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All sourcesNASA NTRSDOE OSTI
NASA NTRS1991

Isotopic composition of Murchison organic compounds: Intramolecular carbon isotope fractionation of acetic acid. Simulation studies of cosmochemical organic syntheses

Recently, in our laboratories, samples of Murchison acetic acid were decarboxylated successfully and the carbon isotopic composition was measured for the methane released by this procedure. These analyses showed significant differences in C-13/C-12 ratios for the methyl and carboxyl carbons of the acetic acid molecule, strongly suggesting that more than one carbon source may be involved in the synthesis of the Murchison organic compounds. On the basis of this finding, laboratory model systems simulating cosmochemical synthesis are being studied, especially those processes capable of involving two or more starting carbon sources.

Yuen, G. U.↗
DOE OSTI2025

Natural isotopic compositions of titanium, iron, and nickel observed in commercial fuel pellets – Promising candidate elements for stable isotope tagging

Stable isotope taggants would constitute unique identifiers for nuclear fuel cycle materials, resulting in expedited timelines and high confidence provenance assessments for nuclear forensics investigations. However, reliably identifying and interpreting stable isotope taggants in nuclear materials recovered from outside of regulatory control will largely be predicated on the assumption that the taggant element intrinsic to the untagged nuclear material exhibits natural isotopic ratios. Here, we present high-precision Ti, Fe, and Ni isotope compositions in 13 commercial low-enriched uranium (LEU) fuel pellets to assess the suitability of these transition metals as stable isotope taggants. Our investigations reveal limited isotope variations among the fuel pellets in all three elements, which are consistent with small mass-dependent isotope fractionations, comparable to variations previously reported for natural samples. In practice, isotopically tagged nuclear materials are expected to fall along isotopic mixing lines, since intrinsic background levels of taggant elements dilute the taggant towards natural isotope compositions. Furthermore, the observation that Ti, Fe, and Ni isotope compositions in a suite of LEU fuel pellets are close to or indistinguishable from estimates for the Bulk Silicate Earth demonstrates that a two end-member mixing assumption would be valid for these transition metals, indicating that all three are promising candidate elements for stable isotope tagging. Finally, we present mass balance calculations to quantify isotopic perturbations expected from admixing isotopically anomalous Ti, Fe, and Ni taggants to assess the interplay between elemental and taggant concentrations and find favorable compromises for facilitating successful taggant identification with current analytical methods.

Intentional forensics↗
NASA NTRS2023

The Magnesium Isotope Composition of Samples Returned From Asteroid Ryugu

The nucleosynthetic isotope composition of planetary materials provides a record of the heterogeneous distribution of stardust within the early solar system. In 2020 December, the Japan Aerospace Exploration Agency Hayabusa2 spacecraft returned to Earth the first samples of a primitive asteroid, namely, the Cb-type asteroid Ryugu. This provides a unique opportunity to explore the kinship between primitive asteroids and carbonaceous chondrites. We report high-precision μ 26 Mg* and μ 25 Mg values of Ryugu samples together with those of CI, CM, CV, and ungrouped carbonaceous chondrites. The stable Mg isotope composition of Ryugu aliquots defines μ 25 Mg values ranging from –160 ± 20 ppm to –272 ± 30 ppm, which extends to lighter compositions relative to Ivuna-type (CI) and other carbonaceous chondrite groups. We interpret the μ 25 Mg variability as reflecting heterogeneous sampling of a carbonate phase hosting isotopically light Mg (μ 25 Mg ∼ –1400 ppm) formed by low temperature equilibrium processes. After correcting for this effect, Ryugu samples return homogeneous μ 26 Mg* values corresponding to a weighted mean of 7.1 ± 0.8 ppm. Thus, Ryugu defines a μ 26 Mg* excess relative to the CI and CR chondrite reservoirs corresponding to 3.8 ± 1.1 and 11.9 ± 0.8 ppm, respectively. These variations cannot be accounted for by in situ decay of 26 Al given their respective 27 Al/ 24 Mg ratios. Instead, it requires that Ryugu and the CI and CR parent bodies formed from material with a different initial 26 Al/ 27 Al ratio or that they are sourced from material with distinct Mg isotope compositions. Thus, our new Mg isotope data challenge the notion that Ryugu and CI chondrites share a common nucleosynthetic heritage.

Solar system evolution↗
DOE OSTI2021

The gallium isotopic composition of the Moon

Here, in this study, we present new Ga isotope data from a suite of 28 mare basalts and lunar highland rocks. The δ 71 Ga values of these samples range from -0.10 to +0.66‰ (where δ 71 Ga is the relative difference between the 71 Ga/ 69 Ga ratio of a sample and the Ga-IPGP standard), which is an order of magnitude more heterogeneous than δ 71 Ga values in terrestrial magmatic rocks. The cause of this isotopic heterogeneity must be established to estimate the bulk δ 71 Ga value of the Moon. In general, low-Ti basalts and ferroan anorthosite suite (FAS) rocks have δ 71 Ga values that are lower than high-Ti basalts and KREEP-rich rocks. The observation that rocks derived from later forming LMO cumulates have higher δ 71 Ga values suggests that Ga isotopes are fractionated by processes that operate within the chemically evolving LMO, rather than localized degassing or volatile redistribution. Correlations between indices of plagioclase removal from the LMO (e.g. Eu/Eu*) with Ga isotope ratios suggest that a Δ 71 Ga plagioclase-melt of -0.3‰, (where Δ 71 Ga plagioclase-melt is the isotopic fractionation associated with crystallization of plagioclase from a melt), could drive the observed isotopic fractionation in high-Ti mare basalts and KREEP-rich rocks. This would be consistent with the observation that FAS rocks have δ 71 Ga values that are lower than mare basalts. However, the addition of KREEP-like material into the mare basalt source regions would not contribute enough Ga to perturb the isotopic composition outside of analytical uncertainty. Thus, basalts derived from early formed LMO cumulates such as those from Apollo 15, would preserve light Ga isotopic compositions despite containing modest amounts of urKREEP. We estimate that the δ 71 Ga value of the LMO was ~0.14‰ prior to the onset of plagioclase crystallization and extraction. Whether this δ 71 Ga value is representative of the initial BSM cannot be ascertained from the current dataset. It remains plausible that the Moon accreted with a heavier Ga isotopic composition than the Earth. Alternatively, the Moon and Earth could have accreted with similar isotopic compositions (BSE = 0.00 ± 0.06‰, Kato et al., 2017) and volatile loss drove the LMO to higher δ 71 Ga values prior to formation of the lunar crust.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2001

In-Situ Oxygen Isotopic Composition of Tagish Lake: An Ungrouped Type 2 Carbonaceous Chondrite

We have measured the oxygen isotopic composition of several components of Tagish Lake by ion microprobe. This meteorite constitutes the best preserved sample of C2 matter presently available for study. It presents two different lithologies (carbonate-poor and -rich) which have fairly comparable oxygen isotopic composition, with regard to both the primary or secondary minerals. For the olivine and pyroxene grains, their delta O-18 values range from - 10.5% to + 7.4% in the carbonate-poor lithology, with a mean Delta O-17 value of - 3.7 2.4%. In the carbonate-rich lithology, delta O-18 varies from - 7.9% to + 3.3%, and the mean Delta O-17 value is - 4.7 +/- 1.4%. Olivine inclusions (Fo(sub >99)) with extreme O-16-enrichment were found in both lithologies: delta O-18 = - 46.1 %, delta O-187= - 48.3% and delta O-18 = - 40.6%, delta O-17 = - 41.2% in the carbonate-rich lithology; delta O-18 = - 41.5%, delta O-17 = -43.4%0 in the carbonate-poor lithology. Anhydrous minerals in the carbonate-poor lithology are slightly more O-16-rich than in the carbonate-rich one. Four low-iron manganese-rich (LIME) olivine grains do not have an oxygen isotopic composition distinct from the other "normal" olivines. The phyllosilicate matrix presents the same range of oxygen isotopic compositions in both lithologies: delta O-18 from approximately 11 % to approximately 6%, with an average Delta. O-17 approximately 0%. Because the bulk Tagish Lake oxygen isotopic composition given by Brown et al. is on the high end of our matrix analyses, we assume that this "bulk Tagish Lake" composition probably only represents that of the carbonate-rich lithology. Calcium carbonates have delta O-18 values up to 35%, with Delta O-17 approximately 0.5%0. Magnetite grains present very high Delta O-17 values approximately + 3.4%0 +/- 1.2%. Given our analytical uncertainties and our limited carbonate data, the matrix and the carbonate seem to have formed in isotopic equilibrium. In that case, their large isotopic fractionation would argue for a low temperature (CM-like, T approximately 0 deg) formation. Magnetite probably formed during a separate event. Tagish Lake magnetite data is surprisingly compatible with that of R-chondrites and unequilibrated ordinary (LL3) chondrites. Our oxygen isotope data strongly supports the hypothesis of a single precursor for both lithologies. Drastic mineralogical changes between the two lithologies not being accompanied with isotopic fractionation seem compatible with the alteration model presented by Young et aI. Tagish Lake probably represents the first well preserved large sample of the C2 matter that dominates interplanetary matter since the formation of the solar system.

Zolensky, Michael E.↗
NASA NTRS2004

Variations in Urine Calcium Isotope: Composition Reflect Changes in Bone Mineral Balance in Humans

Changes in bone mineral balance cause rapid and systematic changes in the calcium isotope composition of human urine. Urine from subjects in a 17 week bed rest study was analyzed for calcium isotopic composition. Comparison of isotopic data with measurements of bone mineral density and metabolic markers of bone metabolism indicates the calcium isotope composition of urine reflects changes in bone mineral balance. Urine calcium isotope composition probably is affected by both bone metabolism and renal processes. Calcium isotope. analysis of urine and other tissues may provide information on bone mineral balance that is in important respects better than that available from other techniques, and illustrates the usefulness of applying geochemical techniques to biomedical problems.

Skulan, Joseph↗
NASA NTRS2003

Molybdenum Isotopic Composition of Iron Meteorites, Chondrites and Refractory Inclusions

Recent Mo isotopic studies of meteorites reported evidence for differences in isotopic compositions for whole rocks of some primitive and differentiated meteorites relative to terrestrial materials. Enrichments of r- and p-process isotopes of up to 3-4 units (e unit = parts in 10(exp 4) over s-process dominated isotopes are the most prominent features. Certain types of presolar grains show large enrichments in s-process isotopes, however, it was concluded on grounds of mass balance that incomplete digestion of such grains cannot explain the enrichments of r- and p-process isotopes in whole rocks of primitive chondrites. If the reported variability in r- and p-process isotope enrichments reflects the true isotopic characteristics of the whole rocks, the implications are quite profound. It would suggest the presence of large scale Mo isotopic heterogeneity within the solar accretion disk with likely collateral effects for other elements. However, such effects were not found for Ru isotopes, nor for Zr isotopes. Another recent Mo isotopic study by multi collector ICP-MS could not confirm the reported deviations in Allende, Murchison or iron meteorites. Here, we present new results for the Mo isotopic composition of iron meteorites, chondrites and CAIs obtained by negative thermal ionization mass spectrometry (NTIMS). We discuss analytical aspects and the homogeneity of Mo isotopic compositions in solar system materials.

Becker, H.↗
DOE OSTI2020

Factors controlling the oxygen isotopic composition of lacustrine authigenic carbonates in Western China: implications for paleoclimate reconstructions

Abstract In the carbonate-water system, at equilibrium, the oxygen isotopic composition of carbonate is dependent not only on the temperature but also on the isotopic composition of host water in which the carbonate is formed. In this study, lake surface sediment and water samples were collected from 33 terminal lakes in Western China to evaluate controls on the oxygen isotopic composition of lacustrine authigenic carbonates (δ 18 O carb ) and its spatial distribution. Our results show that water oxygen isotopic composition (δ 18 O water ) rather than lake summer water temperature (T water ), is the main determinant of δ 18 O carb , irrespective of whether oxygen isotope equilibrium is achieved. There are significant linear correlations between δ 18 O carb and elevation, as well as that between δ 18 O carb and latitude for lakes located on the Tibetan Plateau. In Western China, the spatial distribution of δ 18 O carb is consistent with that of δ 18 O water , and is ultimately controlled by the isotopic composition of local precipitation (δ 18 O precipitation ) that depends on the source of water vapor. Therefore, changes in δ 18 O carb can be predominantly interpreted as variations of δ 18 O water , which in turn represent changes in δ 18 O precipitation for paleoclimate reconstructions in this region, and may be relevant to studies of other areas.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1979

The isotopic composition of Nd in different ocean masses

The paper examines the isotopic composition of Nd in marine environments. The Sm-Nd data for authigenic ferromanganese sediments indicate that the Atlantic, Pacific, and Indian Oceans have a distinct range in Nd isotopic composition characteristics of each ocean basin and reflect the dissolved load of Nd in the water mass. Measurements of the Nd isotopic seawater composition of seawater indicate that the rare earth elements (REE) in ferromanganese sediments are derived by direct precipitation of these elements out of seawater. It is believed that the Nd isotopic variations in these sediments represent true variations in the dissolved Nd isotopic composition which reflect the age and (Sm-147)/(Nd-144) ratios of the continental masses sampled believed to be the major source of REE in seawater.

Piepgras, D. J.↗
NASA NTRS1991

Isotopic compositions of carbonates and organic carbon from upper Proterozoic successions in Namibia: stratigraphic variation and the effects of diagenesis and metamorphism

The carbon isotope geochemistry of carbonates and organic carbon in the late Proterozoic Damara Supergroup of Namibia, including the Nama, Witvlei, and Gariep groups on the Kalahari Craton and the Mulden and Otavi groups on the Congo Craton, has been investigated as an extension of previous studies of secular variations in the isotopic composition of late Proterozoic seawater. Subsamples of microspar and dolomicrospar were determined, through petrographic and cathodoluminescence examination, to represent the "least-altered" portions of the rock. Carbon-isotopic abundances in these phases are nearly equal to those in total carbonate, suggesting that 13C abundances of late Proterozoic fine-grained carbonates have not been significantly altered by meteoric diagenesis, although 18O abundances often differ significantly. Reduced and variable carbon-isotopic differences between carbonates and organic carbon in these sediments indicate that isotopic compositions of organic carbon have been altered significantly by thermal and deformational processes, likely associated with the Pan-African Orogeny. Distinctive stratigraphic patterns of secular variation, similar to those noted in other, widely separated late Proterozoic basins, are found in carbon-isotopic compositions of carbonates from the Nama and Otavi groups. For example, in Nama Group carbonates delta 13C values rise dramatically from -4 to +5% within a short stratigraphic interval. This excursion suggests correlation with similar excursions noted in Ediacaran-aged successions of Siberia, India, and China. Enrichment of 13C (delta 13C> +5%) in Otavi Group carbonates reflects those in Upper Riphean successions of the Akademikerbreen Group, Svalbard, its correlatives in East Greenland, and the Shaler Group, northwest Canada. The widespread distribution of successions with comparable isotopic signatures supports hypotheses that variations in delta 13C reflect global changes in the isotopic composition of late Proterozoic seawater. Within the Damara basin, carbon-isotopic compositions of carbonates provide a potentially useful tool for the correlation of units between the Kalahari and Congo cratons. Carbonates depleted in 13C were deposited during and immediately following three separate glacial episodes in Namibia. The correspondence between ice ages and negative delta 13C excursions may reflect the effects of lowered sea levels; enhanced circulation of deep, cold, O2-rich seawater; and/or the upwelling of 13C-depleted deep water. Iron-formation is additionally associated with one of the glacial horizons, the Chuos tillite. Carbon-13 enriched isotopic abundances in immediately pre-glacial carbonates suggest that oceanographic conditions favored high rates of organic burial. It is likely that marine waters were stratified, with deep waters anoxic. A prolonged period of ocean stratification would permit the build-up of ferrous iron, probably from hydrothermal sources. At the onset of glaciation, upwelling would have brought 13C-depleted and iron-rich deep water onto shallow shelves where contact with cold, oxygenated surface waters led to the precipitation of ferric iron.

NASA Program Exobiology↗
NASA NTRS2021

Mineralogy, Petrology, and Oxygen-isotope Compositions of Magnetite ± Fayalite Assemblages in CO3, CV3, and LL3 Chondrites

We report on the mineralogy, petrology, and O-isotope compositions of magnetite and fayalite (Fa90−100) from several metasomatically altered and weakly metamorphosed carbonaceous (Y-81020 [CO3.05], EET 90043 [CO3.1], MAC 88107 [CO3.1-like], and Kaba [oxidized Bali-like CV3.1]) and unequilibrated ordinary chondrites (UOCs; Semarkona [LL3.00], MET 00452 [LL3.05], MET 96503 [LL3.05], EET 910161 [LL3.05], Ngawi [LL3.0−3.6 breccia], and Vicencia [LL3.2]). In MAC 88107, EET 90043, and Kaba, nearly pure fayalite (Fa98−100) associates with phyllosilicates, magnetite, Fe, Ni-sulfides, and hedenbergite (Fs~50Wo~50), and occurs in all chondritic components—chondrules, matrices,and refractory inclusions. In UOCs, nearly pure fayalite (Fa95−98) associates withphyllosilicates and magnetite, and occurs mainly in matrices and fine-grained chondrulerims. Oxygen-isotope compositions of fayalite and magnetite in UOCs, COs, CVs, and MAC 88107 are in disequilibrium with those of chondrule olivine and low-Ca pyroxene phenocrysts, and plot along mass-dependent fractionation lines with slope of~0.5, butdifferent 17O (~+4.3 1.4‰,−0.2 0.6‰,−1.5 1‰, and−1.8 0.8‰, respectively). Based on the mineralogical observations, thermodynamic analysis, O-isotope compositions, and recently reported experimental data, we infer that (1) fayalite and magnetite in COs,CVs, MAC 88107, and UOCs resulted from aqueous fluid–rock interaction on the chondrite parent asteroids that occurred at low local water-to-rock mass ratios (0.1−0.4) and elevated temperatures (~100−300°C), and (2) 17O of fayalite and magnetite reflects O-isotope compositions of aqueous fluids on the host meteorite parent bodies. The observed differences in 17O of fayalite–magnetite assemblages in UOCs, CVs, COs, and MAC 88107suggest that water ices that accreted into the ordinary chondrite and carbonaceous chondrite parent asteroids had different 17O, implying spatial and/or temporal variations in O-isotope compositions of water in the protoplanetary disk.

Alexander N Krot↗
NASA NTRS2002

Sulfur Isotope Composition of Putative Primary Troilite in Chondrules

Sulfur isotope compositions of putative primary troilites in chondrules from Bishunpur were measured by ion probe. These primary troilites have the same S isotope compositions as matrix troilites and thus appear to be isotopically unfractionated. Additional information is contained in the original extended abstract.

Tachibana, Shogo↗
NASA NTRS1994

Chemical production of chondrule oxygen isotopic composition

Defining the source of observed meteoritic O isotopic anomalies remains a fundamental challenge. The O isotopic composition of chondrules are particularly striking. There are at least three types of chemical processes that produce the isotopic compositions observed in chondrules and Ca-Al-rich inclusions (CAI's). The processes are rather general, viz, they require no specialized processes and the processes associated with chondrule production are likely to produce the observed compositions.

Thiemens, M. H.↗
NASA NTRS1974

The charge and isotopic composition of solar cosmic rays

The charge and isotopic composition of solar cosmic rays potentially contain a wealth of information on the acceleration and confinement of energetic particles at the sun. As the experimental techniques have improved and with the increasing number of measurements, this potential is now being realized. It is convenient to divide the composition studies into three areas: (1) helium-iron, with energies above 10 MeV per nuc; (2) helium-iron, and the trans-iron elements, with energies below 2 MeV per nuc; (3) the isotopic composition. In the first area at energies above 10 MeV per nuc, the solar cosmic rays appear to provide a representative sample of the solar corona. At lower energies complex enhancement effects are noted. These increase with Z and decrease with energy.

Mcdonald, F. B.↗
NASA NTRS1987

The effect of the isotopic composition of oxygen on the non-mass-dependent isotopic fractionation in the formation of ozone by discharge of O2

Isotopic fractionation processes in the formation of O3 by 20-kV 60-kHz discharge of O2 in a fused silica container at 77 K are investigated experimentally, with a focus on the effects of changes in the isotopic composition of O2, the O2 pressure, the degree of O3 formation, and the discharge geometry on the isotope abundances in the postdischarge O2 and O3. The results are presented in tables and graphs and compared with the predictions of theoretical models involving vibrational anharmonicity and symmetry effects on O3 predissociation. In experiments using O2 enriched with O-17 and O-18, the heavy isotope is enriched in the residual O2 and not in the O3, whereas the opposite is true when atmospheric isotope abundances are used. It is inferred that the predissociation rate depends on the symmetry and mass of the O3 molecules and not on self-shielding or symmetry effects in the reactant O2. The potential value of the present findings for studies of anomalous isotope abundances in meteorites is indicated.

Yang, Jongmann↗
NASA NTRS1978

Measurements of the isotopic composition of cosmic-ray nuclei with Z=10-14

Measurements are reported of the isotopic composition of cosmic-ray nuclei with Z=10-14 using a Cerenkov x total energy technique. These measurements are for an energy interval 40-120 MeV/nuc at a typical energy of about 500 MeV/nuc at the top of the atmosphere. The mass resolution sigma varies between 0.4 and 0.5 AMU in this charge range. A total of about 450 events are analyzed for their isotopic composition. These studies indicate that the isotopic composition of these elements at the source must be very similar to the known solar abundances.

Simpson, G. A.↗
DOE OSTI2024

The distinct conditions of atmospheric and underground nuclear tests revealed by Zn isotopic compositions of nuclear debris samples

We analyzed the Zn isotopic compositions of nuclear debris samples from atmospheric and underground nuclear tests. Samples from the site of atmospheric tests exhibit a range of Zn isotopic fractionation (δ 66 Zn JMC-Lyon = 0.23–0.86 ‰) while samples from underground tests exhibit Zn isotopic compositions with minimal variation among samples and from terrestrial igneous rock standards (δ 66 ZnJMC-Lyon = 0.28–0.39 ‰). In conclusion, the larger range of δ 66 Zn JMC-Lyon observed in atmospheric test samples relative to underground test samples is likely the result of the open system characteristics of atmospheric nuclear tests and the closed system characteristics of underground nuclear tests.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗