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1.
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   

2.
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   

3.
Titan's haze is composed of aerosols containing long chain polymers of acetylene with some hydrogen cyanide. These polymers have alternating double/single and triple/single bonds, which can open spontaneously or under the action of UV radiation or particle impact. Once opened, they can induce the opening of a double or triple bond in an adjacent chain and link to it. This cross-linking and chain elongation hardens or “ages” the polymer particles, making them less sticky. As observed experimentally and calculated theoretically, newly formed polymer particles grow by collecting other polymer chains and by complete merging into symmetrical spheres. However, when aged, they merely adhere to each other and do not merge. Eventually, when hard enough, they do not even adhere to each other. In this paper we calculate the spontaneous aging process as applied to Titan's atmospheric conditions and find that the surface tension and viscosity of the aerosols below H∼570 km are one order of magnitude harder than when the aerosols formed. Furthermore, UV irradiation and particle impacts reduce both viscosity and surface tension by an additional factor of 10-100. Thus, the aerosol particles expected to be encountered by the descending Huygens probe will, most likely, be quite hard.  相似文献   

4.
Discovery by Cassini's plasma instrument of heavy positive and negative ions within Titan's upper atmosphere and ionosphere has advanced our understanding of ion neutral chemistry within Titan's upper atmosphere, primarily composed of molecular nitrogen, with ~2.5% methane. The external energy flux transforms Titan's upper atmosphere and ionosphere into a medium rich in complex hydrocarbons, nitriles and haze particles extending from the surface to 1200 km altitudes. The energy sources are solar UV, solar X-rays, Saturn's magnetospheric ions and electrons, solar wind and shocked magnetosheath ions and electrons, galactic cosmic rays (GCR) and the ablation of incident meteoritic dust from Enceladus’ E-ring and interplanetary medium. Here it is proposed that the heavy atmospheric ions detected in situ by Cassini for heights >950 km, are the likely seed particles for aerosols detected by the Huygens probe for altitudes <100 km. These seed particles may be in the form of polycyclic aromatic hydrocarbons (PAH) containing both carbon and hydrogen atoms CnHx. There could also be hollow shells of carbon atoms, such as C60, called fullerenes which contain no hydrogen. The fullerenes may compose a significant fraction of the seed particles with PAHs contributing the rest. As shown by Cassini, the upper atmosphere is bombarded by magnetospheric plasma composed of protons, H2+ and water group ions. The latter provide keV oxygen, hydroxyl and water ions to Titan's upper atmosphere and can become trapped within the fullerene molecules and ions. Pickup keV N2+, N+ and CH4+ can also be implanted inside of fullerenes. Attachment of oxygen ions to PAH molecules is uncertain, but following thermalization O+ can interact with abundant CH4 contributing to the CO and CO2 observed in Titan's atmosphere. If an exogenic keV O+ ion is implanted into the haze particles, it could become free oxygen within those aerosols that eventually fall onto Titan's surface. The process of freeing oxygen within aerosols could be driven by cosmic ray interactions with aerosols at all heights. This process could drive pre-biotic chemistry within the descending aerosols. Cosmic ray interactions with grains at the surface, including water frost depositing on grains from cryovolcanism, would further add to abundance of trapped free oxygen. Pre-biotic chemistry could arise within surface microcosms of the composite organic-ice grains, in part driven by free oxygen in the presence of organics and any heat sources, thereby raising the astrobiological potential for microscopic equivalents of Darwin's “warm ponds” on Titan.  相似文献   

5.
Strong experimental evidence is presented that the northern polar cloud observed in Titan's atmosphere by the Cassini orbiter (VIMS) was indeed composed of ethane aerosol as proposed by Griffith et al. [2006. Science 313, 1620-1622]. We report on the condensation and phase behavior of ethane aerosol under atmospheric conditions of Titan (145 hPa, 40 km altitude, 70-90 K, 10-30 ppm ethane in nitrogen). The results were obtained in an in-situ collisional cooling experiment combined with Fourier-transform infrared (FTIR) spectroscopy. Apart from the liquid phase, three crystalline phases (solid I, solid II, metastable) and the transitions into each other have been observed in the ethane aerosol. The phases were found to have a significant effect on the particles' IR spectra, their growth dynamics and the final size of the aerosols which varies between 0.5 and 4 μm (compared to 1-3 μm observed on Titan). This has strong implications on the ethane vapor pressure, precipitation and optical aerosol detection.  相似文献   

6.
The main gas-phase constituents of Titan's upper atmosphere, N2 and CH4, are photolyzed and radiolyzed by solar photons and magnetospheric electrons, respectively. The primary products of these chemical interactions evolve to heavier organic compounds that are likely to associate into the particles of haze layers that hide Titan's surface. The different theories and models that have been put forward to explain the characteristics and properties of the haze composites require a knowledge of their optical properties, which are determined by the complex refractive index. We present a new set of values for refractive index n and extinction coefficient k calculated directly from the transmittance and reflectance curves exhibited by a laboratory analogue of Titan's aerosols in the 200-900 nm range. Improvements in the aerosol analogue quality have been made. The effects of variables such as the uncertainty in sample thickness, aerosol porosity, and amount of scattered light on the final n and k values are assessed and discussed. Within the studied wavelength domain, n varies from 1.53 to 1.68 and k varies from 2.62×10−4 to 2.87×10−2. These final n and k values should be considered as a new reference to modelers who compute the properties of Titan's aerosols in trying to explain the atmospheric dynamics and surface characteristics.  相似文献   

7.
The formation of organic compounds in the atmosphere of Titan is an ongoing process of the generation of complex organics from the simplest hydrocarbon, methane. Solar radiation and magnetosphere electrons are the main energy sources that drive the reactions in Titan's atmosphere. Since energy from solar radiation is 200 times greater than that from magnetosphere electrons, we have investigated the products formed by the action of UV radiation (185 and 254 nm) on a mixture of gases containing nitrogen, methane, hydrogen, acetylene, ethylene, and cyanoacetylene, the basic gas mixture (BGM) that simulates aspects of Titan's atmosphere using a flow reactor [Tran, B.N., Ferris, J.P., Chera, J.J., 2003a. Icarus 162, 114-124; Tran, B.N., Joseph, J.C., Force, M., Briggs, R.G., Vuitton, V., Ferris, J.P., 2005. Icarus 177, 106-115]. The present research extends these studies by the addition of carbon monoxide and hydrogen cyanide to the BGM. Quantum yields for the loss of reactants and the formation of volatile products were determined and compared with those measured in the absence of the hydrogen cyanide and carbon monoxide. The GCMS analyses of the volatile photolysis products from the BGM, with added hydrogen cyanide, had a composition similar to that of the BGM while the photolysis products of the BGM with added carbon monoxide contained many oxygenated compounds. The infrared spectrum of the corresponding solid product revealed the absorption band of a ketone group, which was probably formed from the reaction of carbon monoxide with the free radicals generated by photolysis of acetylene and ethylene. Of particular interest was the observation that the addition of HCN to the gas mixture only resulted in a very small change in the C/N ratio and in the intensity of the CN frequency at 2210 cm−1 in the infrared spectrum suggesting that little HCN is incorporated into the haze analog. The C/N ratio of the haze analogs was found to be in the 10-12 range. The UV spectra of the solid products formed when HCN or CO added to the BGM is similar to the UV absorption formed from the BGM alone. This result is consistent with absence of additional UV chromophores to the solid product when these mixtures are photolyzed. The following photoproducts, which were not starting materials in our photochemical studies, have been observed on Titan: acetonitrile, benzene, diacetylene, ethane, propene, propane, and propyne.  相似文献   

8.
Titan's tholins are used as analogs of Titan's aerosols and N-rich organic solids present on many icy surfaces. However, it is not clear whether or not they are relevant analogs, and which kind of tholins should be used among a wide set available in literature. This paper presents reflectance spectral data of two tholins selected as end-members of a series of samples covering a very wide range of continuous chemical and optical properties. These samples were formed under experimental conditions fairly consistent with Titan's stratosphere. A general framework for using these laboratory data to the analysis of spectral observation of Titan's surface or other objects is suggested. Furthermore, the study reports the first in situ unambiguous identification of aromatics compounds and evidences variations in the sp2 carbon structure, which controls the absorption properties in the visible/NIR. These results also point out it is very unlikely to derive quantitative chemical information (e.g., N content, sp2/sp3 ratio) from remote sensing reflectance data.  相似文献   

9.
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   

10.
Organic aerosols play a significant role in the properties and evolution of Titan's atmosphere. But our knowledge of them and their physico-chemical mechanisms of formation and evolution are currently limited to a few data obtained by Titan observations from the Earth or from space probes. For this reason, laboratory experiments are developed to simulate the atmospheric chemistry and produce analogues of these aerosols in order to understand better their properties and how they are formed. The plasma discharges are the most efficient devices for the production of such analogues. However, the existing plasmas simulations introduce experimental biases compared with the conditions of aerosols production in Titan's atmosphere: chemistry is induced by electrons instead of photons; the solid analogues are produced and deposited on solid surfaces; direct analysis of the particles inside the reactive chamber is not easy. In order to avoid some of these experimental problems, we have developed another method of production of Titan's aerosols analogues. It is based on a capacitively coupled radio-frequency (RF) cold plasma system at low pressure in a N2-CH4 gaseous mixture. In this plasma, solid particles produced from the gas phase are in levitation, thus preventing any wall effect on their production, and allowing the study of the formation and growth of the particles directly in the plasma. Moreover, the electron energy distribution of this plasma can be compared with the solar spectrum. This article describes the RF plasma experiment and presents the first results obtained with an initial N2-CH4 (90:10) gaseous mixture which produced our first studied analogues of Titan's aerosols.  相似文献   

11.
Erika L. Barth  Owen B. Toon 《Icarus》2006,182(1):230-250
Theoretical arguments point to and recent observations confirm the existence of clouds in Titan's atmosphere, yet we possess very little data on their particle size, composition and formation mechanism. A time-dependent microphysical model is used to study the evolution of ice clouds in Titan's atmosphere. The model simulates nucleation, condensational growth, evaporation, coagulation, and transport of particles in a column of atmosphere. A variety of cloud compositions are studied, including pure ethane clouds, pure methane clouds, and mixed methane-ethane clouds (all with tholin cores). The abundance of methane cloud particles may be limited by the number of ethane coated tholin nuclei rather than the number of tholins with hydrocarbon coatings. However, even the condensation of methane onto these relatively sparse ethane/tholin cloud particles is sufficient to keep the methane close to saturation. Typical methane supersaturations are of order 0.06 on the average. For simulations which take into account recent lab measurements indicating it is relatively easy for methane to nucleate onto tholin particles without an ethane-layer present, the three types of clouds (methane, ethane, and mixed) exist simultaneously. Pure methane clouds are the most abundant cloud type and serve to lower the supersaturation to about 0.04. Cloud production does not require a continuous surface source of methane. However, clouds produced by mean motions are not the visible methane clouds seen in recent Cassini and ground-based observations. Ethane clouds in the troposphere almost instantaneously nucleate methane to form mixed clouds. However, a thin ethane ‘haze’ remains just above the tropopause for some scenarios and the mixed clouds at the tropopause remain ?50% ethane by mass. Also, evaporation of methane from the mixed cloud particles near the surface leaves a thicker layer of ethane cloud particles at ∼10 km. Nevertheless, the precipitation rate of methane to Titan's surface is between 0.001 and 0.5 cm/terrestrial-year, depending on various initial conditions such as critical saturation, size and abundance of cloud condensation nuclei, surface sources and eddy diffusion.  相似文献   

12.
Thermal conductivity measurements, presented in this paper (Fig. 3), were made during the descent of the Huygens probe through the atmosphere of Titan below the altitude of 30 km. The measurements are broadly consistent with reference values derived from the composition, pressure and temperature profiles of the atmosphere; except in narrow altitude regions around 19 km and 11 km, where the measured thermal conductivity is lower than the reference by 1% and 2%, respectively. Only single data point exists at each of the two altitudes mentioned above; if true however, the result supports the case for existence for molecules heavier than nitrogen in these regions (such as: ethane, other primordial noble gases, carbon dioxide, and other hydrocarbon derivatives). The increasing thermal conductivity observed below 7 km altitude could be due to some liquid deposition during the descent; either due to condensation and/or due to passing through layers of fog/cloud containing liquid nitrogen-methane. Thermal conductivity measurements do not allow conclusions to be drawn about how such liquid may have entered the sensor, but an estimate of the cumulative liquid content encountered in the last 7 km is 0.6% by volume of the Titan's atmosphere sampled during descent.  相似文献   

13.
We quantify the charge states of submicrometer aerosols and aromatic macromolecules in Titan's organic haze. The aerosol charge is balanced between the recombination of positive ions with the aerosol plus the ejection of electrons from the aerosol via the UV-driven photoelectric effect and the recombination of electrons with the aerosol. During the day, the dominant charge state for submicro-meter aerosols is positive. Macromolecules composed of fewer than 32 carbon atoms with low electron affinities (<1.0 eV) are neutral, while the rest are mainly neutral and negatively charged with a small fraction (∼10%) becoming positively charged at higher (≥300 km) altitudes. At night, Titan's aerosol population becomes uniformly neutral and negatively charged. The time taken for a nighttime aerosol to change from being negatively charged to its most probable daytime positive charge is on the order of a few seconds for the largest submicrometer aerosols, while macromolecules tend to persist in an anionic charge state for one to several Earth days. Charging strongly influences aerosol agglomeration via Coulomb attraction and may account for the seasonal variations in the albedo of the Titan haze at midrange (∼200-250 km) altitudes. Enhanced agglomeration may also efficiently produce a source of condensation nuclei for the daily rainout of methane. In addition, the difference in aerosol charge between Titan's day and night (or summer and winter) phases will produce dramatically different chemistries which must be accounted for in future photochemical models. Finally, if there are PAH-like macromolecules in the Titan haze, Cassini Huygens should be able to observe these charge differences, with neutral macromolecules emitting strongly at 3.3 and 11.2 μm, cationic macromolecules emitting between 6.2 and 8.6 μm, and anionic macromolecules emitting in both infrared spectral regions.  相似文献   

14.
The Descent Imager/Spectral Radiometer (DISR) of the Huygens probe was in an excellent position to view aspects of rain as it descended through Titan's atmosphere. Rain may play an important part of the methane cycle on Titan, similar to the water cycle on Earth, but rain has only been indirectly inferred in previous studies. DISR detected two dark atmospheric layers at 11 and 21 km altitude, which can be explained by a local increase in aerosol size by about 5-10%. These size variations are far smaller than those in rain clouds, where droplets grow some 1000-fold. No image revealed a rainbow, which implies that the optical depth of raindrops was less than ∼0.0002/km. This upper limit excludes rain and constrains drizzle to extremely small rates of less than 0.0001 mm/h. However, a constant drizzle of that rate over several years would clear the troposphere of aerosols faster than it can be replenished by stratospheric aerosols. Hence, either the average yearly drizzle rate near the equator was even less (<0.1 mm/yr), or the observed aerosols came from somewhere else. The implied dry environment is consistent with ground-based imaging showing a lack of low-latitude clouds during the years before the Huygens descent. Features imaged on Titan's surface after landing, which might be interpreted as raindrop splashes, were not real, except for one case. This feature was a dewdrop falling from the outermost baffle of the DISR instrument. It can be explained by warm, methane-moist air rising along the bottom of the probe and condensing onto the cold baffle.  相似文献   

15.
Greenhouse warming due to carbon dioxide atmospheres may be responsible for maintaining the early Earth's surface temperature above freezing and may even have allowed for liquid water on early Mars. However, the high levels of CO2 required for such warming should have also resulted in the formation of CO2 clouds. These clouds, depending on their particle size, could lead to either warming or cooling. The particle size in turn is determined by the nucleation and growth conditions. Here we present laboratory studies of the nucleation and growth of carbon dioxide on water ice under martian atmospheric conditions. We find that a critical saturation, S=1.34, is required for nucleation, corresponding to a contact parameter between solid water and solid carbon dioxide of m=0.95. We also find that after nucleation occurs, growth of CO2 is very rapid, and we report the growth rates at a number of supersaturations. Because growth would be expected to continue until the CO2 pressure is lowered to its vapor pressure, we expect particles larger than those being currently suggested for the present and past martian atmospheres. Using this information in a microphysical model described in a companion paper, we find that CO2 clouds are best described as “snow,” having a relatively small number of large particles.  相似文献   

16.
We investigate the chemical transition of simple molecules like C2H2 and HCN into aerosol particles in the context of Titan's atmosphere. Experiments that synthesize analogs (tholins) for these aerosols can help illuminate and constrain these polymerization mechanisms. Using information available from these experiments, we suggest chemical pathways that can link simple molecules to macromolecules, which will be the precursors to aerosol particles: polymers of acetylene and cyanoacetylene, polycyclic aromatics, polymers of HCN and other nitriles, and polyynes. Although our goal here is not to build a detailed kinetic model for this transition, we propose parameterizations to estimate the production rates of these macromolecules, their C/N and C/H ratios, and the loss of parent molecules (C2H2, HCN, HC3N and other nitriles, and C6H6) from the gas phase to the haze. We use a one-dimensional photochemical model of Titan's atmosphere to estimate the formation rate of precursor macromolecules. We find a production zone slightly lower than 200 km altitude with a total production rate of 4×10−14 g cm−2 s−1 and a C/N?4. These results are compared with experimental data, and to microphysical model requirements. The Cassini/Huygens mission will bring a detailed picture of the haze distribution and properties, which will be a great challenge for our understanding of these chemical processes.  相似文献   

17.
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   

18.
Viorel Badescu 《Icarus》2011,216(2):485-491
Bodies with water, ammonia or ethane oceans are possible in interstellar space. This may happen for optically thick atmospheres of methane, ethane and carbon dioxide.  相似文献   

19.
Though Titan is in synchronous rotation around Saturn, it experiences gravitational tides as a consequence of its eccentric orbit. It is proposed that the vertical transport of aerosols by these tides produces the haze layers in Titan's upper atmosphere. Analysis shows that the zonal winds in Titan's superrotating atmosphere have a profound influence on which tidal components are effective in establishing the multiple detached-haze layers. If the Huygens Doppler winds are representative of the equatorial global superrotation, then the westward propagating s=2 mode is the responsible tidal component even though its forcing is significantly weaker than that of the s=0 and eastward s=2 components. The eastward s=2 tidal mode is eliminated by critical levels while the s=0 mode is viscously damped in the strong high altitude winds. At polar latitudes, however, the gravest s=0 mode is the one most likely to produce layering. It is also suggested that the atmospheric gravitational tides could be responsible for decelerating the superrotating atmosphere as seen in the Huygens Doppler wind velocity profile at about 80 km altitude.  相似文献   

20.
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   

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