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Synthesis of Mg2IrH5: A potential pathway to high-Tc hydride superconductivity at ambient pressure

Following long-standing predictions associated with hydrogen, high-temperature superconductivity has recently been observed in several hydride-based materials. Nevertheless, these high-Tc phases only exist at extremely high pressures, and achieving high transition temperatures at ambient pressure remains a major challenge. Recent predictions of the complex hydride Mg2IrH6 may help overcome this challenge with calculations of high-Tc superconductivity (65K

High-temperature superconductors↗

Superconductivity in Ruddlesden–Popper nickelates: a review of recent progress, focusing on thin films

The discovery of superconductivity with Tc ∼ 80 K in the nickelate Ruddlesden-Popper bilayer La3Ni2O7 at high pressure has opened a new platform for unconventional superconductivity, followed by the subsequent observation of superconductivity in trilayer La4Ni3O10, also at high pressure. Remarkably, ambient-pressure superconductivity was also observed recently in La3Ni2O7 ultra-thin films when grown on substrates that provide compressive strain. This discovery significantly extends the type of experimental techniques that can be used in nickelates, previously limited due to the high-pressure constraint. Discussing the similarities and differences among these nickel oxides will provide new insights into understanding the mechanism of high-Tc superconductivity in correlated electron systems. In this paper, we review the experimental and theoretical progress on Ruddlesden–Popper nickelates, with emphasis on thin films, and discuss future perspectives and research directions.

Zhang, Yang [ORNL] (ORCID:0000000336235883)↗

Designing multicomponent hydrides with potential high T c superconductivity

While hydrogen-rich materials have been demonstrated to exhibit high T c 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$\overline{3}$ m RH 3 structures that exhibit strong hydrogen network connectivity, as defined through the electron localization function. The first class [RH 11 X 3 Y] is based on a Pm$\overline{3}$m structure showing moderately high T c , where the T c estimate from electronic properties is compared with direct Eliashberg calculations and found to be surprisingly accurate. The second class of structures [(RH 11 ) 2 X 6 YZ] improves on this with promisingly high density of states with dominant hydrogen character at the Fermi energy, typically enhancing T c . The third class [(R 1 H 11 )(R 2 H 11 )X 6 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 T c and the structural stability of complex hydrides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis and electronic characterization of Nd2−xSrxNiO4 thin films (0≤x≤1.4)

Layered nickelates have been studied extensively over the last three decades due to their structural similarities to the high-Tc superconducting cuprates. Using reactive oxide molecular beam epitaxy (MBE), we synthesize Nd2−xSrxNiO4 thin films for x=0−1.4 to probe the properties and electronic structure as a function of hole doping. The samples with lower doping show semiconducting behavior across the temperatures probed with an onset of metallic conductivity at x=1.4. We also present polarization-dependent O K and Ni L2,3 x-ray absorption spectra to track the evolution of the oxygen-nickel hybridization, distribution of holes between O 2p and Ni 3d states and the nickel oxidation state across the series. Angle-resolved photoemission spectroscopy (ARPES) measurements reveal a Fermi surface that comprises a cupratelike hole pocket of dx2−y2 character with an additional electron pocket of d3z2−r2 character at Γ. The emergence of a quasiparticle peak at the Fermi vector for x=1.4 corroborates the insulator-to-metal transition at x∼1. Finally, observe a fully two-dimensional Fermi surface with no momentum-dependent pseudogap, in contrast to measurements of the related bulk compound, Eu0.9Sr1.1NiO4.

Taylor, Nicole K↗

Wafer-Scale MgB 2 Superconducting Devices

Progress in superconducting device and detector technologies over the past decade has realized practical applications in quantum computers, detectors for far-infrared telescopes, and optical communications. Superconducting thin-film materials, however, have remained largely unchanged, with aluminum still being the material of choice for superconducting qubits and niobium compounds for high-frequency/high kinetic inductance devices. Magnesium diboride (MgB 2 ), known for its highest transition temperature (T c = 39 K) among metallic superconductors, is a viable material for elevated temperature and higher frequency superconducting devices moving toward THz frequencies. However, difficulty in synthesizing wafer-scale thin films has prevented implementation of MgB 2 devices into the application base of superconducting electronics. Here, we report ultrasmooth (<0.5 nm root-mean-square roughness) and uniform MgB 2 thin (<100 nm) films over 100 mm in diameter and present prototype devices fabricated with these films demonstrating key superconducting properties including an internal quality factor over 10 4 at 4.5 K and high tunable kinetic inductance in the order of tens of pH/sq in a 40 nm thick film. This advancement will enable development of elevated temperature, high-frequency superconducting quantum circuits, and devices.

Boron↗

A high-efficiency cryogenic neutron spin flipper for IMAGINE-X at the high flux isotope reactor

The Laue neutron macromolecular crystallography beamline, IMAGINE, at the High Flux Isotope Reactor (HFIR) is undergoing a major upgrade to incorporate the dynamic nuclear polarization (DNP) technique. Upon completion, the new IMAGINE-X instrument is expected to enhance the signal-to-noise ratio of the diffraction data by an order of magnitude. To take full advantage of the benefits of DNP, both a highly polarized neutron beam and a high-efficiency neutron spin flipper are required. We have developed a compact cryogenic spin flipper utilizing the Meissner effect in high-Tc yttrium–barium–copper–oxide superconducting films. The flipper has been successfully tested at two HFIR neutron development beamlines, Larmor and Poplar, with neutron wavelengths of 5.3 and 2.4 Å respectively. At Larmor, a flipping efficiency of 0.995 ± 0.004 was achieved for 5.3 Å neutrons, and at Poplar, efficiency of up to 0.9987 ± 0.0004 was obtained for 2.4 Å neutrons. Both tests demonstrated the flipper’s excellent performance and suitability for integration into IMAGINE-X.

Fu, Sichao [Oak Ridge National Laboratory (ORNL), ↗

Is Ba 3 In 2 O 6 a high- T c superconductor?

It has been suggested that Ba 3 In 2 O 6 might be a high-Tc superconductor. Experimental investigation of the properties of Ba 3 In 2 O 6 was long inhibited by its instability in air. Recently epitaxial Ba 3 In 2 O 6 with a protective capping layer was demonstrated, which finally allows its electronic characterization. The optical bandgap of Ba3In2O6 is determined to be 2.99 eV in-the (001) plane and 2.83 eV along the c-axis direction by spectroscopic ellipsometry. First-principles calculations were carried out, yielding a result in good agreement with the experimental value. Various dopants were explored to induce (super-)conductivity in this otherwise insulating material. Neither A- nor B-site doping proved successful. The underlying reason is predominately the formation of oxygen interstitials as revealed by scanning transmission electron microscopy and first-principles calculations. Additional efforts to induce superconductivity were investigated, including surface alkali doping, optical pumping, and hydrogen reduction. To probe liquid-ion gating, Ba 3 In 2 O 6 was successfully grown epitaxially on an epitaxial SrRuO 3 bottom electrode. So far none of these efforts induced superconductivity in Ba 3 In 2 O 6 , leaving the answer to the initial question of whether Ba 3 In 2 O 6 is a high-T c superconductor to be 'no' thus far.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The Quest for High-Temperature Superconductivity in Nickelates under Ambient Pressure

Recently, superconductivity with Tc ≈ 80 K was discovered in La3Ni2O7 under extreme hydrostatic pressure (>14 GPa). For practical applications, we needed to stabilize this state at ambient pressure. It was proposed that this could be accomplished by substituting La with Ba. To put this hypothesis to the test, we used the state-of-the-art atomic-layer-by-layer molecular beam epitaxy (ALL-MBE) technique to synthesize (La1−xBax)3Ni2O7 films, varying x and the distribution of La (lanthanum) and Ba (barium). Regrettably, none of the compositions we explored could be stabilized epitaxially; the targeted compounds decomposed immediately into a mixture of other phases. So, this path to high-temperature superconductivity in nickelates at ambient pressure does not seem promising.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tuning the Superconducting Transition Temperature of Co-sputtered Iridium and Platinum Films

A superconducting film with a tunable low transition temperature (Tc) is required in high-resolution Transition-Edge Sensor (TES) detectors, which have applications including dark matter detection, low threshold coherent elastic neutrino nucleus scattering measurement, and X-ray spectroscopy. We have been investigating a new approach to tune the Tc of superconducting thin films fabricated by co-sputtering Iridium and Platinum. The effects of Pt concentration and deposition parameters on the films' structural, electrical, and superconducting properties have been studied. AFM and XRD techniques and low temperature resistance measurements have been utilized for film characterization. By varying the Pt concentration and deposition parameters when co-sputtering, we have successfully achieved controllable tuning of Tc in the range of 30-200 mK. The experimental results demonstrate co-sputtering as a viable method for controlling the Tc of Ir-based thin films that can be applied to fabricating high-resolution TESs.

Yefremenko, V. G.↗

Noise limits for dc SQUID readout of high- Q resonators below 300 MHz

We present the limits on noise for the readout of cryogenic high-Q resonators using dc Superconducting Quantum Interference Devices (SQUIDs) below 300 MHz. This analysis uses realized first-stage SQUIDs (previously published), whose performance is well described by Tesche–Clarke (TC) theory, coupled directly to the resonators. We also present data from a prototype second-stage dc SQUID array designed to couple to this first-stage SQUID as a follow-on amplifier with high system bandwidth. This analysis is the first full consideration of dc SQUID noise performance referred to a high-Q resonator over this frequency range and is presented relative to the standard quantum limit. We include imprecision, backaction, and backaction–imprecision noise correlations from TC theory, the noise contributed by the second-stage SQUIDs, wiring, and preamplifiers, and optimizations for both on-resonance measurements and off-resonance scan sensitivity. This architecture has modern relevance due to the increased interest in axion searches and the requirements of the DMRadio-m 3 axion search, which uses dc SQUIDs in this frequency range.

Bosons↗

Coupling of Klein-Andreev resonant states in B⁢i 2 ⁢S⁢r 2 ⁢CaC⁢u 2 ⁢O 8+𝑥 -graphene-B⁢i 2⁢ S⁢r 2 ⁢CaC⁢u 2 ⁢O 8+𝑥 devices

Quantum devices require coherent coupling over macroscopic distances. Recently, resonances due to Klein tunneling and Andreev reflection states (KARS) have been observed in a naturally occurring p-n junction at the interface between B⁢i 2 ⁢S⁢r 2 ⁢CaC⁢u 2 ⁢O 8+𝑥 (BSCCO), a high−⁢𝑇 c superconductor (HTS), and graphene. The resonances appear as conductance oscillations with gating. Here, in this study, we show coupling between the KARS in BSCCO-graphene-BSCCO devices of varying separation (L). The coupling is evidenced by a power-law decay of resonance period as L increases from tens of nanometers to microns. These results demonstrate the long-distance coupling of KARS cavities in graphene-HTS junctions. The length dependence seen in experiments is supported by single-particle spectral functions which show KARS are coupled by transport modes in graphene. The strong coupling between KARS in BSCCO-graphene-BSCCO devices showcases the possibility of HTS-graphene junctions for quantum circuits and unconventional Josephson junctions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Pathway to tune sputter coated Nb$_3$Sn with Zr

Superconducting radio frequency (SRF) cavities are essential elements of many modern-day particle accelerators such as, European XFEL (DESY), LCLS II-HE (SLAC) and PIP II (Fermilab). Nb$_3$Sn superconducting material promises significant potential to exceed the performance of conventional niobium based SRF cavities. We aim to advance the ongoing R$&$D efforts to achieve Nb$_3$Sn coated cavities with high material quality. In this work, we have developed to achieve a route for effectively reducing the intrinsic defects in magnetron sputter coated Nb$_3$Sn SRF cavities and eventually improve the overall RF performance. We have observed that Zr is mainly being incorporated as ZrO$_2$ precipitates of average dimensions ranging from 20-100nm. By increasing the concentration of Zr, we have three major effects in the physical properties. Firstly, we noted that the density of the surface and bulk voids as well as their average dimensions are dramatically reduced on increasing the Zr content in Nb$_3$Sn. These surface voids are believed to be detrimental to cavity applications due to increase the local dissipation of electric and magnetic fields. These results indicate that inclusion of Zr in Nb$_3$Sn sputtered coating will improve the material quality and might help to reduce the overall RF power dissipation. Secondly, we observed that increasing Zr concentration from 0 to 2.4% substantially improves both superconducting transition temperature (Tc) and upper critical magnetic field (Hc2). However, on further increasing the Zr concentration to 24%, we noticed a small decrement in the Hc2 value. These results infer that the increase in Zr concentration up to an optimal concentration will be beneficial to enhance the superconducting properties. Increase in Tc promises lesser RF losses and improvement in accelerating gradient, whereas the increase in Hc2 suggests more efficient flux pinning which could give rise to high quality factors in presence of multi-Tesla magnetic field. Additionally, we also observed that increasing Zr concentration possibly prevents the oxygen diffusion and leads to thinner formation of primary surface oxide (Nb$_2$O$_5$ and SnO). This study gives a route to tune Zr fraction in Nb3Sn to modify the physical properties that control the high field performance of Nb3Sn RF cavities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Re-entrant unconventional superconductivity induced by rare-earth substitution in Nd 1-x Eu x NiO 2 thin films

High temperature superconductivity is typically associated with strong coupling and a large superconducting gap, yet these characteristics have not been demonstrated in the nickelates. Here, we provide experimental evidence that Eu substitution in the spacer layer of Nd 1-x Eu x NiO 2 (NENO) thin films enhances the superconducting gap, driving the system toward a strong-coupling regime. This is accompanied by a magnetic-exchange-driven magnetic-field-enhanced superconductivity. We investigate the upper critical magnetic field, H c2 , and the superconducting gap of superconducting NENO thin films with x = 0.2 to 0.35. Magnetoresistance measurements reveal magnetic-field-enhanced superconductivity in NENO films. We interpret this phenomenon as a result of an interaction between magnetic Eu ions and superconducting states in the Ni d x2-y2 orbital. The upper critical magnetic field strongly violates the weak-coupling Pauli limit. Infrared spectroscopy confirms a large gap-to-Tc ratio $2\Delta /{k}_{B}{T}_{{\rm{c}}}\simeq 5-6$, indicating a stronger coupling pairing mechanism in NENO relative to the Sr-doped NdNiO 2 . The substitution of Eu in the rare-earth layer causes pronounced modifications of the superconducting gap and magnetic interactions in Nd-based nickelates, opening new pathways to engineer high- T c superconductivity in infinite-layer nickelates.

36 MATERIALS SCIENCE↗

Radiatively cooled quantum microwave amplifiers

Superconducting microwave amplifiers are essential for sensitive signal readout in superconducting quantum processors. Typically based on Josephson junctions, these amplifiers require operation at milli-Kelvin temperatures to achieve quantum-limited performance. Here, we demonstrate a quantum microwave amplifier that employs radiative cooling to operate at elevated temperatures and maintain near quantum-limited added noise. This kinetic-inductance-based parametric amplifier, patterned from a single layer of relatively high-Tc NbN thin film, maintains a high gain and meanwhile enables low added noise of 1.3 quanta when operated at 1.5 K. Remarkably, this represents only a 0.2 quanta increase compared to the performance at a base temperature of 0.1 K. Based on our findings, we also discuss the practicality of such an operating scheme for various quantum applications. By uplifting the parametric amplifiers from the mixing chamber without compromising readout efficiency, this work represents an important step toward more scalable microwave quantum technologies.

Physics↗

Data Science Enabled Enabled Discovery of Superconductors (Final Progress Report)

This Final Technical Report describes efforts by 4 PIs at the University of Florida (Peter Hirschfeld, Richard Hennig, Greg Stewart and James Hamlin), over the period September 2019-August 2023, to use data science and machine learning techniques to discover new conventional superconductors. The PIs constructed a discovery loop with two theorists and two experimentalists to: develop algorithms to machine learn descriptors correlating strongly with the critical temperature Tc (PI's Peter Hirschfeld, UF Physics and Richard Hennig, UF Materials Science and En), synthesize and measure properties of promising materials, and feed back the knowledge gained into the prediction algorithm. This work was motivated by the theoretical prediction and experimental discovery of high-pressure, high-pressure hydride superconductors, and to find ways to recreate the high critical temperatures in these systems at ambient pressure. Highlights from the grant include: 1) a new equation for Tc in terms of moments of the electron-phonon spectral function, improving on the so-called Allen-Dynes equation (1975); 2) study of the metastable A15 superconductor Nb3Si, formed under explosive compression at ~1000GPa to determine the kinetic barrier to the ground state structure; 3) the development of ultra-fast machine-learned atomic potentials for molecular dynamics, and 4) the discovery of superconductivity at 19K in WB2 arising from metastable defect structures in the crystal.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Preparation and Characterization of YBa 2 Cu 4 O 8 Superconductor

Solid-state reaction of appropriate amounts of Y 2 O 3 , BaCOs, and CuO for 2 h at 800°C in flowing oxygen with a total pressure of 2.7 x 10 2 Pa (2 mm Hg), followed by cooling and annealing at 750°C for 10 h in oxygen at ambient pressure, has produced orthorhombic YBa 2 Cu 4 O 8 (124) as the main phase with YBa 2 Cu 3 O x (123) as an impurity phase. After the as-calcined powder was annealed in oxygen at 800°C for 24 h under ambient pressure, the phase purity improved considerably. Calcined 124 powder was pressed into pellets and rapidly annealed at temperatures from 870°C to 935°C. At these temperatures, the 124 decomposed into 123. The superconducting transition temperature, T c , of the annealed samples depended upon the annealing temperature and atmosphere. The decomposed samples have been characterized by low field RF SQUID magnetometer and high resolution transmission electron microscopy.

36 MATERIALS SCIENCE↗