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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Evaluation of the Radioactive Material Release in the Harborview Research and Training Building and Implications for Emergency Response

On May 2, 2019, during the 137 Cs source recovery operation, a source capsule in a research irradiator containing approximately 77.1 TBq was breached. Based on a geometric reconstruction analysis of the damage to the capsule, approximately 46.3 GBq (0.04%) was impacted by the chop saw (grinder) inside a Mobile Hot Cell (MHC) on the loading dock at the University of Washington Harborview Research and Training (HRT) Building. A very small fraction of the material impacted, less than 1%) was released from the Mobile Hot Cell and then to the rest of the HRT Building. The objectives of this project were to assess the accidental release of 137 CsCl and its implications related to emergency response methods and the ramifications of 137 CsCl transport. The phenomenology of this event was also compared with past alkali halide dispersal events. The vast number of measurements and samples collected by the remediation contractors, the Department of Energy's Nuclear Emergency Support Team, and the small number of retrospective samples collected by the authors informed the analysis. The techniques included (1) autoradiography and electron microscopy of samples collected from the HRT Building and the irradiator, (2) 3D visualization of deposition on surfaces and within the ventilation system, and (3) a study of the damage to the source capsule to evaluate the Cs particle size and particle composition due to the grinding accident. Subsequently, the cesium contaminant transport through the numerous pathways in the building was reconstructed to assess the deposition on surfaces as a function of particle size. The implications for emergency response are relevant to data quality and management. A Data Quality Objective (DQO) guides data collection methods so that they have appropriate accuracy and precision for the intended application. Recommendations were made with respect to the sample collection protocols and sample archival.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2024

Efficient simulations of charge density waves in the transition metal Dichalcogenide TiSe 2

Charge density waves (CDWs) in transition metal dichalcogenides are the subject of growing scientific interest due to their rich interplay with exotic phases of matter and their potential technological applications. Here, using density functional theory with advanced meta-generalized gradient approximations (meta-GGAs) and linear response time-dependent density functional theory (TDDFT) with state-of-the-art exchange-correlation kernels, we investigate the electronic, vibrational, and optical properties in 1T-TiSe 2 with and without CDW. In both bulk and monolayer TiSe 2 , the electronic bands and phonon dispersions in either normal or CDW (semiconducting) phase are described well via meta-GGAs, which separate the valence and conduction bands just as HSE06 does but with significantly more computational feasibility. The experimentally observed humps of electron energy loss spectroscopy are successfully reproduced in TDDFT. Our work opens the door to simulating these complexities in CDW compounds from first principles by revealing meta-GGAs as an accurate low-cost alternative to HSE06.

Electronic properties and materials↗
DOE OSTI2022

Design considerations for gallium arsenide pulse compression photoconductive switch

In this paper, we present the physics and design-space exploration of a novel pulse compression photoconductive switch (PCPS) using semi-insulating gallium arsenide (GaAs) operating in the negative differential mobility (NDM) regime of electron transport. We systematically quantify the relationship between the PCPS performance and various design options, including contact separation, laser energy and placement, and trap dynamics. Specifically, we report the full-width at half-maximum and the peak output current generated by the PCPS as a function of applied electrical and optical bias. We discuss the optimal spacing between the electrodes and the distance of the laser spot to the anode to achieve higher electron confinement and superior radio-frequency (RF) metrics. Reducing the laser energy is important to prevent the appearance of secondary peaks due to diffusive transport, but there exists a trade-off between the bandwidth and the maximum current of the PCPS. We also compare the PCPS response with and without trap dynamics and find that the electrostatic screening from the trap-induced space charge is time-independent when the trapping time constant is set larger than the recombination lifetime. Overall, trap dynamics are detrimental to performance, unless the compensation doping scheme to achieve semi-insulating GaAs is carefully selected. Results presented in this paper can be used by experimentalists to fine-tune the PCPS design parameters to meet the specifications of various RF applications. Moreover, our results will provide a strong theoretical basis to the measurements of PCPS devices using GaAs and other NDM materials under investigation.

42 ENGINEERING↗
DOE OSTI2020

Innovation in Radiological Security, Part 2 of 2 – Insights into Developing a Cloud-hosted Security Technology

A Sentry Remote Monitoring System (Sentry-RMS) is a stand-alone security system that provides detection, assessment, and communication of priority alarms as an additional means of thwarting internal and external threats to sites that maintain radiological material. The SEntry-RMS CommUnications and REsponse (Sentry-SECURE) platform is an optional feature of the Sentry-RMS that relays priority alarm information to the identified response stakeholders. Sentry-SECURE is hosted in a cloud environment that abstracts the data owner’s and data consumer’s platforms to allow for greater information sharing. This promotes situational awareness amongst authorized users and enables future innovation among modern response platforms. When securely architecting a cloud solution such as this, the use of design paradigms can be an effective tool to increase the accuracy and reliability of cyber- and information-security-related decisions made throughout the development process. This approach also supports the categorization of design considerations into three levels: industry concepts, project approaches, and data protections for digital processes. Industry concepts consist of the notional underpinnings that guide or motivate a security process, system, or design but often lack any tangible attributes. Project approaches represent decisions made during the design and development process to prioritize a solution, method, or practice above another that may provide a comparable functional output but lacks a desired security benefit. Data protections for digital processes represent the selection, integration, and implementation of specific controls for a given asset. This paper will explore specific examples of how Sentry-SECURE has been designed to account for considerations at each of these three levels, while balancing the operational intent of the platform with the security enhancements necessary to maintain data integrity, availability, and confidentiality.

assessment, RMS, security, physical, cloud, Cyber ↗
DOE OSTI2022

Screening of bimetallic electrocatalysts for water purification with machine learning

Electrocatalysis provides a potential solution to NO 3 - pollution in wastewater by converting it to innocuous N 2 gas. However, materials with excellent catalytic activity are typically limited to expensive precious metals, hindering their commercial viability. Here, in response to this challenge, we have conducted the most extensive computational search to date for electrocatalysts that can facilitate NO 3 - reduction reaction, starting with 59 390 candidate bimetallic alloys from the Materials Project and Automatic-Flow databases. Using a joint machine learning- and computation-based screening strategy, we evaluated our candidates based on corrosion resistance, catalytic activity, N 2 selectivity, cost, and the ability to synthesize. We found that only 20 materials will satisfy all criteria in our screening strategy, all of which contain varying amounts of Cu. Our proposed list of candidates is consistent with previous materials investigated in the literature, with the exception of Cu–Co and Cu–Ag based compounds that merit further investigation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Toward Decoding the Relationship between Domain Structure and Functionality in Ferroelectrics via Hidden Latent Variables

Polarization switching mechanisms in ferroelectric materials are fundamentally linked to local domain structure and the presence of the structural defects, which both can act as nucleation and pinning centers and create local electrostatic and mechanical depolarization fields affecting wall dynamics. However, the general correlative mechanisms between domain structure and polarization dynamics are only weakly explored, precluding insight into the associated physical mechanisms. In this work, the correlation between local domain structures and switching behavior in ferroelectric materials is explored using convolutional encoder–decoder networks, enabling image to spectral (im2spec) and spectral to image (spec2im) translations via encoding of latent variables. The latter reflect the assumption that the relationship between domain structure and polarization switching is parsimonious, i.e., is based upon a small number of local mechanisms. The analysis of latent variables distributions and their real-space representations provides insight into the predictability of the local switching behavior and hence associated physical mechanisms. We further pose that the regions where these correlative relationships are violated, i.e., predictability of the polarization dynamics from domain structure is reduced, represent the obvious target for detailed studies, e.g., in the context of automated experiments. This approach provides a workflow to establish the presence of correlation between local spectral responses and local structure and can be universally applied to spectral imaging techniques such as piezoresponse force microscopy (PFM), scanning tunneling microscopy (STM) and spectroscopy, and electron energy loss spectroscopy (EELS) in scanning transmission electron microscopy (STEM).

36 MATERIALS SCIENCE↗
DOE OSTI2024

Failure Analysis for Molten Salt Thermal Energy Storage Tanks for In-Service CSP Plants

Thermal Energy Storage (TES) is a fundamental component in concentrating solar power (CSP) plants to increase the plant's dispatchability, capacity factor, while reducing the levelized cost of electricity. In central receivers CSP plants, nitrate molten salts have been used for several years for operation temperatures of up to 565 degrees C. Despite many efforts to advance nitrate salt to higher operation temperatures (even considering a replacement with molten chloride salts) to achieve higher energy conversion efficiencies, the 565 degrees C temperature is currently considered the state-of-the art. Although molten salt tanks have been broadly deployed in commercial CSP plants worldwide, several failures have been reported in these tanks after a few months or years of operation, causing significant economic loss and mistrust in CSP technologies. Most of these failures are associated with the infancy of the technology and multiple issues related to tank design, fabrication, commissioning, and aggressive operation. A technical standard dedicated to the design and fabrication of molten nitrate TES tanks does not exist today. Current in-service molten salt tanks have been generally designed based on the American Petroleum Institute's (API) 650 and ASME Section II standards. The API 650 code provides guidelines for dimensions and fabrication for oil storage tanks up to 260 degrees C. The ASME standard provides allowable stress values for various materials at a range of temperatures and conditions. Both standards seem to be limited for molten salt TES tanks where high temperatures, thermal cycling, and transient conditions are expected. In 2020, NREL released the Concentrating Solar Power Best Practices Study (NREL/TP-5500-75763) that summarized multiple issues in CSP plants, along with potential alternatives and recommendations to address those issues based on information collected from participants representing about 80% of operating CSP plants in the world. One of the recommendations from this study was the development of accurate and validated models to evaluate the plant's transient operation, capable of capturing the effect of short-term clouds and operator response, while being flexible in being adapted to various spatial and temporal resource data. The "Failure Analysis for Molten Salt Thermal Energy Tanks for In-Service CSP Plants" project was inspired on this recommendation and was focused on (1) the development and validation of a physics-based model for a representative, commercial-scale molten salt tank, (2) performing simulations to evaluate the behavior of the tank as a function of typical plant operation conditions, (3) understanding tank failures mechanisms, (4) determining the residual stress and distortion in the tank floor after welding fabrication and evaluating their impact in the stresses developed in the tank during operation, (5) assessing the impact of key operation parameters on the temperature and stress distribution, (6) conduct a preliminary evaluation of design features to reduce stress and improve tank's reliability, and (7) estimate the tank's service life based on the stress developed under diverse operation scenarios. From the analysis conducted in the project and presented in this report, it was found that maximum stresses surpassing the yield strength point of the stainless steel (SS) 347H are developed on the tank floor near the perimeter. These large stresses are strongly influenced by the initial residual stresses and distortion of the tank floor after welding fabrication. During operation, large stresses are developed in the tank floor at high operation temperatures with large salt inventory levels during transient operation. High stresses are also related to elevated temperature gradients in the tank floor that could be attributed to insufficient mixing within the salt inflow and the salt inventory. Based on the analysis, creep is the predominant failure mechanism. However, the large stress levels could favor the plastic deformation into buckles, and crack formation due to stress relaxation cracking during cycle operation. A lifetime below 3 years was estimated for the typical plant operation conditions and a specific initial residual stress and deformation distribution of the tank floor. The estimated life agrees with the service time to failure reported in several commercial molten salt tanks. Desing and operation guidelines can be extracted from the analysis presented in this report, which could be adopted by tank manufacturers and CSP operators to advance toward an ultimate solution for tank failures by reducing residual and operational stresses to achieve a tank service life of more than 30 years. Addressing failures in molten salt TES tanks is fundamental for the CSP industry's survivability, but it is also important for other industrial and power generation applications using this technology, including nuclear and concentrating solar thermal.

14 SOLAR ENERGY↗
DOE OSTI2026

Transitions, Dynamics, and Driven States in Quantum Magnets (Final Report Revised)

Transitions into unusual electronic, optical, and magnetic states at the absolute zero of temperature display special properties that teach us about fundamental quantum mechanics and also underlie important technologies. These so-called quantum phase transitions intertwine the static and dynamical responses of the materials changing state. They are extremely sensitive to the effects of disorder and etch in high relief the role of quantum fluctuations. There are ample questions remaining about the character of such transitions and the nature of the competing quantum states. There are also opportunities to drive quantum materials out of equilibrium, with the possibility of new types of correlated and coherent order, and new ways to access the dynamical evolution of ground and excited states. We have investigated how the order develops in time and space, and the nature of the final configurations. We are able to compare and contrast classical and quantum excitations in our experimental system of choice, and thereby can trace the relative speed by which the system settles into its lowest-energy ground state. This comparison of quantum and classical annealing protocols lies at the heart of strategies for harnessing the power of quantum computers dedicated to optimization problems. A combination of magnetic susceptibility measurements at finite frequency where the magnetic spins are queried by an external ac field, dc magnetometry measurements that characterize the macroscopic strength of magnetic order and its resistance to change, noise measurements that reveal the microscopic fluctuations of the spins as they prepare to change state, and microwave spectroscopy to look at the response of both the electronic and nuclear degrees of freedom, have been performed as functions of temperature, magnetic field, frequency, excitation amplitude, magnetic spin concentration, and disorder. This combination of probes addresses issues of stability over time, overlap between spin states, the ability of the spins to respond independently or coherently, and the promise of control on the nanometer length scale. The research reported here provides insights into fundamental quantum physics. It also addresses the question of how best to use complex systems, such as magnetic solids, to stably process quantum information.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Pressure-induced evolution of the lattice dynamics for selected UO 3 polymorphs

Uranium trioxide (UO 3 ) is a stable chemical form of uranium oxide with multiple polymorphs found throughout the nuclear fuel cycle. The pressure-induced changes in the structure and lattice dynamics of four of these polymorphs are simulated with density functional perturbation theory and analyzed. Two phases, α- and δ-UO 3 are found to exhibit an isotropic response to pressure and do not undergo any changes in coordination geometry up to ~40 GPa. In contrast, the other two phases investigated, β- and γ-UO 3 , exhibit an anisotropic response to pressure. Decomposition of the phonon eigenvectors allows us to assign specific pressure-induced structural changes to individual phonon modes. Here, this analysis has been performed on a per atom basis for the relatively simple α- and δ-UO 3 structures, which have one symmetrically unique uranium site, and on a per coordination environment basis for β- and γ-UO 3 , which have multiple U sites.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Fabrication of metal-organic framework thin films for luminescent sensing applications

Metal−organic frameworks (MOFs) have emerged as an exciting material class due to their nearly infinite design space: an inexhaustible combination of metal centers, organic linkers, and reaction conditions may be leveraged to obtained desired optical, physical, and chemical properties. This rich synthetic diversity enables properties such as pore dimensions and functionality to be rationally tailored for highly selective and sensitive detection of target analytes. Luminescent MOF-based sensors in particular offer advantages including low cost, portability, and ease-of-use. Often, performance is maximized by utilizing the luminescent MOF in thin film form, for example by integrating the film onto an optical fiber, yet the synthesis of high-quality MOF thin films often requires tedious, expensive, and/or slow approaches. Here, we demonstrate a rapid, simple strategy for growing copper MOFs using metal oxide templates; the concept is first demonstrated with a well-studied system, copper-1,3,5-benznetricarboxylate (Cu-BTC). Variables such as the choice of solvent, pH, and the choice of the copper salt anion all govern thin film quality. We then extend this method to synthesize a solvent and metal-responsive copper MOF that is particularly effective at detecting aluminum, an economically critical metal, at trace concentrations using a fully portable luminescence spectrometer. Taken together, this work demonstrates a convenient, versatile, and sustainable method for developing high quality MOF thin film-based optical sensors.

Crawford, Scott↗
DOE OSTI2022

Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance

Abstract Metal oxides are an important class of functional materials, and for many applications, ranging from solid oxide fuel/electrolysis cells, oxygen permeation membranes, and oxygen storage materials to gas sensors (semiconducting and electrolytic) and catalysts, the interaction between the surface and oxygen in the gas phase is central. Ubiquitous Si‐impurities are known to impede this interaction, commonly attributed to the formation of glassy blocking layers on the surface. Here, the surface oxygen exchange coefficient ( k chem ) is examined for Pr 0.1 Ce 0.9 O 2‐δ (PCO), a model mixed ionic electronic conductor, via electrical conductivity relaxation measurements, and the area‐specific resistance (ASR) by electrochemical impedance spectroscopy. It is demonstrated that even low silica levels, introduced by infiltration, depress k chem by a factor 4000, while the ASR increases 40‐fold and we attribute this to its acidity relative to that of PCO. The ability to fully regenerate the poisoned surface by the subsequent addition of basic Ca‐ or Li‐species is further shown. This ability to not only recover Si‐poisoned surfaces by tuning the relative surface acidity of an oxide surface, but subsequently outperform the pre‐poisoned response, promises to extend the operating life of materials and devices for which the catalytic oxygen/solid interface reaction is central.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2020

All-solid-state Z-scheme BiVO 4 –Bi 6 O 6 (OH) 3 (NO 3 ) 3 heterostructure with prolonging electron-hole lifetime for enhanced photocatalytic hydrogen and oxygen evolution

As a visible-light response photocatalyst, BiVO 4 is widely used in photocatalytic oxygen evolution. In this study, a novel BiVO 4 –Bi 6 O 6 (OH) 3 (NO 3 ) 3 (BBN) heterostructure fabricates via a simple one-pot hydrothermal approach is certified to effectively restrain the recombination of carriers by efficient spatial charge separation. By employing BBN as a reductive-function photocatalyst, a solid-state Z-scheme is constructed to improve the photo-redox capacity of BiVO 4 and hydrogen production is realized in the BiVO 4 –BBN heterostructure for the first time. Furthermore, the solid-state Z-scheme introduced in the BiVO 4 –BBN ensures the photoexcited carriers with the powerful redox capacity to participate in the photocatalytic reaction.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields

A key component of cooling devices is the transfer of entropy from the cold load to heat sink. An electrocaloric (EC) polymer capable of generating both large electrocaloric effect (ECE) and substantial electroactuation can enable EC cooling devices to pump heat without external mechanisms, resulting in compact designs and enhanced efficiency. However, achieving both high ECE and significant electroactuation remains challenging. Herein, it is demonstrated that poly(vinylidene fluoride‐trifluoroethylene‐chlorofluoroethylene‐double bond) [P(VDF‐TrFE‐CFE‐DB)] tetrapolymers can simultaneously generate high electrocaloric effects and electroactuations under low fields. These P(VDF‐TrFE‐CFE‐DB) tetrapolymers are synthesized through the dehydrochlorination of P(VDF‐TrFE‐CFE) terpolymer. By facile tuning the composition of the initial terpolymer to avoid pure relaxor state, tetrapolymers with optimal DB compositions are achieved, near the critical endpoint of normal ferroelectric phase with diffused phase transition. The nearly vanishing energy barriers between the nonpolar to polar phases result in a strong electrocaloric response and significant electroactuation. Specifically, the P(VDF‐TrFE‐CFE‐DB) tetrapolymer exhibits an EC entropy change Δ S of 100 J kg −1 K −1 under 100 MV m −1 : comparable to state‐of‐the‐art (SOA) EC polymers, while delivering nearly twice the electroactuation of the SOA EC polymers. This work presents a general strategy for developing EC materials that combine large electrocaloric effect and electroactuation at low electric fields.

36 MATERIALS SCIENCE↗
DOE OSTI2021

All-aerosol-jet-printed highly sensitive and selective polyaniline-based ammonia sensors: a route toward low-cost, low-power gas detection

In this work, we report the design and scalable fabrication of a low-cost and low-power polyaniline-based (PANI) ammonia (NH3) gas sensor on polyimide (PI) substrates using additive manufacturing techniques. The silver interdigitated electrode (IDE) arrays and conducting polymer films are printed onto PI using a direct-write technology of aerosol-jet printing. Morphological characteristics are examined by scanning electron microscopy and energy-dispersive X-ray analysis which reveal homogeneously printed PANI film on the IDE platform. The gas sensing performance is evaluated in the analytical early leak detection range of 5–1000 ppm NH3 in air as a function of both thermal (23 °C, 50 °C, 80 °C) and relative humidity (RH = 0%, 30%, 50%) exposures. The sensor exhibits sensitivity down to 5 ppm NH3 with a sub-ppm detection limit and good repeatability. We observe rapid NH3 detection at 0% RH with very extended times for equilibration and recovery. However, at both 30 and 50% RH, the room temperature response and recovery times are reduced to only about 1 min and 5 min, respectively. Experiments also reveal good sensitivity toward the analyte even at higher operating temperatures. Present results merit the practical application of aerosol-jet-printed, low-power sensors for industrial applications where low-level hazardous gas detection is essential.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Mesoscale simulations of High Burnup Fuel Fragmentation: Applying phase-field modeling to understand high burnup fuel fragmentation during loss of coolant accident conditions

During a loss-of-coolant accident (LOCA) in a nuclear power plant, a rapid increase in temperature is experienced in the fuel. In commercial light water reactors (LWRs), the high burnup structure (HBS) forms in regions of the UO 2 fuel where local burnup is high, characterized by smaller grain sizes and large, overpressurized bubbles. During a LOCA transient, fuel in the HBS region is susceptible to fine fragmentation, where the fuel breaks up into micron-size fragments (sometimes referred to as pulverization). To better understand the mechanisms behind this phenomenon, mesoscale computational modeling using the Idaho National Laboratory code Marmot has been employed to simulate the process of HBS formation and response to a LOCA transient. The process of complete and partial HBS formation was demonstrated in prototypical LWR conditions. The simulated HBS microstructures from these simulations were passed to a phase-field model of fracture. To provide a more direct comparison with experiments, a set of experiments conducted by Studsvik on fine fragmentation/pulverization during LOCA conditions was simulated using the BISON fuel performance code. The temperature profiles from the BISON simulations were passed to a phase-field model to determine the gas bubble pressure as a function of time. These pressure histories were used in a phase-field model of fracture to determine under what conditions and in which types of bubbles fine fragmentation was likely to occur.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Size-dependent errors in real-time electron density propagation

Real-time (RT) electron density propagation with time-dependent density functional theory (TDDFT) or Hartree–Fock (TDHF) is one of the most popular methods to model the charge transfer in molecules and materials. However, both RT-TDHF and RT-TDDFT within the adiabatic approximation are known to produce inaccurate evolution of the electron density away from the ground state in model systems, leading to large errors in charge transfer and erroneous shifting of peaks in absorption spectra. Given the poor performance of these methods with small model systems and the widespread use of the methods with larger molecular and material systems, here we bridge the gap in our understanding of these methods and examine the size-dependence of errors in RT density propagation. We analyze the performance of RT density propagation for systems of increasing size during the application of a continuous resonant field to induce Rabi-like oscillations, during charge-transfer dynamics, and for peak shifting in simulated absorption spectra. We find that the errors in the electron dynamics are indeed size dependent for these phenomena, with the largest system producing the results most aligned with those expected from linear response theory. The results suggest that although the RT-TDHF and RT-TDDFT methods may produce severe errors for model systems, the errors in charge transfer and resonantly driven electron dynamics may be much less significant for more realistic, large-scale molecules and materials.

Chemistry↗
DOE OSTI2022

Vacancy-Driven Disorder and Elevated Dielectric Response in the Pyrochlore Pb 1.5 Nb 2 O 6.5

Lone pair-driven distortions are a hallmark of many technologically important lead (Pb)-based materials. Here, the role of Pb 2+ in polar perovskites is well understood and easily manipulated for applications in piezo- and ferroelectricity, but the control of ordered lone pair behavior in Pb-based pyrochlores is less clear. Crystallographically and geometrically more complex than the perovskite structure, the pyrochlore structure is prone to geometric frustration of local dipoles due to a triangular arrangement of cations on a diamond lattice. The role of vacancies on the O' site of the pyrochlore network has been implicated as an important driver for the expression and correlation of stereochemically active lone pairs in pyrochlores such as Pb 2 Ru 2 O 6.5 and Pb 2 Sn 2 O 6 . In this work we report on the structural, dielectric, and heat capacity behavior of the cation- and anion-deficient pyrochlore Pb 1.5 Nb 2 O 6.5 upon cooling. We find that local distortions are present at all temperatures that can be described by cristobalite-type cation ordering, and this ordering persists to longer length scales upon cooling. From a crystallographic perspective, the material remains disordered and does not undergo an observable phase transition. In combination with density function calculations, we propose that the stereochemical activity of the Pb 2+ lone pairs is driven by proximity to O' vacancies, and the crystallographic site disorder of the O' vacancies prohibits long range correlation of lone pair-driven distortions. This in turn prevents a low-temperature phase transition and results in an elevated dielectric permittivity across a broad temperature range.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Need for advanced research reactors for the next-generation reactor physics, analysis tools, and technology

Full text of publication follows. There is an urgent need for design and deployment of advanced research and test reactors in support of design, licensing and operation of advanced power reactors and education of next generation nuclear workforce. Existing research reactors mostly were designed and constructed decades ago with the main objectives of training operators, performing reactor physics experiments, and educating nuclear engineers and scientists. There are already gaps and significant concern about future capabilities for the existing research reactor facilities to address modern instrumentation and/or flexible environments for: performing reactor physics studies for advanced designs which have significantly different core materials forms and compositions, reactor shapes and size; validation of advanced high-fidelity software; development of machine learning algorithms for enhancement of human-machine collaboration in support of reactor monitoring, operation and safeguards; and, effective education of the next-generation workforce. The authors will focus on the need for advanced research reactors to improve and validate fast and accurate simulation tools for high-fidelity modeling and analysis of nuclear reactors in support of their design, optimization, licensing, operation, and monitoring. In the past, simulation tools were limited to relatively coarse models using approximate methodologies that benefited from two main factors: i) allowance for large margins and tolerances; ii) ability to construct prototype (e.g., zero power) reactors for adjustment of approximate methodologies. The next generation reactors have to be designed mainly by using novel high-fidelity computational tools that are accurate and fast, and therefore can be used for parametric studies and uncertainty quantification. To sufficiently demonstrate the accuracy of these tools, advanced research reactors are needed. The authors argue the need for new computational paradigms such as the MRT (Multistage, Response- function Transport) methodology which has resulted in the development of the novel high-fidelity RAPID (Real-time Analysis for Particle-transport and In-situ Detection) code system. Such code systems have to be robust in modeling any complex system, and should be fast and accurate, henceforth their uncertainties can be quantified at reasonable costs. Again, advanced research reactors are needed for the validation of the fidelity and accuracy of new computational tools. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗