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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Artificial Intelligence for Isotopes: Report on the 2022 Workshop on Artificial Intelligence for Isotope R&D and Production

The Department of Energy Isotope Program (DOE IP) hosted a virtual workshop on Artificial Intelligence (AI) for Isotope R&D and Production on March 17 and April 14, 2022. The purpose of the workshop was for DOE IP to further its understanding of the potential roles for and subsequent opportunities to incorporate AI into its activities. The workshop brought over 80 participants together from both the AI and isotope science communities. Participants contributed ideas through plenary talks, lightning talks, and breakout discussion sessions. The primary focus of all discussions was related to isotope production and processing. However, isotope enrichment, workforce development, and supply chain management were also discussed. This report documents the information presented and discussed at the workshop.

07 ISOTOPE AND RADIATION SOURCES↗
NASA NTRS2009

Chlorine Isotopes: As a Possible Tracer of Fluid/Bio-Activities on Mars and a Progress Report on Chlorine Isotope Analysis by TIMs

Significantly large mass fractionations between chlorine isotopes (Cl-35, Cl-37) have been reported for terrestrial materials including both geological samples and laboratory materials. Also, the chlorine isotopic composition can be used as a tracer for early solar system processes. Moreover, chlorine is ubiquitous on the Martian surface. Typical chlorine abundances in Gusev soils are approx.0.5 %. The global surface average chlorine abundance also is approx.0.5 %. Striking variations among outcrop rocks at Meridiani were reported with some chlorine abundances as high as approx.2%. Characterizing conditions under which chlorine isotopic fractionation may occur is clearly of interest to planetary science. Thus, we have initiated development of a chlorine isotopic analysis technique using TIMS at NASA-JSC. We present here a progress report on the current status of development at JSC and discuss the possible application of chlorine isotopic analysis to Martian meteorites in a search for fluid- and possibly biological activity on Mars.

Nakamura, N.↗
NASA NTRS2011

FE and MG Isotopic Analyses of Isotopically Unusual Presolar Silicate Grains

Interstellar and circumstellar silicate grains are thought to be Mg-rich and Fe-poor, based on astronomical observations and equilibrium condensation models of silicate dust formation in stellar outflows. On the other hand, presolar silicates isolated from meteorites have surprisingly high Fe contents and few Mg-rich grains are observed. The high Fe contents in meteoritic presolar silicates may indicate they formed by a non-equilibrium condensation process. Alternatively, the Fe in the stardust grains could have been acquired during parent body alteration. The origin of Fe in presolar silicates may be deduced from its isotopic composition. Thus far, Fe isotopic measurements of presolar silicates are limited to the Fe-54/Fe-56 ratios of 14 grains. Only two slight anomalies (albeit solar within error) were observed. However, these measurements suffered from contamination of Fe from the adjacent meteorite matrix, which diluted any isotopic anomalies. We have isolated four presolar silicates having unusual O isotopic compositions by focused ion beam (FIB) milling and obtained their undiluted Mg and Fe isotopic compositions. These compositions help to identify the grains stellar sources and to determine the source of Fe in the grains.

Nguyen, A. N.↗
NASA NTRS2011

Carbon Isotope Measurements of Experimentally-Derived Hydrothermal Mineral-Catalyzed Organic Products by Pyrolysis-Isotope Ratio Mass Spectrometry

We report results of experiments to measure the C isotope composition of mineral catalyzed organic compounds derived from high temperature and high pressure synthesis. These experiments make use of an innovative pyrolysis technique designed to extract and measure C isotopes. To date, our experiments have focused on the pyrolysis and C isotope ratio measurements of low-molecular weight intermediary hydrocarbons (organic acids and alcohols) and serve as a proof of concept for making C and H isotope measurements on more complicated mixtures of solid-phase hydrocarbons and intermediary products produced during high temperature and high pressure synthesis on mineral-catalyzed surfaces. The impetus for this work stems from recently reported observations of methane detected within the Martian atmosphere [1-4], coupled with evidence showing extensive water-rock interaction during Martian history [5-7]. Methane production on Mars could be the result of synthesis by mineral surface-catalyzed reduction of CO2 and/or CO by Fischer-Tropsch Type (FTT) reactions during serpentization reactions [8,9]. Others have conducted experimental studies to show that FTT reactions are plausible mechanisms for low-molecular weight hydrocarbon formation in hydrothermal systems at mid-ocean ridges [10-12]. Further, recent experiments by Fu et al. [13] focus on examining detailed C isotope measurements of hydrocarbons produced by surface-catalyzed mineral reactions. Work described in this paper details the experimental techniques used to measure intermediary organic reaction products (alcohols and organic acids).

Socki, Richard A.↗
NASA NTRS2016

Hydrogen Isotopic Composition of Apatite in Northwest Africa 7034: A Record of the "Intermediate" H-Isotopic Reservoir in the Martian Crust?

Northwest Africa (NWA) 7034 and its pairings comprise a regolith breccia with a basaltic bulk composition [1] that yields a better match than any other martian meteorite to visible-infrared reflectance spectra of the martian surface measured from orbit [2]. The composition of the fine-grained matrix within NWA 7034 bears a striking resemblance to the major element composition estimated for the martian crust, with several exceptions. The NWA 7034 matrix is depleted in Fe, Ti, and Cr and enriched in Al, Na, and P [3]. The differences in Al and Fe are the most substantial, but the Fe content of NWA 7034 matrix falls within the range reported for the southern highlands crust [6]. It was previously suggested by [4] that NWA 7034 was sourced from the southern highlands based on the ancient 4.4 Ga ages recorded in NWA 7034/7533 zircons [4, 5]. In addition, the NWA 7034 matrix material is enriched in incompatible trace elements by a factor of 1.2-1.5 [7] relative to estimates of the bulk martian crust. The La/Yb ratio of the bulk martian crust is estimated to be approximately 3 [7], and the La/Yb of the NWA 7034 matrix materials ranges from approximately 3.9 to 4.4 [3, 8], indicating a higher degree of LREE enrichment in the NWA 7034 matrix materials. This elevated La/Yb ratio and enrichment in incompatible lithophile trace elements is consistent with NWA 7034 representing a more geochemically enriched crustal terrain than is represented by the bulk martian crust, which would be expected if NWA 7034 represents the bulk crust from the southern highlands. Given the similarities between NWA 7034 and the martian crust, NWA 7034 may represent an important sample for constraining the composition of the martian crust, particularly the ancient highlands. In the present study, we seek to constrain the H isotopic composition of the martian crust using Cl-rich apatite in NWA 7034. Usui et al., [9] recently proposed that a H isotopic reservoir exists within the martian crust that has a H-isotopic composition that is intermediate (δD of 1000-2000per mille) between an isotopically light mantle (Delta D is less than 275per mille [10]) and an isotopically heavy atmosphere (δD of 2500-6100per mille [11, 12]). Apatites in NWA 7034 occur in a number of lithologic domains, however apatites across all lithologic domains have been affected by a Pb-loss event at about 1.5 Ga before present [5], so they are unlikely to have retained a primary composition and are more likely to have equilibrated with fluids within the martian crust that may or may not have exchanged with the martian atmosphere. Equilibration of apatite with crustal fluids is further supported by the chlorine-rich compositions exhibited by apatites in NWA 7034 in comparison to apatites from other martian meteorites (Figure 1; [13]). Cl is more hydrophilic than F, which promotes formation of Cl-rich apatite compositions in fluid-rich systems [e.g., 14, 15-17].

McCubbin, F. M.↗
NASA NTRS2017

Utilizing Stable Isotopes and Isotopic Anomalies to Study Early Solar System Formation Processes

Chondritic meteorites contain a diversity of particle components, i.e., chondrules and calcium-, aluminum-rich refractory inclusions (CAIs), that have survived since the formation of the Solar System. The chemical and isotopic compositions of these materials provide a record of the conditions present in the protoplanetary disk where they formed and can aid our understanding of the processes and reservoirs in which solids formed in the solar nebula, an important step leading to the accretion of planetesimals. Isotopic anomalies associated with nucleosynthetic processes are observed in these discrete materials, and can be compared to astronomical observations and astrophysical formation models of stars and more recently proplyds. The existence and size of these isotopic anomalies are typically thought to reflect a significant state of isotopic heterogeneity in the earliest Solar System, likely left over from molecular cloud heterogeneities on the grain scale, but some could also be due to late stellar injection. The homogenization of these isotopic anomalies towards planetary values can be used to track the efficiency and timescales of disk wide mixing,

Simon, Justin↗
DOE OSTI2024

A common isotopic reservoir for amoeboid olivine aggregates (AOAs) and calcium-aluminum-rich inclusions (CAIs) revealed by Ti and Cr isotopic compositions

Amoeboid olivine aggregates (AOAs) are the most abundant type of refractory inclusions found in most carbonaceous chondrite groups. AOAs are thought to be genetically related to calcium-aluminum-rich inclusions (CAIs) and potential chondrule precursor components, although the precise physical and temporal details of AOA formation and their relationship to other chondritic components remain unclear. In this study, we measured the chromium and titanium isotopic compositions of eight AOAs from four different CV chondrites with the goal of evaluating potential genetic links between AOAs, CAIs, and chondrules. These are the first Cr and Ti isotopic data reported beyond a single AOA previously measured for Cr and a different single AOA previously measured for Ti. The results presented here show that the ε 54 Cr and ε 50 Ti isotopic compositions of AOAs are indistinguishable from those of CAIs, suggesting that AOAs and CAIs formed from a common region of the disk. Here, we also demonstrate, based on the comparison of the Cr and Ti isotopic composition of AOAs to previously measured chondrules, that mixing between AOAs and an NC compositional endmember alone cannot fully explain the range of measured chondrule compositions. Although AOAs may have been important chondrule precursor components along with AOA olivine, CAIs, fragments of earlier generation chondrules, and fine-grained matrix material, this observation requires another currently unknown component to be involved in chondrule formation.

58 GEOSCIENCES↗
DOE OSTI2022

U–Pb Geochronology and Stable Isotope Geochemistry of Terrestrial Carbonates, Lower Cretaceous Cedar Mountain Formation, Utah: Implications for Synchronicity of Terrestrial and Marine Carbon Isotope Excursions

The terrestrial Lower Cretaceous Cedar Mountain Formation, Utah, is a critical archive of paleoclimate, tectonics, and vertebrate ecology and evolution. Early Cretaceous carbon cycle perturbations associated with ocean anoxia have been interpreted from this succession, as expressed in stable carbon isotopes. However, refining the timing of the observed stable isotope excursions remains a key challenge in understanding how marine anoxia affects the Earth system, and is ultimately recorded in the terrestrial realm. The geochronology and geochemistry of a terrestrial carbonate near the base of this succession, which potentially records the Ap7 global carbon isotope excursion, is studied here. Petrographic and geochemical analyses are used to test plausible mechanisms for U incorporation into the calcite lattice in this sample. Using these methods, the hypothesis that the incorporation of U was at or close to the timing of carbonate precipitation is evaluated. U–Pb geochronology of calcite indicates a plausible Early Cretaceous age. However, comparison of the new U–Pb ages of calcite with detrital zircon maximum depositional ages immediately beneath the studied sample indicates a disparity in the apparent sedimentation rates if both types of geochronologic information are interpreted as reflecting the timing of sediment deposition. The totality of data supports an early, and high-temperature, diagenetic timing of U incorporation, with potential for minor leaching of U in subsequent fluid–rock interaction. The most likely mechanism for U transport and immobilization in these samples is hydrothermal fluid–rock interaction. Therefore, the radiometric ages, and corresponding stable isotope composition of U-bearing carbonate domains in this sample, indicate early subsurface fluid–rock interactions and not a record of atmosphere–soil geochemical reactions.

36 MATERIALS SCIENCE↗
DOE OSTI2023

CO 2 electroreduction favors carbon isotope 12 C over 13 C and facilitates isotope separation

We discovered that CO 2 electroreduction strongly favors the conversion of the dominant isotope of carbon ( 12 C) and discriminates against the less abundant, stable carbon 13 C isotope. Both absorption of CO 2 in the alkaline electrolyte and CO 2 electrochemical reduction favor the lighter isotopologue. As a result, the stream of unreacted CO 2 leaving the electrolyzer has an increased 13 C content, and the depletion of 13 C in the product is several times greater than that of photosynthesis. Using a natural abundance feed, we demonstrate enriching of the 13 C fraction to ~1.3% (i.e., +18%) in a single-pass reactor and propose a scalable and economically attractive process to yield isotopes of a commercial purity. Our finding opens pathways to both cheaper and less energy-intensive production of stable isotopes ( 13 C, 15 N) essential to the healthcare and chemistry research, and to an economically viable, disruptive application of electrolysis technologies developed in the context of sustainability transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Using Median Point in Keeling Plot to Reduce the Uncertainty of the Isotopic Composition of Evapotranspiration

Abstract The isotopic composition of evapotranspirationδ ET is a crucial parameter in isotope-based evapotranspiration (ET) partitioning and moisture recycling studies. The Keeling plot method is the most prevalent method to calculateδ ET , though it contains large extrapolated uncertainties from the least squares regression. Traditional Keeling regression uses the mean point of individual measurements. Here, a modified Keeling plot framework was proposed using the median point of individual measurements. We tested theδ ET uncertainty using the mean point [σ ET (mean)] and median point [σ ET (median)]. Multiple resolutions of input and output data from six independent sites were used to test the performance of the two methods. Theσ ET (mean) would be greater thanσ ET (median) when the mean value of inverse vapor concentration () is greater than the median value of inverse vapor concentration []. When applying the filter ofr 2 > 0.8, around 70% ofσ ET (mean) was greater thanσ ET (median). This phenomenon might be due to the normality of the vapor concentrationC υ producing the asymmetric distribution of 1/C υ . The median method could perform significantly better than the mean method when inputting high-resolution measurements (e.g., 1 Hz) and when the water vapor concentrationC υ is relatively low. Compared to the mean method, applying the median method could on average reduce 6.88% of ET partitioning uncertainties and could on average reduce 9.00% of moisture recycling uncertainties. This study provided a new insight of the Keeling plot method and emphasized handling model output uncertainty from multiple perspectives instead of only from input parameters.

Meteorology & Atmospheric Sciences↗
NASA NTRS1989

Nitrogen isotopes in drive tube 79002/79001 - Regolith history and nitrogen isotopic evolution in the solar wind

Variations in abundance and isotopic composition of nitrogen in 79002/79001 drive tube samples result from mixing of two soil components: one mature, N-rich, and isotopically light, resembling breccia material in the core, and the other immature, N-poor, and isotopically heavy. That these materials are common to soil at each stratigraphic level in the core suggests widespread distribution in the local regolith. Preservation of mixing correlations involving nitrogen isotopic compositions and cosmogenic N-15 concentrations suggests relatively recent mixing, perhaps in association with emplacement of the core stratigraphy. Characteristics of nitrogen release from the endmember materials, relationships between their nitrogen contents and maturity, and contrasts in their cosmogenic N-15 contents are consistent with models involving secular increase of the N-15/N-14 ratio of the solar wind.

Stone, J.↗
DOE OSTI2020

Hyperfine structures and isotopic shifts of uranium transitions using tunable laser spectroscopy of laser ablation plumes

We report isotopic shifts and hyperfine structures of selected U transitions employing tunable spectroscopy viz: laser-induced fluorescence and laser absorption spectroscopy of laser ablation plumes. The laser-produced plasmas were produced during ns laser ablation on a natural U metal which contains 0.7% 235U. Our results show that isotopic shifts between 238U and 235U are entangled with hyperfine structures of 235U. The isotopic ratio obtained using laser-induced fluorescence is affected by optical saturation effect. Time-resolved laser absorption spectroscopy is carried out for evaluating the optical absorption and estimating the hyperfine constants.

(020.3260) Isotope shifts↗
DOE OSTI2021

Carbonate clumped isotope analysis (Δ 47 ) of 21 carbonate standards determined via gas‐source isotope‐ratio mass spectrometry on four instrumental configurations using carbonate‐based standardization and multiyear data sets

Rationale Clumped isotope geochemistry examines the pairing or clumping of heavy isotopes in molecules and provides information about the thermodynamic and kinetic controls on their formation. The first clumped isotope measurements of carbonate minerals were first published 15 years ago, and since then, interlaboratory offsets have been observed, and laboratory and community practices for measurement, data analysis, and instrumentation have evolved. Here we briefly review historical and recent developments for measurements, share Tripati Lab practices for four different instrument configurations, test a recently published proposal for carbonate‐based standardization on multiple instruments using multi‐year data sets, and report values for 21 different carbonate standards that allow for recalculations of previously published data sets. Methods We examine data from 4628 standard measurements on Thermo MAT 253 and Nu Perspective IS mass spectrometers, using a common acid bath (90°C) and small‐sample (70°C) individual reaction vessels. Each configuration was investigated by treating some standards as anchors (working standards) and the remainder as unknowns (consistency standards). Results We show that different acid digestion systems and mass spectrometer models yield indistinguishable results when instrument drift is well characterized. For linearity correction, mixed gas‐and‐carbonate standardization or carbonate‐only standardization yields similar results. No difference is observed in the use of three or eight working standards for the construction of transfer functions. Conclusions We show that all configurations yield similar results if instrument drift is robustly characterized and validate a recent proposal for carbonate‐based standardization using large multiyear data sets. Δ 47 values are reported for 21 carbonate standards on both the absolute reference frame (ARF; also refered to as the Carbon Dioxide Equilibrated Scale or CDES) and the new InterCarb‐Carbon Dioxide Equilibrium Scale (I‐CDES) reference frame, facilitating intercomparison of data from a diversity of labs and instrument configurations and restandardization of a broad range of sample sets between 2006, when the first carbonate measurements were published, and the present.

58 GEOSCIENCES↗
DOE OSTI2023

Quantification and purification of isotopic contamination at the ReAccelerator of the Facility for Rare Isotope Beams

At the ReAccelerator within the Facility for Rare Isotope Beams, a combination of an interchangeable aluminum foil and a silicon detector was developed to quantify isobaric contamination in rare isotope beams. The device is simple to operate and is now used routinely. In this article, we describe the system and show an application of the device to determine the level of contamination of an Si-32 rare isotope beam by stable S-32. In addition, we describe how the new diagnostic device helped confirm an enhancement of the beam purity prior to beam delivery to experiments.

Instruments & Instrumentation↗
DOE OSTI2024

Acceleration of uranium beam to record power of 10.4 kW and observation of new isotopes at Facility for Rare Isotope Beams

The Facility for Rare Isotope Beams (FRIB) is a major nuclear physics facility for research with fast, stopped, and reaccelerated beams that was successfully commissioned in May 2022. A key capability of FRIB is the production of an acceleration of the uranium beam, but this capability requires the facility to work at the design limits of the lowest charge-to-mass ratio and the highest power density on the beam intercepting devices. This paper presents techniques for overcoming the significant challenges in accelerating the uranium beam, culminating in the demonstration of 10.4 kW on target, and the discovery of three new isotopes. The high-power uranium beam enabled us to produce and identify G 88 a , A 93 s , and S 96 e , within the first 24 h of operation. The successful uranium operation at FRIB sets a new record for accelerated uranium beam power above 10 kW and opens a new avenue of research with rare isotopes. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗
NASA NTRS1986

A non-mass-dependent oxygen isotope effect in the production of ozone from molecular oxygen - The role of molecular symmetry in isotope chemistry

It was previously reported that the reaction products from the synthesis of ozone in an electric discharge through molecular oxygen display a nonmass-dependent (NoMaDic) oxygen isotope effect. In this paper, a detailed characterization of the isotope effect, including the effect of molecular oxygen pressure, and the presence of a chemically inert third body (helium), is reported. The NoMaDic effect is due to an isotopically selective stabilization of the O3 formation reaction intermediate, possibly resulting from the ability of the different isotopomers to exhibit different molecular symmetries.

Heidenreich, J. E., III↗