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Fe-based superconductors exhibit a diverse interplay between charge, orbital, and magnetic ordering. Variations in atomic geometry affect electron hopping between Fe atoms and the Fermi surface topology, influencing magnetic frustration and the pairing strength through changes of orbital overlap and occupancies. Here, we experimentally demonstrate a systematic approach to realize superconductivity without chemical doping in BaFe2As2, employing geometric design within an epitaxial heterostructure. We control both tetragonality and orthorhombicity in BaFe2As2 through superlattice engineering, which we experimentally find to induce superconductivity when the As-Fe-As bond angle approaches that in a regular tetrahedron. This approach to superlattice design could lead to insights into low-dimensional superconductivity in Fe-based superconductors.
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Atomic layer controlled growth of epitaxial thin films of unconventional superconductors opens the opportunity to discover novel high temperature superconductors. For instance, the interfacial atomic configurations may play an important role in superconducting behavior of monolayer FeSe on SrTiO3 and other Fe-based superconducting thin films. Here, we demonstrate a selective control of the atomic configurations in Co-doped BaFe2As2 epitaxial thin films and its strong influence on superconducting transition temperatures by manipulating surface termination of (001) SrTiO3 substrates. In a combination of first-principles calculations and high-resolution scanning transmission electron microscopy imaging, we show that Co-doped BaFe2As2 on TiO2-terminated SrTiO3 is a tetragonal structure with an atomically sharp interface and with an initial Ba layer. In contrast, Co-doped BaFe2As2 on SrO-terminated SrTiO3 has a monoclinic distortion and a BaFeO3- x initial layer. Furthermore, the superconducting transition temperature of Co-doped BaFe2As2 ultrathin films on TiO2-terminated SrTiO3 is significantly higher than that on SrO-terminated SrTiO3, which we attribute to shaper interfaces with no lattice distortions. This study allows the design of the interfacial atomic configurations and the effects of the interface on superconductivity in Fe-based superconductors.
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Bi2Sr2CaCu2Ox (Bi-2212) conductor is the only high temperature superconductor manufactured as a round wire and is a very promising conductor for very high field applications. One of the key design parameters of Bi-2212 wire is its filament size, which has been previously reported to affect the critical current density (Jc ) and ac losses. Work with 1 bar heat treatment showed that the optimal filament diameter was about 15 µm but it was not well understood at that time that gas bubbles were the main current limiting mechanism. Here we investigated a recent Bi-2212 wire with a 121×18 filament architecture with varying wire diameter (1.0 to 1.5 mm) using 50 bar overpressure processing. This wire is part of a 1.2 km piece length of 1.0 mm diameter made by Oxford Superconducting Technology. We found that Jc is independent of the filament size in the range from 9 to 14 µm, although the n value increased with increasing filament size. A new record Jc (4.2 K, 15 T) of 4200 A/mm2 and JE (4.2 K, 15 T) of 830 A/mm2 were achieved.
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We obtain the through-thickness elastic stiffness coefficient (C33) in nominal 9 nm and 60 nm BaFe2As2 (Ba-122) thin films by using picosecond ultrasonics. Particularly, we reveal the increase in elastic stiffness as film thickness decreases from bulk value down to 9 nm, which we attribute to the increase in intrinsic strain near the film-substrate interface. Our density functional theory (DFT) calculations reproduce the observed acoustic oscillation frequencies well. In addition, temperature dependence of longitudinal acoustic (LA) phonon mode frequency for 9 nm Ba-122 thin film is reported. The frequency change is attributed to the change in Ba-122 orthorhombicity (a-b)/(a+b). This conclusion can be corroborated by our previous ultrafast ellipticity measurements in 9 nm Ba-122 thin film, which exhibit strong temperature dependence and indicate the structural phase transition temperature Ts.
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Fe-based superconductors and in particular K-doped BaFe2As2 (K-Ba122) are materials of interest for possible future high-field applications. However the critical current density (Jc) in polycrystalline Ba122 is still quite low and connectivity issues are suspected to be responsible. In this work we investigated the properties of high-purity, carefully processed, K-Ba122 samples synthesized with two separate heat treatments at various temperatures between 600 and 825 °C. We performed specific heat characterization and Tc-distribution analysis up to 16 T and we compared them with magnetic Tc and Jc characterizations, and transmission-electron-microscopy (TEM) microstructures. We found no direct correlation between the magnetic Tc and Jc, whereas the specific heat Tc-distributions did provide valuable insights. In fact the best Jc-performing sample, heat treated first at 750 °C and then at 600 °C, has the peak of the Tc-distributions at the highest temperatures and the least field sensitivity, thus maximizing Hc2. We also observed that the magnetic Tc onset was always significantly lower than the specific heat Tc: although we partially ascribe the lower magnetization Tc to the small grain size (< λ, the penetration depth) of the K-Ba122 phase, this behaviour also implies the presence of some grain-boundary barriers to current flow. Comparing the Tc-distribution with Jc, our systematic synthesis study reveals that increasing the first heat treatment above 750 °C or the second one above 600 °C significantly compromises the connectivity and suppresses the vortex pinning properties. We conclude that high-purity precursors and clean processing are not yet enough to overcome all Jc limitations. However, our study suggests that a higher temperature Tc-distribution, a larger Hc2 and a better connectivity could be achieved by lowering the second heat treatment temperature below 600 °C thus enhancing, as a consequence, Jc.
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Superconducting joints are one of the key components needed to make Ag-alloy clad Bi2Sr2CaCu2O8+x (Bi-2212) superconducting round wire (RW) successful for high-field, high-homogeneity magnet applications, especially for nuclear magnetic resonance (NMR) magnets in which persistent current mode (PCM) operation is highly desired. In this study, a procedure for fabricating superconducting joints between Bi-2212 round wires during coil reaction was developed. Melting temperatures of Bi-2212 powder with different amounts of Ag addition were investigated by differential thermal analysis (DTA) so as to provide information for selecting the proper joint matrix. Test joints of 1.3 mm dia. wires heat treated in 1 bar flowing oxygen using the typical partial melt Bi-2212 heat treatment (HT) had transport critical currents I c of ~900 A at 4.2 K and self-field, decreasing to ~480 A at 14 T evaluated at 0.1 µV/cm at 4.2 K. Compared to the I c of the open-ended short conductor samples with identical 1 bar HT, the I c values of the superconducting joint are ~20% smaller than that of conductor samples measured in parallel field but ~20% larger than conductor samples measured in perpendicular field. Microstructures examined by scanning electron microscopy (SEM) clearly showed the formation of a superconducting Bi-2212 interface between the two Bi-2212 round wires. Furthermore, a Bi-2212 RW closed-loop solenoid with a superconducting joint heat treated in 1 bar flowing oxygen showed an estimated joint resistance below 5×10-12 Ω based on its field decay rate. This value is sufficiently low to demonstrate the potential for persistent operation of large inductance Bi-2212 coils.
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Fabrication of epitaxial FeSexTe1-x thin films using pulsed laser deposition (PLD) enables improving their superconducting transition temperature (T c) by more than ~40% than their bulk T c. Intriguingly, T c enhancement in FeSexTe1-x thin films has been observed on various substrates and with different Se content, x. To date, various mechanisms for T c enhancement have been reported, but they remain controversial in universally explaining the T c improvement in the FeSexTe1-x films. In this report, we demonstrate that the controversies over the mechanism of T c enhancement are due to the abnormal changes in the chalcogen ratio (Se:Te) during the film growth and that the previously reported T c enhancement in FeSe0.5Te0.5 thin films is caused by a remarkable increase of Se content. Although our FeSexTe1-x thin films were fabricated via PLD using a Fe0.94Se0.45Te0.55 target, the precisely measured composition indicates a Se-rich FeSexTe1-x (0.6 < x < 0.8) as ascertained through accurate compositional analysis by both wavelength dispersive spectroscopy (WDS) and Rutherford backscattering spectrometry (RBS). We suggest that the origin of the abnormal composition change is the difference in the thermodynamic properties of ternary FeSexTe1-x, based on first principle calculations.
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Fe-As based superconductors provide a good system for understanding the relationship between magnetism and superconductivity. Considerable efforts have been expended in understanding the magnetic behavior of the parent compound, BaFe2As2. However, it had not been realized that traces of adsorbed O2 by the material bring about drastic changes in its magnetic behavior. O2 is known to trap electrons, forming O2(-). Guided by this discovery, we observe in the absence of O2 a dynamic transition between intermediate and low spin states of Fe and hysteresis effects, and in the presence of O2 trapping of the magnetic state. These observations are likely to have a bearing on the role of magnetism in superconductivity.
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Mössbauer studies of cobalt- and nickel-doped BaFe(2)As(2) show that the s-electron density at the (57)Fe nuclei, as measured by the isomer shift, is the same as that for the parent BaFe(2)As(2). Apparently, the electron population of the d shell, which shields the s-electron density at the nuclei, remains unchanged. We invoke the involvement of p-orbital hybridization with the d orbital in Fe-As bonding. Furthermore, the shrinkage of the lattice on substitution enhances the As-As sp hybridization, providing a path for the migration of additional electrons. The proposed mechanism is consistent with Hall coefficient and thermoelectric effect measurements.