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Duration of a Magma Ocean and Subsequent Mantle Overturn in Mars: Evidence from Nakhlites

It is now generally accepted that the heat produced by accretion, short-lived radioactive elements such as Al-26, and gravitational energy from core formation was sufficient to at least partially melt the silicate portions of terrestrial planets resulting in a global-scale magma ocean. More particularly, in Mars, the geochemical signatures displayed by shergottites, are likely inherited from the crystallization of this magma ocean. Using the short-lived chronometer Sm-146 - Nd-142 (t(sup 1/2) = 103 Myr), the duration of the Martian magma ocean (MMO) has been evaluated to being less than 40 Myr, while recent and more precise ND-142/ND-144 data were used to evaluate the longevity of the MMO to approximately 100 Myr after the solar system formation. In addition, it has been proposed that the end of the crystallization of the MMO may have triggered a mantle overturn, as a result of a density gradient in the cumulate layers crystallized at different levels. Dating the mantle overturn could hence provide additional constraint on the duration of the MMO. Among SNC meteorites, nakhlites are characterized by high epsilon W-182 of approximately +3 and an epsilon Nd-142 similar to depleted shergottites of +0.6-0.9. It has hence been proposed that the source of nakhlites was established very early in Mars history (approximately 8-10 Myr). However, the times recorded in HF-182-W-182 isotope system, i.e. when 182Hf became effectively extinct (approximately 50 Myr after solar system formation) are less than closure times recorded in the Sm-146-Nd-142 isotope system (with a full coverage of approximately 500 Myr after solar system formation). This could result in decoupling between the present-day measured epsilon W-182 and epsilon Nd-142 as the SM-146 may have recorded later differentiation events in epsilon ND-142 not observed in epsilon W-182 values. With these potential complexities in short-lived chronological data for SNC's in mind, new Hf-176/Hf-177, Nd-143/Nd-144 and Nd-142/Nd-144 were obtained for three nakhlites (Nakhla, MIL03346 and Yamato000593). These new data are combined with previous epsilon W-182 data, to investigate potential discrepancies between the Hf-182-W-182 and Sm-146-Nd-142 systematics, and the relationship between the source of nakhlites and a crystallizing magma ocean

Debaille, V.↗

The Double-Peaked SN 2013ge: A Type Ib/c Sn with an Asymmetric Mass Ejection or an Extended Progenitor Envelope

We present extensive multiwavelength (radio to X-ray) observations of the Type Ib/c supernova (SN Ib c) SN 2013ge from -13 to +457 days relative to maximum light, including a series of optical spectra and Swift UV-optical photometry beginning 2-4 days post-explosion. This data set makes SN 2013ge one of the best-observed normal SNe Ib/c at early times-when the light curve is particularly sensitive to the progenitor configuration and mixing of radioactive elements -and reveals two distinct light curve components in the UV bands. The first component rises over 4-5 days and is visible for the first week post-explosion. Spectra of the first component have blue continua and show a plethora of moderately high velocity (approximately 15,000 km/s) but narrow (approximately 3500 km/s)spectroscopic features, indicating that the line-forming region is restricted. The explosion parameters estimated for the bulk explosion (M(sub ej) approximately 23 solar mass; E(subK) approximately (1-2) x 10(exp 51) erg) are standard for SNe Ib/c, and there is evidence forweak He features at early times-in an object that would have otherwise been classified as Type Ic. In addition,SN 2013ge exploded in a low-metallicity environment (approximately 0.5 atomic mass), and we have obtained some of the deepest radio and X-ray limits for an SN Ib/c to date, which constrain the progenitor mass-loss rate to be M less than 4 x 10(exp -6) solar mass/yr. We are left with two distinct progenitor scenarios for SN 2013ge, depending on our interpretation of the early emission. If the first component is cooling envelope emission, then the progenitor of SN 2013ge either possessed an extended (greater than or approximately 30 solar radius) envelope or ejected a portion of its envelope in the final less than or approximately 1 yr before core collapse. Alternatively, if the first component is due to outwardly mixed Ni-56, then our observations are consistent with the asymmetric ejection of a distinct clump of nickel-rich material at high velocities. Current models for the collision of an SN shock with a binary companion cannot reproduce both the timescale and luminosity of the early emission in SN 2013ge. Finally, the spectra of the first component of SN 2013ge are similar to those of the rapidly declining SN 2002bj.

supernovae: general – supernovae: individual (SN↗

EARLY IMPACT MELTING AND SPACE EXPOSURE HISTORY OF THE PAT91501 LCHONDRITE

Collisions probably occurred frequently in the early history of the asteroid belt. Their effects, which should be recorded in meteorites, must have included heating and melting along with shock alteration of mineral textures. Some non-chondritic meteorite types e.g., eucrites and IIE and IAB irons - do indeed give evidence of extensive impact heating more than 3.4 Gyr ago. The ordinary chondrites, in contrast, show little evidence of early impact heating. The Ar-Ar and Rb-Sr ages of ordinary chondrites that experienced intense shock are for the most part relatively young, many less than 1.5 Gyr. The numerous L-chondrites with Ar- Ar ages clustering near 0.5 Gy are a well-known example. One of them, the 105-kg Chico Lchondrite, shows the effects of unusually intense heating. It is approximately 60% impact melt and likely formed as a dyke beneath a large crater when the L-chondrite parent body underwent a very large impact approximately 0.5 Gyr ago. In rare instances, older shock dates are indicated for ordinary chondrites. Dixon et al show early impact resetting of Ar-Ar ages of a few LL-chondrites including MIL 99301 at 4.23 0.03 Gyr, but in none of these stones did shock lead to extensive melting. As of 2003, searches for chondritic melts attributable to early shock had turned up only the Shaw L-chondrite, which has an Ar-Ar age of approximately 4.42 Gyr. PAT91501 is an 8.55-kg L-chondrite containing vesicles and metal-troilite nodules. It is a unique, near-total impact melt, unshocked, depleted in siderophile and chalcophile elements, and contains only approximately 10% relic chondritic material. The authors conclude that PAT91501 crystallized rapidly and from a much more homogeneous melt than did Shaw. They suggest that PAT resembles Chico and likely formed as an impact melt vein within an impact crater. To define the history of PAT, we have determined its Ar-39-Ar-40 age and measured several radioactive and stable nuclides produced during its space exposure to cosmic rays.

Bogard, Donald D.↗

Subject-specific modeling framework for particle deposition using computational fluid dynamics

Quantifying particle deposition and dose in the respiratory tract requires a physiologically realistic representation and reproducible computational workflows. However, existing modeling frameworks, such as the International Commission on Radiological Protection (ICRP) compartmental models and the Multiple Path Particle Dosimetry (MPPD) tool, lack detailed deposition profiles and subject-specific capabilities. The combination of advances in computer vision algorithms applied to the respiratory tract and Computational Fluid and Particle Dynamics (CFPD) allows high-fidelity simulations of particle behavior in anatomically accurate geometries derived from individual CT scans. The segmentation, preprocessing, and file preparation task for a CFPD simulation was often time-consuming, and no prior studies to-date have yet presented a fully automated framework. This work presents a fully automated workflow to obtain individualized particle deposition profiles in the human respiratory tract. The pipeline starts with segmenting upper and lower airway geometries using morphological and deep learning-based methods, generating three-dimensional (3D) models from CT imaging data. Next, a series of algorithms are presented to quality check and prepare the 3D geometry for a CFD or CFPD simulation. The preprocessing step includes correcting geometric artifacts, enforcing a physically consistent mesh, and automatically identifying and capping multiple outlets, which is required for CFD/CFPD simulations. These processed models are then input into open-source (OpenFOAM) or commercial (StarCCM+) CFD solvers, where flow and transient particle transport equations — including turbulence and particle–wall interactions are solved under realistic breathing conditions. Finally, the resulting particle deposition profiles can be integrated with Monte Carlo radiation transport codes and state-of-the-art computational phantoms to assess organ-specific absorbed doses in scenarios of radioactive aerosol inhalation. The presented work streamlines respiratory tract segmentation, preprocessing for CFD/CFPD simulations, and integration with dose assessment workflows, reducing manual intervention and improving access to high-fidelity, subject-specific modeling. The high precision in predicted particle deposition and dose distributions can improve personalized treatment strategies in respiratory medicine and refine dose estimates for radiation protection.

AI↗

M3SF-25LL010302052 - Radionuclide Interaction with Hydrothermally Altered Repository Materials

This progress report (Level 3 Milestone Number M3SF-25LL010302052) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Host Rock Properties & Processes - LLNL Number SF-25LL01030205. Observed changes in radionuclide sorption after bentonite/clay heating have implications for radionuclide diffusive transport through engineered barriers and must be considered when designing waste disposal repositories. Recent research performed at Los Alamos National Laboratory (LANL) has provided key insights regarding the hydrothermal alteration behavior of bentonite backfill in the presence of repository materials (steel, concrete, etc.). We are examining how this mineral alteration affects retardation behavior of a suite of radionuclides of interest to repository performance assessment. Sorption experiments and data analysis for 233 U were initiated in FY24 following earlier experiments performed on 243 Am, 90 Sr, 137 Cs. In FY25, we completed the 233 U study and initiated and completed a study of 237 Np sorption. Below, we summarize the results and potential impacts of hydrothermal alteration on radionuclide retardation and assess the importance of this process to radionuclide migration from a GHRDC. We also use statistical tools (i.e. PCA) to help us determine the major drivers in affecting changes in measured Kd values induced by hydrothermal alteration. These experiments also allow us to test the predictive ability of our component additivity approach to surface complexation and ion exchange. Our guiding hypothesis is that a robust surface complexation/ion exchange model and associated database can effectively predict changes in radionuclide sorption behavior resulting from the hydrothermal alteration of mineralogy in a repository near field. In November 2024 the paper “Selenium interaction with iron minerals: Quantitative comparison of sorption and coprecipitation impacts on mobility” was published in Applied Geochemistry. A short update of results to date is presented below. In FY25, we also actively supported the DITUSC project, which is part of the EURADII initiative, as associate partners. We are executing the Migration2025 conference and support associated the NEA-TDB and Thermochimie workshops that will provide critical international engagements and develop consensus and synergy in thermodynamics as it relates to supporting the US nuclear waste repository program.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Rise and Fall of the Type Ib Supernova iPTF13bvn Not a Massive Wolf-Rayet Star

Context. We investigate iPTF13bvn, a core-collapse (CC) supernova (SN) in the nearby spiral galaxy NGC 5806. This object was discovered by the intermediate Palomar Transient Factory (iPTF) very close to the estimated explosion date and was classified as a stripped-envelope CC SN, likely of Type Ib. Furthermore, a possible progenitor detection in pre-explosion Hubble Space Telescope (HST) images was reported, making this the only SN Ib with such an identification. Based on the luminosity and color of the progenitor candidate, as well as on early-time spectra and photometry of the SN, it was argued that the progenitor candidate is consistent with a single, massive Wolf-Rayet (WR) star. Aims. We aim to confirm the progenitor detection, to robustly classify the SN using additional spectroscopy, and to investigate if our follow-up photometric and spectroscopic data on iPTF13bvn are consistent with a single-star WR progenitor scenario. Methods. We present a large set of observational data, consisting of multi-band light curves (UBVRI, g′r′i′z′) and optical spectra. We perform standard spectral line analysis to track the evolution of the SN ejecta. We also construct a bolometric light curve and perform hydrodynamical calculations to model this light curve to constrain the synthesized radioactive nickel mass and the total ejecta mass of the SN. Late-time photometry is analyzed to constrain the amount of oxygen. Furthermore, image registration of pre- and post-explosion HST images is performed. Results. Our HST astrometry confirms the location of the progenitor candidate of iPTF13bvn, and follow-up spectra securely classify this as a SN Ib. We use our hydrodynamical model to fit the observed bolometric light curve, estimating the total ejecta mass to be 1.9 solar mass and the radioactive nickel mass to be 0.05 solar mass. The model fit requires the nickel synthesized in the explosion to be highly mixed out in the ejecta. We also find that the late-time nebular r′-band luminosity is not consistent with predictions based on the expected oxygen nucleosynthesis in very massive stars. Conclusions. We find that our bolometric light curve of iPTF13bvn is not consistent with the previously proposed single massive WR-star progenitor scenario. The total ejecta mass and, in particular, the late-time oxygen emission are both significantly lower than what would be expected from a single WR progenitor with a main-sequence mass of at least 30 solar mass.

massive↗

BWR Spent Nuclear Fuel Acquisition and Testing to Support DOE-NE High Burnup Spent Fuel Data Project

The Office of Spent Fuel and Waste Disposition (SFWD) within the US Department of Energy (DOE) Office of Nuclear Energy (NE) established the Spent Fuel and Waste Science and Technology (SFWST) campaign to conduct research and development (R&D) activities related to the storage, transportation, and disposal of spent nuclear fuel (SNF) and high-level radioactive waste. The SFWST program was created within SFWD to address issues of extended or long-term SNF storage and transportation. Some near-term objectives of SFWST are to use a science-based, engineering-driven approach to: Support the enhancement of the technical bases to support the continued safe and secure dry storage of SNF for extended periods; Support the enhancement of the technical bases for retrieving SNF after extended dry storage; Support the enhancement of the technical bases for transporting high burnup (HBU) fuel and transporting low burnup fuel and HBU fuel after dry storage DOE-NE, in partnership with the Electric Power Research Institute, developed the High Burnup Spent Fuel Data Project to perform a large-scale demonstration and laboratory-scale testing of HBU pressurized water reactor (PWR) fuels (exceeding 45 gigawatt-days per metric ton of uranium [GWd/MTU]). Under this project, 25 sister rods—which are rods that have the same design, power histories, and other characteristics—were removed from assemblies at the North Anna Nuclear Power Station and sent to Oak Ridge National Laboratory (ORNL) in January 2016. ORNL performed detailed nondestructive examination (NDE) on all 25 rods. The NDE consisted of visual examinations, gamma and neutron scanning, profilometry and rod length measurements, and eddy current examinations. After completing the NDE, 10 of the sister rods were delivered to Pacific Northwest National Laboratory (PNNL) in a NAC International, Inc. legal-weight truck cask in September 2018 for destructive examination (DE). To date, SFWD work has focused on the PWR fuel that is part of the Sister Rod Test program. No boiling water reactor (BWR) fuel has been tested in the program, and the data needs that were identified for the PWR fuel have not been collected for BWR fuel. The goal to obtain six to nine BWR rods and test them at ORNL will support closing this important data gap. BWR fuel comprises approximately 56% of the total fuel assemblies currently in storage at nuclear power plants in the United States. BWR nuclear fuel and cladding designs and manufacturing are significantly different from PWRs. Differences include the following: BWR fuel pellets are larger than PWR pellets; Variations of Zircaloy-2 (including liners) are used instead of the Zircaloy-4 cladding materials used in PWRs; Clad manufacturing and stress-relief processes are different between PWRs and BWRs; The fuel rod dimensions are different because larger rod diameters and thicker cladding are used in BWRs; BWR fuel typically has lower internal rod pressures and sees vastly different operating conditions than PWR fuel (i.e., two-phase flow); BWR assemblies are “canned,” meaning each assembly is surrounded by a metal fuel channel; BWR cladding is often composed of an inner pure Zr liner that has widely different mechanical properties than the Zircaloy-2 alloy and exhibits a stronger affinity for hydrogen; The BWR SNF generally has more total hydrogen in the cladding/liner than typical PWR fuel; The construction of the PWR and BWR assemblies is vastly different; BWR rods are solidly attached to the assembly nozzles and experience a much different vibration and shock load than PWR rods, which are “floating” within a grid system attached to guide tubes, and the rods sit loosely on the bottom end plates. These numerous differences will affect the way the BWR SNF responds under dry storage preparation processes (e.g., vacuum drying) and during transportation. The results collected in the PWR experimental program must be compared with a subset of similar data collected on BWR SNF to establish a technical basis for whether the larger PWR database is sufficient to bound the BWR SNF end-of-life conditions as is currently assumed for several fuel/clad properties. Changes that occur in both fuel types at HBU could exacerbate any mechanical property differences. As the fuel burnup increases, several changes occur that might affect the performance of the fuel, cladding, and assembly hardware in storage and transportation. These changes include increased cladding corrosion layer thickness, increased cladding hydrogen content, increased cladding creep strains, increased fission gas release, and the formation of the HBU structure at the surface of the fuel pellets. The Nuclear Regulatory Commission (NRC) limits the current maximum rod-averaged burnup to 62 GWd/MTU due to these changes and the lack of data at higher burnups.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Physics Division Strategic Plan Fiscal Years 2020-2024

The vision of the Physics Division (PHY) at Argonne National Laboratory is to continue enhancing its role as a world-leading institution in basic nuclear physics research and its applications. Key to this vision is for PHY to continue to safely and effectively operate and evolve the capabilities of the Argonne Tandem Linac Accelerator System (ATLAS) facility to best serve its users. ATLAS is the Department of Energy (DOE) accelerator facility for low-energy nuclear physics research. The research carried out by PHY covers many themes in contemporary science but can be distilled into five areas of focus. These themes are interconnected, with continuously evolving synergies between the various groups and facilities in PHY and the broader Laboratory. This five-year strategic plan serves to illustrate our current capabilities and new directions related to these five areas of focus (ATLAS also develops an independent strategic plan): Accelerator research and design. The goal of this theme is to design, fabricate, test, and implement novel accelerator systems, with a focus on high-intensity ion and electron systems. These R&D activities have led to enhancements in the ATLAS accelerator system. Among others, the division’s accelerator systems are in use or planned for use at Fermilab, the Advanced Photon Source, and in a broad variety of applications at the Facility for Rare Isotope Beams (FRIB). Atom trapping and fundamental symmetries. The goal of this theme is to explore and exploit the uses of advanced laser cooling and trapping techniques to manipulate atoms. There are three main areas of focus. First is in the application of the atom trap trace analysis (ATTA) technique for age determination of groundwater and ice by using radio-krypton dating. The next two trapping-based programs involve tests of fundamental symmetries in nature: the cooling and trapping of radium-225 with the aim of determining limits on an observation of its electric dipole moment and precision measurements of the beta decay properties of helium-6 to set limits on the tensor coupling constant. This is complemented by measurements of similar properties in lithium-8 and boron-8. Nuclear astrophysics. The goal of this theme is to enhance our understanding of how elements are created in the universe via explosive nucleosynthesis and how stars evolve. To meet the challenges of this theme, many of the capabilities of ATLAS are being enhanced, including the development of new beams through a new in-flight separator (RAISOR) and the anticipated neutron-generator upgrade of the Californium Rare Isotope Breeder Upgrade facility (nuCARIBU). These are coupled to state-of-the-art instruments such as the Canadian Penning Trap, Helical Orbit Spectrometer, Gammasphere, GRETINA, Multi-Sampling Ionization Chamber, the Fragment Mass Analyzer, and Argonne Gas-filled Fragment Analyzer, and a new low-background experimental area for decay studies. Nuclear structure. The goal of this theme is to understand the structure of nuclei, both stable and radioactive, in terms of single-particle properties, their shapes, and the dynamics governing reactions between them. These include questions such as what are the limits of nuclear stability and what are the properties of super heavy nuclei. As with the nuclear astrophysics theme, the capabilities of ATLAS, guided by the ATLAS user community, are continuously being enhanced to this end. The Division has strategic initiatives to play a leading role in the development of instrumentation and research programs at the FRIB. Quantum chromodynamics (QCD) and hadron physics. The goal of this theme is to lead major research programs focused on revealing the quark and gluon structure of protons, neutrons, nuclei, and short-lived mesons and baryons. These involve major programs at Jefferson Lab, Fermilab, and smaller facilities. They are complemented by theoretical endeavors centered on the question of how hadrons and their properties emerge from QCD. Out of these activities arise strategic initiatives to play a major role in the forthcoming Electron-Ion Collider (EIC).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Informing solar blind radioluminescence imaging through a calibrated spectrum

While direct radiation detection methods offer great insight into the origin of ionizing particles and photons, their use to locate contaminated areas or concealed radioactive sources can lead to undue exposure of personnel and equipment to ionizing radiation or the potential for contamination. These same sources induce ultraviolet (UV) optical photon fluorescence in air – a process referred to as radioluminescence – that may be imaged from low dose regions over larger attenuation lengths than ionizing radiation. However, most optical detection methods are limited to low lighting conditions to image the more abundant ultraviolet-A (UV-A) photons. To extend this capability to room light or daytime conditions, the solar blind region (Ultraviolet-C (UV-C), <280 nm) can be tapped. Though the emission yield of UV-C photons is roughly two orders of magnitude lower than that in the UV-A regime, the UV-C offers dramatic improvements in signal-to-noise ratios under bright lighting conditions due to decreased background interferences. The yield of specific UV-C lines, if present in the literature at all, varies widely, which has a large impact in modeling and analyzing standoff UV-C measurement scenarios. Thus, we have captured improved radioluminescence spectra over 250–400 nm and identified observed emission peaks in ambient air. Many of the UV-C photons produced by ionizing radiation excitation result from high-energy, molecular nitrogen Gaydon-Herman transitions which have had limited study to date for this application. Relating these findings to published UV-A yields, we estimate emissions between 0.15–0.19 photons/MeV over 250–280 nm. Additionally, we also use a commercial corona-discharge imaging camera to demonstrate outdoor UV-C radiation mapping of alpha and gamma emitters from 50 and 75 m standoffs, respectively. The imaged “counts” are compared to optically modelled values and show the same trend over distance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Analysis of Hydrology and Interim Measure Performance in the Chromium Plume at Los Alamos National Laboratory - 20498

Hexavalent chromium, Cr(VI), is present in the regional aquifer beneath Los Alamos National Laboratory (LANL) at concentrations greater than the New Mexico groundwater standard (50 ppb). The source of the Cr is blowdown from a power plant where potassium dichromate was used as a corrosion inhibitor from 1956 to 1972. Blowdown comingled with effluent from another source and migrated approximately 3 miles down a canyon, primarily as surface flow, until reaching an alluvial infiltration zone. The infiltrating water moved vertically through a thick (approximately 900 ft), complex stratigraphic sequence of unsaturated tuffs, basalt, and unconsolidated alluvial deposits. Horizontal transport also took place within spatially limited perched groundwater horizons in the vadose zone (VZ). Breakthrough at the regional aquifer water table is thought to have occurred in multiple hydraulic windows or 'drip points' located approximately 3 miles from the initial release site at the power plant. The regional aquifer is highly heterogeneous and anisotropic, and displays unconfined behavior in an upper zone and confined behavior at depth. The Cr(VI) contamination has so far remained confined to the upper approximately 25 m of the aquifer. The ambient hydraulic gradient in the regional aquifer is toward the east/southeast, but the water table is extremely flat in the Cr plume area compared to surrounding areas. There is some local variability in flow direction, potentially related to effects of seasonal pumping from nearby Los Alamos county water-supply wells, which draw from the regional aquifer several hundred feet below the water table. An interim measure (IM) is currently operating at the site to achieve hydraulic control of plume migration using a series of extraction wells, ion-exchange treatment, and injection along the downgradient portion of the plume. The migration of Cr contamination in the aquifer has been previously evaluated using a calibrated probabilistic numerical model, which has also been used to design the spatial configuration of extraction and injection wells for the IM, and to identify locations for monitoring wells. The model is built using the Finite Element Heat and Mass (FEHM) transfer code, and the Model Analysis and Decision Support (MADS) software is used for analyses. To date, the portion of the IM system that has operated in a continuous manner has been very effective at hydraulic control. Modifications to the flow field associated with the influence of IM pumping and injection are evaluated here, with modeling constraints to be provided by recent observations of tracers injected into both monitoring wells and IM injection wells, as well as opportunistic observations of geochemical signatures of treated ion-exchange effluent injected into IM injection wells. The tracer and geochemical data provide insights into modified flow directions within the Cr plume area that cannot be otherwise obtained. Results of the modeling work are being used to inform adaptive management of IM operations and will be a valuable tool for development and refinement of long-term remediation strategies. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

First experimental determination of the ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar reaction cross section and ³⁹Ar production in Earth’s atmosphere

The cosmogenic ³⁹Ar(t1∕2 = 268 years) isotope of argon is used for geophysical dating and tracing of underground and ocean water, as well as ice owing to its appropriate half-life and chemical inertness as a noble gas; ³⁹Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main ³⁹Ar cosmogenic production reaction in the atmosphere, namely ⁴⁰Ar(𝑛, 2𝑛)39 Ar, using 14.8 ± 0.3 MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the ⁴⁰Ar isotope and were monitored by a stack of fast-neutron activation foils. The reaction yield was measured by atom counting of long-lived ³⁹Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon (³⁹Ar/Ar= 8.12 × 10−16 ). A total ⁴⁰Ar(𝑛, 2𝑛)39 Ar cross section of 610 ± 100 mb was determined at 14.8 ± 0.3 MeV incident neutron energy. This result serves as a benchmark for recent theoretical calculations and evaluations, found to reproduce well the experimental total cross section. We use these energy-dependent theoretical cross sections together with experimental spectra of cosmogenic neutrons at different altitudes to calculate the global average rate of neutron-induced ³⁹Ar atmospheric production, resulting in 770 ± 240 39 Ar atoms/cm²/day. The secular equilibrium between the ³⁹Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance ³⁹Ar/Ar = (5.9 ± 1.8) × 10−16 , showing that ≈73% of atmospheric ³⁹Ar is produced by cosmogenic neutrons, the remaining part believed to be induced by muons and high-energy 𝛾 rays. The ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar cross section at 14 MeV is also a key parameter for quantifying the anthropogenic contribution to atmospheric 39 Ar produced during the thermonuclear tests of the 1960s. We estimate that anthropogenic ³⁹Ar accounts for roughly 20% of the present atmospheric inventory.

39 Ar atmospheric production↗

Temperature dependence of uranium and thorium partitioning in igneous zircons

Zircon is a key mineral in geochronology because of its chemical and physical durability and tendency to incorporate radioactive trace elements such as U and Th. Quantifying the partitioning of the actinide elements is critical to constrain initial non-secular equilibrium amounts of 230 Th in zircon. An excess or deficit of 206 Pb will be produced from such an initial excess/deficit of 230 Th from the secular equilibrium condition, which influences the calculated 206 Pb/ 238 U age (Schärer, 1984, Mattinson, 1973). However, there is no standard way to calculate Th/U partitioning ratios when applying age corrections to young igneous zircon, making uncertainties hard to estimate. To better understand U and Th partitioning of zircon/melt that is the cornerstone of the secular disequilibrium correction, zircon was synthesized in one-atmosphere experiments using basaltic andesite, andesite, and rhyolite starting materials, doped with Zr, U, and Th. Different experimental temperatures and oxygen fugacity conditions (ΔQFM−4 to ΔQFM+4) were explored to examine their effects on U and Th partitioning. In addition, we specifically quantify the effects of sector zoning, fractional crystallization, and melt composition on U and Th partitioning. By combining experimental and natural zircon data, we find that temperature has the primary control on the partitioning of U and Th in the zircon and calibrate an inverse relationship between these partition coefficients and crystallization temperatures. The calibrated equation can be applied to the 230 Th correction for an improvement in the accuracy of Th-corrected 206 Pb/ 238 U dates when the zircon crystallization temperature is known.

206Pb/238U dating↗

Performance Criteria for Capture and/or Immobilization Technologies (Revision 1)

The capture and subsequent immobilization of regulated volatile radionuclides from the off-gas streams of a used nuclear fuel (UNF) reprocessing facility has been a topic of substantial research interest for the US Department of Energy and its international counterparts. Removal of specific radionuclides from the plant effluent streams before discharge to the environment is required to meet regulations set forth by the US Environmental Protection Agency. Upon removal, the radionuclides, as well as associated sorbents that cannot be regenerated in a cost-effective manner, are destined for conversion to a waste form. Research in separation and capture methodologies has included a wide range of technology types, and studies of waste forms are correspondingly diverse. In considering the future development and implementation of both sorbents and waste forms, it is necessary to identify benchmark measures of performance to objectively evaluate each sorbent system or waste form. Sets of performance criteria and associated metrics have been developed for sorbent and waste form evaluation. These criteria address physical, radiological, and chemical characteristics, technical practicality, technical maturity, cost, and, for sorbents, system performance. The criteria and metrics appear to be robust and should be applicable despite the eventual waste classification (as either high- or low-level waste). They are flexible enough to address both aqueous reprocessing and electrochemical reprocessing of UNF. These criteria sets can serve as tools to evaluate performance at multiple stages within the development process, and in this revision (Revision 1) they have been used to assess technologies relating to krypton/xenon separations and iodine capture from off-gas streams arising from UNF reprocessing. Assessment of krypton/xenon separations using engineered forms of two zeolite minerals (silver mordenite and hydrogen mordenite in a polyacrylonitrile-based binder [AgZ-PAN/HZ-PAN]) found that the zeolite-based separation is relatively advanced in its development, but several key issues require resolution. First, desorption processes for both krypton and xenon require refinement to provide an understanding of the product purity that can be achieved. Second, adsorption rate data is needed in order to calculate the bed depth required for effective separation. Finally, it is strongly recommended that a technical review of krypton/xenon separation by AgZ-PAN/HZ-PAN be performed to synergize available data and assess the cost savings and operational benefits that may be realized from implementation of this technology. Assessment of metal organic frameworks (MOFs) for their use in the separation of krypton/xenon found that the ideal separation would be performed using a single-column system with a MOF selective for krypton over xenon. A robust research effort should work to identify a krypton-selective MOF designed to operate at temperatures of approximately 0°C or higher, which could be preferred over cryogenic krypton/xenon capture for used fuel reprocessing off-gas streams. In the case of the CaSDB-MOF (the most well-understood xenon sorbent to date), two issues are judged of high importance. First, xenon breakthrough capacity for the CaSDB-MOF in prototypical conditions should be determined. Preliminary research indicates that breakthrough may be near immediate, presenting a substantial obstacle in separative system design. Second, development of desorption methodology should be performed to determine regeneration time, energy requirements, and the product stream composition. Silver-based sorbents (AgZ and AgAero) for use in iodine capture from the dissolver off-gas were evaluated against the established criteria. These sorbents are significantly better understood for this application as a result of research efforts over the past decade. The potential implementation of AgAero at a large scale is hindered by its physical degradation by components of the dissolver off-gas stream. Less is known about the adsorption of iodine by these sorbents from other off-gas streams in the plant. Initial experimental efforts have been closely coordinated in an effort to understand organic iodine (such as would be found in the vessel off-gas) adsorption by AgZ and AgAero. Future work should expand this experimental program, and analysis of other reprocessing facility off-gas streams such as the vitrification off-gas stream should be conducted to better understand other potential applications for iodine sorbents. A review of iodine waste form development shows that this area is diverse and that multiple promising waste forms have been identified for the immobilization of radioactive iodine. Efforts related to the direct conversion of iodine sorbents (including AgZ and AgAero) should be continued because of the advantages of direct conversion in a waste management strategy and other sorbents should continue to be advanced as merited.

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Stormwater Pollution Prevention Plan (SWPPP) for Site Wide Landscaping Project

Kier + Wright, as Qualified SWPPP Developer (QSD), puts forth this Storm Water Pollution Prevention Plan (SWPPP) for the SNL/CA Site Landscaping Project at Sandia National Laboratories/California (SNL/CA), 7011 East Avenue, Livermore, California (SNL/CA). The property is owned by the U.S. Department of Energy, and managed and operated by National Technology & Engineering Solutions of Sandia (NTESS), LLC. The project proposes landscape improvements throughout SNL/CA. Per the California State Water Resources Control Board’s (California State Water Board) Construction General Permit (CGP), a SWPPP is required when 1 acre or more of land is disturbed. The project site area exceeds the minimum acreage threshold of 1 acre and therefore requires SWPPP implementation. QSD has determined the sediment risk for this project, based on soil type at the site and starting and ending dates of construction, to be low (Section 3.4.1 and Appendix B). Receiving water for this project is the Arroyo Seco. QSD has determined the Arroyo Seco to be a high-risk receiving water because it has the three beneficial uses of “spawn”, “cold”, and “migratory” (Sections 3.3 and 3.4.2 and Appendix B). QSD has determined the overall risk level for the site to be Risk Level 2, based on a combination of low sediment risk and high receiving water risk (Appendix B). As such, QSD has delineated a variety of Best Management Practices (BMPs) to be employed during project construction to reduce or eliminate pollutants in stormwater runoff or any other discharges from the Project site. In addition to site-specific BMPs, this SWPPP report provides instruction for on site monitoring. Electronic copies of required documentation such as inspection reports, REAPs, annual report documentation, etc. shall be submitted to NTESS Sandia Delegated Representative via Newforma.

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Implementation of an Experimental Setup Based on the Three-Omega Method for Thermal Conductivity Measurements of Molten Salts

Molten salt reactors (MSRs) are one of the most promising next-generation nuclear reactor designs which use molten salts as the fuel and coolant. To design, model, predict, license, and operate MSRs, the behavior of the fuel and coolant must be understood as a function of temperature and irradiation, i.e., burnup. Of particular importance and complexity is the reliable and reproducible measurement of thermal conductivity of molten salts at high temperatures (> 500 °C). Thermal conductivity provides information on the rate at which heat passes through a specified material and is dependent on chemical composition. Currently, in the national laboratory complex, several methods for measuring thermal conductivity on molten salt systems are under development, however, to date, consistent data have not been produced. Typically, thermal conductivity measurements of high-temperature melts have been conducted by using the Transient Hot Wire (THW) method where thermal conductivity is determined by the change in temperature over time at a certain distance from a heating wire. Another time-dependent technique is the laser flash method, commonly used for solid samples. Laser flash requires prior measurements of density and heat capacity to calculate the thermal conductivity of the sample, introducing additional measurement errors. Steady state and time-dependent measurements such as THW and laser flash have errors from convection and ambient temperature fluctuations (heat radiation). In order to produce high fidelity thermal conductivity data, a measurement technique needs to be developed that will reduce the effect of convection at high temperatures by measuring in a very fast time window. In addition, to measure on actinide and irradiated salts the sample size should be small. Therefore, this project aims to develop a frequency-domain technique based on the three-omega (3?) method, previously proven to work on solids, nanofluids and low temperature solar salts (25 to 250 °C). If the 3?-device can be designed with materials that can withstand high temperatures (>500 °C) and can be configured to reduce errors due to convection, then it would prove to be a valuable technique for ensuring thermal conductivity on molten salt systems needed for MSR development. For this proposal, the 3? instrument will be designed, assembled, and tested on non-radioactive salts before being used on actinide bearing salts. In addition, a thermal model will be developed to determine the thermal conductivity of the sample from the measured thermal oscillation of the sensor. Because 3? is a direct method that requires a small volume of sample and works in a very fast time window, it will aid in suppressing the interference due to convection which is ideal when working with high temperature liquid samples.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Status Update for the Canister Deposition Field Demonstration

This report updates the high-level test plan for evaluating surface deposition on three commercial 32PTH2 spent nuclear fuel (SNF) canisters inside NUTECH Horizontal Modular Storage (NUHOMS) Advanced Horizontal Storage Modules (AHSM) from Orano (formerly Transnuclear Inc.) and provides a description of the surface characterization activities that have been conducted to date. The details contained in this report represent the best designs and approaches explored for testing as of this publication. Given the rapidly developing nature of this test program, some of these plans may change to accommodate new objectives or requirements. The goal of the testing is to collect highly defensible and detailed surface deposition measurements from the surface of dry storage canisters in a marine coastal environment to guide chloride-induced stress corrosion crack (CISCC) research. To facilitate surface sampling, the otherwise highly prototypic dry storage systems will not contain SNF but rather will be electrically heated to mimic the thermal-hydraulic-environment. Instrumentation throughout the canister, storage module, and environment will provide an extensive amount of information for the use of model validation. Manual sampling over a comprehensive portion of the canister surface at regular time intervals will offer a high-fidelity quantification of the conditions experienced in a harsh yet realistic environment.

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A Scintillation Counter System Design To Detect Antiproton Annihilation using the High Performance Antiproton Trap(HiPAT)

The High Performance Antiproton Trap (HiPAT), a system designed to hold up to l0(exp 12) charge particles with a storage half-life of approximately 18 days, is a tool to support basic antimatter research. NASA's interest stems from the energy density represented by the annihilation of matter with antimatter, 10(exp 2)MJ/g. The HiPAT is configured with a Penning-Malmberg style electromagnetic confinement region with field strengths up to 4 Tesla, and 20kV. To date a series of normal matter experiments, using positive and negative ions, have been performed evaluating the designs performance prior to operations with antiprotons. The primary methods of detecting and monitoring stored normal matter ions and antiprotons within the trap includes a destructive extraction technique that makes use of a micro channel plate (MCP) device and a non-destractive radio frequency scheme tuned to key particle frequencies. However, an independent means of detecting stored antiprotons is possible by making use of the actual annihilation products as a unique indicator. The immediate yield of the annihilation event includes photons and pie mesons, emanating spherically from the point of annihilation. To "count" these events, a hardware system of scintillators, discriminators, coincident meters and multi channel scalars (MCS) have been configured to surround much of the HiPAT. Signal coincidence with voting logic is an essential part of this system, necessary to weed out the single cosmic ray events from the multi-particle annihilation shower. This system can be operated in a variety of modes accommodating various conditions. The first is a low-speed sampling interval that monitors the background loss or "evaporation" rate of antiprotons held in the trap during long storage periods; provides an independent method of validating particle lifetimes. The second is a high-speed sample rate accumulating information on a microseconds time-scale; useful when trapped antiparticles are extracted against a target, providing an indication of quantity. This paper details the layout of this system, setup of the hardware components around HiPAT, and applicable checkouts using normal matter radioactive sources.

Martin, James J.↗

An Analysis of Potentially Implementing Standardized Canisters in the U.S. Commercial Waste Management System

This analytical study focuses on loading standardized transportation, aging, and disposal canisters (STADs) at commercial reactor sites and subsequent transportation, e.g., to a consolidated interim storage facility (CISF). Specifically, the amount of spent nuclear fuel (SNF) available to load into STADs with varying deployment dates is explored, and the scenarios are compared with a scenario in which STADs are never loaded at reactor sites. Two key findings are that about half of the U.S. inventory of commercial SNF could be captured in STADs if they were fully deployed by 2035 and that the percentage of SNF available to load into STADs decreases as STAD deployment is delayed.In additional scenarios, the effects of shipping STADs directly from at-reactor spent fuel pools (SFPs) to a CISF are analyzed for a STAD full deployment year of 2035. A key finding from the analysis is that the dry storage of SNF in STADs at reactor sites can be minimized by direct shipment to a CISF from reactor site SFPs. Furthermore, minimizing dry storage at reactor sites means maximizing the receipt rate for STADs at a CISF, and there is likely a more optimal point between the two scenarios for an overall cost-effective operation of waste management systems.

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