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DOE OSTI2024

Characterization of 235 U, 238 U and 239 Pu fission ionization chamber foils by α and γ -ray spectrometry

The masses of thin, electroplated deposits of 235 U, 238 U and 239 Pu on titanium backings have been determined to better than 1.3% precision by employing three complementary measurement techniques: $\alpha$ spectrometry, 2$\pi$ gas counting, and $\gamma$-ray spectrometry. A dedicated $\alpha$ spectrometer was designed and calibrated to allow for repeatable, high-precision measurements of the absolute $\alpha$ activity of a sample. The isotopic composition of the sample was determined by fitting the peaks in the $\alpha$ spectrum, a technique which was demonstrated to be generally consistent with mass spectrometry. Independently, the total activity of the deposits were measured in a 2$\pi$ gas flow proportional counter. A detailed study of the effects of $\alpha$ particle straggling in the actinide deposit and $\alpha$ particle recoil off the sample backing material was performed. The masses of these actinide deposits were also measured via $\gamma$-ray spectrometry. Here, we found that all three systematically independent techniques produced consistent results, and could be combined into a weighted average with further reduced uncertainty. The mass ratios of these actinide deposits were determined to better than 1% precision via $\alpha$ spectrometry, enabling high-precision fission cross section ratio measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Accurate determination of production data of the non-standard positron emitter 86 Y via the 86 Sr(p,n)-reaction

In view of several significant discrepancies in the excitation function of the 86 Sr(p,n) 86g+xm Y reaction which is the method of choice for the production of the non-standard positron emitter 86 Y for theranostic application, we carried out a careful measurement of the cross sections of this reaction from its threshold up to 16.2 MeV at Forschungszentrum Jülich (FZJ) and from 14.3 to 24.5 MeV at LBNL. Thin samples of 96.4% enriched 86 SrCO 3 were prepared by sedimentation and, after irradiation with protons in a stacked-form, the induced radioactivity was measured by high-resolution γ -ray spectrometry. The projectile flux was determined by using the monitor reactions nat Cu(p,xn) 62,63,65 Zn and nat Ti(p,x) 48 V, and the calculated proton energy for each sample was verified by considering the ratios of two reaction products of different thresholds. Additionally, the experimental cross section data obtained agreed well with the results of a nuclear model calculation based on the code TALYS. From the cross section data, the integral yield of 86 Y was calculated. Over the optimum production energy range E p = 14 → 7 MeV the yield of 86 Y amounts to 291 MBq/μA for 1 h irradiation time. This value is appreciably lower than the previous literature values calculated from measured and evaluated excitation functions. It is, however, more compatible with the experimental yields of 86 Y obtained in clinical scale production runs. The levels of the isotopic impurities 87m Y, 87g Y, and 88 Y were also estimated and found to be <2% in sum.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2020

COMBLE-ISLAS water isotopes in precipitation (COMBLEISLASISO)

During the measurement period, precipitation was sampled on daily to sub-daily basis with a sampling kit consiting of a clear plastic box (60x40x40 cm) mounted to a ground structure. Daily sampling lasted from 22 Feb to 24 Mar 2020. At a fixed time of day (10 UTC), samples were collected and the sampling box cleaned for the next sample. Additionally, during intense observations periods (IOPs) announced by ISLAS, ARMS scientists increased sampling frequency to sub-daily sampling. During the campaign period, 2 IOPs were conducted, with in total 12 samples taken. IOP1 lasted from 27 Feb 10 to 02 Mar 2020, and IOP2 lasted from 12 Mar to 14 Mar 2020. Solid precipitation in the box was then melted, transferred to an 8 ml glass vial, sealed and shipped to FARLAB (University of Bergen, Norway) for stable water isotope analysis. Measured stable isotope composition of precipitation samples will be related to conditions at other sampling locations, and at the evaporation site to inform about conservation of water isotope quantities. In the period from 22 Feb to 24 Mar, 23 daily samples were collected at 10 UTC for stable water isotope analysis. During the entire sampling period, a high variability of precipitation phase was encountered. Most samples were recovered in the form of graupel/snow (12 samples), as rain (7 samples), and the remaining samples fell as graupel, snow, rain or frozen rain. Precipitation amounts varied between <1 mm (26 Feb) and 140 mm (25 Feb) within the sampling box. Furthermore, higher-resolution sampling was conducted during 2 intense observation periods (IOPs). During IOP1, lasting from 27 Feb 10 UTC to 02 Mar 10 UTC, 7 samples were collected, all of them as solid phase precipitation. IOP2 lasted from 12 Mar 10 UTC to 14 Mar 09 UTC, and 5 samples (all as graupel/snow) were collected. Samples were processed according to FARLAB standard measurement procedures. In short, samples were transferred to 1.5 ml glass vials with rubber/PTFE septa (part #548-0907, VWR, USA). An autosampler (A0325, Picarro Inc) transferred ca. 2µl per injection into a high-precision vapourizer (A0211, Picarro Inc, USA) heated to 110°C. After blending with dry N2 (< 5 ppm H2O) the gas mixture was directed into the measurement cavity of a Cavity-Ring Down Spectrometer (L2140-i, Picarro Inc) for about 7 min with a typical water concentration of 20 000 ppm. Memory effects were reduced by two times measuring a vapour mixture at a mixing ratio of 50 000 ppm, obtained from 2 injections of 2 µl for 5 min at the beginning of each new sample vial. Thereafter, another 6 injections of 2 µl per sample were measured individually as described above, and averages of the last 5 injections were used for further processing. Three standards were measured at the beginning and end of each batch, including a drift standard DI2 (δD: -50.72±0.73 permil, δ18O: -7.63±0.10 permil), and for calibration the laboratory standards GLW (δD: -307.79±0.75 permil, δ18O: -40.02±0.07 permil) and EVAP2 (δD: 9.52±0.65 permil, δ18O: 1.81±0.13 permil). A detailed calibration report is included with the final uploaded data set.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Complex exposure-burial history and Pleistocene sediment recycling in the dead sea rift with implications for the age of the Acheulean site of ‘Ubeidiya

Here, we present early Pleistocene burial ages of the ‘Ubeidiya Formation sediments in the Jordan Valley, a segment of the Dead Sea Rift Valley. A minimum age of ∼1.1 Ma is constrained both by paleomagnetic analysis and U-Pb dating of Melanopsis shells. Simple cosmogenic burial ages (i.e., one very long exposure period followed by one period of burial) calculated from the ratios of 26 Al to 10 Be and 10 Be concentrations indicate ages of ∼3 Ma, contradicting the geological and paleomagnetic constraints as well as a reasonable age of the ‘Ubeidiya archeological site, as it contains human remains. A more sophisticated way of treating the results, by combining numerical modeling of cosmogenic nuclide build up during repeated burial-exposure cycles, paleomagnetic analysis (indicating reverse polarity) and a minimum burial age of 1.1 Ma set by U-Pb dating of Melanopsis shells, suggests two most probable time slots (1.19-1.77 and 1.93- 2.14 Ma) for the absolute age of the ‘Ubeidiya Formation. However, the skewed distribution of cosmogenic isotope burial ages, with a median age of 2.05 Ma, indicates a much higher probability of the older ages, most likely >1.9 Ma. The exposure-burial history that emerges from the model implies recycling of sediments previously deposited and buried in the rift valley, between 4.5 and 3.2 Ma, and subsequently exhumed, eroded, transported and then redeposited along the ‘Ubeidiya paleo lake shoreline.

Acheulean↗

DOE OSTI2025

𝛾-ray spectroscopy of 140 La decay for nuclear forensics applications

140 La is an important isotope in nuclear forensics. It is typically paired with 140 Ba as a chronometer for dating nuclear events. Here, in this work, we report the results of two measurements performed to fully characterize the decay scheme of 140 La. The experiments were performed using the Gammasphere array at Argonne National Laboratory and the CLARION2 array at Florida State University. Sources of 140 La were produced through neutron irradiation of natural lanthanum (99.9% 139 La) in the University of Massachusetts Lowell research reactor. We identify a total of 40 transitions, three of which were not previously reported. An angular correlation analysis was conducted confirming current literature 𝐽 assignments and mixing ratios. By considering all data available in the literature, we provide new recommended values for the intensities of the strongest transitions commonly used in applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Electric and magnetic dipole strength in 112,114,116,118,120,124 Sn

Background: There is renewed interest in electric dipole strength distributions for a variety of reasons including the extraction of the dipole polarizability related to properties of the symmetry energy and a measure for the neutron skin thickness, understanding the structure of low-energy $\textit{E}$1 strength in nuclei with neutron excess, and establishing the systematics of the isovector giant dipole resonance (IVGDR). Inelastic proton scattering at energies of a few hundred MeV and very forward angles including 0° has been established as a tool for the study of electric and magnetic dipole strength distributions in nuclei. Purpose: The present work aims at a systematic investigation of the electric and magnetic dipole strength distributions in the chain of stable even-mass tin isotopes. Methods: Inelastic proton scattering experiments were performed at the Research Center for Nuclear Physics, Osaka, with a 295-MeV beam covering laboratory angles 0°–6° and excitation energies 6–22 MeV. Cross sections due to $\textit{E}$1 and $\textit{M}$1 excitations were extracted with a multipole decomposition analysis (MDA) and then converted to reduced transition probabilities with the “virtual photon method” for $\textit{E}$1 and the “unit cross section method” for $\textit{M}$1 excitations, respectively. Including a theory-aided correction for the high-excitation-energy region not covered experimentally, the electric dipole polarizability was determined from the $\textit{E}$1 strength distributions. Results: In this work, total photoabsorption cross sections derived from the $\textit{E}$1 and $\textit{M}$1 strength distributions show significant differences compared to those from previous ($\textit{γ, xn}$) experiments in the energy region of the IVGDR. The widths of the IVGDR deduced from the present data with a Lorentz parametrization show an approximately constant value of about 4.5 MeV in contrast to the large variations between isotopes observed in previous work. The IVGDR centroid energies are in good correspondence to expectations from empirical systematics of their mass dependence. Furthermore, a study of the dependence of the IVGDR energies on bulk matter properties is presented. The $\textit{E}$1 strengths below neutron threshold show fair agreement in this work with results from ($\textit{γ, γ'}$) experiments on 112,116,120,124 Sn in the energy region between 6 and 7 MeV, where also isoscalar $\textit{E}$1 strength was found for 124 Sn. At higher excitation energies, large differences are observed, pointing to a different nature of the excited states with small ground-state branching ratios. The isovector spin-$\textit{M}$1 strengths exhibit a broad distribution between 6 and 12 MeV in all studied nuclei. Conclusions: The present results contribute to the solution of a variety of nuclear structure problems including the systematics of the energy and width of the IVGDR, the structure of low-energy $\textit{E}$1 strength in nuclei, new constraints to energy density functionals (EDFs) aiming at a systematic description of the dipole polarizability across the nuclear chart, from which properties of the symmetry energy can be derived, and the systematics of the isovector spin-$\textit{M}$1 strength in heavy nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Measurement of the energy-differential 35 Cl( n, p 0 ) 35 S cross section via the ratio with 6 Li( n, α ) 3 H

Knowledge of the neutron-induced 35 Cl ⁢(n, x) cross sections is vital to the design and certification of molten chloride fast reactors (MCFRs) since the 35 Cl (n, p 0 ) 35 S reaction is believed to be a significant reactor poison. However, recently published measurements are inconsistent with each other and with evaluation. Here, the goal of this work is to measure the 35 Cl (n, p 0 ) reaction cross section using a technique that is different from recent measurements. The experiment was conducted at Lawrence Berkeley National Laboratory's (LBNL) 88-Inch Cyclotron using thick target deuteron breakup from a 14 MeV deuteron beam. Energy-differential 35 Cl (n, p 0 ) 35 S cross sections were obtained via ratio with the 6 Li (n, a)⁢ 3 H reaction using an active target experiment with a Cs 2 ⁢LiYCl 6 (CLYC) scintillator. The 35 Cl (n, p 0 ) reaction cross section was measured from 2.02 to 7.46 MeV. The results are consistent with Kuvin et al., confirming a roughly 50% reduction in magnitude relative to the ENDF/B-VIII.0 evaluation. These data provide new insight into the role of natural Cl as an MCFR poison. The reduction of the 35 Cl (n, p 0 ) reaction cross section compared to evaluation suggests that MCFR criticality is less sensitive to Cl enrichment. This may in turn reduce building and operating costs since isotope separation may not be needed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Brachiopod δ 34 S CAS microanalyses indicate a dynamic, climate-influenced Permo-Carboniferous sulfur cycle

Early isotopic studies of sulfate in carbonate minerals (carbonate associated sulfate; CAS) suggested that carbonates can provide a reliable, well-dated archive of the marine sulfur cycle through time. However, subsequent research has shown that diagenetic alteration can impose highly heterogeneous CAS sulfur isotopic compositions (δ 34 S CAS ) among different carbonate phases within sediments. Such alteration necessitates targeted sampling of well-preserved, primary carbonate phases. Here, we present a new record of Carboniferous and Early Permian brachiopod δ 34 S CAS generated from over 130 measurements of microsampled brachiopod shells. Our record refines existing brachiopod δ 34 S CAS records and confirms a large, ~6.5‰ δ 34 S CAS decrease in the Early Carboniferous. Importantly, the record also features a novel 3–5‰ increase in δ 34 S CAS near the Serpukhovian-Bashkirian boundary (323.4 Ma) that coincides with carbonate δ 13 C and δ 18 O increases. Variability in δ 34 S CAS is minor both within (≤0.3‰) and among (≤2‰) individual co-depositional brachiopod specimens. A taxon-specific δ 34 S CAS offset is present one species (Composita subtilita) that also exhibits a δ 13 C offset, supporting the existence of biological “vital effects” on δ 34 S CAS . Geologic evidence and mathematical modeling of the Permo-Carboniferous carbon and sulfur cycles suggest that changes in the burial ratio of organic carbon to pyrite sulfur (R C:S ) are insufficient to explain the observed mid-Carboniferous δ 34 S CAS record. We find that changes in the 34 S depletion of pyrite relative to seawater sulfate ( 34 ε) or in the δ 34 S of the input to the ocean (δ 34 S in ) are also needed. Large additions of O 2 from organic carbon burial during the Permo-Carboniferous cannot be entirely compensated for with sulfur cycle changes; lower than modern late Visean pO 2 and/or additional O 2 sinks are needed to keep pO 2 at plausible levels. Based on the geologic context surrounding our record's mid-Carboniferous δ 34 S CAS increase, we advocate for simultaneous changes in pyrite burial, 34 ε, and δ 34 S in , driven by sea level or tectonically induced changes in environments of sulfur burial, as a viable mechanism to produce rapid seawater δ 34 S changes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Selenium interaction with iron minerals: Quantitative comparison of sorption and coprecipitation impacts on mobility

Given the significance of selenium (Se) as a micronutrient, the radioactive nature of some of its isotopes, and its affinity to iron (Fe) minerals, extensive research has been conducted on the sorption mechanisms between Se and these minerals. Here, in this study, we employ sorption data sourced from the L-SCIE database and coprecipitation data from available literature to achieve the following objectives: i) establish coherence between adsorption and coprecipitation processes, ii) quantitatively evaluate the importance of these processes in nuclear waste repository science, and iii) propose a forward-looking approach for integrating coprecipitation into reactive transport models. Our findings indicate that a correlation between Se adsorption and coprecipitation can be established using the λ formalism. The comparable log(λ Se(IV) /λ Se(VI) ) ratios derived from adsorption and coprecipitation experiments suggest that these processes can be quantitatively compared and evaluated using our numerical approach. Across all iron oxide phases examined, coprecipitation leads to significantly greater immobilization of Se compared to adsorption. Specifically, for hydrous ferric oxide, hematite, and goethite, coprecipitation is predicted to result in 100–1000 times more Se immobilization compared to adsorption, irrespective of the Se oxidation state (Se(IV) or Se(VI)); notably stronger immobilization potential via coprecipitation was observed for magnetite. The modeling approach and quantitative analysis presented herein clearly highlight the importance of including coprecipitation processes when simulating Se (and other elements) transport, particularly under conditions where mineral compositions are transient or evolving with time. Neglecting coprecipitation in models is likely to lead to significant overestimates of migration.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2026

Mesh-based multiphysics coupling acceleration for fusion neutronics through clustering for fusion blanket applications

Accurate modeling of particle transport within fusion blankets is essential for predicting performance metrics such as heat deposition and the tritium breeding ratio (TBR). However, high-fidelity coupling of thermal fluids from computational fluid dynamics (CFD) to neutronics simulations often incurs significant computational costs due to the complexity of surface intersection calculations in Monte Carlo codes. This paper presents an accelerated multiphysics coupling method for neutronics that utilizes hierarchical agglomerative clustering to map complex material property distributions to a neutronics model. Implemented within the fusion reactor design and assessment (FREDA) framework, the method leverages existing Python packages to automate the creation of clustered geometries for OpenMC. The approach is demonstrated on a sector model of an ARC-class tokamak with an immersion molten salt blanket, and an simple geometry with varying isotopic concentrations. Results show that the clustering method significantly reduces computational burden without compromising fidelity, providing a foundation for agile iteration of neutronics simulations involving multiple coupled material properties.

Bae, Jin Whan [ORNL] (ORCID:0000000326548907)↗

DOE OSTI2020

Development of Gamma Background Radiation Digital Twin with Machine Learning Algorithms: Application of Unsupervised Machine Learning to Detection of Anomalies and Nuisances in Gamma Background Radiation Environmental Screening Data

Environmental screening of gamma radiation consists of detecting weak nuisance and anomaly signal in the presence of strong and highly varying background. In a typical scenario, a mobile detector-spectrometer continuously measures gamma radiation spectra in short, e.g., one-second, signal acquisition intervals. The measurement data is a 2D matrix, where one dimension is gamma ray energy, and the other dimension is the number of measurements or total time. In principle, gamma radiation sources can be detected and identified from the measured data by their unique spectral lines. Detecting sources from data measured in a search scenario is difficult due to the highly varying background because of naturally occurring radioactive material (NORM), and low signal-to-noise ratio (S/N) of spectral signal measured during one-second acquisition intervals. The objective of this work is to explore unsupervised machine learning (ML) algorithms for development of a digital twin of gamma radiation background, and for detection and identification of weak nuisances and anomalies events in the presence of highly fluctuating background. In one segment of work, we developed a gamma background estimation model using a Longshort term memory (LSTM) network for one-step CPS time series prediction. The LSTM model was validated with two data sets of measurements from two independent NaI detectors positioned on a mobile platform. The data sets contained background radiation only and no orphan isotope sources. The LSTM model was constructed and tested using data from one of the detectors. Performance of the LSTM model was validate through one-step prediction of CPS time series of another NaI detector without re-training. This approach allows to create a digital twin for nuclear background estimation. Using LSTM, it could be possible to detect a source through subtraction of the estimated counts from the measured background. In another segment of work, we investigated detection of gamma emitting sources in the presence of complex background using unsupervised machine learning. Spectral lines of isotopes are difficult to observe in one-second measurements. Averaging over the entire measurement campaign data set reveals spectral lines of most common background isotopes. Spectral lines of orphan sources, which might appear only in a few measurements during the campaign, will be washed out if averaging is performed over the entire measurement data set. The approach we have explored consists of extracting one-second measurements containing weak spectral features through data clustering. Averaging one-second spectra in a cluster should reveal the presence of anomaly sources. We created two ML models using K-means clustering and Neural Network Self-organizing Map (SOM). Performance of these ML models was benchmarked using search data. One data set contained 137 Cs source, and another dataset contained 131 I source.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Maximum Cs-137 Curie Loading onto Crystalline Silicotitanate for the Documented Safety Analysis of the Tank Side Cesium Removal Platform

The Tank Side Cesium Removal (TSCR) system is currently being constructed to process Hanford tank waste supernates for vitrification. TSCR incorporates a filtration system and cesium (Cs) removal system using columns filled with crystalline silicotitanate (CST) ion exchanger, produced by Honeywell UOP, LLC. The documented safety analysis (DSA) developed for TSCR limits a single column curie loading to 141,600 Ci; given a 137 Cs isotopic mass fraction of 20% and the planned CST bed size of a TSCR column, this equates to 0.10 mmole Cs per g CST. Factors that influence 137Cs loading onto the CST include, but are not limited to, CST production lot (different production lots behave differently), contact temperature, contact duration, 137Cs mass fraction, and competitors in the tank waste feed. Seventeen tank waste feeds (compositions) were identified by Washington River Protection Solutions to be processed through TSCR. These feed compositions were used to develop a simulant (referred to herein as Stage 1) that would provide an upper bound to the Cs loading onto CST based on maximizing the Cs/Na activity coefficient ratios in solution while maintaining Na at no less than 5.0 M. Building upon this Stage 1 simulant, a series of four additional simulants were developed based on the cationic/anionic species that impact Cs exchange, with each successive formulation relaxing one or more matrix component concentration constraints as show in Table S.1

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Recent Developments in Revealing the Impact of Complex Metal Oxide Reconstruction on Catalysis

Surface reconstruction of complex metal oxides refers to the alterations of the topmost catalyst surface, relative to the bulk structure, following exposure to pretreatment or reaction conditions during heterogeneous catalysis. (1) This structural and electronic transformation may involve (1) changes of the exposed crystallographic facets, (2) changes in chemical composition, such as the enrichment of specific elements, and, (3) morphological variations, including surface roughness and defects (Scheme 1). Beyond relaxation, surface reconstruction here also encompasses disruptions to the periodicity of the sublayers and changes to its stoichiometry. This change significantly influences the chemical properties of the catalyst surface, such as redox sites, (2) acid/base pairs, hydroxyl groups, (3) and surface defects. Surface reconstruction occurs due to the thermodynamic drive to lower the surface energy of the catalyst under the surrounding environment (e.g., temperature, chemical potential of species present). In addition to the treatment or reaction conditions, the extent of reconstruction also depends on the elements in the metal oxide structure. For instance, annealing ABO 3 perovskites (SrTiO 3 , BaTiO 3 , and BaZrO 3 ) at high temperatures (500 °C) in O 2 has a very different impact on the A/B ratio at the surface (ranging from 0.9 to 2.5), depending on the identity of A and B. (4) Metal oxide surface reconstruction under an electric field and exposure to acidic and alkaline media has recently gained increased attention in electrocatalysis, such as in the oxygen evolution reaction (OER); (5,6) however, in this Viewpoint we focus on the impact of surface reconstruction on thermal catalysis, a critical enduring research theme with ongoing challenges. Here, we start showcasing approaches to characterize surface reconstruction at the topmost surface layer, such as low-energy ion scattering (LEIS), discussing advantages and limitations. Next, we connect characterization of surface reconstruction to site-specific kinetic analysis, enabled via steady-state isotopic transient kinetic analysis (SSITKA), and we express our viewpoint on building structure–performance relationships by deeply understanding reconstructed surfaces. Later, we comment on the potential of tuning surface reconstruction to enhance catalytic performance. Finally, we explore the interplay between surface reconstruction and the “intelligent behavior”.

alcohol conversion↗

DOE OSTI2021

A multimillion-year-old record of Greenland vegetation and glacial history preserved in sediment beneath 1.4 km of ice at Camp Century

Understanding the history of the Greenland Ice Sheet (GrIS) is critical for determining its sensitivity to warming and contribution to sea level; however, that history is poorly known before the last interglacial. Most knowledge comes from interpretation of marine sediment, an indirect record of past ice-sheet extent and behavior. Subglacial sediment and rock, retrieved at the base of ice cores, provide terrestrial evidence for GrIS behavior during the Pleistocene. Here, we use multiple methods to determine GrIS history from subglacial sediment at the base of the Camp Century ice core collected in 1966. This material contains a stratigraphic record of glaciation and vegetation in northwestern Greenland spanning the Pleistocene. Enriched stable isotopes of pore-ice suggest precipitation at lower elevations implying ice-sheet absence. Plant macrofossils and biomarkers in the sediment indicate that paleo-ecosystems from previous interglacial periods are preserved beneath the GrIS. Cosmogenic 26 Al/ 10 Be and luminescence data bracket the burial of the lower-most sediment between <3.2 ± 0.4 Ma and >0.7 to 1.4 Ma. In the upper-most sediment, cosmogenic 26 Al/ 10 Be data require exposure within the last 1.0 ± 0.1 My. The unique subglacial sedimentary record from Camp Century documents at least two episodes of ice-free, vegetated conditions, each followed by glaciation. The lower sediment derives from an Early Pleistocene GrIS advance. 26 Al/ 10 Be ratios in the upper-most sediment match those in subglacial bedrock from central Greenland, suggesting similar ice-cover histories across the GrIS. We conclude that the GrIS persisted through much of the Pleistocene but melted and reformed at least once since 1.1 Ma.

58 GEOSCIENCES↗

DOE OSTI2022

Laser-Induced Spectrochemical Assay for Uranium Enrichment (LISA-UE)

Uranium hexafluoride (UF6) is the uranium compound typically involved in uranium enrichment process. As the first line of defense against nuclear proliferation, accurate determinations of the uranium enrichment ratio in UF6 are critical for materials verification, accounting and safeguards. Shipping gaseous UF6 samples off-site for analysis with mass spectrometry is cumbersome and costly, and results are not available for some time (months). In-field UF6 enrichment assay has the potential to substantially reduce the time, logistics and expense of sample handling. At present, COMPUCEA is the only accepted method for UF6 enrichment assay in the field. Laser-Induced Spectrochemical Assay for Uranium Enrichment (LISA-UE) is an all-optical (based on laser induced plasma emission) analytical technique intended for fieldable, accurate, precise and rapid UF6 enrichment assay. In its operation, laser induced plasma is created directly in the gaseous UF6 sample. Because different U isotopes emit at slightly different wavelengths, the isotopic information of the UF6 sample is inherently encoded in the atomic emission from the plasma. Isotopic emissions from 235U and 238U are measured simultaneously, which eliminate correlated noise from the laser induced plasma. Isotopic information of the UF6 sample can be extracted from the acquired spectrum with theoretical multi-variable non-linear spectral fitting. To date, advances made by the LISA-UE research team include optimization of the spectral window for direct gaseous UF6 enrichment assay with laser induced plasma, development of data reduction algorithms, and demonstrations of the LISA-UE technique with gaseous UF6 samples. In this presentation, the technical aspect of LISA-UE will be overviewed, the data reduction algorithm will be described, and performance of the technique will be discussed.

Chan, George↗

DOE OSTI2023

Modeling and Simulation of Xe-100-type Pebble Bed Gas-Cooled Reactor with SCALE

The US Department of Energy (DOE) announced the Advanced Reactor Demonstration Program (ARDP) to accelerate the deployment of advanced reactor concepts. Awardees of ARDP funds are expected to demonstrate the operation of an advanced reactor within 7 years of receiving the award. X-Energy’s advanced reactor concept, the Xe-100, was selected as one of two advanced reactor concepts to receive funding to demonstrate the operation of its high-temperature gas-cooled pebble-bed reactor before the end of this decade. As a result of this push to bring advanced reactors to maturation and commercialization, transition and deployment scenario studies are being performed under the Systems Analysis and Integration (SA&I) campaign within the DOE Office of Nuclear Energy (DOE-NE) to evaluate the transition of the current US commercial fleet of light-water reactors (LWRs) to a future fleet of advanced reactors consisting of a mix of ARDP type reactor concepts and advanced LWRs. To accurately evaluate the front- and back-end resource requirements, it is important to perform reactor physics calculations to determine the discharge burnup and isotopic content, fuel residence time, as well as other parameters. For this purpose, a summer project funded by the SA&I campaign allowed for the setup of SCALE models for full-core Xe-100 type high-temperature gas-cooled pebble-bed reactor and a Xe-100 type slice using publicly available information. The core-averaged equilibrium compositions and zone-wise equilibrium compositions for the slice and 3D models, respectively, were obtained following an iterative depletion method developed by Bostelmann et al. using SCALE’s reactor physics sequence TRITON. The slice model was used with TRITON to generate burnup-dependent cross section libraries at different temperatures which can be used with SCALE’s ORIGAMI code to rapidly determine fuel inventory and therefore to perform quick sensitivity studies on parameters such as the pebble location in the core. The SCALE/TRITON transport and depletion calculation for the Xe-100 type slice model indicates that the isotopic concentrations are in good agreement at 1,300 effective full power days (EFPD) for 235 U. An analysis of 236 U results match 239 Pu results would seem to indicate a typographical error in Mulder and Boyes wherein the reported results of 236 U and 239 Pu are reversed. In addition to SCALE/TRITON calculations, a new capability within SCALE/ORIGAMI for the simulation of pebble-bed reactors was used to study the burnup sensitivity with respect to the pebble pathway through the core. The SCALE/ORIGAMI results show that pebbles that travel closer to the reflector for the entire depletion history have a higher burnup than pebbles that travel through the middle of the core because of the higher thermal to fast flux ratio near the reflector. Consequently, a pebble’s burnup is strongly affected by the pebble’s pathway for each pass. Additional phenomena such as temperature distributions in the core and different travel times of the pebbles in the individual radial zones further affect the burnup distribution. The sensitivity of the discharge vector to the pebble pathways taken during each pass can be evaluated in the future using SCALE/ORIGAMI now that the SCALE inputs have been established.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2020

Model uncertainty in accelerator application simulations

Monte-Carlo nuclear reaction and transport codes are widely used to devise accelerator-based nuclear physics experiments; at the same time, many experiments are performed to validate the Monte-Carlo codes, which can be used for the design of full-scale nuclear power applications or the design of new benchmark experiments. Dedicated model benchmark studies investigate a broad range of nuclear reactions and quantities. Examples of these include isotope formation or secondary particle fluxes that result from the interactions of GeV-range hadrons with monoisotopic targets, which can be used to assess the respective systematic uncertainty of models. Such benchmark studies, as well as many nuclear application experiments and simulations carried out by various groups over the last few decades, enable us to draw methodological lessons. In this work, model uncertainty determined based on available experimental data allow us to identify the effects of practitioner expertise as well as the design of codes (user access to micro-scale parameters) on the range of uncertainties. We found that in cases when simulations are performed by code developers or users that are very experienced in performing simulations, the model to experiment quantity ratios generally agree with the limits determined by dedicated benchmark studies. In other cases, the ratios generally tend to be either smaller (underestimation of model error) or larger (overestimation of model error). A plausible explanation of the aforementioned effects is suggested.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Evidence for ground-state electron capture of K 40

Potassium-40 is a widespread, naturally occurring isotope whose radioactivity impacts estimated geological ages spanning billions of years, nuclear structure theory, and subatomic rare-event searches—including those for dark matter and neutrinoless double-beta decay. The decays of this long-lived isotope must be precisely known for its use as a geochronometer, and to account for its presence in low-background experiments. There are several known decay modes for potassium-40, but a predicted electron-capture decay directly to the ground state of argon-40 has never been observed. The existence of this decay mode impacts several fields, while theoretical predictions span an order of magnitude. Here we report on the first, successful observation of this rare decay mode, obtained by the KDK (potassium decay) Collaboration using a novel combination of a low-threshold x-ray detector surrounded by a tonne-scale, high-efficiency γ -ray tagger at Oak Ridge National Laboratory. A blinded analysis reveals a distinctly nonzero ratio of intensities of ground-state electron-captures ( I EC 0 ) over excited-state ones ( I EC * ) of I EC 0 / I EC * = 0.0095 ± stat 0.0022 ± sys 0.0010 (68% CL), with the null hypothesis rejected at 4 σ [Stukel et al. , Phys. Rev. Lett. 131 , 052503 (2023) ]. In terms of branching ratio, this unambiguous signal yields I EC 0 = 0.098 % ± stat 0.023 % ± sys 0.010 % , roughly half of the commonly used prediction. This first observation of a third-forbidden unique electron capture improves our understanding of low-energy backgrounds in dark-matter searches and has implications for nuclear-structure calculations. For example, a shell-model based theoretical estimate for the neutrinoless double-beta decay half-life of calcium-48 is increased by a factor of 7 - 2 + 3 . Our nonzero measurement shifts geochronological ages by up to a percent; implications are illustrated for Earth and solar system chronologies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗