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At least 73 records · Page 4

The FRIB Decay Station: New Horizons with Rare Isotopes

In May 2022, the Facility for Rare Isotope Beams (FRIB), located on the campus of Michigan State University (MSU), began delivering exotic isotopes to an international community of scientists. New discoveries are now being reported from radioactive decay of neutron-rich nuclei near N = 20 and N = 28.FRIB is expected to produce roughly 80% of the unstable or radioactive isotopes predicted to exist up to uranium (Z = 92). The new user facility is supported by the U.S. Department of Energy, and it is operated by MSU. A high-power superconducting linear accelerator, shaped like a paper-clip, drives the production of these rare isotopes by colliding stable nuclei moving at half the speed of light with a rotating, water-cooled graphite tar-get. These collisions cause the primary stable beam to fragment into a wide variety of unstable nuclei, which can be subsequently filtered through a multistage magnetic separator, the Advanced Rare Isotope Separator, and transported to one of several experimental stations. The FRIB Decay Station initiator (FDSi) (see Figure 1) was developed to enable comprehensive radio-active decay studies of the exotic nuclei produced by FRIB and it was used in the first two experiments in 2022. Further, the FDSi is a highly reconfigurable multidetector system with two focal planes (FP1 for discrete spectroscopy and FP2 for total absorption spectroscopy) that can be optimized for the specific science goals of each experiment. It is designed, built, and operated by a community of users with the sup-port of U.S. funding agencies, including the Department of Energy and National Science Foundation.

07 ISOTOPE AND RADIATION SOURCES↗

CAPE-K_ISO: Water vapor isotopic measurements from Western Tasmania

This dataset provides processed 1-minute water vapor isotope observations from the Water Vapor Isotopic Measurements During CAPE-K project at the Kennaook/Cape Grim Baseline Air Pollution Station in northwestern Tasmania. Measurements were made with a Picarro L-2130 cavity ring-down spectroscopy analyzer during the CAPE-K deployment. The dataset includes water vapor mixing ratio, d18O, dD, deuterium excess, and propagated 1-sigma uncertainties. Isotope ratios are calibrated to the VSMOW/SLAP scale. Calibration intervals, transition periods, and obvious isotope outliers have been removed. The processed record spans 11 June 2024 to 15 October 2025 and is intended for studies of Southern Ocean marine boundary-layer moisture, isotope variability, air-sea exchange, and cloud and precipitation processes.

Water Vapor Isotopic Composition↗

Complete resolution across the neodymium/samarium isotopic envelope with a liquid sampling‐atmospheric pressure glow discharge — Orbitrap mass spectrometer

Rationale Nd and Sm isotope ratios play an important role in geological dating and as nuclear forensic signatures; however, the overlap of the respective 144, 148, 150 Nd/Sm isobars requires prior separations to be performed before analysis on typical MS platforms. The work presented here overcomes these isobaric interferences using ultrahigh‐mass resolution to alleviate interference without prior chemical separations. Methods A liquid sampling‐atmospheric pressure glow discharge ion source was coupled to a standard, QExactive Focus Orbitrap mass spectrometer, providing a mass resolution of ~80 k. A Spectroswiss FTMS booster X2 data acquisition package was used to collect extended transients, providing much higher mass resolution; ~230 k and ~600 k are employed here for Nd and Sm isotopes. Results While the standard Orbitrap resolution is far greater than typical “atomic” MS platforms, it was insufficient to alleviate all isobars. The use of a resolution of ~230 k resulted in baseline separation across the entire isotopic envelope for both Nd and Sm. Isotope ratios obtained from Nd:Sm mixtures using high‐resolution were equivalent to those found for individual‐element solutions, while isotope ratios obtained at a resolution of ~80 k (standard for the OEM data system) showed large deviations. Conclusions Use of ultrahigh‐resolution is an attractive alternative to extensive chemical separations to alleviate severe isobaric interferences. Sufficient mass resolution greatly reduces/eliminates the need for sample manipulations (separations) before analysis while reducing costs and total analysis times.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A new HALEU isotopic certified reference material

Candidate certified reference material (CRM) U196 was prepared by gravimetrically mixing and dissolving NNSA NRMP CRM 112-A (natural uranium metal) and CRM 116-A (highly enriched 93.2% 235 U metal) to achieve a high-assay low-enriched uranium (HALEU) isotopic abundance reference material. CRM U196 will be certified for the 233 U/ 238 U, 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U ratios. Gravimetrically determined uranium isotope amount ratios and values derived from the isotope data were calculated from the buoyancy corrected mass data and from certified values for the metal CRMs used to create the solution. The 235 U isotope amount fraction (·100) and expanded uncertainty is 19.5846 ± 0.0028. For attribute verification, total evaporation and modified total evaporation isotope ratio measurements were performed. In conclusion, the reference material is to be distributed as a unit containing 5 mg uranium as dry uranyl nitrate.

High-assay low-enriched uranium↗

A case study on the use of carbon sticky tabs for microbeam uranium isotope measurement with an emphasis on understanding the influence of subtle variations in substrate composition

In this paper we integrate laser induced breakdown spectroscopy (LIBS), large geometry secondary ion mass spectrometry (LG-SIMS), laser ablation—multi collector—inductively coupled plasma—mass spectrometry (LA-MC-ICP-MS), and trace elemental compositions obtained by bulk digestion from a suite of commercially available carbon sticky tabs to determine if subtle variations in the tab’s composition can be tied to shifts in the observed uranium isotopic composition of the IRMM-2020 standard relative to its ‘true’ value. The results suggest that, although clear differences exist in the relative abundances of carbon and hydrogen across the various carbon sticky tabs examined, as well as differences in their trace elemental and total uranium concentrations, these differences do not appear to influence the LG-SIMS or LA-MC-ICP-MS uranium isotope ratio measurements, or the appearance of the uranium mass spectrum scans. Instead, the quality (i.e., precision and accuracy) of the LG-SIMS and LA-MC-ICP-MS results are directly proportional to the observed signal intensity at the time of analysis. For the LG-SIMS measurements, there does appear to be a direct correlation between 235U1H hydride formation rates and vacuum conditions within the instrument’s analytical chamber. Furthermore, none of the carbon sticky tabs examined by LG-SIMS displayed evidence of elevated background uranium content. While a preliminary correlation was observed between the uranium isotope background signal during LA-MC-ICP-MS and the total uranium concentrations determined by isotope dilution, none of the tabs displayed a high enough analytical background to affect the isotope ratio measurements.

Zirakparvar, Alex [ORNL] (ORCID:0000000337797730)↗

Nuclear charge radii of germanium isotopes around N = 40

Collinear laser spectroscopy measurements were performed on 68−74 Ge isotopes (Z=32) at ISOLDE-CERN, by probing the 4s 2 4p 2 3 P 1 → 4s 2 4p5s 3 P$^{o}_{1}$ atomic transition (269~nm) of germanium. Nuclear charge radii are determined via the measured isotope shifts, revealing a larger local variation than the neighboring isotopic chains. Nuclear density functional theory with the Fayans functionals Fy(Δr,HFB) and Fy(IVP), and the SV-min Skyrme describes the experimental data for the differential charge radii δ⟨r 2 ⟩ and charge radii R c within the theoretical uncertainties. The observed large variation in the charge radii of germanium isotopes is better accounted for by theoretical models incorporating ground state quadrupole correlations. This suggests that the polarization effects due to pairing and deformation contribute to the observed large odd-even staggering in the charge radii of the Ge isotopic chain.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

First measurement of the yield of 8 He isotopes produced in liquid scintillator by cosmic-ray muons at Daya Bay

Here, Daya Bay presents the first measurement of cosmogenic 8 He isotope production in liquid scintillator, using an innovative method for identifying cascade decays of 8 He and its child isotope, 8 Li. We also measure the production yield of 9 Li isotopes using well-established methodology. The results, in units of 10 –8 μ –1 ⁢g –1 cm 2 , are 0.307 ± 0.042, 0.341 ± 0.040, and 0.546 ± 0.076 for 8 He, and 6.73 ± 0.73, 6.75 ± 0.70, and 13.74 ± 0.82 for 9 Li at average muon energies of 63.9 GeV, 64.7 GeV, and 143.0 GeV, respectively. The measured production rate of 8 He isotopes is more than an order of magnitude lower than any other measurement of cosmogenic isotope production. It replaces the results of previous attempts to determine the ratio of 8 He to 9 Li production that yielded a wide range of limits from 0% to 30%. The results provide future liquid-scintillator-based experiments with improved ability to predict cosmogenic backgrounds.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Charge Radii of Neutron-Rich Scandium Isotopes and the Seniority Symmetry in the 0⁢𝑓 7/2 Shell

Nuclear charge radii of neutron-rich 47–49 Sc isotopes were measured using collinear laser spectroscopy at CERN-ISOLDE. The new data reveal that the charge radii of scandium isotopes exhibit a distinct trend between 𝑁 = 20 and 𝑁 = 28, with 41 Sc and 49 Sc isotopes having similar values, mirroring the closeness of the charge radii of 40 Ca and 48 Ca. Theoretical models that successfully interpret the radii of calcium isotopes could not account for the observed behavior in scandium radii, in particular the reduced odd-even staggering. Remarkably, the inclusion of the new 49 Sc radius data has unveiled a similar trend in the charge radii of 𝑁 = 28 isotones and 𝑍 = 20 isotopes when adding the protons atop the 48 Ca core and the neutrons atop the 40 Ca core, respectively. We demonstrate that this trend is consistent with the prediction of the seniority model.

Nuclear charge distribution↗

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↗

Refining Methods to Determine the Isotopic Composition of Uranium Particles by Laser Ablation MC-ICP-MS

We report on efforts to mitigate the generation of isotopic anomalies during the ablation of micrometer-sized uranium oxide particles and analysis by MC-ICP-MS. The results of testing on particles of U200 indicate that laser fluence and frequency can affect isotopic data produced by laser ablation, but no settings were tested that could eradicate the signal spiking effect and generation of anomalous isotopic data for 234U/238U and 236U/238U. These anomalies are more frequent in samples with higher 235U enrichments, which is expected given their higher abundances of 234U and 236U. Of the standards tested here, only U005-A was anomaly-free. Efforts to compare the laser traces for particles with normal and anomalous isotopic compositions showed subtle differences in the behavior of the 234U/238U and 236U/238U ratios. However, it would be challenging to identify anomalous data points from a population of unknowns using this distinction, i.e., this is unlikely to be diagnostic. Thus, using current analytical hardware, we cannot eradicate the signal spiking phenomenon and cannot unambiguously identify isotopic anomalies from laser ablation traces. Ultimately, laser ablation ICP-MS would either require dramatic improvement to the ablation process and generation of more homogenous aerosols and/or improvements to detector electronics to identify and correct for the spiking phenomenon. Even if the reliability of the technique could be improved, a broader question to address is whether current data quality is of a high enough standard for laser ablation MC-ICP-MS to be used as a complementary technique to LG-SIMS for Safeguards.

organic↗

Experimental determination of hydrogen isotopic equilibrium in the system H 2 O (l) -H 2(g) from 3 to 90 °C

Molecular hydrogen (H 2 ) is found in a variety of settings on and in the Earth from low-temperature sediments to hydrothermal vents, and is actively being considered as an energy resource for the transition to a green energy future. The hydrogen isotopic composition of H 2 , given as D/H ratios or δD, varies in nature by hundreds of per mil from ∼−800 ‰ in hydrothermal and sedimentary systems to ∼+450 ‰ in the stratosphere. This range reflects a variety of processes, including kinetic isotope effects associated with formation and destruction and equilibration with water, the latter proceeding at fast (order year) timescales at low temperatures (<100 °C). At isotopic equilibrium, the D/H fractionation factor between liquid water and hydrogen ( D α H2O(l)-H2(g) ) is a function of temperature and can thus be used as a geothermometer for H 2 formation or re-equilibration temperatures. Multiple studies have produced theoretical calculations for hydrogen isotopic equilibrium between H 2 and water vapor. However, only three published experimental calibrations used in geochemistry exist for the H 2 O-H 2 system: two between 51 and 742 °C for H 2 O (g) -H 2(g) (Suess, 1949, Cerrai et al., 1954), and one in the H 2 O (l) -H 2(g) system for temperatures <100 °C (Rolston et al., 1976). Despite these calibrations existing, there is uncertainty on their accuracy at low temperatures (<100 °C; e.g., Horibe and Craig, 1995).

08 HYDROGEN↗

Quantifying uncertainty in physics-based predictions of rare-isotope production cross sections via Bayesian-inspired model averaging across nuclear mass tables

Accurate prediction of fragmentation cross sections is essential for rare-isotope beam production, planning new-isotope searches, and designing experiments to study the most exotic regions of the nuclear chart. However, existing reaction models and phenomenological cross-section parametrizations often exhibit significant deviations over broad regions of mass and charge. In this work, a Bayesian-inspired model-averaging framework is developed to combine abrasion-ablation (AA) calculations based on multiple nuclear mass tables into a single statistically weighted estimate. For the calibrated systems, the model weights are assigned empirically according to the relative quality of fit to measured cross sections, thereby reducing systematic model bias while preserving the underlying physics content of the AA description. The weights are constrained using proton-rich fragmentation data for the 78 Kr and 124 Xe projectiles. The resulting parameter trends are then propagated to the 92 Mo and 144 Sm systems through a controlled scaling procedure. In the present implementation, the excitation-energy prescription is fixed, while the averaging is performed across nuclear-mass inputs; the framework provides both weighted cross sections and associated uncertainty estimates. Applied to proton-rich fragmentation, the present approach provides a practical basis for interpolation and limited extrapolation in regions relevant to rare-isotope production. The resulting predictions are used to assess the production of very proton-rich nuclei, and candidate new isotopes are discussed.

Bayesian methods↗

Isotope Production Education and Research via a Systematic Study of Photo-nuclear Reaction Yields and Excitation Functions

A new collaboration between the New Mexico Institute of Mining and Technology, Idaho State University, and Idaho National Laboratory builds the domestic workforce in isotope production and related science and technologies by conducting research and education programs related to photo-nuclear reactions. Workforce development was identified by the Department of Energy’s Office of Science in the Reaching a New Energy Sciences Workforce (RENEW) program that seeks to engage underrepresented university students in isotope production activities. This collaboration includes coursework development, student training, and isotope production research utilizing photo-nuclear reactions at electron linear accelerators. Bremsstrahlung-weighted excitation functions and cross-sections will be measured and the use of nanomaterials to exploit kinematic recoil reactions will be investigated. Students will be hosted at the Idaho National Laboratory where mentors will provide opportunities to explore careers in nuclear science and technology. This presentation regards the ongoing progress of the research and education objectives of the collaboration that was performed under the Office of Science Isotopes Program under award number D000-22-2765.

07 ISOTOPE AND RADIATION SOURCES↗

Comparative clumped isotope temperature relationships in freshwater carbonates

Lacustrine, riverine and spring carbonates represent archives of terrestrial climates and their geochemistry has been used to study palaeoenvironments. Clumped isotope thermometry is an emerging tool that has been applied to freshwater carbonates. Limited work has been done to evaluate comparative relationships between clumped isotopes and temperature in different types of modern freshwater carbonates. This study assembles an extensive calibration data set with 135 samples of modern freshwater carbonates from 96 sites and constrains the relationship between independent observations of water temperature and the clumped isotopic composition of carbonates (denoted by Δ 47 ), including new measurements, and recalculates published data in accordance with current community-defined standard values. For temperature reconstruction, the study reports a composite freshwater calibration and material-specific calibrations for biogenic carbonates (freshwater gastropods and bivalves), fine-grained carbonate (e.g. micrites), biologically mediated carbonates (microbialites and tufas) and travertines. Material-specific calibration trends show a convergence of slopes that are in agreement with recently published syntheses, but statistically significant differences in intercepts occur between some materials (e.g. some biogenics, fine-grained carbonates). These differences may arise due to unresolved seasonal biases, kinetic isotope effects and/or varying degrees of biological influence. The impact of different calibrations is shown through application to new data for glacial and deglacial age travertines from Austria and published data sets. While material-specific calibrations may yield more accurate results for biogenic and fine-grained carbonate samples, the use of material-specific and the composite freshwater calibrations generally produces values within 1.0–1.5°C of each other, and typically fall within calibration uncertainty given limitations of precision.

54 ENVIRONMENTAL SCIENCES↗

California Trees Seasonally Use Augmented Water Sources: Water Isotope Tracking in a Groundwater‐Dependent Ecosystem

Sustainable groundwater management must account for the needs of groundwater dependent ecosystems. To understand the relationship of ecosystems and seasonal water use, we studied the stable isotope composition (δ 18 O and δ 2 H) of water in streamside trees in a semi-arid streamside environment (Livermore, California, USA). We sampled seven trees at two sites every other month from April 2024 through April 2025 for tree xylem stable water isotope signatures. These data were compared to potential source waters: precipitation, imported surface water, soil water and regional groundwaters. Large daily precipitation events were found to be isotopically similar to regional groundwater and were thus treated as one water source. A Bayesian mixing model using stable water isotopes was used to determine the ratios of these three potential source waters (small daily precipitation events, groundwater/large daily precipitation events and imported water) present in tree xylem water. On average, tree water sources include 32% imported water (SD = 9%), 35% small daily precipitation events (SD = 10%) and 33% groundwater (SD = 3%), with significant seasonal variation (t summer-winter = 30.8, p < 0.01), particularly drawing more imported water (more than 55%) in the summer. While small daily precipitation events contribute only 10% of the total precipitation in our dataset, it represents a third of water used by trees. In addition, while these ecosystems are designated as groundwater dependent ecosystems, the trees use approximately one third imported water and even more during dry summer months. This approach provides water managers with a practical tool for quantifying ecosystem water needs, supporting data-driven decisions and regulatory compliance. While California's Sustainable Groundwater Management Act emphasizes supporting groundwater dependent ecosystems, it allows flexibility in demonstrating benefits. In conclusion, our methodology provides a way to document that management actions (such as managed aquifer recharge with imported water) deliver measurable co-benefits to GDEs.

Geosciences↗

How Rains and Floods Become Groundwater: Understanding Recharge Pathways With Stable and Cosmogenic Isotopes

Anthropogenic climate change leads to increased precipitation intensity and exacerbated droughts in California, challenging the reliability and drought resiliency of water supply. Storing floodwater underground via managed aquifer recharge can mitigate these effects through direct infiltration or streambed infiltration. Seasonally dry streams (arroyos) already play an important part in managing groundwater recharge to the Livermore basin (CA). Understanding how, when and where stormwater and arroyo water infiltrate is critical to effectively utilise this strategy. To track water from recent storms (water year 2022–2023, WY23) into the Livermore Valley Groundwater Basin, we analysed stable water isotopes (δ 18 O and δ 2 H) in combination with naturally occurring radioactive isotopic tracers, sulphur-35 ( 35 S, t ½ = 87 days) and tritium ( 3 H, t ½ = 12.3 years). By comparing measurements of δ 18 O, 35 S and 3 H in arroyos to precipitation and groundwater, we classified the relative age and identified source of recharge to 16 wells near two arroyos. Two wells contained water with recent recharge (from WY23) from local precipitation. One well had recent recharge from variable (precipitation and imported water) sources. One well contained imported water recharge. Three wells contained water from mixed recent and older (pre-WY23) waters, from local precipitation sources. Two wells contained recent recharge from local mine settling ponds. Seven wells had older recharge from local precipitation sources. This combination of isotopes allows us to delineate where local and imported water recharges in this highly managed basin and identify locations where managed aquifer recharge is contributing to rapid groundwater infiltration. Our combined interpretation of isotopic water ages and sources in the context of land use shows that local infiltration of precipitation in open spaces is an important recharge mechanism, in addition to the managed arroyo recharge. Finally, a broader familiarity with 35 S will enable more extensive research on the infiltration of urban floodwaters.

58 GEOSCIENCES↗

Neutron capture signatures determined from gadolinium isotope compositions of uranium ore concentrates using MC-ICPMS

We present Gd isotope compositions on 25 well-characterized uranium ore concentrates (UOCs). About half the UOCs have isotope depletions in 157 Gd coupled with anticorrelated excesses in 158 Gd due to neutron capture effects. UOCs from older ore bodies and with higher U contents show larger neutron capture effects than UOCs from younger ore bodies with lower U contents. These Gd data are correlated with their previously measured Sm isotope compositions, and we use the Sm data to estimate the neutron fluence of these samples. In conclusion, this work demonstrates how Gd isotope signatures can be employed as a new tool for nuclear forensics.

Earth Sciences↗

Parametric optimization of the liquid sampling-atmospheric pressure glow discharge ionization source coupled to an Orbitrap mass spectrometer for neodymium isotope ratio determinations

Isotope ratio determinations are a valuable tool in several application areas. In nuclear forensics, the isotope ratios of uranium and plutonium are commonly used as a signature for the nuclear material's provenance and processing history. However, signatures from other coexisting elements, such as neodymium and samarium, can offer additional insights. Here, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source coupled to an Orbitrap mass spectrometer (MS) has demonstrated its utility for actinide measurements. This instrumental platform can leverage the high resolution offered by the Orbitrap MS to overcome potential isobaric interferences, such as 144 Nd- 144 Sm, 148 Nd- 148 Sm, and 150 Nd- 150 Sm pairs. The work presented herein demonstrates the rapid, accurate, and precise determination of the isotope ratios for neodymium using the LS-APGD/Orbitrap MS. Both the LS-APGD and Orbitrap MS parameters were optimized systematically, with NdO + found to be the most abundant, most reduced species after applying the optimal collision-induced dissociation modalities. A limit of detection of 3 pg of 142 Nd was achieved when data was acquired and processed using the FTMS Booster, an external data acquisition and processing system offered by Spectroswiss. Excellent accuracy of better than 99 % and precision of <1 % RSD were achieved when a solution of the well-characterized neodymium standard (JNdi-1 standard) was analyzed under the optimized condition, indicating the LS-APGD/Orbitrap's great potential for isotope ratio analysis of Nd and other REEs for diverse applications.

47 OTHER INSTRUMENTATION↗