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Oxygen Isotopic Composition of Refractory Inclusions from the Miller Range (MIL) 090019 Carbonaceous Chondrite

Introduction: Primitive meteorites contain Calcium-Aluminum-rich Inclusions (CAIs)that preserve the records of the earliest times in the Solar System. CAIs record O isotopic variations with time and/or location from solar (16O-rich) to planetary (16O-poor) compositions [e.g., 1, 2].However, CAIs were also affected by parent body processing to varying degrees. The goal of this work was to identify the processes that resulted in the fine-scale spatial variations in oxygen isotopic compositions within the most ancient Solar System solids. We report oxygen isotopic composition of CAIs from MIL 090019 CO3.1 carbonaceous chondrite. MIL 090019 contains a high abundance of CAIs showing mineralogical as well as textural variations [3]. Methods: We analyzed 10 CAIs with different mineralogical assemblages, classified as corundum-bearing, grossite-bearing, hibonite-bearing, melilite-bearing, anorthite-bearing inclusions and amoeboid olivine aggregates(AOA’s). The mineralogical and petrological characterization of CAIs was performed using the JOEL Hyperprobe 8530 electron microprobe at NASA JSC. Oxygen isotopic imaging of the CAIs was done using the Cameca NanoSIMS 50L ion microprobe at NASA JSC. We followed the analytical protocol described in [4]. O-isotopic maps of the CAI were acquired by rastering a ~3 pA primary Cs+beam at 16 keVover an area of 20 ×20μm2over a period of ~7 hours. Negative secondary ions of 16O−, 17O−, 18O−, 28Si−, 24Mg16O−, 27Al16O−, and 40Ca16O−were simultaneously acquired using electron multiplier detectors at a mass resolving power sufficient to resolve the 16OH−interference from the 17O−peak, where the contribution of 16OH−was <0.1%.An electron flood gun was used to mitigate sample charging during the analyses. We used San Carlos olivine and Madagascar hibonite as isotopic standards to correct for the instrumental mass fractionation. The O-isotopic ratios were corrected for the quasi simultaneous arrival (QSA) effect and the detector dead time. All reported errors are 1 sigma. Results: The MIL 090019 carbonaceous chondrite hosts refractory inclusions varying in their mineralogies and textures[2, 3]. We found the oxygen isotopic compositions of mineral phases in MIL 090019 CAIs show large variations with Δ17O values varying from -27 to 0‰. A corundum-bearing inclusion records isotopic variations with corundum, melilite, perovskite, and anorthite showing Δ17Ovalues of -20 ±2.5, -10.2 ± 6.5, -10.7 ± 1.3,and -1.2 ± 3.2‰ respectively. A grossite-hibonite-bearing inclusion also records O-isotopic heterogeneity, where grossite, hibonite, Mg-rich spinel, and melilite show -3.7 ± 2.7, -22.9 ± 2.5, -21.4 ± 2.6, and -17.3 ± 2.8‰ respectively, whereas perovskite grains record a heterogenous isotopic composition ranging from -22.6 to -13.9‰. A hibonite-bearing inclusion shows average Δ17Ο values of -17.6 ± 5.3 ‰ and -15.1 ± 4.8 ‰ for hibonite and spinel respectively. The two perovskite grains also show relatively 16O-poor composition (Δ17Ο = -11.8 ± 6.4 ‰ and -8.6 ± 5.2 ‰). Anorthite has ~0.1 wt% Na2O and ~0.52 wt% FeO and a Δ17Ο value of -7.2 ± 5.0 ‰, whereas diopside records a Δ17Ο value of -3.5 ± 5.0 ‰. A hibonite-spinel-rich inclusion contains spinel and hibonite that are16O-rich (Δ17Οvalues -21.3 ± 2.8‰ and -19.4 ± 3.0‰, respectively). Melilite shows heterogenous oxygen isotopic composition, with an inner 16O-rich region and an outer 16O-poor region separated by a sharp boundary, with a bulk Δ17Ο= -16.2 ± 2.1‰, whereas two perovskite grains are relatively 16O-poor (Δ17Ο= -13.2 ± 3.7‰ and -7.1 ± 3.4‰).A spinel-rich inclusion contains perovskite grains with Δ17Οranging from -27.0 to -22.8 ‰and spinel with average Δ17Οvalue of -21.4 ± 2.8 ‰. In a melilite and spinel-rich CAI, perovskite, spinel, diopside, melilite, and Al-Ti-rich pyroxene record Δ17Ο values of-26.9 ± 4.6‰, -22.4 ± 4.3‰,-23.4 ± 4.9, -19.3 ± 3.4, and -19.0 ± 4.3 ‰ respectively. Olivine and spinel components of 2 AOA’s record a 16O-rich composition with Δ17O~-23‰. Discussion: The coexistence of 16O-rich and 16O-poor minerals within CAIs has been attributed to differing degrees of O isotopic exchange, reflecting a wide range of O diffusion rates[5]. However, the O isotopic heterogeneity observed in these CAIs cannot be explained by oxygen diffusion in nebular or parent body settings alone. The isotopic imaging of CAIs from the MIL 090019 meteorite shows variations in the O isotopic composition recorded in their mineral components, suggesting that these CAIs record the oxygen isotopic heterogeneity in the nebular gas from which they condensed. The coexistence of 16O-rich and 16O-poor mineral components in the CAI-forming region suggests that the gas in this region was not well-mixed and consisted of distinct 16O-rich and 16O-poor gaseous reservoirs.

P Mane↗
NASA NTRS1992

Comets: Role and importance to exobiology

The transfer of organic compounds from interstellar space to the outskirts of a protoplanetary disk, their accretion into cometary objects, and the transport of the latter into the inner solar system by orbital diffusion throw a new light on the central problem of exobiology. It suggests the existence of a cosmic mechanism, working everywhere, that can supply prebiotic compounds to ubiquitous rocky planets, in search of the proper environment to start life in many places in the Universe. Under the heading of chemistry of the cometary nucleus, the following topics are covered: radial homogeneity of the nucleus; the dust-to-ice ratio; nature of the dust grains; origin of the dust in comets; nature of the volatile fraction; the CO distribution in comet Halley; dust contribution to the volatile fraction; elemental balance sheet of comet Halley; quantitative molecular analysis of the volatile fraction; and isotopic ratios. Under the heading of exogenous origin of carbon on terrestrial planets the following topics are covered: evidence for a high-temperature phase; from planetesimals to planets; a veneer of volatile and organic material; and cometary contribution.

Delsemme, Armand H.↗
NASA NTRS1997

Detection and Monitoring of Stratigraphic Markers and Temperature Trends at the Greenland Ice Sheet Project 2 Using Passive-Microwave Remote-Sensing Data

Satellite passive-microwave sensors provide a sensitive means of studying ice-sheet surface processes that assists ice-core interpretation and can extend local observations across regional scales. Analysis of special sensor microwave/imager (SSM/I) brightness temperature (TB) data supports ice-core research in two specific ways. First, the summer hoar complex layers used to date the Holocene portion of the Greenland Ice Sheet Project 2 ice core can be defined temporally and spatially by SSM/I 37-GHz vertically (V) and horizontally (H) polarized B ratio (V/H) trends. Second, comparison of automatic weather station temperatures to SSM/I 37-GHz V TB data shows that they are an effective proxy temperature record in this region. Also, the TB data can be correlated with proxy temperature trends from stable-isotope-ratio (delta O-18 and delta-D) profiles from snow pits and this allows the assignment of dates to specific snow depths.

Shuman, C. A.↗
NASA NTRS2012

Carbon and Hydrogen Isotope Measurements of Alcohols and Organic Acids by Online Pyroprobe-GC-IRMS

The detection of methane in the atmosphere of Mars, combined with evidence showing widespread water-rock interaction during martian history, suggests that the production of methane on Mars may be the result of mineral surface-catalyzed CO2 and or CO reduction during Fisher-Tropsch Type (FTT) reactions. A better understanding of these reaction pathways and corresponding C and H isotope fractionations is critical to deciphering the synthesis of organic compounds produced under abiotic hydrothermal conditions. Described here is a technique for the extraction and analysis of both C and H isotopes from alcohols (C1-C4) and organic acids (C1-C6). This work is meant to provide a "proof of concept" for making meaningful isotope measurements on complex mixtures of solid-phase hydrocarbons and other intermediary products produced during high-temperature and high-pressure synthesis on mineral-catalyzed surfaces. These analyses are conducted entirely "on-line" utilizing a CDS model 5000 Pyroprobe connected to a Thermo Trace GC Ultra that is interfaced with a Thermo MAT 253 isotope ratio mass spectrometer operating in continuous flow mode. Also, this technique is designed to carry a split of the GC-separated product to a DSQ II quadrupole mass spectrometer as a means of making semi-quantitative compositional measurements. Therefore, both chemical and isotopic measurements can be carried out on the same sample.

Socki, Richard A.↗
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↗
NASA NTRS1996

Calcium kinetics with microgram stable isotope doses and saliva sampling

Studies of calcium kinetics require administration of tracer doses of calcium and subsequent repeated sampling of biological fluids. This study was designed to develop techniques that would allow estimation of calcium kinetics by using small (micrograms) doses of isotopes instead of the more common large (mg) doses to minimize tracer perturbation of the system and reduce cost, and to explore the use of saliva sampling as an alternative to blood sampling. Subjects received an oral dose (133 micrograms) of 43Ca and an i.v. dose (7.7 micrograms) of 46Ca. Isotopic enrichment in blood, urine, saliva and feces was well above thermal ionization mass spectrometry measurement precision up to 170 h after dosing. Fractional calcium absorptions determined from isotopic ratios in blood, urine and saliva were similar. Compartmental modeling revealed that kinetic parameters determined from serum or saliva data were similar, decreasing the necessity for blood samples. It is concluded from these results that calcium kinetics can be assessed with micrograms doses of stable isotopes, thereby reducing tracer costs and with saliva samples, thereby reducing the amount of blood needed.

Clinical Trial↗
NASA NTRS2019

Multiple Reservoirs of Volatiles in the Moon Revealed by the Isotopic Composition of Chlorine in Lunar Basalts

The isotopes of chlorine (37Cl and 35Cl) are highly fractionated in lunar samples compared to most other Solar System materials. Recently, the chlorine isotope signatures of lunar rocks have been attributed to large-scale degassing processes that occurred during the existence of a magma ocean. In this study we investigated how well a suite of lunar basalts, most of which have not previously been analyzed, conform to previous models. The Cl isotope compositions (δ37Cl (‰) = [(37Cl/35Clsample/37Cl/35ClSMOC) − 1] × 1000, where SMOC refers to standard mean ocean chloride) recorded range from ∼+7 to +14‰ (Apollo 15), +10 to +19‰ (Apollo 12), +9 to +15‰ (70017), +4 to +8‰ (MIL 05035), and +15 to +22‰ (Kalahari 009). The Cl isotopic data from the present study support the mixing trends previously reported by Boyce et al. (2015) and Barnes et al. (2016), as the Cl isotopic composition of apatites are positively correlated with bulk-rock incompatible trace element abundances in the low-Ti basalts, inclusive of low-Ti and KREEP basalts. This trend has been interpreted as evidence that incompatible trace elements, including Cl, were concentrated in the urKREEP residual liquid of the lunar magma ocean, rather than the mantle cumulates, and that urKREEP Cl had a highly fractionated isotopic composition. The source regions for the basalts were thus created by variable mixing between the mantle (Cl-poor and relatively unfractionated) and urKREEP. The high-Ti basalts show much more variability in measured Cl isotope ratios and scatter around the trend formed by the low-Ti basalts. Most of the data for lunar meteorites also fits the mixing of volatiles in their sources, but Kalahari 009, which is highly depleted in incompatible trace elements, contains apatites with heavily fractionated Cl isotopic compositions. Given that Kalahari 009 is one of the oldest lunar basalts and ought to have been derived from very early-formed mantle cumulates, a heavy Cl isotopic signature is likely not related to its mantle source, but more likely to magmatic or secondary alteration processes, perhaps via impact-driven vapor metasomatism of the lunar crust.

Mccubbin, Francis M.↗
NASA NTRS1984

The isotopic composition of cosmic rays

Observations of the isotopic composition of the elements carbon, nitrogen, oxygen, neon, magnesium, silicon, sulfur, calcium, iron and nickel are reviewed and 'best' values of selected isotope ratios are derived from the collected data. A simple model of cosmic ray propagation is employed to deduce cosmic ray source abundance ratios both from these best values and from the observations made in a recent high resolution satellite experiment. General features of the cosmic ray source composition are discussed, with emphasis on the enhanced abundances of various neutron rich nuclides and on the distinctly nonsolar character of the nitrogen isotopic abundances.

Wiedenbeck, M. E.↗
NASA NTRS1993

Factors that control the stable carbon isotopic composition of methane produced in an anoxic marine sediment

The carbon isotopic composition of methane produced in anoxic marine sediment is controlled by four factors: (1) the pathway of methane formation, (2) the isotopic composition of the methanogenic precursors, (3) the isotope fractionation factors for methane production, and (4) the isotope fractionation associated with methane oxidation. The importance of each factor was evaluated by monitoring stable carbon isotope ratios in methane produced by a sediment microcosm. Methane did not accumulate during the initial 42-day period when sediment contained sulfate, indicating little methane production from 'noncompetitive' substrates. Following sulfate depletion, methane accumulation proceeded in three distinct phases. First, CO2 reduction was the dominant methanogenic pathway and the isotopic composition of the methane produced ranged from -80 to -94 per thousand. The acetate concentration increased during this phase, suggesting that acetoclastic methanogenic bacteria were unable to keep pace with acetate production. Second, acetate fermentation became the dominant methanogenic pathway as bacteria responded to elevated acetate concentrations. The methane produced during this phase was progressively enriched in C-13, reaching a maximum delta(C-13) value of -42 per thousand. Third, the acetate pool experienced a precipitous decline from greater than 5 mM to less than 20 micro-M and methane production was again dominated by CO2 reduction. The delta(C-13) of methane produced during this final phase ranged from -46 to -58 per thousand. Methane oxidation concurrent with methane production was detected throughout the period of methane accumulation, at rates equivalent to 1 to 8 percent of the gross methane production rate. Thus methane oxidation was too slow to have significantly modified the isotopic signature of methane. A comparison of microcosm and field data suggests that similar microbial interactions may control seasonal variability in the isotopic composition of methane emitted from undisturbed Cape Lookout Bight sediment.

Alperin, M. J.↗
NASA NTRS1992

Past and present water budget of Venus

Attention is given to a detailed analysis of Pioneer Venus large-probe neutral mass spectrometer data which confirm an earlier report that the abundance of Venus deuterium relative to hydrogen is two orders of magnitude larger than that of terrestrial deuterium. The D/H ratio in the bulk atmosphere of Venus today is found to be between 0.014 and 0.02. The argument that present-day HDO can be in a steady state with exogenous (cometary) sources is based on an underestimate of the hydrogen abundance and an overestimate of current escape rates. The large isotope ratio requires that Venus once had above-surface water amounting to at least a few tenths of a percent of a terrestrial ocean and has since lost almost all of the associated hydrogen.

Donahue, T. M.↗
NASA NTRS2012

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS: Application to Analysis of Experimentally Derived Hydrothermal Mineral-Catalyzed Organic Products

We report results of experiments to measure the H isotope composition of organic acids and alcohols. These experiments make use of a pyroprobe interfaced with a GC and high temperature extraction furnace to make quantitative H isotope measurements. This work compliments our previous work that focused on the extraction and analysis of C isotopes from the same compounds [1]. Together with our carbon isotope analyses our experiments serve as a "proof of concept" for making C and H isotope measurements on more complex mixtures of organic compounds on mineral surfaces in abiotic hydrocarbon formation processes at elevated temperatures and pressures. Our motivation for undertaking this work stems from observations of methane detected within the Martian atmosphere [2-5], coupled with evidence showing extensive water-rock interaction during Mars history [6-8]. 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 [9,10]. 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 [11-13]. Our H isotope measurements utilize an analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). This technique is designed to carry a split of the pyrolyzed GC-separated product to a Thermo DSQII quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Socki, Richard A.↗
NASA NTRS2012

Unusual Nonterrestrial L-proteinogenic Amino Acid excesses in the Tagish Lake Meteorite

The distribution and isotopic and enantiomeric compositions of amino acids found in three distinct fragments of the Tagish Lake C2-type carbonaceous chondrite were investigated via liquid chromatography with fluorescence detection and time-of-flight mass spectrometry and gas chromatography isotope ratio mass spectrometry. Large L-enantiomeric excesses (L(sub ee) approximately 43-59%) of the alpha-hydrogen aspartic and glutamic amino acids were measured in Tagish Lake, whereas alanine, another alpha hydrogen protein amino acid, was found to be nearly racemic (D much approximately L) using both techniques. Carbon isotope measurements of D- and L-aspartic acid and 1)- and L-alanine in Tagish Lake fall well outside of the terrestrial range and indicate that the measured aspartic acid enantioenrichment is indigenous to the meteorite. Alternate explanations for the L-excesses of aspartic acid such as interference from other compounds present in the sample, analytical biases, or terrestrial amino acid contamination were investigated and rejected. These results can be explained by differences in the solid-solution phase behavior of aspartic acid, which can form conglomerate enantiopure solids during crystallization, and alanine, which can only form racemic crystals. Amplification of a small initial L-enantiomer excess during aqueous alteration on the meteorite parent body could have led to the large L-enrichments observed for aspartic acid and other conglomerate amino acids in Tagish Lake. The detection of non terrestrial L-proteinogenic amino acid excesses in the Tagish Lake meteorite provides support for the hypothesis that significant enantiomeric enrichments for some amino acids could form by abiotic processes prior to the emergence of life.

Glavin, Daniel P.↗
NASA NTRS2015

The Mineralogical Record of Oxygen Fugacity Variation and Alteration in Northwest Africa 8159: Evidence for Interaction Between a Mantle Derived Martian Basalt and a Crustal Component(s)

A prominent geochemical feature of basaltic magmatism on Mars is the large range in initial Sr isotopic ratios (approx. 0.702 - 0.724) and initial epsilon-Nd values (approx. -10 to greater than +50). Within this range, the shergottites fall into three discreet subgroups. These subgroups have distinct bulk rock REE patterns, mineral chemistries (i.e. phosphate REE patterns, Ni, Co, V in olivine), oxygen fugacity of crystallization, and stable isotopes, such as O. In contrast, nakhlites and chassignites have depleted epsilon-Nd values (greater than or equal to +15), have REE patterns that are light REE enriched, and appear to have crystallized near the FMQ buffer. The characteristics of these various martian basalts have been linked to different reservoirs in the martian crust and mantle, and their interactions during the petrogenesis of these magmas. These observations pose interesting interpretive challenges to our understanding of the conditions of the martian mantle (e.g. oxygen fugacity) and the interaction of mantle derived magmas with the martian crust and surface. Martian meteorite NWA 8159 is a unique fine-grained augite basalt derived from a highly depleted mantle source as reflected in its initial epsilon-Nd value, contains a pronounced light REE depleted pattern, and crystallized presumably under very oxidizing conditions. Although considerably older than both shergottites and nahklites, it has been petrogenetically linked to both styles of martian magmatism. These unique characteristics of NWA 8159 may provide an additional perspective for deciphering the petrogenesis of martian basalts and the nature of the crust of Mars.

Shearer, Charles K.↗
NASA NTRS2005

Neutral Mass Spectrometry for Venus Atmosphere and Surface

The assignment is to make precise (better than 1 %) measurements of isotope ratios and accurate (5-10%) measurements of abundances of noble gas and to obtain vertical profiles of trace chemically active gases from above the clouds all the way down to the surface. Science measurement objectives are as follows: 1) Determine the composition of Venus atmosphere, including trace gas species and light stable isotopes; 2) Accurately measure noble-gas isotopic abundance in the atmosphere; 3) Provide descent, surface, and ascent meteorological data; 4) Measure zonal cloud-level winds over several Earth days; 5) Obtain near-IR descent images of the surface from 10-km altitude to the surface; 6) Accurately measure elemental abundances & mineralogy of a core from the surface; and 7) Evaluate the texture of surface materials to constrain weathering environment.

Mahaffy, Paul↗
NASA NTRS2012

Enrichment of Non-Terrestrial L-Proteinogenic Amino Acids by Aqueous Alteration on the Tagish Lake Meteorite Parent Body

The distribution and isotopic and enantiomeric compositions of amino acids found in three distinct fragments of the Tagish Lake C2-type carbonaceous chondrite were investigated via liquid chromatography fluorescence detection time-of-flight mass spectrometry and gas chromatography isotope ratio mass spectrometry. Large L-enantiomeric excesses (L(sub ee) approx. 43 to 59%) of the a-hydrogen aspartic and glutamic amino acids were measured in Tagish Lake, whereas alanine, another alpha-hydrogen protein amino acid, was found to be nearly racemic (D approx. L) using both techniques. Carbon isotope measurements of D- and L-aspartic acid and D- and L-alanine in Tagish Lake fall well outside of the terrestrial range and indicate that the measured aspartic acid enantioenrichment is indigenous to the meteorite. Alternate explanations for the Lexcesses of aspartic acid such as interference from other compounds present in the sample, analytical biases, or terrestrial amino acid contamination were investigated and rejected. These results can be explained by differences in the solid-solution phase behavior of aspartic acid, which can form conglomerate enantiopure solids during crystallization, and alanine, which can only form racemic crystals.

Glavin, Daniel P.↗
NASA NTRS1986

Seasonal variations in the stable carbon isotopic signature of biogenic methane in a coastal sediment

Systematic seasonal variations in the stable carbon isotopic signature of methane gas occur in the anoxic sediments of Cape Lookout Bight, a lagoonal basin on North Carolina's Outer Banks. Values for the carbon isotope ratio of methane range from -57.3 per mil during summer to -68.5 per mil during winter in gas bubbles with an average methane content of 95 percent. The variations are hypothesized to result from changes in the pathways of microbial methane production and cycling of key substrates including acetate and hydrogen. The use of stable isotopic signatures to investigate the global methane cycle through mass balance calculations, involving various sediment and soil biogenic sources, appears to require seasonally averaged data from individual sites.

Martens, C. S.↗
NASA NTRS1992

The interstellar gas experiment: Analysis in progress

The interstellar gas experiment (IGE) exposed thin metallic foils in order to collect neutral interstellar particles which penetrate the solar system due to their motion relative to the sun. These atoms were entrapped in the collecting foils along with precipitating magnetospheric ions and with ambient atmospheric atoms. For the entire duration of the LDEF mission, seven of the foils collected particles arriving from seven different directions as seen from the spacecraft. In the mass spectrometric analysis of the trapped noble gas component, we detected the He-3, He-4, Ne-20, and Ne-22 isotopes. In order to infer the isotopic ratios in the interstellar medium from the measured concentrations found in the foil piece, several lines of investigation had to be initiated. The flux of incident noble gas atoms from the ambient atmosphere was estimated by detailed calculations. The contributions proved to be negligible, supporting the experimental evidence. Foil and machine backgrounds for the four isotopes which were measured had to be assessed individually. While this was easy for He-4, spurious foil background of He-3 had to be monitored carefully by analyzing unflown foil pieces. Trapped Ne concentrations are not far above the background. During the flight, a stuck electrical relay precluded the foil-trays from sequencing as designed. Therefore, we could not use the seasonal variation of the direction of the incoming interstellar atoms to make the distinction between interstellar and magnetospheric components of the trapped particles. Instead, we had to try the method of stepwise heating to extract the interstellar component at lower temperatures than we use to extract the magnetospheric component (the interstellars hit the foil with lower energies than most of the magnetospherics). New limiting values for the isotopic composition of the interstellar medium, unavailable yet from any other method of measurement, are emerging from this analysis.

Buehler, F.↗
NASA NTRS2011

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS

One possible process responsible for methane generation on Mars is abiotic formation by Fischer-Tropsch-type (FTT) synthesis during serpentinization reactions. Measurement of carbon and hydrogen isotopes of intermediary organic compounds can help constrain the origin of this methane by tracing the geochemical pathway during formation. Of particular interest within the context of this work is the isotopic composition of organic intermediaries produced on the surfaces of mineral catalysts (i.e. magnetite) during hydrothermal experiments, and the ability to make meaningful and reproducible hydrogen isotope measurements. Reported here are results of experiments to characterize the hydrogen isotope composition of low molecular weight organic acids and alcohols. The presence of these organic compounds has been suggested by others as intermeadiary products made during mineral surface catalyzed reactions. This work compliments our previous study characterizing the carbon isotope composition of similar low molecular weight intermediary organic compounds (Socki, et al, American Geophysical Union Fall meeting, Abstr. #V51B-2189, Dec., 2010). Our hydrogen isotope measurements utilize a unique analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). Our technique is unique in that it carries a split of the pyrolyzed GC-separated product to a Thermo DSQ-II? quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Socki, Richard A.↗