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1.
Saturn's moon Titan has been considered as one of the few places in our Solar System, where atmospheric and surface conditions could have produced organic compounds essential as precursors for an evolution of life. The Cassini-Huygens mission has provided new data on Titan's atmosphere and surface, which enabled us to simulate the chemical processes occurring under these conditions. Possible lightning events on Titan cannot only produce higher hydrocarbons, but also allow surface water ice to participate in the reaction scenario, resulting in CHO, CHN, and CHON compounds including several molecules relevant for the formation of amino acids and nucleic acids.  相似文献   

2.
Ultraviolet spectral reflectance properties (200-400 nm) of a large number of minerals known or presumed to exist on the surfaces of Mars, the Moon, and asteroids, and in many meteorites, were investigated. Ultraviolet reflectance spectra (200-400 nm) of these minerals range from slightly blue-sloped (reflectance decreasing toward longer wavelengths) to strongly red-sloped (reflectance increasing toward longer wavelengths). Most exhibit one or two absorption features that are attributable to FeO charge transfers involving Fe3+ or Fe2+. The UV region is a very sensitive indicator of the presence of even trace amounts (<0.01 wt%) of Fe3+ and Fe2+. The major Fe3+O absorption band occurs at shorter wavelengths (∼210-230 nm), and is more intense than the major Fe2+O absorption band (∼250-270 nm). Ti-bearing minerals, such as ilmenite, rutile and anatase exhibit UV absorption bands attributable to Ti4+O charge transfers. While the positions of metal-O charge transfer bands sometimes differ for different minerals, the variation is often not diagnostic enough to permit unique mineral identification. However, iron oxides and oxyhydroxides can generally be distinguished from Fe-bearing silicates in the 200-400 nm region on the basis of absorption band positions. Within a given mineral group (e.g., low-calcium pyroxene, olivine, plagioclase feldspar), changes in Fe2+ or Fe3+ abundance do not appear to result in a measurable change in absorption band minima positions. Absorption band positions can vary as a function of grain size, however, and this variation is likely due to band saturation effects. The intensity of metal-O charge transfers means that some minerals will exhibit saturated UV absorption bands even for fine-grained (<45 μm) powders. In cases where absorption bands are not saturated (e.g., Fe2+O bands in some plagioclase feldspars and pyroxenes), changes in Fe2+ content do not appear to cause variations in band position. In other minerals (e.g., olivine), changes in band positions are correlated with compositional and/or grain size variations, but this is likely due to increasing band saturation rather than compositional variations. Overall, we find that the UV spectral region is sensitive to different mineral properties than longer wavelength regions, and thus offers the potential to provide complementary capabilities and unique opportunities for planetary remote sensing.  相似文献   

3.
Denis Lacelle  David Fisher 《Icarus》2008,197(2):458-469
In this study, various approaches that can potentially distinguish between vapor- and liquid-derived ground ice in the martian regolith (petrography, geochemistry, stable OH isotopes, CO2O2N2Ar gas composition) are examined using terrestrial ground ice examples. Although the stable OH isotope composition ratios can distinguish between vapor- and liquid-derived terrestrial ground ice, there might be to much mixing between the various water reservoirs on Mars to effectively use it, and, like on Earth, petrographic and geochemical approaches need to be complemented with additional supporting evidences. Of the different approaches currently being employed to determine the origin of terrestrial massive ground ice and icy sediments, it is the concentration of CO2 and the O2/Ar, N2/Ar and N2/O2 ratios of air entrapped in the ice that has proven to be the less ambiguous and most discriminatory. This is because the molar ratios of atmospheric gases change during their dissolution in water due to differences in their relative solubilities, thus providing distinctive ratios for the dissolved gases. The gas composition of air entrapped in the ice not only distinguishes between vapor- and liquid-derived ground ice, but any deviation from the theoretical dissolved values can provide insights into potential physical and biological processes operating in the subsurface, a key component for astrobiology.  相似文献   

4.
Material of low geometric albedo (pV?0.1) is found on many objects in the outer Solar System, but its distribution in the saturnian satellite system is of special interest because of its juxtaposition with high-albedo ice. In the absence of clear, diagnostic spectral features, the composition of this low-albedo (or “dark”) material is generally inferred to be carbon-rich, but the form(s) of the carbon is unknown. Near-infrared spectra of the low-albedo hemisphere of Saturn's satellite Iapetus were obtained with the Visible-Infrared Mapping Spectrometer (VIMS) on the Cassini spacecraft at the fly-by of that satellite of 31 December 2004, yielding a maximum spatial resolution on the satellite's surface of ∼65 km. The spectral region 3-3.6 μm reveals a broad absorption band, centered at 3.29 μm, and concentrated in a region comprising about 15% of the low-albedo surface area. This is identified as the CH stretching mode vibration in polycyclic aromatic hydrocarbon (PAH) molecules. Two weaker bands attributed to CH2 stretching modes in aliphatic hydrocarbons are found in association with the aromatic band. The bands most likely arise from aromatic and aliphatic units in complex macromolecular carbonaceous material with a kerogen- or coal-like structure, similar to that in carbonaceous meteorites. VIMS spectra of Phoebe, encountered by Cassini on 11 June 2004, also show the aromatic hydrocarbon band, although somewhat weaker than on Iapetus. The origin of the PAH molecular material on these two satellites is unknown, but PAHs are found in carbonaceous meteorites, cometary dust particles, circumstellar dust, and interstellar dust.  相似文献   

5.
The H2CO production rates measured in Comet C/1995 O1 (Hale-Bopp) from radio wavelength observations [Biver, N., and 22 colleagues, 2002a. Earth Moon Planets 90, 5-14] showed a steep increase with decreasing heliocentric distance. We studied the heliocentric evolution of the degradation of polyoxymethylene (formaldehyde polymers: (CH2O)n, also called POM) into gaseous H2CO. POM decomposition can indeed explain the H2CO density profile measured in situ by Giotto spacecraft in the coma of Comet 1P/Halley, which is not compatible with direct release from the nucleus [Cottin, H., Bénilan, Y., Gazeau, M.-C., Raulin, F., 2004. Icarus 167, 397-416]. We show that the H2CO production curve measured in Comet C/1995 O1 (Hale-Bopp) can be accurately reproduced by this mechanism with a few percents by mass of solid POM in grains. The steep heliocentric evolution is explained by the thermal degradation of POM at distances less than 3.5 AU. This study demonstrates that refractory organics present in cometary dust can significantly contribute to the composition of the gaseous coma. POM, or POM-like polymers, might be present in cometary grains. Other molecules, like CO and HNC, might also be produced by a similar process.  相似文献   

6.
A number of mineral species were exposed to martian surface conditions of atmospheric pressure and composition, temperature, and UV light regime, and their evolution was monitored using reflectance spectroscopy. The stabilities for different groups varied widely. Phyllosilicate spectra all showed measurable losses of interlayer H2O, with some structural groups showing more rapid H2O loss than others. Loss of OH from the phyllosilicates is not always accompanied by a change in metal-OH overtone absorption bands. OH-bearing sulfates, such as jarosite and alunite, show no measurable change in spectral properties, suggesting that they should be spectrally detectable on Mars on the basis of diagnostic absorption bands in the 0.4-2.5 μm region. Fe3+- and H2O-bearing sulfates all showed changes in the appearance and/or reduction in depths of hydroxo-bridged Fe3+ absorption bands, particularly at 0.43 μm. The spectral changes were often accompanied by visible color changes, suggesting that subsurface sulfates exposed to the martian surface environment may undergo measurable changes in reflectance spectra and color over short periods of time (days to weeks). Organic-bearing geological materials showed no measurable change in CH related absorption bands, while carbonates and hydroxides also showed no systematic changes in spectral properties. The addition of ultraviolet irradiation did not seem to affect mineral stability or rate of spectral change, with one exception (hexahydrite). In some cases, spectral changes could be related to the formation of specific new phases. The data also suggest that hydrated minerals detected on Mars to date retain their diagnostic spectral properties that allow their unique identification.  相似文献   

7.
David E. Woon  Jin-Young Park 《Icarus》2009,202(2):642-680
Barrierless reactions between unsaturated hydrocarbons and the ethynyl radical (C2H) can contribute to the growth of organic particulates in the haze-forming regions of Titan's atmosphere as well as in the gas giants and in the interstellar medium. We employed a combination of quantum chemistry and statistical rate theories to characterize reactions between ground state C2H and seven alkenes of the general structure R1R2C′C″R3R4 containing up to six carbons. The alkenes included ethene (C2H4); propene (C3H6); 1-butene, 2-butene, and isobutene (C4H8); trimethylethene (C5H10); and tetramethylethene (C6H12). Density functional theory calculations at the B3LYP/6-31 + G∗∗ level were used to characterize the adducts, isomers, products, and the intervening transition states for the addition-elimination reactions of all seven species. A multiple-well treatment was then employed to determine the outcome distributions for the range of temperatures and pressures relevant to Titan's atmosphere, the interstellar medium, and the outer atmospheres of the gas giants. Finally, trajectory calculations using an ROMP2 potential energy surface were used to calculate kinetic rates for the ethene + C2H reaction, where the agreement between the computed and measured values is very good. At low pressure and temperature, vinyl acetylene is a dominant product of several of the reactions, and all of the reactions yield at least one dominant product with both a double and a triple CC bond.  相似文献   

8.
Powdered samples of carbon-nitrogen-hydrogen “tholins” that mimic Titan's atmosphere aerosols were produced under levitation conditions in the laboratory with a dusty plasma (PAMPRE experiment) using different initial N2:CH4 gas mixtures and studied using UV Raman and infrared spectroscopy, X-ray diffraction and high resolution transmission electron microscopy (HRTEM). Comparison between the tholins produced in the PAMPRE experiments and samples prepared by other techniques reveal that they form a fairly homogeneous family of hydrogenated carbon nitride materials. Wall effects during the PAMPRE deposition experiments and other were found to have little effect on the chemical structure of tholins. The first-order UV Raman bands of the disordered carbonaceous materials point to a large contribution of sp2 clusters present compared with olefinic CN or CC groupings, whereas features at 690 and 980 cm−1 suggest C3N3 rings are present as a species inserted in the macromolecular network. Diffraction techniques do not indicate the presence of large polyaromatic species in any of the tholins studied, whatever their nitrogen concentration, in disagreement with certain previous observations. This precludes the idea that the nature and degree of absorption in the visible range is controlled by the size of polyaromatic species, as has been observed in series of carbon-based materials obtained via thermal processing. Infrared spectroscopy analysis of the tholins has confirmed earlier identifications of chemical groups present including primary amines, nitriles, and alkyl moieties such as CH2/CH3, but has ruled out CH2/CH3 branches appearing on secondary or tertiary amines. Similar analyses were also performed on a polymeric (HCN)x material, which was found to present several similarities with the tholins, hence suggesting similar polymerization processes.  相似文献   

9.
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10.
We report a study on the broadband ultraviolet photolysis of methane-water ice mixtures, at low methane concentrations and temperatures relevant to the icy satellites of the outer Solar System. The photochemistry of these mixtures is dominated by the action of hydroxyl radicals on methane and the resulting products. This implies that, given sufficient exposure time, the methane will eventually be completely oxidized to carbon dioxide. The presence of methane inhibits the formation of hydrogen peroxide by serving as a trap for hydroxyl radicals. The distribution of photochemical products is broadly similar to that previously conducted using ion and electron sources, with some differences possibly attributable to the difference in radiation source. The results are applicable to a variety of icy bodies in the Solar System. On Enceladus, where methane mixed with water is measured in the plumes, methane in the surface ices is subject to oxidation and will eventually be converted to CO2. The CH stretch feature detected in the VIMS spectra of the Enceladus surface ice suggests that methane is currently being supplied to the surface ice, likely from re-condensation of the plume gas.  相似文献   

11.
Zagami, a well characterized SNC meteorite, represents a reference sample to verify the feasibility of the non-destructive infrared micro-spectroscopy technique to extract spectral signatures from individual mineral phases in a meteorite sample. For the first time individual infrared spectra of the major mineral phases, in the 6000-600 cm−1 (1.67-16.7 μm) spectral interval, whose identification is confirmed by energy dispersive X-ray analysis and backscattered imaging, are measured. The signatures of the main mineral phases we identified in the Zagami chip are: (1) maskelynite characterized by broad and smooth SiO vibrational bands in the 1000 cm−1 spectral region; (2) crystalline pyroxenes showing well defined fine structures; and (3) an oxide mineral phase with an almost featureless and flat spectrum. In the part of the spectrum centered around 2 μm, by analyzing the different positions of the Fe2+ bands, we were able to discern the high-Ca from the low-Ca pyroxene phases. This result demonstrates that by means of the infrared micro-spectroscopy technique it is possible to retrieve directly the composition of pyroxenes in the En-Fs-Wo system, without relying on the use of deconvolution techniques. In addition IR signatures due to water and aliphatic hydrocarbons were observed to be more abundant in the pyroxenes than in maskelynite. This could be an indication that the organic and water signatures are due to indigenous compounds in Zagami rather than laboratory contamination, however, further investigations are necessary before this conclusion can be confirmed.  相似文献   

12.
This paper looks at the possibilities opened by reaction of NH with methyl radical. A general survey of the potential surface by ab initio Möller-Plesset (MP2) and density functional theory has been performed, including determination of transition states on the pathways considered and vibrational analysis of all stationary points. Energetical data have been obtained using coupled cluster molecular orbital methods (CCSD(T)). It is shown that HCN is not formed from these starting reactants, but that CH2NH, a possible precursor of tholins and of prebiotic compounds through hydration is the major product.  相似文献   

13.
Galina M. Chaban 《Icarus》2007,187(2):592-599
An absorption band at ∼4.26 μm wavelength attributed to the asymmetric stretching mode of CO in CO2 has been found on two satellites of Jupiter and several satellites of Saturn. The wavelength of pure CO2 ice determined in the laboratory is 4.2675 μm, indicating that the CO2 on the satellites occurs either trapped in a host material, or in a chemical or physical complex with other materials, resulting in a blue shift of the wavelength of the band. In frequency units, the shifts in the satellite spectra range from 3.7 to 11.3 cm−1. We have performed ab initio quantum chemical calculations of CO2 molecules chemically complexed with one, two, and more H2O molecules and molecules of CH3OH to explore the possibility that the blue shift of the band is caused by chemical complexing of CO2 with other volatile materials. Our computations of the harmonic and anharmonic vibrational frequencies using high levels of theory show a frequency shift to the blue by 5 cm−1 from pure CO2 to CO-H2O, and an additional 5 cm−1 from CO2-H2O to CO2-2H2O. Complexing with more than two H2O molecules does not increase the blue shift. Complexes of CO2 with one molecule of CH3OH and with one CH3OH plus one H2O molecule produce smaller shifts than the CO2-2H2O complex. Laboratory studies of CO2:H2O in a solid N2 matrix also show a blue shift of the asymmetric stretching mode.  相似文献   

14.
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15.
M.E. Varela  G. Kurat 《Icarus》2005,178(2):553-569
Glasses, in the Kaba CV3 chondrite, occur as mesostasis in chondrules and aggregates and as inclusions in olivines, both confined or open and connected to the mesostasis. The inclusions in olivine and the glassy mesostasis of aggregates seem to have formed contemporaneously. The confined glass inclusions and open inclusions in olivine were formed during olivine growth and the mesostasis glass during olivine aggregation. All glasses have high trace element contents (10-20×CI) with unfractionated CI-normalized abundances of refractory trace elements. In contrast, V, Mn, Li, and Cr are depleted in all glasses with respect to the refractory trace elements, as is Rb in the glass inclusions in olivine but not in the mesostasis glass. This abundance pattern indicates vapor fractionation and a common condensation origin for both glasses. Glasses of confined glass inclusions in olivine have a SiAlCa-rich composition with a chondritic Ca/Al ratio. Glasses of open glass inclusions and mesostasis are poor in Ca and enriched in alkalis. However, Ca contents of olivines indicate crystallization from a Ca-rich melt of a composition similar to that of the glass inclusions. In addition, trace element abundances indicate that these glasses (liquids) probably had an original composition similar to that of the inclusion glass. They apparently lost Ca in exchange for alkalis in a metasomatic exchange reaction, presumably with the vapor. There is now growing evidence that liquids can indeed condense from a solar nebula gas, provided the gas/dust ratio is sufficiently low. In these regions with enhanced oxygen fugacity as compared to that of a nebula of solar composition, liquids (the glass precursor) probably played an important role in growing crystals from the vapor by liquid-phase epitaxy. The glasses appear to be the remnants of this thin liquid layer interface that supported the growth of olivine from the vapor following the Vapor-Liquid-Solid process. This liquid will have a refractory composition and will have trace element contents which are in equilibrium with the vapor, and, therefore, will not change much during the time of olivine growth. The composition of the liquid seems to be unconstrained by the phases it is in contact with. Samples of this liquid will be retained as glass inclusions in olivine. The glassy mesostasis could also be a sample of this liquid that got trapped in inter-crystal spaces. The mesostasis glass subsequently behaved as an open system and its Ca was exchanged—presumably with the vapor—for the alkali elements Na, K, and Rb. In contrast, glass inclusions in olivine were protected by the host, could not react, and thus preserved the original composition of this liquid.  相似文献   

16.
We present the discovery of a new vibrational band system of isotopic CO2 (carbon dioxide) near 3.3 μm, with multiple strong P, Q and R lines in the prime spectral region used to search for Mars CH4 (methane). The band system was discovered on Mars using high-resolution spectrometers (λ/δλ>40,000, CSHELL and NIRSPEC) at telescopes (NASA-IRTF and Keck-2) atop Mauna Kea, HI. The observed line intensities and frequencies agree very well with values predicted by a vibrational band model that we developed using known parameters for the molecular levels involved. Using this model, we synthesized spectra for different observing conditions (from Space and ground-based telescopes) and for different spectral resolving powers (5000 to 40,000). Although the total atmospheric burden on Mars is more than 150 times smaller than on Earth, the greater mixing ratio of CO2 ensures that its column abundance on Mars is almost 20 times greater than on Earth. Thus, weak telluric CO2 band systems appear much stronger on Mars. Many molecules of possible biological and geothermal interest have strong signatures at these wavelengths, in particular hydrocarbons owing to their strong ro-vibrational CH stretching modes. For example, the new isotopic CO2 band-system encompasses lines of CH4, C2H6 (ethane), CH3OH (methanol) and H2O (water). Implications for previous and future searches of biomarker gases are presented.  相似文献   

17.
We report the detection of 13CH3D in Titan's stratosphere from Cassini/CIRS infrared spectra near 8.7 μm. Fitting simultaneously the ν6 bands of both 13CH3D and 12CH3D and the ν4 band of CH4, we derive a D/H ratio equal to and a 12C/13C ratio in deuterated methane of , consistent with that measured in normal methane.  相似文献   

18.
We review our recent results on the vacuum ultraviolet (VUV) photochemistry of small biomolecules. The experimental techniques used, mass spectrometry and photofragment fluorescence spectroscopy, are described. Emphasis is laid on our mass spectrometric results obtained for five nucleic acid bases and five amino acids. Ionisation and appearance energies are determined from photoionisation mass spectrometry, many for the first time. From this, fragmentation pathways following 6-22 eV photoexciation are derived. The adiabatic ionisation energies of the biomolecules studied lie between 8.2 eV (adenine) and 9.6 eV (α-amino-isobutyric acid). We show that the nucleic acid monocations, and chemically related molecular cations, do not fragment even when formed with large internal energies (Eint) ranging from 1.80 to 5.35 eV. In contrast, amino acid monocations are unstable and rapid fragmentation occurs via rupture of the CC(OOH) bond, except for β-alanine, where rupture of the bond between the α-C and β-C is the lowest lying ionic dissociation channel. The VUV photochemistry of the prebiotic species formic acid, acetic acid and methylformate, studied in more detail previously by several techniques, including fluorescence spectroscopy, is also reviewed. Astrophysical implications of our work are discussed in the conclusion.  相似文献   

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