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All sourcesNASA NTRSDOE OSTI
NASA NTRS2000

Amino Acid Chemistry as a Link Between Small Solar System Bodies and Carbonaceous Chondrites

Establishing chemical links between meteorites and small solar system bodies, such as comets and asteroids, provides a tool for investigating the processes that occurred during the formation of the solar system. Carbonaceous meteorites are of particular interest, since they may have seeded the early Earth with a variety of prebiotic organic compounds including amino acids, purines and pyrimidines, which are thought to be necessary for the origin of life. Here we report the results of high-performance liquid chromatography (HPLC) based amino acid analyses of the acid-hydrolyzed hot water extracts from pristine interior pieces of the CI carbonaceous chondrites Orgueil and Ivuna and the CM meteorites Murchison and Murray. We found that the CI meteorites Orgueil and Ivuna contained high abundances of beta-alanine and glycine, while only traces of other amino acids like alanine, alpha-amino-n-butryic acid (ABA) and alpha-aminoisobutyric acid (AIB) were detected in these meteorites. Carbon isotopic measurements of beta-alanine and glycine in Orgueil by gas chromatography combustion-isotope ratio mass spectrometry clearly indicate an extraterrestrial origin of these amino acids. The amino acid composition of Orgueil and Ivuna was strikingly different from the CM chondrites Murchison and Murray. The most notable difference was the high relative abundance of B-alanine in Orgueil and Ivuna compared to Murchison and Murray. Furthermore, AIB, which is one of the most abundant amino acids found in Murchison and Murray, was present in only trace amounts in Orgueil and Ivuna. Our amino acid data strongly suggest that the CI meteorites Orgueil and Ivuna came from a different type of parent body than the CM meteorites Murchison and Murray, possibly from an extinct comet. It is generally thought that carbonaceous meteorites are fragments of larger asteroidal bodies delivered via near Earth objects (NEO). Orbital and dynamic studies suggest that both fragments of main belt asteroids and comets replenish the NEO population, therefore extinct comets may contribute up to half of all NEO's. A comparison of an amino acid analysis of a returned NEO sample to CI and CM carbonaceous chondrites would help establish a link between small solar system bodies and meteorites. Based on our amino acid measurements of CI and CM chondrites, amino acid chemistry can be included as an additional set of criteria to constrain the nature of meteorite parent bodies.

Glavin, Daniel P.↗
NASA NTRS2022

Calcium Isotope Constraints on Recycled Carbonates in Subduction-related Magmas

Calcium isotope ratios are readily mass-fractionated by low-temperature depositional processes that can be recorded in sedimentary rocks and, therefore, have the potential to track distinct geochemical signatures of recycled materials in mantle-derived igneous rocks. In this study, I report calcium isotopic compositions for well-characterized lavas from the Central American volcanic arc that exhibit a range of trace element and radiogenic isotope signatures that have been used to indicate variable amounts of subducted marine carbonate and hemipelagic sedimentary rocks, fresh carbonatite lavas from Oldoinyo Lengai Volcano, Tanzania, and an intrusive carbonatite clast erupted 12.8 ka from the Laacher See Volcano, Germany. I observed no calcium isotope evidence for recycled sedimentary rocks in the Central American arc magmas or in the Oldoinyo Lengai carbonatite volcanic rocks. They all exhibit isotopic compositions similar to rocks dominated by a primitive, mantle-like, bulk silicate Earth (BSE) composition. The exception in this work is the calcium isotope composition measured in the intrusive Laacher See carbonatite that is resolvable from BSE (δ^44 Ca = 0.0). Although this calcium isotopic signature might be related to ancient carbonate recycling, the magnitude and relatively light calcium isotopic composition (δ^44 Ca = –0.4) of this carbonatite could also reflect an origin that involved partial melting of altered lithospheric mantle, from which isotopically heavy Ca-bearing fluids have been lost. The decoupled signatures between trace elements and their radiogenic isotopes and those recorded by calcium isotope data are important because they likely reflect different sources and processes, and demonstrate that sediment subduction is not a bulk mixing process.

Ca isotopes↗
DOE OSTI2023

Characterization of actinide abundances and isotopic compositions by HR-ICP-MS. Part 2: Results from actinide doping studies

Previously, we presented actinide isotopic and elemental data from fallout melt glass that was measured using high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS). Direct comparison between these measurements and ‘gold standard’ data obtained by multi-collector ICP-MS showed broad overlap, indicating that HR-ICP-MS is a potentially valuable technique for producing actinide elemental and isotopic data on a relatively rapid timescale. To test the usefulness of this technique further, we doped varying amounts of uranium certified reference materials (CRMs) into a rhyolitic rock standard to establish the effects of uranium concentration and isotopic composition on the accuracy of uranium isotopic analyses by HR-ICP-MS. This also enabled us to quantify peak tailing effects from 238 U on the measurement of 239 Pu and 237 Np, which in turn allows us to constrain correction factors based on measured 237 Np/ 238 U and 239 Pu/ 238 U ratios. A second doping study involved the addition of a mixed actinide standard into three samples with different matrix compositions (termed soil, city, and seawater) to assess whether sample chemistry affects the accuracy and precision of these analyses. Results suggest that this is not the case. Systematic offsets were not observed in elemental or isotopic data derived from the three matrix samples. Results indicate that useful actinide isotopic data can be obtained from whole rock solutions by HR-ICP-MS. Our findings also have implications for solid sampling techniques such as laser ablation ICP-MS, which do not require sample dissolution.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS2015

Gusev-Meridiani-Type Soil Component Dissolved in Some Shock Glasses in Shergottites

Modal analysis, based on APXS, MiniTES and Mossbauer results obtained at Gusev and Meridiani sites on Mars, indicates that Martian soils consist predominantly of igneous minerals such as olivine, pyroxene and feldspar (approximately70 - 80%), with the balance consisting of alteration minerals such as sulfates, silica and chlorides]. These studies also showed that soil alteration did not occur in-situ and igneous and alteration components are derived from different sources. Below, we analyse the chemical abundance data obtained from shock glasses in shergottites using mass balance mixing models. In these models, the two main end members used are (a) host rock chemical composition and (b) the GM soils average composition as the second component. Here, we consider the S-bearing phases as indicators of added alteration phases in the shock glasses and GM soils. Although the S-bearing phase in shock glasses occurs as micron sized sulfide blebs, we showed in earlier abstracts that sulfur was originally present as sulfate in impact glass-precursor materials and was subsequently reduced to sulfide during shock melting. This conclusion is based on results obtained from S-K XANES studies, Fe/S atomic ratios in sulfide blebs and 34S/32S isotopic measurements in these sulfide blebs. Additionally, sulfur in several EET79001 Lith. A glasses is found to correlate positively with Al2O3 and CaO (and negatively with FeO and MgO), suggesting the presence of Al- and Ca- sul-fate-bearing phases. The distribution of the 87Sr/86Sr iso-topic ratios determined in Lith. A glasses (,27 &,188 and,54) indicate that Martian soil gypsum and host rock material were mixed with each other in the glass precursors. In some vugs in Lith A glass,27 detected gypsum laths. Furthermore, the Martian regolith-de-rived component (where sulfur typically occurs as sul-fate) is identified in these glasses by determining neutron produced isotopic excesses/deficits in 80Kr and 149Sm isotopes. Moreover, the suggestion that the large amount of sulfur found in,507 was sourced from pyrrhotite in the host rock, would require that excessive quantities of host rock would need to be stripped of sulfur to make this sulfide-rich glass. These results provide ample evidence that S occurred as sulfate and was added to glass precursor materials prior to impact shock.

Ross, D. K.↗
NASA NTRS1992

Energy expenditure in space flight (doubly labelled water method) (8-IML-1)

The objective of the Energy Expenditure in Space Flight (ESS) experiment is to demonstrate and evaluate the doubly labeled water method of measuring the energy expended by crew members during approximately 7 days in microgravity. The doubly labeled water technique determines carbon dioxide production which is then used to calculate energy expenditure. The method relies on the equilibrium between oxygen in respiratory carbon dioxide and oxygen in body water. Because of this equilibrium, the kinetic of water turnover and respiration are interdependent. Under normal conditions, man contains small but significant amounts of deuterium and oxygen 18. Deuterium is eliminated from the body as water while oxygen 18 is eliminated as water and carbon dioxide. The difference in the turnover rates in the two isotopes is proportional to the carbon dioxide production. Deliberately enriching the total body water with both of these isotopes allows the isotope turnovers to be accurately measured in urine, plasma, or saliva samples. The samples are taken to the laboratory for analysis using an ion-ratio spectrometer.

Parsons, Howard G.↗
NASA NTRS1990

Implications for the evolution of continental crust from Hf isotope systematics of Archean detrital zircons

Results from the fractionation of zircon by sedimentary processes into continental margin sandstone yield information on the preservation of preexisting continental crust in the form of zircon, making it possible to distinguish between the contrasting theories of gradual growth versus constant volume of continental crust over geologic time. In this work, Hf-176/Hf-177 ratios were determined for detrital zircon fractions from 2.0-2.5, 2.6-3.0, and pre-3.0 Gyr old sandstones from the Canadian-Shield, the North-Atlantic, the Wyoming, and the Kaapvaal Cratons. Results pointed to small amounts of continental crust prior to 3.0 Gyr ago and a rapid addition of continental crust between 2.5 and 3.0 Gyr ago, consistent with the gradual growth of continental crust, and giving evidence against no-growth histories.

Stevenson, Ross K.↗
NASA NTRS1973

U-Th-Pb systematics of some Apollo 16 lunar samples

U, Th, and Pb concentrations and lead isotopic compositions of Apollo 16 samples are interpreted as follows: (1) an early period of lunar differentiation of either global or regional scale occurred about 4.47 b.y. ago; (2) the Imbrian impact event affected many Apollo 16 samples about 3.99 b.y. ago; (3) some Apollo 16 metaclastic rocks and breccias contain a large amount of KREEP-like material; (4) lead produced in the early history of the moon has been concentrated in lunar highland soils yielding high Pb-207/Pb-206 ratios corresponding to apparent ages of more than 4.8 b.y.; and (5) South Ray Crater soils reflect the approximately 2-b.y.-old event previously proposed for the Apollo 12 and 14 samples.

Nunes, P. D.↗
DOE OSTI2022

Measurement of Mass-Independent Perturbations of Cadmium in Nuclear Debris Samples

The isotopic composition of cadmium in nuclear debris was measured by multi-collector inductively coupled plasma-mass spectrometry (MC-ICP-MS). Mass-independent perturbations due to fission product decay on the isotopes of Cd were observed. Relative fission yields for masses 111, 112, 114 and 116 were determined in each sample of nuclear debris and compared with reported values found in irradiated plutonium and uranium fuels. Mass spectrometry measurements of the valley fission product endpoints are extremely challenging due to the low cumulative fission yields and small amounts of each isotope that are produced. To overcome these challenges, a new purification method for Cd was developed and validated by examination of a number of geological reference materials.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS2001

Natural abundance deuterium and 18-oxygen effects on the precision of the doubly labeled water method

The doubly labeled water method for measuring total energy expenditure is subject to error from natural variations in the background 2H and 18O in body water. There is disagreement as to whether the variations in background abundances of the two stable isotopes covary and what relative doses of 2H and 18O minimize the impact of variation on the precision of the method. We have performed two studies to investigate the amount and covariance of the background variations. These were a study of urine collected weekly from eight subjects who remained in the Madison, WI locale for 6 wk and frequent urine samples from 14 subjects during round-trip travel to a locale > or = 500 miles from Madison, WI. Background variation in excess of analytical error was detected in six of the eight nontravelers, and covariance was demonstrated in four subjects. Background variation was detected in all 14 travelers, and covariance was demonstrated in 11 subjects. The median slopes of the regression lines of delta2H vs. delta18O were 6 and 7, respectively. Modeling indicated that 2H and 18O doses yielding a 6:1 ratio of final enrichments should minimize this error introduced to the doubly labeled water method.

NASA Discipline Regulatory Physiology↗
DOE OSTI2026

High sensitivity measurement of femtogram-level 238 Pu by thermal ionization mass spectrometry with correction of background 238 U

Low-concentration plutonium isotopic measurements provide a valuable fingerprint to identify possible material origins in the context of environmental contamination monitoring, environmental tracing, nuclear safeguards, nuclear forensics, and treaty monitoring. Thermal ionization mass spectrometry (TIMS) has long been recognized as one of the most sensitive techniques for plutonium isotopic measurement, but has not generally been utilized for 238 Pu determination, especially at low concentrations, due to an isobaric interference from 238 U, prevalent as background. Here, this work demonstrates a new analytical technique for correction of background 238 U from the 238 Pu counts collected during a TIMS analysis. The technique takes advantage of the higher ionization temperature of U relative to Pu and uses a 235 U tracer added after plutonium purification chemistry for 238 U semi-quantitative determination. This technique has been successfully applied to the determination of 238 Pu concentration and the 238 Pu/ 239 Pu ratio in sample types including single-isotope standards, isotopic certified reference materials, matrix-containing environmental reference materials, and simulated nuclear detonation debris. The results have been directly compared on a sample-by-sample basis to alpha spectrometry results. The detection limit by this new technique is 0.23 fg 238 Pu, which was previously unachievable by mass spectrometry and is possible in around 1 h of analysis time post-chemistry compared to weeks of required counting time by alpha spectrometry (at the same atom amount). We also present original, high precision data for Pu isotope concentrations in IAEA-384, Fangataufa Sediment, including 242 Pu results for the first time. The new technique allows measurement of a key isotope, 238 Pu, that was previously not measured in small environmental or nuclear forensics collections.

238Pu↗
NASA NTRS1977

The composition of the atmosphere at the surface of Mars

The current status is summarized of investigations of the composition of the Martian atmosphere, in which use was made of the mass spectrometers that function as the analytical component of the molecular analysis experiments on the two Viking landers. The following points seem well established: N2, Ar-40, Ne, Kr, Xe, and the primordial isotope of Ar are present. The present atmosphere of Mars represents only a small fraction of the total amount of volatiles outgassed by the planet, so that high surface pressure and abundant water may have been present. The noble gases in the Martian atmosphere exhibit a relative abundance pattern similar to that in the earth's atmosphere and (except for Xe) to that in the primordial component of meteorites. The existence of a 'planetary component' is thus proven, supporting the arguments of those who favor a fractionation of noble gases prior to the formation of the planets. In spite of these similarities, the isotopic ratios of nitrogen, argon, and xenon indicate that the histories of the Martian and the earth's atmospheres have been very different.

Owen, T.↗
NASA NTRS1992

Phase transformations in 40-60-GPa shocked gneisses from the Haughton Crater (Canada): An Analytical Transmission Electron Microscopy (ATEM) study

In order to better understand phase transformations, chemical migration, and isotopic disequilibrium in highly shocked rocks, we have performed a microprobe and an ATEM study on gneisses shocked up to 60 GPa from the Haughton Crater. This study reveals the following chemical and structural characteristics: (1) SiO2 dominant areas are formed by a mixture of pure SiO2 polycrystalline quartz identified by electron diffraction pattern and chemical analysis and a silica-rich amorphous phase containing minor amounts of aluminium, potassium, and iron; (2) Areas with biotitelike composition are formed by less than 200-nm grains of iron-rich spinels embedded in a silica-rich amorphous phase that is very similar to the one described above; (3) Layers with feldsparlike composition are constituted by 100-200-nm-sized alumina-rich grains (the indexation of the crystalline structure is under progress) and the silica-rich amorphous phase; (4) Zones characterized by the unusual Al/Si ratio close to 1 are formed by spinel grains (200-nm-sized) embedded in the same silica-rich amorphous phase; and (5) The fracturated sillimanites contain domains with a lamellar structure, defined by the intercalation of 100-nm-wide lamellae of mullite crystals and of a silica-rich amorphous phase. These mullite crystals preserved the crystallographical orientation of the preshock sillimanite. All compositional domains, identified at the microprobe scale, can thus be explained by a mixture in different proportion between the following phases: (1) a silica-rich amorphous phase, with minor Al and K; (2) quartz crystals; (3) spinel crystals and alumina-rich crystals; (4) sillimanite; and (5) mullite. Such mixtures of amorphous phases and crystals in different proportions explain disturbed isotope systems in these rocks and chemical heterogeneities observed on the microprobe.

Martinez, I.↗
NASA NTRS1974

Studies of K-Ar dating and xenon from extinct radioactivities in breccia 14318; implications for early lunar history

The lunar breccia 14318 is one of three Apollo-14 breccias containing substantial amounts of parentless xenon from the spontaneous fission of extinct Pu-244. The argon and xenon contained in this breccia were studied by stepwise heating of pristine and neutron-irradiated samples. The isotopic composition of xenon from fission, determined by an improved method, is shown to be from Pu-244. Concentrations of this fissiogenic xenon are in substantial excess (15-fold) of what could be produced by spontaneous fission of U-238. The breccia is found to contain abundant trapped argon with an Ar-40/Ar-36 ratio of roughly 14. Otherwise, the argon is radiogenic and gives a convincing K-Ar age of 3.69 plus or minus 0.09 b.y. by the stepwise Ar-40/Ar-39 method, nearly in agreement with ages for other Apollo-14 breccias.

Reynolds, J. H.↗
NASA NTRS1979

Isotopic anomalies of noble gases in meteorites and their origins. IV - C3 /Ornans/ carbonaceous chondrites

The C3O chondrites Kainsaz, Lance, and Ornans were studied by an acid dissolution technique to characterize the noble gas components in 3 mineral fractions: HF, HCl-solubles, chromite and carbon, and 'phase Q', a trace mineral containing Ar, Kr, Xe. For all fractions, gas contents decline in the order Kainsaz, Lance, Ornans; this trend parallels volatile contents but not heterogeneity of olivine composition or degree of metamorphism, and reflects progressively higher condensation temperature from the solar nebula. The Ar/Xe ratios and compositions of the three mineral fractions are discussed, and it is concluded that in all primitive chondrites the amount and the chemical separability of CCFXe parallel the abundance of primordial noble gases and other volatiles, such as C, N, Tl, Bi, and In. The close correlation of CCFXe with properties of local origin, such as volatile content and petrologic type, is more consistent with a local than with an extrasolar origin of the component.

Alaerts, L.↗
NASA NTRS2024

Precipitation -17 O-Excess Altered During Tropical Convection: Evidence From Monsoon Cold Surges in Singapore

Despite the recent recognition of -17 O-excess as a promising new tracer for hydrological processes, our knowledge of the control mechanisms underlying -17 O-excess in tropical regions remains limited. To understand how microphysical processes during tropical convection affect precipitation isotope ratios, particularly -17 O-excess, in Singapore, we collected precipitation samples at minute intervals from six rain events associated with cold surges during the Northeast Monsoon seasons and analyzed their triple oxygen isotopes. Our results show that precipitation δ -18 O decreases in the convective zones and then gradually increases in the stratiform zones, while d-excess exhibits an inverse trend. This correlation between δ -18 O and d-excess indicates that rain evaporation plays a crucial role in regulating precipitation isotopes. Moreover, the rain events with a higher upstream rainout amount have lower δ -18 O and higher -17 O-excess values, suggesting that precipitation δ -18 O and -17 O-excess likely reflect the integrated upstream convective activity. Microphysical processes associated with upstream convection, such as rain evaporation and vapor recycling, are potential mechanisms that increase -17 O-excess values along moisture transport pathways for a rain event, and hence, undermine the effectiveness of -17 O-excess as a tracer of moisture source humidity. Contrary to the negative correlation observed in monthly precipitation, there is generally a positive correlation between d-excess and -17 O-excess at the event scale. However, this correlation weakens as convective rain intensifies, suggesting that stronger convection can attenuate the positive correlation between d-excess and -17 O-excess. Therefore, it is crucial to consider how tropical convection alters -17 O-excess when utilizing this tracer to interpret atmospheric dynamics and hydrological processes.

tropical weather systems↗
NASA NTRS1988

X-ray fluorescence surface contaminant analyzer: A feasibility study

The bonding of liner material to the inner metal surfaces of solid rocket booster cases is adversely affected by minute amounts of impurities on the metal surface. Suitable non-destructive methods currently used for detecting these surface contaminants do not provide the means of identifying their elemental composition. The feasibility of using isotopic source excited energy dispersive X-ray fluorescence as a possible technique for elemental analysis of such contaminants is investigated. A survey is made of the elemental compositions of both D-6ac steel, a common construction material for the booster cases, and Conoco HD-2 grease, a common surface contamination. Source and detector choices that maximize signal to noise ratio in a Recessed Source Geometry are made. A Monte Carlo simulation is then made of the optimized device incorporating the latest available X-ray constants at the energy of the chosen source to determine the device's response to a D-6ac steel surface contained with Conoco HD-2 grease.

Eldridge, Hudson B.↗
NASA NTRS2020

Strong Sensitivity of the Isotopic Composition of Methane to the Plausible Range of Tropospheric Chlorine

The C-13 isotopic ratio of methane, δC-13 of CH4, provides additional constraints on the CH4 budget to complement the constraints from CH4 observations. The interpretation of δC-13 observations is complicated, however, by uncertainties in the methane sink. The reaction of CH4 with Cl is highly fractionating, increasing the relative abundance of 13CH4, but there is currently no consensus on the strength of the tropospheric Cl sink. Global model simulations of halogen chemistry differ strongly from one another in terms of both the magnitude of tropospheric Cl and its geographic distribution. This study explores the impact of the inter-model diversity in Cl fields on the simulated δC-13 of CH4. We use a set of GEOS global model simulations with different predicted Cl fields to test the sensitivity of the δC-13 of CH4 to the diversity of Cl output from chemical transport models. We find that δC-13 is highly sensitive to both the amount and geographic distribution of Cl. Simulations with Cl providing 0.28% or 0.66% of the total CH4 loss bracket the δC-13 observations for a fixed set of emissions. Thus, even when Cl provides only a small fraction of the total CH4 loss and has a small impact on total CH4, it provides a strong lever on δC-13. Consequently, it is possible to achieve a good representation of total CH4 using widely different Cl concentrations, but the partitioning of CH4 loss between the OH and Cl reactions leads to strong differences in isotopic composition depending on which model’s Cl field is used. Comparing multiple simulations, we find that altering the tropospheric Cl field leads to approximately a 0.5‰ increase in δ(13)CH4for each percent increase in how much CH4 is oxidized by Cl. The geographic distribution and seasonal cycle of Cl also impacts the hemispheric gradient and seasonal cycle of δC-13. The large effect of Cl on δC-13 compared to total CH4 broadens the range of CH4 source mixtures that can be reconciled with δC-13 observations. Stronger constraints on tropospheric Cl are necessary to improve estimates of CH4 sources from δC-13 observations.

Global model simulations of halogen chemistry↗
NASA NTRS1990

The 158 micrometer (CII) line: A measure of global star formation activity in galaxies

Some 158 micron (CII) fine structure line observations from a sample of fourteen gas rich galaxies are reported. These measurements confirm and generalize previous basic results that the (CII) line is bright amounting to approximately 0.1 to 1 percent of the Far Infra Red (FIR) luminosity of the nuclear regions of galaxies; the (CII) line is formed in the warm (temperature of the gas is greater than 200 K), dense (n sub H greater than 1000/cu cm) photodissociated gas at the interfaces between giant molecular clouds and ionized gas regions and is therefore associated with the molecular gas component in spiral galaxies; the (CII) line tracks the FIR continuum in a manner consistent with the PDR models; the integrated (CII) to isotope (12)CO (transition 1 to 0) line ratio is large (greater than or equal to 1000) in all galaxies studied, and is similarly large for galactic molecular clouds; the (CII) line is therefore energetically very important for the study of giant molecular clouds. Conclusions obtained from these results are given.

Stacey, G. J.↗