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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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912 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Developing And Scaling an OpenFOAM Model to Study Turbulent Flow in a HFIR Coolant Channel

Improving the understanding of how computational fluid dynamics (CFD) direct numerical simulations (DNS) of flows in the High Flux Isotope Reactor (HFIR) perform when run in parallel using the high performance computing (HPC) platform Summit at the Oak Ridge Leadership Computing Facility (OLCF) is of particular importance to boost the computational tools used to support HFIR conversion to low enriched fuel (LEU). Evaluation of scaling performance was driven by the increasing importance of graphics processing unit (GPU) usage in HPC, which is becoming the standard for modern supercomputers such as Summit. The desired results are to obtain a strong positive correlation between the computational resources dedicated to a problem and the relative speed-up of the simulation in comparison to a benchmark. This capability will allow substantially improvement in HFIR flow analytical capabilities, specifically when predicting turbulence properties at high Reynolds numbers. The study leverages previous simulation results performed with code PHASTA (finite element) on HPC platforms Cori (NERSC) and Theta (ALCF) [1] with computing options provided in the computing platform OpenFOAM (finite volume) at OLCF. Transitioning from PHASTA to OpenFOAM will (1) eliminate dependence on third-party software for mesh generation and manipulation, (2) reduce resource needs by employing modern architectures, and (3) build expertise for future modeling of HFIR-specific problems like heat transfer in involute geometry, entrance effects, flow structure in channel corners, and so on—all important issues when defining the available thermal margins in the transition to LEU. CPUs and GPUs differ significantly in their architecture and utilization, as discussed in the literature [2]. The most important differences are in the approach to computations and their memory. A single GPU contains a large quantity of cores, enabling it to perform with a much higher throughput than a CPU, but execution requires a different approach. GPU codes execute instructions using the Single-Instruction Multiple-Thread (SIMT) approach in which a single instruction is used for groups of threads called warps. A warp typically consists of 32 threads which must execute the same set of instructions, although on separate threads. Alternately, a CPU has far fewer cores that are much more flexible in their operation, excelling at quickly performing more complex serial computations. This is why GPUs have greater throughput when properly utilized. The second important difference is seen when comparing their memory spaces. Limited memory allocations and CPU–GPU communications cause a significant bottleneck in GPU-accelerated programs. Further study was required to properly take advantage of GPU resources. A comprehensive analysis of code performance and the model-specific features of turbulence constitutes the core of this work. In this study, a DNS simulation of HFIR channel turbulence was performed with the finite volume CFD code OpenFOAM v2112 and CUDA v11.0 on Red Hat Enterprise Linux v8.2. The OpenFOAM installation had AMGx integrated to enable GPU acceleration and utilizes the PETSc4FOAM library. The computational resources and the problem size were scaled on CPU and CPU + GPU architectures to gain a better understanding of the performance of a DNS problem on modern computing hardware. The study aimed to analyze the scaling of the code exclusively on CPUs and then to examine the scaling of the codes with GPU acceleration enabled. Scaling studies included CPU and GPU acceleration on a mesh of varying resolution to analyze the impact of problem size relative to computational resources. In the course of preparing the GPU configuration on Summit, mainly using the AMGX solvers, difficulties were encountered stemming from constant changes resulting from extensive ongoing development activities and the changing environment. This resulted in the inability to complete the GPU portion of the work. The code was compiled and tested, but production runs to assess acceleration were not performed because the used discretional compute time allocation expired as year-end approached. The Summit HPC platform is scheduled for decommissioning in 2024, making it unattractive for future use with Nvidia-based GPUs. Therefore, the work will be moved onto NERSC machines in FY24. An application was prepared and submitted, and sufficient node-hours were awarded to continue the research in the next calendar year. This report summarizes work performed thus far, which mostly focused on CPU OpenFOAM computing.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRS2001

Validation of the galactic cosmic ray and geomagnetic transmission models

A very high-momentum resolution particle spectrometer called the Alpha Magnetic Spectrometer (AMS) was flown in the payload bay of the Space Shuttle in a 51.65 degrees x 380-km orbit during the last solar minimum. This spectrometer has provided the first high statistics data set for galactic cosmic radiation protons, and helium, as well as limited spectral data on carbon and oxygen nuclei in the International Space Station orbit. First measurements of the albedo protons at this inclination were also made. Because of the high-momentum resolution and high statistics, the data can be separated as a function of magnetic latitude. A related investigation, the balloon borne experiment with a superconducting solenoid spectrometer (BESS), has been flown from Lynn Lake, Canada and has also provided excellent high-resolution data on protons and helium. These two data sets have been used here to study the validity of two galactic cosmic ray models and the geomagnetic transmission function developed from the 1990 geomagnetic reference field model. The predictions of both the CREME96 and NASA/JSC models are in good agreement with the AMS data. The shape of the AMS measured albedo proton spectrum, up to 2 GeV, is in excellent agreement with the previous balloon and satellite observations. A new LIS spectrum was developed that is consistent with both previous and new BESS 3He observations. Because the astronaut radiation exposures onboard ISS will be highest around the time of the solar minimum, these AMS measurements and these models provide important benchmarks for future radiation studies. AMS-02 slated for launch in September 2003, will provide even better momentum resolution and higher statistics data. Published by Elsevier Science Ltd.

unmanned↗
NASA NTRS1995

Collapse and fragmentation of molecular cloud cores. 2: Collapse induced by stellar shock waves

The standard scenario for low-mass star formation involves 'inside-out' collapse of a dense molecular cloud core following loss of magnetic field support through ambipolar diffusion. However, isotopic anomalies in presolar grains and meteoritical inclusions imply that the collapse of the presolar cloud may have been triggered by a stellar shock wave. This paper explores 'outside-in' collapse, that is, protostellar collapse initiated directly by the compression of quiescent dense cloud cores impacted by relatively slow stellar shock waves. A second-order accurate, gravitational hydrodynamics code has been used to study both the spherically symmetrical and three-dimensional evolution of initially centrally condensed, isothermal, self-gravitating, solar-mass cloud cores that are struck by stellar shock waves with velocities up to 25 km/s and postshock temperatures of 10 to 10,000 K. The models show that such mild shock waves do not completely shred and destroy the cloud, and that the dynamical ram pressure can compress the cloud to the verge of self-gravitational collapse. However, compression caused by a high postshock temperature is a considerably more effective means of inducing collapse. Shock-induced collapse produces high initial mass accretion rates (greater than 10(exp -4) solar mass/yr in a solar-mass cloud) that decline rapidly to much lower values, depending on the presence (approximately 10(exp -6) solar mass/yr) or absence (approximately 10(exp -8) to 10(exp -7) solar mass/yr) of an infinite reservoir of mass. Stellar mass accretion rates approximately 10(exp -7) solar mass/yr have been previously inferred from the luminosities of T Tauri stars; balanced mass accretion (stellar rate = envelope rate) at approximately 10(exp -7) solar mass/yr could then be possible if accretion occurs from a finite mass reservoir. Fluid tracers are used to determine what fraction of the stellar shock material is incorporated into the resulting protostellar object and disk; roughly half the impinging material is injected into the collapsing cloud core when there is a high postshock temperature. The models are consistent with a scenario where an AGB star wind triggered the collapse of the presolar cloud while injecting about 0.01 solar mass of matter derived from the AGB star envelope, as has been separately inferred on the basis of nucleosynthesis calculations.

Boss, Alan P.↗
DOE OSTI2021

Ground-state and decay properties of neutron-rich 106 Nb

The ground-state properties of neutron-rich 106 Nb and its β decay into 106 Mo have been studied using the CARIBU radioactive-ion-beam facility at Argonne National Laboratory. Niobium-106 ions were extracted from a 252 Cf fission source and mass separated before being delivered as low-energy beams to the Canadian Penning Trap, as well as the X-Array and SATURN β-decay-spectroscopy station. The measured 106 Nb ground-state mass excess of –66202.0(13) keV is consistent with a recent measurement but has three times better precision; this work also rules out the existence of a second long-lived, β-decaying state in 106 Nb above 5 keV in excitation energy. The decay half-life of 106 Nb was measured to be 1.097(21) s, which is 8% longer than the adopted value. Here, the level scheme of the decay progeny, 106 Mo, has been expanded up to ≈ 4 MeV. The distribution of decay strength and considerable population of excited states in 106 Mo of J ≥ 3 emphasizes the need to revise the adopted J π = 1 – ground-state spin-parity assignment of 106 Nb; it is more likely to be J ≥ 3.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

ENDF/B-VIII.1: Thermal Neutron Scattering Sublibrary

The thermal neutron scattering law (TSL) sublibrary aims to describe the interaction of incident neutrons at thermal or sub-thermal energies with different compound materials such fuels, moderators and special-purpose materials. In ENDF/B-VIII.1 there was a large number of new and updated TSL evaluations, including traditional moderators (light water, Beryllium metal, Beryllium Oxide, Calcium Hydride, plastics (Polystyrene and Lucite), graphite (reactor-grade and crystalline), anhydrous Hydrogen Fluoride, and heavy paraffinic oil); exotic moderators (Beryllium Carbide, Zirconium Hydride, Yttrium Hydride, Lithium-7 Hydride and Deuteride), FLiBe molten salt, structural materials and cladding (Silicon Carbide, Silicon Dioxide, Zirconium Carbide), fuels (Plutonium Dioxide, Uranium Carbide, Uranium metal, Uranium Nitride, Uranium Dioxide, Uranium Hydride), and special purpose materials. In ENDF/B-VIII.1 we also distribute alongside the evaluated files, a comma-separated file (CSV), named TSL_MAT_numbers.csv, which lists all evaluated files in the current release and their corresponding unique MAT number.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Cross-sections for 43 Sc, 44 m Sc, and 44 g Sc from two heavy ion reactions

Two different heavy ion reactions were used to produce 43 Sc (t$_{\frac12}$ = 3.891 h), 44g Sc (t$_{\frac12}$ = 4.042 h), and 44m Sc (t$_{\frac12}$ = 58.61 h) among other stable or long-lived chemically separable products. Production cross sections for 19 F + 27 Al and the reverse kinematic reaction 35 Cl + nat B were measured using an MC-SNICS ion source and the Notre Dame FN Tandem Accelerator. 19 F beams from 35 to 60 MeV were produced with beam currents between 40–80 pnA and 35 Cl beams were produced at six entrance energies with comparable beam currents. This work reports nuclear reaction cross sections 27 Al ( 19 F, x) 43 Sc, 27 Al ( 19 F, pn) 44g Sc, and 27 Al ( 19 F, pn) 44m Sc at six energies between 35 and 60 MeV lab energy. Cross sections within the same energy range were measured for 27 Al ( 19 F, 3pn) 42 K and 27 Al ( 19 F, 3p) 43 K. Comparative measurements were performed for the same compound nucleus produced from nat B( 35 Cl, x) 43 Sc, nat B( 35 Cl, pn) 44g Sc, and nat B( 35 Cl, pn) 44m Sc. The measured thin target cross sections show an overestimation by several statistical models for the scandium radioisotopes. This is corroborated by the measured thick target production rates for both entrance channels. This may be due to angular momentum effects of a heavy ion entrance channel compared to light-ion production, but additional work is required to understand this discrepancy. Finally, these measurements demonstrate that the medically useful 43 Sc, 44g Sc, and 44m Sc radioisotopes can be free of the long-lived contaminant 46 Sc without the use of enriched targets, using heavy ion beams and robust target materials.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

AGR-5/6/7 Irradiation Test Final As-run Report

This document presents the as-run analysis of the Advanced Gas Reactor (AGR) 5/6/7 irradiation experiment. AGR-5/6/7 is the last of a series of experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) in support of the development and qualification of tri-structural isotropic (TRISO) low enriched fuel for use in high-temperature gas-cooled reactors (HTGR). The test train contained five separate capsules that were independently controlled and monitored. Each capsule contained multiple 24.91-mm-long and 12.25-mm-dimeter compacts filled with low-enriched uranium carbide/oxide tri-structural isotropic fuel particles. The objectives of the AGR 5/6/7 experiment were to: 1. Irradiate reference-design fuel particles to support fuel qualification. 2. Establish operating margins for the fuel, beyond normal operating conditions. 3. Provide irradiated-fuel performance data and irradiated-fuel samples for post irradiation examination and safety testing. The primary objective of the AGR-5/6 test (Capsules 1, 2, 4, and 5) was to verify the successful performance of the reference-design fuel under normal operating conditions. The AGR-7 test (Capsule 3) was designed to explore fuel performance at higher temperatures. Its primary objective is to demonstrate the capability of the fuel to withstand conditions beyond normal operating conditions, in support of plant design and licensing. AGR 5/6/7 will also provide irradiated-fuel performance data based on the fission gas release from particles during irradiation. To achieve the test objectives, the AGR-5/6/7 experiment was irradiated in the northeast (NE) flux trap of the ATR with a planned duration of 500 effective full-power days (EFPDs). The NE flux trap was selected because its larger diameter provided greater flexibility for test-train design compared to the Large B positions used for the AGR-1 and AGR-2 irradiations, significantly enhancing test capabilities for the combined irradiation campaigns. Due to delays in the ATR schedule, the AGR-5/6/7 irradiation was significantly shorter than the originally planned 13-cycle schedule. Irradiation began on February 16, 2018 and ended on July 22, 2020, spanning nine ATR cycles (162B?168A) over two and a half years. Thus, the AGR-5/6/7 fuel compacts were irradiated for a total of approximately 360.9 EFPDs. Final burnup values, on a per-compact basis, ranged from 5.66% to 15.26% fissions per initial heavy metal atom, while fast fluence values ranged from 1.62 to 5.55 × 1025 n/m2 (E >0.18 MeV). Time-averaged volume-averaged fuel temperatures on a capsule basis at the end of irradiation ranged from 756°C in Capsule 5 to 1313°C in Capsule 3 excluding days with significantly lower temperature during the two short powered axial locator mechanism cycles, 163A and 167A. By the end of irradiation, 48 out of 54 installed thermocouples (TC) had failed (the bottom three capsules lost all TCs). During the first five cycles (162B ? 165A), fission-gas isotope release-rate-to-birthrate (R/B) ratios were stable in the 10-8?10-6 range, and no in-pile particle failures were observed based on the gross gamma counts. During this time, the high exposed kernel fraction and high fuel particle temperatures in Capsule 1 led to the maximum R/B value of around 2 ? 10-6 for Kr-85m. The fission gas release in all capsules started to increase from the second half of Cycle 166A, when a large number of in-pile particle failures occurred in Capsule 1 and a gas line problem in this capsule caused fission gas leakage at various degrees into the other four capsules. This gas line problem also prevented fission gas release measurement for Capsule 1 during the last three cycles due to gas flow isolation. By the end of irradiation, it is estimated that approximately 15 particle failures in Capsule 3, which was considered possible at the start of the irradiation, since the experiment was designed to operate beyond the high-temperature gas-cooled reactor (HTGR) normal operating temperature range. A few hundred in-pile particle failures were estimated for Capsule 1 by the end of Cycle 166A, but the total number of failures is unknown due to lack of fission gas release data in the later cycles. Additionally, four potential in-pile failures were identified for Capsule 2 during the last cycle, 168A. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on absence of the typical spikes in gross gamma counts and low failure estimates using the AGR-3/4 R/B per exposed kernel model.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

AGR-5/6/7 Irradiation Test Final As-run Report

This document presents the as-run analysis of the Advanced Gas Reactor (AGR)-5/6/7 irradiation experiment. AGR-5/6/7 is the last of a series of experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory in support of the development and qualification of tri-structural isotropic low-enriched fuel for use in high-temperature gas-cooled reactors. The test train contained five separate capsules that were independently controlled and monitored. Each capsule contained multiple 24.91-mm-long and 12.25-mm-dimeter compacts filled with low-enriched uranium carbide/oxide tri-structural isotropic fuel particles. The objectives of the AGR-5/6/7 experiment were to: • Irradiate reference-design fuel particles to support fuel qualification. • Establish operating margins for the fuel, beyond normal operating conditions. • Provide irradiated-fuel performance data and irradiated-fuel samples for post-irradiation examination and safety testing. The primary objective of the AGR-5/6 test (Capsules 1, 2, 4, and 5) was to verify the successful performance of the reference-design fuel under normal operating conditions. The AGR-7 test (Capsule 3) was designed to explore fuel performance at higher temperatures. Its primary objective was to demonstrate the capability of the fuel to withstand conditions beyond normal operating conditions, in support of plant design and licensing. AGR-5/6/7 will also provide irradiated-fuel performance data based on the fission gas release from particles during irradiation. To achieve the test objectives, the AGR-5/6/7 experiment was irradiated in the northeast flux trap of the ATR with a planned duration of 500 effective full-power days. The northeast flux trap was selected because its larger diameter provided greater flexibility for test-train design compared to the Large B positions used for the AGR-1 and AGR-2 irradiations, significantly enhancing test capabilities for the combined irradiation campaigns. Due to delays in the ATR schedule, the AGR-5/6/7 irradiation was significantly shorter than the originally planned 13-cycle schedule. Irradiation began on February 16, 2018 and ended on July 22, 2020, spanning nine ATR cycles (162B–168A) over two and a half years. Thus, the AGR-5/6/7 fuel compacts were irradiated for a total of approximately 360.9 effective full-power days. Final burnup values, on a per-compact basis, ranged from 5.66 to 15.26% fissions per initial heavy metal atom, while fast fluence values ranged from 1.62 to 5.55 × 1025 n/m2 (E >0.18 MeV). Time-averaged volume-averaged fuel temperatures on a capsule basis at the end of irradiation ranged from 756°C in Capsule 5 to 1313°C in Capsule 3 excluding days with significantly lower temperature during the two short powered axial locator mechanism cycles, 163A and 167A. By the end of irradiation, 48 out of 54 installed thermocouples had failed (the bottom three capsules lost all thermocouples). During the first five cycles (162B – 165A), the fission-gas isotope release-rate-to-birthrate (R/B) ratios were stable in the 10-8–10-6 range, and no in-pile particle failures were observed based on the gross gamma counts. During this time, the high exposed kernel fraction and high fuel particle temperatures in Capsule 1 led to a maximum R/B value of around 2 ? 10-6 for Kr-85m. The fission gas release in all capsules started to increase from the second half of Cycle 166A, when a large number of in-pile particle failures occurred in Capsule 1 and a gas line problem in this capsule caused fission gas leakage at various degrees into the other four capsules. This gas line problem also prevented a fission gas release measurement for Capsule 1 during the last three cycles due to gas flow isolation. By the end of irradiation, it is estimated that approximately 15 particles failed in Capsule 3, which was considered possible because the experiment was designed to operate beyond the high-temperature gas-cooled reactor normal operating temperature range. A few hundred in-pile particle failures were estimated for Capsule 1 by the end of Cycle 166A, but the total number of failures is unknown due to the lack of fission gas release data in the later cycles. Additionally, four potential in-pile failures were identified for Capsule 2 during the last cycle, Cycle 168A. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on the absence of the typical spikes in gross gamma counts and low failure estimates using the AGR-3/4 R/B per exposed kernel model.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Data from: "Warming of alpine tundra enhances belowground production and shifts community towards resource acquisition traits"

This archive contains data used to draw conclusions in “Warming of alpine tundra enhances belowground production and shifts community towards resource acquisition traits”, by Yang et al. 2020. Data were collected on Niwot Ridge, in an alpine meadow within the Alpine Treeline Warming Experiment (ATWE) field sites in Colorado, USA. Samples were also processed in the U.S. Geological Survey Forest and Rangeland Ecosystem Science Center, in Boise, Idaho. File formats in this archive include comma-separated values (.csv), portable document format (.pdf), Microsoft Excel (.xlsx), and two types of geospatial files: keyhole markup language (.kml), and ESRI shapefiles (.shp). Leaf scans are .jpg images, and root scans are .tiff/.tif images.The .csv files can be opened using R, Microsoft Excel, or any simple text-editing software such as TextEdit and Notepad. Microsoft Excel files can be opened using Microsoft Excel, and .pdf files can be opened with Adobe Acrobat Reader, Preview, or other compatible programs. Scanned images can be opened using any photo and/or picture viewing software.The .kml file can be opened using Google Earth and Google Maps, and the shapefiles can be opened by any programs compatible with shapefiles, such as the ArcGIS Desktop suite, and QGIS.------------------------------------------------------------------------------------------------------------------------------------------------------------------------------------------------Measures of belowground net primary productivity (BNPP) are required to understand whether aboveground net primary production (ANPP) changes reflect changes in allocation or are indicative of a whole plant NPP response. Plant functional traits provide a key way to scale from the individual plant to the community level, and provide insight into drivers of NPP responses to environmental change. We used infrared heaters to warm an alpine plant community at Niwot Ridge, Colorado, and applied supplemental water to compensate for soil water loss induced by warming. We measured ANPP, BNPP, and leaf and root functional traits across treatments after 5 years of continuous warming. Community-level ANPP and total NPP (ANPP + BNPP) did not respond to heating or watering, but BNPP increased in response to heating. Heating decreased community-level leaf dry matter content and increased total root length, indicating a shift in strategy from resource conservation to acquisition in response to warming.

13C/12C isotope ratio↗
DOE OSTI2024

Models, data, and scripts associated with “Prediction of Distributed River Sediment Respiration Rates using Community-Generated Data and Machine Learning”

This data package is associated with the publication “Prediction of Distributed River Sediment Respiration Rates using Community-Generated Data and Machine Learning’’ submitted to the Journal of Geophysical Research: Machine Learning and Computation (Scheibe et al. 2024). River sediment respiration observations are expensive and labor intensive to obtain and there is no physical model for predicting this quantity. The Worldwide Hydrobiogeochemisty Observation Network for Dynamic River Systems (WHONDRS) observational data set (Goldman et al.; 2020) is used to train machine learning (ML) models to predict respiration rates at unsampled sites. This repository archives training data, ML models, predictions, and model evaluation results for the purposes of reproducibility of the results in the associated manuscript and community reuse of the ML models trained in this project. One of the key challenges in this work was to find an optimum configuration for machine learning models to work with this feature-rich (i.e. 100+ possible input variables) data set. Here, we used a two-tiered approach to managing the analysis of this complex data set: 1) a stacked ensemble of ML models that can automatically optimize hyperparameters to accelerate the process of model selection and tuning and 2) feature permutation importance to iteratively select the most important features (i.e. inputs) to the ML models. The major elements of this ML workflow are modular, portable, open, and cloud-based, thus making this implementation a potential template for other applications. This data package is associated with the GitHub repository found at Please see the file level metadata (flmd; “sl-archive-whondrs_flmd.csv”) for a list of all files contained in this data package and descriptions for each. Please see the data dictionary (dd; “sl-archive-whondrs_dd.csv”) for a list of all column headers contained within comma separated value (csv) files in this data package and descriptions for each. The GitHub repository is organized into five top-level directories: (1) “input_data” holds the training data for the ML models; (2) “ml_models” holds machine learning models trained on the data in “input_data”; (3) “scripts” contains data preprocessing and postprocessing scripts and intermediate results specific to this data set that bookend the ML workflow; (4) “examples” contains the visualization of the results in this repository including plotting scripts for the manuscript (e.g., model evaluation, FPI results) and scripts for running predictions with the ML models (i.e., reusing the trained ML models); (5) “output_data” holds the overall results of the ML model on that branch. Each trained ML model resides on its own branch in the repository; this means that inputs and outputs can be different branch-to-branch. Furthermore, depending on the number of features used to train the ML models, the preprocessing and postprocessing scripts, and their intermediate results, can also be different branch-to-branch. The “main-*” branches are meant to be starting points (i.e. trunks) for each model branch (i.e. sprouts). Please see the Branch Navigation section in the top-level README.md in the GitHub repository for more details. There is also one hidden directory “.github/workflows”. This hidden directory contains information for how to run the ML workflow as an end-to-end automated GitHub Action but it is not needed for reusing the ML models archived here. Please the top-level README.md in the GitHub repository for more details on the automation.

13C↗
DOE OSTI2024

Role of the likelihood for elastic scattering uncertainty quantification

In the last decade, uncertainty quantification (UQ) for optical model potentials (OMPs) has become a focal point for nuclear reaction theory, and several competing approaches for OMP UQ have recently been developed. Here, we clarify recent efforts to compare frequentist and Bayesian approaches in the context of OMP UQ [G. B. King et al., Phys. Rev. Lett. 122, 232502 (2019)]. We replicate a portion of that OMP UQ study but use independent statistical tools. Specifically, we compare two methods for OMP parameter inference from elastic scattering data: the Levenberg-Marquardt algorithm for χ 2 minimization on one hand and Markov chain Monte Carlo (MCMC) sampling on the other. Separately, we assess the common practice of using a renormalized likelihood (χ 2 /N), N being the number of data points, instead of the canonical weighted-least-squares likelihood (χ 2 ), as a way of accounting for unknown data correlations. Here, we show that for a generic linear model and for a five-parameter OMP analysis, frequentist and uniform-prior Bayesian approaches recover the same optimum and uncertainty estimates—not systematically larger uncertainties for the Bayesian approach, as was concluded in G. B. King et al., Phys. Rev. Lett. 122, 232502 (2019). Further, we show that if an additional, near-degenerate parameter is introduced into the same OMP analysis such that the parameter posterior becomes non-Gaussian, then covariance-based estimates of uncertainty become unreliable. Finally, we show that regardless of optimization approach, if χ 2 /N is used for the likelihood, the resulting parametric uncertainties increase by $\sqrt{N}$, and that this is responsible for the conclusions drawn in the revisited study. Based on our replication results, we find that a fortuitous cancellation of unreported errors and the renormalization factor can lead to improvement in empirical coverages, as was the case in the original comparative study. We emphasize that developing and applying a realistic likelihood function is an essential task in a UQ analysis, and that several recent UQ studies that employed a renormalized likelihood (i.e., including a 1/N factor) may have yielded unrealistically large uncertainties for elastic-scattering observables. If the parameter posterior deviates from multivariate-normal, a sampling-based approach like MCMC has a clear advantage over methods that assume the Laplace approximation holds. We note that empirical coverage can serve as an important internal check for the analyst whose model or data may have additional, unaccounted-for uncertainties.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Non–linear bonding trends in maleonitrile-1,2–dithiolate complexes of the transuranium actinides

The trivalent actinides are produced in the nuclear fuel cycle during power production and provide the largest long-term radiation dose in used nuclear fuel. It is ideal for these elements to be removed from used nuclear fuel for disposal and a necessity for fuel recycling. A key challenge to this is the similarity of chemical behavior of the trivalent actinides to the lanthanides that are also present as fission products in used fuel. Thus far, some of the most effective separations of actinides from lanthanides utilise chelating agents containing sulfur moieties such as dithiophosphinates that selectively bind to actinide ions because of a greater bond covalency relative to lanthanide ions. Typically, greater differences between actinide and lanthanide ions are observable the more ligands and chelators bonds have a covalent character. Here, a series of complexes of the trivalent actinides Np(III) through Cf(III) (excluding Bk(III)) with maleonitrile-1,2-dithiolate (mnt 2– ) are synthesized along with their lanthanide counterparts (La(III) – Nd(III), Sm(III) – Gd(III), Dy(III)), in order to characterize the nature of chemical bonds with these metal ions and a polarizable, non-innocent, sulfur-donor ligand. The metal-sulfur bonds in these complexes trend shorter than measured for lanthanides with equivalent ionic radii. However, particularly large deviations are observed in the neptunium and plutonium complexes in both structure and bonding, resulting in a nonlinear bond length trendline for the actinide series. Density Functional Theory (DFT) calculations with Quantum Theory of Atoms in Molecules (QTAIM) and Natural Bond Order (NBO) analyses indicate that for the neptunium and plutonium complexes, the presence of increased 5f-orbital participation, energy degeneracy of the metal and ligand orbitals, and the structure packing result in shortened M–S bonds. The stabilization of the energy of the 5f-orbitals and the decrease in f-contribution to bonding orbitals in the later actinides results in structural properties more similar to the lanthanide complexes.

07 ISOTOPE AND RADIATION SOURCES↗