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DOE OSTI2023

SERAPH: Wavelike Dark Matter Searches with SRF Cavities

Haloscopes consisting of a microwave cavity with a high quality factor (Q) connected to low-noise electronics have been deployed to detect wavelike axions and dark photons. But the dark matter mass is unknown, so haloscopes must be tunable to search through the photon coupling vs. mass parameter space. Therefore, the scan rate for haloscope experiments is a crucial figure of merit and is proportional to the cavity’s quality factor. State-of-the-art experiments like ADMX currently use copper cavities with 𝑄∼80000. However, implementing superconducting cavities with 𝑄∼1010 can increase the instantaneous scan rate by possibly a factor of 105. This presentation will report progress on the SERAPH experiment, a family of superconducting haloscopes being developed by the Superconducting Quantum Materials and Systems (SQMS) Center. In this presentation, I will first discuss the principles behind operating a haloscope whose bandwidth is much narrower than the dark matter halo energy distribution. I will then describe the first SERAPH experiments implementing a 1.3 GHz Niobium cavity with an ultra-high quality factor (Q~1010) that has achieved the best sensitivity and deepest exclusion to wavelike dark photon dark matter by almost an order of magnitude. Next, I will discuss progress on the next phase of SERAPH, which will search dark photon dark matter using a widely-tunable SRF cavity (4-7 GHz). I will finally describe plans for subsequent SERAPH experiments to search for dark photons and axions with tunable SRF cavities tolerant to multi-Tesla magnetic fields and quantum sensors that subvert the Standard Quantum Limit.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

SERAPH: Wavelike Dark Matter Searches with SRF Cavities

Haloscopes consisting of a microwave cavity with a high quality factor (Q) connected to low-noise electronics have been deployed to detect wavelike axions and dark photons. But the dark matter mass is unknown, so haloscopes must be tunable to search through the photon coupling vs. mass parameter space. Therefore, the scan rate for haloscope experiments is a crucial figure of merit and is proportional to the cavity’s quality factor. State-of-the-art experiments like ADMX currently use copper cavities with 𝑄∼80000. However, implementing superconducting cavities with 𝑄∼1010 can increase the instantaneous scan rate by possibly a factor of 105.This presentation will report progress on the SERAPH experiment, a family of superconducting haloscopes being developed by the Superconducting Quantum Materials and Systems (SQMS) Center. In this presentation, I will first discuss the principles behind operating a haloscope whose bandwidth is much narrower than the dark matter halo energy distribution. I will then describe the first SERAPH experiments implementing a 1.3 GHz Niobium cavity with an ultra-high quality factor (Q~1010) that has achieved the best sensitivity and deepest exclusion to wavelike dark photon dark matter by almost an order of magnitude. Next, I will discuss progress on the next phase of SERAPH, which will search dark photon dark matter using a widely-tunable SRF cavity (4-7 GHz). I will finally describe plans for subsequent SERAPH experiments to search for dark photons and axions with tunable SRF cavities tolerant to multi-Tesla magnetic fields and quantum sensors that subvert the Standard Quantum Limit.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Probing magnetic configuration-mediated topological phases via high harmonic generation in MnBi 2 Te 4

Compared to a space group, a magnetic space group is much more complex, as both magnetic structure and magnetic moment direction can change the original symmetries of materials. The interplay between space symmetry and magnetism can generate versatile novel quantum states. However, detecting these topological phases experimentally, achieved through manipulating the magnetic configuration, has been restricted. It is mainly because the intrinsic link between the theory and the available experimental technique remains elusive. Here, we show that high harmonic generation (HHG) can identify these topological quantum states. In this work, we use rhombohedral MnBi 2 Te 4 film as an example, and analyze the symmetry-dependent harmonic order and signal by combining first-principles calculations and time-dependent Liouville equation numerical computations. Our results provide a fundamental basis for using HHG to study the topological quantum phases mediated by various magnetic configurations that can be easily realized by applying an external magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

NaCo 2 (SeO 3 ) 2 (OH): competing magnetic ground states of a new sawtooth structure with 3d 7 Co 2+ ions

While certain magnetic sublattices have long been known theoretically to give rise to emergent physics via competing magnetic interactions and quantum effects, finding such configurations in real materials is often deeply challenging. Here we report the synthesis and characterization of a new such material, NaCo 2 (SeO 3 ) 2 (OH) which crystallizes with a highly frustrated sublattice of sawtooth Co 2+ chains. Single crystals of NaCo 2 (SeO 3 ) 2 (OH) were synthesized using a low-temperature hydrothermal method. X-ray single crystal structure analysis reveals that the material crystallizes in orthorhombic space group of Pnma (no. 62). Its crystal structure exhibits one-dimensional chains of corner-sharing isosceles triangles that are made of two crystallographically distinct 3d 7 Co 2+ sites (Co(1) and Co(2)). The chains run along the b-axis and are interconnected via [SeO 3 ] groups to form a three-dimensional structure mediating super-exchange interactions. The temperature dependent magnetization data show a ferromagnetic-like (FM) transition at 11 K (T 1 ) followed by an antiferromagnetic (AFM) transition at about 6 K (T 2 ). Neutron-powder diffraction measurements reveal that at T 1 = 11 K only the Co(2) site orders magnetically, forming ferromagnetic zigzag chains along the b-axis. Below T 2 = 6 K, both Co(1) and Co(2) sites order in a nearly orthogonal configuration, with Co(1) moments lying inside the plane of the sawtooth chain while Co(2) moments cant out of the plane. The canting of the magnetic moments leads to a net ferromagnetic component along b-axis, parallel to the chain direction. The ordered moments are fully compensated in the ac-plane. Inelastic neutron scattering measurements reveal crystal field excitations that are consistent with the presence of a spin–orbital entangled pseudo-spin state J eff = 1/2 for the Co 2+ ions. Low-energy spin-wave excitations are observed below the second magnetic transition. The analysis of powder excitation spectrum suggests complex exchange interactions that go beyond a Heisenberg Hamiltonian model with nearest neighbor couplings. Our results demonstrate the richness of the magnetic properties of sawtooth-type structures and encourage the study of similar structures with different oxyanion groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Field-induced magnetic phases in a qubit Penrose quasicrystal

Unveiling the fundamental dynamics of naturally or artificially formed magnetic quasicrystals in the presence of an external magnetic field remains a difficult problem that may have implications for the design of information processing devices. By embedding a qubit magnetic Penrose quasicrystal into a quantum annealer, we were able to reproduce the formation of magnetic phases driven by specific physical parameter selections, allowing us to distinguish a wide range of frustrated magnetic configurations at the single-spin scale. In our experiments, we observe some spins dynamically activate, while others remain static, all within an average magnetization space defined by competing structural and magnetic degrees of freedom. Static spin structure factors reveal ferromagnetic and ferrimagnetic modulations that are compatible with a variety of spin textures. This research demonstrates that introducing structural aperiodicity in magnetic devices that exploit spin degeneracy in a single, richly intraconnected finite object can enable the engineering of quantum states in both the effective low-temperature and thermally excited regimes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Measurement of the muon anomalous precession frequency at the Muon g − 2 Experiment at Fermilab

The anomalous magnetic moment of the muon, $a_\mu = \frac{g-2}{2}$ is the fractional deviation of the muon $g$-factor from the value of 2. It emerges as the cumulative effect of the virtual particles participating in the muon interaction with a magnetic field via quantum loop corrections. Its value encodes all the possible interactions between the virtual particles and, for this reason, represents an important test of the Standard Model (SM). In particular, any deviation from the SM theoretical evaluation could be due to new physics contributions. The new Muon $g-2$ (E989) Experiment at Fermilab is currently operating to repeat and improve the previous E821 experiment at Brookhaven National Laboratory (BNL), aiming to reduce the experimental error by a factor of 4 to the final accuracy of 140 parts per billion (ppb). On April 7th, 2021, the E989 collaboration published the first result based on the first year of data taking (Run-1), measuring $a_\mu = 0.001~165~920~40(54)$ with a precision of 460 ppb. The measured value is consistent with the BNL measurement and strengthens the long-standing tension with the data-driven SM prediction to a combined discrepancy of 4.2$\sigma$. On the theory side, however, new efforts involving lattice-QCD techniques are starting to question the current consensus on the theoretical prediction, demanding new improvements on both the experimental and theoretical sides. The E989 collaboration is now finalizing the analysis of Run-2 and Run-3 data and a new publication is expected in the first half of 2023 with a combined statistical uncertainty of 200 ppb. The anomalous magnetic moment $a_\mu$ is measured as the ratio between the muon spin anomalous precession frequency, $\omega_a$, and the average magnetic field experienced by the muons as they circulate in the storage ring. This thesis presents a precession frequency analysis of the Run-1 data and an evaluation of the related systematic uncertainties. A new positron reconstruction developed for the analysis of the subsequent data-taking periods, aiming to reduce some of the major systematic uncertainties of the $\omega_a$ measurement, is presented. The author's involvement in the production of the Run-2/5 data and in the precise calibration of the detectors is discussed. Finally, the complete Run-1 $a_\mu$ result is presented.

43 PARTICLE ACCELERATORS↗

DOE OSTI2023

Integrating magnons for quantum information

Magnons, the quanta of collective spin excitations in magnetically ordered materials, have distinct properties that make them uniquely appealing for quantum information applications. They can have ultra-small wavelengths down to the nanometer scale even at microwave frequencies. Here, they can provide coupling to a diverse set of other quantum excitations, and their inherently gyrotropic dynamics forms the basis for pronounced nonreciprocities. In this article, we discuss what the current research challenges are for integrating magnetic materials into quantum information systems and provide a perspective on how to address them.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Magnetic impurities in Kondo insulators: An application to samarium hexaboride

Impurities and defects in Kondo insulators can have an unusual impact on dynamics that blends with effects of intrinsic electron correlations. Such crystal imperfections are difficult to avoid, and their consequences are incompletely understood. In this work, we study magnetic impurities in Kondo insulators via perturbation theory of the s-d Kondo impurity model adapted to small-band-gap insulators. The calculated magnetization and specific heat agree with recent thermodynamic measurements in samarium hexaboride (SmB 6 ). This qualitative agreement supports the physical picture of multichannel Kondo screening of local moments by electrons and holes involving both intrinsic and impurity bands. Specific heat is thermally activated in zero field by Kondo screening through subgap impurity bands and exhibits a characteristic upturn as the temperature is decreased. In contrast, magnetization obtains a dominant quantum correction from partial screening by virtual particle-hole pairs in intrinsic bands. We point out that magnetic impurities could impact de Haas–van Alphen quantum oscillations in SmB6, through the effects of Landau quantization in intrinsic bands on the Kondo screening of impurity moments.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Observation of Quantum Anomalous Hall Effect and Exchange Interaction in Topological Insulator/Antiferromagnet Heterostructure

Integration of a quantum anomalous Hall insulator with a magnetically ordered material provides an additional degree of freedom through which the resulting exotic quantum states can be controlled. Here, an experimental observation is reported of the quantum anomalous Hall e?ect in a magnet-ically-doped topological insulator grown on the antiferromagnetic insulator Cr?O?. The exchange coupling between the two materials is investigated using ?eld-cooling-dependent magnetometry and polarized neutron re?ec-tometry. Both techniques reveal strong interfacial interaction between the antiferromagnetic order of the Cr?O? and the magnetic topological insulator, manifested as an exchange bias when the sample is ?eld-cooled under an out-of-plane magnetic ?eld, and an exchange spring-like magnetic depth pro?le when the system is magnetized within the ?lm plane. These results identify antiferromagnetic insulators as suitable candidates for the manipula-tion of magnetic and topological order in topological insulator ?lms.

Pan, Lei↗

DOE OSTI2023

Magnetic ac susceptibility of superconducting Ta films for quantum computing

Recently, breakthroughs were reported in the long coherence time (>0.5 ms) transmon qubit using tantalum films (Ta). Identifying the loss mechanism in Ta films will help further improve the performance of Ta-based superconducting qubits. We report a study of superconducting properties in two sets of Ta films grown on c-cut and a-cut sapphires respectively using contact transport and noncontact magnetic ac susceptibility measurements. Although the resistive transition appears to be similar in both films, we found strikingly different responses in their complex magnetic susceptibilities χ' + iχ'$^{'}$ .χ'$^{'}$ in the c-cut films exhibits a sharp peak at superconducting transition Tc and becomes featureless below Tc indicating a strongly coupled superconducting state. In contrast, χ'$^{'}$ \ in the a-cut films exhibits a broad peak near Tc and a second peak appears below Tc, indicating granular superconductivity behavior. This second peak χ'$^{'}$ in is associated with the hysteresis loss at weak-link-type grain boundaries, which is believed to be a leading source of decoherence in the a-cut Ta films. The derived magnetic loss tangent in the a-cut films is about one order of magnitude higher than in the c-cut films. This study demonstrates that ac susceptibility is an excellent probe for characterizing bulk superconducting properties of the constituent superconducting materials used in qubits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1975

Role of magnetic fields in physics and astrophysics; Proceedings of the Conference, Copenhagen, Denmark, June 5-7, 1974

The papers deal with the role of magnetism in astrophysics and the properties of matter in the presence of unusually large magnetic fields. Topics include a quantum-mechanical treatment of high-energy charged particles radiating in a homogeneous magnetic field, the solution and properties of the Dirac equation for magnetic fields of any strength up to 10 to the 13th power gauss, experimental difficulties encountered and overcome in generating megagauss fields, the effect of strong radiation damping for an ultrarelativistic charge in an external electromagnetic field, magnetic susceptibilities of nuclei and elementary particles, and Compton scattering in strong external electromagnetic fields. Other papers examine static uniform electric and magnetic polarizabilities of the vacuum in arbitrarily strong magnetic fields, quantum-mechanical processes in neutron stars, basic ideas of mean-field magnetohydrodynamics, helical MHD turbulence, relations between cosmic and laboratory plasma physics, and insights into the nature of magnetism provided by relativity and cosmology. Individual items are announced in this issue.

Canuto, V.↗

DOE OSTI2026

Nanoscale Observation and Control of Quasiparticle Induced Magnetic Noise in a Superconducting Resonator

Superconducting circuits are arguably taking a leading role in driving the ongoing quantum technological revolution. A detailed knowledge of the microscopic fluctuating electromagnetic properties plays an important role in advancing the circuitry design, testing, and material integration of cutting-edge superconducting quantum electronics. Here, in this work, we report scanning nitrogen-vacancy (NV) quantum sensing of local magnetic noise environment of an on-chip superconducting resonator. We find that quasiparticle-induced fluctuating magnetic fields can drive NV spin relaxation, which shows a peak value around the superconducting transition point of niobium at the thermal equilibrium state. External microwave driving at the resonator mode frequency significantly increases the quasiparticle density, leading to enhancement of magnetic noise. We further perform optically detected magnetic resonance measurements to demonstrate quasiparticle magnetic noise mediated off-resonant dipole coupling between the NV center and niobium resonator. Our Letter reports experimental observation of the Hebel-Slichter peak signature by an external sensor outside of a superconductor. The presented study also highlights the advantages of quantum sensors in investigating miniaturized superconducting devices, providing insights into their future performance improvements.

Li, Senlei [Georgia Institute of Technology]↗

DOE OSTI2026

In Crystallo Synthesis of a Triplet Silver Nitrene

Reactive silver nitrenes are proposed intermediates in Ag-catalyzed C–H amination and olefin aziridination reactions. Synthesis and characterization of reactive Ag nitrenes has proven elusive due to fleeting lifetimes and argentophilic aggregation of Ag(I) precursors in solution. Here, we report the templated in crystallo synthesis and characterization of a mononuclear Ag nitrene supported by a tris(pyrazolyl)borate ligand. Photolytic N 2 elimination from the corresponding aryl azide complex yields a structurally defined Ag nitrene with a triplet ground state, as confirmed by crystallography, magnetic measurements, and quantum chemical calculations. This species displays both stoichiometric and catalytic nitrene transfer reactivity, enabling carbazole and indole formation from organic azides. These results leverage in crystallo templating to isolate a mononuclear triplet nitrene of Ag and provide a platform to experimentally elucidate ligand-controlled selectivity in Ag-catalyzed nitrene transfer catalysis.

Azides↗

DOE OSTI2022

Theory of the Kitaev model in a [111] magnetic field

Recent numerical studies indicate that the antiferromagnetic Kitaev honeycomb lattice model undergoes a magnetic-field-induced quantum phase transition into a new spin-liquid phase. This intermediate-field phase has been previously characterized as a gapless spin liquid. By implementing a recently developed variational approach based on the exact fractionalized excitations of the zero-field model, we demonstrate that the field-induced spin liquid is gapped and belongs to Kitaev’s 16-fold way. Specifically, the low-field non-Abelian liquid with Chern number C = ±1 transitions into an Abelian liquid with C = ±4. The critical field and the field-dependent behaviors of key physical quantities are in good quantitative agreement with published numerical results. Furthermore, we derive an effective field theory for the field-induced critical point which readily explains the ostensibly gapless nature of the intermediate-field spin liquid.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

Iron pnictides and chalcogenides: a new paradigm for superconductivity

Superconductivity is a remarkably widespread phenomenon observed in most metals cooled down to very low temperatures. The ubiquity of such conventional superconductors, and the wide range of associated critical temperatures, is readily understood in terms of the celebrated Bardeen Cooper-Schrieffer (BCS) theory. Occasionally, however, unconventional superconductors are found, such as the iron-based materials, which extend and defy this understanding in new and unexpected ways. In the case of the iron-based superconductors, this includes a new appreciation of the ways in which the presence of multiple atomic orbitals can manifest in unconventional superconductivity, giving rise to a rich landscape of gap structures that share the same dominant pairing mechanism. Besides superconductivity, these materials have also led to new insights into the unusual metallic state governed by the Hund’s interaction, the control and mechanisms of electronic nematicity, the impact of magnetic fluctuations and quantum criticality, and the significance of topology in correlated states. Furthermore, over the thirteen years since their discovery, they have proven to be an incredibly fruitful testing ground for the development of new experimental tools and theoretical approaches, both of which have extensively influenced the wider field of quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

6⁢𝐻-perovskite dimer lattice with antiferromagnetic interactions: Ba 3⁢ Zn 1−𝑥⁢ Ca 𝑥 ⁢Ru 2 ⁢O 9

Here, we investigate the magnetic behavior of the 6⁢𝐻-perovskite dimer lattice Ba 3 ⁢Zn 1−𝑥 ⁢Ca 𝑥 ⁢Ru 2 ⁢O 9 using analytical theory, density functional theory, inelastic neutron scattering, and modeling of historical magnetization and neutron-scattering data. A dimer mean-field theory built upon classical Luttinger–Tisza analysis generates a phase diagram revealing a transition from a nonmagnetic singlet to a finite-moment ground state as interdimer couplings increase. A (generalized) linear spin-wave theory captures multiplet mixing, excitation gap closing, and fluctuation-induced moment suppression. Density-functional-theory calculations on selected compounds, together with neutron spectroscopy of dilute Ba 3 ⁢Zn⁢(Ru 1−𝑥 ⁢Sb 𝑥 ) 2 ⁢O 9 , confirm the exchange hierarchy, enabling quantification of previously published experiments within this framework. Our results identify three mechanisms for magnetic moment suppression—quantum fluctuations, ligand hybridization, and nonmagnetic-singlet/magnetic-multiplet mixing.

Pajerowski, Daniel M. [Oak Ridge National Laborato↗

DOE OSTI2020

Energy spectrum and current-phase relation of a nanowire Josephson junction close to the topological transition

A semiconducting nanowire proximitized by an $\textit{s}$-wave superconductor can be tuned into a topological state by an applied magnetic field. This quantum phase transition is marked by the emergence of Majorana zero modes at the ends of the wire. The fusion of Majorana modes at a junction between two nanowires results in a 4π-periodic Josephson effect. Here, we elucidate how the 4π periodicity arises across the topological phase transition in a highly-transparent short nanowire junction. Owing to a high transmission coefficient, Majorana zero modes coming from different wires are strongly coupled, with an energy scale set by the proximity-induced, field-independent pairing potential. At the same time, the topological spectral gap—defined by competition between superconducting correlations and Zeeman splitting—becomes narrow in the vicinity of the transition point. The resulting hybridization of the fused Majorana states with the spectral continuum strongly affects the electron density of states at the junction and its Josephson energy. We study the manifestations of this hybridization in the energy spectrum and phase dependence of the Josephson current. We pinpoint the experimentally observable signatures of the topological phase transition, focusing on junctions with weak backscattering.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Anisotropic hybridization in CeRhSn

The optical conductivity σ⁡(ω, T) of CeRhSn was studied by broadband infrared spectroscopy. Temperature-dependent spectral weight transfer occurs over high energy (0.8 eV) and temperature (~500 K) scales, classifying CeRhSn as a mixed-valent compound. The optical conductivity reveals a substantial anisotropy in the electronic structure. Renormalization of σ⁡(ω, T) occurs as a function of temperature to a coherent Kondo state with concomitant effective mass generation. Associated spectroscopic signatures were reproduced remarkably well by the combination of density functional theory and dynamical mean-field theory using a momentum-independent self-energy. The theory shows that the anisotropy for energies > 10 meV is mainly driven by the bare three-dimensional electronic structure that is renormalized by local electronic correlations. The possible influence of magnetic frustration and quantum criticality is restricted to lower energies.

36 MATERIALS SCIENCE↗