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PubMed1990

[Chemistry of alpha-aminonitriles. Aziridine-2-carbonitrile: photochemical formation from 2-aminopropenenitrile].

2-Aminopropenenitrile in solvents such as MeCN, MeOH, or H2O is photoisomerized by UV light to racemic aziridine-2-carbonitrile (rac-2); the larger part of the starting material, however, fragments to HCN and MeCN. The observed photocyclization constitutes a structural connection within an ensemble of C3H4N2 compounds considered to be potentially relevant to prebiotic chemistry.

Acetonitriles↗
PubMed1992

Cumulative atomic multipole moments complement any atomic charge model to obtain more accurate electrostatic properties.

The quality of several atomic charge models based on different definitions has been analyzed using cumulative atomic multipole moments (CAMM). This formalism can generate higher atomic moments starting from any atomic charges, while preserving the corresponding molecular moments. The atomic charge contribution to the higher molecular moments, as well as to the electrostatic potentials, has been examined for CO and HCN molecules at several different levels of theory. The results clearly show that the electrostatic potential obtained from CAMM expansion is convergent up to R-5 term for all atomic charge models used. This illustrates that higher atomic moments can be used to supplement any atomic charge model to obtain more accurate description of electrostatic properties.

Biopolymers↗
PubMed1991

Diversity of micro-fungi in an Antarctic dry valley.

The fungal microflora of a dry valley in Southern Victoria Land near McMurdo Sound, Antarctica, was investigated. Samples were collected from introduced objects such as a mummified penguin and spent chewing tobacco in addition to the sparse soil found in rock fissures, isolated moss colonies, shoreline deposit materials, CaCO3 precipitates, and microbial mat debris obtained from the frozen surface of the lake in the basin of Taylor Valley. Using conventional media and techniques, all collection sites yielded populations of yeasts and filamentous fungi. Water samples and live microbial mats from beneath the lake ice yielded species of fungi along with an abundance of bacteria.

Antarctic Regions↗
PubMed1991

Ab initio study of the electrostatic multipole nature of torsional potentials in CH3SSCH3, CH3SSH, and HOOH.

The origin of torsional potentials in H3CSSCH3, H3CSSH, and HOOH and the anisotropy of the local charge distribution has been analyzed in terms of atomic multipoles calculated from the ab initio LCAO-MO-SCF wave function in the 6-31G* basis set. The results indicate that for longer -S-S-bonds the major contribution to these torsional barriers are electrostatic interactions of the atomic multipoles located on two atoms forming the rotated bond. This finding demonstrates the important role of electrostatic 1-2 interatomic interactions, usually neglected in conformational studies. It also opens the possibility to derive directly from accurate ab initio wave functions a simple nonempirical torsional potential involving atomic multipoles of two bonded atoms defining the torsional angle. For shorter -O-O- bonds, use of more precise models and inclusion of 1-3 interactions seems to be necessary.

Chemistry, Organic↗
PubMed1995

Isolation, characterization, and primary structure of rubredoxin from the photosynthetic bacterium, Heliobacillus mobilis.

Rubredoxin is a small nonheme iron protein that serves as an electron carrier in bacterial systems. Rubredoxin has now been isolated and characterized from the strictly anaerobic phototroph, Heliobacillus mobilis. THe molecular mass (5671.3 Da from the amino acid sequence) was confirmed and partial formylation of the N-terminal methionyl residue was established by matrix-assisted laser desorption mass spectroscopy. The complete 52-amino-acid sequence was determined by a combination of N-terminal sequencing by Edman degradation and C-terminal sequencing by a novel method using carboxypeptidase treatment in conjunction with amino acid analysis and laser desorption time of flight mass spectrometry. The molar absorption coefficient of Hc. mobilis rubredoxin at 490 nm is 6.9 mM-1 cm-1 and the midpoint redox potential at pH 8.0 is -46 mV. The EPR spectrum of the oxidized form shows resonances at g = 9.66 and 4.30 due to a high-spin ferric iron. The amino acid sequence is homologous to those of rubredoxins from other species, in particular, the gram-positive bacteria, and the phototrophic green sulfur bacteria, and the evolutionary implications of this are discussed.

Amino Acid Sequence↗
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

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↗
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

A photochemical model of the martian atmosphere.

The factors governing the amounts of CO, O2, and O3 in the martian atmosphere are investigated using a minimally constrained, one-dimensional photochemical model. We find that the incorporation of temperature-dependent CO2 absorption cross sections leads to an enhancement in the water photolysis rate, increasing the abundance of OH radicals to the point where the model CO abundance is smaller than observed. Good agreement between models and observations of CO, O2, O3, and the escape flux of atomic hydrogen can be achieved, using only gas-phase chemistry, by varying the recommended rate constants for the reactions CO + OH and OH + HO2 within their specified uncertainties. Similar revisions have been suggested to resolve discrepancies between models and observations of the terrestrial mesosphere. The oxygen escape flux plays a key role in the oxygen budget on Mars; as inferred from the observed atomic hydrogen escape, it is much larger than recent calculations of the exospheric escape rate for oxygen. Weathering of the surface may account for the imbalance. Quantification of the escape rates of oxygen and hydrogen from Mars is a worthwhile objective for an upcoming martian upper atmospheric mission. We also consider the possibility that HOx radicals may be catalytically destroyed on dust grains suspended in the atmosphere. Good agreement with the observed CO mixing ratio can be achieved via this mechanism, but the resulting ozone column is much higher than the observed quantity. We feel that there is no need at this time to invoke heterogeneous processes to reconcile models and observations.

Atmosphere↗
PubMed1994

Temperature of nitrogen ice on Pluto and its implications for flux measurements.

Previous work by K.A. Tryka et al. (Science 261, 751-754, 1993) has shown that the profile of the 2.148-micrometers band of solid nitrogen can be used as a "thermometer" and determined the temperature of nitrogen ice on Triton to be 38(+2)-1 K. Here we reevaluate that data and refine the temperature value to 38 +/- 1 K. Applying the same technique to Pluto we determine that the temperature of the N2 ice on that body is 40 +/- 2 K. Using this result we have created a nonisothermal flux model of the Pluto-Charon system. The model treats Pluto as a body with symmetric N2 polar caps and an equatorial region devoid of N2. Comparison with the infrared and millimeter flux measurements shows that the published fluxes are consistent with models incorporating extensive N2 polar caps (down to +/- 15 degrees or +/- 20 degrees latitude) and an equatorial region with a bolometric albedo < or = 0.2.

Astronomical Phenomena↗
PubMed1995

Photodissociation of cyanoacetylene: application to the atmospheric chemistry of Titan.

The quantum yield and reaction threshold for the photochemical dissociation of cyanoacetylene into a hydrogen atom and the cyanoethynyl radical have been determined. The quantum yield at 185 nm is approximately 0.09. The threshold is approximately 240 nm. Combination of this data with literature values shows that production of excited-state cyanoacetylene is the major primary process resulting from irradiation between 185 and 254 nm. Also determined are the relative rate constants for the abstraction of a hydrogen atom from hydrogen, methane, and ethane by the cyanoethynyl radical (k(H2):k(CH4):k(C2H6) = 1:9.3:63). Implications of these results for the proposal that hydrogen abstraction plays an important role in the conversion of methane to ethane and in the protection of unsaturated compounds from photoconsumption in the atmosphere of Titan are discussed.

Acetylene↗
PubMed1996

Hydrocarbon photochemistry in the upper atmosphere of Jupiter.

The hydrocarbon photochemistry in the upper atmosphere of Jupiter is investigated using a one-dimensional, photochemical-diffusive, and diurnally averaged model. The important chemical cycles and pathways among the major species are outlined and a standard model for the North Equatorial Belt region is examined in detail. It is found that several traditionally dominant chemical pathways among the C and C2 species are replaced in importance by cycles involving C-C4 species. The pressure and altitude profiles of mixing ratios for several observable hydrocarbon species are compared with available ultraviolet- and infrared-derived abundances. The results of sensitivity studies on the standard model with respect to variations in eddy diffusion profile, solar flux, atomic hydrogen influx, latitude, temperature, and important chemical reaction rates are presented. Measured and calculated airglow emissions of He at 584 angstroms and H at 1216 angstroms are also used to provide some constraints on the range of model parameters. The relevance of the model results to the upcoming Galileo mission is briefly discussed. The model is subject to considerable improvement; there is a great need for laboratory measurements of basic reaction rates and photodissociation quantum yields, even for such simple species as methylacetylene and allene. Until such laboratory measurements exist there will be considerable uncertainty in the understanding of the C3 and higher hydrocarbons in the atmospheres of the jovian planets.

Astronomy↗
PubMed1988

Band structure of the solar system: an objective test of the grouping of planets and satellites.

Alfvén in his early work on the origin of the solar system (1942-1946) noted a pronounced band structure in the gravitational potential distribution of secondary bodies, and suggested this feature to be directly related to the formation process. When the critical velocity phenomenon was later discovered, a close agreement was found between the planet-satellite bands on one hand, and the critical velocity limits of the major compound elements in the interstellar medium on the other, suggesting a specific emplacement mechanism for the dusty plasma which presumably constituted the solar nebula. Since the originally perceived band structure was outlined in a qualitative fashion, an attempt is made here to analyze the distribution by a statistical technique, testing the significance of clustering of the observational data in the bands. The results show that, with proper scaling of the parameters, such a band structure indeed appears, with features closely similar to those originally conceived. Some deviations are indicated by the cluster analysis, however; their significance is discussed in terms of process involved in the formation of the solar system.

Astronomical Phenomena↗
PubMed1989

Lipophilic pigments from the benthos of a perennially ice-covered Antarctic lake.

The benthos of a perennially ice-covered Antarctic lake, Lake Hoare, contained three distinct 'signatures' of lipophilic pigments. Cyanobacterial mats found in the moat at the periphery of the lake were dominated by the carotenoid myxoxanthophyll; carotenoids: chlorophyll a ratios in this high light environment ranged from 3 to 6.8. Chlorophyll c and fucoxanthin, pigments typical of golden-brown algae, were found at 10 to 20 m depths where the benthos is aerobic. Anaerobic benthic sediments at 20 to 30 m depths were characterized by a third pigment signature dominated by a carotenoid, tentatively identified as alloxanthin from planktonic cryptomonads, and by phaeophytin b from senescent green algae. Pigments were not found associated with alternating organic and sediment layers. As microzooplankton grazers are absent from this closed system and transformation rates are reduced at low temperatures, the benthos beneath the lake ice appears to contain a record of past phytoplankton blooms undergoing decay.

Antarctic Regions↗
PubMed1989

Perennially ice-covered Lake Hoare, Antarctica: physical environment, biology and sedimentation.

Lake Hoare (77 degrees 38' S, 162 degrees 53' E) is a perennially ice-covered lake at the eastern end of Taylor Valley in southern Victoria Land, Antarctica. The environment of this lake is controlled by the relatively thick ice cover (3-5 m) which eliminates wind generated currents, restricts gas exchange and sediment deposition, and reduces light penetration. The ice cover is in turn largely controlled by the extreme seasonality of Antarctica and local climate. Lake Hoare and other dry valley lakes may be sensitive indicators of short term (< 100 yr) climatic and/or anthropogenic changes in the dry valleys since the onset of intensive exploration over 30 years ago. The time constants for turnover of the water column and lake ice are 50 and 10 years, respectively. The turnover time for atmospheric gases in the lake is 30-60 years. Therefore, the lake environment responds to changes on a 10-100 year timescale. Because the ice cover has a controlling influence on the lake (e.g. light penetration, gas content of water, and sediment deposition), it is probable that small changes in ice ablation, sediment loading on the ice cover, or glacial meltwater (or groundwater) inflow will affect ice cover dynamics and will have a major impact on the lake environment and biota.

Antarctic Regions↗
PubMed1992

Prebiotic sugar synthesis: hexose and hydroxy acid synthesis from glyceraldehyde catalyzed by iron(III) hydroxide oxide.

Iron(III) hydroxide oxide [Fe(OH)O] efficiently catalyzed the condensation of 25 mM DL-glyceraldehyde to ketohexoses at 25 degrees C (pH 5-6). At 16 days the yields were sorbose (15.2%), fructose (12.9%), psicose (6.1%), tagatose (5.6%), and dendroketose (2.5%) with 19.6% of triose unreacted. Analysis at 96 days showed no decomposition of hexoses. Under these conditions Fe(OH)O also catalyzed the isomerization and rearrangement of glyceraldehyde to dihydroxyacetone and lactic acid, respectively. In these reactions, about 10% of the glyceraldehyde was oxidized to glyceric acid with concurrent reduction of the iron(III) to iron(II). The partial reduction of Fe(OH)O did not noticeably reduce its ability to catalyze hexose synthesis. The relationship of these results to prebiotic sugar synthesis is discussed.

Carbohydrates↗
PubMed1991

Isotopic analysis of cometary organic matter.

Carbon isotope ratios have been measured for CN in the coma of comet Halley and for several CHON particles emitted by Halley. Of these, only the CHON-particle data may be reasonably related to organic matter in the cometary nucleus, but the true range of 13C/12C values in those particles is quite uncertain. The D/H ratio in H2O in the Halley coma resembles that in Titan/Uranus. The next decade should substantially improve our understanding of the distribution of C, H, N, and O isotopes in cometary organics. The isotopic composition of meteoritic organic matter is better understood and can serve as a useful analog for the cometary case.

Carbon↗