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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Relationship between isotope ratios in precipitation and stream water across watersheds of the National Ecological Observation Network

The timescales associated with precipitation moving through watersheds reveal processes that are critical to understanding many hydrologic systems. Measurements of environmental stable water isotope ratios (δ 2 H and δ 18 O) have been used as tracers to study hydrologic timescales by examining how long it takes for incoming precipitation tracers become stream discharge, yet limited measurements both spatially and temporally have bounded macroscale evaluations so far. Here in this observation driven study across North American biomes within the National Ecological Observation Network (NEON), we examined δ 18 O and δ 2 H stable water isotope in precipitation (δP) and stream water (δQ) at 26 co-located sites. With an average 54 precipitation samples and 139 stream water samples per site collected over 2014–2022, assessment of local meteoric water lines and local stream water lines showed geographic variation across North America. Taking the ratio of estimated seasonal amplitudes of δP and δQ to calculate young water fractions (F yw ), showed a Fyw range from 1% to 93% with most sites having F yw below 20%. Calculate d mean transit times (MTT) based on a gamma convolution model showed a MTT range from 0.10 to 13.2 years, with half of the sites having MTT estimates lower than 2 years. Significant correlations were found between the F yw and watershed area, longest flow length, and the longest flow length/slope. Significant correlations were found between MTT and site latitude, longitude, slope, clay fraction, temperature, precipitation magnitude, and precipitation frequency. The significant correlations between water timescale metrics and the environmental characteristics we report share some similarities with those reported in prior studies, demonstrating that these quantities are primarily driven by site or area specific factors. The analysis of isotope data presented here provides important constraints on isotope variation in North American biomes and the timescales of water movement through NEON study sites.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment (BIRDIE) (Final Report)

The Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment or BIRDIE was a precipitation collection campaign designed to measure cosmogenic isotopes of beryllium in rainfall and other forms of precipitation across the DOE Southern Great Plains (SGP) Atmospheric Radiation Measurement (ARM) site. Precipitation samples were collected over three weeks (May 21-June 10, 2022) at 11 SGP sites across a 120 km 2 domain in northern and central Oklahoma. The field campaign targeted summer-time convection rain events. We aimed to capture any spatial and/or temporal variability in the concentrations of beryllium-10 (10Be) and beryllium-7 (7Be) across the SGP ARM site during these rainfall events. The ratio of 10Be to 7Be (10/7Be) has been shown to be a powerful tracer for transport processes in the stratosphere-troposphere exchange (STE) system (e.g., Koch and Rind 1998). Any observed variability is analyzed to see if it could be linked to STE processes, including overshooting of deep convection clouds which penetrate the lower stratosphere. Six wet weather system events were collected within our three-week span. Five out of six of these rainfall events are classified as moderately to strongly convective. Those events are studied in more detail. The five systems also follow each other over a short time period of eleven days. In our rainfall samples we observed spatial and event variability in the concentrations of beryllium-10 and -7 which resulted in variability of 10/7 Be ratios. Each weather event appeared to exhibit a unique 10/7Be pattern across the domain that was not directly linked to storm total precipitation amount. To better understand the causes for this spatial variability, cloud characteristics in the domain were looked at to assess cloud type, cloud height and depth information. We also ran Hysplit back trajectories to identify possible air mass and moisture origins across our events. Detailed analysis is still on-going. The purpose of this technical report is to provide background on using cosmogenic isotopes as atmospheric tracers, describe the experimental design, and present the beryllium concentration and ratio data.

58 GEOSCIENCES↗
DOE OSTI2023

Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment (BIRDIE) (Field Campaign Report)

The Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment or BIRDIE was a precipitation collection campaign designed to measure cosmogenic isotopes of beryllium in rainfall and other forms of precipitation across the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Southern Great Plains (SGP) atmospheric observatory. Precipitation samples were collected over three weeks (May 21-June 10, 2022) at 11 SGP sites across a 120-km 2 domain in northern and central Oklahoma. The field campaign targeted summertime convection rain events. We aimed to capture any spatial and/or temporal variability in the concentrations of beryllium-10 (10Be) and beryllium-7 (7Be) across the ARM SGP site during these rainfall events. The ratio of 10Be to 7Be (10/7Be) has been shown to be a powerful tracer for transport processes in the stratosphere-troposphere exchange (STE) system (e.g., Koch and Rind 1998). Any observed variability is analyzed to see if it could be linked to STE processes, including overshooting of deep convection clouds that penetrate the lower stratosphere. Six wet weather system events were collected within our three-week span. Five out of six of these rainfall events are classified as moderately to strongly convective. Those events are studied in more detail. The five systems also follow each other over a short period of 11 days. In our rainfall samples we observed spatial and event variability in the concentrations of beryllium-10 and -7 that resulted in variability of 10/7Be ratios. Each weather event appeared to exhibit a unique 10/7Be pattern across the domain that was not directly linked to storm total precipitation amount. To better understand the causes for this spatial variability, cloud characteristics in the domain were looked at to assess cloud type, cloud height, and depth information. We also ran Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model back trajectories to identify possible air mass and moisture origins across our events. Detailed analysis is ongoing. The purpose of this technical report is to provide background on using cosmogenic isotopes as atmospheric tracers, describe the experimental design, and present the beryllium concentration and ratio data. Lastly, we note that BIRDIE coincided with two other deep convection field campaigns in the area: The National Aeronautics and Space Administration (NASA)’s Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) experiment (https://dcotss.org/) centered in Salina, Kansas, and the Targeted Observation by Radars and (uncrewed aerial systems) UAS of Supercells (TORUS) experiment (https://catalog.eol.ucar.edu/torus_2022) across the U.S. Central Plains. Additionally, a Lawrence Livermore National Laboratory ( LLNL) team at DCOTSS attempted to measure 10Be/7Be ratios on aerosols collected in situ in the lower and mid-stratosphere over Kansas using high-altitude balloons. Precipitation samples were also collected on the ground in Salina, Kansas.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

A dendritic strontium river isoscape for fisheries applications in the Sacramento River basin, California, USA

Objective Understanding the origins and movements of fish is fundamental to effective conservation and fisheries management. Strontium isotope ratios ( 87 Sr/ 86 Sr) in otoliths provide a powerful tracer of natal origin and migratory pathways. However, existing 87 Sr/ 86 Sr isoscapes for the Sacramento River basin, an ecosystem that supports ecologically and economically important salmon populations, rely on discrete classification approaches that overlook unsampled habitats and do not incorporate spatial uncertainty. Our objective was to develop a continuous, network-explicit 87 Sr/ 86 Sr isoscape with quantified uncertainty to fill in data gaps and enable probabilistic assignments of fish origin and movement. Methods We used river water 87 Sr/ 86 Sr data from 106 sites (1997–2021) to develop spatial stream network models that use dendritic connectivity and watershed characteristics (lithology, bedrock age, and land cover) to predict river water 87 Sr/ 86 Sr throughout the basin. Models were fitted using maximum and restricted likelihood and were evaluated via Akaike’s information criterion and leave-one-out cross validation. We produced both historical (pre-dam) and present-day (below-dam) isoscapes, delineated uncertainty-informed isotopic ranges using k -means clustering, and applied a proof-of-concept Bayesian assignment to estimate natal origins and early rearing habitats for two endangered winter-run Chinook Salmon Oncorhynchus tshawytscha. Results Cross validation indicated strong performance of the 87 Sr/ 86 Sr model (leave-one-out cross validation: R 2 = 0.91; root mean square error = 0.0005). Uncertainty-informed clustering identified 19 isotopic “suites” (reaches with indistinguishable 87 Sr/ 86 Sr values) in present-day anadromous habitats and 25 suites in the historical network. Example natal and early rearing assignments included predictions that challenged expectations for juvenile salmon migration based on predicted river 87 Sr/ 86 Sr compositions. Conclusions This study developed a continuous, network-explicit 87 Sr/ 86 Sr isoscape that integrates existing river data to predict 87 Sr/ 86 Sr in unsampled reaches and the likely achievable range and resolution of otolith-based origin and life history inference. The resulting river isoscape provides a valuable tool to predict salmon movements and identify habitats supporting their survival and growth that otherwise might remain undetected. Coupling these predictions with complementary approaches that ground-truth juvenile presence (e.g., targeted fish surveys) represents an important step toward science-informed restoration and management of critical habitats throughout the Sacramento River basin.

Environmental sciences↗
DOE OSTI2024

The BIRDIES Experiment: Measuring Beryllium Isotopes to Resolve Dynamics in the Stratosphere

Cosmogenic beryllium-10 and beryllium-7, and the ratio of the two (10Be/7Be), are powerful atmospheric tracers of stratosphere–troposphere exchange (STE) processes; however, measurements are sparse for altitudes well above the tropopause. We present a novel high-altitude balloon campaign aimed to measure these isotopes in the mid-stratosphere called Beryllium Isotopes for Resolving Dynamics in the Stratosphere (BIRDIES). BIRDIES targeted gravity waves produced by tropopause-overshooting convection to study their propagation and impact on STE dynamics, including the production of turbulence in the stratosphere. Two custom-designed payloads called FiSH and GASP were flown at altitudes approaching 30 km to measure in situ turbulence and beryllium isotopes (on aerosols), respectively. These were flown on nine high-altitude balloon flights over Kansas, USA, in summer 2022. The atmospheric samples were augmented with a ground-based rainfall collection targeting isotopic signatures of deep convection overshooting. Our GASP samples yielded mostly negligible amounts of both 10Be and 7Be collected in the mid-stratosphere but led to design improvements to increase aerosol capture in low-pressure environments. Observations from FiSH and the precipitation collection were more fruitful. FiSH showed the presence of turbulent velocity, temperature, and acoustic fluctuations in the stratosphere, including length scales in the infra-sonic range and inertial subrange that indicated times of elevated turbulence. The precipitation collection, and subsequent statistical analysis, showed that large spatial datasets of 10Be/7Be can be measured in individual rainfall events with minimum terrestrial contamination. While the spatial patterns in rainfall suggested some evidence for overshooting convection, inter-event temporal variability was clearly observed and predicted with good agreement using the 3D chemical transport model GEOS-CHEM.

58 GEOSCIENCES↗
NASA NTRS1981

Experiment K-317: Bone resorption in rats during spaceflight

Direct measurement of bone resorption in flight and synchronous control rats is described. Continuous tracer administration techniques were used, with replacement of dietary calcium with isotopically enriched Ca40 and measurement by neutron activation analysis of the Ca48 released by the skeleton. There is no large change in bone resorption in rats. Based on the time course of changes, the measured 20-25% decrease in resorption is probably secondary to a decrease in total body calcium turnover. The excretion of sodium, potassium and zinc all increase during flight, sodium and potassium to a level 4-5 times control values.

Cann, C. E.↗
NASA NTRS1983

Bone resorption and mineral excretion in rats during spaceflight

Bone resorption was measured directly in flight and synchronous control rats during COSMOS 1129. Continuous tracer administration techniques were used, with replacement of dietary calcium with isotopically enriched Ca-40 and measurement by neutron activation analysis of the Ca-48 released by the skeleton. There is no large change in bone resorption in rats at the end of 20 days of spaceflight as has been found for bone formation. Based on the time course of changes, the measured 20-25 percent decrease in resorption is probably secondary to a decrease in total body calcium turnover. The excretion of sodium, potassium, and zinc all increase during flight, sodium and potassium to a level four to five times control values.

Cann, C. E.↗
DOE OSTI2023

Accelerator-Based Production of Scandium Radioisotopes for Applications in Prostate Cancer: Toward Building a Pipeline for Rapid Development of Novel Theranostics

In the field of nuclear medicine, the β + -emitting 43 Sc and β - -emitting 47 Sc are promising candidates in cancer diagnosis and targeted radionuclide therapy (TRT) due to their favorable decay schema and shared pharmacokinetics as a true theranostic pair. Additionally, scandium is a group-3 transition metal (like 177 Lu) and exhibits affinity for DOTA-based chelators, which have been studied in depth, making the barrier to implementation lower for 43/47 Sc than for other proposed true theranostics. Before 43/47 Sc can see widespread pre-clinical evaluation, however, an accessible production methodology must be established and each isotope’s radiolabeling and animal imaging capabilities studied with a widely utilized tracer. As such, a simple means of converting an 18 MeV biomedical cyclotron to support solid targets and produce 43 Sc via the 42 Ca(d,n) 43 Sc reaction has been devised, exhibiting reasonable yields. The Nat Ti(γ,p) 47 Sc reaction is also investigated along with the successful implementation of chemical separation and purification methods for 43/47 Sc. The conjugation of 43/47 Sc with PSMA-617 at specific activities of up to 8.94 MBq/nmol and the subsequent imaging of LNCaP-ENZaR tumor xenografts in mouse models with both 43/47 Sc-PSMA-617 are also presented.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
NASA NTRS1993

Continental water recycling and H2(18)-O concentrations

Using a General Circulation Model (GCM) fitted with tracer diagnostics, we examine how continental moisture recycling affects the stable water isotope content of precipitation, focusing on its contribution to the 'noise' in the well-established relationship between temperature and delta O-18. On a global basis, for temperatures between -30 and 15 C, continental recycling explains more than a third of the variability in annual delta O-18 that is not explained by temperature. Recycling appears almost as important as temperature in defining delta O-18 distributions during northern hemisphere summer.

Koster, Randal D.↗
NASA NTRSDate not supplied

Isotopically Tracking Nitrogen Oxides, Nitrous Acid, And Nitric Acid, Particulate Nitrate from Wildfire During FIREX-AQ

Wildfires are an important source of reactive nitrogen species including nitrogen oxides (NOx = NO + NO2) and nitrous acid (HONO), as well as products such as nitric acid (HNO3) and particulate nitrate (p-NO3-). These species have strongly influence air quality and climate. In summer of 2019 (July 25 —August 21), as part of the FIREX-AQ ground mission, we drove ~3000 miles and sampled smoke of different ages in both daytime and nighttime from 5 different wildfires in the western US. Using recently developed methods that have been validated in both laboratory and field settings, we conducted high time resolution collection of NOx, NO2, HONO, HNO3, and p-NO3- for off-line characterization of isotopic composition δ15N, δ18O and Δ17O (=δ17O−0.52 δ18O). δ15N serves as a potential tracer for tracking sources and reactive nitrogen cycling pathways, δ18O and Δ17O provide key information about oxidation pathways (i.e. O3 versus RO2). Our measured δ15N for HONO ranges from -4.9‰ to +5.2‰ and -8‰ to +5.2‰ respectively, in the majority overlapping with our prior lab controlled burning results, which suggests the capability of δ15N for tracing the biomass burning emissions against other sources including vehicular emissions and soil emissions. In addition, our measurements show δ18O and Δ17O for NO2 and HONO vary significantly day vs night, as well as in young smoke vs aged smoke, likely reflecting different oxidizing mechanisms under different smoke conditions. Preliminary results of isotopic signatures of all the above reactive nitrogen species will be presented, and their relationships will be explored to identify wildfire derived reactive nitrogen source signatures and to constrain atmospheric processing pathways (e.g. secondary formation of HONO) for different fires under various smoke conditions depending on fuel types, fire conditions and meteorological conditions.

Jiajue Chai↗
NASA NTRS2013

Radiogenic Ingrowth of 40CA from Decay of 40K Provides a Powerful Tracer for Understanding the Origins of Felsic Magmas

Over time high K/Ca continental crust produces a unique Ca isotopic reservoir, with measurable 40Ca excesses compared to Earth's mantle (ɛCa=0). Thus, values of ɛCai > 1 indicate a significant crustal contribution to a magma. Values of ɛCai (<1) indistinguishable from mantle Ca indicate that the Ca in those magmas is either directly from the mantle, or is from partial melting of newly formed crust. So, whereas 40Ca excesses clearly define crustal contributions, mantle-like 40Ca/44Ca ratios are not as definitive. Here we present Ca isotopic measurements of intermediate to felsic igneous rocks from the western United States, and two crustal xenoliths found within the Fish Canyon Tuff (FCT). The two crustal xenoliths found within the 28.2 Ma FCT of the southern Rocky Mountain volcanic field (SRMVF) yield ɛCa values of ~4 and ~7.5, respectively. The 40Ca excesses of these possible source rocks are due to long-term in situ 40K decay and suggest that they are Precambrian in age. However, the FCT (ɛCai ~0.3) is within uncertainty of the mantle 40Ca/44Ca. Together, these data indicate that little Precambrian crust was involved in the petrogenesis of the FCT. Nd isotopic analyses of the FCT imply that it was generated from 10- 75% of an enriched component, and the Ca isotopic data appear to restrict that component to newly formed lower crust, or enriched mantle. However, the Ca isotopic data do permit assimilation of some crust with low Ca/Nd; decreasing the 143Nd/144Nd without adding much excess 40Ca to the FCT. Several other large tuffs from the SRMVF and from Yellowstone have ɛCai indistinguishable from the mantle. However, a few large tuffs from the SRMVF show significant 40Ca excesses. These tuffs (Wall Mountain, Blue Mesa, and Grizzly Peak) are likely sourced from near, or within the Colorado Mineral Belt. New isotopic measurements of Mesozoic and Tertiary granites from across the northern Great Basin show a range of ɛCai from 0 to ~3. In these samples ɛCai is generally correlated with ɛSri and is broadly negatively correlated with ɛNdi. However, for granites with similar ɛNdi at a given general location ɛCai can vary significantly (1 to 2 epsilon units). In rocks where low ɛNdi could also be due to melting from enriched reservoirs in the mantle lithosphere, the combination of high ɛCai with low ɛNdi clearly identifies crustal melts.

Mills, Ryan D.↗
NASA NTRS1987

Oxygen-18 tracer study of the passive thermal oxidation of silicon

This work focuses on the thermal oxidation of silicon near 1273 K using the double-tracer oxidation method. The results confirm that oxidation occurs by the transport of electrically neutral nonnetwork oxygen through the interstitial space of the vitreous silica (v-SiO2) scale. Simultaneously, self- (or isotopic-) diffusion occurs in the network, resulting in characteristic isotopic fraction distributions near the gas-scale interface. The self-diffusion coefficients calculated from these profiles agree with those reported for tracer diffusion in v-SiO2, and the diffusion coefficient calculated from the scale growth is consistent with reported O2 permeation data. An important parameter that describes the double-oxidation behavior is a ratio relating the scale thickness grown during the second oxidation, the network self-diffusion coefficient for oxygen, and the time of the second oxidation.

Cawley, J. D.↗
DOE OSTI2022

The incorporation of environmentally derived 87 Sr / 86 Sr and Sr/Ca in early otolith formation of Chinook salmon

Abstract Effective species management often requires understanding patterns of movement and habitat use. A common approach in identifying where individuals reside relies upon chemical tracers from the environment that are incorporated into an individual's tissues. For fish, isotopes in their otoliths, specifically the portion of their otolith formed during their larval stage, have been used to identify the natal origin. Complicating this work, however, is the fact that during this life stage, there is a shift in the source of isotopes deposited onto the growing otolith from maternally to environmentally derived. The objective of this study was to identify the portion of the otolith representing this transition to environmentally derived isotopes so as to accurately investigate questions of natal origin for a threatened population of fall Chinook salmon ( Oncorhynchus tshawytscha ). We exposed developing larvae to four treatments that differed in terms of their water strontium isotope ratio ( 87 Sr/ 86 Sr) and used change‐point analysis of otolith 87 Sr/ 86 Sr and strontium to calcium ratio (Sr/Ca) to identify the otolith radius corresponding to the transition to environmentally derived isotopes. Our results indicated this transition occurred, on average, at 132 μm ( 87 Sr/ 86 Sr; ±50 μm standard deviation) and 127 μm (Sr/Ca; ±29 μm) from the otolith core, which corresponded to the developmental time between hatching and exogenous feeding. A substantial proportion of our otoliths (i.e., 61%) did not show convergence between otolith and water 87 Sr/ 86 Sr by the end of the 113‐day experiment, which was likely due to the dietary contribution of marine‐based feed. Therefore, we were unable to recommend an otolith radius to target for the purposes of reconstructing natal origin apart from being beyond approximately 130 μm.

Chittaro, Paul↗
NASA NTRS1986

Speculations on nature and extent of Archean basement in Labrador as indicated by SR, ND and PB isotopic systematics of proterozoic intrusives

The Sm-Nd and Rb-Sr isotopic compositions of mid to late Proterozoic (approximately 1.6 to 1.1 Ga) massif-type anorthosites and mafic intrusives in the eastern Canadian shield are correlated with geographic location. Complexes in the Grenville province have positive epsilon sub Nd values and initial Sr-87/Sr-86 (I sub Sr) generally less than 0.703, suggesting derivation from depleted mantle. In Labrador, similar complexes close to or northwest of a line roughly corresponding to the Grenville Front have negative epsilon sub Nd values and I sub Sr 0.703. This contrast was intrepreted as reflecting either enriched mantle under the Nain Province, or contamination of the Nain intrusives with older crustal components. Lead isotopic compositions, however, favor the latter. The possibility of using these Proterozoic intrusives as tracers to characterize the nature and extent of older basement types in Labrador is discussed.

Ashwal, L. D.↗
NASA NTRS1994

D/H ratios and H2O contents of mantle-derived amphibole megacrysts from Dish Hill, California

D/H ratios are, in principle, useful in characterizing reservoirs of mantle hydrogen and as tracers of volatile transfer processes in Earth's interior. In practice, however, interpretation of isotopic measurements on mantle derived H is complicated by surface processes such as contamination and degassing which may alter the primary D/H ratio. Although there are indications that water associated with subduction zones and certain chemically enriched basalts is enriched in D relative to 'typical' upper mantle water, the extent of isotopic heterogeneity of mantle H remains uncertain. Kaersutitic amphibole megacrysts in alkaline basalts are one of the most widespread sources of mantle water and are therefore potentially useful for large-scale regional studies of D/H variation. However, D/H ratios of these amphiboles vary widely (from plus 8 to minus 113 percent), even in samples from the same locality, so that this potential has yet to be realized. In order to investigate the origin of this variability, and to explore the possibility that primary mantle D/H ratios may be deduced from these amphiboles, we analyzed the D/H ratios and chemical compositions of a suite of 17 kaersutitic amphiboles from Dish Hill, California. This work contrasts with previous studies in which sampling is widespread, but representatives from any given locality are few. Samples were collected from a restricted area on the southern flank of the volcanic center and are associated with the basal volcanic breccia. Fourteen of the samples were large single crystals or crystal fragments (megacrysts, 0.4 to 30 grams), believed to derive from pegmatitic veins crystallized from melts in the mantle. Two were coarse-grained intergrowths of amphibole with olivine and spinel, and one was a thin (2 mm) selvage on a peridotite xenolith.

Bell, David R.↗
DOE OSTI2025

Elemental and Isotopic Yields from T Coronae Borealis: Predictions and Uncertainties

T Coronae Borealis (T CrB) is a symbiotic recurrent nova system expected to undergo its next outburst within the next 2 yr. Recent hydrodynamic simulations have predicted the nucleosynthetic yields for both carbon–oxygen (CO) and oxygen–neon (ONe) white-dwarf models, but without accounting for thermonuclear reaction rate uncertainties. We perform detailed Monte Carlo postprocessing nucleosynthesis calculations based on updated thermonuclear reaction rates and uncertainties from the 2025 evaluation. We quantify the resulting abundance uncertainties and identify the key nuclear reactions that dominate them. Our results show that both the CO and ONe nova models robustly produce characteristic CNO isotopes. More pronounced abundance differences emerge for elements with A ≥ 20. Sulfur is the most robust observational discriminator between the CO and ONe nova models, with a model-to-model difference of a factor of ≈30 and minimal sensitivity to reaction rate uncertainties. Neon, silicon, and phosphorus exhibit even larger abundance differences (factors of ≈150–250), providing strong diagnostic potential. While their predicted yields are subject to larger uncertainties, these remain smaller than the model-to-model differences, allowing these elements to serve as useful, though less precise, tracers of white-dwarf composition. Chlorine, argon, and potassium also differ between models, but the 1σ-abundance ranges for the CO and ONe models overlap, reducing their present usefulness as composition tracers. We find that only nine nuclear reactions dominate the abundance uncertainties of the most diagnostically important isotopes, and their influence is largely independent of the underlying white-dwarf composition. These results provide guidance for future experimental efforts and for interpreting ejecta compositions in the next eruption of T CrB.

Chemical Abundances↗
NASA NTRS2016

Evaluation of Observed and Modelled Aerosol Lifetimes Using Radioactive Tracers of Opportunity and an Ensemble of 19 Global Models

Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (Cs-137) and xenon-133 (Xe-133) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. Cs-137 size distribution measurements taken close to the power plant suggested that accumulation mode (AM) sulfate aerosols were the main carriers of cesium. Hence, Cs-137 can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas Xe-133 behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of Cs-137that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and Xe-133 emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled Cs-137and Xe-133 concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95% confidence interval 13.1-15.7 days). The equivalent modelled e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.42.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (Xe-133) concentrations in the Arctic as well but to a smaller extent than for the aerosol (Cs-137) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Radioactive isotopes↗
DOE OSTI2025

Utilization of traceable standards to validate plutonium isotopic purification and separation of plutonium progeny using AG MP-1M resin for nuclear forensic investigations

Radio-chronometric studies on plutonium (Pu) materials require independent measurement of the Pu (parent) content and isotopic distribution as well as concentration and isotopic distribution of the plutonium isotopic decay products. We performed a series of experiments to demonstrate the consistency of separations using the Lewatit MP 800 macroporous anion exchange resin and the AG MP-1M resin with traceable Pu isotopic certified reference material (CRM) standards 136, 137, 138, and 126-A. Two different mesh-sizes of the AG MP-1M resin were tested and the 50–100 mesh size resin was found to work more efficiently for the separation task. Both Lewatit and AG MP-1M resins were found to perform satisfactorily for quantitatively extracting the americium (Am) and uranium (U) progeny as well as gallium (Ga) present as a tracer in the Pu material. Both resins were effective in removing isobaric interferences from the Pu fraction used in isotopic measurements by thermal ionization mass spectrometry (TIMS). To address the co-elution of uranium and gallium, Alizarin red S (ARS) was used as a colorimetric dye to determine the behavior of UO 2 2+ and Ga 3+ on AG MP-1M resin with various acidic solutions as eluents using UV–vis spectra. Poor resolution of these peaks complicated quantitative analysis by UV–vis spectroscopy, but these results were informative in planning automated separation experiments by HPLC. LA-UR-24-28919.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗