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1.
Solar UV is the principal energy source impinging the atmosphere of Titan while the energy from the electrons in Saturn's magnetosphere is less than 0.5% of the UV light. Titan haze analogs were prepared by the photolysis of a mixture of gases that simulate the composition of its atmosphere (nitrogen, methane, hydrogen, acetylene, ethylene, and cyanoacetylene). The real (n) and imaginary (k) parts of the complex refractive index of haze analogs formed from four different gas mixtures were calculated from the spectral properties of the solid polymer in UV-visible, near infrared and infrared wavelength spectral regions. The value of n was constant at 1.6±0.1 throughout the 0.2-2.5 μm region. The variation of k with wavelength for the values derived for Titan has a lower error than the absolute values of k so the more significant comparisons are with the slopes of the k(λ) plots in the UV-VIS region. Three of the photochemical Titan haze analogs had slopes comparable to those derived for Titan from the Voyager data (Rages and Pollack, 1980, Icarus 41, 119-130; McKay and Toon, 1992, in: Proceedings of the Symposium on Titan, in: ESA SP, Vol. 338, pp. 185-190). The slopes of the k(λ) plots for haze analogs prepared by spark discharge (Khare et al., 1984, Icarus 60, 127-137) and plasma discharge (Ramirez et al., 2002, Icarus 156, 515-529) were also comparable to Titan's. These finding show that the k(λ) plots do not differentiate between different laboratory simulations of atmospheric chemistry on Titan in the UV-VIS near IR region (0.2-2.5 microns). There is a large difference between the k(λ) in the infrared between the haze analogs prepared photochemically and analogs prepared using a plasma discharges (Khare et al., 1984, Icarus 60, 127-137; Coll et al., 1999, Planet. Space Sci. 47, 1331-1340; Khare et al., 2002, Icarus 160, 172-182). The C/N ratio in the haze analog prepared by discharges is in the 2-11 range while that of the photochemical analogs is in the 18-24 range. The use of discharges and UV light for initiating the chemistry in Titan's atmosphere is discussed.  相似文献   

2.
Photochemical reaction pathways in Titan's atmosphere were investigated by irradiation of the individual components and the mixture containing nitrogen, methane, hydrogen, acetylene, ethylene, and cyanoacetylene. The quantum yields for the loss of the reactants and the formation of products were determined. Photolysis of ethylene yields mainly saturated compounds (ethane, propane, and butane) while photolysis of acetylene yields the same saturated compounds as well as ethylene and diacetylene. Irradiation of cyanoacetylene yields mainly hydrogen cyanide and small amounts of acetonitrile. When an amount of methane corresponding to its mixing ratio on Titan was added to these mixtures the quantum yields for the loss of reactants decreased and the quantum yields for hydrocarbon formation increased indicative of a hydrogen atom abstraction from methane by the photochemically generated radicals. GC/MS analysis of the products formed by irradiation of mixtures of all these gases generated over 120 compounds which were mainly aliphatic hydrocarbons containing double and triple bonds along with much smaller amounts of aromatic compounds like benzene, toluene and phenylacetylene. The reaction pathways were investigated by the use of 13C acetylene in these gas mixtures. No polycyclic aromatic compounds were detected. Vapor pressures of these compounds under conditions present in Titan's atmosphere were calculated. The low molecular weight compounds likely to be present in the atmosphere and aerosols of Titan as a result of photochemical processes are proposed.  相似文献   

3.
The spectrometers of the Cassini mission to the Saturn system have detected haze layers reaching up to 800 km in Titan’s atmosphere. Knowledge of the complex refractive index (k) of the haze is important for modeling the surface and atmosphere of Titan and retrieving some information about the functional groups present in the aerosols. Plasma discharges or ultraviolet radiation are commonly used to drive the formation of solid organics assumed to be good analogs of the Titan aerosols. [Tran, B.N., Ferris, J.P., Chera, J.J., 2003a. The photochemical formation of a Titan haze analog. Structural analysis by X-ray photoelectron and infrared spectroscopy. Icarus 162, 114-124; Tran, B.N., Force, M., Briggs, R., Ferris J.P., Persans, P., Chera, J.J., 2008. Photochemical processes on Titan: Irradiation of mixtures of gases that simulate Titan’s atmosphere. Icarus 177, 106-115] reported the index of refraction of analogs synthesized by far ultraviolet irradiation of various gas mixtures. k was determined in the 200-800 nm wavelength range from transmission and reflection spectroscopy. However, this technique is limited by (i) uncertainties in the absorption values because of the small amounts of organics available, (ii) light scattering by the surface roughness and particulates in the sample. These limitations prompted us to perform new measurements using photothermal deflection spectroscopy (PDS), a technique based on the conversion of absorbed light into heat in the material of interest. By combining traditional spectroscopy (λ < 500 nm) and PDS (λ > 500 nm), we determined values of k over the 375-1550 nm range. k values as low as 10−4 above 1000 nm were determined. This is one order of magnitude lower than the measurements generally used as a reference for Titan’s aerosols analogs [Khare, B.N., Sagan, C., Arakawa, E.T., Suits, F., Callicott, T.A., Williams, M.W., 1984. Optical-constants of organic Tholins produced in a simulated Titanian atmosphere—from soft-X-ray to microwave-frequencies. Icarus 60(1), 127-137]. We recommend that these results were used in models to describe the optical properties of the aerosols produced in Titan’s stratosphere.  相似文献   

4.
One of the key components controlling the chemical composition and climatology of Titan's atmosphere is the removal of reactive atomic hydrogen from the atmosphere. A proposed process of the removal of atomic hydrogen is the heterogeneous reaction with organic aerosol. In this study, we investigate the effect of heterogeneous reactions in Titan's atmospheric chemistry using new measurements of the heterogeneous reaction rate [Sekine, Y., Imanaka, H., Matsui, T., Khare, B.N., Bakes, E.L.O., McKay, C.P., Sugita, S., 2008. Icarus 194, 186-200] in a one-dimensional photochemical model. Our results indicate that 60-75% of the atomic hydrogen in the stratosphere and mesosphere are consumed by the heterogeneous reactions. This result implies that the heterogeneous reactions on the aerosol surface may predominantly remove atomic hydrogen in Titan's stratosphere and mesosphere. The results of our calculation also indicate that a low concentration of atomic hydrogen enhances the concentrations of unsaturated complex organics, such as C4H2 and phenyl radical, by more than two orders in magnitude around 400 km in altitude. Such an increase in unsaturated species may induce efficient haze production in Titan's mesosphere and upper stratosphere. These results imply a positive feedback mechanism in haze production in Titan's atmosphere. The increase in haze production would affect the chemical composition of the atmosphere, which might induce further haze production. Such a positive feedback could tend to dampen the loss and supply cycles of CH4 due to an episodic CH4 release into Titan's atmosphere.  相似文献   

5.
Titan, the largest satellite of Saturn, has a thick nitrogen/methane atmosphere with a thick global organic haze. A laboratory analogue of Titan's haze, called tholin, was formed in an inductively coupled plasma from nitrogen/methane=90/10 gas mixture at various pressures ranging from 13 to 2300 Pa. Chemical and optical properties of the resulting tholin depend on the deposition pressure in cold plasma. Structural analyses by IR and UV/VIS spectroscopy, microprobe laser desorption/ionization mass spectrometry, and Raman spectroscopy suggest that larger amounts of aromatic ring structures with larger cluster size are formed at lower pressures (13 and 26 Pa) than at higher pressures (160 and 2300 Pa). Nitrogen is more likely to incorporate into carbon networks in tholins formed at lower pressures, while nitrogen is bonded as terminal groups at higher pressures. Elemental analysis reveals that the carbon/nitrogen ratio in tholins increases from 1.5-2 at lower pressures to 3 at 2300 Pa. The increase in the aromatic compounds and the decrease in C/N ratio in tholin formed at low pressures indicate the presence of the nitrogen-containing polycyclic aromatic compounds in tholin formed at low pressures. Tholin formed at high pressure (2300 Pa) consists of a polymer-like branched chain structure terminated with CH3, NH2, and CN with few aromatic compounds. Reddish-brown tholin films formed at low pressures (13-26 Pa) shows stronger absorptions (almost 10 times larger k-value) in the UV/VIS range than the yellowish tholin films formed at high pressures (160 and 2300 Pa). The tholins formed at low pressures may be better representations of Titan's haze than those formed at high pressures, because the optical properties of tholin formed at low pressures agree well with that of Khare et al. (1984a, Icarus 60, 127-137), which have been shown to account for Titan's observed geometric albedo. Thus, the nitrogen-containing polycyclic aromatic compounds we find in tholin formed at low pressure may be present in Titan's haze. These aromatic compounds may have a significant influence on the thermal structure and complex organic chemistry in Titan's atmosphere, because they are efficient absorbers of UV radiation and efficient charge exchange intermediaries. Our results also indicate that the haze layers at various altitudes might have different chemical and optical properties.  相似文献   

6.
In Titan's atmosphere consisting of N2 and CH4, large amounts of atomic hydrogen are produced by photochemical reactions during the formation of complex organics. This atomic hydrogen may undergo heterogeneous reactions with organic aerosol in the stratosphere and mesosphere of Titan. In order to investigate both the mechanisms and kinetics of the heterogeneous reactions, atomic deuterium is irradiated onto Titan tholin formed from N2 and CH4 gas mixtures at various surface-temperatures of the tholin ranging from 160 to 310 K. The combined analyses of the gas species and the exposed tholin indicate that the interaction mechanisms of atomic deuterium with the tholin are composed of three reactions; (a) abstraction of hydrogen from tholin resulting in gaseous HD formation (HD recombination), (b) addition of D atom into tholin (hydrogenation), and (c) removal of carbon and/or nitrogen (chemical erosion). The reaction probabilities of HD recombination and hydrogenation are obtained as ηabst=1.9(±0.6)×10−3×exp(−300/T) and ηhydro=2.08(±0.64)×exp(−1000/T), respectively. The chemical erosion process is very inefficient under the conditions of temperature range of Titan's stratosphere and mesosphere. Under Titan conditions, the rates of hydrogenation > HD recombination ? chemical erosion. Our measured HD recombination rate is about 10 times (with an uncertainty of a factor of 3-5) the prediction of previous theoretical model. These results imply that organic aerosol can remove atomic hydrogen efficiently from Titan's atmosphere through the heterogeneous reactions and that the presence of aerosol may affect the subsequent organic chemistry.  相似文献   

7.
Solar and X-ray radiation and energetic plasma from Saturn's magnetosphere interact with the upper atmosphere producing an ionosphere at Titan. The highly coupled ionosphere and upper atmosphere system mediates the interaction between Titan and the external environment. A model of Titan's nightside ionosphere will be described and the results compared with data from the Ion and Neutral Mass Spectrometer (INMS) and the Langmuir probe (LP) part of the Radio and Plasma Wave (RPWS) experiment for the T5 and T21 nightside encounters of the Cassini Orbiter with Titan. Electron impact ionization associated with the precipitation of magnetospheric electrons into the upper atmosphere is assumed to be the source of the nightside ionosphere, at least for altitudes above 1000 km. Magnetospheric electron fluxes measured by the Cassini electron spectrometer (CAPS ELS) are used as an input for the model. The model is used to interpret the observed composition and structure of the T5 and T21 ionospheres. The densities of many ion species (e.g., CH+5 and C2H+5) measured during T5 exhibit temporal and/or spatial variations apparently associated with variations in the fluxes of energetic electrons that precipitate into the atmosphere from Saturn's magnetosphere.  相似文献   

8.
A combination of laboratory experiments, theoretical modeling, and spacecraft observations is employed to characterize the aerosols in the atmosphere of Titan. The scattering properties of model aerosols were measured using the Microwave Analog Light Scattering Facility at the University of Florida and complemented with theoretical modeling of single scattering characteristics and radiative transfer in Titan's atmosphere. This study compares these modeling results with photopolarimetric observations made over a range of phase angles by the Pioneer 11 and Voyagers 1 and 2 spacecraft. Important results of this work include a survey of the scattering properties of different particle morphologies and compositions necessary to accurately interpret these observations without introducing non-physical assumptions about the particles or requiring additional free parameters to the radiative transfer models. Previous studies use calculation methods which, due to computing memory and processing time requirements, a priori exclude much of the parameter space that the microwave analog laboratory is ideal for exploring. The goal of the present work, to directly constrain aerosol physical characteristics, is addressed by studying in a consistent manner how a variety of particle morphologies and refractive indices affect the polarization and intensity reflected by Titan's atmosphere. Based on comparisons of model results to spacecraft observations, many model morphologies are excluded from further consideration. The most plausible physical particle models suggest that a combination of Rayleigh-like single particles and aggregates that are larger than those previously suggested and investigated [West, R.A., Smith, P.H., 1991. Evidence for aggregate particles in the atmospheres of Titan and Jupiter. Icarus 90, 330-333; Rannou, P., Cabane, M., Botet, R., Chassefière, E., 1997. A new interpretation of scattered light measurements at Titan's limb. J. Geophys. Res. 102, 10997-11013] provide the best fit to the existing data. Additional laboratory experiments and more refined modeling awaits the results of the new rich observational dataset from the Cassini/Huygens encounter with Titan.  相似文献   

9.
The near-infrared spectrum of Titan, Saturn's largest moon and one of the Cassini/Huygens' space mission primary targets, covers the 0.8 to 5 micron region in which it shows several weak CH4 absorption regions, and in particular one centered near 2.75 micron. Due to the interference of telluric absorption, only part of this window region (2.9-3.1 μm) has previously been observed from the ground [Noll, K.S., Geballe, T.R., Knacke, R., Pendleton, F., Yvonne, J., 1996. Icarus 124, 625-631; Griffith, C.A., Owen, T., Miller, G.A., Geballe, T., 1998. Nature 395, 575-578; Griffith, C.A., Owen, T., Geballe, T.R., Rayner, J., Rannou, P., 2003. Science 300, 628-630; Geballe, T.R., Kim, S.J., Noll, K.S., Griffith, C.A., 2003. Astrophys. J. 583, L39-L42]. We report here on the first spectroscopic observations of Titan covering the whole 2.4-4.9 μm region by two instruments on board the Infrared Space Observatory (ISO) in 1997. These observations show the 2.75-μm window in its complete extent for the first time. In this study we have also used a high-resolution Titan spectrum in the 2.9-3.6 μm region taken with the Keck [Geballe, T.R., Kim, S.J., Noll, K.S., Griffith, C.A., 2003. Astrophys. J. 583, L39-L42; Kim, S.J., Geballe, T.R., Noll, K.S., Courtin, R., 2005. Icarus 173, 522-532] to infer information on the atmospheric parameters (haze extinction, single scattering albedo, methane abundance, etc.) by fitting the methane bands with a detailed microphysical model of Titan's atmosphere (updated from Rannou, P., McKay, C.P., Lorenz, R.D., 2003. Planet. Space Sci. 51, 963-976). We have included in this study an updated version of a database for the CH4 absorption coefficients [STDS, Wenger, Ch., Champion, J.-P., 1998. J. Quant. Spectrosc. Radiat. Transfer 59, 471-480. See also http://www.u-bourgogne.fr/LPUB/TSM/sTDS.html for latest updates; Boudon, V., Champion, J.-P., Gabard, T., Loëte, M., Michelot, F., Pierre, G., Rotger, M., Wenger, Ch., Rey, M., 2004. J. Mol. Spectrosc. 228, 620-634]. For the atmosphere we find that (a) the haze extinction profile that best matches the data is one with higher (by 40%) extinction in the atmosphere with respect to Rannou et al. (2003) down to about 30 km where a complete cut-off occurs; (b) the methane mixing ratio at Titan's surface cannot exceed 3% on a disk-average basis, yielding a maximum CH4 column abundance of 2.27 km-am in Titan's atmosphere. From the derived surface albedo spectrum in the 2.7-3.08 micron region, we bring some constraints on Titan's surface composition. The albedo in the center of the methane window varies from 0.01 to 0.08. These values, compared to others reported in the other methane windows, show a strong compatibility with the water ice spectrum in the near-infrared. Without confirming its existence from this work alone, our data then appear to be compatible with water ice. A variety of other ices, such as CO2, NH3, tholin material or hydrocarbon liquid cannot be excluded from our data, but an additional unidentified component with a signature around 2.74 micron is required to satisfy the data.  相似文献   

10.
Saturn's largest moon, Titan, provides an interesting opportunity to study how dense atmospheres interact with the surrounding plasma environment. Without an intrinsic magnetic field, this satellite's nitrogen-rich atmosphere is relatively unprotected from plasma interactions. Therefore, the energy-deposition rate is important for understanding chemistry and dynamics in Titan's atmosphere. Since the plasma environment can vary significantly we focus here on the T18 Titan encounter using in-situ data from instruments on board the Cassini spacecraft. These instruments cannot provide in-situ information below the spacecraft closest approach altitude (∼>960 km) so we use the Cassini magnetospheric imaging instrument (MIMI) ion-neutral camera (INCA) to remotely image energetic hydrogen particle fluxes (20-80 keV) at altitudes below Titan closest approach. We also use the MIMI low-energy magnetosphere measurements system (LEMMS) to measure the incident ion fluxes as the spacecraft approaches Titan and combine these data sets with an atmospheric model to first reproduce INCA images. We then use this model to calculate the energy-deposition profiles for the observed incident proton flux. Our model is able to reproduce the INCA observations and give the energy density deposited vs. altitude in Titan's atmosphere; however, we find that the incident fluxes and energy-deposition profiles vary significantly during the encounter.  相似文献   

11.
We present a quantitative analysis of CO thermal emissions discovered on the nightside of Titan by Baines et al. [2005. The atmospheres of Saturn and Titan in the near-infrared: First results of Cassini/VIMS. Earth, Moon, and Planets, 96, 119–147]. in Cassini/VIMS spectral imagery. We identify these emission features as the P and R branches of the 1-0 vibrational band of carbon monoxide (CO) near 4.65 μm. For CH3D, the prominent Q branch of the ν2 fundamental band of CH3D near 4.55 μm is apparent. CO2 emissions from the strong v3 vibrational band are virtually absent, indicating a CO2 abundance several orders of magnitude less than CO, in agreement with previous investigations. Analysis of CO emission spectra obtained over a variety of altitudes on Titan's nightside limb indicates that the stratospheric abundance of CO is 32±15 ppm, and together with other recent determinations, suggests a vertical distribution of CO nearly constant at this value from the surface throughout the troposphere to at least the stratopause near 300 km altitude. The corresponding total atmospheric content of CO in Titan is 2.9±1.5×1014 kg. Given the long lifetime of CO in the oxygen-poor Titan atmosphere (0.5–1.0 Gyr), we find a mean CO atmospheric production rate of 6±3×105 kg yr−1. Given the lack of primordial heavy noble gases observed by Huygens [Niemann et al., 2005. The abundances of constituents of Titan's atmosphere from the GCMS on the Huygens probe. Nature, 438, 779–784], the primary source of atmospheric CO is likely surface emissions. The implied CO/CH4 mixing ratio of near-surface material is 1.8±0.9×10−4, based on an average methane surface emission rate over the past 0.5 Gyr of 1.3×10−13 gm cm−2 s−1 as required to balance hydrocarbon haze production via methane photolysis [Wilson and Atreya, 2004. Current state of modeling the photochemistry of Titan's mutually dependent atmosphere and ionosphere. J. Geophys. Res. 109, E06002 Doi:10.1029/2003JE002181]. This low CO/CH4 ratio is much lower than expected for the sub-nebular formation region of Titan and supports the hypothesis [e.g., Atreya et al., 2005. Methane on Titan: photochemical-meteorological-hydrogeochemical cycle. Bull. Am. Astron. Soc. 37, 735] that the conversion of primordial CO and other carbon-bearing materials into CH4-enriched clathrate-hydrates occurs within the deep interior of Titan via the release of hydrogen through the serpentinization process followed by Fischer–Tropsch catalysis. The time-averaged predicted emission rate of methane-rich surface materials is 0.02 km3 yr−1, a value significantly lower than the rate of silicate lava production for the Earth and Venus, but nonetheless indicative of significant active geological processes reshaping the surface of Titan.  相似文献   

12.
Ronen Jacovi 《Icarus》2008,196(1):302-304
Titan's haze, formed by photolysis of C2H2, C2H4 and HCN, was found experimentally to trap Ar, Kr and Xe with efficiencies of 3.5 × 10−4, 1.9 × 10−3 and 6.5 × 10−2 [noble gas atom]/[carbon atom] in the polymer, respectively. The rate of aerosol formation and settling down of 3 × 10−13 kg m−2 s−1, as inferred from our experiments on CH4 photolysis in the far UV [Podolak, M., Bar-Nun, A., 1979. Icarus 39, 272-276], is sufficient to reduce the mixing ratios of 36Ar and 40Ar to their low values of (2.8 ± 0.3) × 10−7 and (4.3 ± 0.1) × 10−3, respectively, and those of Kr and Xe to below the detection limit of 10−8.  相似文献   

13.
Titan, Saturn's largest moon, has a thick nitrogen/methane atmosphere. The temperature and pressure conditions in Titan's atmosphere are such that the methane vapor should condense near the tropopause to form clouds. Several ground-based measurements have observed sparse cloud-like features in Titan's atmosphere, while the Cassini mission to Saturn has provided large scale images of the clouds. However, Titan's cloud formation conditions remain poorly constrained. Heterogeneous nucleation (from the vapor phase onto a solid or liquid aerosol surface) greatly enhances cloud formation relative to homogeneous nucleation. In order to elucidate the cloud formation mechanism near the tropopause, we have performed laboratory measurements of the adsorption of methane and ethane onto solid organic particles (tholins) representative of Titan's photochemical haze. We find that monolayers of methane adsorb onto tholin particles at saturation ratios less than unity. We also find that solid methane nucleates onto the adsorbed methane at a saturation ratio of S=1.07±0.008. This implies that Titan's methane clouds should form easily. This is consistent with recent measurements of the column of methane ruling out excessive methane supersaturation. In addition, we find ethane adsorbs onto tholin particles in a metastable phase prior to nucleation. However, ethane nucleation onto the adsorbed ethane occurs at a relatively high saturation ratio of S=1.36±0.08. These findings are consistent with the recent report of polar ethane clouds in Titan's lower stratosphere.  相似文献   

14.
A global-mean model of coupled neutral and ion chemistry on Titan has been developed. Unlike the previous coupled models, the model involves ambipolar diffusion and escape of ions, hydrodynamic escape of light species, and calculates the H2 and CO densities near the surface that were assigned in some previous models. We tried to reduce the numbers of species and reactions in the model and remove all species and reactions that weakly affect the observed species. Hydrocarbon chemistry is extended to C12H10 for neutrals and C10H+11 for ions but does not include PAHs. The model involves 415 reactions of 83 neutrals and 33 ions, effects of magnetospheric electrons, protons, and cosmic rays. UV absorption by Titan's haze was calculated using the Huygens observations and a code for the aggregate particles. Hydrocarbon, nitrile, and ion chemistries are strongly coupled on Titan, and attempt to calculate them separately (e.g., in models of ionospheric composition) may result in significant error. The model densities of various species are typically in good agreement with the observations except vertical profiles in the stratosphere that are steeper than the CIRS limb data. (A model with eddy diffusion that facilitates fitting to the CIRS limb data is considered as well.) The CO densities are supported by the O+ flux from Saturn's magnetosphere. The ionosphere includes a peak at 80 km formed by the cosmic rays, steplike layers at 500-700 and 700-900 km and a peak at 1060 km (SZA = 60°). Nighttime densities of major ions agree with the INMS data. Ion chemistry dominates in the production of bicyclic aromatic hydrocarbons above 600 km. The model estimates of heavy positive and negative ions are in reasonable agreement with the Cassini results. The major haze production is in the reactions C6H + C4H2, C3N + C4H2, and condensation of hydrocarbons below 100 km. Overall, precipitation rate of the photochemical products is equal to 4-7 kg cm−2 Byr−1 (50-90 m Byr−1 while the global-mean depth of the organic sediments is ∼3 m). Escape rates of methane and hydrogen are 2.9 and 1.4 kg cm−2 Byr−1, respectively. The model does not support the low C/N ratio observed by the Huygens ACP in Titan's haze.  相似文献   

15.
A 3-D Monte Carlo model is used to describe the ejection of N and N2 from Titan due to the interaction of Saturn's magnetospheric N+ ions and molecular pick-up ions with its N2 atmosphere. Based on estimates of the ion flux into Titan's corona, atmospheric sputtering is an important source of both atomic and molecular nitrogen for the neutral torus and plasma in Saturn's outer magnetosphere, a region now being studied by the Cassini spacecraft.  相似文献   

16.
The detection of CH4 in the martian atmosphere, at a mixing ratio of about 10 ppb, prompted Krasnopolsky et al. [Krasnopolsky, V.A., Maillard, J.P., Owen, T.C., 2004. Icarus 172, 537-547] and Krasnopolsky [Krasnopolsky, V.A., 2006. Icarus 180, 359-367] to propose that the CH4 is of biogenic origin. Bar-Nun and Dimitrov [Bar-Nun, A., Dimitrov, V., 2006. Icarus 181, 320-322] proposed that CH4 can be formed in the martian atmosphere by photolysis of H2O in the presence of CO. We based our arguments on a clear demonstration that CH4 is formed in our experiments, and on thermodynamic equilibrium calculations, which show that CH4 formation is favored even in the presence of oxygen at a mixing ratio 1.3×10−3, as observed on Mars. In the present comment, Krasnopolsky [Krasnopolsky, V.A., 2007. Icarus, in press (this issue)] presents his arguments against the suggestion of Bar-Nun and Dimitrov [Bar-Nun, A., Dimitrov, V., 2006. Icarus 181, 320-322], based on the effect of O2 on CH4 formation, the absence of kinetic pathways for CH4 formation and on the inadequacy of thermodynamic equilibrium calculations to describe the martian atmosphere. In this rebuttal we demonstrate that experiments with molecular oxygen at a ratio of O2/CO2=(8.9-17)×10−3, exceeding the martian ratio, still form CH4. Thermodynamic equilibrium calculations replicate the experimental CH4 mixing ratio to within a factor of 1.9 and demonstrate that CH4 production is favored in the martian atmosphere, which is obviously not in thermodynamic equilibrium. Consequently, we do not find the presence of methane to be a sign of biological activity on Mars.  相似文献   

17.
V. Vuitton  J.-F. Doussin  F. Raulin 《Icarus》2006,185(1):287-300
None of the Titan photochemical models currently available have been able to reproduce the full set of stratospheric molecular mixing ratios inferred from observations. In order to assess how well reaction sets describe hydrocarbon chemistry, theoretical modeling predictions were compared to the results of a laboratory experiment. A CH4-C2H2 mixture was irradiated at 185 nm in an atmospheric simulation chamber and the evolution of the gas mixture was followed in situ and in real time by infrared spectroscopy. In parallel, a 0D theoretical model of the laboratory experiment was developed. A new reaction set describing Titan's chemistry was built and incorporated in the model. Lebonnois et al. [Lebonnois, S., Toublanc, D., Hourdin, F., Rannou, P., 2001. Icarus 152, 384-406] reaction set was also used for comparison. The presence of small amounts of atmospheric O2 in the experiment was properly accounted for and led us to suggest that oxygenated chemistry might be a source of C2H4 in Titan's atmosphere. With Lebonnois et al. [Lebonnois, S., Toublanc, D., Hourdin, F., Rannou, P., 2001. Icarus 152, 384-406] reaction set, the model could not fit at all the experimental evolution of the compounds. This is explained by some of the choices made for crucial kinetic parameters such as the quantum yield of photolysis of C2H2. Also, the absence of some reactions led to the enhancement of pathways that would otherwise be negligible. For example, the lack of reactions between C4H4 and radicals induced an erroneously high photolysis rate for this species. With the reaction set built in this study, the model much better fits the experiment, especially when the “soot,” which includes C4H4, is recycled into C2H2. This shows that photochemistry of the larger species has a role in determining the lighter species concentrations and that considering that they are simply lost from the system is not a valid assumption. Including even an abridged set of C4 + hydrocarbon reactions will be required in future photochemical models. Especially, photolysis rates and yields for C2H2, C4H2, and C4H4, are important parameters in need of a better determination.  相似文献   

18.
Methane is key to sustaining Titan's thick nitrogen atmosphere. However, methane is destroyed and converted to heavier hydrocarbons irreversibly on a relatively short timescale of approximately 10-100 million years. Without the warming provided by CH4-generated hydrocarbon hazes in the stratosphere and the pressure induced opacity in the infrared, particularly by CH4-N2 and H2-N2 collisions in the troposphere, the atmosphere could be gradually reduced to as low as tens of millibar pressure. An understanding of the source-sink cycle of methane is thus crucial to the evolutionary history of Titan and its atmosphere. In this paper we propose that a complex photochemical-meteorological-hydrogeochemical cycle of methane operates on Titan. We further suggest that although photochemistry leads to the loss of methane from the atmosphere, conversion to a global ocean of ethane is unlikely. The behavior of methane in the troposphere and the surface, as measured by the Cassini-Huygens gas chromatograph mass spectrometer, together with evidence of cryovolcanism reported by the Cassini visual and infrared mapping spectrometer, represents a “methalogical” cycle on Titan, somewhat akin to the hydrological cycle on Earth. In the absence of net loss to the interior, it would represent a closed cycle. However, a source is still needed to replenish the methane lost to photolysis. A hydrogeochemical source deep in the interior of Titan holds promise. It is well known that in serpentinization, hydration of ultramafic silicates in terrestrial oceans produces H2(aq), whose reaction with carbon grains or carbon dioxide in the crustal pores produces methane gas. Appropriate geological, thermal, and pressure conditions could have existed in and below Titan's purported water-ammonia ocean for “low-temperature” serpentinization to occur in Titan's accretionary heating phase. On the other hand, impacts could trigger the process at high temperatures. In either instance, storage of methane as a stable clathrate-hydrate in Titan's interior for later release to the atmosphere is quite plausible. There is also some likelihood that the production of methane on Titan by serpentinization is a gradual and continuous on-going process.  相似文献   

19.
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20.
Morente et al. [Morente, J.A., Portí, J.A., Salinas, A., Navarro, E.A., 2008. Icarus. doi:10.1016/j.icarus.2008.02.004] have recently presented a new analysis of the Permittivity, Wave and Altimetry (PWA) measurements made during the descent of the Huygens Probe through the atmosphere of Titan. They claimed the identification of several Schumann resonance harmonics and concluded in favor of a lightning activity on Titan. We report here several reasons for not endorsing this paper.  相似文献   

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