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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 OSTI2020

The ongoing need for high-resolution regional climate models: Process understanding and stakeholder information

Regional climate modeling addresses our need to understand and simulate climatic processes and phenomena unresolved in global models. High resolution models are generally more skillful in simulating extremes, such as heavy precipitation, strong winds, and severe storms. In addition, research has shown that fine-scale features such as mountains, coastlines, lakes, irrigation, land use, and urban heat islands can substantially influence a region’s climate and its response to changing forcings. Regional climate simulations explicitly simulating convection are now being performed, providing an opportunity to illuminate new physical behavior that previously was represented by parameterizations with large uncertainties. Regional and global models are both advancing toward higher resolution, as computational capacity increases. However, the resolution and ensemble size necessary to produce a sufficient statistical sample of these processes in global models has proven too costly for contemporary supercomputing systems. Regional climate models are thus indispensable tools that complement global models for understanding regional climate variability and change, and are critical for supporting societal responses to changing climate.

Gutowski, William↗
DOE OSTI2015

A combined maximum-likelihood analysis of the high-energy astrophysical neutrino flux measured with IceCube

Evidence for an extraterrestrial flux of high-energy neutrinos has now been found in multiple searches with the IceCube detector. The first solid evidence was provided by a search for neutrino events with deposited energies ≳30 TeV and interaction vertices inside the instrumented volume. Recent analyses suggest that the extraterrestrial flux extends to lower energies and is also visible with throughgoing, ν{sub μ}-induced tracks from the Northern Hemisphere. Here, we combine the results from six different IceCube searches for astrophysical neutrinos in a maximum-likelihood analysis. The combined event sample features high-statistics samples of shower-like and track-like events. The data are fit in up to three observables: energy, zenith angle, and event topology. Assuming the astrophysical neutrino flux to be isotropic and to consist of equal flavors at Earth, the all-flavor spectrum with neutrino energies between 25 TeV and 2.8 PeV is well described by an unbroken power law with best-fit spectral index −2.50 ± 0.09 and a flux at 100 TeV of (6.7{sub −1.2}{sup +1.1})×10{sup −18} GeV{sup −1} s{sup −1} sr{sup −1} cm{sup −2}. Under the same assumptions, an unbroken power law with index −2 is disfavored with a significance of 3.8σ (p = 0.0066%) with respect to the best fit. This significance is reduced to 2.1σ (p = 1.7%) if instead we compare the best fit to a spectrum with index −2 that has an exponential cut-off at high energies. Allowing the electron-neutrino flux to deviate from the other two flavors, we find a ν{sub e} fraction of 0.18 ± 0.11 at Earth. The sole production of electron neutrinos, which would be characteristic of neutron-decay-dominated sources, is rejected with a significance of 3.6σ (p = 0.014%).

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Mechanical Performance and Mesostructure Analysis of Proton-Irradiated Fused Filament Fabrication Acrylonitrile Butadiene Styrene Material

The use of fused filament fabrication (FFF) acrylonitrile butadiene styrene (ABS) and other thermoplastics in radiation environments is beginning to be studied as possible replacements for traditionally manufactured parts and tools. Interlayer adhesion within the mesostructure has been shown in published literature to be an integral component in the strength of FFF ABS. Research of irradiated 3D printed polymers has primarily focused on the influence of gamma irradiation on the mechanical properties of FFF ABS samples, without evaluating its impact on the mesostructure of the samples. The purpose of this paper is to understand the mechanical damage caused by proton radiation on FFF ABS samples through the evaluation of the mesostructure of the ABS samples. To achieve this objective, proton radiation at 40 MeV was applied to FFF ABS samples at radiation doses up to 1.0 MGy at a dose rate of 1 MGy/hr. Following the irradiation, tensile testing was performed on the samples. Here, the fractured surfaces of the tested samples were subsequently observed using a scanning electron microscope. The mechanical test results show an increase in the ultimate tensile strength (UTS) and a decrease in the ductility of the irradiated samples. Statistical analysis on the results shows that there is a statistically significant difference in the UTS and the ductility of unirradiated and 1.0 MGy irradiated samples and between irradiated samples and 1.0 MGy samples. In addition, the percentage elongation at break has statistically significant differences in the means between irradiated samples and 1.0 MGy samples. The UTS has statistically significant differences in the means between 0.1 MGy and 1.0 MGy. The difference in the means between the unirradiated and the 1.0 MGy samples is the most significant for both the UTS and elongation at break. The scanning electron microscopy (SEM) results indicated that interlayer adhesion improved as a function of radiation dose corresponding to the increase in tensile strength. The SEM results also showed that crazing and plastic deformation were reduced; aligning with the loss in ductility observed in the tensile tests results. The proton radiation is causing these mechanical and physical changes through two mechanisms: (1) dose rate effects on ionizing radiation-induced oxidative degradation; and (2) radiation heating effects of high energy (>1 MeV) charged particles.

electron microscopy↗
DOE OSTI2025

First observation of antiproton annihilation at rest on argon in the LArIAT experiment

We report the first observation and measurement of antiproton annihilation at rest on argon track and shower multiplicities and particle identification conducted with the LArIAT experiment. Stopping antiprotons from the Fermilab Test Beam Facility’s charged particle test beam are identified using beamline instrumentation and LArIAT’s liquid argon time projection chamber (LArTPC). The charged particle multiplicity from the annihilation vertex is manually evaluated via hand scanning, yielding a mean of 3.2 ± 0.4 tracks and a standard deviation of 1.3 tracks, consistent with a semiautomated reconstruction resulting in 2.8 ± 0.4 tracks and a standard deviation of 1.2 tracks. Both methods are consistent with Monte Carlo simulations within statistical uncertainty. The shower multiplicities and particle identification for outgoing tracks are also consistent with eant4 model predictions. These results, obtained from a low-statistics sample, provide a foundation for higher-statistics studies in larger LArTPCs, which could refine modeling of intranuclear annihilation on argon and inform scenarios such as neutron-antineutron oscillations. Published by the American Physical Society 2025

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

S0 Uncrewed Aircraft System Measurement Characterization Field Campaign Report

The lower atmosphere contributes directly to the modulation of weather and climate. Understanding the importance of this part of the atmosphere, scientists have worked to improve the representation of the atmospheric boundary layer in numerical prediction tools. Such work depends upon information from observing systems, including remote sensors, weather balloons, and research aircraft. Recent years have seen significant advances in uncrewed aircraft systems (UAS) for atmospheric research. Those efforts have provided new perspectives on atmospheric and surface conditions, particularly from smaller UAS (sUAS) platforms. This field campaign included collection of data using several sUAS, and comparing the sUAS data to those from different observing facilities at the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s Southern Great Plains (SGP) observatory in Oklahoma. Over the course of one week, the Black Swift Technologies and University of Nebraska teams conducted flights for the sole purpose of system evaluation and intercomparison. In addition, these teams conducted joint flight operations at the Marshall, Oklahoma Mesonet site alongside teams from the University of Colorado, University of Oklahoma, and Oklahoma State University to collect additional data for side-by-side comparison. Platforms operated by Black Swift Technologies and the University of Nebraska under this project included one fixed-wing and two rotary-wing platforms, as well as an instrumented surface vehicle. These include the Black Swift Technologies S0 UAS, the University of Nebraska M600 UAS, a University of Nebraska-operated Meteomatics Meteodrone UAS, and the University of Nebraska CoMeT (Combined Mesonet and Tracker) vehicle. Additional details on all of these platforms can be found in de Boer et al. (in prep). In total, 95 sUAS flights were conducted for a combined total of 18.6 flight hours. The S0 was operated both to the south and north of the SGP 60 m tower, while the M600 and Meteodrone were operated directly to the east of the tower. Weather conditions were generally good, with moderate winds. Flights were conducted both to follow the extra radiosondes that were launched as part of this campaign, as well as to conduct extended statistical sampling at tower instrument heights. The later flights also provided data for statistical platform intercomparison.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Foundational Principles for Large-Scale Inference: Illustrations Through Correlation Mining

When can reliable inference be drawn in the ‘‘Big Data’’ context? This article presents a framework for answering this fundamental question in the context of correlation mining, with implications for general large-scale inference. In large-scale data applications like genomics, connectomics, and eco-informatics, the data set is often variable rich but sample starved: a regime where the number n of acquired samples (statistical replicates) is far fewer than the number p of observed variables (genes, neurons, voxels, or chemical constituents). Much of recent work has focused on understanding the computational complexity of proposed methods for ‘‘Big Data.’’ Sample complexity, however, has received relatively less attention, especially in the setting when the sample size n is fixed, and the dimension p grows without bound. To address this gap, we develop a unified statistical framework that explicitly quantifies the sample complexity of various inferential tasks. Sampling regimes can be divided into several categories: 1) the classical asymptotic regime where the variable dimension is fixed and the sample size goes to infinity; 2) the mixed asymptotic regime where both variable dimension and sample size go to infinity at comparable rates; and 3) the purely high-dimensional asymptotic regime where the variable dimension goes to infinity and the sample size is fixed. Each regime has its niche but only the latter regime applies to exa-scale data dimension. We illustrate this high-dimensional framework for the problem of correlation mining, where it is the matrix of pairwise and partial correlations among the variables that are of interest. Correlation mining arises in numerous applications and subsumes the regression context as a special case. We demonstrate various regimes of correlation mining based on the unifying perspective of high-dimensional learning rates and sample complexity for different structured covariance models and different inference tasks.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

(U) A General-Purpose Code for Correlated Sampling Using Batch Statistics with MCNP6 for Fixed-Source Problems

Correlated sampling can be used to reduce the uncertainty of a difference of tallies by taking advantage of the negative covariance term in the sandwich formula. Booth first showed how correlated sampling can be applied with batch statistics using MCNP’s tally fluctuation chart (TFC) to reduce the uncertainty of a difference of tallies in fixed-source problems. Booth presented a problem in which a 1273% uncertainty in a difference was reduced to 8% by accounting for correlations. Researchers He and Su recently studied correlated sampling using the TFC in MCNP version 5. They determined that the code did not print enough digits in the TFC tally means for accurate batch statistics in some cases. After modifying the source code, they concluded that “correlated sampling can yield a standard deviation of about one magnitude smaller than that predicted by the direct, un-correlated simulation when the changes in system response are small (say about 1%), which is equivalent to saving in CPU time by a factor of 100. Such saving [sic] becomes less significant as the change in system response becomes larger.” He and Su provided the formulas needed to apply batch statistics to compute the correlated uncertainty of a difference of tallies. In this report, we follow up on their work by providing the formulas needed to apply batch statistics to compute the correlated uncertainty of a ratio of tallies and of a difference of two tallies divided by a third tally. We extend these formulas to differences and ratios of ratios. These formulas are applied to reduce the uncertainty associated with calculating a relative sensitivity. He and Su did not investigate the accuracy of their correlated sampling uncertainty estimates. We use their test problems and evaluate the accuracy of the uncertainty estimates by comparing with results obtained from random sampling, and, in simple cases, with theoretical values of the “exact” uncertainties. We find that the uncertainties obtained from batch statistics are accurate as long as at least 100 batches are used. We present a new computer code, COSUBS (COrrelated Sampling Using Batch Statistics), that reads MCNP6 TFCs and applies correlated sampling using batch statistics for the tally combinations that the user specifies. COSUBS is a very general tool that compares all TFCs for a base case and one or two perturbed cases. It computes uncertainties for ratios if given only a base case. This report is organized as follows. The equations to apply batch statistics to the difference of random tallies are reviewed in Sec. II. Section III presents the equations for applying batch statistics to a ratio of random tallies; this is useful for computing relative sensitivities using a one-sided finite difference and the relative sensitivity using the differential operator method. Section IV presents the equations for applying batch statistics to a difference of two random tallies divided by a third; this is useful for computing a relative sensitivities using a central difference. Section V presents the equations for applying batch statistics to a difference of two ratios with four random tallies. Section VI presents the equations for applying batch statistics to a one-sided finite difference estimate of the relative sensitivity of a ratio (this uses four random tallies). Section VII presents the equations for applying batch statistics to a central difference estimate of the relative sensitivity of a ratio (this uses six random tallies). Section VIII presents the equations for applying batch statistics to a sum of random tallies. Section IX discusses how to apply batch statistics using MCNP6. Section X presents COSUBS, describing its command-line options and logic. Sections XI through XVI present numerical results for various test problems. Section XVII is a summary and conclusions. Appendix A derives the theoretical Monte Carlo tally variance given certain assumptions; these variances are used to verify the batch statistics for some of the problems. Appendix B lists the MCNP6 input for the unperturbed example problem. Appendix C presents modifications made to MCNP6.3 to support this work.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2016

THE ALFALFA H α SURVEY. I. PROJECT DESCRIPTION AND THE LOCAL STAR FORMATION RATE DENSITY FROM THE FALL SAMPLE

The ALFALFA H α survey utilizes a large sample of H i-selected galaxies from the ALFALFA survey to study star formation (SF) in the local universe. ALFALFA H α contains 1555 galaxies with distances between ∼20 and ∼100 Mpc. We have obtained continuum-subtracted narrowband H α images and broadband R images for each galaxy, creating one of the largest homogeneous sets of H α images ever assembled. Our procedures were designed to minimize the uncertainties related to the calculation of the local SF rate density (SFRD). The galaxy sample we constructed is as close to volume-limited as possible, is a robust statistical sample, and spans a wide range of galaxy environments. In this paper, we discuss the properties of our Fall sample of 565 galaxies, our procedure for deriving individual galaxy SF rates, and our method for calculating the local SFRD. We present a preliminary value of log(SFRD[ M {sub ⊙} yr{sup −1} Mpc{sup −3}]) = −1.747 ± 0.018 (random) ±0.05 (systematic) based on the 565 galaxies in our Fall sub-sample. Compared to the weighted average of SFRD values around z ≈ 2, our local value indicates a drop in the global SFRD of a factor of 10.2 over that lookback time.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Parametric description of intermittent probability distribution functions in solar wind and magnetohydrodynamic turbulence

ABSTRACT In this work, we find empirical evidence that the scale-dependent statistical properties of solar wind and magnetohydrodynamic (MHD) turbulence can be described in terms of a family of parametric probability distribution functions (PDFs) known as Normal Inverse Gaussian (NIG). Understanding these PDFs is one of the most important goals in turbulence theory, as they are inherently connected to the intermittent properties of solar wind turbulence. We investigate the properties of PDFs of Elsasser increments based on a large statistical sample from solar wind observations and high-resolution numerical simulations of MHD turbulence. In order to measure the PDFs and their corresponding properties, three experiments are presented: fast and slow solar wind for experimental data and a simulation of reduced MHD (RMHD) turbulence. Conditional statistics on a 23-yr-long sample of WIND data near 1 au and high-resolution pseudo-spectral simulation of steadily driven RMHD turbulence on a $2048^3$ mesh are used to construct scale-dependent PDFs. The empirical PDFs are fitted to NIG distributions, which depend on four free parameters. Our analysis shows that NIG distributions accurately capture the evolution of the PDFs, with scale-dependent parameters, from large scales characterized by a Gaussian distribution, turning to exponential tails within the inertial range and stretched exponentials at dissipative scales. We also show that empirically-measured NIG parameters exhibit well-defined scaling properties that are similar across the three empirical data sets, which may be indicative of universal behaviour.

Astronomy & Astrophysics↗
DOE OSTI2017

Statistical interpretation of the Amerithrax “morph” assay results

In the Amerithrax investigation PCR–based “morph assays” were used to link the anthrax letters with the RMR–1029 flask at USAMRIID. Quantitative data reported for several of these assays are not consistent with Poisson sampling statistics, but instead exhibit “Taylor's Law” behavior where the variance greatly exceeds the mean. A plausible statistical model for this behavior can explain the large number of observed negative and “inconclusive” findings, and implies a high likelihood that a repository sample could contain a “morph” mutant at concentrations well above the nominal detection limit but nonetheless give a negative or inconclusive test result. A Bayesian framework relates the assay results to the probability that a sample actually contains all four morph mutants, even though it tested negative for at least one. The analysis implies that the observed false negative rate actually does not significantly weaken the conclusion that the morph assays correctly excluded all but the stocks derived from RMR–1029 as possible sources of the letter powders, at least when the test results were unambiguous. In conclusion, these findings expand upon and resolve some of the issues cited in recent reviews, and indicate the importance of developing a rigorous statistical framework for interpreting “morph” assay data.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2015

Neutron/Gamma-ray discrimination through measures of fit

Statistical tests and their underlying measures of fit can be utilized to separate neutron/gamma-ray pulses in a mixed radiation field. In this article, first the application of a sample statistical test is explained. Fit measurement-based methods require true pulse shapes to be used as reference for discrimination. This requirement makes practical implementation of these methods difficult; typically another discrimination approach should be employed to capture samples of neutrons and gamma-rays before running the fit-based technique. In this article, we also propose a technique to eliminate this requirement. These approaches are applied to several sets of mixed neutron and gamma-ray pulses obtained through different digitizers using stilbene scintillator in order to analyze them and measure their discrimination quality. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Measurements of three-flavor neutrino oscillations from a PISCES two-detector fit to the NOvA Experiment data

NOvA is a long-baseline neutrino oscillation experiment with two functionally identical detectors: a Near Detector (ND) at Fermilab, placed 1 km from the neutrino source, and a Far Detector (FD) located 810 km away from the ND in Minnesota. NOvA s primary physics goals are to measure the neutrino oscillation parameters $\theta_{23}$ and $\Delta m^2_{32}$ with high precision, determine the neutrino mass hierarchy, and constrain the value of $\delta_{CP}$, primarily via the study of muon neutrino to electron neutrino oscillation. Extracting values for oscillation parameters from fits to data usually relies on treating systematic uncertainties as nuisance parameters, a strategy that suffers from poor scalability as the number of uncertainties becomes larger. This work introduces PISCES (Parameter Inference with Systematic Covariance and Exact Statistics), a novel method that circumvents this scalability problem by encoding systematic uncertainties into a covariance matrix. PISCES utilizes a nested minimization in which optimal systematic pulls are first computed using the covariance matrix in an inner minimization step, then the oscillation parameters are profiled over in the outer minimization. PISCES also uses a Poisson Likelihood term, making it ideal for the inclusion of low-statistic samples in the fits. PISCES is a flexible framework that also supports complex fits, such as a joint Near and Far detector fit. In the standard NOvA analysis, oscillation parameters are extracted using an extrapolation technique in which the ND data indirectly constrain the FD prediction via a ratio method. PISCES, on the other hand, enables a simultaneous ND+FD fit, allowing the high-statistics ND data to directly constrain systematic uncertainties across all samples. This thesis presents the full PISCES joint ND+FD fit for the NOvA three-flavor analysis, details its implementation, and evaluates its performance through extensive robustness tests and fake data studies. It also provides a comparison between the PISCES joint ND+FD results and the standard NOvA extrapolation method using the full NOvA 10-year data set. The results demonstrate that PISCES can successfully fit NOvA data while incorporating the constraints from the ND detectors consistently, using physically motivated systematic uncertainties to account for data/MC discrepancies.

Rajaoalisoa, Miriama [Cincinnati U.]↗
DOE OSTI2017

Exploratory Spectroscopy of Magnetic Cataclysmic Variables Candidates and Other Variable Objects

The increasing number of synoptic surveys made by small robotic telescopes, such as the photometric Catalina Real-Time Transient Survey (CRTS), provides a unique opportunity to discover variable sources and improves the statistical samples of such classes of objects. Our goal is the discovery of magnetic Cataclysmic Variables (mCVs). These are rare objects that probe interesting accretion scenarios controlled by the white-dwarf magnetic field. In particular, improved statistics of mCVs would help to address open questions on their formation and evolution. We performed an optical spectroscopy survey to search for signatures of magnetic accretion in 45 variable objects selected mostly from the CRTS. In this sample, we found 32 CVs, 22 being mCV candidates, 13 of which were previously unreported as such. If the proposed classifications are confirmed, it would represent an increase of 4% in the number of known polars and 12% in the number of known IPs. A fraction of our initial sample was classified as extragalactic sources or other types of variable stars by the inspection of the identification spectra. Despite the inherent complexity in identifying a source as an mCV, variability-based selection, followed by spectroscopic snapshot observations, has proved to be an efficient strategy for their discoveries, being a relatively inexpensive approach in terms of telescope time.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Simulated effects of sample size and grain neighborhood on the modeling of extreme value fatigue response

Assessing the size of representative volume elements (RVEs) for fatigue-related applications is challenging. A RVE relevant to random microstructure requires a volume of material that is sufficiently large to capture the grain/phase heterogeneity that captures all statistical moments of the distribution of the driving force for fatigue crack formation at “hot spot” grains. Consequently, the large size of a microstructure RVE required to study fatigue phenomena is largely computationally intractable and difficult to explore. A more realistic objective in this work is to systematically study, as a function of the size of a statistical sample of microstructure, trends towards convergence of the simulated distribution of driving force for fatigue crack formation. Our present work accordingly leverages the recently developed open-source PRISMS-Fatigue framework to examine the trends in convergence of extreme value distributions (EVD) of Fatigue Indicator Parameters (FIPs) in progressively larger polycrystalline microstructure realizations of FCC Al alloy 7075-T6 using crystal plasticity finite element method simulations. The results are compared to the traditional method in which ensembles of statistical volume elements (SVEs) are simulated to build up statistics intended to approximate those associated with a larger volume of material. The convergence of EVDs with increase of size of a SVE of microstructure is closely related to the extent of grain nearest neighbor (NN) interactions. Accordingly, the sensitivity of the local micromechanical response at hot spot grains is quantitatively investigated by systematically varying the orientations of NN grains. Results indicate that SVEs with cubic crystallographic texture tend towards convergence of the EVD of FIPs with tens of thousands of grains while the random and rolled textures require larger volumes. Simple relationships based on microstructure parameters (e.g., Schmid Factor, grain size, NN misorientation) do not completely correlate to fatigue hot spot grains. Finally, the sensitivity of the extreme value fatigue response at hot spot grains extends to the 3rd NN when a single neighborhood grain orientation is altered.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Dark Energy Survey Year 6 Results: MagLim++ Lens Sample Selection and Measurements of Galaxy Clustering

Galaxy clustering is a sensitive probe of the expansion history and growth of structure of the universe, and key degeneracies can be broken by combining these data with measurements of cosmic shear and galaxy-galaxy lensing (a so-called 3$\times$2pt analysis). The largest and least biased statistical samples of galaxies for use in clustering analyses can be collected photometrically through large imaging surveys. However, selecting clean photometric subsamples for cosmology are crucial for avoiding contamination that can bias cosmological constraints. Here we present the MagLim++ galaxy sample, selected to optimize for cosmological constraining power and incorporating an array of novel quality cuts to identify and remove residual contamination. This sample comes from the full six years of observations from the Dark Energy Survey. We present measurements of the two-point angular clustering ($w(θ)$) of 9,186,205 galaxies distributed over 4031 sq. degrees and in six tomographic redshift bins centered at $\bar{z}\approx$ [0.31, 0.44, 0.62, 0.78, 0.90, 1.01]. These measurements are used as part of the 3$\times$2pt and other DES Y6 legacy cosmological analyses in companion works. We describe the battery of null tests and mitigation schemes implemented to address observational, astrophysical, and methodological systematics in the analysis. The resulting $w(θ)$ measurements have a S/N = 149 (90.2 for linear scales only), which we use to place galaxy-clustering-only constraints on the matter density of the Universe, $Ω_m=0.311^{+0.023}_{-0.035}$, and amplitude of galaxy clustering in each redshift bin, $b_iσ_8=[1.16^{+0.04}_{-0.06},\ 1.40^{+0.04}_{-0.06},\ 1.57^{+0.04}_{-0.06},\ 1.59^{+0.04}_{-0.05},\ 1.50^{+0.04}_{-0.05},\ 1.74^{+0.06}_{-0.08}]$.

Weaverdyck, N. [BCCP, Berkeley; UC, Berkeley; LBL,↗
DOE OSTI2020

Status Update on the High Precision Isotopic Measurements on High Burnup LWR Fuel in 2020

The US Department of Energy (DOE) Office of Nuclear Energy (NE) is currently investigating the feasibility of directly disposing dual-purpose (storage and transportation) canisters (DPCs) in a spent nuclear fuel (SNF) repository. Criticality during the repository performance period (10,000 years or more) is one of the major concerns related to direct disposal of DPCs, specifically as the system undergoes degradation in the repository environment and timeframe. Oak Ridge National Laboratory (ORNL) is developing an as-loaded criticality analysis methodology using full (actinides + fission products) burnup credit that exploits the inherent criticality margin associated with actual canister-specific loading configuration. Burnup credit criticality analysis requires validation of the depletion/decay codes used to generate the burned isotopic inventory of an assembly by comparing the code-predicted inventory with experimentally determined isotopic data. Currently, isotopic measurement data for boiling water reactors (BWR) SNF are limited, and additional measurements will be highly beneficial for BWR burnup credit analysis, which is essential to demonstrate disposability of BWR DPCs. Moreover, new pressurized water reactor (PWR) samples of isotopic measurements will expand the PWR sample population and consequently will greatly improve sample statistics. In turn, this will reduce uncertainty in the computational determination of the isotopic composition of commercial SNF and eliminate additional penalties currently used for lack of data. As part of the isotopic analysis task, eight diverse, high burnup (HBU) samples from several PWR rods are being dissolved and isotopically analyzed to provide high-quality measurement data for PWR SNF to reducing the uncertainties associated with PWR isotopic depletion validation. The isotopics of interest focus on nuclides important to burnup credit, shielding, and decay heat in PWR SNF. Additionally, eight high burnup BWR fuel samples from the Limerick nuclear power plant have been identified for measurement to support reducing uncertainties associated with BWR isotopic depletion validation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Intricate short-range order in GeSn alloys revealed by atomistic simulations with highly accurate and efficient machine-learning potentials

GeSn alloys hold promise for silicon-compatible integrated applications in electronics, photonics, and topological quantum devices. However, understanding their intricate structures using density functional theory (DFT) calculations is hindered by spatiotemporal constraints. To overcome this limitation, we develop highly accurate and efficient machine-learning interatomic potentials based on a neuroevolution potential approach with farthest point sampling on a comprehensive DFT data set. The application of the developed machine-learning potential in large-scale atomistic simulations bridges the spatiotemporal gap between modeling and advanced characterizations, and facilitates the discovery of structural intricacies in GeSn alloys. Through extensive statistical sampling, we identify a type of short-range order (SRO) that is distinguished by both its structural signature and electronic band gap from the SRO structure previously predicted. Modeling based on a large simulation cell reveals the coexistence of nano SRO domains with various degrees of ordering, demonstrating a complex spatial heterogeneity of SRO structure. Finally, our study not only reinforces the significance of fine-level structural information in alloys, but it also constitutes an effective framework for exploring SRO in a broad range of complex alloys based on highly accurate and effective machine-learning potentials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

High-Throughput Discovery Illuminates Design Principles and Limits for Long-Lived Charged Species in Organic Electrolytes

The chemical stability of charged molecules in all-organic redox flow batteries (RFBs) is required for the prolonged operation of these devices. Molecular engineering and electrolyte optimization are used to mitigate parasitic reactions and extend the lifetimes of the charge carriers. However, how much can structural variation extend the lifetime? To probe this query, we designed a high-throughput kinetic study of the radical cation of N-methylphenothiazinium, guided by statistical sampling and learning algorithms. Using Argonne’s autonomous discovery facility, we conducted over 6,000 kinetic experiments with robotic sample preparation, parallel kinetic measurements, and machine learning inputs, testing 188 solvent molecules selected from a space of over 540 candidates from 11 chemical classes. Algorithmic selections guided us to stable solvent candidates, which were further tested in high concentration with and without supporting electrolyte. Our findings reveal the inherent difficulty of exceeding the current state of the art through solvent variation. The desired stability is statistically rare and poorly predictable. Among the many tested, only three solvents significantly outperformed our baseline, acetonitrile─and none by more than a factor of 3─suggesting a general challenge in achieving the necessary techno-economic targets. Furthermore, we suggest that self-discharge through solvent homolysis is the cause of the observed limitations. Several structural motifs contribute to >1,000 h half-life stability including molecular simplicity, symmetry, oxidation complement, and strategic fluorination. Importantly, this workflow establishes effective assays for diagnosing and predicting oxidative stress for highly stable liquid electrolytes in all batteries.

Batteries↗