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DOE OSTI2024

Proximity-Induced Superconductivity in a 2D Kondo Lattice of an f -Electron-Based Surface Alloy

Realizing hybrids of low-dimensional Kondo lattices and superconducting substrates leads to fascinating platforms for studying the exciting physics of strongly correlated electron systems with induced superconducting pairing. Here, we report a scanning tunneling microscopy and spectroscopy study of a new type of two-dimensional (2D) La–Ce alloy grown epitaxially on a superconducting Re(0001) substrate. We observe the characteristic spectroscopic signature of a hybridization gap evidencing the coherent spin screening in the 2D Kondo lattice realized by the ultrathin La–Ce alloy film on normal conducting Re(0001). Upon lowering the temperature below the critical temperature of rhenium, a superconducting gap is induced exhibiting an energy asymmetry of the coherence peaks that arises from the interaction of residual unscreened magnetic moments with the superconducting substrate. A positive correlation between the Kondo hybridization gap and the asymmetry of the coherence peaks is found.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Tailoring Superconductivity with Quantum Dislocations

Despite the established knowledge that crystal dislocations can affect a material’s superconducting properties, the exact mechanism of the electron-dislocation interaction in a dislocated superconductor has long been missing. Being a type of defect, dislocations are expected to decrease a material’s superconducting transition temperature (T c ) by breaking the coherence. Yet experimentally, even in isotropic type I superconductors, dislocations can either decrease, increase, or have little influence on T c . These experimental findings have yet to be understood. Although the anisotropic pairing in dirty superconductors has explained impurity-induced T c reduction, no quantitative agreement has been reached in the case a dislocation given its complexity. By generalizing the one-dimensional quantized dislocation field to three dimensions, we reveal that there are indeed two distinct types of electron-dislocation interactions. Besides the usual electron-dislocation potential scattering, there is another interaction driving an effective attraction between electrons that is caused by dislons, which are quantized modes of a dislocation. The role of dislocations to superconductivity is thus clarified as the competition between the classical and quantum effects, showing excellent agreement with existing experimental data. In particular, the existence of both classical and quantum effects provides a plausible explanation for the illusive origin of dislocation-induced superconductivity in semiconducting PbS/PbTe superlattice nanostructures. A quantitative criterion has been derived, in which a dislocated superconductor with low elastic moduli and small electron effective mass and in a confined environment is inclined to enhance T c . This provides a new pathway for engineering a material’s superconducting properties by using dislocations as an additional degree of freedom.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Structure and Superconductivity of Hydrogenated TiZr Alloys Under High Pressure

The effects of pressure on the structure and electrical transport properties, including electrical resistance and critical magnetic field values for superconductivity in pristine and hydrogenated TiZr alloys, were investigated. As pressure increased from ambient to 55 GPa, the structure of the pristine TiZr alloys transformed from hcp to bcc via an intermediate ω phase. The superconducting transition temperature (T c ) significantly increased from 1.76 K at ambient pressure to 15.5 K at 52.2 GPa, accompanied by an extrapolated upper critical field of 24.5 T at T = 0 K. In contrast, the hydrogenated samples exhibited substantially lower T c values compared to the pristine ones, with a T c of 4.6 K at 50.5 GPa and an extrapolated upper critical field of 1.8 T at T = 0 K. Upon decompression, the superconductivity in the hydrogenated sample persisted down to 25 GPa, disappearing when the pressure was reduced to 19 GPa. Synchrotron X-ray diffractions (XRD) analysis revealed the formation of three hydrides: I4/mmm-(Ti, Zr)H 2 , P6 3 /mmc-(Ti, Zr)H 3 , and I4̅3d-(Ti,Zr) 4 H 15 . Finally, by combining XRD and electrical resistance data, we tentatively propose that the P6 3 /mmc-(Ti, Zr)H 3 predominantly induces superconductivity. In contrast to superhydrides, where electron–phonon interactions increase the superconducting temperature at high pressure, hydrogen atoms in hcp-(Ti, Zr)H 3 reduce T c .

36 MATERIALS SCIENCE↗
DOE OSTI2021

Two-Dimensional 2M-WS 2 Nanolayers for Superconductivity

Recently, a newly discovered VIB group transition metal dichalcogenide (TMD) material, 2M-WS 2 , has attracted extensive attention due to its interesting physical properties such as topological superconductivity, nodeless superconductivity, and anisotropic Majorana bound states. However, the techniques to grow high-quality 2M-WS 2 bulk crystals and the study of their physical properties at the nanometer scale are still limited. In this work, we report a new route to grow high-quality 2M-WS 2 single crystals and the observation of superconductivity in its thin layers. The crystal structure of the as-grown 2M-WS 2 crystals was determined by X-ray diffraction (XRD) and scanning tunneling microscopy (STM). The chemical composition of the 2M-WS 2 crystals was determined by energy dispersive X-ray spectroscopy (EDS) analysis. At 77 K, we observed the spatial variation of the local tunneling conductance (dI/dV) of the 2M-WS2 thin flakes by scanning tunneling spectroscopy (STS). Our low temperature transport measurements demonstrate clear signatures of superconductivity of a 25 nm-thick 2M-WS 2 flake with a critical temperature (T C ) of ~8.5 K and an upper critical field of ~2.5 T at T = 1.5 K. Our work may pave new opportunities in studying the topological superconductivity at the atomic scale in simple 2D TMD materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Superconductivity in a chiral nanotube

Chirality of materials are known to affect optical, magnetic and electric properties, causing a variety of nontrivial phenomena such as circular dichiroism for chiral molecules, magnetic Skyrmions in chiral magnets and nonreciprocal carrier transport in chiral conductors. On the other hand, effect of chirality on superconducting transport has not been known. Here we report the nonreciprocity of superconductivity—unambiguous evidence of superconductivity reflecting chiral structure in which the forward and backward supercurrent flows are not equivalent because of inversion symmetry breaking. Such superconductivity is realized via ionic gating in individual chiral nanotubes of tungsten disulfide. The nonreciprocal signal is significantly enhanced in the superconducting state, being associated with unprecedented quantum Little-Parks oscillations originating from the interference of supercurrent along the circumference of the nanotube. The present results indicate that the nonreciprocity is a viable approach toward the superconductors with chiral or noncentrosymmetric structures

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Superconductivity: The persistence of pairs

Superconductivity stems from a weak attraction between electrons that causes them to form bound pairs and behave much like bosons. These so-called Cooper pairs are phase coherent, which leads to the astonishing properties of zero electrical resistance and magnetic flux expulsion typical of superconducting materials. This coherent state may be qualitatively understood within the Bose–Einstein condensate (BEC) model, which predicts that a gas of interacting bosons will become unstable below a critical temperature and condense into a phase of matter with a macroscopic, coherent population in the lowest energy state, as happens in 4 He or cold atomic gases. The successful theory proposed by Bardeen, Cooper and Schrieffer (BCS) predicts that at the superconducting transition temperature T c , electrons simultaneously form pairs and condense, with no sign of pairing above T c . Theorists have long surmised that the BCS and BEC models are opposite limits of a single theory and that strong interactions or low density can, in principle, drive the system to a paired state at a temperature Tpair higher than T c , making the transition to the superconducting state BEC-like (Fig. 1). Yet most superconductors to date are reasonably well described by BCS theory or its extensions, and there has been scant evidence in electronic materials for the existence of pairing independent of the full superconducting state (though an active debate rages over the cuprate superconductors). Writing in Nature, Jeremy Levy and colleagues have now used ingenious nanostructured devices to provide evidence for electron pairing1. Perhaps surprisingly, the material they have studied is a venerable, yet enigmatic, low-temperature superconductor, SrTiO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Anisotropic superconductivity induced by periodic multiferroic domain patterns

Abstract The competition between order parameters, such as ferroelectricity, ferromagnetism, and superconductivity, is one of the most fascinating topics in condensed matter physics. Here, we report intriguing anisotropic superconductivity in YBa 2 Cu 3 O 7 − x films induced by a multiferroic, BiFeO 3 , with periodic domain patterns. The anisotropic superconductivity was investigated by transport measurements and supported by phase-field simulations, and then the detailed local electronic structures were revealed by cross-sectional scanning tunneling microscopy. We found that the oxygen redistribution in YBa 2 Cu 3 O 7 − x modulated by the ferroelectric polarization in BiFeO 3 was the key mechanism driving this anisotropic superconductivity. The presented heteroarchitecture of a high-temperature superconductor and a domain-engineered multiferroic provides a new approach to tune superconductivity and offers potential advantages for the design of future multifunctional devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Tuning Ising superconductivity with layer and spin–orbit coupling in two-dimensional transition-metal dichalcogenides

Systems simultaneously exhibiting superconductivity and spin–orbit coupling are predicted to provide a route toward topological superconductivity and unconventional electron pairing, driving significant contemporary interest in these materials. Monolayer transition-metal dichalcogenide (TMD) superconductors in particular lack inversion symmetry, yielding an antisymmetric form of spin–orbit coupling that admits both spin-singlet and spin-triplet components of the superconducting wavefunction. Here, we present an experimental and theoretical study of two intrinsic TMD superconductors with large spin–orbit coupling in the atomic layer limit, metallic 2H-TaS 2 and 2H-NbSe 2 . We investigate the superconducting properties as the material is reduced to monolayer thickness and show that high-field measurements point to the largest upper critical field thus reported for an intrinsic TMD superconductor. In few-layer samples, we find the enhancement of the upper critical field is sustained by the dominance of spin–orbit coupling over weak interlayer coupling, providing additional candidate systems for supporting unconventional superconducting states in two dimensions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Local orthorhombic lattice distortions in the paramagnetic tetragonal phase of superconducting NaFe1-xNixAs

Understanding the interplay between nematicity, magnetism and superconductivity is pivotal for elucidating the physics of iron-based superconductors. Here we use neutron scattering to probe magnetic and nematic orders throughout the phase diagram of NaFe 1-x Ni x As, finding that while both static antiferromagnetic and nematic orders compete with superconductivity, the onset temperatures for these two orders remain well separated approaching the putative quantum critical points. We uncover local orthorhombic distortions that persist well above the tetragonal-to-orthorhombic structural transition temperature T s in underdoped samples and extend well into the overdoped regime that exhibits neither magnetic nor structural phase transitions. These unexpected local orthorhombic distortions display Curie–Weiss temperature dependence and become suppressed below the superconducting transition temperature T c , suggesting that they result from the large nematic susceptibility near optimal superconductivity. Finally, our results account for observations of rotational symmetry breaking above T s , and attest to the presence of significant nematic fluctuations near optimal superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Creating superconductivity in WB 2 through pressure-induced metastable planar defects

High-pressure electrical resistivity measurements reveal that the mechanical deformation of ultra-hard WB 2 during compression induces superconductivity above 50 GPa with a maximum superconducting critical temperature, T c of 17 K at 91 GPa. Upon further compression up to 187 GPa, the T c gradually decreases. Theoretical calculations show that electron-phonon mediated superconductivity originates from the formation of metastable stacking faults and twin boundaries that exhibit a local structure resembling MgB 2 (hP3, space group 191, prototype AlB 2 ). Synchrotron x-ray diffraction measurements up to 145 GPa show that the ambient pressure hP12 structure (space group 194, prototype WB 2 ) continues to persist to this pressure, consistent with the formation of the planar defects above 50 GPa. The abrupt appearance of superconductivity under pressure does not coincide with a structural transition but instead with the formation and percolation of mechanically-induced stacking faults and twin boundaries. The results identify an alternate route for designing superconducting materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Tunable superconductivity and its origin at KTaO3 interfaces

Abstract What causes Cooper pairs to form in unconventional superconductors is often elusive because experimental signatures that connect to a specific pairing mechanism are rare. Here, we observe distinct dependences of the superconducting transition temperature T c on carrier density n 2D for electron gases formed at KTaO 3 (111), (001) and (110) interfaces. For the (111) interface, a remarkable linear dependence of T c on n 2D is observed over a range of nearly one order of magnitude. Further, our study of the dependence of superconductivity on gate electric fields reveals the role of the interface in mediating superconductivity. We find that the extreme sensitivity of superconductivity to crystallographic orientation can be explained by pairing via inter-orbital interactions induced by an inversion-breaking transverse optical phonon and quantum confinement. This mechanism is also consistent with the dependence of T c on n 2D . Our study may shed light on the pairing mechanism in other superconducting quantum paraelectrics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Two-component nematic superconductivity in 4Hb-TaS 2

Most superconductors have an isotropic, single component order parameter and are well described by the standard (BCS) theory for superconductivity. Unconventional, multiple-component superconductors are exceptionally rare and are much less understood. Here, we combine scanning tunneling microscopy and angle-resolved macroscopic transport for studying the candidate chiral superconductor, 4Hb-TaS 2 . We reveal quasi-periodic one-dimensional modulations in the tunneling conductance accompanied by two-fold symmetric superconducting critical field. The strong modulation of the in-plane critical field, H c2 , points to a nematic, unconventional order parameter. However, the imaged vortex core is isotropic at low temperatures. We suggest a model that reconciles this apparent discrepancy and takes into account previously observed spontaneous time-reversal symmetry breaking at low temperatures. The model describes a competition between a dominating chiral superconducting order parameter and a nematic one. The latter emerges close to the normal phase. Our results strongly support the existence of two-component superconductivity in 4Hb-TaS 2 and can provide valuable insights into other systems with coexistent charge order and superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Enhanced superconductivity and ferroelectric quantum criticality in plastically deformed strontium titanate

The properties of quantum materials are commonly tuned using experimental variables such as pressure, magnetic field and doping. Here we explore a different approach using irreversible, plastic deformation of single crystals. We show that compressive plastic deformation induces low-dimensional superconductivity well above the superconducting transition temperature (Tc) of undeformed SrTiO3, with evidence of possible superconducting correlations at temperatures two orders of magnitude above the bulk Tc. The enhanced superconductivity is correlated with the appearance of self-organized dislocation structures, as revealed by diffuse neutron and X-ray scattering. We also observe deformation-induced signatures of quantum-critical ferroelectric fluctuations and inhomogeneous ferroelectric order using Raman scattering. Our results suggest that strain surrounding the self-organized dislocation structures induces local ferroelectricity and quantum-critical dynamics that strongly influence Tc, consistent with a theory of superconductivity enhanced by soft polar fluctuations. Our results demonstrate the potential of plastic deformation and dislocation engineering for the manipulation of electronic properties of quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Superconductivity in a quintuple-layer square-planar nickelate

Since the discovery of high-temperature superconductivity in the copper oxide materials, there have been sustained efforts to both understand the origins of this phase and discover new cuprate-like superconducting materials. One prime materials platform has been the rare-earth nickelates and indeed superconductivity was recently discovered in the doped compound Nd 0.8 Sr 0.2 NiO 2 . Undoped NdNiO 2 belongs to a series of layered square-planar nickelates with chemical formula Nd n+1 Ni n O 2n+2 and is known as the 'infinite-layer' (n=∞) nickelate. Furthermore, we report the synthesis of the quintuple-layer (n=5) member of this series, Nd 6 Ni 5 O 12 , in which optimal cuprate-like electron filling (d 8.8 ) is achieved without chemical doping. We observe a superconducting transition beginning at ~13 K. Electronic structure calculations, in tandem with magnetoresistive and spectroscopic measurements, suggest that Nd 6 Ni 5 O 12 interpolates between cuprate-like and infinite-layer nickelate-like behavior. In engineering a distinct superconducting nickelate, we identify the square-planar nickelates as a new family of superconductors which can be tuned via both doping and dimensionality.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Proximity-induced superconducting gap in the quantum spin Hall edge state of monolayer WTe2

The quantum spin Hall insulator is characterized by a bandgap in the two-dimensional (2D) interior and helical 1D edge states 1 , 2 , 3 . Inducing superconductivity in the helical edge state results in a 1D topological superconductor, a highly sought-after state of matter at the core of many proposals for topological quantum computing 4 . In the present study, we report the coexistence of superconductivity and the quantum spin Hall edge state in a van der Waals heterostructure, by placing a monolayer of 1T'-WTe 2 , a quantum spin Hall insulator 1 , 2 , 3 , on a van der Waals superconductor, NbSe 2 . Using scanning tunnelling microscopy and spectroscopy (STM/STS), we demonstrate that the WTe 2 monolayer exhibits a proximity-induced superconducting gap due to the underlying superconductor and that the spectroscopic features of the quantum spin Hall edge state remain intact. Taken together, these observations provide conclusive evidence for proximity-induced superconductivity in the quantum spin Hall edge state in WTe 2 , a crucial step towards realizing 1D topological superconductivity and Majorana bound states in this van der Waals material platform.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Signatures of tunable superconductivity in a trilayer graphene moiré superlattice

Understanding the mechanism of high-transition-temperature (high-T c ) superconductivity is a central problem in condensed matter physics. It is often speculated that high-Tc superconductivity arises in a doped Mott insulator1 as described by the Hubbard model 2,3,4 . An exact solution of the Hubbard model, however, is extremely challenging owing to the strong electron–electron correlation in Mott insulators. Therefore, it is highly desirable to study a tunable Hubbard system, in which systematic investigations of the unconventional superconductivity and its evolution with the Hubbard parameters can deepen our understanding of the Hubbard model. Here we report signatures of tunable superconductivity in an ABC-trilayer graphene (TLG) and hexagonal boron nitride (hBN) moiré superlattice. Unlike in ‘magic angle’ twisted bilayer graphene, theoretical calculations show that under a vertical displacement field, the ABC-TLG/hBN heterostructure features an isolated flat valence miniband associated with a Hubbard model on a triangular superlattice 5,6 where the bandwidth can be tuned continuously with the vertical displacement field. Upon applying such a displacement field we find experimentally that the ABC-TLG/hBN superlattice displays Mott insulating states below 20 kelvin at one-quarter and one-half fillings of the states, corresponding to one and two holes per unit cell, respectively. Upon further cooling, signatures of superconductivity (‘domes’) emerge below 1 kelvin for the electron- and hole-doped sides of the one-quarter-filling Mott state. The electronic behaviour in the ABC-TLG/hBN superlattice is expected to depend sensitively on the interplay between the electron–electron interaction and the miniband bandwidth. By varying the vertical displacement field, we demonstrate transitions from the candidate superconductor to Mott insulator and metallic phases. Our study shows that ABC-TLG/hBN heterostructures offer attractive model systems in which to explore rich correlated behaviour emerging in the tunable triangular Hubbard model.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Proximity-effect-induced Superconducting Gap in Topological Surface States – A Point Contact Spectroscopy Study of NbSe 2 /Bi 2 Se 3 Superconductor-Topological Insulator Heterostructures

Proximity-effect-induced superconductivity was studied in epitaxial topological insulator Bi 2 Se 3 thin films grown on superconducting NbSe 2 single crystals. A point contact spectroscopy (PCS) method was used at low temperatures down to 40 mK. An induced superconducting gap in Bi 2 Se 3 was observed in the spectra, which decreased with increasing Bi 2 Se 3 layer thickness, consistent with the proximity effect in the bulk states of Bi 2 Se 3 induced by NbSe 2 . At very low temperatures, an extra point contact feature which may correspond to a second energy gap appeared in the spectrum. For a 16 quintuple layer Bi 2 Se 3 on NbSe 2 sample, the bulk state gap value near the top surface is ~159 μeV, while the second gap value is ~120 μeV at 40 mK. The second gap value decreased with increasing Bi 2 Se 3 layer thickness, but the ratio between the second gap and the bulk state gap remained about the same for different Bi 2 Se 3 thicknesses. It is plausible that this is due to superconductivity in Bi 2 Se 3 topological surface states induced through the bulk states. In conclusion, the two induced gaps in the PCS measurement are consistent with the three-dimensional bulk state and the two-dimensional surface state superconducting gaps observed in the angle-resolved photoemission spectroscopy (ARPES) measurement.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Low-temperature microstructural studies on superconducting CaFe2As2

Abstract Undoped CaFe 2 As 2 (Ca122) can be stabilized in two slightly different non-superconducting tetragonal phases, PI and PII, through thermal treatments. Upon proper annealing, superconductivity with a T c up to 25 K emerges in the samples with an admixture of PI and PII phases. Systematic low-temperature X-ray diffraction studies were conducted on undoped Ca122 samples annealed at 350 °C over different time periods. In addition to the diffraction peaks associated with the single-phase aggregation of PI and PII, a broad intermediate peak that shifts with annealing time was observed in the superconducting samples only. Our simulation of phase distribution suggests that the extra peak is associated with the admixture of PI and PII on the nanometer scale. High-resolution transmission electron microscopy confirms the existence of these nano-scale phase admixtures in the superconducting samples. These experimental results and simulation analyses lend further support for our conclusion that interfacial inducement is the most reasonable explanation for the emergence of superconductivity in undoped Ca122 single crystals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗