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PubMed2004

Dual column capillary gas chromatographic system for the in situ analysis of volatile organic compounds on a cometary nucleus.

Two Wall Coated Open Tubular capillary columns, coated with poly(cyanopropylphenyl-dimethyl)siloxane and poly(diphenyl-dimethyl)siloxane stationary phases, have been selected for use in the COmetary SAmpling and Composition space experiment for the separation and identification of the wide range of volatile organic compounds which could be present in cometary nuclei. This article presents the main characteristics of the tandem column system for the analysis of solutes of cometary interest within the constraints of space instrumental operating conditions. The high efficiency of the columns is demonstrated and the influence of the operating conditions on their separation properties are investigated. The studied columns exhibit complementary retention pattern: their use in a dual column system makes it possible to achieve the separation and the identification of the compounds of interest. Finally, the good analytical behavior of the columns when analyzing samples which include large amounts of water, the main presumed volatile in comets, is demonstrated. The presented results thus show the suitability of the selected tandem columns system for the desired analyses, and their performance on adaptation to in-situ cometary chemical investigation.

Chromatography, Gas↗
PubMed1986

Molecular selection in a unified evolutionary sequence.

With guidance from experiments and observations that indicate internally limited phenomena, an outline of unified evolutionary sequence is inferred. Such unification is not visible for a context of random matrix and random mutation. The sequence proceeds from Big Bang through prebiotic matter, protocells, through the evolving cell via molecular and natural selection, to mind, behavior, and society.

Amino Acids↗
PubMed2004

Assignment of quinone derivatives as the main compound class composing 'interstellar' grains based on both polarity ions detected by the 'Cometary and Interstellar Dust Analyser' (CIDA) onboard the spacecraft STARDUST.

The 'Cometary and Interstellar Dust Analyser' (CIDA) is a particle impact time-of-flight mass spectrometer onboard the NASA spacecraft STARDUST. A series of positive and negative ion mass spectra from the impact of (apparently) interstellar dust particles has been collected since 1999. In the meantime laboratory work has been performed to better understand the ion formation processes of organic grains impacting at those speeds (>15 km/s) and to relate them to some other ion formation methods. The key ion types were the negative ions, with some additional information from the positive ions. Here, first the principal ion formation rules are briefly reviewed. Secondly, the common substance class is inferred mainly by the application of exclusion principles, and appears to be partly condensed aromatic and quinonoid compounds with high oxygen and low nitrogen content. Oxygen appears to be present in quinone-type structures with condensed aromatic rings, possibly with furan substructures and some hydroxyl moieties. Some nitrogen may be present in pyrrole- or quinoline-type structures. Considerations of thermodynamics and radiation physics of these dust particles within the solar system are consistent with this interpretation. Quinoenzyme cofactors such as the known compound pyrroloquinoline-quinone (PQQ) and its subconstituents would be expected to yield similar mass spectra.

Dust↗
PubMed1993

Habitable zones around main sequence stars.

A one-dimensional climate model is used to estimate the width of the habitable zone (HZ) around our Sun and around other main sequence stars. Our basic premise is that we are dealing with Earth-like planets with CO2/H2O/N2 atmospheres and that habitability requires the presence of liquid water on the planet's surface. The inner edge of the HZ is determined in our model by loss of water via photolysis and hydrogen escape. The outer edge of the HZ is determined by the formation of CO2 clouds, which cool a planet's surface by increasing its albedo and by lowering the convective lapse rate. Conservative estimates for these distances in our own Solar System are 0.95 and 1.37 AU, respectively; the actual width of the present HZ could be much greater. Between these two limits, climate stability is ensured by a feedback mechanism in which atmospheric CO2 concentrations vary inversely with planetary surface temperature. The width of the HZ is slightly greater for planets that are larger than Earth and for planets which have higher N2 partial pressures. The HZ evolves outward in time because the Sun increases in luminosity as it ages. A conservative estimate for the width of the 4.6-Gyr continuously habitable zone (CHZ) is 0.95 to 1.15 AU. Stars later than F0 have main sequence lifetimes exceeding 2 Gyr and, so, are also potential candidates for harboring habitable planets. The HZ around an F star is larger and occurs farther out than for our Sun; the HZ around K and M stars is smaller and occurs farther in. Nevertheless, the widths of all of these HZs are approximately the same if distance is expressed on a logarithmic scale. A log distance scale is probably the appropriate scale for this problem because the planets in our own Solar System are spaced logarithmically and because the distance at which another star would be expected to form planets should be related to the star's mass. The width of the CHZ around other stars depends on the time that a planet is required to remain habitable and on whether a planet that is initially frozen can be thawed by modest increases in stellar luminosity. For a specified period of habitability, CHZs around K and M stars are wider (in log distance) than for our Sun because these stars evolve more slowly. Planets orbiting late K stars and M stars may not be habitable, however, b ecause they can become trapped in synchronous rotation as a consequence of tidal damping. F stars have narrower (log distance) CHZ's than our Sun because they evolve more rapidly. Our results suggest that mid-to-early K stars should be considered along with G stars as optimal candidates in the search for extraterrestrial life.

Atmosphere↗
PubMed1993

Secondary processing of chondrules and refractory inclusions (CAIs) by gasdynamic heating.

A theoretical model of aerodynamic heating of a meteoric particle upon entry into a parent body atmosphere is presented. The model includes the effects of melting, vaporization, and heat conduction into the particle interior. Properties of chondrule rims are interpreted in the context of the model. We conclude that the formation of true melt rims by atmospheric entry requires that a low-melting-temperature component be fractionated in the outer part of the chondrule prior to rim formation, and that the range of thermal alteration effects observed in UOC chondrites reflects the variety of encounter conditions and chondrite types. Further tests of the model are suggested.

Atmosphere↗
PubMed1993

What can meteorites tell us about nebular conditions and processes during planetesimal accretion?

Analysis of the most primitive meteorites can yield detailed information about environmental conditions and physical/chemical processes in the earliest Solar System, including the nebular stage during which planetesimals were accreted. Such information pertains to time scales, thermal and chemical evolution, inhomogeneity and mixing, magnetic fields, and grain growth in the solar nebula. Nebular processes identified include evaporation, condensation, localized melting, and fractionation both of solids from gas and among different solids. Little direct evidence remains even in primitive meteorites of the actual accretion process. The absence of intrinsic factors capable of enhancing accretion among meteoritic constituents suggests that gravitational instabilities might have been important in promoting planetesimal accretion.

Chemical Phenomena↗
PubMed1993

Formation of planetary embryos: effects of fragmentation, low relative velocity, and independent variation of eccentricity and inclination.

An earlier investigation of the formation of approximately 10(26) g planetary embryos from much smaller planetesimals (G.W. Wetherill and G.R. Stewart 1989, Icarus 77, 350-357) has been extended to include the effects of collisional fragmentation, the low relative velocity regime in which the effects due to solar gravity are important, and independent perturbations of eccentricity and inclination. In agreement with this earlier work, it if found that at 1 AU runaway growth occurs on a approximately 10(-5)-year time scale as a consequence of equipartition of energy between large and small planetesimals. It is now seen that the runaway is initiated after approximately 10(4) years, when the relative velocities of the larger bodies temporarily fall into the low-velocity regime, lowering their inclinations and increasing their gravitational capture rates. After approximately 2 X 10(4) years, relative velocities between most bodies emerge from the low-velocity regime, and these higher velocities tend to inhibit further runaway growth. This rapid runaway growth is self-regulated, however, by these same higher velocities, causing fragmentation of the smaller bodies. The velocities of the collision fragments are reduced by gas drag, facilitating their capture by the growing runaway embryos. Variations in which different fragmentation models are used, or long-range forces between nonrunaway bodies are absent, give similar results. When fragmentation is not included, the time scale for growth increases to approximately 3 X 10(5) years as a result of loss of the self-regulating process described above.

Astronomical Phenomena↗
PubMed1993

Hydrothermal processing of cometary volatiles--applications to Triton.

Subsequent to its capture by Neptune, Triton could have experienced an episode of tidal heating sufficient to melt its icy mantle and possibly its rocky core as well. This heating would have driven hydrothermal circulation at the core-rock/mantle-ocean boundary. We consider the chemical consequences of this hydrothermal reprocessing on Triton's volatile budget by assuming an initial cometary composition for the icy mantle and evaluating the effects of changes in temperature and oxidation state. We assume that the latter would have been controlled by mineral assemblages in the rock. Such reprocessing could explain the lack of carbon monoxide in the atmosphere of Triton and its depletion relative to N2 and (apparently) CO2 in the satellite's surface ices. Our calculations also show that whatever the original source of nitrogen in Triton, N2 and/or NH3 are likely abundant products of hydrothermal reprocessing. Depending on the temperature and prevailing oxidation state, acetic acid, ethanol, urea, methanol, and ethanamine are possible important components, in addition to ammonia, of the resulting mantle material. Triton may thus preserve the organic chemistry that might have led to the origin of life in early terrestrial hydrothermal systems.

Ammonia↗
PubMed1993

The condensation and vaporization behavior of ices containing SO2, H2S, and CO2: implications for Io.

In an extension of previously reported work on ices containing CO, CO2, H2O, CH3OH, NH3, and H2, measurements of the physical and infrared spectral properties of ices containing molecules relevant to Jupiter's moon Io are presented. These include studies on ice systems containing SO2, H2S, and CO2. The condensation and sublimation behaviors of each ice system and surface binding energies of their components are discussed. The surface binding energies can be used to calculate the residence times of the molecules on a surface as a function of temperature and thus represent important parameters for any calculation that attempts to model the transport of these molecules on Io's surface. The derived values indicate that SO2 frosts on Io are likely to anneal rapidly, resulting in less fluffy, "glassy" ices and that H2S can be trapped in the SO2 ices of Io during night-time hours provided that SO2 deposition rates are on the order of 5 micrometers/hr or larger.

Carbon Dioxide↗
PubMed1994

Magnetically enhanced coagulation of very small iron grains.

Laboratory experiments, in which very small (approximately 20 nm) grains are produced in the presence of a magnetic field on the order of 100 Gauss in a low-pressure hydrogen atmosphere, have demonstrated that such smokes can become permanently magnetized. We show that magnetization results in an enormous enhancement in the coagulation efficiency of such materials even in the absence of external magnetic fields. Small iron grains should have been produced in the solar nebula by thermal processing of preexisting interstellar grains. If such processing occurred via high-energy electromagnetic events then the resultant magnetized grains could have triggered the formation of centimeter- to meter-sized protoplanetessimals by acting as "nets" capable of sweeping up nonconductive silicates suspended in the gas. It is possible that the presence of conductive fractal aggregates observed in modern-day protostellar disks could be explained by the enhanced coagulation efficiency of very small magnetized iron particles.

Astronomical Phenomena↗
PubMed1994

The organic surface of 5145 Pholus: constraints set by scattering theory.

No known body in the Solar System has a spectrum redder than that of object 5145 Pholus. We use Hapke scattering theory and optical constants measured in this laboratory to examine the ability of mixtures of a number of organic solids and ices to reproduce the observed spectrum and phase variation. The primary materials considered are poly-HCN, kerogen, Murchison organic extract, Titan tholin, ice tholin, and water ice. In a computer grid search of over 10 million models, we find an intraparticle mixture of 15% Titan tholin, 10% poly-HCN, and 75% water ice with 10-micrometers particles to provide an excellent fit. Replacing water ice with ammonia ice improves the fits significantly while using a pure hydrocarbon tholin, Tholin alpha, instead of Titan tholin makes only modest improvements. All acceptable fits require Titan tholin or some comparable material to provide the steep slope in the visible, and poly-HCN or some comparable material to provide strong absorption in the near-infrared. A pure Titan tholin surface with 16-micrometers particles, as well as all acceptable Pholus models, fit the present spectrophotometric data for the transplutonian object 1992 QB1. The feasibility of gas-phase chemistry to generate material like Titan tholin on such small objects is examined. An irradiated transient atmosphere arising from sublimating ices may generate at most a few centimeters of tholin over the lifetime of the Solar System, but this is insignificant compared to the expected lag deposit of primordial contaminants left behind by the sublimating ice. Irradiation of subsurface N2/CH4 or NH3/CH4 ice by cosmic rays may generate approximately 20 cm of tholin in the upper 10 m of regolith in the same time scale but the identity of this tholin to its gas-phase equivalent has not been demonstrated.

Ammonia↗
PubMed1994

Is H2O present on Io? The detection of a new strong band near 3590 cm-1 (2.79 micrometers).

A strong absorption band at 3590 +/- 20 cm-1 (2.790 +/- 0.015 micrometers) has been discovered in the spectrum of Io using the Kuiper Airborne Observatory (KAO). The 2 nu1 + nu3 combination mode of solid SO2 falls at this position. Since SO2 is abundant on Io it must contribute to the new band. However, a band due to H2O was predicted near this frequency in Io's spectrum based on laboratory experiments of H2O:SO2 mixed Io ice analogs which were used to assign the two weak, variable features of 3370 and 3170 cm-1 (2.97 and 3.15 micrometers) to trace amounts of H2O frozen in solid SO2 on Io. The new band probably originates from both SO2 and H2O. Unfortunately, the spectral resolution of the data is insufficient to settle the issue of whether there are two resolvable components.

Aircraft↗
PubMed1994

The collision of Jupiter and Comet Shoemaker-Levy 9.

A simple description of the disruption and deceleration of 100-m- to 5-km-diameter comets striking Jupiter is combined with numerical simulations of the subsequent explosions to predict the fate of Comet Shoemaker-Levy 9. Kilometer-size objects of density 1 g/cm3 explode at about the 10-bar level; a fragment of the same diameter but of density 0.3 g/cm3 explodes at about the 2-bar level. Detailed numerical simulations of the first 3 min of the explosion were performed using the astrophysical hydrodynamics program ZEUS-3D. Our numerical simulations begin either with hot cylinders with dimensions suggested by the disruption and deceleration model or with an initial wake constructed from a moving line charge. In all cases, extensive plumes of hot gas are expelled from the atmosphere. The models with wakes evolve about twice as fast as the initially confined models. Models of both types generate similar pressure waves into the planet. Temperatures and negative hydrogen ion opacities were computed by solving a battery of Saha equations. For atmospheric entry, light curves were computed assuming thermal radiation by clean jovian air with a surface area consistent with the (changing) cross-sectional area of the impactor. On entry the largest bolides could be very bright, possibly as bright as Jupiter for observers placed to see them, although for kilometer-size impactors the luminosity peak is obscured by clouds. The timescale is about 10 sec. For the fireball, light curves were computed from the numerical simulations assuming a grey atmosphere. Metals from the vaporized comet provide electrons that dramatically increase the opacity of Jovian air at low temperature; the resulting effective radiating temperature of the fireball is of order 3000 K. The fireball rises through and above the atmosphere, brightening at first as its surface area increases, but later fading to invisibility as its temperature drops and its opacity plummets. The timescale is about 100 sec.

Astronomy↗
PubMed1994

Chemical investigation of Titan and Triton tholins.

We report chromatographic and spectroscopic analyses of both Titan and Triton tholins, organic solids made from the plasma irradiation of 0.9:0.1 and 0.999:0.001 N2/CH4 gas mixtures, respectively. The lower CH4 mixing ratio leads to a nitrogen-richer tholin (N/C > 1), probably including nitrogen heterocyclic compounds. Unlike Titan tholin, bulk Triton tholin is poor in nitriles. From high-pressure liquid chromatography, ultraviolet and infrared spectroscopy, and molecular weight estimation by gel filtration chromatography, we conclude that (1) several H2O-soluble fractions, each with distinct UV and IR spectral signatures, are present, (2) these fractions are not identical in the two tholins, (3) the H2O-soluble fractions of Titan tholins do not contain significant amounts of nitriles, despite the major role of nitriles in bulk Titan tholin, and (4) the H2O-soluble fractions of both tholins are mainly molecules containing about 10 to 50 (C + N) atoms. We report yields of amino acids upon hydrolysis of Titan and Triton tholins. Titan tholin is largely insoluble in the putative hydrocarbon lakes or oceans on Titan, but can yield the H2O-soluble species investigated here upon contact with transient (e.g., impact-generated) liquid water.

Amino Acids↗
PubMed1994

Clouds, hazes, and the stratospheric methane abundance in Neptune.

Analysis of high-spatial-resolution (approximately 0.8 arcsec) methane band and continuum imagery of Neptune's relatively homogeneous Equatorial Region yields significant constraints on (1) the stratospheric gaseous methane mixing ratio (fCH4,s), (2) the column abundances and optical properties of stratospheric and tropospheric hydrocarbon hazes, and (3) the wavelength-dependent single-scattering albedo of the 3-bar opaque cloud. From the center-to-limb behavior of the 7270-angstroms and 8900-angstrom sCH4 bands, the stratospheric methane mixing ratio is limited to fCH4,s < 1.7 x 10(-3), with a nominal value of fCH4,s = 3.5 x 10(-4), one to two orders of magnitude less than pre-Voyager estimates, but in agreement with a number of recent ultraviolet and thermal infrared measurements, and largely in agreement with the tropopause mixing ratio implied by Voyager temperature measurements. Upper limits to the stratospheric haze mass column abundance and 6190-angstroms and 8900-angstroms haze opacities are 0.61 microgram cm-2 and 0.075 and 0.042, respectively, with nominal values of 0.20 microgram cm-2 and 0.025 and 0.014 for the 0.2-micrometer radius particles preferred by the recent Voyager PPS analysis of Pryor et al. (1992, Icarus 99, 302-316). The tropospheric CH4 haze opacities are comparable to that found in the stratosphere, upper limits of 0.104 and 0.065 at 6190 angstroms and 8900 angstroms, respectively, with nominal values of 0.085 and 0.058. This indicates a column abundance less than 11.0 micrograms cm-2, corresponding to the methane gas content within a well-mixed 3% methane tropospheric layer only 0.1 cm thick near the 1.5-bar CH4 condensation level. Constraints on the single-scattering albedos of these hazes include (1) for the stratospheric component, 6190-angstroms and 8900-angstroms imaginary indices of refraction less than 0.047 and 0.099, respectively, with 0.000 (conservative scattering) being the nominal value at both wavelengths, and (2) CH4 haze single-scattering albedos greater than 0.85 and 0.50 at these two wavelengths, with conservative scattering again begin the preferred value. However, conservative scattering is ruled out for the opaque cloud near 3 bars marking the bottom of the visible atmosphere. Specifically, we find cloud single-scattering albedos of 0.915 +/- 0.006 at 6340 angstroms, 0.775 +/- 0.012 at 7490 angstroms, and 0.803 +/- 0.010 at 8260 angstrom. Global models utilizing a complete global spectrum confirm the red-absorbing character of the 3-bar cloud. The global-mean model has approximately 7.7 times greater stratospheric aerosol content then the Equatorial Region. An analysis of stratospheric haze precipitation rates indicates a steady-state haze production rate of 0.185-1.5 x 10(-14) g cm-2 sec-1, in agreement with recent theoretical photochemical estimates. Finally, reanalysis of the Voyager PPS 7500-angstroms phase angle data utilizing the fCH4,s value derived here confirms the Pryor et al. result of a tropospheric CH4 haze opacity of a few tenths in the 22-30 degrees S latitude region, several times that of the Equatorial Region or of the globe. The factor-of-10 reduction in fCH4,s below that assumed by Pryor et al. implies decreased gas absorption and consequently a decrease in the forward-scattering component of tropospheric aerosols.

Aerosols↗
PubMed1994

H2O-H2SO4 system in Venus' clouds and OCS, CO, and H2SO4 profiles in Venus' troposphere.

A coupled problem of diffusion and condensation is solved for the H2SO4-H2O system in Venus' cloud layer. The position of the lower cloud boundary and profiles of the H2O and H2SO4 vapor mixing ratios and of the H2O/H2SO4 ratio of sulfuric acid aerosol and its flux are calculated as functions of the column photochemical production rate of sulfuric acid, phi H2SO4. Variations of the lower cloud boundary are considered. Our basic model, which is constrained to yield fH2O (30 km) = 30 ppm (Pollack et al. 1993), predicts the position of the lower cloud boundary at 48.4 km coinciding with the mean Pioneer Venus value, the peak H2SO4 mixing ratio of 5.4 ppm, and the H2SO4 production rate phi H2SO4 = 2.2 x 10(12) cm-2 sec-1. The sulfur to sulfuric acid mass flux ratio in the clouds is 1 : 27 in this model, and the mass loading ratio may be larger than this value if sulfur particles are smaller than those of sulfuric acid. The model suggests that the extinction coefficient of sulfuric acid particles with radius 3.7 micrometers (mode 3) is equal to 0.3 km-1 in the middle cloud layer. The downward flux of CO is equal to 1.7 x 10(12) cm-2 sec-1 in this model. Our second model, which is constrained to yield fH2SO4 = 10 ppm at the lower cloud boundary, close to the value measured by the Magellan radiooccultations, predicts the position of this boundary to be at 46.5 km, which agrees with the Magellan data; fH2O(30 km) = 90 ppm, close to the data of Moroz et al. (1983) at this altitude; phi H2SO4 = 6.4 x 10(12) cm-2 sec-1; and phi co = 4.2 x 10(12) cm-2 sec-1. The S/H2SO4 flux mass ratio is 1 : 18, and the extinction coefficient of the mode 3 sulfuric acid particles is equal to 0.9 km-1 in the middle cloud layer. A strong gradient of the H2SO4 vapor mixing ratio near the bottom of the cloud layer drives a large upward flux of H2SO4, which condenses and forms the excessive downward flux of liquid sulfuric acid, which is larger by a factor of 4-7 than the flux in the middle cloud layer. This is the mechanism of formation of the lower cloud layer. Variations of the lower cloud layer are discussed. Our modeling of the OCS and CO profiles in the lower atmosphere measured by Pollack et al. (1993) provides a reasonable explanation of these data and shows that the rate coefficient of the reaction SO3 + CO --> CO2 + SO2 is equal to 10(-11) exp(-(13,100 +/- 1000)/T) cm3/s. The main channel of the reaction between SO3 and OCS is CO2 + (SO)2, and its rate coefficient is equal to 10(-11) exp(-(8900 +/- 500)T)cm3/s. In the conditions of Venus' lower atmosphere, (SO)2 is removed by the reaction (SO)2 + OCS --> CO + S2 + SO2. The model predicts an OCS mixing ratio of 28 ppm near the surface.

Atmosphere↗
PubMed1994

First measurement of helium on Mars: implications for the problem of radiogenic gases on the terrestrial planets.

108 +/- 11 photons of the martian He 584-angstroms airglow detected by the Extreme Ultraviolet Explorer satellite during a 2-day exposure (January 22-23, 1993) correspond to the effective disk average intensity of 43 +/- 10 Rayleigh. Radiative transfer calculations, using a model atmosphere appropriate to the conditions of the observation and having an exospheric temperature of 210 +/- 20 K, result in a He mixing ratio of 1.1 +/- 0.4 ppm in the lower atmosphere. Nonthermal escape of helium is due to electron impact ionization and pickup of He+ by the solar wind, to collisions with hot oxygen atoms, and to charge exchange with molecular species with corresponding column loss rates of 1.4 x 10(5), 3 x 10(4), and 7 x 10(3) cm-2 sec-1, respectively. The lifetime of helium on Mars is 5 x 10(4) years. The He outgassing rate, coupled with the 40Ar atmospheric abundance and with the K:U:Th ratio measured in the surface rocks, is used as input to a single two-reservoir degassing model which is applied to Mars and then to Venus. A similar model with known abundances of K, U, and Th is applied to Earth. The models for Earth and Mars presume loss of all argon accumulated in the atmospheres during the first billion years by large-scale meteorite and planetesimal impacts. The models show that the degassing coefficients for all three planets may be approximated by function delta = delta (0)(t(0)/t)1/2 with delta (0) = 0/1, 0.04, and 0.0125 Byr-1 for Earth, Venus, and Mars, respectively. After a R2 correction this means that outgassing processes on Venus and Mars are weaker than on Earth by factors of 3 and 30, respectively. Mass ratios of U and Th are almost the same for all three planets, while potassium is depleted by a factor of 2 in Venus and Mars. Mass ratios of helium and argon are close to 5 x 10(-9) and 2 x 10(-8) g/g in the interiors of all three planets. The implications of these results are discussed.

Argon↗
PubMed1994

Near-infrared spectroscopy of dark asteroids.

Near-infrared (J, H and K bands) spectra of nine dark asteroids (chosen among a sample of supposed primitive objects between C and D classes) have been obtained at the Mauna Kea Observatory (Hawaii) with the 2.2-m telescope using KSPEC as spectrograph. The aim of this work was to search for evidence of the presence of organic materials in these objects as found in other planetary bodies as 5145 Pholus, and in some cometary nuclei. A careful analysis of the data has revealed flat or slightly redder spectra than the solar one for all observed asteroids. No evidence of distinct absorption features was found.

Astronomy↗