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PubMed1992

Alkyl phosphonic acids and sulfonic acids in the Murchison meteorite.

Homologous series of alkyl phosphonic acids and alkyl sulfonic acids, along with inorganic orthophosphate and sulfate, have been identified in water extracts of the Murchison meteorite after conversion to their t-butyl dimethylsilyl (tBDMS) derivatives. The methyl, ethyl, propyl, and butyl compounds have been observed in both series. Five of the eight possible alkyl phosphonic acids and seven of the eight possible alkyl sulfonic acids through C4 have been identified. Abundances decrease with increasing carbon number as observed of other homologous series indigenous to Murchison. Concentrations range downward from approximately 380 nmol/gram in alkyl sulfonic acid series, and from 9 nmol/gram in the alkyl phosphonic acid series. Inorganic phosphate is present at about 25 micromoles/gram.

Alkanesulfonic Acids↗
PubMed1992

Noble metal abundances in an Early Archean impact deposit.

We report detailed analyses on the concentrations of the noble metals Pd, Os, Ir, Pt, and Au in an early Archean spherule bed (S4) of probable impact origin from the lower Fig Tree Group, Barberton Greenstone Belt, South Africa. Compared to other sedimentary deposits of known or suspected impact origin, some noble metals are present in exceptionally high concentrations. Noble metal abundances are fractionated relative to abundances in chondrites with ratios of Os/Ir, Pt/Ir, Pd/Ir, and Au/Ir at only 80, 80, 41, and 2% of these values in CI chondrites. Although an extraterrestrial source is favored for the noble metal enrichment, the most plausible cause of the fractionation is by regional hydrothermal/metasomatic alteration.

Earth, Planet↗
PubMed1992

Iron in Precambrian rocks: implications for the global oxygen budget of the ancient Earth.

Banded iron formations (BIF) are prominent in sediments older than 2 Ga. However, little is known about the absolute abundance of BIF in Archean and Early Proterozoic sediments, and the source of the Fe is still somewhat uncertain. Also unknown is the role that Fe may have played in the maintenance of low oxygen pressures in the Archean and Early Proterozoic atmosphere. An analysis of the chemical composition of Precambrian rocks provides some insight into the role of Fe in Precambrian geochemical cycles. The Fe content of igneous rocks is well correlated with their Ti content. Plots of Fe vs. Ti in Precambrian sandstones and graywackes fall very close to the igneous rock trend. Plots of Fe vs. Ti in Precambrian shales also follow this trend but show a definite scatter toward an excess of Fe. Phanerozoic shales and sandstones lie essentially on the igneous rock trend and show surprisingly little scatter. Mn/Ti relations show a stronger indication of Precambrian Mn loss, perhaps due to weathering under a less oxidizing early atmosphere. These data show that Fe was neither substantially added to nor significantly redistributed in Archean and early Proterozoic sediments. Enough hydrothermal Fe was added to these sediments to increase the average Fe content of shales by at most a factor of 2. This enrichment would probably not have greatly affected the near-surface redox cycle or atmospheric oxygen levels. Continued redistribution of Fe and mixing with weathered igneous rocks during the recycling of Precambrian sediments account for the excellent correlation of Fe with Ti in Phanerozoic shales and for the similarity between their Fe/Ti ratio and that of igneous rocks.

Atmosphere↗
PubMed1992

The photochemistry of manganese and the origin of Banded Iron Formations.

The photochemical oxidation of Fe(2+) -hydroxide complexes dissolved in anoxic Precambrian oceans has been suggested as a mechanism to explain the deposition of Banded Iron Formations (BIFs). Photochemical studies have not yet addressed the low levels of manganese in many of these deposits, which probably precipitated from solutions bearing similar concentrations of Fe2+ and Mn2+. Depositional models must also explain the stratigraphic separation of iron and manganese ores in manganiferous BIFs. In this study, solutions containing 0.56 M NaCl and approximately 180 micromoles MnCl2 with or without 3 to 200 micromoles FeCl2 were irradiated with filtered and unfiltered UV light from a medium-pressure mercury-vapor lamp for up to 8 hours. The solutions were deaerated and buffered to pH approximately 7, and all experiments were conducted under O2-free (< 1 ppm) atmospheres. In experiments with NaCl + MnCl2, approximately 20% of the Mn2+ was oxidized and precipitated as birnessite in 8 hours. Manganese precipitation was only observed when light with lambda < 240 nm was used. In experiments with NaCl + MnCl2 + FeCl2, little manganese was lost from solution, while Fe2+ was rapidly oxidized to Fe3+ and precipitated as gamma-FeOOH or as amorphous ferric hydroxide. The Mn:Fe ratio of these precipitates was approximately 1:50, similar to the ratios observed in BIFs. A strong upper limit on the rate of manganese photo-oxidation during the Precambrian is estimated to be 0.1 mg cm-2 yr-1, a factor of 10(3) slower than the rate of iron photo-oxidation considered reasonable in BIF depositional basins. Thus, a photochemical model for the origin of oxide facies BIFs is consistent with field observations, although models that invoke molecular O2 as the oxidant of Fe2+ and Mn2+ are not precluded. Apparently, oxide facies BIFs could have formed under anoxic, as well as under mildly oxygenated atmospheres.

Earth, Planet↗
PubMed1992

Experimental dehydration of natural obsidian and estimation of DH2O at low water contents.

Water diffusion experiments were carried out by dehydrating rhyolitic obsidian from Valles Caldera (New Mexico, USA) at 510-980 degrees C. The starting glass wafers contained approximately 0.114 wt% total water, lower than any glasses previously investigated for water diffusion. Weight loss due to dehydration was measured as a function of experiment duration, which permits determination of mean bulk water diffusivity, mean Dw. These diffusivities are in the range of 2.6 to 18 X 10(-14) m2/s and can be fit with the following Arrhenius equation: ln mean Dw (m2/s) = -(25.10 +/- 1.29) - (46,480 +/- 11,400) (J/mol) / RT, except for two replicate runs at 510 degrees C which give mean Dw values much lower than that defined by the above equation. When interpreted according to a model of water speciation in which molecular H2O is the diffusing species with concentration-independent diffusivity while OH units do not contribute to the transport but react to provide H2O, the data (except for the 510 degrees C data) are in agreement with extrapolation from previous results and hence extend the previous data base and provide a test of the applicability of the model to very low water contents. Mean bulk water diffusivities are about two orders of magnitude less than molecular H2O diffusivities because the fraction of molecular H2O out of total water is very small at 0.114 wt% total water and less. The 510 degrees C experimental results can be interpreted as due to slow kinetics of OH to H2O interconversion at low temperatures.

Desiccation↗
PubMed1993

Carbon and nitrogen isotopic compositions of alkyl porphyrins from the Triassic Serpiano oil shale.

The carbon and nitrogen isotopic compositions of seven of the most abundant alkylporphyrins from the Serpiano oil shale (marine, Triassic) were determined. For the C31 and C32 butanoporphyrins, values of delta 13CPDB and delta 15NAIR averaged -24.0% and -3.1%. In contrast, the C31 and C32 methylpropanoporphyrins, DPEP, and a C30 13-nor etioporphyrin had delta 13C and delta 15N values averaging -27.5 and -3.3%, respectively. Carbon and nitrogen isotopic values for kerogen averaged -30.8 and -0.9, whereas those for total extract averaged -31.6, and -4.0%. The butanoporphyrins apparently derive from a biological source different from that giving rise to the other porphyrins, their 13C enrichment not being related to carbon isotopic fractionation accompanying diagenetic reactions. The delta 15N values for all the porphyrins indicate that the depletion of 15N observed in the kerogen is of primary origin. Consistent with the very high abundance of hopanoids and methyl hopanoids in the aliphatic hydrocarbon fraction, it is suggested that cyanobacterial fixation of N2 may have been the main cause of 15N depletion.

Biological Evolution↗
PubMed1993

The anaerobic degradation of organic matter in Danish coastal sediments: iron reduction, manganese reduction, and sulfate reduction.

We used a combination of porewater and solid phase analysis, as well as a series of sediment incubations, to quantify organic carbon oxidation by dissimilatory Fe reduction, Mn reduction, and sulfate reduction, in sediments from the Skagerrak (located off the northeast coast of Jutland, Denmark). In the deep portion of the basin, surface Mn enrichments reached 3.5 wt%, and Mn reduction was the only important anaerobic carbon oxidation process in the upper 10 cm of the sediment. In the less Mn-rich sediments from intermediate depths in the basin, Fe reduction ranged from somewhat less, to far more important than sulfate reduction. Most of the Mn reduction in these sediments may have been coupled to the oxidation of acid volatile sulfides (AVS), rather than to dissimilatory reduction. High rates of metal oxide reduction at all sites were driven by active recycling of both Fe and Mn, encouraged by bioturbation. Recycling was so rapid that the residence time of Fe and Mn oxides, with respect to reduction, ranged from 70-250 days. These results require that, on average, an atom of Fe or Mn is oxidized and reduced between 100-300 times before ultimate burial into the sediment. We observed that dissolved Mn2+ was completely removed onto fully oxidized Mn oxides until the oxidation level of the oxides was reduced to about 3.8, presumably reflecting the saturation by Mn2+ of highly reactive surface adsorption sites. Fully oxidized Mn oxides in sediments, then, may act as a cap preventing Mn2+ escape. We speculate that in shallow sediments of the Skagerrak, surface Mn oxides are present in a somewhat reduced oxidation level (< 3.8) allowing Mn2+ to escape, and perhaps providing the Mn2+ which enriches sediments of the deep basin.

Adsorption↗
PubMed1993

A photoautotrophic source for lycopane in marine water columns.

Suspended particulate matter and recent sediments from diverse oceanic sites have been investigated for their contents of lycopane. Lycopane was present in all samples, including both oxic and anoxic water column and sediments. The highest concentrations in the water column were found in surface waters of the central Pacific gyre (1.5 ng/L) and in the anoxic waters of the Cariaco Trench (1.1 ng/L) and the Black Sea (0.3 ng/L). Vertical concentration profiles suggest that lycopane is probably algal in origin. Moreover, biogeochemical conditions in anoxic zones apparently result in a secondary production of lycopane from an as yet unidentified precursor. Compound-specific carbon isotopic analyses have been carried out on lycopane from water column and sediment samples. Isotopic compositions of lycopane range between -23.6% and -32.9% and are consistent with a photoautotrophic origin. We postulate that some lycopane is produced in surface waters of the ocean, while additional lycopane is produced in anoxic zones by anaerobic microbial action on an algal precursor.

Anaerobiosis↗
PubMed1994

REE chemistry and Sm-Nd systematics of late Archean weathering profiles in the Fortescue Group, Western Australia.

Two weathering profiles, each consisting of an upper, sericite-rich zone and a lower, chlorite-rich zone, are preserved between flows of the Mt. Roe Basalt in the Fortescue Group, Hamersley Basin, Western Australia. REE concentrations in samples from these two profiles, which originally developed ca 2,760 Ma, show large variations depending on stratigraphic position. LREE abundances and (La/Yb)N are greatest at depths of 3-6 m below the paleosurface of the Mt. Roe #1 profile and are somewhat lower in samples above this level. The LREEs reach concentrations 6-9 times greater than in the underlying basalt, and thus appear to have been mobilized downward in the paleosol and concentrated in its middle part. LREE concentrations in the #2 profile show a similar distribution but with a sharp increase in all REE concentrations within 50 cm of the paleosurface. The distinction between the REE profiles in the two paleosols may be related to the difference in the overlying material. The #1 paleosol is overlain by a few meters of sediments and then by basalt, whereas the #2 paleosol is directly overlain by basalt. The LREEs appear to have been mobilized both during chemical weathering of the parental basalt and during later lower-greenschist-facies metamorphism and metasomatism of the paleosols. Remobilization of the REEs during the regional metamorphism of the Fortescue Group is confirmed by a whole-rock Sm-Nd reference isochron of Mt. Roe #1 samples with an age of 2,151 +/- 360 Ma. Variable initial 143Nd/144Nd values of unweathered basalt samples which may represent the paleosol protolith prevents a confident determination of the magnitude of LREE mobility. Both the initial mobilization of the REEs during weathering and the metasomatic remobilization appear to have taken place under redox conditions where Ce was present dominantly as Ce3+, because Ce anomalies are not developed within the sericite zone samples regardless of concentration. Europium anomalies in the paleoweathering profile are somewhat variable and were probably modified by mobilization of Eu2+ at metamorphic conditions. In all samples, the HREEs appear to have been relatively immobile and correlate with Al, Ti, Cr, V, Zr, and Nb. Sm-Nd systematics and REE patterns of four unweathered basalt samples indicate derivation of the Mt. Roe Basalts from a heterogeneous and enriched source having epsilon Nd between -4.0 and -7.4. Initial 143Nd/144Nd values of these basalts are even lower than those reported by NELSON et al. (1992) for Fortescue Group basalts and indicate a substantial crustal component in the generation of Mt. Roe Basalts.

Atmosphere↗
PubMed1996

Reflectance spectroscopy and geochemical analyses of Lake Hoare sediments, Antarctica: implications for remote sensing of the Earth and Mars.

Visible to infrared reflectance spectroscopic analyses (0.3-25 micromoles) have been performed on sediments from the Dry Valleys region of Antarctica. Sample characterization for these sediments includes extensive geochemical analyses and X-ray diffraction (XRD). The reflectance spectra and XRD indicate major amounts of quartz, feldspar, and pyroxene in these samples and lesser amounts of carbonate, mica, chlorite, amphibole, illite, smectite, and organic matter. Calcite is the primary form of carbonate present in these Lake Hoare sediments based on the elemental abundances and spectroscopic features. The particle size distribution of the major and secondary components influences their detection in mixtures and this sensitivity to particle size is manifested differently in the "volume scattering" and "surface scattering" infrared regions. The Christiansen feature lies between these two spectral regimes and is influenced by the spectral properties of both regions. For these mixtures the Christiansen feature was found to be dependent on physical parameters, such as particle size and sample texture, as well as the mineralogy. Semiquantitative spectroscopic detection of calcite and organic material has been tested in these quartz- and feldspar-rich sediments. The relative spectral band depths due to organics and calcite correlate in general with the wt% C from organic matter and carbonate. The amounts of organic matter and carbonate present correlate with high Br and U abundances and high Ca and Sr abundances, respectively. Variation in the elemental abundances was overall minimal, which is consistent with a common sedimentary origin for the forty-two samples studied here from Lake Hoare.

Antarctic Regions↗
PubMed1986

Ultranarrowband searches for extraterrestrial intelligence with dedicated signal-processing hardware.

Multichannel spectroscopy with millihertz resolution constitutes an attractive strategy for a microwave search for extraterrestrial intelligence (SETI), assuming the transmission of a narrow-band radiofrequency beacon. Such resolution matches the properties of the interstellar medium, and the necessary receiver Doppler corrections provide a high degree of interference rejection. We have constructed a frequency-agile swept receiver with an 8,388,608-channel spectrum analyzer, on-line signal recognition, and multithreshold archiving. A search of 250 Sun-like stars at 1.4 and 2.8 GHz has been carried out with the Arecibo 305-m antenna, and a meridian transit search of the northern sky is in progress at the Harvard-Smithsonian 26-m antenna. Successive spectra of 400 kHz at 0.05 Hz resolution are searched for features characteristic of an intentional narrowband beacon transmission. These spectra are centered on guessable ("magic") frequencies (such as the 21-cm hydrogen hyperfine line), referenced successively to the local standard of rest, the galactic barycenter, and the cosmic blackbody rest frame.

Astronomy↗
PubMed1988

The 2.5-12 micrometers spectrum of comet Halley from the IKS-VEGA experiment.

The infrared instrument IKS flown on board the VEGA space probes was designed for the detection of emission bands of parent molecules, and for a measurement of the size and temperature of the thermal emitting nuclear region. The instrument had three channels with cooled detectors: an "imaging channel" designed to modulate the signal of the nucleus and two spectroscopic channels operating at 2.5-5 and 6-12 micrometers, respectively, equipped with circular variable filters of resolving power approximately 50. This paper presents and discusses the results from the spectral channels. On VEGA 1, usable spectra were obtained at distances D from the comet nucleus ranging from 250,000 to 40,000 km corresponding to fields of view 4000 and 700 km in diameter, respectively. The important internal background signal caused by the instrument itself, which could not be cooled, had to be eliminated. Since no sky chopping was performed, we obtain difference spectra between the current spectrum and a reference spectrum with little or no cometary signal taken at the beginning of the observing sequence (D approximately 200,000 km). Final discrimination between cometary signal and instrumental background is achieved using their different time evolution, since the instrumental background is proportional to the slow temperature drift of the instrument, and the cometary signal due to parent molecules or dust grains is expected to vary in first order as D-1. The 2.5-5 micrometers IKS spectra definitely show strong narrow signals at 2.7 and 4.25 micrometers, attributed to the nu 3 vibrational bands of H2O and CO2, respectively, and a broader signal in the region 3.2-3.5 micrometers, which may be attributed to CH-bearing molecules. All these signals present the expected D-1 intensity variation. Weaker emission features at 3.6 and 4.7 micrometers could correspond to the nu 1 and nu 5 bands of H2CO and the (1 - 0) band of CO, respectively. Molecular production rates are derived from the observed emissions, assuming that they are due to resonance fluorescence excited by the Sun's infrared radiation. For the strong bands of H2O and CO2, the rovibrational lines are optically thick, and radiative transfer is taken into account. We derive production rates, at the moment of the VEGA 1 flyby, of approximately 10(30) sec-1 for H2O, approximately 2.7 x 10(28) sec-1 for CO2, approximately 5 x 10(28) sec-1 for CO, and 4 x 10(28) sec-1 for H2CO, if attributions to CO and H2CO are correct. The production rate of carbon atoms in CH-bearing molecules is approximately 9 x 10(29) sec-1 assuming fluorescence of molecules in the gas phase, but could be much less if the 3.2-3.5 micrometers emission is attributed to C-H stretch in polycyclic aromatic hydrocarbons or small organic grains. In addition, marginal features are present at 4.85 and 4.45 micrometers, tentatively attributed to OCS and molecules with the CN group, respectively. Broad absorption at 2.8-3.0 micrometers, as well as a narrow emission at 3.15 micrometers, which follow well the D-1 intensity variation, might be due to water ice. Emission at 2.8 micrometers is also possibly present, and might be due to OH created in vibrationally excited states after water photodissociation. The 6-12 micrometers spectrum does not show any molecular emission, nor emission in the 7.5-micrometers region. The spectrum is dominated by silicate emission showing a double structure with maxima at 9.0 and 11.2 micrometers, which suggests the presence of olivine.

Astronomy↗
PubMed1988

Evolution of a steam atmosphere during Earth's accretion.

We have modeled the evolution of an impact-generated steam atmosphere surrounding an accreting Earth. The model assumes Safronov accretion; it includes degassing of planetesimals upon impact, thermal blanketing by a steam atmosphere, interchange of water between the surface and the interior, shock heating and convective cooling of Earth's interior, and hydrogen escape, both by a solar extreme ultraviolet (EUV) powered planetary wind and by impact erosion (atmospheric cratering). The model does not include atmophiles other than water, chemical reaction of water with metallic iron, core formation, compression, and spatial and temporal inhomogeneity of accretion. If the incoming planetesimals were too dry or the EUV flux too high, very little water would accumulate at the surface. Essentially all water retained by such a planet would be through rehydration of silicates. If rehydration were inefficient, very little water would be retained in any form. Degassing of wetter planetesimals produces a steam atmosphere over a magma ocean, the energy of accretion being sufficient to maintain a runaway greenhouse atmosphere. The mass of the atmosphere is limited by water's solubility in the (partial) melt. This type of solution is produced for a wide range of model parameters. During accretion, approximately 30 bars of water could have kept the surface at 1500 degrees K. As the accretional energy input declined below the runaway greenhouse threshold, the steam atmosphere rained out. Outgassing of dissolved water at the close of accretion is quantitatively important. These models can leave from approximately 100 to more than 300 bars of water at the surface at the close of accretion. In general, most of the water accreted remains dissolved in the mantle. H2 could have escaped as rapidly as it formed only if the planetesimals were relatively dry. Consequently H2 should have accumulated until it reached chemical equilibrium with water vapor. Impact erosion (escape caused by impact) is a critical but poorly understood process. It can prevent the accumulation of a steam atmosphere if the planetesimals are sufficiently dry, or for wetter impactors if it is much more effective than we have assumed. Impact erosion of a steam atmosphere is less important; it is equivalent to a slightly drier rain of impactors. If a hypothetical Moon-forming impact took place before the collapse of the runaway greenhouse, relatively little water (approximately 30-100 bars) would have been in the atmosphere; hence little could have been lost. If the event took place later, the potential damage could have been greater.

Atmosphere↗
PubMed1988

Estimation of the reaction rate for the formation of CH3O from H + H2CO: implications for chemistry in the Solar System.

It is argued that the formation of the methoxy radical (CH3O) from H + H2CO may play an essential role in the reduction of CO to CH4. The rate coefficient for this reaction has been estimated using the approximate theory of J. Troe (1977a, J. Chem. Phys. 66, 4745) and transition state theory. We briefly discuss the implications of this reaction for the chemistry of CO on Jupiter, in the solar nebula, for interpreting the laboratory experiments of A. Bar-Nun and A. Shaviv (1975, Icarus 24, 197) and A. Bar-Nun and S. Chang (1983, J. Geophys. Res. 88, 6662) and for organic synthesis in the prebiotic terrestrial atmosphere.

Atmosphere↗
PubMed1988

Runaway and moist greenhouse atmospheres and the evolution of Earth and Venus.

A one-dimensional climate model is used to study the response of an Earth-like atmosphere to large increases in solar flux. For fully saturated, cloud-free conditions, the critical solar flux at which a runaway greenhouse occurs, that is, the oceans evaporate entirely, is found to be 1.4 times the present flux at Earth's orbit (S0). This value is close to the flux expected at Venus' orbit early in solar system history. Is is nearly independent of the amount of CO2 present in the atmosphere, but is sensitive to the H2O absorption coefficient in the 8- to 12-micrometers window region. Clouds should tend to depress the surface temperature on a warm, moist planet; thus, Venus may originally have had oceans if its initial water endowment was close to that of Earth. It lost them early in its history, however, because of rapid photodissociation of water vapor followed by escape of hydrogen to space. The critical solar flux above which water is rapidly lost could be as low as 1.1S0. The surface temperature of a runaway greenhouse atmosphere containing a full ocean's worth of water would have been in excess of 1500 degrees K--above the solidus for silicate rocks. The presence of such a steam atmosphere during accretion may have significantly influenced the early thermal evolution of both Earth and Venus.

Atmosphere↗
PubMed1988

HDO in the Martian atmosphere: implications for the abundance of crustal water.

The physical and chemical processes that lead to the preferential escape of hydrogen over deuterium in the Martian atmosphere are studied in detail using a one-dimensional photochemical model. Comparison of our theory with recent observations of HDO suggests that, averaged over the planet, Mars contains 0.2 m of crustal water that is exchangeable with the atmosphere. Our estimate is considerably lower than recent estimates of subsurface water on Mars based on geomorphological analysis of Viking images. The estimate can be reconciled if only a small fraction of crustal water can exchange with the atmosphere.

Atmosphere↗
PubMed1990

Mass fractionation of noble gases in diffusion-limited hydrodynamic hydrogen escape.

Mass fractionation by hydrodynamic hydrogen escape is a promising mechanism for explaining the observed elemental and isotopic abundance patterns in terrestrial planet atmospheres. Previous work has considered only pure hydrogen winds. Here, the theory of mass fractionation by hydrogen escape is extended to atmospheres in which hydrogen is not the only major constituent. Analytical solutions are derived for cases in which all relevant atmospheric constituents escape; both analytical and numerical solutions are obtained for cases in which important heavy constituents are retained. In either case the fractionation patterns that result can differ significantly from those produced by pure hydrogen winds. Three applications of the theory are discussed: (1) The observed fractionation of terrestrial atmospheric neon with respect to mantle neon can be explained as a by-product of diffusion-limited hydrogen escape from a steam atmosphere toward the end of accretion. (2) The anomalously high Martian (SNC) 38Ar/36Ar ratio is attributed to hydrodynamic fractionation by a vigorously escaping, nearly pure hydrogen wind. (3) It is possible that the present high Martian D/H ratio was established during the same hydrodynamic escape phase that fractionated argon, but the predicted degree of D/H enrichment is sensitive to other, less well constrained parameters.

Argon↗