Unconventional Superconductivity Research Articles

Unconventional superconductivity without doping in infinite-layer nickelates under pressure

High-temperature unconventional superconductivity quite generically emerges from doping a strongly correlated parent compound, often (close to) an antiferromagnetic insulator. The recently developed dynamical vertex approximation is a state-of-the-art technique that has quantitatively predicted the superconducting dome of nickelates. Here, we apply it to study the effect of pressure in the infinite-layer nickelate SrxPr1−xNiO2. We reproduce the increase of the critical temperature (Tc) under pressure found in experiment up to 12 GPa. According to our results, Tc can be further increased with higher pressures. Even without Sr-doping the parent compound, PrNiO2, will become a high-temperature superconductor thanks to a strongly enhanced self-doping of the Ni 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 under pressure. With a maximal Tc of 100 K around 100 GPa, nickelate superconductors can reach that of the best cuprates.

Spin-charge-lattice couplings and Co doping effect in Ba(Fe1-xCox)2As2: An ab initio molecular dynamics study

Abstract As one of the typical iron-based superconductors, Ba(Fe1-xCox)2As2 exhibits a dome-like evolution of superconducting transition temperature T c with the Co doping (x), which provides an ideal platform to explore the mechanism of unconventional superconductivity. Through ab initio molecular dynamics (AIMD) studies, we find that the spin, charge, and lattice degrees of freedom in Ba(Fe1-xCox)2As2 are intimately coupled with a characteristic frequency around 5.5 THz, which originates from the A1g phonon mode of the As atoms. Compared with the undoped BaFe2As2, the spin dynamics in Ba(Fe1-xCox)2As2 (x = 0.0625, 0.1250, 0.1875) shows enhanced spatial inhomogeneities, though the features of the charge dynamics are rarely modified. Along with the increasing Co doping, the spatial inhomogeneities of Fe spin dynamics display nonmonotonic changes, mean-while the lattice vibrational spectra first show peak broadening and then restore the main peak around 5.5 THz, being both consistent with the nonmonotonic behavior of superconducting T c. Our study provides a molecular dynamics approach to investigate the couplings of spin, charge, and lattice in doped BaFe2As2, which could also be applied to explore the dome-like evolution of superconductivity in other Fe-based superconductors.

Uniaxial stress effect on the electronic structure of quantum materials

Uniaxial stress has proven to be a powerful experimental tuning parameter for effectively controlling lattice, charge, orbital, and spin degrees of freedom in quantum materials. In addition, its ability to manipulate the symmetry of materials has garnered significant attention. Recent technical progress to combine uniaxial stress cells with quantum oscillation and angle-resolved photoemission techniques allowed to study the electronic structure as function of uniaxial stress. This review provides an overview on experimental advancements in methods and examines studies on diverse quantum materials, encompassing the semimetal WTe2, the unconventional superconductor Sr2RuO4, Fe-based superconductors, and topological materials.

Interfacially enhanced superconductivity in Fe(Te,Se)/Bi4Te3 heterostructures.

Realizing topological superconductivity by integrating high-transition-temperature (TC) superconductors with topological insulators can open new paths for quantum computing applications. Here, we report a new approach for increasing the superconducting transition temperature by interfacing the unconventional superconductor Fe(Te,Se) with the topological insulator Bi-Te system in the low-Se doping regime, near where superconductivity vanishes in the bulk. The critical finding is that the of Fe(Te,Se) increases from nominally non-superconducting to as high as 12.5K when Bi2Te3 is replaced with the topological phase Bi4Te3. Interfacing Fe(Te,Se) with Bi4Te3 is also found to be critical for stabilizing superconductivity in monolayer films where can be as high as 6K. Measurements of the electronic and crystalline structure of the Bi4Te3 layer reveal that a large electron transfer, epitaxial strain, and novel chemical reduction processes are critical factors for the enhancement of superconductivity. This novel route for enhancing TC in an important epitaxial system provides new insight on the nature of interfacial superconductivity and a platform to identify and utilize new electronic phases. This article is protected by copyright. All rights reserved.

Theory of majorana zero modes in unconventional superconductors

Abstract Majorana fermions are spin-1/2 neutral particles that are their own antiparticles and were initially predicted by Ettore Majorana in particle physics but their observation still remains elusive. The concept of Majorana fermions has been borrowed into condensed matter physics, where, unlike particle physics, Majorana fermions emerge as zero-energy quasiparticles that can be engineered by combining electrons and holes and have therefore been coined Majorana zero modes. In this review, we provide a pedagogical explanation of the basic properties of Majorana zero modes in unconventional superconductors and their consequences in experimental observables, putting a special emphasis on the initial theoretical discoveries. In particular, we first show that Majorana zero modes are self-conjugated and emerge as a special type of zero energy surface Andreev bound states at the boundary of unconventional superconductors. We then explore Majorana zero modes in one-dimensional spin-polarized p-wave superconductors, where we address the formation of topological superconductivity and the physical realization in superconductor-semiconductor hybrids. In this part we highlight that Majorana quasiparticles appear as zero-energy edge states, exhibiting charge neutrality, spin-polarized, and spatial nonlocality as unique properties that can be already seen from their energies and wavefunctions. Next, we discuss analytically obtained Green’s functions of p-wave superconductors and demonstrate that the emergence of Majorana zero modes is always accompanied by the formation of odd-frequency spin-triplet pairing as a unique result of the self-conjugate nature of Majorana zero modes. We finally address the signatures of Majorana zero modes in tunneling spectroscopy, including the anomalous proximity effect, and the phase-biased Josephson effect.

Unconventional superconductivity and charge ordering in an extended ionic Hubbard model on the triangular lattice

To address the issues of superconducting and charge properties in hydrated sodium cobalt, we investigate an extended ionic Hubbard model on the triangular lattice, which includes off-site attractions between sites with minor charges. Our quantum Monte Carlo simulations show that close to quarter filling, the off-site attractions induce a significant enhancement of d-wave and extended s-wave pairing correlations. Simultaneously, they render an increase of the charge structure factor at most of wave vectors. A combination with charge correlations in real space indicates the development of short-range finite-q charge density waves on the sites with minor charges. Our findings provide a new perspective on the superconducting mechanism in hydrated sodium cobalt based on the electronic structure which explicitly takes the effect of sodium atoms into account.

Robust Superconductivity in Infinite-Layer Nickelates.

The recent discovery of nickelate superconductivity represents an important step toward understanding the four-decade mastery of unconventional high-temperature superconductivity. However, the synthesis of the infinite-layer nickelate superconductors shows great challenges. Particularly, surface capping layers are usually unitized to facilitate the sample synthesis. This leads to an important question whether nickelate superconductors with d9 configuration and ultralow valence of Ni1+ are in metastable state and whether nickelate superconductivity can be robust? In this work, a series of redox cycling experiments are performed across the phase transition between perovskite Nd0.8Sr0.2NiO3 and infinite-layer Nd0.8Sr0.2NiO2. The infinite-layer Nd0.8Sr0.2NiO2 is quite robust in the redox environment and can survive the cycling experiments with unchanged crystallographic quality. However, as the cycling number goes on, the perovskite Nd0.8Sr0.2NiO3 shows structural degradation, suggesting stability of nickelate superconductivity is not restricted by the ultralow valence of Ni1+, but by the quality of its perovskite precursor. The observed robustness of infinite-layer Nd0.8Sr0.2NiO2 up to ten redox cycles further indicates that if an ideal high-quality perovskite precursor can be obtained, infinite-layer nickelate superconductivity can be very stable and sustainable under environmental conditions. This work provides important implications for potential device applications for nickelate superconductors.

Multiple topological phase transitions unveiling gapless topological superconductivity in magnet/unconventional superconductor hybrid platform

We propose a theoretical framework for generating gapless topological superconductivity (GTSC) hosting Majorana flat edge modes (MFEMs) in the presence of a two-dimensional (2D) array of magnetic adatoms with noncollinear spin texture deposited on top of an unconventional superconductor. Our observations reveal two distinct topological phase transitions within the emergent Shiba band depending on the exchange coupling strength (J) between magnetic adatom spins and superconducting electrons: the first one designates transition from gapless non-topological to gapless topological phase at lower J, while the second one denotes transition from gapless topological to a trivial gapped superconducting phase at higher J. The gapless topological superconducting phase survives at intermediate values of J, hosting MFEMs. Furthermore, we investigate the nature of the bulk effective pairings, which indicate that GTSC appears due to the interplay between pseudo “s-wave” and pseudo “px+py” types of pairing. Consequently, our study opens a promising avenue for the experimental realization of GTSC in 2D Shiba lattice based on d-wave superconductors as a high-temperature platform.

Enhancement of superconductivity and phase diagram of Ta-doped Kagome superconductor CsV3Sb5

Kagome superconductors AV3Sb5 (A = K, Rb, and Cs) have attracted enormous interest due to the coexistence of charge density wave (CDW) order, unconventional superconductivity (SC) and anomalous Hall effect (AHE). In this paper, we reported an intensive investigation on Cs(V1−xTax)3Sb5 single crystals with systematic Ta doping. Ta was confirmed to be doped into V-site in the Kagome layer from both single crystal X-ray diffraction structural refinement and scanning transmission electron microscopy observation. The highest Ta doping level was found to be about 16%, which is more than twice as much as 7% in Nb-doped CsV3Sb5. With the increase of Ta doping, CDW order was gradually suppressed and finally vanished when the doping level reached to more than 8%. Meanwhile, superconductivity was enhanced with a maximum critical temperature (Tc) of 5.3 K, which is the highest Tc in the bulk crystal of this Kagome system at ambient pressure so far. The μ0Hc2(T) behavior demonstrates that the system is still a two-band superconductor after Ta doping. Based on the electrical transport measurement, a phase diagram was set up to exhibit the evolution of CDW and SC in the Cs(V1−xTax)3Sb5 system. These findings pave a new way to search for new superconductors with higher Tc in the AV3Sb5 family and establish a new platform for tuning and controlling the multiple orders and superconducting states.

Environmental response characteristics of epitaxial superconducting La0.8Sr0.2NiO2 thin films

Despite the discovery of superconducting properties in thin films with an infinite-layer structured nickelate has paved the way for exploring unconventional superconductivity, opening up new possibilities in this field. However, the challenges related to fabricating these samples have greatly restricted research in this area. In this study, we successfully fabricated superconducting thin films of La0.8Sr0.2NiO2 and investigated their tolerance to different environmental factors. To analyze the stability of the superconducting La0.8Sr0.2NiO2 thin films, we assessed their tolerance to temperature by examining the peak intensities in X-ray diffraction (XRD) and monitoring the changes in resistance curves at varying temperatures. In addition, we investigated the films’ sensitivity to acidity and alkalinity by immersing them in acidic and alkaline solutions for various durations. We also studied the stability of the thin films under various conditions, including heating in air, heating in a vacuum, exposure to acid and alkali, as well as exposure to the organic solvent acetone solution. Our findings highlight the successful preparation of superconducting La0.8Sr0.2NiO2 thin films and shed light on their stability in different environments. This research provides valuable insights for further exploration of their potential applications and laid the foundation for advancements in the field of unconventional superconductivity.

Moiré-enabled topological superconductivity in twisted bilayer graphene

Twisted van der Waals materials have risen as highly tunable platforms for realizing unconventional superconductivity. Here we demonstrate how a topological superconducting state can be driven in a twisted graphene multilayer at a twist angle of approximately 1.6 degrees proximitized to other 2D materials. We show that an encapsulated twisted bilayer subject to induced Rashba spin–orbit coupling, s-wave superconductivity, and exchange field generates a topological superconducting state enabled by the moiré pattern. We demonstrate the emergence of a variety of topological states with different Chern numbers, that are highly tunable through doping, strain, and bias voltage. Our proposal does not depend on fine-tuning the twist angle, but solely on the emergence of moiré minibands and is applicable for twist angles between 1.3 and 3 degrees. Our results establish the potential of twisted graphene bilayers to create topological superconductivity without requiring ultraflat dispersions.

Engineering Flat Bands in Twisted-Bilayer Graphene away from the Magic Angle with Chiral Optical Cavities.

Twisted bilayer graphene (TBG) is a recently discovered two-dimensional superlattice structure which exhibits strongly correlated quantum many-body physics, including strange metallic behavior and unconventional superconductivity. Most of TBG exotic properties are connected to the emergence of a pair of isolated and topological flat electronic bands at the so-called magic angle, θ≈1.05°, which are nevertheless very fragile. In this work, we show that, by employing chiral optical cavities, the topological flat bands can be stabilized away from the magic angle in an interval of approximately 0.8°<θ<1.3°. As highlighted by a simplified theoretical model, time reversal symmetry breaking (TRSB), induced by the chiral nature of the cavity, plays a fundamental role in flattening the isolated bands and gapping out the rest of the spectrum. Additionally, TRSB suppresses the Berry curvature and induces a topological phase transition, with a gap closing at the Γ point, towards a band structure with two isolated flat bands with Chern number equal to 0. The efficiency of the cavity is discussed as a function of the twisting angle, the light-matter coupling and the optical cavity characteristic frequency. Our results demonstrate the possibility of engineering flat bands in TBG using optical devices, extending the onset of strongly correlated topological electronic phases in moiré superlattices to a wider range in the twisting angle.

Toward Reliable Synthesis of Superconducting Infinite Layer Nickelate Thin Films by Topochemical Reduction.

Infinite layer (IL) nickelates provide a new route beyond copper oxides to address outstanding questions in the field of unconventional superconductivity. However, their synthesis poses considerable challenges, largely hindering experimental research on this new class of oxide superconductors. That synthesis is achieved in a two-step process that yields the most thermodynamically stable perovskite phase first, then the IL phase by topotactic reduction, the quality of the starting phase playing a crucial role. Here, a reliable synthesis of superconducting IL nickelate films is reported after successive topochemical reductions of a parent perovskite phase with nearly optimal stoichiometry. Careful analysis of the transport properties of the incompletely reduced films reveals an improvement in the strange metal behavior of their normal state resistivity over subsequent topochemical reductions, offering insight into the reduction process.

Strain Engineering of Twisted Bilayer Graphene: The Rise of Strain-Twistronics.

The layer-by-layer stacked van der Waals structures (termed vdW hetero/homostructures) offer a new paradigm for materials design-their physical properties can be tuned by the vertical stacking sequence as well as by adding a mechanical twist, stretch, and hydrostatic pressure to the atomic structure. In particular, simple twisting and stacking of two layers of graphene can form a uniform and ordered Moiré superlattice, which can effectively modulate the electrons of graphene layers and lead to the discovery of unconventional superconductivity and strong correlations. However, the twist angle of twisted bilayer graphene (tBLG) is almost unchangeable once the interlayer stacking is determined, while applying mechanical elastic strain provides an alternative way to deeply regulate the electronic structure by controlling the lattice spacing and symmetry. In this review, diverse experimental advances are introduced in straining tBLG by in-plane and out-of-plane modes, followed by the characterizations and calculations toward quantitatively tuning the strain-engineered electronic structures. It is further discussed that the structural relaxation in strained Moiré superlattice and its influence on electronic structures. Finally, the conclusion entails prospects for opportunities of strained twisted 2D materials, discussions on existing challenges, and an outlook on the intriguing emerging field, namely "strain-twistronics".

Two-Dimensional Os2Se3 Nanosheet: A Ferroelectric Metal with Room-Temperature Ferromagnetism.

Two-dimensional (2D) ferroelectric metals (FEMs) possess intriguing characteristics, such as unconventional superconductivity and the nonlinear anomalous Hall effect. However, their occurrence is exceedingly rare due to mutual repulsion between ferroelectricity and metallicity. In addition, further incorporating other features like ferromagnetism into FEMs to enhance their functionalities poses a significantly greater challenge. Here, via first-principles calculations, we demonstrate a case of an FEM that features a coexistence of room-temperature ferromagnetism, ferroelectricity, and metallicity in a thermodynamically stable 2D Os2Se3. It presents a vertical electric polarization of 3.00 pC/m that exceeds those of most FEMs and a moderate polarization switching barrier of 0.22 eV per formula unit. Moreover, 2D Os2Se3 exhibits robust ferromagnetism (Curie temperature TC ≈ 527 K) and a sizable magnetic anisotropy energy (-30.87 meV per formula unit). Furthermore, highly magnetization-dependent electrical conductivity is revealed, indicative of strong magnetoelectric coupling. Berry curvature calculation suggests that the FEM might exhibit nontrivial band topology.

Spectral form factors of unconventional superconductors

Spectral form factors of unconventional superconductors

Charge transfer and spin-valley locking in 4Hb-TaS2

Abstract4Hb-TaS2 is a superconductor that exhibits unique characteristics such as time-reversal symmetry breaking, hidden magnetic memory, and topological edge modes. It is a naturally occurring heterostructure comprising of alternating layers of 1H-TaS2 and 1T-TaS2. The former is a well-known superconductor, while the latter is a correlated insulator with a possible non- trivial magnetic ground state. In this study, we use angle resolved photoemission spectroscopy to investigate the normal state electronic structure of this unconventional superconductor. Our findings reveal that the band structure of 4Hb-TaS2 fundamentally differs from that of its constituent materials. Specifically, we observe a significant charge transfer from the 1T layers to the 1H layers that drives the 1T layers away from half-filling. In addition, we find a substantial reduction in inter-layer coupling in 4Hb-TaS2 compared to the coupling in 2H-TaS2 that results in a pronounced spin-valley locking within 4Hb-TaS2.

Mott Gap Filling by Doping Electrons through Depositing One Sub-Monolayer Thin Film of Rb on Ca2CuO2Cl2

Understanding the doping evolution from a Mott insulator to a superconductor probably holds the key to resolve the mystery of unconventional superconductivity in copper oxides. To elucidate the evolution of the electronic state starting from the Mott insulator, we dose the surface of the parent phase Ca2CuO2Cl2 by depositing Rb atoms, which are supposed to donate electrons to the CuO2 planes underneath. We successfully achieved the Rb sub-monolayer thin films in forming the square lattice. The scanning tunneling microscopy or spectroscopy measurements on the surface show that the Fermi energy is pinned within the Mott gap but close to the edge of the charge transfer band. In addition, an in-gap state appears at the bottom of the upper Hubbard band (UHB), and the Mott gap will be significantly diminished. Combined with the Cl defect and the Rb adatom/cluster results, the electron doping is likely to increase the spectra weight of the UHB for the double occupancy. Our results provide information to understand the electron doping to the parent compound of cuprates.

Beyond Conventional Charge Density Wave for Strongly Enhanced 2D Superconductivity in 1H-TaS2 Superlattices.

Noncentrosymmetric transition metal dichalcogenide (TMD) monolayers offer a fertile platform for exploring unconventional Ising superconductivity (SC) and charge density waves (CDWs). However, the vulnerability of isolated monolayers to structural disorder and environmental oxidation often degrade their electronic coherence. Herein, an alternative approach is reported for fabricating stable and intrinsic monolayers of 1H-TaS2 sandwiched between SnS blocks in a (SnS)1.15TaS2 van der Waals (vdW) superlattice. The SnS block layers not only decouple individual 1H-TaS2 sublayers to endow them with monolayer-like electronic characteristics, but also protect the 1H-TaS2 layers from electronic degradation. The results reveal the characteristic 3 × 3 CDW order in 1H-TaS2 sublayers associated with electronic rearrangement in the low-lying sulfur p band, which uncovers a previously undiscovered CDW mechanism rather than the conventional Fermi surface-related framework. Additionally, the (SnS)1.15TaS2 superlattice exhibits a strongly enhanced Ising-like SC with a layer-independent Tc of ≈3.0 K, comparable to that of the isolated monolayer 1H-TaS2 sample, presumably attributed to their monolayer-like characteristics and retained Fermi states. These results provide new insights into the long-debated CDW order and enhanced SC of monolayer 1H-TaS2, establishing bulk vdW superlattices as promising platforms for investigating exotic collective quantum phases in the 2D limit.

Electronic and superconducting properties of CoSi[formula omitted] films on silicon—An unconventional superconductor with technological potential

We report the observation of unusual normal-state electronic conduction properties and superconducting characteristics of high-quality CoSi2/Si films grown on silicon Si(100) and Si(111) substrates. A good understanding of these features shall help to address the underlying physics of the unconventional pairing symmetry recently discovered in transparent CoSi2/TiSi2 heterojunctions (Chiu et al., 2021; Chiu et al., 2023), where CoSi2/Si is a superconductor with a superconducting transition temperature Tc≃ (1.1–1.5) K, dependent on its dimensions, and TiSi2 is a normal metal. In CoSi2/Si films, we find a pronounced positive magnetoresistance caused by the weak-antilocalization effect, indicating a strong Rashba spin–orbit coupling (SOC). This SOC generates two-component superconductivity in CoSi2/TiSi2 heterojunctions. The CoSi2/Si films are stable under ambient conditions and have ultralow 1/f noise. Moreover, they can be patterned via the standard lithography techniques, which might be of considerable practical value for future scalable superconducting and quantum device fabrication.