The composition and origin of Titan's atmosphere

The discovery that Titan had an atmosphere was made by the identification of methane in the satellite's spectrum in 1944. But the abundance of this gas and the identification of other major constituents required the 1980 encounter by the Voyager 1 spacecraft. In the intervening years, traces of C₂H₂, C₂H₄, C₂H₆ and CH₃D had been posited to interpret emission bands in Titan's i.r. spectrum. The Voyager Infra-red Spectrometer confirmed that these gases were present and added seven more. The atmosphere is now known to be composed primarily of molecular nitrogen. But the derived mean molecular weight suggests the presence of a significant amount of some heavier gas, most probably argon. It is shown that this argon must be primordial, and that one can understand the evolution of Titan's atmosphere in terms of degassing of a mixed hydrate dominated by CH₄, N₂ and ³⁶Ar. This model satisfactorily explains the absence of neon and makes no special requirements on the satellite's surface temperature.     

Trapping of noble gases in proton-irradiated silicate smokes

Abstract— We have measured Ne, Ar, Kr and Xe in Si₂O₃ “smokes” that were condensed on Al substrates, vapor-deposited with various mixtures of CH₄, NH₃, H₂O and noble gases at 10 K and subsequently irradiated with 1 MeV protons to simulate conditions during grain mantle formation in interstellar clouds. The noble gases were analyzed using conventional stepwise heating and static noble gas mass spectrometry. Neither Ne nor Ar is retained by the samples upon warming to room temperature, but Xe is very efficiently trapped and retained. Kr is somewhat less effectively retained, typically depleted by factors of about 10–20 relative to Xe. Isotopic fractionation favoring the heavy isotopes of Xe and Kr of about 5–10‰/amu is observed. Correlations between the specific chemistry of the vapor deposition and heavy noble gas retention are most likely the result of competition by the various species for irradiation-produced trapping sites. The concentration of Xe retained by some of these smokes exceeds that observed in phase Q of meteorites and, like phase Q, they do not seem to be carriers of the light noble gases. Such artificially prepared material may, therefore, offer clues concerning the incorporation of the heavy planetary noble gases in meteoritic material and the nature of phase Q.     

The sodium and hydrogen gas clouds of Io

Models are developed to describe the spatial distribution of gases emitted by Io and are applied to recent observations which indicate extensive gas clouds of hydrogen and sodium in orbit around Jupiter. Hydrogen and sodium atoms are emitted from Io with velocities in the range 2 to 3 km sec^?1, with fluxes of about 10¹⁰ and 10⁸cm^?2sec^?1 for hydrogen and sodium respectively. Hydrogen atoms may be formed by photodecomposition of gases such as NH₃ or H₂S released from the satellite surface and may escape thermally from an exosphere whose temperature is about 500 K. Sodium may be ejected from the surface by energetic particles or by ultraviolet radiation and it appears that a non-thermal mechanism drawing energy from Jupiter's magnetic field is required in order to account for its release to space.     

Trapping and release of gases by water ice and implications for icy bodies

The trapping and release of H₂, CO, CO₂, CH₄, Ar, Ne, and N₂ by amorphous water ice was studied experimentally under dynamic conditions, at low temperatures starting at 16°K, with gas pressure of 5 × 10^?8?10^?6 Torr. CO, CH₄, Ar, and N₂ were found to be released in three or four distinct temperature ranges, each resulting from a different trapping mechanism: (a) 30–55°K, where the gas frozen on the water ice evaporates; (b) 135–155°K, where gas is squeezed out of the water ice during the transformation of amorphous ice to cubic ice; (c) 165–190°K, where gas and water are released simultaneously, probably by the evaporation of a clathrate hydrate, and, occasionally (d) 160–175°K, where deeply buried gas is released during the transformation of cubic ice to hexagonal ice. If the third range is indeed due to clathrate formation, CO was found to form this compound. CO₂ did not form a clathrate under the experimental conditions. Excess hydrogen did not affect the occlusion of other gases. Hydrogen itself was trapped only at 16°K. Neon was not trapped at 25°K. With cubic ice, the only trapping mechanism is freezing of gas on the ice surface. No fractionation between the gas phase and the ice was observed with a mixture of CO and Ar. Massive ejection of ice grains was observed during the evaporation of the gas in three (a,c,d) out of the four ranges. The experimental results are used to explain several cometary phenomena, especially those occurring at large heliocentric distances, and are applied also to Titan's atmospheric composition and to the possible ejection of ice grains from Enceladus.     

A theoretical investigation into the trapping of noble gases by clathrates on Titan

In this paper, we use a statistical thermodynamic approach to quantify the efficiency with which clathrates on the surface of Titan trap noble gases. We consider different values of the Ar, Kr, Xe, CH₄, C₂H₆ and N₂ abundances in the gas phase that may be representative of Titan's early atmosphere. We discuss the effect of the various parameters that are chosen to represent the interactions between the guest species and the ice cage in our calculations. We also discuss the results of varying the size of the clathrate cages. We show that the trapping efficiency of clathrates is high enough to significantly decrease the atmospheric concentrations of Xe and, to a lesser extent, of Kr, irrespective of the initial gas phase composition, provided that these clathrates are abundant enough on the surface of Titan. In contrast, we find that Ar is poorly trapped in clathrates and, as a consequence, that the atmospheric abundance of argon should remain almost constant. We conclude that the mechanism of trapping noble gases via clathration can explain the deficiency in primordial Xe and Kr observed in Titan's atmosphere by Huygens, but that this mechanism is not sufficient to explain the deficiency in Ar.     

Quantitative evolved gas analysis: Winchcombe in comparison with other CM2 meteorites

Two bulk Winchcombe along with six other CM2 meteorite samples were subjected to quantitative evolved gas analysis. The observed release patterns for almost all volatile species demonstrate close similarity for all the samples and especially between those for Winchcombe. This can be considered as a fingerprint for this petrological type of meteorites. We identified several gases including H₂, H₂O, O₂, CO, CO₂, and SO₂ released in different temperature ranges. The sources and mechanisms of their release were also established. Some of the gases, H₂, CO, and CO₂, are released as a result of oxidation of macromolecular organic material from oxygen derived from oxygen-bearing minerals (a part of CO₂ is also released as a result of decomposition of carbonates). The others, O₂ and H₂O, are associated with the phase transformation/decomposition of phyllosilicates and (oxy)hydrates, while a high-temperature release of SO₂ is associated mostly with the decomposition of sulfides and in few cases also with sulfates. A low-temperature release of SO₂ is due to evaporation and oxidation of elemental sulfur from the meteoritic matrix and organic material. The total concentrations of H (mostly represented by H₂O), C, and S, calculated according to calibration of the quadrupole mass spectrometer with reference gases and decomposition of solid samples (CaSO₄·2H₂O and NaHCO₃) are in reasonable agreement with those determined by independent methods. Variations in the ratio of the carbon amounts released as CO₂ and CO ( $$/C_CO) between the samples could be an indicator of their terrestrial weathering.     

Outgassing of ordinary chondritic material and some of its implications for the chemistry of asteroids, planets, and satellites

We used chemical equilibrium calculations to model thermal outgassing of ordinary chondritic material as a function of temperature, pressure, and bulk composition and use our results to discuss outgassing on asteroids and the early Earth. The calculations include ∼1000 solids and gases of the elements Al, C, Ca, Cl, Co, Cr, F, Fe, H, K, Mg, Mn, N, Na, Ni, O, P, S, Si, and Ti. The major outgassed volatiles from ordinary chondritic material are CH₄, H₂, H₂O, N₂, and NH₃ (the latter at conditions where hydrous minerals form). Contrary to widely held assumptions, CO is never the major C-bearing gas during ordinary chondrite metamorphism. The calculated oxygen fugacity (partial pressure) of ordinary chondritic material is close to that of the quartz-fayalite-iron (QFI) buffer. Our results are insensitive to variable total pressure, variable volatile element abundances, and kinetic inhibition of C and N dissolution in Fe metal. Our results predict that Earth's early atmosphere contained CH₄, H₂, H₂O, N₂, and NH₃; similar to that used in Miller—Urey synthesis of organic compounds.     

Silicon tetrafluoride on Io

Silicon tetrafluoride (SiF₄) is observed in terrestrial volcanic gases and is predicted to be the major F-bearing species in low-temperature volcanic gases on Io [Schaefer, L., Fegley Jr., B., 2005b. Alkali and halogen chemistry in volcanic gases on Io. Icarus 173, 454-468]. SiF₄ gas is also a potential indicator of silica-rich crust on Io. We used F/S ratios in terrestrial and extraterrestrial basalts, and gas/lava enrichment factors for F and S measured at terrestrial volcanoes to calculate equilibrium SiF₄/SO₂ ratios in volcanic gases on Io. We conclude that SiF₄ can be produced at levels comparable to the observed NaCl/SO₂ gas ratio. We also considered potential loss processes for SiF₄ in volcanic plumes and in Io's atmosphere including ion-molecule reactions, electron chemistry, photochemistry, reactions with the major atmospheric constituents, and condensation. Photochemical destruction (t_chem ∼266 days) and/or condensation as Na₂SiF₆ (s) appear to be the major sinks for SiF₄. We recommend searching for SiF₄ with infrared spectroscopy using its 9.7 μm band as done on Earth.     

Penetration of solar uv radiation and photodissociation in the Jovian atmosphere

We present computations of the photodissociation coefficients for NH₃, N₂H₄, PH₃, and H₂S in the Jupiter atmosphere. The calculations take into account multiple scattering and absorption using the radiative-transfer method known as δ-Eddington approximation. The atmospheric models include two cloud layers of variable thickness and haze layers above the upper cloud and between the clouds. One of the results of the radiative computations deal with the reflectivity of the Jovian atmosphere as a function of wavelength. A comparison with available data on the albedo of the planet gives some important indications about mixing ratios and distributions of gases and aerosols. The results for the photolysis rates are compared with similar rates obtained by considering either the direct flux or the flux determined by the molecular gas absorption alone. The latter is usually the approximation used in aeronomic models. The results of this comparison show that a considerable difference exists with direct flux photodissociation but significant differences with molecular absorption flux exist only in atmospheric regions where photodissociation is relatively small.     

Constraints on bulk composition,seasonal variation,and global dynamics of Pluto's atmosphere

Cosmic abundance, vapor pressure, and molecular weight considerations restrict the likely gas candidates for Pluto's atmosphere to Ne, N₂, CO, O₂, and Ar, in addition to the already detected CH₄. The vapor pressures and cosmic abundances of these gases indicate that all except Ne should be saturated in Pluto's atmosphere. The vapor pressure of Ne is so high that the existence of solid or liquid Ne on Pluto's surface is very unlikely; cosmic abundance arguments imply that Ne cannot attain saturation in Pluto's atmosphere. At both perihelion, N₂ should dominate the saturated gases. CO₂ should have the next highest mixing ratio, followed by O₂ and Ar. CH₄ should have the smallest mixing ratio. Because vapor pressures of these gases vary with temperature at diverse rates, the bulk and constituent mixing ratios of Pluto's atmosphere should vary with season. Between perihelion and aphelion, the column abundance of CH₄ may change by a factor of 260 while that of N₂ changes by only a factor of 52. The potential seasonal variation of Pluto's atmosphere was investigated by considering the behavior of these gases when individually mixed with CH₄. The effects of diurnal and latitudinal variation of insolation and eclipses on the atmosphere also were investigated. Seasonal effects are shown to dominate. It was shown that the atmospheric bulk may not be a minimum near aphelion but rather at intermediate distances from the Sun during summer/winter inadequate ice deposits may allow the atmosphere to collapse by freezing out over winter latitudes. If the atmosphere does not collapse, its weight is sufficient to keep it distributed uniformly around Pluto's surface. In this case, the atmosphere tends to regulate the surface temperature to a seasonally dependent value which is uniform over the globe.Finally, the likely global circulation regimes for each model atmosphere as a function of temperature were investigated and it was concluded that if CH₄, O₂, or CO dominates the atmosphere, Pluto will exhibit cyclic variations between an axially symmetric circulation system at perihelion and a baroclinic wave regime at aphelion. However, if N₂ dominates, as is likely, the wave regime should hold continuously. If the atmosphere collapses to a thin halo during summer/winter seasons, only a weak, symmetric circulation should occur.     

Chemistry of atmospheres formed during accretion of the Earth and other terrestrial planets

We used chemical equilibrium and chemical kinetic calculations to model chemistry of the volatiles released by heating different types of carbonaceous, ordinary and enstatite chondritic material as a function of temperature and pressure. Our results predict the composition of atmospheres formed by outgassing during accretion of the Earth and other terrestrial planets. Outgassing of CI and CM carbonaceous chondritic material produces H₂O-rich (steam) atmospheres in agreement with the results of impact experiments. However, outgassing of other types of chondritic material produces atmospheres dominated by other gases. Outgassing of ordinary (H, L, LL) and high iron enstatite (EH) chondritic material yields H₂-rich atmospheres with CO and H₂O being the second and third most abundant gases. Outgassing of low iron enstatite (EL) chondritic material gives a CO-rich atmosphere with H₂, CO₂, and H₂O being the next most abundant gases. Outgassing of CV carbonaceous chondritic material gives a CO₂-rich atmosphere with H₂O being the second most abundant gas. Our results predict that the atmospheres formed during accretion of the Earth and Mars were probably H₂-rich unless the accreted material was dominantly CI and CM carbonaceous chondritic material. We also predict significant amounts of S, P, Cl, F, Na, and K in accretionary atmospheres at high temperatures (1500-2500 K). Finally, our results may be useful for interpreting spectroscopic observations of accreting extrasolar terrestrial planets.     

Optimized running conditions and sensitivity for direction sensitive detectors of WIMP dark matter

Optimum fill pressures for direction-sensitive dark matter detectors based on tracking in gases are considered. Given the minimum resolvable track length and the gas fill, the Lindhard–Scharf stopping model leads to the existence of an optimum pressure which maximizes the specific event rate R (event rate per unit detector volume). In addition, maximizing the detectibility of the recoil nucleus diurnal asymmetry is considered. Optimum fill pressures are calculated for Ar, CF₄, CS₂ and Xe gas fills, as a function of the WIMP mass and the minimum resolvable track length. The associated minimum target volumes required to achieve currently competitive WIMP-nucleon cross-section sensitivity are also calculated. The standard isothermal sphere model of the galactic WIMP halo is used throughout, but the method could be extended to use any desired WIMP distribution function.     

Atmospheric Losses Under Dust Bombardment in the Ancient Atmospheres

We have considered the new process of atmospheric losses - “sputtering” under bombardment by interplanetary dust. It is demonstrated that “sputtering” due to collisions with the interplanetary dust is an effective way of atmospheric gas loss (10^–4–10^–3 of the dust particles' accreting mass) and that it changes the composition of the atmospheric gases. In calculations we have taken that the dust particles collide elastically with the atoms and molecules of the atmosphere. Estimation of the effects of inelastic collisions was also considered. As a result of these collisions a part of the atmospheric atoms and molecules will have “upward” velocity and enough energy to escape. It was considered that escaping atoms can collide with the atoms of the “main” gas of the upper atmosphere. The atmospheric gas composition is assumed to be just as in the modern Martian atmosphere - the “main” gases in the upper atmosphere were taken to be O and CO₂. In our computations we pay particular attention to the abundance of noble gases in planetary atmospheres since these gases are very important for theories of atmospheric origin. We computed that under “sputtering” by the interplanetary dust, atmospheres were enriched by the “heavy” elements and isotopes in the wide range of the upper atmospheric parameters O/CO₂, T/g (O/CO₂– on the level of homosphere;T is temperature of the exosphere,g is gravitational acceleration). However the loss efficiency for “heavy” gases is relatively high compared to other known gas loss processes. In the case of noble gases for the specific parameters of the upper atmosphere (small T/g ratio; high O/CO₂ on the level of homosphere) we have got the unique result: despite the diffusion separation in the upper atmosphere the loss efficiency of Xe > Kr > Ar. The effect of “sputtering” of the planetary atmospheres was strongest during the early stages of the planetary evolution - when the rate of the dust accretion was intrinsically higher than now because of collisions of planetesimals. In light of the new escape process, the main peculiarities of the noble gases abundance in the planetary atmospheres could be explained. This revised version was published online in July 2006 with corrections to the Cover Date.     

Atmospheric Chemistry in Giant Planets, Brown Dwarfs, and Low-Mass Dwarf Stars: I. Carbon, Nitrogen, and Oxygen

The chemical species containing carbon, nitrogen, and oxygen in atmospheres of giant planets, brown dwarfs (T and L dwarfs), and low-mass stars (M dwarfs) are identified as part of a comprehensive set of thermochemical equilibrium and kinetic calculations for all elements. The calculations cover a wide temperature and pressure range in the upper portions of giant planetary and T-, L-, and M-dwarf atmospheres. Emphasis is placed on the major gases CH₄, CO, NH₃, N₂, and H₂O but other less abundant gases are included. The results presented are independent of particular model atmospheres, and can be used to constrain model atmosphere temperatures and pressures from observations of different gases. The influence of metallicity on the speciation of these key elements under pressure-temperature (P-T) conditions relevant to low-mass object atmospheres is discussed. The results of the thermochemical equilibrium computations indicate that several compounds may be useful to establish temperature or pressure scales for giant planet, brown dwarf, or dwarf star atmospheres. We find that ethane and methanol abundance are useful temperature probes in giant planets and methane dwarfs such as Gl 229B, and that CO₂ can serve as a temperature probe in more massive objects. Imidogen (NH) abundances are a unique pressure-independent temperature probe for all objects. Total pressure probes for warmer brown dwarfs and M dwarfs are HCN, HCNO, and CH₂O. No temperature-independent probes for the total pressure in giant planets or T-dwarf atmospheres are identified among the more abundant C, N, and O bearing gases investigated here.     

Pressure dependent trace gas trapping in amorphous water ice at 77 K: Implications for determining conditions of comet formation

The nature of cometary volatile materials is subject to debate. Theoretical models of cometary nuclei and laboratory studies suggest that these objects could be made of amorphous water ice in addition to other volatile molecules and refractory grains. This water ice structure has the ability to encapsulate the gases of surrounding environment, reflecting the physical and chemical conditions during their deposition. Therefore, the knowledge of the chemical composition of volatile molecules trapped in amorphous water ice provides a tool for probing the formation environment of cometary ice grains. Experimental studies of gas trapping efficiency in amorphous water ice have been previously conducted mostly under kinetic conditions, where dynamic pumping and temperature gradients prevented rigorous calibrations. In this work, we investigated the trapping efficiencies of Ar, CO, CH₄, Kr and N₂ by depositing water vapor as ice in the presence of trace gases in a volume submerged in liquid nitrogen at 77 K. The gas trapping efficiencies were determined simply by monitoring the pressure difference of the trace gases before and after the deposition of a known amount of water molecules as amorphous ice.Our results show that the trapped gas to water molecule ratio in amorphous ice is controlled primarily by the partial pressure of the gas during water ice deposition, and is independent of the ice deposition rate as well as the gas to water ratio in the vapor phase. The trapping efficiencies of gases decrease in the order of Kr > CH₄ > CO > Ar > N₂ in accordance with previous studies. Assuming that the water ice structure of comets is at least partially amorphous water ice at the time of their formation, these results suggest that the total pressure and composition of the surrounding environment of amorphous ice formation are significant controlling factors of trace gas concentrations in cometary ice. This further indicates that the evolution of the solar nebula and timing of cometary ice condensation can also be important parameters in linking the volatile contents of comets and their formation process.     

Observations of the inner coma of C/1995O1 (Hale-Bopp)—gas and dust production

Hale-Bopp (C/1995 O1) was the most productive recent comet observed in terms of gas and dust output. Since its discovery in 1995 at a distance of 7.14 AU from the Sun, the comet has been well observed, revealing the dynamics of a rare and large comet. Hale-Bopp showed strong emissions of the principle cometary gases CN, C₃, and C₂, as well as an abundance of dust. The production rates of these gases were found to be 1.45×10²⁸, 1.71×10²⁸, and , respectively, with dust production, in terms of Afρ, , as measured in the green continuum (5260 Å). The observations for this paper are presented in two groups spanning 10 days each, one group centered near 32 days prior to and the other 21 days after perihelion. The averages of dust and gas production rates show a slightly higher value for each prior to perihelion than after perihelion, consistent with a possible peak in production a few weeks prior to perihelion passage.     

Identification of magnetite in lunar regolith breccia 60016: Evidence for oxidized conditions at the lunar surface

Lunar regolith breccias are temporal archives of magmatic and impact bombardment processes on the Moon. Apollo 16 sample 60016 is an “ancient” feldspathic regolith breccia that was converted from a soil to a rock at ~3.8 Ga. The breccia contains a small (70 × 50 μm) rock fragment composed dominantly of an Fe‐oxide phase with disseminated domains of troilite. Fragments of plagioclase (An_95‐97), pyroxene (En_74‐75, Fs_21‐22,Wo_3‐4), and olivine (Fo_66‐67) are distributed in and adjacent to the Fe‐oxide. The silicate minerals have lunar compositions that are similar to anorthosites. Mineral chemistry, synchrotron X‐ray absorption near edge spectroscopy (XANES) and X‐ray diffraction (XRD) studies demonstrate that the oxide phase is magnetite with an estimated Fe³⁺/ΣFe ratio of ~0.45. The presence of magnetite in 60016 indicates that oxygen fugacity during formation was equilibrated at, or above, the Fe‐magnetite or wüstite–magnetite oxygen buffer. This discovery provides direct evidence for oxidized conditions on the Moon. Thermodynamic modeling shows that magnetite could have been formed from oxidization‐driven mineral replacement of Fe‐metal or desulphurisation from Fe‐sulfides (troilite) at low temperatures (<570 °C) in equilibrium with H₂O steam/liquid or CO₂ gas. Oxidizing conditions may have arisen from vapor transport during degassing of a magmatic source region, or from a hybrid endogenic–exogenic process when gases were released during an impacting asteroid or comet impact.     

Experimental investigation of the critical ionization velocity in gas mixtures

The critical ionization velocity which is of cosmogonic and astrophysical interest has hitherto mainly been investigated for pure gases. Since in space we always have gas mixtures, it is of interest also to study gas mixtures. The present report, which is a summary of a more detailed report (Axnäs, 1976), summarizes the results of systematic experiments on the critical ionization velocity as a function of the mixing ratio for binary gas mixtures of H₂, He, N₂, O₂, Ne and Ar. The apparatus used is a coaxial plasma gun with an azimuthal magnetic field. The discharge parameters are chosen so that the plasma is weakly ionized. In some of the mixtures it is found that one of the components tends to dominate in the sense that only a small amount (regarding volume) of that component is needed for the discharge to adopt a limiting velocity close to that for the pure component. Thus in a mixture between a heavy and a light component having nearly equal ionization potentials, the heavy component dominates. Also, if there is a considerable difference in ionization potential between the components, the component with the lowest ionization potential tends to dominate.Paper dedicated to Professor Hannes Alfvén on the occasion of his 70th birthday, 30 May, 1978.     

Greenhouse gas emissions from a managed grassland

Managed grasslands contribute to global warming by the exchange of the greenhouse gases carbon dioxide, nitrous oxide and methane. To reduce uncertainties of the global warming potential of European grasslands and to assess potential mitigation options, an integrated approach quantifying fluxes from all three gases is needed. Greenhouse gas emissions from a grassland site in the SE of Scotland were measured in 2002 and 2003. Closed static chambers were used for N₂O and CH₄ flux measurements, and samples were analysed by gas chromatography. Closed dynamic chambers were used for soil respiration measurements, using infrared gas analysis. Three organic manures and two inorganic fertilizers were applied at a rate of 300 kg N ha⁻¹ a⁻¹ (available N) and compared with a zero-N control on grassland plots in a replicated experimental design. Soil respiration from plots receiving manure was up to 1.6 times larger than CO₂ release from control plots and up to 1.7 times larger compared to inorganic treatments (p<0.05). A highly significant (p<0.001) effect of fertilizer and manure treatments on N₂O release was observed. Release of N₂O from plots receiving inorganic fertilizers resulted in short term peaks of up to 388 g N₂O–N ha⁻¹ day⁻¹. However losses from plots receiving organic manures were both longer lasting and greater in magnitude, with an emission of up to 3488 g N₂O–N ha⁻¹ day⁻¹ from the sewage sludge treatments. During the 2002 growing season the cumulative total N₂O flux from manure treatments was 25 times larger than that from mineral fertilizers. CH₄ emissions were only significantly increased (p<0.001) for a short period following applications of cattle slurry. Although soil respiration in manure plots was high, model predictions and micrometeorological flux measurements at an adjacent site suggest that all plots receiving fertilizer or manure acted as a sink for CO₂. Therefore in terms of global warming potentials the contribution of N₂O from manure treatments becomes particularly important. There were considerable variations in N₂O and CO₂ fluxes between years, which was related to annual variations in soil temperature and rainfall.     

Primordial noble gases in “phase Q” in carbonaceous and ordinary chondrites studied by closed‐system stepped etching

Abstract— The HF/HCI‐resistant residues of the chondrites CM2 Cold Bokkeveld, CV3 (ox.) Grosnaja, CO3.4 Lancé, CO3.7 Isna, LL3.4 Chainpur, and H3.7 Dimmitt have been measured by closed‐system stepped etching (CSSE) in order to better characterise the noble gases in “phase Q”, a major carrier of primordial noble gases. All isotopic ratios in phase Q of the different meteorites are quite uniform, except for (²⁰Ne/²²Ne)_Q. As already suggested by precise earlier measurements (Schelhaas et al., 1990; Wieler et al., 1991, 1992), (²⁰Ne/²²Ne)_Q is the least uniform isotopic ratio of the Q noble gases. The data cluster ～10.1 for Cold Bokkeveld and Lancé and 10.7 for Chainpur, Grosnaja, and Dimmitt, respectively. No correlation of (²⁰Ne/²²Ne)_Q with the classification or the alteration history of the meteorites has been found. The Ar, Kr, and Xe isotopic ratios for all six samples are identical within their uncertainties and similar to earlier Q determinations as well as to Ar‐Xe in ureilites. Thus, an unknown process probably accounts for the alteration of the originally incorporated Ne‐Q. The noble gas elemental compositions provide evidence that Q consists of at least two carbonaceous carrier phases “Q1” and “Q2” with slightly distinct chemical properties. Ratios (Ar/Xe)_Q and (Kr/Xe)_Q reflect both thermal metamorphism and aqueous alteration. These parent‐body processes have led to larger depletions of Ar and Kr relative to Xe. In contrast, meteorites that suffered severe aqueous alteration, such as the CM chondrites, do not show depletions of He and Ne relative to Ar but rather the highest (He/Ar)_Q and (Ne/Ar)_Q ratios. This suggests that Q1 is less susceptible to aqueous alteration than Q₂. Both subphases may well have incorporated noble gases from the same reservoir, as indicated by the nearly constant, though very large, depletion of the lighter noble gases relative to solar abundances. However, the elemental ratios show that Q₁ and Q₂ must have acquired (or lost) noble gases in slightly different element proportions. Cold Bokkeveld suggests that Q₁ may be related to presolar graphite. Phases Q₁ and Q₂ might be related to the subphases that have been suggested by Gros and Anders (1977). The distribution of the ²⁰Ne/²²Ne ratios cannot be attributed to the carriers Q₁ and Q₂. The residues of Chainpur and Cold Bokkeveld contain significant amounts of Ne‐E(L), and the data confirm the suggestion of Huss (1997) that the ²²Ne‐E(L) content, and thus the presolar graphite abundances, are correlated with the metamorphic history of the meteorites.