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At least 91 records · Page 5

Quasiparticle spectroscopy in tantalum films with different Ta/sapphire interfaces

One of the crucial aspects of current research in quantum information science is the identification and control of loss mechanisms in superconducting (SC) circuits. Although microwave measurements directly quantify device performance, additional techniques that probe quasiparticle excitations in SC films are needed to understand the microscopic mechanisms underlying dissipation and decoherence. Here, we present results from quasiparticle spectroscopy of Ta/sapphire films by measuring the Meissner-state magnetic susceptibility using a precision frequency-domain resonator specifically designed for thin films. We find direct evidence for additional low-energy excitations in samples with lower internal quality factors. These excitations are consistent with deep subgap states due to two-level systems, Yu–Shiba–Rusinov states near the gap edge, and perhaps other pair-breaking mechanisms. The developed non-destructive frequency-domain quasiparticle spectroscopy is a valuable addition to the quantum materials toolbox.

metal/substrate interlayer↗

Universal signal scaling in microwave impedance microscopy

Microwave impedance microscopy (MIM) is an emerging scanning probe technique that measures the local complex dielectric function using near-field microwave. Although it has made significant impacts in diverse fields, a systematic, quantitative understanding of the signal's dependence on various important design parameters is lacking. Here, we show that for a wide range of MIM implementations, given a complex tip-sample admittance change ΔΥ, the MIM signal—the amplified change in the reflected microwave amplitude—is –G · ΔΥ/2Υ 0 · η 2 · V in , where η is the ratio of the microwave voltage at the probe to the incident microwave amplitude, Y o is the system admittance, and G is the total voltage gain. For linear circuits, η is determined by the circuit design and does not depend on V in . We show that the maximum achievable signal for different designs scales with η 2 or η when limited by input power or sample perturbation, respectively. Furthermore, this universal scaling provides guidance on diverse design goals, including maximizing narrow-band signal for imaging and balancing bandwidth and signal strength for spectroscopy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Microwave-photonic control of optically accessible spin defects in diamond

A growing variety of optically accessible spin qubits have emerged in recent years as key components for quantum sensors, computers, and memories. However, the scalability of conventional spin-based quantum architectures remains limited by direct microwave delivery, which introduces thermal noise, electromagnetic crosstalk, and design constraints for cryogenic, high-field, and distributed systems. In this work, we present a unified framework for RF-over-fiber (RFoF) control of spins accessible through optically detected magnetic resonance (ODMR) spectroscopy of nitrogen-vacancy (NV) centers in diamond. The RFoF platform relies on an intensity-modulated 1310 nm laser carrying microwave signals over fiber and a high-speed photodiode for optical-to-electrical conversion to drive NV spin transitions. We report an RFoF power-conversion efficiency of 3.42% for an RF output PRF,out=-5.5 dBm at 2.87 GHz, enabling clear resolution of Zeeman splitting in

Rahman, M Reefaz [ORNL] (ORCID:0000000323541611)↗

Stimulated Rayleigh Scattering Enhanced by a Longitudinal Plasma Mode in a Periodically Driven Dirac Semimetal Cd 3 As 2

Using broadband (12–45 THz) multi-terahertz spectroscopy, we show that stimulated Rayleigh scattering dominates the transient optical conductivity of cadmium arsenide, a Dirac semimetal, under an optical driving field at 30 THz. Here, the characteristic dispersive line shape with net optical gain is accounted for by optical transitions between light-induced Floquet subbands, strikingly enhanced by the longitudinal plasma mode. Stimulated Rayleigh scattering with an unprecedentedly large refractive index change may pave the way for slow light generation in conductive solids at room temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Microwave-Assisted Production of Polycarbonate Diols using Carbon Dioxide

Carbon dioxide (CO2) is a cheap and readily available resource that can be converted to value-added chemicals including fuels, polymers, and other products. One lucrative option is polycarbonate diols, which are the precursor to polyurethanes that find wide applications in automotive and aerospace industries. The traditional process for the synthesis of polycarbonate diols involves using hazardous phosgene and alcohols in a strongly basic medium that generates significant amounts of salt. Alternately, CO2 can be reacted with alkanediols over CeO2 catalysts to produce polycarbonate diols. For the current work, a microwave-assisted atmospheric flow system was investigated for converting CO2 into polycarbonate diols and was compared against a thermal system. Various parameters such as type and ratio of solvents, and the addition of dehydrating agents for the microwave system was tested. The different CeO2 catalysts used were characterized using Brunauer–Emmett–Teller (BET) surface area analysis, Raman spectroscopy, X-ray diffraction, and temperature programmed desorption (NH3-TPD and CO2-TPD).

CO2 utilization↗

Mitigating coherent loss in superconducting circuits using molecular self-assembled monolayers

In planar superconducting circuits, decoherence due to materials imperfections, especially two-level-system (TLS) defects at different interfaces, is a primary hurdle for advancing quantum computing and sensing applications. Traditional methods for mitigating TLS loss, such as etching oxide layers at metal and substrate interfaces, have proven to be inadequate due to the persistent challenge of oxide regrowth. In this work, we introduce a novel approach that employs molecular self-assembled monolayers (SAMs) to chemically bind at different interfaces of superconducting circuits. This technique is specifically tested here on coplanar waveguide (CPW) resonators, in which this method not only impedes oxide regrowth after surface etching but can also tailors the dielectric properties at different resonators interfaces. The deployment of SAMs results in a consistent improvement in the measured quality factors across multiple resonators, surpassing those with only oxide-etched resonators. The efficiency of our approach is supported by microwave measurements of multiple devices conducted at millikelvin temperatures and correlated with detailed X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) characterizations of SAM-passivated resonators. The compatibility of SAMs materials with the established fabrication techniques offers a promising route to improve the performance of superconducting quantum devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nanoscale imaging of He-ion irradiation effects on amorphous TaO x toward electroforming-free neuromorphic functions

Resistive switching in thin films has been widely studied in a broad range of materials. Yet, the mechanisms behind electroresistive switching have been persistently difficult to decipher and control, in part due to their non-equilibrium nature. Here, we demonstrate new experimental approaches that can probe resistive switching phenomena, utilizing amorphous TaO x as a model material system. Specifically, we applied scanning microwave impedance microscopy and cathodoluminescence (CL) microscopy as direct probes of conductance and electronic structure, respectively. These methods provide direct evidence of the electronic state of TaO x despite its amorphous nature. For example, CL identifies characteristic impurity levels in TaO x , in agreement with first principles calculations. We applied these methods to investigate He-ion-beam irradiation as a path to activate conductivity of materials and enable electroforming-free control over resistive switching. However, we find that even though He-ions begin to modify the nature of bonds even at the lowest doses, the films' conductive properties exhibit remarkable stability with large displacement damage and they are driven to metallic states only at the limit of structural decomposition. Finally, we show that electroforming in a nanoscale junction can be carried out with a dissipated power of <20 nW, a much smaller value compared to earlier studies and one that minimizes irreversible structural modifications of the films. Importantly, the multimodal approach described here provides a new framework toward the theory/experiment guided design and optimization of electroresistive materials.

36 MATERIALS SCIENCE↗

Oxide-nitride heteroepitaxy for low-loss dielectrics in superconducting quantum circuits

Superconducting qubits show great promise for the realization of fault-tolerant quantum computing, but lossy, amorphous dielectrics limit current technology. Identifying highly crystalline and stoichiometric dielectrics with intrinsically low microwave loss is therefore a central materials challenge, yet experimentally validated platforms remain scarce. In this work, we integrate a crystalline dielectric into a heteroepitaxial TiN/$γ$-Al$_2$O$_3$/TiN trilayer grown via pulsed laser deposition. Correlative high-resolution imaging, diffraction, and spectroscopy measurements confirm the single-crystal quality and chemical integrity of all layers, with minimal defects and limited anion interdiffusion across the oxide-nitride interfaces. Using microwave lumped-element resonators with parallel-plate capacitors, we report the first direct measurement of the dielectric loss of epitaxial $γ$-Al$_2$O$_3$, for which we find a low intrinsic two-level system loss, $δ_{\text{TLS}}^0 = (2.8 \pm 0.1) \times 10^{-5}$. These results establish heteroepitaxial oxides on transition metal nitrides as an attractive materials platform for superconducting quantum circuits, particularly for integration into compact device architectures such as merged-element transmons and microwave kinetic inductance detectors.

Garcia-Wetten, David A. [Northwestern U.]↗

Tunable Cr 4+ Molecular Color Centers

The inherent atomistic precision of synthetic chemistry enables bottom-up structural control over quantum bits, or qubits, for quantum technologies. Tuning paramagnetic molecular qubits that feature optical-spin initialization and readout is a crucial step toward designing bespoke qubits for applications in quantum sensing, networking, and computing. In this work, we demonstrate that the electronic structure that enables optical-spin initialization and readout for S = 1, Cr(aryl) 4 , where aryl = 2,4-dimethylphenyl (1), o-tolyl (2), and 2,3-dimethylphenyl (3), is readily translated into Cr(alkyl) 4 compounds, where alkyl = 2,2,2-triphenylethyl (4), (trimethylsilyl)methyl (5), and cyclohexyl (6). The small ground state zero field splitting values (<5 GHz) for 1–6 allowed for coherent spin manipulation at X-band microwave frequency, enabling temperature-, concentration-, and orientation-dependent investigations of the spin dynamics. Electronic absorption and emission spectroscopy confirmed the desired electronic structures for 4–6, which exhibit photoluminescence from 897 to 923 nm, while theoretical calculations elucidated the varied bonding interactions of the aryl and alkyl Cr 4+ compounds. The combined experimental and theoretical comparison of Cr(aryl) 4 and Cr(alkyl) 4 systems illustrates the impact of the ligand field on both the ground state spin structure and excited state manifold, laying the groundwork for the design of structurally precise optically addressable molecular qubits.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Using convolutional neural networks to detect edge localized modes in DIII-D from Doppler backscattering measurements

In H-mode tokamak plasmas, the plasma is sometimes ejected beyond the edge transport barrier. These events are known as edge localized modes (ELMs). ELMs cause a loss of energy and damage the vessel walls. Understanding the physics of ELMs, and by extension, how to detect and mitigate them, is an important challenge. In this paper, we focus on two diagnostic methods—deuterium-alpha (D α ) spectroscopy and Doppler backscattering (DBS). The former detects ELMs by measuring Balmer alpha emission, while the latter uses microwave radiation to probe the plasma. DBS has the advantages of having a higher temporal resolution and robustness to damage. These advantages of DBS diagnostic may be beneficial for future operational tokamaks, and thus, data processing techniques for DBS should be developed in preparation. In sight of this, we explore the training of neural networks to detect ELMs from DBS data, using D α data as the ground truth. With shots found in the DIII-D database, the model is trained to classify each time step based on the occurrence of an ELM event. The results are promising. When tested on shots similar to those used for training, the model is capable of consistently achieving a high f1-score of 0.93. Furthermore, this score is a performance metric for imbalanced datasets that ranges between 0 and 1. We evaluate the performance of our neural network on a variety of ELMs in different high confinement regimes (grassy ELM, RMP mitigated, and wide-pedestal), finding broad applicability. Beyond ELMs, our work demonstrates the wider feasibility of applying neural networks to data from DBS diagnostic.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

AlGaN/GaN metal–insulator–semiconductor high electron mobility transistors (MISHEMTs) using plasma deposited BN as gate dielectric

AlGaN/GaN metal–insulator–semiconductor high electron mobility transistors (MISHEMTs) were fabricated on Si substrates with a 10 nm boron nitride (BN) layer as a gate dielectric deposited by electron cyclotron resonance microwave plasma chemical vapor deposition. The material characterization of the BN/GaN interface was investigated by X-ray photoelectric spectroscopy (XPS) and UV photoelectron spectroscopy. The BN bandgap from the B1s XPS energy loss is ~5 eV consistent with sp2 bonding. The MISHEMTs exhibit a low off-state current of 1 × 10 –8 mA/mm, a high on/off current ratio of 10 9 , a threshold voltage of –2.76 V, a maximum transconductance of 32 mS/mm at a gate voltage of –2.1 V and a drain voltage of 1 V, a subthreshold swing of 69.1 mV/dec, and an on-resistance of 12.75 Ω·mm. The interface state density (D it ) is estimated to be less than 8.49 × 10 11 cm –2 eV –1 . Gate leakage current mechanisms were investigated by temperature-dependent current–voltage measurements from 300 K to 500 K. The maximum breakdown electric field is no less than 8.4 MV/cm. Poole–Frenkel emission and Fowler–Nordheim tunneling are indicated as the dominant mechanisms of the gate leakage through the BN gate dielectric at low and high electric fields, respectively.

36 MATERIALS SCIENCE↗

Magneto-optical spectroscopy based on pump-probe strobe light

Here, we demonstrate a pump-probe strobe light spectroscopy for sensitive detection of magneto-optical dynamics in the context of hybrid magnonics. The technique uses a combinatorial microwave-optical pump-probe scheme, leveraging both the high-energy resolution of microwaves and high-efficiency detection using optical photons. In contrast with conventional stroboscopy using continuous-wave light, we apply microwave and optical pulses with varying pulse widths, and demonstrate magneto-optical detection of magnetization dynamics in Y 3 Fe 5 O 12 films. The detected magneto-optical signals depend strongly on the characteristics of both the microwave and the optical pulses, as well as their relative time delays. We show that good magneto-optical sensitivity and coherent stroboscopic character are maintained, even at a microwave pump pulse of 1.5 ns and an optical probe pulse of 80 ps, under a 7 MHz clock rate, corresponding to a pump-probe footprint of approximately 1% in one detection cycle. Our results show that time-dependent strobe light measurement of magnetization dynamics can be achieved in the gigahertz frequency range under a pump-probe detection scheme.

36 MATERIALS SCIENCE↗

Nitrogen plasma passivated niobium resonators for superconducting quantum circuits

Microwave loss in niobium metallic structures used for superconducting quantum circuits is limited by a native surface oxide layer formed over a timescale of minutes when exposed to an ambient environment. Here, in this work, we show that nitrogen plasma treatment forms a niobium nitride layer at the metal–air interface, which prevents such oxidation. X-ray photoelectron spectroscopy confirms the doping of nitrogen more than 5 nm into the surface and a suppressed oxygen presence. This passivation remains stable after aging for 15 days in an ambient environment. Cryogenic microwave characterization shows an average filling-factor-adjusted two-level-system loss tangent Fδ TLS of (2.9±0.5)·10 –7 for resonators with a 3 μm center strip and (1.0±0.3)·10 –7 for a 20 μm center strip, exceeding the performance of unpassivated samples by a factor of four.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Methods for Color Center Preserving Hydrogen‐Termination of Diamond

Abstract Chemical functionalization of diamond surfaces by hydrogen is an important method for controlling the charge state of near‐surface fluorescent color centers, an essential process in fabricating devices such as diamond field‐effect transistors and chemical sensors, and a required first step for realizing families of more complex terminations through subsequent chemical processing. In all these cases, termination is typically achieved using hydrogen plasma sources that can etch or damage the diamond, as well as deposited materials or embedded color centers. This work explores alternative methods for lower‐damage hydrogenation of diamond surfaces, specifically the annealing of diamond samples in high‐purity, non‐explosive mixtures of nitrogen and hydrogen gas, and the exposure of samples to microwave hydrogen plasmas in the absence of intentional stage heating. The effectiveness of these methods are characterized by x‐ray photoelectron spectroscopy (XPS), and comparison of the results to density‐functional modelling of the surface hydrogenation energetics implicates surface oxygen ligands as the primary factor limiting the termination quality of annealed samples. Finally, photoluminescence (PL) spectroscopy is used to verify that both the annealing and reduced sample temperature plasma methods are non‐destructive to near‐surface ensembles of nitrogen‐vacancy (NV) centers, in stark contrast to plasma treatments that use heated sample stages.

36 MATERIALS SCIENCE↗

Carrier Recombination Dynamics of Surface-Passivated Epitaxial (100)Ge, (110)Ge, and (111)Ge Layers by Atomic Layer Deposited Al2O3

Germanium (Ge) and its heterostructures with compound semiconductors offer a unique optoelectronic functionality due to its pseudo-bandgap nature, that can be transformed to a direct bandgap material by providing strain and/or mixing with tin. Moreover, two crystal surfaces, (100)Ge and (110)Ge, that are technologically important for ultralow power fin or nanosheet transistors, could offer unprecedented properties with reduced surface defects after passivating these surfaces by atomic layer deposited (ALD) dielectrics. In this work, the crystallographically oriented epitaxial Ge/AlAs heterostructures were grown and passivated with ALD Al2O3 dielectrics, and the microwave photoconductive decay (u-PCD) technique was employed to evaluate carrier lifetimes at room temperature. The X-ray photoelectron spectroscopy analysis reveals no role of orientation effect in the quality of the ALD Al2O3 dielectric on oriented Ge layers. The carrier lifetimes measured using the u-PCD technique were benchmarked against unpassivated Ge/AlAs heterostructures. Excitation wavelengths of 1500 and 1800 nm with an estimated injection level of ~10^13 cm-3 were selected to measure the orientation-specific carrier lifetimes. The carrier lifetime was increased from 390 ns to 565 ns for (100)Ge and from 260 ns to 440 ns for (110)Ge orientations with passivation, whereas the carrier lifetime is almost unchanged for (111)Ge after passivation. This behavior indicates a strong dependence of the measured lifetime on surface orientation and surface passivation. The observed increase (>1.5x) in lifetime with Al2O3-passivated (100)Ge and (110)Ge surfaces is due to the lower surface recombination velocity compared to unpassivated Ge/AlAs heterostructures. The enhancement of carrier lifetime from passivated Ge/AlAs heterostructures with (100)Ge and (110)Ge surface orientations offers a path for the development of nanoscale transistors due to the reduced interface state density.

Al2O3↗

Transverse-Field Ising Dynamics in a Rydberg-Dressed Atomic Gas

Here, we report on the realization of long-range Ising interactions in a cold gas of cesium atoms by Rydberg dressing. The interactions are enhanced by coupling to Rydberg states in the vicinity of a Förster resonance. We characterize the interactions by measuring the mean-field shift of the clock transition via Ramsey spectroscopy, observing one-axis twisting dynamics. We furthermore emulate a transverse-field Ising model by periodic application of a microwave field and detect dynamical signatures of the paramagnetic-ferromagnetic phase transition. Our results highlight the power of optical addressing for achieving local and dynamical control of interactions, enabling prospects ranging from investigating Floquet quantum criticality to producing tunable-range spin squeezing.

74 ATOMIC AND MOLECULAR PHYSICS↗

Spin Dynamics of SCRPs in ZnO Quantum Dot–Organic Molecule Conjugates Studied with Pulsed EPR

Photogenerated spin-correlated radical pairs (SCRPs) are emerging as promising new candidates for Quantum Information Science applications, where they act as electron spin qubit pairs (SQPs). Historically, these pairs have been mostly investigated in natural photosynthesis and in molecular organic donor–(linker)–acceptor systems. Recently, we have shown that these spin pairs can also be observed by time-resolved electron-paramagnetic resonance (EPR) spectroscopy in hybrid inorganic–organic conjugates. The current study builds on recent work (ACS Nano, 2025, 19, 12194–12207), in which we systematically prepared hybrid inorganic–organic molecule systems with tunable geometries that can host SCRPs/SQPs. Here, we demonstrate using pulsed EPR spectroscopy that we can generate, study, and manipulate the spins in these photogenerated SCRPs hosted on highly tailorable inorganic–organic hybrid systems. Microwave pulse-based spin manipulation is the first step toward developing quantum computing and quantum sensing applications with these promising spin-based qubit materials, which can be reversibly photogenerated in highly spin-polarized states at moderate temperatures. An attractive feature of this new class of hybrid materials is that the g-factor of the unpaired electron spin in the ZnO QD (as part of the SCRP/SQP) can be adjusted using the quantum size effect in these QDs, which allows for the selective addressability of each spin in the SCRP using microwave pulses. Additionally, we also observed a difference between the g-values of the unpaired electron in the ZnO QD in the transient SCRP state and stable photoreduced state. We hypothesize that the unpaired electron in the SCRP is delocalized as a band-like conduction electron, while in the stable photoreduced state, the electron is delocalized in a shallow electron trap state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hyperspectral X-ray Imaging with TES Detectors for Nanoscale Chemical Speciation Mapping

We are developing an imaging capability (“Hyperspectral X-ray Imaging”) for mapping chemical information (molecular formula, phase, oxidation state, hydration) that is based on ultra-high-resolution X-ray emission spectroscopy with large transition-edge sensor microcalorimeter arrays in the scanning electron microscope. By combining microcalorimeter arrays with hundreds of pixels, high-bandwidth microwave frequency-division multiplexing, and fast digital electronics for near real-time data processing, our goal is to enable measurements using laboratory-scale instrumentation rather than synchrotron beamlines. Our application focus here is on mapping the chemical form of uranium compounds on the nanoscale. Furthermore, we will present our approach to developing the Hyperspectral X-ray Imaging capability, progress toward a 128-pixel microwave multiplexed X-ray fluorescence instrument at LANL, and the path to high-throughput nanoscale chemical mapping.

47 OTHER INSTRUMENTATION↗