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At least 55 records · Page 3

An improved long range potential for O(1D)+H2

Several dynamics studies have indicated that the product isotopic distributions and vibrational energy distributions in the reaction O(1D) + H2(HD) are very sensitive to the long range interaction of the reactants. In this paper, an improved calculation of the reactant region of the potential energy surface is reported. In agreement with previous work, no barrier is found to edge-on insertion (1 A-prime ground state water surface), but a smaller (less than 0.2 kcal/mol) barrier to collinear addition, 1 Sigma (+) surface, is found than in previous work. The long range potential obtained in the present work most closely resembles the SL3 surface.

Walch, Stephen P.↗

Carbon and nitrogen in Type 2 supernova diamonds

Abundant diamonds found in meteorites seem either to have condensed within supernova interiors during their expansions and coolings or to have been present around those explosions. Either alternative allows implantation of Xe-HL prior to interstellar mixing. A puzzling feature is the near normalcy of the carbon isotopes, considering that the only C-rich matter, the He-burning shell, is pure C-12 in that region. That last fact has caused many to associate supernova carbon with C-12 carbon, so that its SUNOCONS have been anticipated as very C-12-rich. We show that this expectation is misleading because the C-13-rich regions of Type 2's have been largely overlooked in this thinking. We here follow the idea that the diamonds nucleated in the C-12-rich He shell, the only C-rich site for nucleation, but then attached C-13-rich carbon during turbulent encounters with overlying C-13-rich matter. That is, the initial diamonds continued to grow during the same collisional encounters that cause the Xe-HL implantation. Instead of interacting with the small carbon mass having 13/12 = 0.2 in the upper He zone, however, we have calculated the remnants of the initial H-burning core, which left behind C-13-rich matter as it receded during core hydrogen burning. Howard et al. described why the velocity mixing would be essential to understanding the implantation of both the Xe-H and Xe-L components. Velocity mixing is now known to occur from the X-ray and gamma-ray light curves of supernova 1987A. Using the stellar evolution code developed at Goettingen, we calculated at Clemson the evolution of a grid of massive stars up to the beginning of core He burning. We paid attention to all H-burning reactions throughout the star, to the treatment of both convection and semiconvection, and to the recession of the outer boundary of the convective H-burning core as the star expands toward a larger redder state. This program was to generate a careful map of the CNO isotope distribution as He burning begins. Our result for the 30 solar mass star is shown.

Clayton, Donald D.↗

The isotopic composition of iron-group galactic cosmic rays

Results from studies of the isotopic composition of iron group elements in the galactic cosmic radiation are reviewed, emphasizing recently reported measurements from the ISEE-3 spacecraft. The observed isotope distributions for the elements Ti through Mn are in good agreement with those expected for a propagated solar-like source composition, with the possible exception of an enhanced abundance of Ti-50. It is found that a significant fraction of the radioactive secondary nuclide Mn-54 has decayed, indicating a confinement time of iron group cosmic rays in the galaxy of at least 2 Myr. The source ratio Fe-54/Fe-56 is found to be consistent with the solar value, but the ratio Ni-60/Ni-58 is greater than solar by a factor of 2.8+/-1.0. The measured abundance of Co-59 is significantly greater than the calculated secondary contribution, suggesting that this nuclide has been produced in the source regions by the electron capture decay of Ni-59 and implying a time delay between nucleosynthesis and acceleration approximately greater than 10(exp 5) yr.

Wiedenbeck, M. E.↗

Mars Solar Balloon Landed Gas Chromatograph Mass Spectrometer

A Mars surface lander Gas Chromatograph Mass Spectrometer (GCMS) is described to measure the chemical composition of abundant and trace volatile species and isotope ratios for noble gases and other elements. These measurements are relevant to the study of atmospheric evolution and past climatic conditions. A Micromission plan is under study where a surface package including a miniaturized GCMS would be delivered to the surface by a solar heated hot air balloon based system. The balloon system would be deployed about 8 km above the surface of Mars, wherein it would rapidly fill with Martian atmosphere and be heated quickly by the sun. The combined buoyancy and parachuting effects of the solar balloon result in a surface package impact of about 5 m/sec. After delivery of the package to the surface, the balloon would ascend to about 4 km altitude, with imaging and magnetometry data being taken for the remainder of the daylight hours as the balloon is blown with the Martian winds. Total atmospheric entry mass of this mission is estimated to be approximately 50 kg, and it can fit as an Ariane 5 piggyback payload. The GCMS would obtain samples directly from the atmosphere at the surface and also from gases evolved from solid phase material collected from well below the surface with a Sample Acquisition and Transport Mechanism (SATM). The experiment envisioned in the Mars Micromission described would obtain samples from a much greater depth of up to one meter below the surface, and would search for organic molecules trapped in ancient stratified layers well below the oxidized surface. Insitu instruments on upcoming NASA missions working in concert with remote sensing measurement techniques have the potential to provide a more detailed investigation of mineralogy and the extent of simple volatiles such as CO2 and H2O in surface and subsurface solid phase materials. Within the context of subsequent mission opportunities such as those provided by the Ariane 5 piggyback payload based Micromissions, it is essential to implement an even broader chemical analysis and to enable a significant extension of previous isotope measurements. Such a development would enhance the presently very active study of questions of atmospheric evolution and loss and past climatic conditions. The method selected to implement this program can be based on well-established mass spectrometry techniques. Sampled gas is chemically and physically processed to separate the gas mixture into components using gas chromatograph and related enrichment techniques. This allows trace species to be identified and reveals isotopic distributions in many cases with improved precision. Samples of interest, such as organic molecules, may lie deep below the highly oxidized surface layer and the suggested program includes enhanced sampling techniques to measure volatiles preserved in solid phase material deep below the surface as well as gas from the well mixed atmosphere.

Mahaffy, P.↗

Assessment of the Interstellar Processes Leading to Deuterium Enrichment in Meteoritic Organics

The presence of isotopic anomalies is the most unequivocal demonstration that meteoritic material contains circumstellar or interstellar components. In the case of organic compounds in meteorites and interplanetary dust particles (IDPs), the most useful isotopic tracer has been deuterium (D). We discuss four processes that are expected to lead to D enrichment in interstellar materials and describe how their unique characteristics can be used to assess their relative importance for the organics in meteorites. These enrichment processes are low temperature gas phase ion-molecule reactions, low temperature gas-grain reactions, gas phase unimolecular photodissociation, and ultraviolet photolysis in D-enriched ice mantles. Each of these processes is expected to be associated with distinct regiochemical signatures (D placement on the product molecules, correlation with specific chemical functionalities, etc.), especially in the molecular population of polycyclic aromatic hydrocarbons (PAHs). We describe these differences and discuss how they may be used to delineate the various interstellar processes that may have contributed to meteoritic D enrichments. We also briefly discuss how these processes may affect the isotopic distributions in C, 0, and N in the same compounds.

Sandford, Scott A.↗

Fe Isotopic Composition of Presolar SiC Mainstream Grains

Iron isotopic distribution was measured in SiC mainstream grains from the Murchison meteorite by time-of-flight resonance ionization mass spectrometry. All grains exhibit 54Fe depletions of 50 to 200, lower than what are predicted by calculations of s-process nucleosynthesis in AGB stars. Additional information is contained in the original extended abstract.

Tripa, C. E.↗

Plume Collection Strategies for Icy World Sample Return

Three icy worlds in the solar system display evidence of pluming activity. Water vapor and ice particles emanate from cracks near the south pole of Saturn's moon Enceladus. The plume gas contains simple hydrocarbons that could be fragments of larger, more complex organics. More recently, observations using the Hubble and Herschel space telescopes have hinted at transient water vapor plumes at Jupiter's moon Europa and the dwarf planet Ceres. Plume materials may be ejected directly from possible sub-surface oceans, at least on Enceladus. In such oceans, liquid water, organics, and energy may co-exist, making these environments habitable. The venting of habitable ocean material into space provides a unique opportunity to capture this material during a relatively simple flyby mission and return it to Earth. Plume collection strategies should enable investigations of evidence for life in the returned samples via laboratory analyses of the structure, distribution, isotopic composition, and chirality of the chemical components (including biomolecules) of plume materials. Here, we discuss approaches for the collection of dust and volatiles during flybys through Enceladus' plume, based on Cassini results and lessons learned from the Stardust comet sample return mission. We also highlight areas where sample collector and containment technology development and testing may be needed for future plume sample return missions.

Stardust Collector↗

Atom Probe Tomography and Three-Dimensional Atomic Scale Characterisation of Interplanetary Dust Particles: Inorganic and Organic, Hydrous and Anhydrous Assemblages

Interplanetary dust particles (IDPs)preserve primordial fragments from our Solar System and external stellar systems, sampled from a vast range of dust forming bodies that often display smaller degrees of parent body processing than is seen in meteorites. IDPs preserve some of the smallest astromaterials from our Solar System, many of which are believed to be among the most important materials for studying physical and chemical processing, and formation mechanisms occurring within the interstellar medium (ISM), Solar Nebula and external planetary systems[1]. However, their formation processes and provenance are poorly constrained, owing in part to spatial resolution limitations of traditional analytical techniques. Atom probe tomography (APT) uses a pulsed laser to field-evaporate material at the atomic scale from needle-shaped samples, and time-of-flight spectrometry for 3D reconstruction of element and isotope distribution in samples after data acquisition. This technique has the highest spatial resolution available of any technique used within the geoscience field[2]. However, measuring multi-phase specimens and porous media in APT can be challenging, two primary characteristics of IDPs. Here we present a custom method for APT needle design and the first results of a 3Datomic scale study of interplanetary dust particles, salt crystals and extraterrestrial insoluble and soluble organic matter designed to overcome the challenges of studying IDP-like materials.

N D Nevill↗

Coordinated Analysis of Isotopically Anomalous Nanoglobules and Insoluble Organic Matter in Quick-Look Samples From Asteroid Bennu

Spectral characterization of B-type asteroid Bennu by the Origins, Spectral Interpretation, Resource Identification, and Security–Regolith Explorer (OSIRIS-REx) spacecraft indicated abundant organic matter with similarities to insoluble organic matter (IOM) in meteorites. IOM in chondritic samples occurs in multiple forms, including a fluffy morphology and submicron-sized rounded nanoglobules. Isotopic anomalies in H, C, and N have been observed in both morphologies and are postulated to result from low-temperature chemical reactions in the molecular cloud or outer protoplanetary disk [e.g., 2,3]. We tested the hypothesis that Bennu also contains such isotopically anomalous organic matter by conducting coordinated in situ analysis of “quick-look” samples collected from the avionics deck of the OSIRIS-REx sample canister. This study expands our understanding of the fundamental nature of Bennu and its pre-accretionary environment by investigating the morphologies and isotopic distribution of presolar organic matter in Bennu.

A N Nguyen↗

Isotopic Ordering in Atmospheric O2 as a Tracer of Ozone Photochemistry and the Tropical Atmosphere

The distribution of isotopes within O2 molecules can be rapidly altered when they react with atomic oxygen. This mechanism is globally important: while other contributions to the global budget of O2 impart isotopic signatures, the O(3P) + O2 reaction resets all such signatures in the atmosphere on subdecadal timescales. Consequently, the isotopic distribution within O2 is determined by O3 photochemistry and the circulation patterns that control where that photochemistry occurs. The variability of isotopic ordering in O2 has not been established, however. We present new measurements of 18O18O in air (reported as delta36 values) from the surface to 33 km altitude. They confirm the basic features of the clumped-isotope budget of O2: Stratospheric air has higher delta36 values than tropospheric air (i.e., more 18O18O), reflecting colder temperatures and fast photochemical cycling of O3. Lower delta36 values in the troposphere arise from photochemistry at warmer temperatures balanced by the influx of high-delta36 air from the stratosphere. These observations agree with predictions derived from the GEOS-Chem chemical transport model, which provides additional insight. We find a link between tropical circulation patterns and regions where delta36 values are reset in the troposphere. The dynamics of these regions influences lapse rates, vertical and horizontal patterns of O2 reordering, and thus the isotopic distribution toward which O2 is driven in the troposphere. Temporal variations in delta36 values at the surface should therefore reflect changes in tropospheric temperatures, photochemistry, and circulation. Our results suggest that the tropospheric O3 burden has remained within a +/-10 percent range since 1978.

oxygen↗

Comparison of dynamic isotope power systems for distributed planet surface applications

Dynamic isotope power system (DIPS) alternatives were investigated and characterized for the surface mission elements associated with a lunar base and subsequent manned Mars expedition. System designs based on two convertor types were studied. These systems were characterized parametrically and compared over the steady-state electrical output power range 0.2 to 20 kWe. Three methods of thermally integrating the heat source and the Stirling heater head were considered, depending on unit size. Figures of merit were derived from the characterizations and compared over the parametric range. Design impacts of mission environmental factors are discussed and quantitatively assessed.

Bents, David J.↗

Microscale Distribution of Hydrogen Isotopes in Two Carbonaceous Chondrites

Hydrogen isotopes are highly variable among primitive meteorites and interplanetary dust particles (IDPs) [1, 2]. In particular, many primitive objects exhibit D (and N-15) enrichments, relative to terrestrial values, thought to represent partial preservation of presolar material fractionated in molecular clouds. However, the diversity of D/H ratios among IDPs and chondrites indicates a complex history of processing in the solar nebula and on meteorite parent bodies. Deconvolving this record requires identification and characterization of the carriers of D enrichments in different objects. Isotopic imaging has proven to be a powerful method to quantitatively explore the distribution of D/H ratios on a one to several m scale in IDPs [2-4] and the CR chondrite Renazzo [5, 6]. In this study, we have used ion imaging to explore the microscale D/H distribution of two carbonaceous chondrites, Tagish Lake (unique) and Al Rais (CR2). Previous D/H measurements (on a ~tens of microns scale) of Tagish Lake matrix fragments by Messenger [7] and Engrand et al. [8] have found different results, most likely related to the analytical techniques used. Previous work has also shown a large range of D/H ratios in CR chondrites, including very large variations on a scale of a few microns [5, 6, 9].

Young, A. F.↗

Isotopic signatures and distribution of nitrogen and trapped and radiogenic xenon in the Acapulco and FRO90011 meteorites

Acapulco metal and silicate show distinct N isotopic signatures. Trapped heavy noble gases are carried by 'magnetic' opx and radiogenic Xe-129 excesses are observed in phosphate and in minor surficial phases on metal grains. N and Xe isotopic signatures in FRO90011 do not agree with those observed in Acapulco. The Acapulco meteorite is unique in having achondritic texture and chondritic composition. Its mineralogical study shows the record of high temperature (1100 C) recrystallization. However, this meteorite shows abundances of volatile elements close to the levels observed in carbonaceous chondrites and concentrations of heavy noble gases comparable to those observed in type 4 ordinary chondrites, not expected for a presumed highly equilibrated object. Nitrogen measurements in bulk Acapulco revealed two different isotopic signatures, in apparent conflict with evidence for a high degree of recrystallization. N and Xe were studied in separated mineral phases to search for the carriers in order to better understand the formation and thermal history of the Acapulco parent body.

Kim, Y.↗

Molecular Distribution, 13C-Isotope, and Enantiomeric Compositions of Carbonaceous Chondrite Monocarboxylic Acids

The water-soluble organic compounds in carbonaceous chondrite meteorites constitute a record of the synthetic reactions occurring at the birth of the solar system and those taking place during parent body alteration and may have been important for the later origins and development of life on Earth. In this present work, we have developed a novel methodology for the simultaneous analysis of the molecular distribution, compound-specific (delta)(exp 13)C, and enantiomeric compositions of aliphatic monocarboxylic acids (MCA) extracted from the hot-water extracts of 16 carbonaceous chondrites from CM, CR, CO, CV, and CK groups. We observed high concentrations of meteoritic MCAs, with total carbon weight percentages which in some cases approached those of carbonates and insoluble organic matter. Moreover, we found that the concentration of MCAs in CR chondrites is higher than in the other meteorite groups, with acetic acid exhibiting the highest concentration in all samples. The abundance of MCAs decreased with increasing molecular weight and with increasing aqueous and/or thermal alteration experienced by the meteorite sample. The (delta)(exp 13)C isotopic values of MCAs ranged from 52 to +27(0/00), and aside from an inverse relationship between (delta)(exp 13)C value and carbon straight-chain length for C3–C6 MCAs in Murchison, the 13C-isotopic values did not correlate with the number of carbon atoms per molecule. We also observed racemic compositions of 2-methylbutanoic acid in CM and CR chondrites. We used this novel analytical protocol and collective data to shed new light on the prebiotic origins of chondritic MCAs.

Aponte, Jose C.↗

Distribution, abundance and carbon isotopic composition of gaseous hydrocarbons in Big Soda Lake, Nevada - An alkaline, meromictic lake

The study of the distribution and isotopic composition of low molecular weight hydrocarbon gases at the Big Soda Lake, Nevada, has shown that while neither ethylene nor propylene were found in the lake, ethane, propane, isobutane and n-butane concentrations all increased with water column depth. It is concluded that methane has a biogenic origin in both the sediments and the anoxic water column, and that C2-C4 alkanes have biogenic origins in the monimolimnion water and shallow sediments. The changes observed in delta C-13/CH4/ and CH4/(C2H6 + C3H8) with depth in the water column and sedimeents are probably due to bacterial processes, which may include anaerobic methane oxidation and different rates of methanogenesis, and C2-to-C4 alkane production by microorganisms.

Oremland, R. S.↗