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DOE OSTI2013

Inelastic Neutron Scattering Study of a Nonmagnetic Collapsed Tetragonal Phase in Nonsuperconducting CaFe2As2: Evidence of the Impact of Spin Fluctuations on Superconductivity in the Iron-Arsenide Compounds

The relationship between antiferromagnetic spin fluctuations and superconductivity has become a central topic of research in studies of superconductivity in the iron pnictides. We present unambiguous evidence of the absence of magnetic fluctuations in the nonsuperconducting collapsed tetragonal phase of CaFe2As2 via inelastic neutron scattering time-of-flight data, which is consistent with the view that spin fluctuations are a necessary ingredient for unconventional superconductivity in the iron pnictides. We demonstrate that the collapsed tetragonal phase of CaFe2As2 is nonmagnetic, and discuss this result in light of recent reports of high-temperature superconductivity in the collapsed tetragonal phase of closely related compounds.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Superconductivity Induced by Aging and Annealing in K{sub 1-{delta}}Cr{sub 3}As{sub 3}H{sub x}.

There has been a puzzling discrepancy on the physical property of quasi-one-dimensional Cr-based compound KCr3As3. While the polycrystalline KCr3As3 was originally reported to be nonsuperconducting with a spin-glass ground state, the single-crystalline KCr3As3 was later found to exhibit superconductivity at similar to 5 K. Here we demonstrate that both the polycrystals and single crystals can be made either nonsuperconducting or superconducting. The pristine samples show a spin-glass behavior only, and superconductivity below 5 K is actually induced by the post-aging and/or post-annealing. The result can be understood in terms of hydrogen intercalation into the one-dimensional Cr3As3 tubes, which was discovered very recently by K. M. Taddei et al. (arXiv:1905.03360). In addition, significant K deficiency and microscopic inhomogeneity have been revealed, suggesting a phase separation scenario with columnar superconductivity in K1-delta Cr3As3Hx. The possible processes of the hydrogen intercalation are given.

Xiang, Jin-Jin↗

DOE OSTI2024

Electronic Band Structure of a Superconducting Nickelate Probed by the Seebeck Coefficient in the Disordered Limit

Superconducting nickelates are a new family of strongly correlated electron materials with a phase diagram closely resembling that of superconducting cuprates. While analogy with the cuprates is natural, very little is known about the metallic state of the nickelates, making these comparisons difficult. We probe the electronic dispersion of thin-film superconducting five-layer ( n = 5 ) and metallic three-layer ( n = 3 ) nickelates by measuring the Seebeck coefficient S . We find a temperature-independent and negative S / T for both n = 5 and n = 3 nickelates. These results are in stark contrast to the strongly temperature-dependent S / T measured at similar electron filling in the cuprate La 1.36 Nd 0.4 Sr 0.24 CuO 4 . The electronic structure calculated from density-functional theory can reproduce the temperature dependence, sign, and amplitude of S / T in the nickelates using Boltzmann transport theory. This demonstrates that the electronic structure obtained from first-principles calculations provides a reliable description of the fermiology of superconducting nickelates and suggests that, despite indications of strong electronic correlations, there are well-defined quasiparticles in the metallic state. Finally, we explain the differences in the Seebeck coefficient between nickelates and cuprates as originating in strong dissimilarities in impurity concentrations. Our study demonstrates that the high elastic scattering limit of the Seebeck coefficient reflects only the underlying band structure of a metal, analogous to the high magnetic field limit of the Hall coefficient. This opens a new avenue for Seebeck measurements to probe the electronic band structures of relatively disordered quantum materials. Published by the American Physical Society 2024

Grissonnanche, G. (ORCID:0000000251153125)↗

DOE OSTI2021

Quench Protection Study of Superconducting Magnets for the Materials Plasma Exposure Experiment

To advance the understanding of plasma material interactions, the Material Plasma Exposure eXperiment (MPEX) is a new linear plasma device that will generate and deliver plasma relevant to future fusion reactor divertors. The operation of MPEX is planned to be steady-state in order to facilitate high fluence exposures of plasma facing materials and components. The desire for steady-state operation along with the magnetic field requires the utilization of superconducting coils. The superconducting magnet system for MPEX has been developed. The baseline model has six superconducting magnet and one room-temperature magnet subsystems. In order to protect multiple superconducting magnet systems, quench analysis was carried out to determine the best protection approach for each magnet type. Because the mutual inductance accounts for approximately 35% of the stored energy in the entire system, this must be considered when determining the peak voltages and temperatures during a quench. Two approaches for passive quench protection are considered: (1) self-protecting magnets and (2) use of diodes to sub-divide the coils. For both approaches, active quench detection will be used to ensure all coils are de-energized in the event of a quench. Results of the quench analysis for several quench scenarios are presented.

Burkhardt, Earle↗

DOE OSTI2016

Phase stability, electronic structures, and superconductivity properties of the BaPb 1 -x Bi x O 3 and Ba 1 -x K x BiO 3 perovskites

With extensive first-principles calculations, we investigate the phase stability,electronic structures, and superconductivity properties of the BaPb 1 -x Bi x O 3 (BPBO) and Ba 1 -x K x BiO 3 (BKBO) perovskites with the cubic (C), tetragonal (T), and orthorhombic (O) phases. Our calculations show that the tetragonal superconducting phases of both perovskites are metastable. However, the orthorhombicphase of the BPBO perovskite in the superconductivity region is only slightly more stable than the tetragonal phase. The small energy difference between the T and O phases and the discontinuous T-to-O phase transition account for the experimentally observed coexistence of the T and O phases. On the other hand, the BKBO perovskite involves a large energy difference between the T and O phases,which induces a low equilibrium temperature of the discontinuous T-to-O phase transition, in agreement with the experimental observation that the tetragonal BKBO is maintained down to low temperatures. Moreover, the electronic structures of both BPBO and BKBO superconductors show a flat band near the Fermi level, which is favorable for superconductivity. Furthermore, we find that the longer the total length of the flat band segment is, the higher the critical temperature of the BPBO or BKBO perovskite is. This key finding could be generalized straightforwardly to other unconventional superconductors and can be used to design and find optimal composition with maximum Tc for new unconventional superconductors.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Charged skyrmions and topological origin of superconductivity in magic-angle graphene

Topological solitons, a class of stable nonlinear excitations, appear in diverse domains as in the Skyrme model of nuclear forces. Here, we argue that similar excitations play an important role in a remarkable material obtained on stacking and twisting two sheets of graphene. Close to a magic twist angle, insulating behavior is observed, which gives way to superconductivity on doping. Here, we propose a unifying description of both observations. A symmetry breaking condensate leads to the ordered insulator, while topological solitons in the condensate—skyrmions—are shown to be charge 2 e bosons. Condensation of skyrmions leads to a superconductor, whose physical properties we calculate. More generally, we show how topological textures can mitigate Coulomb repulsion and provide a previously unexplored route to superconductivity. Our mechanism not only clarifies why several other moiré materials do not show superconductivity but also points to unexplored platforms where robust superconductivity is anticipated.

36 MATERIALS SCIENCE↗

DOE OSTI2025

High-field superconducting halo in UTe 2

The heavy fermion material UTe 2 is a candidate topological superconductor that exhibits multiple magnetic field–induced superconducting phases. One such phase exists only at fields greater than 40 tesla, a considerable scale given its critical temperature of only 2 K. Here, in this work, we extend measurements of this state with fields outside of the bc crystallographic plane and reveal its core structure: The superconducting phase wraps around the b axis in a halo-like fashion and appears to be stabilized by a field component perpendicular to the magnetic easy axis. This angle dependence points to a multicomponent spin-triplet order parameter with a finite angular momentum of the Cooper pairs. The pairing mechanism remains enigmatic, and UTe 2 ’s specific magnetophilic superconducting tendencies seem incompatible with existing models for field-enhanced superconductivity.

Lewin, Sylvia K. [National Inst. of Standards and ↗

DOE OSTI2017

Dependence of the maximal superconducting current on the resonance frequency in a shunted Josephson junction

We have analyzed the phase dynamics and current–voltage characteristics of a Josephson junction shunted by an LC circuit. When the Josephson frequency ω{sub J} becomes equal to the natural frequency ω{sub rc} of the formed resonance circuit, the I–V curve acquires additional branches. We have studied the features of the rc branch and the superconducting circuit for different values of the resonance frequency. It is shown that the maximal superconducting current through the Josephson junction on the rc-branch depends on the resonance frequency and is determined by the closeness of the end point of the rc branch to the critical current. We have determined the dependence of the maximal superconducting current on the resonance frequency for different values of the dissipation parameters. The limiting value of the maximal superconducting current is independent (to within 1%) of the parameters of the system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2013

Insights to Superconducting Radio-Frequency Cavity Processing from First Principles Calculations and Spectroscopic Techniques

Insights to the fundamental processes that occur during the manufacturing of niobium superconducting radio-frequency (SRF) cavities are provided via analyses of density functional theory calculations and Raman, infrared, and nuclear magnetic resonance (NMR) spectra. I show that during electropolishing fluorine is bound and released by the reaction of the acid components in the solution: HF + H 2 SO 4 <-> HFSO 3 + H 2 O. This result implies that new recipes can possibly be developed on the principle of controlled release of fluorine by a chemical reaction. I also show that NMR or Raman spectroscopy can be used to monitor the free fluorine when polishing with the standard electropolishing recipe. Density functional theory was applied to calculate the properties of common processing impurities – hydrogen, oxygen, nitrogen, and carbon – in the niobium. These impurities lower the superconducting transition temperature of niobium, and hydride precipitates are at best weakly superconducting. I modeled several of the niobium hydride phases relevant to SRF cavities, and explain the phase changes in the niobium hydrogen system based on the charge transfer between niobium and hydrogen and the strain field inside of the niobium. I also present evidence for a niobium lattice vacancy serving as a nucleation center for hydride phase formation. In considering the other chemical impurities in niobium, I show that the absorption of oxygen into a niobium lattice vacancy is preferred over the absorption of hydrogen, which indicates that oxygen can block these phase nucleation centers. I also show that dissolved oxygen atoms can trap dissolved hydrogen atoms to prevent niobium hydride phase formation. Nitrogen and carbon were studied in less depth, but behaved similarly to oxygen. Based on these results and a literature survey, I propose a mechanism for the success of the low-temperature anneal applied to niobium SRF cavities. Finally, I present the beginning of a model to describe magnetic impurities in niobium SRF cavities, which can cause a loss of local superconductivity. I calculated magnetic configurations of niobium hydrides and oxides, and show that stoichiometric hydride and oxide structures are nonmagnetic, but defective oxide structures retain local magnetic moments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Design and fabrication of a 30 T superconducting solenoid using overpressure processed Bi2212 round wire

High field superconducting magnets are used in particle colliders, fusion energy devices, and spectrometers for medical imaging and advanced materials research. Magnets capable of generating fields of 20-30 T are needed by future accelerator facilities. A 20-30 T magnet will require the use of high-temperature superconductors (HTS) and therefore the challenges of high field HTS magnet development need to be addressed. Superconducting Bi 2 Sr 2 CaCu 2 O x (Bi2212) conductors fabricated by the oxide-powder-in-tube (OPIT) technique have demonstrated the capability to carry large critical current density of 10 5 A/cm 2 at 4.2 K and in magnetic fields up to 45 T. Available in round wire multi-filamentary form, Bi2212 may allow fabrication of 20-50 T superconducting magnets. Until recently the performance of Bi2212 has been limited by challenges in realizing high current densities (J c ) in long lengths. This problem now is solved by the National High Magnetic Field Lab using an overpressure (OP) processing technique, which uses external pressure to process the conductor. OP processing also helps remove the ceramic leakage that results when Bi-2212 liquid leaks out from the sheath material and reacts with insulation, coil forms, and flanges. Significant advances have also been achieved in developing novel insulation materials (TiO 2 coating) and Ag-Al sheath materials that have higher mechanical strengths than Ag-0.2wt.% Mg, developing heat treatment approaches to broadening the maximum process temperature window, and developing high-strength, mechanical reinforced Bi-2212 cables. In the Phase I work, we leveraged these new opportunities to prototype overpressure processed solenoids and test them in background fields of up to 14 T. Additionally a design of a fully superconducting 30 T solenoid was produced. This work in conjunction with the future path outlined in the Phase II proposal would provide a major step toward qualifying Bi2212 technology for use in high-field accelerator magnets. Additionally, the performance parameters match key requirements of a final muon beam cooling solenoid. This technology will also be of interest to high-field NMR manufacturers.

43 PARTICLE ACCELERATORS↗

DOE OSTI2016

The Path to High Q-Factors in Superconducting Accelerating Cavities: Flux Expulsion and Surface Resistance Optimization

Accelerating cavities are devices resonating in the radio-frequency (RF) range used to accelerate charged particles in accelerators. Superconducting accelerating cavities are made out of niobium and operate at the liquid helium temperature. Even if superconducting, these resonating structures have some RF driven surface resistance that causes power dissipation. In order to decrease as much as possible the power losses, the cavity quality factor must be increased by decreasing the surface resistance. In this dissertation, the RF surface resistance is analyzed for a large variety of cavities made with different state-of-the-art surface treatments, with the goal of finding the surface treatment capable to return the highest Q-factor values in a cryomodule-like environment. This study analyzes not only the superconducting properties described by the BCS surface resistance, which is the contribution that takes into account dissipation due to quasi-particle excitations, but also the increasing of the surface resistance due to trapped flux. When cavities are cooled down below their critical temperature inside a cryomodule, there is always some remnant magnetic field that may be trapped increasing the global RF surface resistance. This thesis also analyzes how the fraction of external magnetic field, which is actually trapped in the cavity during the cooldown, can be minimized. This study is performed on an elliptical single-cell horizontally cooled cavity, resembling the geometry of cavities cooled in accelerator cryomodules. The horizontal cooldown study reveals that, as in case of the vertical cooldown, when the cooling is performed fast, large thermal gradients are created along the cavity helping magnetic flux expulsion. However, for this geometry the complete magnetic flux expulsion from the cavity equator is more difficult to achieve. This becomes even more challenging in presence of orthogonal magnetic field, that is easily trapped on top of the cavity equator causing temperature rising. The physics behind the magnetic flux expulsion is also analyzed, showing that during a fast cooldown the magnetic field structures, called vortices, tend to move in the same direction of the thermal gradient, from the Meissner state region to the mixed state region, minimizing the Gibbs free energy. On the other hand, during a slow cool down, not only the vortices movement is limited by the absence of thermal gradients, but, also, at the end of the superconducting transition, the magnetic field concentrates along randomly distributed normal-conducting region from which it cannot be expelled anymore. The systematic study of the surface resistance components performed for the different surface treatments, reveals that the BCS surface resistance and the trapped flux surface resistance have opposite trends as a function of the surface impurity content, defined by the mean free path. At medium field value, the BCS surface resistance is minimized for nitrogen-doped cavities and significantly larger for standard niobium cavities. On the other hand, Nitrogen-doped cavities show larger dissipation due to trapped flux. This is consequence of the bell-shaped trend of the trapped flux sensitivity as a function of the mean free path. Such experimental findings allow also a better understanding of the RF dissipation due to trapped flux. The best compromise between all the surface resistance components, taking into account the possibility of trapping some external magnetic field, is given by light nitrogen-doping treatments. However, the beneficial effects of the nitrogen-doping is completely lost when large amount of magnetic field is trapped during the cooldown, underlying the importance of both cooldown and magnetic field shielding optimization in high quality factors cryomodules.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Material and Interface Engineering Strategies to Mitigate Decoherence in Superconducting Qubits

While significant strides have been made to increase the coherence time of superconducting qubits, further advancements are essential for realizing scalable quantum computing. Decoherence is often a result of loss and noise stemming from two-level systems and excess quasiparticles, arising due to material defects, fabrication processes, and ambient exposure, particularly at surfaces and interfaces. Our recent efforts to mitigate these decoherence mechanisms have employed a variety of strategies, including low-loss surface encapsulation materials, advanced substrate preparation techniques, modifications to metal film growth, and the development of novel fabrication processes. The structural and chemical properties of materials, surfaces, and interfaces are studied using scanning probe microscopy, electron microscopy, photoelectron spectroscopy, mass spectrometry, and X-ray diffraction, which is correlated to device performance metrics, including superconducting resonator internal quality factor and qubit T1 time. This information is used to identify and understand material sources of loss and their origins in the device fabrication process. Through multi-institution efforts within SQMS we have identified the loss mechanism of interstitial hydrogen in niobium-based devices and shown how standard fabrication processes introduce these hydrides, developing strategies to mitigate their formation.1 Furthermore, we have characterized the metal-substrate interface, including the loss of niobium-silicides formed at that interface, and developed silicon surface treatments that reduce atomic scale roughness and oxygen content at the metal-substrate and Josephson junction interfaces.2-4 By developing the connection between materials properties and the overall performance of superconducting quantum circuitry, we can develop fabrication strategies to mitigate material losses, thus supporting the ongoing efforts to enhance coherence time in superconducting quantum devices. 1. Torres-Castanedo, C. G.*, Goronzy, D. P.*, et al., Adv. Funct. Mater., 2401365 (2024) 2. Lu, X., et al., Phys. Rev. Materials 6, 064402 (2022) 3. Berti, G., Appl. Phys. Lett. 122, 192605 (2023) 4. Kopas, C. J., Goronzy, D. P., et al., arXiv:2408.02863 (2024)

Goronzy, Dominic P.↗

DOE OSTI2026

Identifying Decoherence Mechanisms in Superconducting Qubits through Advanced Materials Characterization

Although superconducting qubits have emerged as a leading technology platform for quantum computing through large improvements in device coherence times and gate fidelity in recent years, the presence of defects and impurities at the interfaces and surfaces in the constituent materials continue to limit performance and serve as a critical barrier in achieving scalable quantum systems. Understanding and eliminating these sources of quantum decoherence in superconducting qubit devices requires dedicated studies aimed at establishing robust structure-property relationships that will enable researchers to target and eliminate defects strategically. As part of the Superconducting Materials and Systems (SQMS) center, we have extensively employed state-of-the-art materials characterization techniques, including scanning/transmission electron microscopy, secondary ion mass spectrometry, atom probe tomography, x-ray diffraction, and x-ray photoelectron spectroscopy in conjunction with device measurements to elucidate such relationships. In this talk, I will discuss some of our recent findings, including linking atomic defects to microwave loss in surface oxides, linking impurities in the Josephson Junction to qubit parameters, and linking low temperature precipitates to device performance. By applying these insights, we have been able to strategically develop and implement mitigation strategies for reliable fabrication of high coherence superconducting qubits.

Murthy, A. [Fermilab] (ORCID:0000000176776866)↗

DOE OSTI2026

Identifying Decoherence Mechanisms in Superconducting Qubits through Advanced Materials Characterization

Murthy, A. [Fermilab] (ORCID:0000000176776866)↗

DOE OSTI2026

A Cryogenic Muon Tagging System Integrated with a Superconducting Qubit Device for Radiation-Induced Error Mitigation

Superconducting qubits are highly sensitive to ionizing radiation, which can induce correlated errors and limit scalable fault-tolerant quantum computing. In particular, cosmic-ray muons can deposit energy in the substrate, generating phonon bursts that break Cooper pairs and produce quasiparticles, leading to correlated decoherence events across multiple qubits. We present the development of a cryogenic muon tagging system based on Kinetic Inductance Detectors (KIDs) and its integration with superconducting quantum hardware. Originally developed within the ACE-SuperQ project and validated as a standalone detector, the system demonstrated a muon tagging efficiency of approximately 90% and excellent agreement with Monte Carlo simulations. Building on this validation, the tagging system has been integrated with a multi-qubit superconducting chip operated in a dilution refrigerator. The detector configuration consists of a multi-layer KID stack arranged above and below the quantum device, enabling time-coincident identification of muon-induced events within the same cryogenic environment. The integrated setup has been successfully commissioned, enabling simultaneous operation of the qubit chip and the muon tagging system. A first measurement campaign has been carried out, and preliminary data show time-correlated events between the muon tagging detectors and the qubit readout. A quantitative analysis of radiation-induced effects on qubit performance is currently ongoing. This work represents a step toward the implementation of event-level radiation tagging as a tool for characterizing and potentially mitigating correlated errors in superconducting quantum processors, while establishing a modular platform for future studies at the interface between particle physics and quantum information science.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗

DOE OSTI2021

Superconducting Radio Frequency Resonators for Quantum Computing: A Short Review

Superconducting radiofrequency (SRF) technology is being used not only in discovery science programs and basic research but also for several applications that benefit society more directly. The advantage of superconducting resonators over those made of normal-conducting metal is their ability to store electromagnetic energy with much lower dissipation. The high-quality factor and longer dissipation time provided by these superconducting resonators can deliver superior performance. Currently, the quantum processing architecture uses resonators and interconnecting circuits operating in the microwave regime with superconducting strip-line technology and low noise electronic devices for switching and communication. The performance of these devices can be enhanced by embedding them in 3D SRF cavity resonators to prolong the coherence time, which improves the utility of the device by reducing error rates and allowing more manipulations (calculations) before the quantum state decays. Here, we present a short review of current microwave technology used in quantum computers and progress towards the 3D resonators to enhance thecoherence time.

Dhakal, Pashupati↗

DOE OSTI2021

Extremely Overdoped Superconducting Cuprates via High Pressure Oxygenation Methods

Within the cuprate constellation, one fixed star has been the superconducting dome in the quantum phase diagram of transition temperature vs. the excess charge on the Cu in the CuO2-planes, p, resulting from O-doping or cation substitution. However, a more extensive search of the literature shows that the loss of the superconductivity in favor of a normal Fermi liquid on the overdoped side should not be assumed. Many experimental results from cuprates prepared by high-pressure oxygenation show Tc converging to a fixed value or continuing to slowly increase past the upper limit of the dome of p = 0.26–0.27, up to the maximum amounts of excess oxygen corresponding to p values of 0.3 to > 0.6. These reports have been met with disinterest or disregard. Our review shows that dome-breaking trends for Tc are, in fact, the result of careful, accurate experimental work on a large number of compounds. This behavior most likely mandates a revision of the theoretical basis for high-temperature superconductivity. That excess O atoms located in specific, metastable sites in the crystal, attainable only with extreme O chemical activity under HPO conditions, cause such a radical extension of the superconductivity points to a much more substantial role for the lattice in terms of internal chemistry and bonding.

Sederholm, Linda (ORCID:0000000172090509)↗

NASA NTRS1972

Superconductivity in the alkali metal intercalates of molybdenum disulphide

The complete series of alkali metals, lithium through cesium, have been intercalated into molybdenum disulphide, using both the liquid ammonia and vapor techniques. All the intercalates with the exception of lithium yielded full superconducting transitions with onset temperatures of 6 K for AxMoS2(Ax=K,Rb,Cs) and 4 K for BxMoS2(Bx=Li,Na). The superconducting transition for lithium was incomplete down to 1.5 K. Stoichiometries and unit cell parameters have been determined for the intercalation compounds. Both rhombohedral and hexagonal polymorphs of MoS2 have been intercalated and found to exhibit the same superconductivity behavior. The nature of the extraneous superconducting transition of some intercalated samples on exposure to air was elucidated.

Somoano, R. B.↗