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NASA NTRS2012

Isotopic Ratios in Titan's Methane: Measurements and Modeling

The existence of methane in Titan's atmosphere (approx. 6% level at the surface) presents a unique enigma, as photochemical models predict that the current inventory will be entirely depleted by photochemistry in a timescale of approx 20 Myr. In this paper, we examine the clues available from isotopic ratios (C-12/C-13 and D/H) in Titan's methane as to the past atmosphere history of this species. We first analyze recent infrared spectra of CH4 collected by the Cassini Composite Infrared Spectrometer, measuring simultaneously for the first time the abundances of all three detected minor isotopologues: (13)CH4, (12)CH3D, and (13)CH3D. From these we compute estimates of C-12/C-13 = 86.5 +/- 8.2 and D/H = (1.59 +/- 0.33) x 10(exp -4) , in agreement with recent results from the Huygens GCMS and Cassini INMS instruments. We also use the transition state theory to estimate the fractionation that occurs in carbon and hydrogen during a critical reaction that plays a key role in the chemical depletion of Titan's methane: CH4 + C2H yields CH3 + C2H2. Using these new measurements and predictions we proceed to model the time evolution of C-12/C-13 and D/H in Titan's methane under several prototypical replenishment scenarios. In our Model 1 (no resupply of CH4), we find that the present-day C-12/C-13 implies that the CH4 entered the atmosphere 60-1600 Myr ago if methane is depleted by chemistry and photolysis alone, but much more recently-most likely less than 10 Myr ago-if hydrodynamic escape is also occurring. On the other hand, if methane has been continuously supplied at the replenishment rate then the isotopic ratios provide no constraints, and likewise for the case where atmospheric methane is increasing, We conclude by discussing how these findings may be combined with other evidence to constrain the overall history of the atmospheric methane.

Nixon, C. A.↗
NASA NTRS1987

Boundary conditions for the paleoenvironment: Chemical and physical processes in the pre-solar nebula

Detailed study of the first interstellar hydrocarbon ring, cyclopropenylidene (C3H2), is continuing. The singly deuterated isotope of this molecule, C3HD, was observed in several cold interstellar clouds. The results of a large survey for C3H2 in galactic sources of various types will soon be completed. It appears that cyclopropenylidene is present in virtually all interstellar clouds of at least moderate density. In order to make the first determinations of the CO2/CO abundance ratio in interstellar sources, observations of protonated CO2 were pursued. The spectrum from 18.5 to 22 GHz for several interstellar clouds is being systematically measured. Particular attention is being given to the cold, dark clouds TMC-1 and L124N, which may be formation sites for solar mass stars. The phenomena of maser emission from molecules of methanol is being studied in certain interstellar clouds. A comparison of 1 millimeter continuum emission from dust with the column density of carbon monoxide as determined from the rare C(18)O isotope for 4 molecular clouds in the Galaxy is nearing completion. Papers published during the period of this report are listed.

Irvine, William M.↗
NASA NTRS1975

Heavy particle emission of unusual composition from the sun

Sustained emission of low energy (0.6-4 MeV/nuc) solar particles with a composition richer in iron than in oxygen is observed in three time periods of 1974. The relative abundances of Ne, Mg, Si, and S-Ca to O are also enhanced as compared to those of the sun and of solar cosmic rays. During all three periods, a large H-3/H-4 isotope ratio was also observed; for two cases, it is in the order of unity. On the other hand, the d/H-4 and the T/He-4 are less than 0.04 and 0.02 respectively. The solar activity during the time periods of the reported emission was low. At present, it is not clear whether the emission processes which yielded enriched heavy ions also produced the He-3 enhancement. It seems that any explanation of heavy ion enrichments in solar cosmic rays has to explain also the He-3 enrichment.

Hovestadt, D.↗
NASA NTRS1976

Oxygen isotopes in the Martian atmosphere - Implications for the evolution of volatiles

Nonthermal escape of oxygen by recombination of exospheric O2(+) combined with diffusive separation of gases at lower altitude provides a mechanism through which the Martian atmosphere may be enriched in O-18 relative to O-16. Measurement of the abundance of O-18 relative to O-16 together with a determination of the turbopause may be used to develop important constraints on the history of Martian volatiles. Models for the interpretation of these data are developed and discussed in light of present information.

Mcelroy, M. B.↗
NASA NTRS1986

Properties of the Guin ungrouped iron meteorite - The origin of Guin and of group-IIE irons

The composition and structure of the Guin ungrouped iron meteorite inclusions have been investigated experimentally. The structural characteristics of polished and etched slabs of the meteorite were studied microscopically in reflected light. Modal abundances of troilite nodules and silicate inclusions were determined by weighing paper traces. The bulk composition of the silicate inclusions was calculated by combining modal phase abundances and mineral compositions. It is found that the largest silicate inclusion (2 x 4 cm) consists mostly of a shock-melted plagioclase-rich matrix surrounding large, partly melted augite grains. The oxygen isotopic composition of the inclusion is near that of LL chondrites. The inclusion is found to be similar in composition to selected melt pocket glasses in ordinary chondrites produced in situ by preferential melting of plagioclase rock due to shock compression. It is suggested that the Guin assemblage was formed by impact melting on a chondritic parent body. Silicate inclusions in IIE irons share many of the compositional and petrological characteristics of the Guin inclusions, indicating that IIE irons also formed by impact-melting of chondritic materials. Black and white photomicrographs of the silicate inclusions are provided.

Rubin, A. E.↗
NASA NTRS2014

Searching for Reduced Carbon on the Surface of Mars: The SAM Combustion Experiment

The search for reduced carbon has been a major focus of past and present missions to Mars. Thermal evolved gas analysis was used by the Viking and Phoenix landers and is currently in use by the Sample Analysis at Mars (SAM) instrument suite on the Mars Science Laboratory (MSL) to characterize volatiles evolved from solid samples, including those associated with reduced organic species. SAM has the additional capability to perform a combustion experiment, in which a sample of Mars regolith is heated in the presence of oxygen and the composition of the evolved gases is measured using quadrupole mass spectrometry (QMS) and tunable laser spectrometry (TLS) [1]. Organics detection on the Martian surface has been complicated by oxidation and destruction during heating by soil oxidants [2], including oxychlorine compounds, and terrestrial organics in the SAM background contributed by one of the SAM wet chemistry reagents MTBSTFA (N-Methyl-N-tertbutyldimethylsilyl- trifluoroacetamide) [3,4]. Thermal Evolved Gas Analysis (TEGA) results from Phoenix show a mid temperature CO2 release between 400 C - 680 C speculated to be carbonate, CO2 adsorbed to grains, or combustion of organics by soil oxidants [5]. Low temperature CO2 evolutions (approx. 200 C - 400 C) were also present at all three sites in Gale Crater where SAM Evolved Gas Analysis (EGA) was performed, and potential sources include combustion of terrestrial organics from SAM, as well as combustion and/or decarboxylation either indigenous martian or exogenous organic carbon [4,6]. By performing an experiment to intentionally combust all reduced materials in the sample, we hope to compare the bulk abundance of CO2 and other oxidized species evolved by combustion to that evolved during an EGA experiment to estimate how much CO2 could be contributed by reduced carbon sources. In addition, C, O, and H isotopic compositions of CO2 and H2O measured by TLS can contribute information regarding the potential sources of these volatiles.

Stern, J. C.↗
NASA NTRS2002

Comet Grains: Their IR Emission and Their Relation to ISM Grains

Comets and the chodritic, porous interplanetary dust particles (CP IDPs) that they shed in their comae are reservoirs of primitive solar nebula materials. The high porosity and fragility of cometary grains and CP IDPs, and anomalously high deuterium contents of highly fragile, pyroxene-rich Cluster IDPs imply these aggregate particles contain significant abundances of grains from the interstellar medium (ISM). IR spectra of comets (3 - 40 micron) reveal the presence of a warm (nearIR) featureless emission modeled by amorphous carbon grains. Broad and narrow resonances near 10 and 20 microns are modeled by warm chondritic (50% Fe and 50% Mg) amorphous silicates and cooler Mg-rich crystalline silicate minerals, respectively. Cometary amorphous silicates resonances are well matched by IR spectra of CP IDPs dominated by GEMS (0.1 micron silicate spherules) that are thought to be the interstellar Fe-bearing amorphous silicates produced in AGB stars. Acid-etched ultramicrotomed CP IDP samples, however, show that both the carbon phase (amorphous and aliphatic) and the Mg-rich amorphous silicate phase in GEMS are not optically absorbing. Rather, it is Fe and FeS nanoparticles embedded in the GEMS that makes the CP IDPs dark. Therefore, CP IDPs suggest significant processing has occurred in the ISM. ISM processing probably includes in He' ion bombardment in supernovae shocks. Laboratory experiments show He+ ion bombardment amorphizes crystalline silicates, increases porosity, and reduces Fe into nanoparticles. Cometary crystalline silicate resonances are well matched by IR spectra of laboratory submicron Mg-rich olivine crystals and pyroxene crystals. Discovery of a Mg-pure olivine crystal in a Cluster IDP with isotopically anomalous oxygen indicates that a small fraction of crystalline silicates may have survived their journey from AGB stars through the ISM to the early solar nebula. The ISM does not have enough crystalline silicates (<5%) , however, to account for the deduced abundance of crystalline silicates in comet dust. An insufficient source of ISM Mg-rich crystals leads to the inference that most Mg-rich crystals in comets are primitive grains processed in the early solar nebula prior to their incorporation into comets. Mg-rich crystals may condense in the hot (approx. 1450 K), inner zones of the early solar nebula and then travel large radial distances out to the comet-forming zone. On the other hand, Mg-rich silicate crystals may be ISM amorphous silicates annealed at approx. 1000 K and radially distributed out to the comet-forming zone or annealed in nebular shocks at approx. 5 - 10 AU. Determining the relative abundance of amorphous and crystalline silicates in comets probes the relative contributions of ISM grains and primitive grains to small, icy bodies in the solar system. The life cycle of dust from its stardust origins through the ISM to its incorporation into comets is discussed.

Wooden, Diane H.↗
NASA NTRS1977

Nitrogen isotopes in lunar soils as a measure of cosmic-ray exposure and regolith history

Previous studies have shown that the bulk of the nitrogen in soils has been implanted by the solar wind, that the N-15/N-14 ratio of the implanted nitrogen has apparently increased with time, and that both soils and rocks contain a nitrogen component greatly enriched in N-15, relative to natural abundance ratios, due to cosmic-ray spallation. An investigation was, therefore, conducted to test the feasibility of using spallation-produced N-15 for determining cosmic-ray exposure ages. Samples from several depths in the Apollo 15 deep drill core were analyzed. The data obtained have also been evaluated with regard to possible models for the prior history of the material now in the Apollo 15 core. In addition, analyses have been performed of several other soil samples considered for various reasons to be of particular interest, such as orange soil 74220 and its companion 74240, Apollo 16 drill core sample 60002, and the apparently peculiar fillet soil 67461. Wherever possible, analyses were carried out by step-wise heating rather than by total pyrolysis. On the basis of the results of the investigation it is concluded that nitrogen isotope ratio determinations provide a usable method for determining cosmic-ray exposures for soils.

Becker, R. H.↗
DOE OSTI2026

Metabolic flux and resource balance in the oleaginous yeast Rhodotorula toruloides

The yeast Rhodotorula toruloides is a promising bioproduction organism due to its high lipid yields and ability to grow on cheap and abundant substrates. Quantitative, systems-level assessment of its metabolic activity is accordingly merited. Resource-balance analysis (RBA) models capture not only reaction stoichiometry but also enzyme requirements for catalysis, providing valuable tools for understanding metabolic trade-offs and optimizing metabolic engineering strategies. Here, in this work, we present systems-level measurements of R. toruloides metabolic flux based on isotope tracing and metabolic flux analysis. In combination with new proteomic measurements, these flux data are used to parameterize a genome-scale resource balance model rtRBA. We find that S. cerevisiae and R. toruloides grow at nearly indistinguishable rates using similar biosynthetic but dramatically different central metabolic programs. R. toruloides consumes one-fifth as much glucose, which it metabolizes primarily via the pentose phosphate pathway and TCA cycle unlike primarily glycolysis in S. cerevisiae . Overall, across these two divergent yeasts, protein abundances aligned more closely than metabolic flux. Resource balance modeling of these metabolic programs predicts superior theoretical yields but lower productivities in R. toruloides than S. cerevisiae for industrial chemicals, highlighting the value of rapid glucose uptake for productivity but respiratory metabolism for yields.

60 APPLIED LIFE SCIENCES↗
NASA NTRS1975

A chart of cosmic ray isotopes

A chart has been prepared that lists some of the properties relevant to cosmic ray studies of all the significant nuclides between lithium and nickel. On this chart there are shown all the possible decays that might be of interest in the unique conditions experienced by cosmic ray nuclei, various abundance figures and the probable nucleosynthesis processes of origin.

Waddington, C. J.↗
NASA NTRS2015

Isotopic Composition of Carbon Dioxide Released from Confidence Hills Sediment as Measured by the Sample Analysis at Mars (SAM) Quadrupole Mass Spectrometer

In October 2014, the Mars Science Laboratory (MSL) "Curiosity" rover drilled into the sediment at the base of Mount Sharp in a location namsed Cionfidence Hills (CH). CH marked the fifth sample pocessed by the Sample Analysis at Mars (SAM) instrument suite since Curiosity arrived in Gale Crater, with previous analyses performed at Rocknest (RN), John Klein (JK), Cumberland (CB), and Windjana (WJ). Evolved gas analysis (EGA) of all samples has indicated H2O as well as O-, C- and S-bearing phases in the samples, often at abundances that would be below the detection limit of the CheMin instrument. By examining the temperatures at which gases are evolved from samples, SAM EGA data can help provide clues to the mineralogy of volatile-bearing phases when their identities are unclear to CheMin. SAM may also detect gases evolved from amorphous material in solid samples, which is not suitable for analysis by CheMin. Finally, the isotopic composition of these gases may suggest possible formation scenarios and relationships between phases. We will discuss C isotope ratios of CO2 evolved from the CH sample as measured with SAM's quadrupole mass spectrometer (QMS) and draw comparisons to samples previously analyzed by SAM.

Franz, H. B.↗
NASA NTRS2016

Evidence for a Heterogeneous Distribution of Water in the Martian Interior

The abundance and distribution of H2O within the terrestrial planets, as well as its timing of delivery, is a topic of vital importance for understanding the chemical and physical evolution of planets and their potential for hosting habitable environments. Analysis of planetary materials from Mars, the Moon, and the eucrite parent body (i.e., asteroid 4Vesta) have confirmed the presence of H2O within their interiors. Moreover, H and N isotopic data from these planetary materials suggests H2O was delivered to the inner solar system very early from a common source, similar in composition to the carbonaceous chondrites. Despite the ubiquity of H2O in the inner Solar System, the only destination with any prospects for past or present habitable environments at this time, outside of the Earth, is Mars. Although the presence of H2O within the martian interior has been confirmed, very little is known regarding its abundance and distribution within the martian interior and how the martian water inventory has changed over time. By combining new analyses of martian apatites within a large number of martian meteorite types with previously published volatile data and recently determined mineral-melt partition coefficients for apatite, we report new insights into the abundance and distribution of volatiles in the martian crust and mantle. Using the subset of samples that did not exhibit crustal contamination, we determined that the enriched shergottite mantle source has 36-73 ppm H2O and the depleted shergottite mantle source has 14-23 ppm H2O. This result is consistent with other observed geochemical differences between enriched and depleted shergottites and supports the idea that there are at least two geochemically distinct reservoirs in the martian mantle. We also estimated the H2O content of the martian crust using the revised mantle H2O abundances and known crust-mantle distributions of incompatible lithophile elements. We determined that the bulk martian crust has approximately 1400 ppm H2O, which is likely distributed toward the martian surface. This crustal water abundance would equate to a global equivalent layer (GEL) of water at a depth of-229 m, which can account for at least some of the surface features on Mars attributed to flowing water and may be sufficient to support the past presence of a shallow sea on Mars' surface.

McCubbin, Francis↗
DOE OSTI2021

r-Process Radioisotopes from Near-Earth Supernovae and Kilonovae

The astrophysical sites where r-process elements are synthesized remain mysterious: it is clear that neutron star mergers (kilonovae (KNe)) contribute, and some classes of core-collapse supernovae (SNe) are also possible sources of at least the lighter r-process species. The discovery of 60Fe on the Earth and Moon implies that one or more astrophysical explosions have occurred near the Earth within the last few million years, probably SNe. Intriguingly, 244 Pu has now been detected, mostly overlapping with 60 Fe pulses. However, the 244 Pu flux may extend to before 12 Myr ago, pointing to a different origin. Here, motivated by these observations and difficulties for r-process nucleosynthesis in SN models, we propose that ejecta from a KN enriched the giant molecular cloud that gave rise to the Local Bubble, where the Sun resides. Accelerator mass spectrometry (AMS) measurements of 244 Pu and searches for other live isotopes could probe the origins of the r-process and the history of the solar neighborhood, including triggers for mass extinctions, e.g., that at the end of the Devonian epoch, motivating the calculations of the abundances of live r-process radioisotopes produced in SNe and KNe that we present here. Given the presence of 244 Pu, other r-process species such as 93 Zr, 107 Pd, 129 I, 135 Cs, 182 Hf, 236 U, 237 Np, and 247 Cm should be present. Their abundances and well-resolved time histories could distinguish between the SN and KN scenarios, and we discuss prospects for their detection in deep-ocean deposits and the lunar regolith. We show that AMS 129 I measurements in Fe–Mn crusts already constrain a possible nearby KN scenario.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1988

Mass extinctions, atmospheric sulphur and climatic warming at the K/T boundary

The possible climatic effects of a drastic decrease in cloud condensation nuclei (CCN) associated with a severe reduction in the global marine phytoplankton abundance are investigated. Calculations suggest that a reduction in CCN of more than 80 percent and the resulting decrease in marine cloud albedo could have produced a rapid global warming of 6 C or more. Oxygen isotope analyses of marine sediments from many parts of the world have been interpreted as indicating a marked warming coincident with the demise of calcareous nannoplankton at the K/T boundary. Decreased marine cloud albedo and resulting high sea surface temperatures could have been a factor in the maintenance of low productivity in the 'Strangelove Ocean' period following the K/T extinctions.

Rampino, Michael R.↗
NASA NTRS2004

Chondrules and Isolated Grains in the Fountain Hills Bencubbinite

The Fountain Hills (FH) meteorite was recently classified as a Bencubbin-like (CB(sub a)) chondrite, which are part of the CR clan [1]. The FH O-isotopic composition is indistinguishable from CB(sub a) chondrites. Metal and silicate compositions are consistent with the CB(sub a) classification. Significant differences between FH and the other CB(sub a) chondrites were noted. These include abundant porphyritic chondrules and complete lack of sulfide minerals. We are furthering this investigation by analyzing silicate chondrules and isolated grains in FH to determine more about its composition, thermal history, and implications for chondrule formation in the early solar system.

LaBlue, A. R.↗
NASA NTRS2007

Coordinated Chemical and Isotropic Studies of IDPS: Comparison of Circumstellar and Solar GEMS Grains

Silicate stardust in IDPs and meteorites include forsterite, amorphous silicates, and GEMS grains [1]. Amorphous presolar silicates are much less abundant than expected based on astronomical models [2], possibly destroyed by parent body alteration. A more accurate accounting of presolar silicate mineralogy may be preserved in anhydrous IDPs. Here we present results of coordinated TEM and isotopic analyses of an anhydrous IDP (L2005AL5) that is comprised of crystalline silicates and sulfides, GEMS grains, and equilibrated aggregates embedded in a carbonaceous matrix. Nanometer-scale quantitative compositional maps of all grains in two microtome thin sections were obtained with a JEOL 2500SE. These sections were then subjected to O and N isotopic imaging with the JSC NanoSIMS 50L. Coordinated high resolution chemical maps and O isotopic com-positions were obtained on 11 GEMS grains, 8 crystalline grains, and 6 equilibrated aggregates.

Keller, L. P.↗
NASA NTRS2010

Mineralogy of Pyroxene and Olivine in the Almahata Sitta Ureilite

The Almahata Sitta meteorite (hereafter "Alma") is the first example of a recovered asteroidal sample that fell to earth after detection still in the orbit (2008TC3 asteroid), and thus is critical to understand the relationship between meteorites and their asteroidal parent bodies [1]. Alma is a polymict ureilite showing a fine-grained brecciated texture with variable lithologies from black, porous to denser, white stones [1]. It is an anomalous ureilite because of wide compositional ranges of silicates with abundant pores often coated by vapor-deposit crystals [1]. Nevertheless, Alma has general similarities to all ureilites because of reduction textures of silicates suggestive of rapid cooling from high temperature as well as heterogeneous oxygen isotope compositions [e.g., 1-5]. Alma is especially unique because it spans the compositional range of known ureilites [1]. In this abstract we report detailed mineralogical and crystallographic investigations of two different fragments to further constrain its thermal history with regards to the nature of the ureilite parent body.

Mikouchi, T.↗
NASA NTRS2017

Interpretation of Ferroan Anorthosite Ages and Implications for the Lunar Magma Ocean

Ferroan Anorthosites (FANs) are considered to have purportedly crystallized directly from the lunar magma ocean (LMO) as a flotation crust. LMO modeling suggests that such anorthosites started to form only after greater than 70 percent of the LMO had crystallized. Recent age dates for FANs have questioned this hypothesis as they span too large of an age range. This means a younger age for the Moon-forming giant impact or the LMO hypothesis is flawed. However, FANs are notoriously difficult to age-date using the isochron method. We have proposed a mechanism for testing the LMO hypothesis through using plagioclase trace element abundances to calculate equilibrium liquids and compare them with LMO crystallization models. We now examine the petrography of the samples that have Sm-Nd (Samarium-Neodymium) age dates (Rb-Sr (Rubidium-Strontium) isotopic systematics may have been disturbed) and propose a relative way to age date FANs.

Neal, C. R.↗