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DOE OSTI2025

Exciton dressing by extreme nonlinear magnons in a layered semiconductor

Collective excitations presenting nonlinear dynamics are fundamental phenomena with broad applications. A prime example is nonlinear optics, where diverse frequency mixing processes are central to communication, sensing, wavelength conversion, and attosecond physics. Leveraging recent progress in van der Waals magnetic semiconductors, we demonstrate nonlinear opto-magnonic coupling by presenting exciton states dressed by up to 20 harmonics of magnons, resulting from their nonlinearities, in the layered antiferromagnetic semiconductor CrSBr. We also create tunable optical side bands from sum- and difference-frequency generation between two optically bright magnon modes under symmetry breaking magnetic fields. Moreover, the observed difference-frequency generation mode can be continuously tuned into resonance with one of the fundamental magnons, resulting in parametric amplification of magnons. These findings realize the modulation of the optical frequency exciton with the extreme nonlinearity of magnons at microwave frequencies, which could find applications in magnonics and hybrid quantum systems, and provide new avenues for implementing opto-magnonic devices.

Diederich, Geoffrey M.↗

DOE OSTI2024

Broadband coplanar-waveguide-based impedance-transformed Josephson parametric amplifier

Quantum-limited Josephson parametric amplifiers play a pivotal role in advancing the field of circuit quantum electrodynamics by enabling the fast and high-fidelity measurement of weak microwave signals. Therefore, it is necessary to develop robust parametric amplifiers with low noise, broad bandwidth, and reduced design complexity for microwave detection. However, current broadband parametric amplifiers either have degraded noise performance or rely on complex designs. Here, we present a device based on the broadband impedance-transformed Josephson parametric amplifier that integrates a hornlike coplanar waveguide transmission line, which significantly decreases the design and fabrication complexity while keeping comparable performance. The device shows an instantaneous bandwidth of 700 (200) MHz for 15 (20) dB gain with an average input saturation power of − 110 dBm and near quantum-limited added noise. The operating frequency can be tuned over 1.4 GHz using an external flux bias. We further demonstrate the negligible backaction from our device on a transmon qubit. The amplification performance and simplicity of our device promise its wide adaptation in quantum metrology, quantum communication, and quantum information processing. Published by the American Physical Society 2024

Qing, Bingcheng (ORCID:0000000345227017)↗

DOE OSTI2025

KIPM Detector Characterization in QUIET

Kinetic Inductance Phonon‑Mediated (KIPM) detectors are superconducting microwave resonators on silicon that sense bursts of energy through tiny shifts in their resonance. In this work, we installed new devices in the QUIET facility's cryogenic test setup and used a network analyzer to drive them across a range of power levels. At each setting, we measured the transmitted signal and fit it to a simple notch‑filter model, allowing us to extract key performance metrics. And despite the increased noise at low power, our model consistently captured the resonance behavior. We observed that the resonant frequency stayed stable across most powers, the device s internal quality factor improved with stronger signals, and its coupling strength peaked mid‑range before leveling off. Overall, these findings confirm the detector s performance, laying groundwork for future work on energy calibration with pulsed optical sources.

Savitala, Akash [Washington U., Seattle; Fermilab]↗

DOE OSTI2026

Realization of a Quantum Slide Rule for 1+1 Dimensional Quantum Field Theories Using Josephson Superconducting Circuits

We have built a special type of electronic circuit—a “superconducting quantum simulator”—that allows us to mimic the behavior of complex quantum systems that are impossible to compute with ordinary computers. Our device is a long transmission line made of thousands of tiny superconducting junctions, acting as a one-dimensional “vacuum” for microwave photons. By terminating this line with a tunable, weak Josephson junction, we can control how strongly photons interact with each other.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2021

Electro-Optical Measurement Techniques

Utilize the unique characteristics of photons across different regions of the electromagnetic spectrum to probe the optical and electronic properties of chemical systems, materials and devices for energy conversion technologies.

absorption↗

DOE OSTI2020

Interplay between phonon downconversion efficiency, density of states at Fermi energy, and intrinsic energy resolution for microwave kinectic inductance detectors

Microwave Kinetic Inductance detectors (MKIDs) have been recognized as a powerful new tool for single photon detection. These highly multiplexed superconducting devices give timing and energy measurement for every detected photon. However, the full potential of MKID single photon spectroscopy has not been reached , the achieved energy resolution is lower than expected from first principles. Here, we study the efficiency in the phonon downconversion process following the absorption of energetic photons in MKIDs. Assuming previously published material properties, we measure an average downconversion efficiency for three TiN resonators is $\eta$=0.14. We discuss how this efficiency can impact the intrinsic energy resolution of MKID, and how any uncertainty in the unknown density of electron states at the Fermi energy directly affects the efficiency estimations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Multimode Characterization Approach for Understanding Cell-Level PV Performance and Degradation

Cell-level degradation processes impact the economic viability and large-scale deployment prospects for both established and emerging photovoltaic (PV) technologies. This project addresses the need to develop experimental and device-modeling approaches for studying cell-level degradation processes in photovoltaic (PV) devices using a variety of characterization techniques that provide access to complementary material and device properties. Our results demonstrate that by coupling characterization results with device modeling it is possible to develop comprehensive understanding of processes leading to performance limitations and degradation. This project developed a suite of novel measurement techniques including pulsed-light-bias operando X-ray and photoelectron spectroscopy (popXPS), light-biased scanning microwave impedance microscopy (sMIM), and near-field transport imaging (TI). In addition, operando characterization methodologies and in situ stressing capabilities have been developed and applied for techniques including electron-beam-induced current (EBIC), cathodoluminescence (CL), and Kelvin probe force microscopy (KPFM). Device-physics models were developed and applied to simulate correlative, multi-mode measurements to extract material and device parameters that control performance degradation. These characterization and modeling techniques were applied in a multi-mode approach to probe cell-level degradation mechanisms in Cd(Se,Te) and hybrid perovskite PV devices. Together these efforts contribute to foundational PV degradation science by establishing a framework for understanding PV performance degradation at the cell level and benefit the U.S. PV industry by providing resources in the form of novel experimental capabilities, knowledge gained, and available expertise that can accelerate research and development of improved PV device materials and architectures. The project provided a comprehensive understanding of degradation in baseline Cd(Se,Te) solar cells provided by our collaborators at Colorado State University (CSU). EBIC and CL-based measurements and revealed unusual collection and recombination profiles in these devices, which underwent significant changes with during stressing. KPFM and operando XPS measurements showed that device stressing permanently alters energy-band alignments at the (Mg,Zn)O/Cd(Se,Te) interface, which in turn account for an observed loss in fill factor. Studies on hybrid perovskite devices were hampered to a significant extent by delays related to the pandemic. Nevertheless, a set of hybrid perovskite devices (supplied through an NREL-industry partnership) were stress tested and characterized with techniques including EBIC, sMIM, popXPS/popUPS and optically excited TI. Available results from these measurements informed the device modeling effort and suggest that defects and related band offsets at the C60/LiF/hybrid perovskite interface are the primary source of degradation in these devices.

14 SOLAR ENERGY↗

DOE OSTI2026

Cryogenic growth of aluminum: Structural morphology, optical properties, superconductivity, and microwave dielectric loss

We explore the molecular beam epitaxy synthesis of superconducting aluminum thin films grown on c-plane sapphire substrates at cryogenic temperatures of 6 K and compare their behavior with films synthesized at room temperature. We demonstrate that cryogenic growth increases structural disorder, producing crystalline grains that modify the optical, electrical, and superconducting properties of aluminum. We observe that cryogenic deposition changes the color of aluminum from fully reflective to yellow and correlate the pseudodielectric function and reflectance with structural changes in the film. We find that smaller grain sizes enhance the superconductivity of aluminum, increasing its critical temperature and critical field. We then estimate the superconducting gap and coherence length of Cooper pairs in aluminum in the presence of disorder. In conclusion, we fabricate superconducting microwave resonators on these films and find that, independently of the growth temperature, the system is dominated by two-level system loss with similar quality factors in the high- and low-power regimes. We further measure a higher kinetic inductance in the cryogenically grown films.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Pushing the Boundaries of Coherence in Superconducting Quantum Systems at the SQMS Center for Computing, Sensing, and Metrology

This talk will highlight recent advances at the SQMS Center in understanding and mitigating decoherence in superconducting quantum systems, focusing on both transmon qubits and 3D superconducting cavities. I will present results from systematic studies of materials and devices, aimed at identifying key sources of loss: including two-level systems (TLS), quasiparticles, and other noise mechanisms. These studies span microwave loss characterization in materials such as niobium, tantalum, aluminum, and their native oxides, as well as substrate losses in silicon and sapphire. Using both qubits and cavities, we disentangle subsystem contributions to loss and develop a hierarchy of mitigation strategies. Through these efforts, we have achieved transmon coherence times exceeding one millisecond. I will also present investigations into quasiparticle dynamics, including bursts observed in qubits located above ground and in the Gran Sasso underground laboratory. Additional studies explore temperature dependence to distinguish between TLS and quasiparticle losses, and reveal that applying a magnetic field can reduce temporal T1 fluctuations in transmons. Building on these results, we demonstrate a record-coherence two-cell cavity-qudit system with coherence times exceeding 20 milliseconds. By leveraging sideband interactions and error-resilient protocols including measurement-based correction and post-selection, we achieve high-fidelity quantum state control. This includes preparation of Fock states up to N = 20 with fidelities over 95%, and two-mode entanglement with coherence-limited fidelities reaching 99.9% after post-selection. These achievements position the SQMS platform as a powerful foundation for scalable quantum information processing and high-dimensional qudit encodings. Finally, I will discuss how these ultra-coherent systems are being deployed in emerging quantum sensing applications, including dark matter searches and gravitational wave detection.

Roy, Tanay [Fermilab]↗

DOE OSTI2023

Precision Measurement of the Microwave Dielectric Loss of Sapphire in the Quantum Regime with Parts-per-Billion Sensitivity

Dielectric loss is known to limit state-of-the-art superconducting qubit lifetimes. Recent experiments imply upper bounds on bulk dielectric loss tangents on the order of 100 parts per billion but because these inferences are drawn from fully fabricated devices with many loss channels, these experiments do not definitely implicate or exonerate the dielectric. To resolve this ambiguity, we devise a measurement method capable of separating and resolving bulk dielectric loss with a sensitivity at the level of 5 ×10 –9 . The method, which we call the dielectric dipper, involves the in situ insertion of a dielectric sample into a high-quality microwave cavity mode. Smoothly varying the participation of the sample in the cavity mode enables a differential measurement of the dielectric loss tangent of the sample. The dielectric dipper can probe the low-power behavior of dielectrics at cryogenic temperatures and does so without the need for any lithographic process, enabling controlled comparisons of substrate materials and processing techniques. We demonstrate the method with measurements of sapphire grown by edge-defined film-fed growth (EFG) in comparison to high-grade sapphire grown by the heat-exchanger method (HEMEX). For EFG sapphire, we infer a bulk loss tangent of 63⁢(8) ×10 –9 and a substrate-air interface loss tangent of 15⁢(3) ×10 –4 (assuming a sample surface thickness of 3 nm). For a typical transmon, this bulk loss tangent would limit device quality factors to Q ≲20 ×10 6 , suggesting that bulk loss is likely the dominant loss mechanism in the longest-lived transmons on sapphire. We also demonstrate this method on HEMEX sapphire and bound its bulk loss tangent to be less than 19⁢(6) ×10 –9 . As this bound is about 3 times smaller than the bulk loss tangent of EFG sapphire, the use of HEMEX sapphire as a substrate would lift the bulk dielectric coherence limit of a typical transmon qubit to several milliseconds.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

KIPM Detector Characterization in QUIET

Kinetic Inductance Phonon‑Mediated (KIPM) detectors are superconducting microwave resonators that sense energy depositions in the substrate through a transient shift in their resonant frequency. In this work, I installed new devices in the QUIET cryogenic facility and used a network analyzer to drive them across a range of power levels. At each setting, I measured the transmitted signal and fit it to a simple notch‑filter model, allowing us to extract key performance metrics. Despite the increased noise at low power, the model consistently captured the resonance behavior. I first measured the resonance parameters as a function of RF drive power, then repeated the measurement across a range of temperatures to test whether the device behaved like an MKID. While the notch-filter fits captured the resonance reliably, the observed temperature dependence did not match the expected MKID signature — indicating that these first in-house fabricated chips are not yet functioning as true MKIDs. Overall, this reframes our work as a study of resonance parameter extraction and identification, pointing towards future iterations of device design and fabrication to get the true MKID response.

Savitala, Akash [U. Washington, Seattle (main); Fe↗

DOE OSTI2022

Predicting Solar Cell Performance from Terahertz and Microwave Spectroscopy

Abstract Mobilities and lifetimes of photogenerated charge carriers are core properties of photovoltaic materials and can both be characterized by contactless terahertz or microwave measurements. Here, the expertise from fifteen laboratories is combined to quantitatively model the current‐voltage characteristics of a solar cell from such measurements. To this end, the impact of measurement conditions, alternate interpretations, and experimental inter‐laboratory variations are discussed using a (Cs,FA,MA)Pb(I,Br) 3 halide perovskite thin‐film as a case study. At 1 sun equivalent excitation, neither transport nor recombination is significantly affected by exciton formation or trapping. Terahertz, microwave, and photoluminescence transients for the neat material yield consistent effective lifetimes implying a resistance‐free JV‐curve with a potential power conversion efficiency of 24.6 %. For grainsizes above ≈20 nm, intra‐grain charge transport is characterized by terahertz sum mobilities of ≈32 cm 2 V −1 s −1 . Drift‐diffusion simulations indicate that these intra‐grain mobilities can slightly reduce the fill factor of perovskite solar cells to 0.82, in accordance with the best‐realized devices in the literature. Beyond perovskites, this work can guide a highly predictive characterization of any emerging semiconductor for photovoltaic or photoelectrochemical energy conversion. A best practice for the interpretation of terahertz and microwave measurements on photovoltaic materials is presented.

14 SOLAR ENERGY↗

DOE OSTI2025

Electrolyte Immersion Increases Photoconductivity in a Model Polymer Photocathode

Immersing polymer solar cells in aqueous electrolyte for photoelectrochemical (PEC) hydrogen production is likely to cause photophysical changes that could present both challenges and opportunities for engineering functional and durable devices. Herein we study the bulk heterojunction blend poly(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-2,6-diyl)-alt-(2-(((2-ethylhexyl)oxy)carbonyl)-3-fluorothieno[3,4-b]thiophene-4,6-diyl):poly(N,N'-di(2-octyldodecyl)naphthalene-1,8:4,5-bis(dicarboximide)-2,6-diyl)-alt-(2,2-bithiophene-5,5'-diyl) (PTB7-Th:N2200) excited-state dynamics in electrolyte from femtosecond to millisecond time scales using pump-probe microwave conductivity and absorption spectroscopy. While the blend swells very little, electrolyte exposure increases the microwave-frequency mobility and possibly the yield of photogenerated charges while also decreasing crystallinity. These results indicate an enhancement in key performance metrics, implying that any limitations on the performance of PEC test devices do not arise from active layer-electrolyte interactions. For the PTB7-Th:N2200 blend or similar photocathode systems, our results indicate that improving the interfacial kinetics and/or the carrier lifetime should be prioritized, not protecting the active layer from the electrolyte. Since this observation may not be universal to all polymer systems, future research should focus on identifying their limiting photophysical processes. electrolyte.

14 SOLAR ENERGY↗

DOE OSTI2021

Facile microwave synthesis of zirconium metal-organic framework thin films on gold and silicon and application to sensor functionalization

Zirconium-based metal-organic frameworks, including UiO-66 and related frameworks, have become the focus of considerable research in the area of chemical warfare agent (CWA) decontamination. However, little work has been reported exploring these metal-organic frameworks (MOFs) for CWA sensing applications. For many sensing approaches, the growth of high-quality thin films of the active material is required, and thin film growth methods must be compatible with complex device architectures. Several approaches to synthesize thin films of UiO-66 have been described but many of these existing methods are complex or time consuming. In this work, we describe the development of a simple and rapid microwave assisted synthesis of oriented UiO-66 thin films on unmodified silicon (Si) and gold (Au) substrates. Thin films of UiO-66 and UiO-66-NH 2 can be grown in as little as 2 min on gold substrates and 30 min on Si substrates. The film morphology and orientation are characterized and the effects of reaction time and temperature on thin film growth on Au are investigated. Both reaction time and temperature impact the overgrowth of protruding discrete crystallites in the thin film layer but, surprisingly, no strong correlation is observed between film thickness and reaction time or temperature. We also briefly describe the synthesis of Zr/Ce solid solution thin films of UiO-66 on Au and report the first synthesis of a solid solution thin film MOF. Finally, we demonstrate the utility of the microwave method for the facile functionalization of two sensor architectures, plasmonic nanohole arrays and microresonators, with UiO-66 thin films.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Development of Quantum Interconnects (QuICs) for Next-Generation Information Technologies

Just as “classical” information technology rests on a foundation built of interconnected information-processing systems, quantum information technology (QIT) must do the same. A critical component of such systems is the “interconnect,” a device or process that allows transfer of information between disparate physical media, for example, semiconductor electronics, individual atoms, light pulses in optical fiber, or microwave fields. While interconnects have been well engineered for decades in the realm of classical information technology, quantum interconnects (QuICs) present special challenges, as they must allow the transfer of fragile quantum states between different physical parts or degrees of freedom of the system. The diversity of QIT platforms (superconducting, atomic, solid-state color center, optical, etc.) that will form a “quantum internet” poses additional challenges. As quantum systems scale to larger size, the quantum interconnect bottleneck is imminent, and is emerging as a grand challenge for QIT. For these reasons, it is the position of the community represented by participants of the NSF workshop on “Quantum Interconnects” that accelerating QuIC research is crucial for sustained development of a national quantum science and technology program. Given the diversity of QIT platforms, materials used, applications, and infrastructure required, a convergent research program including partnership between academia, industry, and national laboratories is required.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Trap-Filling Magnetoconductance as an Initialization and Readout Mechanism of Triplet Exciton Spins

Photoexcited triplet states are promising candidates for hybrid qubit systems, as they can be used as a controlling gate for nuclear spins. But microwave readout schemes do not generally offer the sensitivity needed to approach the single-molecule limit or the scope to integrate such systems into devices. In this report we demonstrate the possibility of electrical readout of triplet spins at room temperature through a specific mechanism of magnetoconductance (MC) in polycrystalline pentacene. We show that hole-only pentacene devices exhibit a positive photoinduced MC response that is consistent with a trap-filling mechanism. Spin and magnetic-field-dependent quenching of photogenerated triplets by holes quantitatively explains the MC response we observe. These results are distinct in both sign and proposed mechanism compared to previous reports on polyacene materials and provide clear design rules for future spintronic devices based on this spin-sensing mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Materials loss measurements using superconducting microwave resonators

The performance of superconducting circuits for quantum computing is limited by materials losses. In particular, coherence times are typically bounded by two-level system (TLS) losses at single photon powers and millikelvin temperatures. The identification of low loss fabrication techniques, materials, and thin film dielectrics is critical to achieving scalable architectures for superconducting quantum computing. Superconducting microwave resonators provide a convenient qubit proxy for assessing performance and studying TLS loss and other mechanisms relevant to superconducting circuits such as non-equilibrium quasiparticles and magnetic flux vortices. In this review article, we provide an overview of considerations for designing accurate resonator experiments to characterize loss, including applicable types of losses, cryogenic setup, device design, and methods for extracting material and interface losses, summarizing techniques that have been evolving for over two decades. Results from measurements of a wide variety of materials and processes are also summarized. Finally, we present recommendations for the reporting of loss data from superconducting microwave resonators to facilitate materials comparisons across the field.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Temperature-dependent anisotropic magnetoresistance and spin-torque-driven vortex dynamics in a single microdisk

Spin-orbit-torque-driven dynamics have recently gained interest in the field of magnetism due to the reduced requirement of current densities and an increase in efficiency, as well as the ease of implementation of different devices and materials. From a practical point of view, the low-frequency dynamics below 1GHz is particularly interesting since dynamics associated with magnetic domains lie in this frequency range. While spin-torque excitation of high-frequency modes has been extensively studied, the intermediate low-frequency dynamics have received less attention, although spin torques could potentially be used for both manipulation of the spin texture and the excitation of dynamics. In this paper, we demonstrate that it is possible to drive magnetic vortex dynamics in a single microdisk by spin-Hall torque at varying temperatures and relate the results to transport properties. We find that the gyrotropic mode of the core couples to the low-frequency microwave signal and produces a measurable voltage. The dynamic measurements are in agreement with magnetic transport measurements and are supported by micromagnetic simulations. Our results open the door for integrating magnetic vortex devices in spintronic applications.

36 MATERIALS SCIENCE↗