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PubMed2006

Anharmonic analysis of the vibrational spectra of some cyanides and related molecules of astrophysical importance.

A detailed analysis of the vibrational spectra of carbonyl cyanide, diethynyl ketone and acetyl cyanide has been conducted in harmonic and anharmonic approximations. RHF, MP2 and density functional theory (DFT) methods with 6-311++G(2df,2p) basis sets and B3LYP functionals have been employed. Spectroscopic constants such as anharmonicity constants, rotational and centrifugal distortion constants, rotation-vibration coupling constants and Coriolis coupling coefficients have been calculated for each molecule and compared with the experimental data, where available. A close agreement between the calculated and experimental values of the spectroscopic constants has been obtained. Complete assignments have been provided to the fundamental bands, overtones and combination tones of the molecules. Density functional theory based anharmonic frequencies compare well with the experimental frequencies within +/-18 cm(-1) on an average. RHF and MP2 methods, however, give much higher values for the frequencies that need scaling even in the anharmonic approximation.

Alkynes↗
PubMed1998

Accretion and differentiation of carbon in the early Earth.

The abundance of C in carbonaceous and ordinary chondrites decreases exponentially with increasing shock pressure as inferred from the petrologic shock classification of Scott et al. [Scott, E.R.D., Keil, K., Stoffler, D., 1992. Shock metamorphism of carbonaceous chondrites. Geochim. Cosmochim. Acta 56, 4281-4293] and Stoffler et al. [Stoffler, D., Keil, K., Scott, E.R.D., 1991. Shock metamorphism of ordinary chondrites. Geochim. Cosmochim. Acta 55, 3845-3867]. This confirms the experimental results of Tyburczy et al. [Tyburczy, J.A., Frisch, B., Ahrens, T.J., 1986. Shock-induced volatile loss from a carbonaceous chondrite: implications for planetary accretion. Earth Planet. Sci. Lett. 80, 201-207] on shock-induced devolatization of the Murchison meteorite showing that carbonaceous chondrites appear to be completely devolatilized at impact velocities greater than 2 km s-1. Both of these results suggest that C incorporation would have been most efficient in the early stages of accretion, and that the primordial C content of the Earth was between 10(24) and 10(25) g C (1-10% efficiency of incorporation). This estimate agrees well with the value of 3-7 x 10(24) g C based on the atmospheric abundance of 36Ar and the chondritic C/36Ar (Marty and Jambon, 1987). Several observations suggest that C likely was incorporated into the Earth's core during accretion. (1) Graphite and carbides are commonly present in iron meteorites, and those iron meteorites with Widmanstatten patterns reflecting the slowest cooling rates (mostly Group I and IIIb) contain the highest C abundances. The C abundance-cooling rate correlation is consistent with dissolution of C into Fe-Ni liquids that segregated to form the cores of the iron meteorite parent bodies. (2) The carbon isotopic composition of graphite in iron meteorites exhibits a uniform value of -5% [Deines, P., Wickman, F.E. 1973. The isotopic composition of 'graphitic' carbon from iron meteorites and some remarks on the troilitic sulfur of iron meteorites. Geochim. Cosmochim. Acta 37, 1295-1319; Deines, P., Wickman, F.E., 1975. A contribution to the stable carbon isotope geochemistry of iron meteorites. Geochim. Cosmochim. Acta 39, 547-557] identical to the mode in the distribution found in diamonds, carbonatites and oceanic basalts [Mattey, D.P., 1987. Carbon isotopes in the mantle. Terra Cognita 7, 31-37]. (3) The room pressure solubility of C in molten iron is 4.3 wt% C. Phase equilibria confirm that the Fe-C eutectic persists to 12 GPa, and thermochemical calculations for the Fe-C-S system by Wood [Wood, B.J., 1993. Carbon in the core. Earth Planet. Sci. Lett. 117, 593-607] predict that C is soluble in Fe liquids at core pressures. The abundance of 36Ar in chondrites decreases exponentially with increasing shock pressure as observed for C. It is well known that noble gases are positively correlated and physically associated with C in meteorites [e.g. Otting, W., Zahringer J., 1967. Total carbon content and primordial rare gases in chondrites. Geochim. Cosmochim. Acta 31, 1949-1960; Reynolds, J.H., Frick, U., Niel, J.M., Phinney, D.L., 1978. Rare-gas-rich separates from carbonaceous chondrites. Geochim. Cosmochim. Acta, 42, 1775-1797]. This suggests a mechanism by which primordial He and other noble gases may have incorporated into the Earth during accretion. The abundance of He in the primordial Earth required to sustain the modern He flux for 4 Ga (assuming a planetary 3 He/4 He; Reynolds et al. [Reynolds, J.H., Frick, U., Niel, J.M., Phinney, D.L., 1978. Rare-gas-rich separates from carbonaceous chondrites. Geochim. Cosmochim. Acta 42, 1775-1797] is calculated to be > or = 10(-8) cm3 g-1. This minimum estimate is consistent with a 1-10% efficiency of noble gas retention during accretion and the observed abundance of He in carbonaceous chondrites (10(-5) to 10(-4) cm3 g-1 excluding spallogenic contributions).

Argon↗
PubMed1997

Origin of magnetite in oxidized CV chondrites: in situ measurement of oxygen isotope compositions of Allende magnetite and olivine.

Magnetite in the oxidized CV chondrite Allende mainly occurs as spherical nodules in porphyritic-olivine (PO) chondrules, where it is associated with Ni-rich metal and/or sulfides. To help constrain the origin of the magnetite, we measured oxygen isotopic compositions of magnetite and coexisting olivine grains in PO chondrules of Allende by an in situ ion microprobe technique. Five magnetite nodules form a relatively tight cluster in oxygen isotopic composition with delta 18O values from -4.8 to -7.1% and delta 17O values from -2.9 to -6.3%. Seven coexisting olivine grains have oxygen isotopic compositions from -0.9 to -6.3% in delta 18O and from -4.6 to -7.9% in delta 17O. The delta 17O values of the magnetite and coexisting olivine do not overlap; they range from -0.4 to -2.6%, and from -4.0 to -5.7%, respectively. Thus, the magnetite is not in isotopic equilibrium with the olivine in PO chondrules, implying that it formed after the chondrule formation. The delta 17O of the magnetite is somewhat more negative than estimates for the ambient solar nebula gas. We infer that the magnetite formed on the parent asteroid by oxidation of metal by H2O which had previously experienced minor O isotope exchange with fine-grained silicates.

Ferrosoferric Oxide↗
PubMed1998

Preservation of extraterrestrial 3He in 480-Ma-old marine limestones.

We have measured the helium abundance and isotopic composition of a suite of Lower Ordovician marine limestones and associated fossil meteorites from Kinnekulle, Sweden. Limestone 3He/4He ratios as high as 11.5 times the atmospheric value in fused samples and up to 23 times atmospheric in a single step-heat fraction indicate the presence of extraterrestrial helium, and demonstrate that at least a fraction of the extraterrestrial 3He carried by interplanetary dust particles must be retained against diffusive and diagenetic losses for up to 480 Ma. The carrier phase has not been identified but is not magnetic. Extrapolation of high-temperature 3He diffusivities in these sediments is consistent with strong retention of extraterrestrial 3He under ambient Earth-surface conditions. Combination of the observed helium concentrations with sedimentation rates estimated from conodont biostratigraphy suggest that the flux of extraterrestrial 3He in the Early Ordovician was about 0.5 x 10(-12) cm3 STP cm-2 ka-1, ignoring potential post-deposition helium loss. This value is indistinguishable from the average 3He flux estimated for the Cenozoic Era. In contrast, previous studies of fossil meteorites, Ir abundances, and Os isotopic ratios in the limestone suggest that the total accretion rate of extraterrestrial material during the studied interval was at least an order of magnitude higher than the Cenozoic average. This disparity may reflect significant post-depositional loss of 3He from IDPs within these old limestones; if so, the match between the Ordovician flux and the Cenozoic average would be fortuitous. Alternatively, the size distribution of infalling objects during the Early Ordovician may have been enriched only in extraterrestrial material too large to retain 3He during atmospheric entry heating (> approximately 30 micrometers). The fossil meteorites themselves also preserve extraterrestrial helium. Meteorite 3He concentrations of 2 to 9 x 10(-12) cm3 STP g-1 are several orders of magnitude lower than found in most modern meteorites, suggesting very substantial helium loss (probably >99.9%) from these chemically altered objects. The Meteorites carry 3He concentrations only a factor of a few higher than the host limestones. The meteorites themselves cannot be the source of the extraterrestrial 3He observed in the limestones.

Calcium Carbonate↗
PubMed1999

The origin of organic matter in the Martian meteorite ALH84001.

Stable carbon isotope measurements of the organic matter associated with the carbonate globules and the bulk matrix material in the ALH84001 Martian meteorite indicate that two distinct sources are present in the sample. The delta 13C values for the organic matter associated with the carbonate globules averaged -26% and is attributed to terrestrial contamination. In contrast, the delta 13C values for the organic matter associated with the bulk matrix material yielded a value of -15%. The only common sources of carbon on the Earth that yield similar delta 13C values, other then some diagenetically altered marine carbonates, are C4 plants. A delta 13C value of -15%, on the other hand, is consistent with a kerogen-like component, the most ubiquitous form of organic matter found in carbonaceous chondrites such as the Murchison meteorite. Examination of the carbonate globules and bulk matrix material using laser desorption mass spectrometry (LDMS) indicates the presence of a high molecular weight organic component which appears to be extraterrestrial in origin, possibly derived from the exogenous delivery, of meteoritic or cometary debris to the surface of Mars.

Antarctic Regions↗
PubMed2000

Bacteria in the Tatahouine meteorite: nanometric-scale life in rocks.

We present a study of the textural signature of terrestrial weathering and related biological activity in the Tatahouine meteorite. Scanning and transmission electron microscopy images obtained on the weathered samples of the Tatahouine meteorite and surrounding soil show two types of bacteria-like forms lying on mineral surfaces: (1) rod-shaped forms (RSF) about 70-80 nm wide and ranging from 100 nm to 600 nm in length; (2) ovoid forms (OVF) with diameters between 70 and 300 nm. They look like single cells surrounded by a cell wall. Only Na, K, C, O and N with traces of P and S are observed in the bulk of these objects. The chemical analyses and electron diffraction patterns confirm that the RSF and OVF cannot be magnetite or other iron oxides, iron hydroxides, silicates or carbonates. The sizes of the RSF and OVF are below those commonly observed for bacteria but are very similar to some bacteria-like forms described in the Martian meteorite ALH84001. All the previous observations strongly suggest that they are bacteria or their remnants. This conclusion is further supported by microbiological experiments in which pleomorphic bacteria with morphology similar to the OVF and RSF objects are obtained from biological culture of the soil surrounding the meteorite pieces. The present results show that bacteriomorphs of diameter less than 100 nm may in fact represent real bacteria or their remnants.

Bacteria↗
PubMed2000

The role of vaterite and aragonite in the formation of pseudo-biogenic carbonate structures: implications for Martian exobiology.

A simple synthesis of various forms of calcium carbonate with spherical and 'floral' morphologies is reported. Vaterite formation occurs at approximately 25 degrees C, aragonite at approximately 70 degrees C and calcite at about approximately 80 degrees C. These are produced when CO2 is reacted with an aqueous solution of calcium chloride in the presence of ammonia. These conditions may have existed at the surface of Mars in the past, leading us to conclude that such mineral formations may be common there. Although the initial phases are modified over time with changing temperature and pressure conditions, they still influence the final morphology of the carbonates observed. A comparison of these structures with those found in the Martian meteorite ALH84001 suggests, but does not confirm, a non-biogenic origin for the ALH84001 carbonates.

Calcium Carbonate↗
PubMed2000

Elongated prismatic magnetite crystals in ALH84001 carbonate globules: potential Martian magnetofossils.

Using transmission electron microscopy (TEM), we have analyzed magnetite (Fe3O4) crystals acid-extracted from carbonate globules in Martian meteorite ALH84001. We studied 594 magnetites from ALH84001 and grouped them into three populations on the basis of morphology: 389 were irregularly shaped, 164 were elongated prisms, and 41 were whisker-like. As a possible terrestrial analog for the ALH84001 elongated prisms, we compared these magnetites with those produced by the terrestrial magnetotactic bacteria strain MV-1. By TEM again, we examined 206 magnetites recovered from strain MV-1 cells. Natural (Darwinian) selection in terrestrial magnetotactic bacteria appears to have resulted in the formation of intracellular magnetite crystals having the physical and chemical properties that optimize their magnetic moment. In this study, we describe six properties of magnetite produced by biologically controlled mechanisms (e.g., magnetotactic bacteria), properties that, collectively, are not observed in any known population of inorganic magnetites. These criteria can be used to distinguish one of the modes of origin for magnetites from samples with complex or unknown histories. Of the ALH84001 magnetites that we have examined, the elongated prismatic magnetite particles (similar to 27% of the total) are indistinguishable from the MV-1 magnetites in five of these six characteristics observed for biogenically controlled mineralization of magnetite crystals.

Biomarkers↗
PubMed1997

The primitive matrix components of the unique carbonaceous chondrite Acfer 094: a TEM study.

The mineralogical and chemical characteristics of the fine-grained matrix (< or = 3 micrometers) of the unique primitive carbonaceous chondrite Acfer 094 have been investigated in detail by scanning electron microscopy (SEM) and analytical transmission electron microscopy (ATEM). Generally, the fine-grained matrix represents a highly unequilibrated assemblage of an amorphous material, small forsteritic olivines (200-300 nm), low Ca-pyroxenes (300-400 nm), and Fe,Ni-sulfides (100-300 nm). The matrix is basically unaffected by secondary processes. Only minor amounts of serpentine and ferrihydrite, as products of hydrous alteration, are present. Texturally, the amorphous material acts as a groundmass to olivines, pyroxenes, and sulfides, mostly exhibiting rounded or elongated morphologies. Only very few clastic mineral grains have been found. The texture and chemical composition of the amorphous material are consistent with an origin by disequilibrium condensation in either the cooling solar nebula or a circumstellar environment. As such, the amorphous material may be considered as a possible precursor of matrix materials in other types of chondrites. The non-clastic matrix olivines (Fo98-99) and pyroxenes (En97-100) are suggested to have formed either by condensation in the solar nebula under highly oxidizing conditions or by recrystallization from the amorphous material. The formation of these grains by fragmentation of chondrule components is unlikely due to chemical and microstructural reasons. Rapid cooling caused the observed intergrowths of clino/orthoenstatite in the Mg-rich matrix pyroxenes. Although some similarities exist comparing the fine-grained matrix of Acfer 094 with the matrices of the unequilibrated CO3 chondrite ALHA77307 and the unique type 3 chondrite Kakangari, Acfer 094 remains unique. Since it contains the highest measured concentrations of circumstellar SiC and the second highest of diamond (highest is Orgueil), it seems reasonable to suggested that at least parts of the amorphous material in the fine-grained matrix may be of circumstellar origin.

Carbon↗
PubMed1996

Magnetite whiskers and platelets in the ALH84001 Martian meteorite: evidence of vapor phase growth.

Nanometer-sized magnetite crystals associated with carbonates in fracture zones within Martian meteorite ALH84001 have been examined using analytical transmission electron microscopy. Some of the crystals exhibit distinctive morphologies: filamentary rods and ribbon, and platelets. The rods and ribbons are elongated along the crystallographic [100] and [111] directions. Some of the rods contain microstructural defects indicating that they grew by spiral growth about screw dislocations. Platelets are flattened along the [100] and [110] directions. These unique morphologies and microstructures constrain the growth conditions of magnetite. The whiskers and platelets most likely formed in the temperature range 500-800 degrees C by direct condensation from a vapor or precipitation from a supercritical fluid, and their properties are inconsistent with a biogenic origin.

Carbonates↗
PubMed1997

Polycyclic aromatic hydrocarbons (PAHs) in Antarctic Martian meteorites, carbonaceous chondrites, and polar ice.

Recent analyses of the carbonate globules present in the Martian meteorite ALH84001 have detected polycyclic aromatic hydrocarbons (PAHs) at the ppm level (McKay et al., 1996). The distribution of PAHs observed in ALH84001 was interpreted as being inconsistent with a terrestrial origin and were claimed to be indigenous to the meteorite, perhaps derived from an ancient martian biota. We have examined PAHs in the Antarctic shergottite EETA79001, which is also considered to be from Mars, as well as several Antarctic carbonaceous chondrites. We have found that many of the same PAHs detected in the ALH84001 carbonate globules are present in Antarctic carbonaceous chondrites and in both the matrix and carbonate (druse) component of EETA79001. We also investigated PAHs in polar ice and found that carbonate is an effective scavenger of PAHs in ice meltwater. Moreover, the distribution of PAHs in the carbonate extract of Antarctic Allan Hills ice is remarkably similar to that found in both EETA79001 and ALH84001. The reported presence of L-amino acids of apparent terrestrial origin in the EETA79001 druse material (McDonald and Bada, 1995) suggests that this meteorite is contaminated with terrestrial organics probably derived from Antarctic ice meltwater that had percolated through the meteorite. Our data suggests that the PAHs observed in both ALH84001 and EETA79001 are derived from either the exogenous delivery of organics to Mars or extraterrestrial and terrestrial PAHs present in the ice meltwater or, more likely, from a mixture of these sources. It would appear that PAHs are not useful biomarkers in the search for extinct or extant life on Mars.

Antarctic Regions↗
PubMed1997

Petrography and bulk chemistry of Martian orthopyroxenite ALH84001: implications for the origin of secondary carbonates.

New petrologic and bulk geochemical data for the SNC-related (Martian) meteorite ALH84001 suggest a relatively simple igneous history overprinted by complex shock and hydrothermal processes. ALH84001 is an igneous orthopyroxene cumulate containing penetrative shock deformation textures and a few percent secondary extraterrestrial carbonates. Rare earth element (REE) patterns for several splits of the meteorite reveal substantial heterogeneity in REE abundances and significant fractionation of the REEs between crushed and uncrushed domains within the meteorite. Complex zoning in carbonates indicates nonequilibrium processes were involved in their formation, suggesting that CO2-rich fluids of variable composition infiltrated the rock while on Mars. We interpret petrographic textures to be consistent with an inorganic origin for the carbonate involving dissolution-replacement reactions between CO2-charged fluids and feldspathic glass in the meteorite. Carbonate formation clearly postdated processes that last redistributed the REE in the meteorite.

Carbon Dioxide↗
PubMed1997

Modification of amino acids at shock pressures of 3.5 to 32 GPa.

Amino acids were subjected to shock impact over a pressure range of 3.5 to 32 GPa both within and without meteoritic mineral matrices. The extent of amino acid destruction, racemization, and conversion to secondary amino acids was examined. Abundances of parent compounds decreased by a factor of 10(3) over this pressure range. Racemization also occurred, but some residual optical activity remained in the amino acids surviving shocks up to 32 GPa. Secondary amino acids formed in the high peak pressure range; those identified were beta-alanine, glycine, alanine, gamma-aminobutyric acid, and beta-aminoisobutyric acid. At 30 GPa, the abundances of these daughter compounds exceeded those of the remaining initial amino acids. As the concomitant effects of high mechanical stress and temperature accompanying shocks cannot be separated in this work, their relative contribution to the observed transformations cannot be estimated. The survival of amino acids in shock experiments suggests that, after formation or emplacement of amino acids in carbonaceous chondrite parent bodies, these objects never experienced impact velocities greater than 5 km/s, which suffices to generate 30 GPa for typical silicate/silicate impacts. These results also provide guidelines for choosing appropriate capture media for interplanetary dust particles on Earth-orbiting platforms.

Aluminum↗
PubMed1997

Ar-Ar chronology of the Martian meteorite ALH84001: evidence for the timing of the early bombardment of Mars.

ALH84001, a cataclastic cumulate orthopyroxenite meteorite from Mars, has been dated by Ar-Ar stepped heating and laser probe methods. Both methods give ages close to 3,900 Ma. The age calculated is dependent on assumptions made about 39Ar recoil effects and on whether significant quantities of 40Ar from the Martian atmosphere are trapped in the meteorite. If, as suggested by xenon and nitrogen isotope studies, Martian atmospheric argon is present, then it must reside predominantly in the K-rich phase maskelynite. Independently determined 129Xe abundances in the maskelynite can be used to place limits on the concentration of the atmospheric 40Ar. These indicate a reduction of around 80 Ma to ages calculated on the assumption that no Martian atmosphere is present. After this correction, the nominal ages obtained are: 3940 +/- 50, 3870 +/- 80, and 3970 +/- 100 Ma. by stepped heating, and 3900 +/- 90 Ma by laser probe (1 sigma statistical errors), giving a weighted mean value of 3,920 Ma. Ambiguities in the interpretation of 39Ar recoil effects and in the contribution of Martian atmospheric 40Ar lead to uncertainties in the Ar-Ar age which are difficult to quantify, but we suggest that the true value lies somewhere between 4,050 and 3,800 Ma. This age probably dates a period of annealing of the meteorite subsequent to the shock event which gave it its cataclastic texture. The experiments provide the first evidence of an event occurring on Mars coincident with the time of the late heavy bombardment of the Moon and may reflect a similar period of bombardment in the Southern Highlands of Mars. Whether the age determined bears any relationship to the time of carbonate deposition in ALH84001 is not known. Such a link depends on whether the temperature associated with the metasomatic activity was sufficient to cause argon loss from the maskelynite and/or whether the metasomatism and metamorphism were linked in time through a common heat source.

Argon↗
PubMed2000

Non-racemic amino acids in the Murray and Murchison meteorites.

Small (1.0-9.2%) L-enantiomer excesses were found in six alpha-methyl-alpha-amino alkanoic acids from the Murchison (2.8-9.2%) and Murray (1.0-6.0%) carbonaceous chondrites by gas chromatography-mass spectroscopy of their N-trifluoroacetyl or N-pentafluoropropyl isopropyl esters. These amino acids [2-amino-2,3-dimethylpentanoic acid (both diastereomers), isovaline, alpha-methyl norvaline, alpha-methyl valine, and alpha-methyl norleucine] are either unknown or rare in the terrestrial biosphere. Enantiomeric excesses were either not observed in the four alpha-H-alpha-amino alkanoic acids analyzed (alpha-amino-n-butyric acid, norvaline, alanine, and valine) or were attributed to terrestrial contamination. The substantial excess of L-alanine reported by others was not found in the alanine in fractionated extracts of either meteorite. The enantiomeric excesses reported for the alpha-methyl amino acids may be the result of partial photoresolution of racemic mixtures caused by ultraviolet circularly polarized light in the presolar cloud. The alpha-methyl-alpha-amino alkanoic acids could have been significant in the origin of terrestrial homochirality given their resistance to racemization and the possibility for amplification of their enantiomeric excesses suggested by the strong tendency of their polymers to form chiral secondary structure.

Amino Acids↗
PubMed2000

Gas chromatography for in situ analysis of a cometary nucleus. II. Analysis of permanent gases and light hydrocarbons with a carbon molecular sieve porous layer open tubular column.

Considering the severe constraints of space instrumentation, a great improvement for the in situ gas chromatographic (GC) determination of permanent and noble gases in a cometary nucleus is the use of a new carbon molecular sieve porous layer open tubular (PLOT) column called Carbobond. No exhaustive data dealing with this column being available, studies were carried out to entirely characterize its analytical performances, especially when used under the operating conditions of the cometary sampling and composition (COSAC) experiment of the European Space Agency (ESA) Rosetta space mission to be launched in 2003 for a rendezvous with comet 46 P/Wirtanen in 2011. The high efficiency and speed of analysis of this column at both atmospheric and vacuum outlet column pressure is demonstrated, and the kinetic mass transfer contribution of this carbon molecular sieve adsorbent is calculated. Besides, differential adsorption enthalpies of several gases and light hydrocarbons were determined from the variation of retention volume with temperature. The data indicate close adsorption behaviors on the Carbobond porous layer adsorbent and on the carbon molecular sieve Carboxen support used to prepare the packed columns. Moreover, taking into account the in situ operating conditions of the experiment, a study of two columns with different porous layer thicknesses allowed one to optimize the separation of the target components and to select the column parameters compatible with the instrument constraints. Comparison with columns of similar selectivity shows that these capillary columns are the first ones able to perform the same work as the packed and micro-packed columns dedicated to the separation of this range of compounds in GC space exploration.

Adsorption↗
PubMed2002

Gas chromatography for in situ analysis of a cometary nucleus III. Multi-capillary column system for the cometary sampling and composition experiment of the Rosetta lander probe.

The cometary sampling and composition (COSAC) experiment is one of the principal experiments of the surface lander probe of the European Space Agency Rosetta mission to be launched in January 2003. The instrument is designed for the in situ chemical analysis of a cometary nucleus as the details of the nucleus composition are of primary importance for understanding both the formation of the solar system, and the origin of life on Earth. The COSAC experiment consists of an evaporation/pyrolysis device and two analytical systems: a multi-column gas chromatograph and a high-resolution time-of-flight mass spectrometer which may either be operated alone or in a coupled mode. The gas chromatograph includes five general purpose chromatographic columns and three chiral ones, all mounted in parallel. Taking into account the chemical species potentially present in the cometary nucleus as well as the space constraints, a set of five complementary columns was selected to perform the separation and identification of the compounds present in the cometary nucleus. This set of columns includes a carbon molecular sieve porous-layer open tubular (PLOT) column used for the separation of both the noble and other permanent gases, and the C1-C2 hydrocarbons. A second PLOT column uses a divinylbenzene-ethylene glycol-dimethylacrylate porous polymer as stationary phase for the analysis of a wide range of C1-C2 organic molecules, Two complementary wall-coated open tubular (WCOT) columns with polydimethylsiloxane (PDMS) liquid stationary phases, one containing cyanopropyl-phenylsiloxane and the other diphenylsiloxane groups, are designed to target the same range of organic compounds (C3-C7) which could be representative of the widest range of cometary compounds. A third WCOT column with an apolar stationary phase made of non-substituted PDMS is used for the separation and identification of higher-molecular-mass compounds (up to C10) and aromatic species (monoaromatic and polyaromatic). This paper describes these five general-purpose capillary PLOT and WCOT columns, selected to be used in the COSAC GC system. The analytical capabilities are examined with a special emphasis on the exobiological and planetological implications.

Chromatography, Gas↗
PubMed2002

Gas chromatography for in situ analysis of a cometary nucleus. IV. Study of capillary column robustness for space application.

As part of the development of the European Space Agency Rosetta space mission to investigate a cometary nucleus, the selection of columns dedicated to the gas chromatographic subsystem of the Cometary Sampling and Composition (COSAC) experiment was achieved. Once the space probe launched, these columns will be exposed to the harsh environmental constraints of space missions: vibrations, radiation (by photons or energetic particles), space vacuum, and large temperature range. In order to test the resistance of the flight columns and their stationary phases, the columns were exposed to these rough conditions reproduced in the laboratory. The comparison of the analytical performances of the columns, evaluated prior and after the environmental tests, demonstrated that all the columns withstand space constraints, and that their analytical properties were preserved. Therefore, all the selected capillary columns, even having porous layer or chiral stationary phases, were qualified for space exploration.

Chromatography, Gas↗