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At least 145 records · Page 8

Plutonium isotope ratio measurements by total evaporation-thermal ionization mass spectrometry (TE-TIMS): an evaluation of uncertainties using traceable standards from the New Brunswick Laboratory

The accuracy and precision of isotope amount ratio measurements using thermal ionization mass spectrometry (TIMS) instrumentation are described, and the measurement of Pu materials is emphasized. The mass fractionation observed for Am, Ga, Pu, and U for isotope amount ratio measurements using the total evaporation (TE) technique is compared with theoretical estimates to demonstrate the advantage of the TE methodology and to investigate systematic biases in the major isotope amount ratios of U and Pu certified reference material (CRM) standards from the U.S. provider of CRMs. The quality of the Pu isotopic data generated by TIMS instruments in an analytical laboratory is demonstrated by the application of the double ratio technique to estimate the 241 Pu half-life. Analytical data on traceable Pu CRMs from the New Brunswick Laboratory (NBL), generated as part of routine measurements supporting various programs, are used for this half-life estimation. Although the 241 Pu abundances in CRMs of 136, 137, 138, and 126-A are approximately 200–2000× smaller than those in the 241 Pu material used in the previous Institute for Reference Materials and Measurements (IRMM) evaluation of the 241 Pu half-life, the half-life value estimated in this work shows excellent agreement with the currently accepted value from the IRMM. This agreement also demonstrates the pedigree of the Pu isotopic standards from the NBL and the quality of the isotope amount ratio measurements using TIMS instrumentation. For both the major and minor Pu isotope amount ratios, this report describes the relative importance of the factors affecting the uncertainty of TIMS measurements, which are considered the gold standard in isotope ratio measurements (LA-UR-24-29199).

07 ISOTOPE AND RADIATION SOURCES↗

RF deflecting cavity for fast radioactive ion beams

Abstract The Facility for Rare Isotope Beams (FRIB) will be a new scientific user facility that produces rare-isotope beams for experiments from the fragmentation of heavy ions at energies of 100–200 MeV/u. During the projectile fragmentation, the rare isotope of interest is produced along with many contaminants that need to be removed before the beam reaches detectors. At FRIB, this is accomplished with a magnetic projectile fragment separator. However, to achieve higher beam purity, in particular for proton-rich rare isotopes, additional purification is necessary. RadiaBeam in collaboration with Michigan State University (MSU) has designed a 20.125 MHz radiofrequency (RF) fragment separator capable of producing a 4 MV kick with 18 cm aperture in order to remove contaminant isotopes based on their time of flight. In this paper, we will discuss the RF and engineering design considerations of this separator cavity.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

New proton emitter 188 At implies an interaction unprecedented in heavy nuclei

We report the discovery of a new atomic nucleus 188 At, which is the heaviest proton-emitting isotope known to date. The new activity was observed through the 107 Ag( 84 Sr, 3n) 188 At fusion-evaporation reaction using the focal-plane spectrometer of the gas-filled recoil separator in the Accelerator Laboratory of the University of Jyväskylä, Finland. To fully interpret the experimental data, we have expanded the non-adiabatic quasiparticle model to treat nuclei in the beyond-lead region. The description reproduced the measured decay rate and pointed towards emission from an extremely prolate-deformed state with a dominant s 1/2 proton component in the wave function. The Thomas-Ehrman shift can be enhanced in low angular momentum states, but such effects have not been observed in heavy nuclei. The single-proton separation energy of 188 At deviates from that extrapolated from the systematics, which can be interpreted as the first evidence of this effect in heavy nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Scaling the Microbial Ecology of Soil Carbon (Final Report)

This work developed new techniques and discoveries in quantitative microbial ecology, focusing on soil carbon. The work advanced a new approach to stable isotope probing (SIP), adding a quantitative way to infer taxon-specific rates of growth, mortality, and associated carbon (C) fluxes in soil microbial communities, a framework that the work demonstrated can scale from individual microbial taxa to the integrated soil system. Among the “-omics” techniques in microbial ecology, those based on stable isotope probing (SIP) hold particular promise for addressing the challenge of scaling from molecules to the major biogeochemical element cycles. Because SIP measures directly the fluxes of elements into nucleic acids, it physically connects element flux to genetic information. The work explored new ways to quantify taxon-specific C-use and growth efficiency and tested hypotheses about responses of the soil microbial community to experimental warming and to latitudinal variation in temperature. This work pushed the frontier of –omics enabled techniques by demonstrating their applicability at the ecosystem scale, and by relating taxon-specific isotope assimilation to dissimilatory processes in the C cycle, thereby enabling the identification of organisms especially responsible for soil C loss, in other words, attributing ecosystem-scale element fluxes to individual microbial taxa.

54 ENVIRONMENTAL SCIENCES↗

In Situ Oxygen Isotope Determination in Serpentine Minerals by SIMS: Addressing Matrix Effects and Providing New Insights on Serpentinisation at Hole BA1B (Samail ophiolite, Oman)

The ability to constrain the petrogenesis of multiple serpentine generations recorded at the microscale is crucial for estimating the extent and conditions of modern versus fossil serpentinisation in ophiolites. To address matrix bias effects during oxygen isotope analysis by SIMS, we present the first investigation analysing antigorite in the compositional range Mg# = 77.5–99.5 mole %, using a CAMECA IMS–1280 secondary ion mass spectrometer. Spot–to–spot homogeneity is ≤ 0.5‰ (2s) for the new antigorite reference materials. The relative bias between antigorite reference materials with different Mg/Fe ratios is described by a second order polynomial, and a maximum difference in bias of ~ 1.8‰ was measured for Mg# ~ 78 to 100. We observed a bias up to ~ 1.0‰ between lizardite and antigorite attributed to their different crystal structure. Orientation effects up to ~ 1‰ were observed in chrysotile. The new analytical protocol allowed the identification of oxygen isotope zoning up to ~ 7‰ in serpentine minerals from two serpentinites recovered from an area of active serpentinisation in the Samail ophiolite. Furthermore in situ analysis is capable of resolving isotopic heterogeneity that may directly reflect changes in the physical and chemical conditions of multiple serpentinisation events in the Samail ophiolite.

47 OTHER INSTRUMENTATION↗

The new Batch Mode Ion Source for stand-alone operation at the Facility for Rare Isotope Beams (FRIB)

Gas stoppers have been used for a long-standing successful science program at Michigan State University with stopped and rare-isotope beams produced by projectile fragmentation. The National Superconducting Cyclotron Laboratory’s Coupled Cyclotron Facility has recently transitioned into the Facility for Rare Isotope Beams (FRIB) laboratory to provide rare isotopes using a high-power superconducting linear accelerator and new production facilities. To allow the science program with stopped and reaccelerated beams to continue during the transition period, a stand-alone capability was added. The Batch Mode Ion Source (BMIS) was built and has been providing beams of long-lived and stable isotopes of a variety of elements for successful user experiments. Finally, the BMIS system is described and results from the production of various beams are presented.

47 OTHER INSTRUMENTATION↗

Elucidating hydrogen isotope transport mechanisms in proton-conducting ceramics with trapping effects using TMAP8

Hydrogen isotopes play an central role in many science and engineering applications such as fuel cells, hydrogen production, and fusion energy. For these applications, hydrogen separation and extraction applications are pivotal aspects of hydrogen transports, where proton-conducting ceramics (PCCs) have shown great potential. In this study, we propose a new model for hydrogen isotope transport in PCC materials, BaZr 0.9 Y 0.1 O 2.95 (BZY) in particular, which captures behavior in both dry and wet environments. The model expands previous efforts and considers diffusion, trapping, and surface reactions (i.e., dissociation and recombination). We then validate and calibrate the model using deuterium transport measurements from experiments in both dry and wet environments. This study highlights the key role of trapping, often neglected, on hydrogen isotope transport in BZY and other PCC materials. It also explains how the commonly observed discrepancy between dry and wet behavior can be attributed to more active surface reactions and saturated traps due to the increased hydrogen presence under the wet environment. These results provide insights to optimize PCC manufacturing and usage as a hydrogen separation and extraction technology in various fields, emphasizing that lowering the trapping can reduce hydrogen isotope retention. These modeling and calibration efforts are performed using the tritium migration analysis program, version 8 (TMAP8), an open-source application designed for hydrogen isotope transport.

36 - MATERIALS SCIENCE↗

Capillary absorption spectroscopy for high temporal resolution measurements of stable carbon isotopes in soil and plant-based systems

Capillary Absorption Spectroscopy (CAS) is a relatively new analytical technique for performing stable isotope analysis. Here, we demonstrate the utility of CAS by recording and quantifying variation in 13C in controlled and biologically relevant applications. We calibrated CAS system response to increased 13CO2, with an observed ~4‰ increase in measured Δ13C for each 0.03 ppm shift in 13CO2 concentration. We leveraged this calibration to quantify rates of biogeochemical processes using a 13C tracer. For example, we monitored microbial respiration of 13C-glucose within an agricultural soil at 10 s quantification intervals and results demonstrated 8.6% ± 0.4 of added glucose was converted to 13CO2 within 1.5 h of incubation. We expanded the demonstration by adapting a rhizobox to permit continuous monitoring of 13CO2 in a soil (as distinct from plant) headspace to track the timing and quantify respiration rates of fresh plant photosynthate and observed a 3.5 h delay between plant exposure to a13CO2 tracer and the first signs of respiration by soil biota. These experiments highlight CAS is effective in producing high temporal resolution quantification of 13CO2 and demonstrate potential applications.

13CO2↗

DIII-D research to provide solutions for ITER and fusion energy

The DIII-D tokamak has elucidated crucial physics and developed projectable solutions for ITER and fusion power plants in the key areas of core performance, boundary heat and particle transport, and integrated scenario operation, with closing the core-edge integration knowledge gap being the overarching mission. New experimental validation of high-fidelity, multi-channel, non-linear gyrokinetic turbulent transport models for ITER provides strong confidence it will achieve Q ≥ 10 operation. Experiments identify options for easing H-mode access in hydrogen, and give new insight into the isotopic dependence of transport and confinement. Analysis of 2,1 islands in unoptimized low-torque IBS demonstration discharges suggests their onset time occurs randomly in the constant β phase, most often triggered by non-linear 3-wave coupling, thus identifying an NTM seeding mechanism to avoid. Pure deuterium SPI for disruption mitigation is shown to provide favorable slow cooling, but poor core assimilation, suggesting paths for improved SPI on ITER. At the boundary, measured neutral density and ionization source fluxes are strongly poloidally asymmetric, implying a 2D treatment is needed to model pedestal fuelling. Detailed measurements of pedestal and SOL quantities and impurity charge state radiation in detached divertors has validated edge fluid modelling and new self-consistent 'pedestal-to-divertor' integrated modeling that can be used to optimize reactors. New feedback adaptive ELM control minimizes confinement reduction, and RMP ELM suppression with sustained high core performance was obtained for the first time with the outer strike point in a W-coated, compact and unpumped small-angle slot divertor. Advances have been made in integrated operational scenarios for ITER and power plants. Wide pedestal intrinsically ELM-free QH-modes are produced with more reactor-relevant conditions, Low torque IBS with W-equivalent radiators can exhibit predator-prey oscillations in Te and radiation which need control. High-β P scenarios with q min > 2, q 95 –7.9, β N > 4, β T –3.3% and H 98y2 > 1.5 are sustained with high density ($\overline{n}$ = 7E19 m -3 , f G –1) for 6 τ E , improving confidence in steady-state tokamak reactors. Diverted NT plasmas achieve high core performance with a non-ELMing edge, offering a possible highly attractive core-edge integration solution for reactors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Multiple Mechanisms Mapped in Aryl Alkyl Ether Cleavage via Aqueous Electrocatalytic Hydrogenation over Skeletal Nickel

We present here detailed mechanistic studies of electrocatalytic hydrogenation (ECH) in aqueous solution over skeletal nickel cathodes to probe the various paths of reductive catalytic C–O bond cleavage among functionalized aryl ethers relevant to energy science. Heterogeneous catalytic hydrogenolysis of aryl ethers is important both in hydrodeoxygenation of fossil fuels and in upgrading of lignin from biomass. The presence or absence of simple functionalities such as carbonyl, hydroxyl, methyl, or methoxyl groups is known to cause dramatic shifts in reactivity and cleavage selectivity between sp3 C–O and sp2 C–O bonds. Specifically, reported hydrogenolysis studies with Ni and other catalysts have hinted at different cleavage mechanisms for the C–O ether bonds in α-keto and α-hydroxy β-O-4 type aryl ether linkages of lignin. Our new rate, selectivity, and isotopic labeling results from ECH reactions confirm that these aryl ethers undergo C–O cleavage via distinct paths. For the simple 2-phenoxy-1-phenylethane or its alcohol congener, 2-phenoxy-1-phenylethanol, the benzylic site is activated via Ni C–H insertion, followed by beta elimination of the phenoxide leaving group. But in the case of the ketone, 2-phenoxyacetophenone, the polarized carbonyl π system apparently binds directly with the electron rich Ni cathode surface without breaking the aromaticity of the neighboring phenyl ring, leading to rapid cleavage. Substituent steric and electronic perturbations across a broad range of β-O-4 type ethers create a hierarchy of cleavage rates that supports these mechanistic ideas while offering guidance to allow rational design of the catalytic method. Furthermore, on the basis of the new insights, the usage of cosolvent acetone is shown to enable control of product selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NEONiso R Package, versions greater than 0.5.2

Carbon fluxes in terrestrial ecosystems and their response to environmental change are a major source of uncertainty in the modern carbon cycle. The National Ecological Observatory Network (NEON) presents the opportunity to merge eddy covariance (EC)-derived fluxes with CO2 isotope ratio measurements to gain insights into carbon cycle processes. Collected continuously and consistently across >40 sites, NEON EC and isotope data facilitate novel integrative analyses. However, currently provisioned atmospheric isotope data are uncalibrated, greatly limiting ability to perform cross-site analyses. Here, we present two approaches to calibrating NEON CO2 isotope ratios, along with an R package to calibrate NEON data. We find that calibrating CO2 isotopologues independently yields a lower d13C bias (<0.05‰) and higher precision (<0.40‰) than directly correcting d13C with linear regression (bias: <0.11‰, precision: 0.42‰), but with slightly higher error and lower precision in calibrated CO2 mole fraction. The magnitude of the corrections to d13C and CO2 mole fractions vary substantially by site, underscoring the need for users to apply a consistent calibration framework to data in the NEON archive. Post-calibration data sets show that site mean annual d13C correlates negatively with precipitation, temperature, and aridity, but positively with elevation. Forested and agricultural ecosystems exhibit larger gradients in CO2 and d13C than other sites, particularly during the summer and at night. The overview and analysis tools developed here will facilitate cross-site analysis using NEON data, provide a model for other continental-scale observational networks, and enable new advances leveraging the isotope ratios of specific carbon fluxes.

Fiorella, Richard↗

Gas generation and intramolecular isotope study in laboratory pyrolysis of the Springfield coal from the Illinois Basin

Position-specific (PS) isotopes of propane have been proposed as a potential geochemical tool to decipher various geological processes (e.g., thermal cracking, biodegradation, H exchange) in natural reservoirs. The limited studies have been conducted on the PS isotopes of propane from the pyrolysis gases from marine shales, and natural gases sourced from lacustrine and marine kerogens, but little is known on gases produced from the humic kerogen. Here, this study investigated the PS δ 13 C of propane in the closed-system pyrolysis of the Springfield coal, Illinois Basin, Indiana, at 310 to 470 °C (Easy %Ro: 0.76 to 3.07). The C kinetic isotope effect (KIE) of CH 4 produced in both this study and previous low-temperature pyrolysis of the same coal indicates the cleavage of C—O bonds is the main generation pathway at the early kerogen cracking stage, followed by the breakdown of alkyl groups. At the wet-gas cracking stage, C 3 H 8 production from thermally stable compounds has a significant influence on the bulk and position-specific C KIE in the pyrolysis of marine Woodford kerogen and Springfield coal. According to the PS δ 13 C of propane, the central site is likely more enriched in 13 C and the δ 13 C of the terminal site is relatively heterogeneous within the propyl group attached to different functional groups of the gas-prone kerogen. Our findings based on the pyrolysis experiments and natural gas samples indicate thermal cracking and biodegradation appear to alter the δ 13 C cen values more significantly than the δ 13 C ter values of propane. The larger magnitude of ΔC c-t in the kMC simulations (Peterson et al., 2018) compared with those from the marine shale and coal possibly implies the non-random distributions of 13 C of propane precursors in the kerogens. As a new dimension of intramolecular isotopic information of propane, the PS δ 13 C values can contribute to fingerprinting the gas origins and identifying the various geological processes (e.g., kerogen cracking, wet-gas cracking, microbial activities) in sedimentary basins.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experimental Validation of Calorimetric Electron Capture Spectral Theory with 193 Pt

Using microcalorimeters, a high statistics, high-resolution calorimetric spectrum of electron capture in 163 Ho can be used to determine the neutrino mass. The spectral shape can be calculated from first principles with various assumptions and approximations. To determine the validity of these choices, the theoretical calculations must be compared to data from multiple isotopes. In this work, new calorimetric data for a 193 Pt-in-Pt absorber measured with a transition edge sensor are presented and compared to theoretical calculations and values from the literature.

74 ATOMIC AND MOLECULAR PHYSICS↗

Incorporating civilian radioxenon background estimates in anomaly detection

A nuclear explosion screening exercise in 2023 (Maurer et al., 2023) found challenges with discerning anomalous radioxenon activity concentrations relative to elevated background concentrations. Research has continued into methods to detect anomalous radioxenon concentrations by comparing samples to estimates of atmospheric radioxenon background concentrations caused by releases at nuclear reactors or medical isotope production facilities. A new approach estimates the sample concentrations using time-varying radioxenon release rates obtained using optimization techniques that constrain the facility release rates to plausible amounts based on historical data or facility knowledge. The purpose of the optimization is to determine whether any combination of plausible release rates from emitting facilities can explain a series of radioxenon measurements at one or more sampling stations. A case study uses radioxenon data collected at three locations in western Europe for a month in 2021 and considers releases from 77 locations. Fewer samples are identified as being anomalous using a simplistic flagging rule than from an application of the current International Monitoring System (IMS) activity concentration-level rule.

Environmental sciences↗

Irradiation performance of a U-7Mo in Al-Si matrix dispersion full-size fuel plate assembly

The Korea Atomic Energy Research Institute (KAERI) is leading the Ki-Jang Research Reactor (KJRR) project with the intent to develop a new reactor for medical isotope production and other nuclear research purposes. The KJRR core is designed to use high density fuel system where uranium alloyed with 7 wt% molybdenum (U-7Mo) particles are dispersed in a matrix of aluminum alloyed with 5 wt% silicon (Al-5Si) and clad in aluminum alloy 6061 (Al-6061) to form fuel plates. KAERI developed a fabrication facility to construct KJRR fuel assemblies and partnered with the Idaho National Laboratory (INL) to irradiate a full-size fuel assembly, with 21 total fuel plates, in the Advanced Test Reactor (ATR). Irradiation testing and subsequent Post Irradiation Exam (PIE) campaigns were performed successfully over a multi-year project. Monte Carlo neutronic calculations, coupling with a depletion code, were performed based on ATR’s as-run power history which showed that the highest power plate (plate 20) reached 83.1 % end-of-life (EOL) local burnup based on initial 235 U content. Additionally, finite element thermal modeling was performed based as-run power history which showed a beginning-of-life (BOL) peak local heat flux of 184 W/cm 2 . No anomalous fuel performance was observed during the irradiation and target test conditions were achieved. PIE showed favorable performance of the fuel assembly regarding all important phenomena. This paper describes the KJRR fuel assembly irradiation conditions and PIE data to support the conclusion that it performed well, without evidence of unexpected or problematic fuel performance, within an irradiation test designed to bound the KJRR design environment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Metal Organic Complexation in Seawater: Historical Background and Future Directions

The speciation of most biologically active trace metals in seawater is dominated by complexation by organic ligands. This review traces the history of work in this area, from the early observations that showed surprisingly poor recoveries using metal preconcentration protocols to the present day, where advances in mass spectroscopy and stable isotope geochemistry are providing new insights into the structure, origin, fate, and biogeochemical impact of organic ligands. Many long-standing hypotheses about the specific biological origin of ligands such as siderophores in seawater are finally being validated. This work has revealed the complexity of organic complexation, with multiple ligands and, in some cases, timescales of ligand exchange that are much slower than originally thought. The influence of organic complexation on scavenging is now a key parameter in biogeochemical models of biologically essential metals, especially iron. New insights about the sources and sinks of ligands are required to enhance the usefulness of these models.

Geochemistry & Geophysics↗

Nuclear Data for Spallation Neutron Radioisotope Production (Final Technical Report)

Over 50 million nuclear medicine procedures are performed annually, leading to a multi-billion dollar market for radioisotope production. The demand for new medical and research isotopes is growing, and radioisotope supply is insufficient. Most radioisotope production today utilizes charged particle or low-energy neutron irradiation of a target. Isotope production with tens to hundred MeV incident energies is a relatively unexplored option. There is a tremendous opportunity associated with a growing number of suitable domestic and international facilities buttressed by hundred million dollar global investments (e.g., the Los Alamos and Brookhaven Isotope Production Facilities, the European Spallation Source in Lund, and the Korean Multi-purpose Accelerator Complex in Gyeongbuk). In part due to a lack of supporting nuclear data that would make modeling radioisotope yields and purities possible, these facilities do not utilize their high-energy neutron fluxes for isotope production. This project attempted to measure neutron reaction excitation functions relevant to the large-scale production of critical radioisotopes, enabling development of cost-efficient isotope production methods, contributing to the improvement of theoretical models, and enhancing the value of national isotope production facilities. Reactions which form 67 Cu, 32 Si, and alpha-emitting isotopes like 225 Ac were chosen for their consistent prioritization by expert panels, representation of diverse reaction mechanisms, and relative lack of supporting nuclear data. Accurate measurement of these data is presently made only using quasi-monoenergetic neutron beams, which are produced by bombarding thin lithium targets with protons at only a few laboratories in the world. Ultimately, the projects efforts were incompletely accomplished due to a combination of multi-year technical issues at the only laboratory in the world which can make the proposed measurements, iThemba Labs in South Africa, and the onset of a global pandemic, which precluded the significant effort and time required to develop an independent measurement capability in the United States.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Simulating Muon Capture with MARLEY

Core-collapse supernovae are intense sources of tens-of-MeV neutrinos. Each explosion releases about 1058 neutrinos in a burst lasting tens of seconds. As neutrinos are weakly interacting, they escape more easily compared to photons, allowing them to be observed before the light signal. Understanding low-energy neutrino interactions with argon will be critical for future supernova measurements with the Deep Underground Neutrino Experiment (DUNE). Interpreting future DUNE supernova neutrino data will require a high-quality model of O(10 MeV) neutrino interactions, but the dominant charged-current cross section has never been measured at these low energies for an argon target. We exploit the theoretical similarities between muon capture, which has been measured, and antineutrino scattering to test MARLEY (Model of Argon Reaction Low Energy Yields), the simulation code used by DUNE to model supernova neutrino reactions. I implemented C++ code to add a muon capture mode to MARLEY and compared the predictions of the new simulation to measured isotope branching ratios of the residual nuclei. The preliminary branching ratios predicted by MARLEY running in muon capture mode demonstrate promising baseline performance when compared to experimental data and are expected to improve with further model adjustments.

Wong, Baker Louie↗