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At least 955 records · Page 53

Reconstructing Masses of Merging Neutron Stars from Stellar r -process Abundance Signatures

We report that neutron star mergers (NSMs) are promising astrophysical sites for the rapid neutron-capture ("r") process, but can their integrated yields explain the majority of heavy-element material in the Galaxy? One method to address this question implements a forward approach that propagates NSM rates and yields along with stellar formation rates and compares those results with observed chemical abundances of r-process-rich, metal-poor stars. In this work, we take the inverse approach by utilizing r-process-element abundance ratios of metal-poor stars as input to reconstruct the properties -especially the masses - of their neutron star (NS) binary progenitors. This novel analysis provides an independent avenue for studying the population of the original NS binary systems that merged and produced the r-process material now incorporated in Galactic metal-poor halo stars. We use ratios of elements typically associated with the limited-r-process and the actinide region to those in the lanthanide region (i.e., Zr/Dy and Th/Dy) to probe the NS masses of the progenitor merger. We find that NSMs can account for all r-process material in metal-poor stars that display r-process signatures, while simultaneously reproducing the present-day distribution of double-NS systems. Notably, with our model assumptions and the studied stellar sample, we postulate that the most r-process enhanced stars (the r–II stars) on their own would require progenitor NSMs of asymmetric systems that are distinctly different from present ones in the Galaxy. We also explore variations to the model and find that the predicted degree of asymmetry is most sensitive to the electron fraction of the remnant disk wind.

79 ASTRONOMY AND ASTROPHYSICS↗

${S}^5$: The destruction of a bright dwarf galaxy as revealed by the chemistry of the Indus stellar stream

The recently discovered Indus stellar stream exhibits a diverse chemical signature compared to what is found for most other streams due to the abundances of two outlier stars, Indus$\_$0 and Indus$\_$13. Indus$\_$13, exhibits an extreme enhancement in rapid neutron-capture ($r$-)process elements with $\mathrm{[Eu/Fe]} = +1.81$. It thus provides direct evidence of the accreted nature of $r$-process enhanced stars. In this paper we present a detailed chemical analysis of the neutron-capture elements in Indus$\_$13, revealing the star to be slightly actinide poor. The other outlier, Indus$\_0$, displays a globular cluster-like signature with high N, Na, and Al abundances, while the rest of the Indus stars show abundances compatible with a dwarf galaxy origin. Hence, Indus$\_0$ provides the first chemical evidence of a fully disrupted dwarf containing a globular cluster. We use the chemical signature of the Indus stars to discuss the nature of the stream progenitor which was likely a chemically evolved system, with a mass somewhere in the range from Ursa Minor to Fornax.

79 ASTRONOMY AND ASTROPHYSICS↗

Kilonovae Across the Nuclear Physics Landscape: The Impact of Nuclear Physics Uncertainties on r-process-powered Emission

Merging neutron stars produce “kilonovae”—electromagnetic transients powered by the decay of unstable nuclei synthesized via rapid neutron capture (the r-process) in material that is gravitationally unbound during inspiral and coalescence. Kilonova emission, if accurately interpreted, can be used to characterize the masses and compositions of merger-driven outflows, helping to resolve a long-standing debate about the origins of r-process material in the Universe. We explore how the uncertain properties of nuclei involved in the r-process complicate the inference of outflow properties from kilonova observations. Using r-process simulations, we show how nuclear physics uncertainties impact predictions of radioactive heating and element synthesis. For a set of models that span a large range in both predicted heating and final abundances, we carry out detailed numerical calculations of decay product thermalization and radiation transport in a kilonova ejecta with a fixed mass and density profile. The light curves associated with our models exhibit great diversity in their luminosities, with peak brightness varying by more than an order of magnitude. We also find variability in the shape of the kilonova light curves and their color, which in some cases runs counter to the expectation that increasing levels of lanthanide and/or actinide enrichment will be correlated with longer, dimmer, redder emission.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Influence of β-decay Rates on r-process Observables

Abstract The rapid neutron capture process ( r -process) is one of the main mechanisms whereby elements heavier than iron are synthesized, and is entirely responsible for the natural production of the actinides. Kilonova emissions are modeled as being largely powered by the radioactive decay of species synthesized via the r -process. Given that the r -process occurs far from nuclear stability, unmeasured beta-decay rates play an essential role in setting the timescale for the r -process. In an effort to better understand the sensitivity of kilonova modeling to different theoretical global beta-decay descriptions, we incorporate these into nucleosynthesis calculations. We compare the results of these calculations and highlight differences in kilonova nuclear energy generation and light-curve predictions, as well as final abundances and their implications for nuclear cosmochronometry. We investigate scenarios where differences in beta-decay rates are responsible for increased nuclear heating on timescales of days that propagates into a significantly increased average bolometric luminosity between 1 and 10 days post-merger. We identify key nuclei, both measured and unmeasured, whose decay rates directly impact nuclear heating generation on timescales responsible for light-curve evolution. We also find that uncertainties in beta-decay rates significantly impact age estimates from cosmochronometry.

79 ASTRONOMY AND ASTROPHYSICS↗

Ignition of Carbon Burning from Nuclear Fission in Compact Stars

Abstract Type Ia supernovae (SN Ia) are powerful stellar explosions that provide important distance indicators in cosmology. Recently, we proposed a new SN Ia mechanism that involves a nuclear fission chain reaction in an isolated white dwarf (WD). The first solids that form as a WD starts to freeze are actinide rich and potentially support a fission chain reaction. In this Letter, we explore thermonuclear ignition from fission heating. We perform thermal diffusion simulations and find at high densities, above about 7 × 10 8 g cm −3 , that fission heating can ignite carbon burning. This could produce an SN Ia or another kind of astrophysical transient.

79 ASTRONOMY AND ASTROPHYSICS↗

Radiological Degradation of Tetraoctyl Diglycolamide in n-Alkyl Solvents: Influence of Solvent Ionization Potential

Reprocessing of used nuclear fuel reduces the requirements for long-term storage repositories. Cost-efficient processes depend on knowledge of radiation effects, but gaps occur in understanding how radiation results in the degradation of fuel separation molecules. This project investigates the influence of different n-alkyl solvents on the radiolytic fragmentation behavior of N,N,N',N'-Tetraoctyl-3-oxapentane-1,5-diamide (TODGA), a promising ligand for extraction of the lanthanides and minor actinides from dissolved nuclear fuel. Findings from this work suggest a linkage between the ionization potential of the solvent and the degradation products observed in the resulting mass spectrum.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Chemical Fractionation is not a Constant: Revisiting Bomb Vapor Chemistry

The debris produced by a nuclear explosion forms a hazard to response, can serve as a record used to interpret the event, and may persist in the environment necessitating long term management. Hence, understanding the radiochemical inventory of nuclear debris remains an important area of study, particularly the behavior and resulting distribution of actinides and fission products. Despite formation in a high energy environment, it has been recognized for decades that the chemical and isotopic composition of debris rarely, if ever, captures a homogenized blend of the bomb products. Instead, during cooling and debris formation, a variety of chemical processes cause separation of the different constituents. This process of chemical fractionation creates debris with a variety of different radionuclide inventories. Here we provide an overdue re-examination of our historic basis for understanding chemical fractionation in nuclear explosions through the context of new characterization of a large set of historical nuclear test data. Finally, we then discuss the implications of our findings for advancing models of radionuclide distribution and postdetonation chemical fractionation.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Lipophilic diglycolamide compounds for extraction of rare earth metals from aqueous solutions

A method for extracting rare earth metals (e.g., lanthanides and/or actinides) from aqueous solution, the method comprising: (i) acidifying an aqueous solution containing said rare earth metals with sulfuric acid to result in an acidified aqueous solution containing 1-12 M concentration of sulfuric acid; and (ii) contacting the acidified aqueous solution with an aqueous-insoluble hydrophobic solution comprising a rare earth extractant molecule dissolved in an aqueous-insoluble hydrophobic solvent to result in extraction of one or more of the rare earth metals into the aqueous hydrophobic solution, wherein the rare earth extractant molecule has the following structure: wherein R1, R2, R3, and R4 are independently selected from hydrocarbon groups containing 1-20 carbon atoms, provided that the total carbon atoms in R1, R2, R3, and R4 is at least 12; and R5 and R6 are independently selected from hydrogen atom and hydrocarbon groups containing 1-3 carbon atoms.

Brigham, Derek↗

University Research to Support the MPACT 2020 Milestone

University research is a strong focus of the Office of Nuclear Energy within the Department of Energy. This research complements existing work in the various program areas and provides support and training for students entering the field. Four university projects have provided support to the Material Protection Accounting and Controls Technologies (MPACT) 2020 milestone focused on safeguards for electrochemical processing facilities. The University of Tennessee Knoxville has examined data fusion of NDA measurements such as Hybrid K-Edge Densitometry and Cyclic Voltammetry. Oregon State University and Virginia Polytechnic Institute have examined the integration of accountancy data with process monitoring data for safeguards. The Ohio State University and the University of Utah have developed a Ni-Pt SiC Schottky diode capable of high temperature alpha spectroscopy for actinide detection of molten salts. Finally, the University of Colorado has developed a key enabling technology for the use of Microcalorimetry.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Design Optimization for EUROPA Critical Experiment

The Experiment for Unresolved Region Of Plutonium Actinides (EUROPA) is an integral critical experiment currently being designed to target the intermediate energy region of plutonium. Intermediate energies, those between 0.625 eV - 100 keV, contain the end of resolved and beginning of the unresolved resonance region, making experiments in this energy range prudent for validating the representation of cross sections in this transition region. Below is the preliminary design of the experiment to be performed at the National Criticality Experiments Research Center (NCERC). Experiment optimization required an exhaustive down selection of several moderating, absorbing, and reflecting materials using Particle Swarm Optimization (PSO) in order to achieve maximum sensitivity to the intermediate energy region.

07 ISOTOPE AND RADIATION SOURCES↗

Sensitivity Studies, Gap Analysis, and Benchmark Experiment Optimization for Reactor Applications

In regards to nuclear data, some reactor applications may lack validation experiments, which reduces confidence in predicted results. This is especially true for emerging advanced reactor, micro reactor, and Accelerator Driven System (ADS) designs. This work presents an approach to design new criticality experiments that have similar k eff cross section sensitivities to an application of interest. This process involves simulations to generate cross-section sensitivities to a parameter of interest (such as k eff ), a gap analysis to determine which existing benchmarks are most similar to the application, and an experiment optimization. This work focuses on cross-section sensitives and gap analysis for three examples relevant to the reactor physics community including a Travelling Wave Reactor (TWR) type-design, Kilopower (a space reactor design), and a lead-bismuth eutectic cooled accelerator-driven system (ADS) to transmute minor actinides.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Integration of Nuclear Material Accounting Data and Process Monitoring Data for Improvement on Detection Probability in Safeguarding Electrochemical Processing Facilities (Final Technical Report)

The KAERI advanced spent fuel conditioning process (ACP) process is a critical component of the US- South Korean nuclear cooperation and the following “123 Agreement.” Its development has received considerable attention in both countries. The ACP is an electrochemical processing (pyroprocessing) that recycles over 96% of the used nuclear fuel (UNF). It is also intrinsically proliferation-resistant in theory. In normal operation, the U/TRU product is very hot radiologically. In addition, the Cm provides a high level of spontaneous neutrons, making the product unsuitable for weapon use. However, as pointed in some study, “the need for safeguards to protect against the diversion and misuse of separated plutonium applies essentially equally to all grades of plutonium.” As pointed by many studies, the well-established traditional Nuclear Material Accounting (NMA) approach cannot be directly applied to electrochemical processing because of the lack of an input accountability tank, the non-continuous material flow, and the unsatisfactory level of confidence in sampling methods. Therefore, nuclear safeguards remain a grand challenge in the developing of commercial electrochemical separations facilities, especially around the heart of such facilities, the electrorefiner (ER) systems. In contrast to NMA data, process monitoring (PM) data is normally an indirect measurement of the SNM and is acquired much more frequently. In a broad sense, PM includes monitoring by various types of equipment, e.g. radiation detectors, cameras, voltage, current sensors. Because it is already being collected by the operator, the additional cost to safeguards is low. It has long been believed that PM data can supplement NMA data and help improve safeguards, although the benefits are hard to quantify. The U.S. DOE’s Material Protection, Accounting, and Control Technology (MPACT) campaign has made substantial investments into innovative PM sensor technology and predictive model development for real- or near real-time measurement and prediction of molten salt density and level, salt composition and actinide concentration especially Pu, the cell voltage, and the cell current to supplement traditional NMA. For aqueous-based reprocessing facilities, it is reported that PM, integrated with traditional NMA, have a high detection probability for specific diversions. For electrochemical reprocessing, preliminary studies have shown that PM data can support traditional NMA in various ways by providing a basis to estimate some of the in-processing nuclear material inventories. Despite early success, further studies on fusion of PM data and NMA data are still needed, which is the goal of this proposed work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Impact of Irradiation-induced Lattice Defects and Dopants on Thermal Transport in Oxide Nuclear Fuels

Advanced nuclear reactor concepts aim to use fuels that must withstand unprecedented temperature and radiation extremes. In these fuels, thermal energy transport under irradiation is directly related to fuel longevity, reactor safety, and is arguably one of the most important performance metrics. Here we provide a comprehensive, first-principles-informed treatment of phonon mediated thermal transport in a defect-bearing actinide oxide with direct comparison to experimental measurements. Pristine and proton irradiated thorium dioxide was chosen as a model system to treat the complexity of thermal transport in the presence of lattice defects. A thermal transport model is implemented using the linearized Boltzmann transport equation (LBTE) with input from first principles calculations and defect evolution models. The output of the LBTE is compared directly to mesoscopic measurements of thermal conductivity on length scales commensurate with defect accumulation. Parametric measurements of conductivity with irradiation dose and temperature reveal a monotonic decrease in conductivity with irradiation dose, in the range of 0.001 dpa to 0.1 dpa. Besides radiation-induced defects, doping the thorium dioxide crystal with small quantities of uranium atoms also results in a drastic reduction in thermal conductivity. Temperature-dependent measurements of thermal conductivity in uranium-doped thorium dioxide single crystals suggests a resonant scattering mechanism is responsible for the observed reduction. This comprehensive, atomistic- to meso-scale treatment provides the necessary basis to investigate thermal transport under irradiation in more complex systems that exhibit strong electron correlation. This is a poster presentation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The Role of Pulse Radiolysis in Advanced Nuclear Fuel Cycles

The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. The complexity and intensity of these effects are greatest during reactor operations and in the management of used nuclear fuel and waste. Radiation-induced processes typically promote the chemical transformation of molecules and materials with the formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of nuclear technologies. Consequently, a molecular-level understanding of radiation effects over multiple time, distance, and material domains is essential for the innovation and deployment of next generation nuclear technologies. Attaining this knowledge necessitates a firm grasp of radiation-induced reaction kinetics, for which pulsed electron radiolysis is the methodology of choice. Presented here are several recent studies from our group that demonstrate the critical role of pulsed electron radiolysis techniques in the advancement of our understanding of radiation-induced chemistry under advanced nuclear fuel cycle conditions. Research topics include late actinide redox chemistry, radiation robustness of used nuclear fuel reprocessing complexants, and the behavior of metal cations in high temperature molten salt media.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Modeling the Fundamental Radiation Chemistry of the Organic Diluent, and the Effect of Metal Ion Complexation on the Radiochemical Behavior of Active Compounds

All used nuclear fuel (UNF) reprocessing technologies must operate efficiently in the presence of an intense, multi-component (predominantly alpha, beta, and gamma) radiation field. Consequently, radiation-induced degradation of reprocessing systems is of concern, as it negatively impacts process performance over time due to the destruction of both active compounds (ligands, phase modifiers, holdback agents, etc.) and the formation of degradation products. Reprocessing solvent system radiolysis has been linked to changes in separation efficiency and physical properties of solvent mixtures, solvent-recycle longevity, crud formation, and other unexpected outcomes that impact the efficient recovery of valuable materials (e.g., the actinides) and the volume of hazardous radioactive waste for final disposal, i.e., in a geological repository. Consequently, a fundamental understanding of radiolytic processes and their effects on reprocessing solvent system performance is critical for: (i) the cost-effective development and innovation of separation technologies; (ii) the design and implementation of predictive radiation chemical models for process monitoring and lifetimes; and (iii) potentially the ability to exploit radiolytic phenomenon to our benefit, e.g., strategic radiolysis of active molecules to liberate specific degradation products that aid subsequent process stages. Despite extensive investigation into the radiolytic behavior of active solvent system compounds, little attention has been given to understanding (i) the radiation chemical behavior and modification of the organic diluent and (ii) the effect of metal ion complexation on the radiochemical behavior of active compounds.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

TMS 2023 - Methodology and Density of PuCl3-NaCl Mixtures

The development of molten salt reactors and their associated components demands reliable and accurate thermophysical property data for design and validation. A candidate fuel salt, PuCl3-NaCl (36 mol% PuCl3) has been synthesized and studied at the Idaho National Laboratory. This study has determined the density of PuCl3-NaCl at multiple compositions and temperatures, providing data for validation of modeling efforts and making improvements on the buoyancy method for density measurements of actinide-bearing molten salts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

PARTITIONING AND TRANSMUTATION OF USED NUCLEAR FUEL IN SUPPORT OF GEOLOGICAL WASTE DISPOSAL

Nuclear energy is a low-carbon technology that generates bulk baseload electricity and supports long-lasting eco-friendly sustainability goals. However, it still faces challenges, such as the securing and managing of long-lived nuclear actinides and fission products—most notably the used fuel, which is considered high-level waste (HLW). Direct geological waste disposal would be the most economical option for HLW but requires highly qualified sites whose geophysical behavior will remain stable for 10,000 years. Partitioning and transmutation (P&T) of used fuel reduces radioactivity and decay heat generation, enabling efficient geological waste disposal. P&T research and development, along with the prospects of P&T techniques such as wet/dry separation and accelerator-driven systems, were reviewed to identify critical needs that must be met to foster their successful implementation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Manufacture of particulate reference materials

Methods for forming particulates that are highly consistent with regard to shape, size, and content are described. Particulates are suitable for use as reference materials. Methods can incorporate actinides and/or lanthanides, e.g., uranium, and can be used for forming certified reference materials for use in the nuclear industry. Methods include formation of an aerosol from an oxalate salt solution, in-line diagnostics, and collection of particles of the aerosol either in a liquid impinger or on a solid surface.

Wellons, Matthew S.↗