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At least 379 records · Page 21

Quantitative chemical exchange saturation transfer with hyperpolarized nuclei (qHyper-CEST): Sensing xenon-host exchange dynamics and binding affinities by NMR

The reversible binding of xenon to host molecules has found numerous applications in nuclear magnetic resonance studies. Quantitative characterization of the Xe exchange dynamics is important to understand and optimize the physico-chemical behavior of such Xe hosts, but is often challenging to achieve at low host concentrations. We have investigated a sensitive quantification technique based on chemical exchange saturation transfer with hyperpolarized nuclei, qHyper-CEST. Using simulated signals we demonstrated that qHyper-CEST yielded accurate and precise results and was robust in the presence of large amounts of noise (10%). This is of particular importance for samples with completely unknown exchange rates. Using these findings we experimentally determined the following exchange parameters for the Xe host cryptophane-A monoacid in dimethyl sulfoxide in one type of experiment: the ratio of bound and free Xe, the Xe exchange rate, the resonance frequencies of free and bound Xe, the Xe host occupancy, and the Xe binding constant. Taken together, qHyper-CEST facilitates sensitive quantification of the Xe exchange dynamics and binding to hydrophobic cavities and has the potential to analyze many different host systems or binding sites. This makes qHyper-CEST an indispensable tool for the efficient design of highly specific biosensors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

SU-E-T-180: Fano Cavity Test of Proton Transport in Monte Carlo Codes Running On GPU and Xeon Phi

Purpose: In proton dose calculation, clinically compatible speeds are now achieved with Monte Carlo codes (MC) that combine 1) adequate simplifications in the physics of transport and 2) the use of hardware architectures enabling massive parallel computing (like GPUs). However, the uncertainties related to the transport algorithms used in these codes must be kept minimal. Such algorithms can be checked with the so-called “Fano cavity test”. We implemented the test in two codes that run on specific hardware: gPMC on an nVidia GPU and MCsquare on an Intel Xeon Phi (60 cores). Methods: gPMC and MCsquare are designed for transporting protons in CT geometries. Both codes use the method of fictitious interaction to sample the step-length for each transport step. The considered geometry is a water cavity (2×2×0.2 cm{sup 3}, 0.001 g/cm{sup 3}) in a 10×10×50 cm{sup 3} water phantom (1 g/cm{sup 3}). CPE in the cavity is established by generating protons over the phantom volume with a uniform momentum (energy E) and a uniform intensity per unit mass I. Assuming no nuclear reactions and no generation of other secondaries, the computed cavity dose should equal IE, according to Fano's theorem. Both codes were tested for initial proton energies of 50, 100, and 200 MeV. Results: For all energies, gPMC and MCsquare are within 0.3 and 0.2 % of the theoretical value IE, respectively (0.1% standard deviation). Single-precision computations (instead of double) increased the error by about 0.1% in MCsquare. Conclusion: Despite the simplifications in the physics of transport, both gPMC and MCsquare successfully pass the Fano test. This ensures optimal accuracy of the codes for clinical applications within the uncertainties on the underlying physical models. It also opens the path to other applications of these codes, like the simulation of ion chamber response.

60 APPLIED LIFE SCIENCES↗

Strain-concentration for fast, compact photonic modulation and non-volatile memory

A critical figure of merit (FoM) for electro-optic (EO) modulators is the transmission change per voltage, d T / d V . Conventional approaches in wave-guided modulators maximize d T / d V via a high EO coefficient or longer light-material interaction lengths but are ultimately limited by material losses and nonlinearities. Optical and RF resonances improve d T / d V at the cost of spectral non-uniformity, especially for high- Q optical cavity resonances. Here, we introduce an EO modulator based on piezo-strain-concentration of a photonic crystal cavity to address both trade-offs: (i) it eliminates the trade-off between d T / d V and waveguide loss—i.e., enhancement of the resonance tuning efficiency d v c / d V for the fixed EO coefficient, waveguide length, and cavity Q —and (ii) at high DC strains it exhibits a non-volatile (NV) cavity tuning Δ v c ,NV for passive memory and programming of multiple devices into resonance despite fabrication variations. The device is fabricated on a scalable silicon nitride-on-aluminum nitride platform. We measure d v c / d V =177±1MHz/V, corresponding to Δ v c =40±0.32GHz for a voltage spanning ±120V with an energy consumption of δ U /Δ v c =0.17nW/GHz. The modulation bandwidth is flat up to ω BW,3dB /2 π =3.2±0.07MHz for broadband DC-AC and 142±17MHz for resonant operation near a 2.8 GHz mechanical resonance. Optical extinction up to 25 dB is obtained via Fano-type interference. Strain-induced beam-buckling modes are programmable under a “read-write” protocol with a continuous, repeatable tuning range of 5±0.25GHz, allowing for storage and retrieval, which we quantify with mutual information of 2.4 bits and a maximum non-volatile excursion of 8 GHz. Using a full piezo-optical finite-element-model (FEM) we identify key design principles for optimizing strain-based modulators and chart a path towards achieving performance comparable to lithium niobate-based modulators and the study of high strain physics on-chip.

Wen, Y. Henry (ORCID:0009000685423628)↗

Small-Molecule CD4-Mimics: Structure-Based Optimization of HIV-1 Entry Inhibition

We report the optimization, based on computational, thermodynamic, and crystallographic data, of a series of small-molecule ligands of the Phe43 cavity of the envelope glycoprotein gp120 of human immunodeficiency virus (HIV) has been achieved. Importantly, biological evaluation revealed that the small-molecule CD4 mimics (4–7) inhibit HIV-1 entry into target cells with both significantly higher potency and neutralization breadth than previous congeners, while maintaining high selectivity for the target virus. Their binding mode was characterized via thermodynamic and crystallographic studies.

60 APPLIED LIFE SCIENCES↗

A Forward Feedback Control Scheme for a Solar Thermochemical Moving Bed Counter-Current Flow Reactor

Abstract Pelletized thermochemical energy storage media has a potential for long-duration energy storage. Production of solid-state energy storage media can be done within a cavity chemical reactor that captures concentrated solar radiation from a solar thermal field. The temperature stability of a solar reactor is directly influenced by the solar flux intercepted. This paper presents a low-order physical model to simulate the dynamic response of temperature inside a tubular plug-flow reactor prototype. Solid granular particles are fed to the reactor from the top whereas a counter-current flowing gas enters the reactor from the bottom. An in-house code was developed to model transient heat transfer of the reactor wall, gas, and moving particles. The model was preliminarily validated with packed beds for different temperature ranges and two gas flowrates. Dynamic response of the reactor temperature is simulated for different input power and gas/particle flowrates. The results show that the system response can be controlled efficiently by utilizing input power (solar flux) as a control parameter. A conventional proportional integral (PI) controller is designed to control the temperature inside the reactor and to maintain it during the solar flux intermittency. The controller parameters are tuned using the Ziegler–Nichols method to ensure optimal system response. The results show that the feedback control model is successful in tracking different reference reactor temperatures within a reasonable settling time of 30 min and eliminated overshoot. This study can be extended to include a hybrid reactor with a multi-input, multi-output variable system.

Energy & Fuels↗

Advanced readout methods for superheated emulsion detectors

Superheated emulsions develop visible vapor bubbles when exposed to ionizing radiation. They consist in droplets of a metastable liquid, emulsified in an inert matrix. The formation of a bubble cavity is accompanied by sound waves. Evaporated bubbles also exhibit a lower refractive index, compared to the inert gel matrix. These two physical phenomena have been exploited to count the number of evaporated bubbles and thus measure the interacting radiation flux. Systems based on piezoelectric transducers have been traditionally used to acquire the acoustic (pressure) signals generated by bubble evaporation. Such systems can operate at ambient noise levels exceeding 100 dB; however, they are affected by a significant dead time (>10 ms). An optical readout technique relying on the scattering of light by neutron-induced bubbles has been recently improved in order to minimize measurement dead time and ambient noise sensitivity. Beams of infra-red light from light-emitting diode (LED) sources cross the active area of the detector and are deflected by evaporated bubbles. The scattered light correlates with bubble density. Planar photodiodes are affixed along the detector length in optimized positions, allowing the detection of scattered light from the bubbles and minimizing the detection of direct light from the LEDs. A low-noise signal-conditioning stage has been designed and realized to amplify the current induced in the photodiodes by scattered light and to subtract the background signal due to intrinsic scattering within the detector matrix. The proposed amplification architecture maximizes the measurement signal-to-noise ratio, yielding a readout uncertainty of 6% (±1 SD), with 1000 evaporated bubbles in a detector active volume of 150 ml (6 cm detector diameter). In this work, we prove that the intensity of scattered light also relates to the bubble size, which can be controlled by applying an external pressure to the detector emulsion. This effect can be exploited during the readout procedure to minimize shadowing effects between bubbles, which become severe when the latter are several thousands. The detector we used in this work is based on superheated C-318 (octafluorocyclobutane), emulsified in 100 μm ± 10% (1 SD) diameter drops in an inert matrix of approximately 150 ml. The detector was operated at room temperature and ambient pressure.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Implanted Silicon Resistor Layers for Efficient Terahertz Absorption

Broadband absorption structures are an essential component of large format bolometer arrays for imaging GHz and THz radiation. We have measured electrical and optical properties of implanted silicon resistor layers designed to be suitable for these absorbers. Implanted resistors offer a low-film-stress, buried absorber that is robust to longterm aging, temperature, and subsequent metals processing. Such an absorber layer is readily integrated with superconducting integrated circuits and standard micromachining as demonstrated by the SCUBA II array built by ROE/NIST (1). We present a complete characterization of these layers, demonstrating frequency regimes in which different recipes will be suitable for absorbers. Single layer thin film coatings have been demonstrated as effective absorbers at certain wavelengths including semimetal (2,3), thin metal (4), and patterned metal films (5,6). Astronomical instrument examples include the SHARC II instrument is imaging the submillimeter band using passivated Bi semimetal films and the HAWC instrument for SOFIA, which employs ultrathin metal films to span 1-3 THz. Patterned metal films on spiderweb bolometers have also been proposed for broadband detection. In each case, the absorber structure matches the impedance of free space for optimal absorption in the detector configuration (typically 157 Ohms per square for high absorption with a single or 377 Ohms per square in a resonant cavity or quarter wave backshort). Resonant structures with -20% bandwidth coupled to bolometers are also under development; stacks of such structures may take advantage of instruments imaging over a wide band. Each technique may enable effective absorbers in imagers. However, thin films tend to age, degrade or change during further processing, can be difficult to reproduce, and often exhibit an intrinsic granularity that creates complicated frequency dependence at THz frequencies. Thick metal films are more robust but the requirement for patterning can limit their absorption at THz frequencies and their heat capacity can be high. patterned absorber structures that offer low heat capacity, absence of aging, and uniform, predictable behavior at THz frequencies. We have correlated DC electrical and THz optical measurements of a series of implanted layers and studied their frequency dependence of optical absorption from .3 to 10 THz at cryogenic temperatures. We have modeled the optical response to determine the suitability of the implanted silicon resistor as a function of resistance in the range 10 Ohms/sq to 300 Ohms/sq.

Chervenak, J. A.↗

Multi-physics Modeling of Radiative Heat Transfer and Fluid Flow for the Reactor Cavity Cooling System

High-temperature gas-cooled reactors (HTGRs) are notable for their high thermal efficiency and potential for combined heat and power applications. These reactors are particularly appealing due to their advanced passive safety features. HTGRs utilize passive safety systems that function without requiring active components like pumps or compressors during emergencies. These reactor designs depend on a Reactor Cavity Cooling System (RCCS) to manage decay heat removal from the reactor pressure vessel (RPV) during accident conditions. The RCCS consists of vertical rectangular channels known as "risers" or riser ducts positioned around the RPV. These risers receive heat from the RPV through both convective and radiative heat transfer mechanisms. Understanding the interplay of multiple physical phenomena, such as fluid dynamics, heat transfer, and neutron interactions, is essential for the effective design and operation of nuclear reactors, particularly for systems like the RCCS. Multi-physics simulations provide a comprehensive approach to studying these interactions, offering detailed insights and enhancing accuracy. They are especially important in RCCS designs, where the interaction between radiative and convective heat transfer can significantly impact system performance. By leveraging multi-physics simulations, complex reactor behaviors can be modeled without compromising the fidelity of the underlying physical processes. This work aims to establish a robust methodology for coupling multiple physical processes in an air-cooled RCCS. By focusing on validating this multi-physics approach, the study involves designing test cases that simulate various conditions to verify the numerical models employed. The outcomes of this research will provide critical insights for accurately modeling and optimizing complex nuclear systems like the RCCS.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Molecular mechanism of respiratory syncytial virus fusion inhibitors

Respiratory syncytial virus (RSV) is a leading cause of pneumonia and bronchiolitis in young children and the elderly. Therapeutic small molecules have been developed that bind the RSV F glycoprotein and inhibit membrane fusion, yet their binding sites and molecular mechanisms of action remain largely unknown. In this paper, we show that these inhibitors bind to a three-fold-symmetric pocket within the central cavity of the metastable prefusion conformation of RSV F. Inhibitor binding stabilizes this conformation by tethering two regions that must undergo a structural rearrangement to facilitate membrane fusion. Inhibitor-escape mutations occur in residues that directly contact the inhibitors or are involved in the conformational rearrangements required to accommodate inhibitor binding. Resistant viruses do not propagate as well as wild-type RSV in vitro, indicating a fitness cost for inhibitor escape. Finally and collectively, these findings provide new insight into class I viral fusion proteins and should facilitate development of optimal RSV fusion inhibitors.

59 BASIC BIOLOGICAL SCIENCES↗

Approaching attometer laser vibrometry

The heterodyne two-beam interferometer has been proven to be the optimal solution for laser-Doppler vibrometry regarding accuracy and signal robustness. The theoretical resolution limit for a two-beam interferometer of laser class 3R (up to 5 mW visible measurement-light) is in the regime of a few femtometer per square-root Hertz and well suited to study vibrations in microstructures. However, some new applications of RF-MEM resonators, nanostructures, and surface-nano-defect detection require resolutions beyond that limit. The resolution depends only on the noise and the sensor sensitivity to specimen displacements. The noise is already defined in nowadays systems by the quantum nature of light for a properly designed optical sensor and more light would lead to an inacceptable influence like heating of a very tiny structure. Thus, noise can only be improved by squeezed-light techniques which require a negligible loss of measurement light which is impossible for almost all technical measurement tasks. Thus, improving the sensitivity is the only possible path which could make attometer laser vibrometry possible. Decreasing the measurement wavelength would increase the sensitivity but would also increase the photon shot noise. In this paper, we discuss an approach to increase the sensitivity by assembling an additional mirror between interferometer and specimen to form an optical cavity. A detailed theoretical analysis of this setup is presented and we derive the resolution limit, discuss the main contributions to the uncertainty budget, and show a first experiment proving the sensitivity amplification of our approach.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Characterization of Low-Temperature, Co-Fired Ceramic-Manufactured Electrostatic Thruster-Closeout Report

The goal of the project was to evaluate prototypes of an experimental thruster developed by the University of Arkansas (UA), Fayetteville, AR. The design under evaluation is a radio frequency (RF) electrostatic thruster that was fabricated using the low-temperature, co-fired ceramic (LTCC) materials and fabrication process. This materials system is analogous to printed circuit board (PCB) technology with the most significant difference being that the laminate is replaced by a ceramic material and the copper layer is replaced by printed sinterable silver paste. LTCC designs are baked after fabrication and assembled to realize an entirely monolithic structure with internal conductors, vias, and cavities. In this process, the LTCC electrostatic thruster (LTCC-ET) that is the subject of the present work becomes a monolithic ceramic thruster capable of withstanding temperatures in excess of 500 ºC. The UA and NASA Marshall Space Flight Center (MSFC) jointly performed prototype testing on the LTCC-ET under a NASA Cooperative Agreement Notice (CAN) award. The LTCC-ET was tested at MSFC in May 2018 over a 1-week period. There were two goals for the test program: (1) Testing to determine the operating parameters required to create plasma ignition in the test articles. This was explored by setting a propellant flowrate and increasing RF power until plasma ignition was observed. Testing was conducted with both argon and krypton. (2) Investigate the thrust and specific impulse (Isp) performance of the thruster as a function of propellant flowrate and grid voltage. This goal was not met during the project as technical challenges in maintaining stable plasma ignition arose due to stress and heating of the RF power feed. In summary, a prototype thruster design (consisting of three packaged units) was fabricated by UA and tested for the first time under vacuum conditions at MSFC to experimentally determine basic performance metrics and functionality. It was found that the design was not sufficiently optimized or robust enough in its initial iteration to support a significant test campaign or characterization program. It was concluded that the propellant outlet channels must be reduced in size with the flowpaths adjusted to increase propellant residence time in the thruster, and that the RF connector must be replaced with a version capable of handling higher power throughput and heating. However, even in its unoptimized form, a plasma could be produced in the LTCCET, demonstrating the efficacy of the design approach. The design is especially compelling due to its low cost to manufacture and, more importantly, its scalability of size and power throughput. Low cost and scalability are also important in that additional functionalities, such as thrust vectoring and plume charge neutralization, can be integrated into future designs with minimal additional cost. This project has matured the LTCC-ET development Technology Readiness Level (TRL) from 1 to 2. The low-cost RF plasma source portion of the LTCC device was matured from TRL 2 to 4 through the demonstration of RF plasma ignition under vacuum conditions.

Huang, P.-H. A.↗

High Quantum Efficiency Uni-Traveling-Carrier Photodiode for Optical to Microwave Transduction

Modern Quantum Information Systems (QIS) employ optical photons for long distance communication, operating at ambient temperature, between microwave cavities, which house microwave photons used in quantum computing and microwave detection. These optical photons, carried by fiber-optic or free-space links, offer a low-cost, uncooled alternative to bulky, expensive microwave coaxial cables, which are lossy, susceptible to EMI, and a significant thermal conductor to the outside ambient environment. To convert between these two types of photons and implement these optical interconnects, it is necessary to develop a high-performance photodetector for optical to microwave transduction. Freedom Photonics and the University of Virginia have a well-established partnership in developing high-performance photodiodes. In this Phase I effort, we collaborated in designing, fabricating, and testing an advanced, high-speed, high quantum efficiency prototype photodiode for transduction from optical to microwave frequencies. These devices have applications not only in quantum computing and axion detection, but also in other optical-cryogenic interconnect applications, in fields such as radio astronomy and quantum cryptography, as well as in quantum metrology and plasmonics. During this Phase I DOE program, we designed, fabricated, and tested prototype PIN GaAs photodiodes which targeted the performance parameters defined by the program. This process involved identifying a new target wavelength, different from that proposed initially, based on conversations with the Oak Ridge National Lab customer. We designed an epitaxial stack, optimized in theory for ≥95% quantum efficiency at 795 nm, ≥5 GHz, per the target objectives of the program. Additionally, we designed a fabrication process and associated mask plates for top-illuminated, AR-coated devices with device diameters ranging from 50 µm to 800 µm. Using these, we fabricated two 3” wafer quarters of devices, and characterized the devices’ dark current, quantum efficiency, and bandwidth for various device diameters. The prototype devices achieved a quantum efficiency of 89% at the target 795 nm detection wavelength. The bandwidth of the devices proved tricky to characterize, but a 50 µm diameter device shows a 3-dB bandwidth of at least 1.6 GHz, possibly a full 5 GHz, depending on the measurement setup. In the future, we plan to characterize the bandwidth of these devices using an impulse response measurement. All tasks for the Phase I were successfully completed, and sample prototype devices were provided to Oak Ridge National Lab Quantum Information Science researchers. The work performed in Phase I has established a strong foundation for future design and fabrication cycles in Phase II, if granted. The early tests at Oak Ridge National Labs will provide guidance for the required photodiode performance in devices to be supplied in Phase II.

42 ENGINEERING↗

Prototype Modeling for a Light-Trapping Planar-Cavity Enclosed Particle Solar Receiver

Concentrating solar thermal (CST) systems present a promising avenue for affordable and reliable energy production. Solar receivers are key components that determine the efficiency and longevity of these systems. Particle-based solar receivers have emerged as a compelling alternative to traditional technologies, offering several advantages that address limitations in current CST systems. This is especially true as next-generation CST technologies target applications including electricity generation, thermochemical processes, and industrial process heat, many of which necessitate higher operating temperatures than current commercial molten salt systems. Molten-salt thermal energy storage (TES) systems, commonly used in CSP, face challenges related to freezing and corrosion. Particle-based TES systems, in contrast, do not experience these issues, as particles are stable at high temperatures, exceeding 1000 degrees Celsius. This capability allows for a wider range of applications, including those requiring higher temperatures for industrial processes and efficient electricity generation. A novel innovation in particle-based solar receiver technology is the light-trapping planar cavity receiver (LTPCR) configuration developed by NREL. The LTPCR design consists of small cavity-like structures using opaque planar surfaces, enabling efficient capture and absorption of solar energy. A high incident flux concentration at the cavity aperture is absorbed on the receiver walls, and subsequently transferred to particles on the inside of cavities. The particles flow through the system, forming a fluidized bed inside of the receiver panels, effectively capturing the absorbed solar heat. Air is used as a fluidizing medium in this process to enhance particle heat transfer and mixing. The effectiveness of this design lies in its ability to manage solar flux conditions and ensure high solar-to-thermal receiver efficiency. A 100-kW prototype is currently being tested at the King Saud University in Saudi Arabia to assess the receiver performance. A range of modeling analyses for the optical, thermal, and mechanical effects were conducted to assess the performance of the receiver under on-sun conditions. The solar flux resulting from the KSU heliostat field was modeled using NREL SolTrace software and produced up to 600 kW/m2 at the receiver aperture. The solar flux absorbed on the receiver walls was then used within a computational fluid dynamics (CFD) model to predict wall temperature distributions along with radiation and convection loss. A two-phase CFD model was developed for the fluidized bed of silica sand inside the receiver panels to predict local wall-to-particle heat transfer coefficients, particle temperature distributions, and outlet temperature of the particles. We have also conducted analyses to understand the thermomechanical behavior of these innovative enclosed light-trapping solar receivers optimized for particle heating. We used finite element analysis (FEA) to predict the receiver's performance using temperature distributions obtained from CFD and based on the resulting stress profiles, evaluated creep-fatigue damage with a goal of achieving a 30-year service life. Analysis showed a significant impact of the particle-to-wall heat transfer coefficients (HTCs) on receiver performance, with higher HTCs resulting in reduced stress and increased lifespan. For instance, when using Inconel 740H, increasing the HTC from 800 W/m2 K to 1400 W/m2 K increased the creep life from 4,000 hours to over 100,000 hours. This highlights the importance of understanding and optimizing heat transfer in the design of high-efficiency receivers.

14 SOLAR ENERGY↗

Solid State Quantum Refrigeration Superconducting, Absorption and Measurement Based (Final Technical Report)

During this DOE grant, DE-SC0017890, in place for the past six years, all proposed research was carried out and published in peer-reviewed papers, as well as other projects that emerged during the research. In that effort the research team accomplished all proposed research, as well as many closely related research projects discovered and conceived of during the grant. These works included “Efficient Quantum Measurement Engines”, a work published in Physical Review Letters, giving a theory of quantum measurement-based engines, which uses quantum measurement as a resource. These engines are designed to efficiently convert energy from the stochastic quantum measurement process into useful work. Further publications include “Experimental Realization of a Quantum Dot Energy Harvester”, a joint theory and experimental work in collaboration with the group of Charles Smith in Cambridge, UK, as well as long time theoretical collaborators, Rafael Sánchez and Björn Sothmann. This work, featured as an Editor’s Suggestion in Physical Review Letters, realized an earlier theoretical proposal of ours, whereby two resonant tunneling quantum dots are connected to a central electronic cavity that is heated by a hot energy source. We also published “Superconducting Quantum Refrigerator: Breaking and Rejoining Cooper Pairs with Magnetic Field Cycles” a work done in collaboration with experimentalist Francesco Giazotto from ENS Pisa, Italy, which also resulted in a patent. This paper, published in Phys. Rev. Applied, advanced the concept of a cyclic fridge based on the normal/superconducting phase transition together with layered materials separated by tunnel junctions. We also completed the proposed research on a heat transistor, publishing “Thermal transistor and thermometer based on Coulomb-coupled conductors”, carried out as a collaboration between my group and theorists Splettstoesser (Lund U., Sweden), Sothmann (U. Duisburg-Essen, Germany), and Sánchez (U. Autónoma de Madrid, Spain). We carried out an analysis of a quantum coupled to a quantum point contact as a sensitive thermometer and heat transistor. We found the optimal statistical estimator for the temperature and compared it with experiments on the same type of devices. We also investigated autonomous quantum absorption refrigerators using quantum dots to cool by using a very hot thermal reservoir to drive heat between two other reservoirs. In the article “Quantifying the quantum heat contribution from a driven superconducting circuit”, we demonstrated that for a driven superconducting circuit, we showed heat flow provided by a hot source to the qubit can be switched on and off by varying external parameters, the frequency and the intensity of the driving. In the work “Stochastic thermodynamic cycles of a mesoscopic thermoelectric engine”, we reconsidered the autonomous thermoelectric heat engine in terms of underlying cycles. Rather than periodic behavior, the cycles were stochastic in nature. Nevertheless, by undertaking a graph theoretical analysis of the elementary transport processed, great quantitative and qualitative insight could be found. We also considered the quantum measurement process and showed that a quantum version of Maxwell’s demon could be related to the work extraction of a quantum system, closely related to arrow-of-time measures for quantum measurement, as described in our article “Thermodynamics of quantum measurement and Maxwell's demon's arrow of time”. This work was selected in Phys. Rev. A as an Editor’s Suggestion. A recent preprint titled “Cyclic Superconducting Quantum Refrigerators Using Guided Fluxon Propagation” accomplished an important piece of this grant: to propose a new kind of quantum refrigerator using the dynamics of fluxons in a type II superconductor. This invention envisioned a race-track type geometry where fluxons are confined. By applying a gradient of magnetic field together with electric current in a Corbino geometry, the circulating fluxons can actively cool a cold reservoir, realizing a new type of cyclic superconducting refrigerator. We also investigated the possibility of thermal control from different points of view. The application of quantum measurement to the system gives a new kind of control on the system of interest – we have pioneered this approach and shown that measurement can boost the thermal power of quantum engines as described in “Continuous measurement boosted adiabatic quantum thermal machines”. The ability to have heat flows on demand is an outstanding challenge, and we have provided new solutions to this problem in Thermal control across a chain of electronic nanocavities” for a chain of electron cavities using gating voltage control. The control methods using qubit/qubit coupling to create absorption fridges at their most fundamental level have also been developed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Operation and Optimization of Microwave-Heated Continuous-Flow Microfluidics

Microwave (MW) technology can be powerful for electrification and process intensification but limited fundamental understanding of scalability and design principles hinders its effective use. In this work, we build a continuous-flow microreactor inside a commercial single-mode MW applicator and the corresponding computational fluid dynamics model to simulate the temperature profile. The model is in good agreement with experiments for various microreactor dimensions and operating conditions. The model indicates that MW heating is greatly influenced by reactor geometry as well as the operating parameters. We observe a strong correlation between parameters and develop a gradient boost regression tree model to predict the outlet temperature accurately. This model is then applied to optimize the dimensions and operating conditions to maximize the outlet temperature and energy efficiency, resulting in a Pareto optimal. We demonstrate computationally and experimentally that it is possible to surpass the Pareto optimal and achieve an energy efficiency of ~90% or greater at temperatures relevant for liquid-phase chemistry via salting of the solvent. The present methodology can be applied to other complex MW reactors. Lastly, the combined numerical and experimental approach provides insights into and a framework for scale-up and optimization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Insight into small molecule binding to the neonatal Fc receptor by X-ray crystallography and 100 kHz magic-angle-spinning NMR

Aiming at the design of an allosteric modulator of the neonatal Fc receptor (FcRn)–Immunoglobulin G (IgG) interaction, we developed a new methodology including NMR fragment screening, X-ray crystallography, and magic-angle-spinning (MAS) NMR at 100 kHz after sedimentation, exploiting very fast spinning of the nondeuterated soluble 42 kDa receptor construct to obtain resolved proton-detected 2D and 3D NMR spectra. FcRn plays a crucial role in regulation of IgG and serum albumin catabolism. It is a clinically validated drug target for the treatment of autoimmune diseases caused by pathogenic antibodies via the inhibition of its interaction with IgG. We herein present the discovery of a small molecule that binds into a conserved cavity of the heterodimeric, extracellular domain composed of an α-chain and β2-microglobulin (β2m) (FcRnECD, 373 residues). X-ray crystallography was used alongside NMR at 100 kHz MAS with sedimented soluble protein to explore possibilities for refining the compound as an allosteric modulator. Proton-detected MAS NMR experiments on fully protonated [ 13 C, 15 N]-labeled FcRnECD yielded ligand-induced chemical-shift perturbations (CSPs) for residues in the binding pocket and allosteric changes close to the interface of the two receptor heterodimers present in the asymmetric unit as well as potentially in the albumin interaction site. X-ray structures with and without ligand suggest the need for an optimized ligand to displace the α-chain with respect to β2m, both of which participate in the FcRn ECD –IgG interaction site. Our investigation establishes a method to characterize structurally small molecule binding to nondeuterated large proteins by NMR, even in their glycosylated form, which may prove highly valuable for structure-based drug discovery campaigns.

59 BASIC BIOLOGICAL SCIENCES↗

Validation Data Acquisition in HTTF during PCC Events

A validation experimental campaign was conducted in an Integral Effect Test (IET) facility of High Temperature Gas Reactors (HTGR), the High-Temperature Test Facility (HTTF) at Oregon State University (OSU). The HTTF simulates Depressurized and Pressurized Conduction Cooldowns (DCC and PCC). This campaign required the development of a new laser spectroscopic diagnostic to measure velocity in the challenging conditions of the HTTF: low speed (~1 m/s) gas flows at HTGR prototypical temperature and 1/10th pressure. This was a collaborative effort between co-PIs at The George Washington University (GW), Oregon State University (OSU), and NASA Langley Research Center. The main accomplishments of this project include the record for dynamic range for velocimetry, highest accuracy obtained with this technique, successful deployment in an IET leading to new validation matrix for CFD. These are detailed below and in manuscript appended to this executive summary. For this project, we introduced a new class of laser spectroscopic diagnostics to Thermal-Hydraulics to measure velocity of gases; furthermore, the diagnostic was demonstrated in-situ in an IET during DCC events. In such scenarios, particles used in mainstream techniques, like Particle Image Velocimetry (PIV) are not appropriate as they settle down too rapidly and also contaminate the experimental facility. Molecular tracers stay mixed within the working gas and can seed the flow in a technique called Molecular Tagging Velocimetry (MTV). In MTV a molecular tracer is photo-dissociated by a first (write) laser into radicals or molecules. The pattern created by the write laser is then interrogated with planar laser-induced fluorescence (PLIF), the read pulse(s), which are recorded with a camera. The pattern is probed and matched at two times (interval or probe time, dt), resulting in a time-of-flight velocimetry technique. This project demonstrated a new application range for MTV in gases. MTV has been extensively used for high-speed gas dynamics: molecules do not suffer from inertia associated with particles in regions of high accelerations (such as shock waves). For high-speed flows, the probe time is on the order of 0.1-10 µs. In time-of-flight techniques, the velocity is reconstructed from the recorded displacement, dx, between time interval dt: U = dx/dt. To first order, the resolution of the pattern matching is typically a (fixed) fraction of a pixel; therefore the resolution of the velocity measurement increases with dx and, for a given flow velocity, dt. For the low-speed flows of interest here, this requires long probe time, and therefore finding tracers that are stable for a long time. After an extensive literature survey we identified 6 tracers that would be suitable. We also worked with Spectra Physics to design a custom laser system that is flexible enough to probe these various tracers. The final instrument is made of 4 lasers that are integrated into a compact and movable cart to facilitate the deployment of the instrument off-site. One unique aspect of the laser system is the tunable dye laser (needed to do PLIF of the radicals). By being pumped by two Nd:YAG lasers, this laser is able to provide two pulses with any probe time (dt) for wavelengths between 200 and 900 nm with a linewidth of 3 pm. Accommodating the dual-pulse capability required customizing the pump lasers and the dye laser, making this system unique. Additionally, a custom UV-intensified CCD camera capable of frame-straddling and exposure time as short as 10 ns was acquired. More than two-third of the instrument cost (~$200k) was covered by a cost sharing from the PI’s startup funds. Of the 6 potential tracers identified, two were tested extensively (H2O and N2O) at high-temperature and elevated pressure at GW prior to conducting the tests at OSU. For both tracers, an Ar-F laser (193 nm, 10 ns, 10 mJ/pulse) photo-dissociates trace amounts (0.1 – 5% molar fraction) of the gases into OH and NO. OH is probed at 281.905 nm and NO at 226.186 nm (4-30mJ, 10 ns pulse). NO is very stable in inert environment and we could reconstruct velocities precisely with probe delay times as long at 40 ms, compared to 2 ms for OH, resulting in increased precision. Therefore, for the tests in the HTTF, N2O was selected as the final tracer and its optimal concentration was determined to be 0.5% molar. In the GW laboratory, we obtained a velocity measurement precision of 4 mm/s at conditions mimicking the HTTF tests. We also demonstrated the benefit of molecular tracers over particles and the flexibility of our instrument by continuously measuring velocity from 1000 to 0.1 m/s in a blow down test. This represents a dynamic range on velocity of 80 dB, which is unprecedented for velocimetry! Once the diagnostic was optimized, two two-week campaigns were conducted in the HTTF. This experimental campaign required numerous practical solutions to successfully and rapidly deploy this very sensitive table-top diagnostic in-situ. This was accomplished thanks to very extensive planning from all parties involved in the project. Due to constraints on availability of the HTTF, only adiabatic DCC tests were conducted. Specifically, the velocity was measured at the exit of the hot leg into the Reactor Cavity Simulation Tank (RCST). We were able to record the gas velocity associated with the air ingress for long times (up to one hour). Depending on the initial conditions (density of the gases in the Reactor Pressure Vessel and the RCST) the lock exchange lasted 30-60 s past the valve openings. Large vortices were identified within the shear layer at the interface of the cross flow. These vortices are an indication of shear-driven instability between the counter streams of different density. After the lock-exchange, a small residual flow was still present and its strength decayed exponentially. It finds its source in a buoyancy difference between the gases in both vessels due to the mixing and diffusion of the gases in the cross-over duct and the RPV lower plenum. We did not expect to capture this part of the transient, which would have been less significant (if not negligible) in the presence of a heated core; the precision of our measurement in the HTTF was 6 mm/s, which exceeded our expectations for such a complex test! Using commercial software (Fluent) we simulated the experiment with Computational Fluid Dynamic (CFD) using Reynolds Averaged Navier-Stokes (RANS) turbulence models. We were not able to accurately reproduce the shear layer instability, mixing, and diffusion captured in our experimental data, even with large 3D meshes (>10 M points). We attributed this to the inadequacy of the RANS models for the flow of interest: our experimental Reynolds number was too low and was outside the applicability range of the RANS models. Instead, we should have employed CFD with less modeling, such as Large Eddy (LES) or even Direct Numerical (DNS) simulations. Unfortunately, we did not have the computational resources to do so. Finally, it should be noted that this experimental technique holds great promises for measuring velocity in thermalhydraulics. MTV has an application domain (highlighted in the narrative) that is complimentary to more established (and simpler) techniques, such as PIV. It has attracted the attention of several thermalhydraulics researchers and sponsors to measure velocity in harsh environments. The spectroscopic nature of this technique also enables to expand it to measure temperature and concentration simultaneously to velocity. In lieu of a narrative, 4 detailed journal publications are appended to this executive summary to describe the various development and accomplishments during this project. They include 2 published manuscripts (Experiments in Fluids and Measurement Science and Technology), and two invited contributions following the NURETH-17 conference (Nuclear Science and Technology). Our current Nuclear Engineering and Design draft is not included at this time.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Extraordinary creep resistance in a non-equiatomic high-entropy alloy from the optimum solid-solution strengthening and stress-assisted precipitation process

Improving creep resistance has commonly been achieved by the optimization of alloy design that results into strong solid-solution strengthening and/or coherent precipitates for dislocation blockage. High-entropy alloys (HEAs), despite their single-phase solid-solution nature, only exhibit creep properties that are comparable to precipitate-strengthened ferritic alloys. Moreover, many HEAs are found to be plagued with many incoherent second phases after long-term annealing, which reduces the lifetime and thus prohibits their usage at elevated temperatures. The present work demonstrates the extraordinary creep resistance of a non-equiatomic Al 0.3 CoCrFeNi HEA, in which the creep strain rate is found to be several orders of magnitude lower than the Cantor alloy and its subsets. Using a suite of characterization tools such as atom probe tomography (APT) and transmission electron microscopy (TEM), it was shown that a B2 precipitate phase that has been widely seen during annealing is suppressed during the early stage of the creep deformation. Currently, metastable and coherent L1 2 precipitates emerge and provide significant creep strengthening. This observation is rationalized by the coupling between the applied stress and the lattice mismatch. In the range of 973 ~ 1033 K, the stress exponent and activation energy were determined to be 3–6.53 and 390–548.2 kJ·mol –1 , respectively. The creep lifetime, on the other hand, is comparable to Cantor subset alloys because the precipitate free zone near the grain boundaries does not provide sufficient constraint for the grain boundary cavity growth. Furthermore, the present work provides a pathway to design novel HEAs with improved creep resistance.

36 MATERIALS SCIENCE↗