with low Tcs, electrons at the Fermi level are localized primarily on B and C π states perpendicular to the BC layers, experiencing minimal influence from atomic oscillations and resulting in weak electron-phonon interactions. Conversely, for a high Tc, electrons are found in σ-bonding states, leading to strong electron-phonon interactions. Electrons at the Fermi level in boron-carbon σ-bonding states seem to be a prerequisite to expect high Tc superconductivity in this kind of compound.

Hydride units filled boron–carbon clathrate: a pathway for high-temperature superconductivity at ambient pressure

Recent advances in the search for room-temperature superconductors have focused on high-temperature superconductivity in compressed hydrides, though sustaining this at ambient pressure remains challenging. Concurrently, sp3-bonded frameworks comprising lightweight elements offer another avenue for ambient-pressure superconductors. However, their critical temperatures (Tc) still fall short of those in hydrides. Here we propose a design strategy for achieving high-temperature superconductivity at ambient pressure by integrating hydride units into B–C clathrate structures. This approach exploits the beneficial properties of hydrogen, the lightest element, to enhance superconductivity beyond that of the parent compounds. Our computational predictions indicate that doping SrB3C3 with ammonium (NH4) produces SrNH4B6C6, with an estimated Tc of 85 K at ambient pressure—over twice that of its precursor (31 K). Further substitutions yield a family of MNH4B6C6 superconductors, with PbNH4B6C6 predicted to reach a Tc of 115 K. These findings offer a promising route to high-Tc superconductors at ambient pressure.

On the mass of the charge carrier in LSCO cuprate: Bose–Einstein condensation of preformed pairs point of view

In this paper, the dependence of the charge carrier mass in the LSCO cuprate on the doping level (x) has been theoretically studied. Our theoretical consideration is based on the bipolaron theory of high-Tc superconductivity, which implies superfluidity of a gas (liquid) of bipolarons (pre-formed pairs). The theoretical explanation of the dependency is achieved by associating the superconducting critical temperature of the LSCO cuprate, Tc, with the temperature of Bose–Einstein condensation of the ideal gas of the intersite bipolarons, TBEC, and calculating the value of (bi)polaron mass at different doping levels. Meanwhile, the anisotropy of the LSCO cuprate crystal lattice is also taken into account to obtain precise results. Our results practically reproduce the known experimental dependencies of the charge carrier mass on the doping level. Besides, they clearly demonstrate the potential of using the pre-formed pair concept in studying the high-Tc superconductivity of the LSCO cuprate.

Collapse of metallicity and high-Tc superconductivity in the high-pressure phase of FeSe0.89S0.11

We investigate the high-pressure phase of the iron-based superconductor FeSe0.89S0.11 using transport and tunnel diode oscillator studies using diamond anvil cells. We construct detailed pressure-temperature phase diagrams that indicate that the superconducting critical temperature is strongly enhanced by more than a factor of four towards 40 K above 4 GPa. The resistivity data reveal signatures of a fan-like structure of non-Fermi liquid behaviour which could indicate the existence of a putative quantum critical point buried underneath the superconducting dome around 4.3 GPa. With further increasing the pressure, the zero-field electrical resistivity develops a non-metallic temperature dependence and the superconducting transition broadens significantly. Eventually, the system fails to reach a fully zero-resistance state, and the finite resistance at low temperatures becomes strongly current-dependent. Our results suggest that the high-pressure, high-Tc phase of iron chalcogenides is very fragile and sensitive to uniaxial effects of the pressure medium, cell design and sample thickness. This high-pressure region could be understood assuming a real-space phase separation caused by nearly concomitant electronic and structural instabilities.

Superconducting transition of GdBa2Cu3O7-x/La0.7A0.3MnO3 (A=Sr and Ca) bilayers governed by tunable interlayer structural coupling

Bilayers composed of high-Tc cuprate superconductors (HTS) with manganites have garnered significant attention due to the complex interaction between two layers, leading to competition among various ordering phenomena. When HTS and manganties are interfaced, new functionalities can emerge that are absent in the individual components. Notably, epitaxial strain can alter crystal structures and electronic states, significantly impacting superconductivity in HTS/manganite heterostructures. In this study, we analyze the superconducting and ferromagnetic behaviors of GdBa2Cu3O7-x(GdBCO)/La0.7A0.3MnO3(LAMO, where A=Sr and Ca) bilayers, maintain a constant GdBCO thickness of 500 nm while varying the LAMO thickness from 25 to 100 nm. We focus on the local structural correlations between the two layers. Temperature-dependent EXAFS spectra were systematically measured at the Cu and Mn K-edges to investigate the local atomic structures of both layers across the superconducting transition temperature (Tc). Our spectroscopic measurements reveal distinct conformations of the MnO6 octahedra near Tc, which are absent in single-layer LSMO, indicating structural coupling between the layers. Additionally, our magnetization studies show a strong relationship between the structural coupling, magnetic anisotropy (MA), and the superconducting transition of the GdBCO/LAMO bilayers. The additional distortion of the MnO6 octahedra in the GdBCO/LAMO bilayer, likely stemming from structural coupling, may account for the changes in the superconducting transition associated with magnetic anisotropy. This modification of structural coupling can be controlled by adjusting the LAMO thickness, yet it remains highly dependent on the bond geometry of LAMO. The Mn-O bond in LCMO is stiffer than in LSMO, resulting in a smaller change in structural coupling with varying thickness in LCMO compared to LSMO. The disparity in structural coupling directly impacts the magnetic properties of the LAMO layer and subsequently influences the superconducting property ΔTc. Our findings highlight the significance of structural coupling as a critical factor affecting the superconductivity of GdBCO/LAMO bilayers. Furthermore, this study provide foundational insight for designing various applications, such as magnetic sensors and spintronic devices, by enhancing our understanding of local dynamics at the interface between ferromagnets and superconductors.

Pressure-induced structural transition and superconductivity in hard compound IrB4

The recent discovery of MoB2 with a superconducting transition temperature (Tc) of up to 32 K at 100 GPa provides new insights into the metallization and subsequently high-Tc superconductivity of diborides, highlighting the potential of transition metals in these compounds. We herein re-evaluated the structure, mechanical, and superconducting properties of IrB4 under pressure up to 300 GPa using first-principles. Our calculations reveal that a new P21/c phase exhibiting a hardness of 15.75 GPa surpasses the stability of the C2/m structure identified through the particle swarm optimization at ambient pressure. Upon compressing, the P21/c phase transforms into an MgB2-type structure with a space group of P63/mmc at 62.5 GPa and then into the orthorhombic Cmca phase above 109 GPa. Unlike semiconductor behavior of the atmospheric pressure phase, the two high-pressure structures are metallic and superconducting, with Tc values of 29.90 for P63/mmc at 62.5 GPa and 13.45 K for Cmca at 125 GPa. Analysis of the electronic structure and electron–phonon coupling (EPC) reveals that the high Tc, similar to MgB2-type MoB2, stems from the Van Hove Singularities (VHS) near the Fermi level donated by transition metal Ir. The effect further enhances the EPC based on the boron contribution. More interestingly, pressure has little impacts on the position of the VHS. These findings provide a new platform for designing advanced high-Tc superconductors.

Three-gap superconductivity with Tc above 80 K in hydrogenated 2D monolayer LiBC

Although the metallization of semiconductor bulk LiBC has been experimentally achieved, various flaws, including the strong lattice distortion, the uncontrollability of phase transition under pressure, usually appear. In this work, based on the first-principles calculations, we propose a new way of hydrogenation to realize metallization. Using the fully anisotropic Migdal-Eliashberg theory, we investigate the superconducting behaviors in the stable monolayers LiBCH and LiCBH, in which C and B atoms are hydrogenated, respectively. Our findings indicate that the monolayers possess the high Tc of 82.0 and 82.5 K, respectively, along with the interesting three-gap superconducting natures. The Fermi sheets showing the obvious three-region distribution characteristics and the abnormally strong electron-phonon coupling are responsible for the high-Tc three-gap superconductivity. Furthermore, the Tc can be dramatically boosted up to 120.0 K under 3.5% tensile strain. To a great extent, the high Tc is beyond the liquid nitrogen temperature (77 K), which is beneficial for the applications in future experiments. This study not only explores the superconducting properties of the monolayers LiBCH and LiCBH, but also offers practical insights into the search for high-Tc superconductors. Published by the American Physical Society 2024

Larger grains in high-Tc superconductors synthesized by the solid-state reaction route

Solid-state synthesis is widely used in exploratory research to study various structural modifications that affect the properties (critical temperature, critical current density, irreversibility field, etc.) of superconductors. The popularity of this method is due to its relative simplicity and availability of the necessary equipment. Combining solid-state synthesis and top-seeded melt growth allows us to increase the grain size in a Tm- and Nd-based 1-2-3 superconductor. Samples with a grain size up to 0.1 mm have been obtained. X-ray diffraction, scanning electron microscopy and magnetization measurements have been used for investigating this superconducting material. The magnetization width ΔM has increased significantly in the synthesized samples. However the temperature dependence of the intragrain critical current density and the pinning force scaling give evidences that the pinning mechanism in the obtained superconductor is essentially the same as in polycrystalline superconductors synthesized by standard solid-state technology. The increase in grain size in the synthesized samples is the main reason for the high values of ΔM.

Vertex corrections on the conductivity of high-Tc superconductors in the spin polaron formulation

Vertex corrections on the conductivity of high-Tc superconductors in the spin polaron formulation

High-TC superconductivity in La3Ni2O7 based on the bilayer two-orbital t-J model

The recently discovered high-Tc superconductor La3Ni2O7 has sparked renewed interest in unconventional superconductivity. Here we study superconductivity in pressurized La3Ni2O7 based on a bilayer two-orbital t−J model, using the renormalized mean-field theory. Our results reveal a robust s±-wave pairing driven by the inter-layer dz2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{{z}^{2}}$$\\end{document} magnetic coupling, which exhibits a transition temperature within the same order of magnitude as the experimentally observed Tc ~ 80 K. We establish a comprehensive superconducting phase diagram in the doping plane. Notably, the La3Ni2O7 under pressure is found to be situated roughly in the optimal doping regime of the phase diagram. When the dx2−y2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{{x}^{2}-{y}^{2}}$$\\end{document} orbital becomes close to half-filling, d-wave and d + is pairing can emerge from the system. We discuss the interplay between Fermi surface topology and different pairing symmetries. The stability of the s±-wave pairing against Hund’s coupling and other magnetic exchange couplings is discussed.

A new perspective on ductile high-Tc superconductors under ambient pressure: few-hydrogen metal-bonded hydrides

Superconducting materials have garnered widespread attention due to their zero-resistance characteristic and complete diamagnetism. After more than 100 years of exploration, various high-temperature superconducting materials including cuprates, nickelates, iron-based compounds, and ultra-high pressure multi-hydrides have been discovered. However, the practical application of these materials is severely hindered by their poor ductility and/or the need for high-pressure conditions to maintain structural stability. To address these challenges, we first provide a new thought to build high-temperature superconducting materials based on few-hydrogen metal-bonded hydrides under ambient pressure. We then review the related research efforts in this article. Moreover, based on the bonding type of atoms, we classify the existing important superconducting materials and propose the new concepts of pseudo-metal and quasi-metal superconductivity, which are expected to be helpful for the design of new high-temperature superconducting materials in the future.

A pulsed current set-up for use in magnetic fields above 30 T; application to high-temperature superconductors

Physical measurements of the normal state of an unconventional or high-temperature superconductor in the zero-temperature limit can provide vital information on the nature of the electronic ground state from which the superconductivity emerges. Viable routes to fully suppress the superconductivity include the application of magnetic fields stronger than the upper critical field Hc 2 or current densities larger than the critical current density Jc . In high-Tc superconductors, Hc 2 is typically higher than the available field strengths, while high currents can often create large heating effects that cause irreparable damage to the sample. Here, we present a technique that combines intense current pulses with high magnetic fields to fully suppress the superconductivity of a candidate high-Tc superconductor while keeping both J and μ 0 H below their critical values. Two adaptable circuit designs are presented with negligible stray field or self-heating effects (below a critical current value). As a proof of principle, we apply the technique to a high-Tc cuprate with nominal μ 0 Hc 2 ∼ 36 T and demonstrate the suppression of superconductivity down to T/Tc ≤ 0.1 in a field strength of just 24 T. Further applications of this dual technique are also discussed.

Prediction of Room-Temperature Superconductivity in Quasi-Atomic H2-Type Hydrides at High Pressure.

Achieving superconductivity at room temperature (RT) is a holy grail in physics. Recent discoveries on high-Tc superconductivity in binary hydrides H3S and LaH10 at high pressure have directed the search for RT superconductors to compress hydrides with conventional electron-phonon mechanisms. Here, an exceptional family of superhydrides is predicated under high pressures, MH12 (M = Mg, Sc, Zr, Hf, Lu), all exhibiting RT superconductivity with calculated Tcs ranging from 313 to 398 K. In contrast to H3S and LaH10, the hydrogen sublattice in MH12 is arranged as quasi-atomic H2 units. This unique configuration is closely associated with high Tc, attributed to the high electronic density of states derived from H2 antibonding states at the Fermi level and the strong electron-phonon coupling related to the bending vibration of H2 and H-M-H. Notably, MgH12 and ScH12 remain dynamically stable even at pressure below 100 GPa. The findings offer crucial insights into achieving RT superconductivity and pave the way for innovative directions in experimental research.

Novel ground state structures of N-doped LuH3

Ab-initio crystal structure searches have played a pivotal role in recent discoveries of high-Tc hydride superconductors under high pressure. Using evolutionary crystal searches, we predict novel ground state structures of N-doped LuH3 at ambient conditions. We find an insulating ground state structure for LuN0.125H2.875 (∼1.0 wt.% N), contrary to earlier studies where assumed structures were all metallic. This insulating behavior of ground state was found to persist up to ∼45 GPa. However our crystal structure searches revealed a metallic state for an H-deficient variant of LuN0.125H2.875. We study bonding characteristics of important structures by calculating electronic density of states, electronic-localization functions and Bader charges. Our Bader charge analysis shows that insulators have both H+ and H− ions whereas metals have only H− ions. We find that H+ ions are bonded to N atoms via a very short covalent bond. Thus we identify a clear relationship between formation of N–H bonds and insulating behavior of materials. Besides this, we perform crystal structure searches for three more compositions with higher N-content (>1.0 wt.%). Analysis of electronic properties shows that the ground states of these compositions are insulator.

Vector substrate-based Josephson junctions

We present a way to fabricate bicrystal Josephson junctions of high-Tc cuprate superconductors that are not grown on bulk bicrystalline substrates. Based on vector substrate technology, this approach makes use of a few tens-of-nanometer-thick bicrystalline membranes transferred onto conventional substrates. We demonstrate 24° [001]-tilt YBa2Cu3O7−x Josephson junctions fabricated on sapphire single crystals by utilizing 10-nm-thick bicrystalline SrTiO3 membranes. This technique allows one to manufacture bicrystalline Josephson junctions of high-Tc superconductors on a large variety of bulk substrate materials, providing distinctive degrees of freedom in designing the junctions and their electronic properties. Furthermore, it offers the capability to replace the fabrication of bulk bicrystalline substrates with thin-film growth methods.

Oxalate and adipate mediated fabrication of CuO nanocrystallites for their electrochemical and supercapacitance studies

Cupric oxide (CuO) has been comprehensively studied in the field of electrochemistry due to its high Tc-Superconducting property. The present work focus on two different CuO materials i.e. CuO-1 and CuO-2 nanocrystallites which are successfully synthesized from their oxalate and adipate precursors respectively. The calcination temperature for the synthesis of CuO from their precursors is ascertained by TGA analysis of the dicarboxylates. Both the CuO materials are thoroughly characterized by SEM–EDS, XRD, IR and XPS spectroscopic techniques. As a candidate for supercapacitor electrode material, CuO-1/C and CuO-2/C showed a specific capacitance of 4.15 F/g and 22.24 F/g using cyclic voltammetry, 10.4 F/g and 46.6 F/g using GCD curves respectively at a current density of 1 A/g. Also, the CuO-1/C and CuO-2/C showed a specific energy density (Es) 1.59 Wh kg−1 and 0.36 Wh kg−1 at a specific power density (Ps) of 0.02 kW kg−1 and 0.025 kW kg−1 respectively. Moreover, the CuO-2/C exhibits ≈ 96.1% coulombic efficiency following 1000 cycles, whereas, CuO-1/C lags in coulombic efficiency with only 51.8%. As a better candidate, CuO-2/C exhibited excellent rate capability with an outstanding cycling stability of 93.7% retention after 1,000 cycles. The factors contributing to the significant specific capacitance of CuO-2/C along with better stability and reproducibility are its low electrolyte resistance Rs (2.47Ω) and charge transfer resistance Rct (1.01 Ω).

Unidirectional Charge Orders Induced by Oxygen Vacancies on SrTiO3(001).

The discovery of high-mobility two-dimensional electron gas and low carrier density superconductivity in multiple SrTiO3-based heterostructures has stimulated intense interest in the surface properties of SrTiO3. The recent discovery of high-Tc superconductivity in the monolayer FeSe/SrTiO3 led to the upsurge and underscored the atomic precision probe of the surface structure. By performing atomically resolved cryogenic scanning tunneling microscopy/spectroscopy characterization on dual-TiO2-δ-terminated SrTiO3(001) surfaces with (√13 × √13), c(4 × 2), mixed (2 × 1), and (2 × 2) reconstructions, we disclosed universally broken rotational symmetry and contrasting bias- and temperature-dependent electronic states for apical and equatorial oxygen sites. With the sequentially evolved surface reconstructions and simultaneously increasing equatorial oxygen vacancies, the surface anisotropy reduces and the work function lowers. Intriguingly, unidirectional stripe orders appear on the c(4 × 2) surface, whereas local (4 × 4) order emerges and eventually forms long-range unidirectional c(4 × 4) charge order on the (2 × 2) surface. This work reveals robust unidirectional charge orders induced by oxygen vacancies due to strong and delicate electronic-lattice interaction under broken rotational symmetry, providing insights into understanding the complex behaviors in perovskite oxide-based heterostructures.