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PubMed1992

Relationship of peroxyacetyl nitrate to active and total odd nitrogen at northern high latitudes: influence of reservoir species on NOx and O3.

Measurements of peroxyacetyl nitrate (PAN), NO, NO2, HNO3, NOy (total odd nitrogen), and O3 were made in the high-latitude troposphere over North America and Greenland (35 degrees to 82 degrees N) during the Arctic Boundary Layer Expedition (ABLE 3A) (July-August 1988) throughout 0-to 6-km altitudes. These data are analyzed to quantitatively describe the relationships between various odd nitrogen species and assess their significance to global tropospheric chemistry. In the free troposphere, PAN was as much as 25 times more abundant than NOx. PAN to NOx ratio increased with increasing altitude and latitude. PAN was found to be the single most abundant reactive nitrogen species in the free troposphere and constituted a major fraction of NOy, PAN to NOy ratios were about 0.1 in the boundary layer and increased to 0.4 in the free troposphere. A 2-D global photochemical model with C1-C3 hydrocarbon chemistry is used to compare model predictions with measured results. A sizable portion (approximately 50%) of the gaseous reactive nitrogen budget is unaccounted for, and unknown organic nitrates and pernitrates are expected to be present. Model calculations (August 1, 70 degrees N) show that a major fraction of the observed NOx (50 to 70% of median) may find its source in the available PAN reservoir. PAN and the unknown reservoir species may have the potential to control virtually the entire NOx availability of the high latitude troposphere. It is predicted that the summer NOx and O3 mixing ratios in the Arctic/sub-Arctic troposphere would be considerably lower in the absence of the ubiquitous PAN reservoir. Conversely, this PAN reservoir may be responsible for the observed temporal increase in tropospheric O3 at high latitudes.

Arctic Regions↗
PubMed1991

Infrared measurements of HF and HCl total column abundances above Kitt Peak, 1977-1990: seasonal cycles, long-term increases, and comparisons with model calculations.

Series of high-resolution (approximately 0.01 cm-1) solar absorption spectra recorded with the McMath Fourier transform spectrometer on Kitt Peak (altitude 2.09 km, 31.9 degrees N, 111.6 degrees W) have been analyzed to deduce total column amounts of HF on 93 different days and HCl on 35 different days between May 1977 and June 1990. The results are based on the analysis of the HF and H35Cl (1-0) vibration-rotation band R(1) lines which are located at 4038.9625 and 2925.8970 cm-1, respectively. All of the data were analyzed using a multilayer, nonlinear least squares spectral fitting procedure and a consistent set of spectroscopic line parameters. The results indicate a rapid increase in total HF and a more gradual increase in total HCl with both trends superimposed on short-term variability. In addition, the total columns of both gases undergo a seasonal cycle with an early spring maximum and an early fall minimum, with peak-to-peak amplitudes equal to 25% for HF and 13% for HCl. In the case of HF, the changes over the 13 years of measurement are sufficiently large to determine that a better fit is obtained assuming a linear rather than an exponential increase with time. For HCl, linear and exponential models fit the data equally well. Referenced to calendar year 1981.0 and assuming a sinusoidal seasonal cycle superimposed on a linear total column increase with time, HF and HCl increase rates of (10.9 +/- 1.1)% yr-1 and (5.1 +/- 0.7)% yr-1 and total columns of (3.17 +/- 0.11) x 10(14) and (1.92 +/- 0.06) x 10(15) molecules cm-2 (2 sigma) are derived, respectively; the corresponding best fit mean exponential increase rates are equal to (7.6 +/- 0.6)% yr-1 and (4.2 +/- 0.5)% yr-1 (2 sigma). Over the 13-year observing period, the HF and HCl total columns increased by factors of 3.2 and 1.8, respectively. Based on HF and HCl total columns deduced from measurements on the same day, the HF/HCl total columns ratio increased from 0.14 in May 1977 to 0.23 in June 1990. Short-term temporal variations in the HF and HCl total columns are highly correlated; these fluctuations are believed to be caused by dynamical variability in the lower stratosphere. The results of this investigation are compared with previously reported measurements and with time-dependent, two-dimensional model calculations of HF and HCl total columns based on emission histories and photo-oxidation rates for the source molecules.

Astronomical Phenomena↗
PubMed1991

Does sedimentary organic delta 13C record variations in quaternary ocean [CO2(aq)]?

Ocean surface water [CO2(aq)] variations based on glacial/interglacial changes in sediment delta 13Corg are shown to compare favorably with reconstructions based on ice core [CO2]. In particular, an approximate 80 microatmospheres increase in atmospheric pCO2 during the last glacial-interglacial transition is calculated to correspond to a 3-4 micromolar increase in ocean surface water [CO2(aq)] at atmospheric equilibrium. A widespread marine delta 13Corg decrease of 1-2% accompanied this event and was not preceded by an equivalent isotopic change in surface water total dissolved inorganic carbon. These observations support the hypothesis that [CO2(aq)] influences photosynthetic isotope fractionation between marine inorganic and organic carbon pools, and therefore that plankton/sediment delta 13Corg may serve as a proxy for surface water [CO2(aq)].

Animals↗
PubMed1992

Volatiles in interplanetary dust particles: a review.

The paper presents a review of the volatiles found within interplanetary dust particles. These particles have been shown to represent primitive material from early in the solar system's formation and also may contain records of stellar processes. The organogenic elements (i.e., H, C, N, O, and S) are among the most abundant elements in our solar system, and their abundances, distributions, and isotopic compositions in early solar system materials permit workers to better understand the processes operating early in the evolutionary history of solar system materials. Interplanetary dust particles have a range of elemental compositions, but generally they have been shown to be similar to carbonaceous chondrites, the solar photosphere, Comet Halley's chondritic cores, and matrix materials of chondritic chondrites. Recovery and analysis of interplanetary dust particles have opened new opportunities for analysis of primitive materials, although interplanetary dust particles represent major challenges to the analyst because of their small size.

Aluminum↗
PubMed1992

Airburst origin of dark shadows on Venus.

A simple analytic model for the catastrophic disruption and deceleration of impactors in a thick atmosphere is used to (1) reproduce observed Venusian cratering statistics and (2) generate radar-dark disks by the impact of atmospheric shock waves with the surface. When used as input to Monte Carlo simulations of Venusian cratering, the model nicely reproduces the observed low diameter cutoff. Venusian craters are found to be more consistent with an asteroidal rather than a cometary source. The radar-dark "shadows" of the title are surface features, usually circular, that have been attributed to airbursting impactors. A typical craterless airburst is the equivalent of a approximately 10(6) megaton explosion. The airburst is treated as a massive, extended explosion using a thin-shell, isobaric cavity approximation. The strong atmospheric shock waves excited by the airbust are then coupled to surface rock using the usual impedance matching conditions. Peak shock pressures experienced by surface rock typically exceed 0.2 GPa for distances 15-30 km from ground zero (the place on the surface immediately beneath the site of the airburst), and 1 GPa for 10-20 km. These high shock pressures are felt to considerable depth, often more than a kilometer. Beneath the airburst the shock could reduce surface rocks to fine rubble, while at greater distance the weaker shock would leave fields of broken blocks, perhaps in part accounting for radar-bright halos that often surround the dark shadows.

Astronomy↗
PubMed1996

Ground-based detectability of terrestrial and Jovian extrasolar planets: observations of CM Draconis at Lick Observatory.

The detection of terrestrial-sized extrasolar planets from the ground has been thought to be virtually impossible due to atmospheric scintillation limits. However, we show that this is not the case especially selected (but nevertheless main sequence) stars, namely small eclipsing binaries. For the smallest of these systems, CM Draconis, several months to a few years of photometric observations with 1-m-class telescopes will be sufficient to detect the transits of any short-period planets of sizes > or = 1.5 Earth radii (RE), using cross-correlation analysis with moderately good photometry. Somewhat larger telescopes will be needed to extend this detectability to terrestrial planets in larger eclipsing binary systems. (We arbitrarily define "terrestrial planets" herein as those whose disc areas are closer to that of Earth's than Neptune's i.e., less than about 2.78 RE.) As a "spin-off" of such observations, we will also be able to detect the presence of Jovian-mass planets without transits using the timing of the eclipse minima. Eclipse minima will drift in time as the binary system is offset by a sufficiently massive planet (i.e., one Jupiter mass) about the binary/giant-planet barycenter, causing a periodic variation in the light travel time to the observer. We present here an outline of present observations taking place at the University of California Lick Observatory using the Crossley 0.9-m telescope in collaboration with other observatories (in South Korea, Crete, France, Canary Islands, and New York) to detect or constrain the existence of terrestrial planets around main sequence eclipsing binary star systems, starting with CM Draconis. We demonstrate the applicability of photometric data to the general detection of gas giant planets via eclipse minima timings in many other small-mass eclipsing binary systems as well.

Astronomy↗
PubMed1987

Concepts for collection of aerosols in Titan's atmosphere.

In this paper we consider design of instruments for collection of aerosols during entry in Titan's atmosphere. Major constraints on designs are small sample collection time, low aerosol column density, and the need to collect 1-10 micrograms of aerosol for gas chromatographic analysis. Thus it is important to maximize aerosol collection through collector design, which includes consideration of various types of collectors and maximizing the collection efficiency of a given type of collector. Sampling systems discussed include inertial impactors, filters, electrostatic devices, and multistage instruments. Aerosol sampling is reviewed in the context of high-altitude (200-70 km) and low-altitude (60-30 km) regions of Titan's atmosphere.

Aerosols↗
PubMed1985

Thickness of ice on perennially frozen lakes.

The dry valleys of southern Victoria Land, constituting the largest ice-free expanse in the Antarctic, contain numerous lakes whose perennial ice cover is the cause of some unique physical and biological properties. Although the depth, temperature and salinity of the liquid water varies considerably from lake to lake, the thickness of the ice cover is remarkably consistent, ranging from 3.5 to 6 m, which is determined primarily by the balance between conduction of energy out of the ice and the release of latent heat at the ice-water interface and is also affected by the transmission and absorption of sunlight. In the steady state, the release of latent heat at the ice bottom is controlled by ablation from the ice surface. Here we present a simple energy-balance model, using the measured ablation rate of 30 cm yr-1, which can explain the observed ice thickness.

Antarctic Regions↗
PubMed1989

Latitudinal variations in plankton delta 13C: implications for CO2 and productivity in past oceans.

The stable-carbon isotopic composition of marine organic material has varied significantly over geological time, and reflects significant excursions in the isotopic fractionation associated with the uptake of carbon by marine biota. For example, low 13C/12C in Cretaceous sediments has been attributed to elevated atmospheric (and hence oceanic) CO2 partial pressures. A similar depletion in 13C present-day Antarctic plankton has also been ascribed to high CO2 availability. We report, however, that this high-latitude isotope depletion develops at CO2 partial pressures (pCO2 levels) that are often below that of the present atmosphere (340 microatmospheres) , and usually below that of equatorial upwelling systems (> 340 microatmospheres). Nevertheless, because of the much lower water temperatures and, hence, greater CO2 solubility at high latitude, the preceding pCO2 measurements translate into Antarctic surface-water CO2 (aq) concentrations that are as much as 2.5 times higher than in equatorial waters. We calculate that an oceanic pCO2 level of > 800 microatmospheres (over twice the present atmospheric pCO2) in a warmer low-latitude Cretaceous ocean would have been required to produce the plankton 13C depletion preserved in Cretaceous sediments.

Animals↗
PubMed1989

Annihilation of ecosystems by large asteroid impacts on the early Earth.

Large asteroid impacts produced globally lethal conditions by evaporating large volumes of ocean water on the early Earth. The Earth may have been continuously habitable by ecosystems that did not depend on photosynthesis as early as 4.44 Gyr BP (before present). Only a brief interval after 3.8 Gyr exists between the time when obligate photosynthetic organisms could continuously evolve and the time when the palaeontological record indicates highly evolved photosynthetic ecosystems.

Biological Evolution↗
PubMed1990

Model of carbon fixation in microbial mats from 3,500 Myr ago to the present.

Biological carbon fixation is an important part of global carbon cycling and ecology. Fixation that took place 3,500 million years ago is recorded in the laminated sedimentary rock structures known as stromatolites, which are fossilized remains of microbial mat communities. Stromatolites are the most abundant type of fossil found in the Proterozoic (2,500 to 590 Myr ago), but they then declined, possibly because of predation and competition. Using modern microbial mats as analogues for ancient stromatolites, we show that the rate of carbon fixation is higher at the greater levels of atmospheric CO2 that were probably present in the past. We suggest that carbon fixation in microbial mats was not carbon-limited during the early Precambrian, but became carbon-limited as the supply of inorganic carbon decreased. Carbon limitation led to a lower rate of carbon fixation, especially towards the end of the Precambrian. Thus, another reason for the decline of the stromatolites could have been a decrease in available CO2.

Atmosphere↗
PubMed1990

Comet dust as a source of amino acids at the Cretaceous/Tertiary boundary.

Large amounts of apparently extraterrestrial amino acids have been detected recently in rocks at the Cretaceous/Tertiary (K/T) boundary at Stevns Klint, Denmark. The amino acids were found a few tens of centimetres above and below the boundary layer, but were absent in the boundary clay itself. If one supposes that these compounds were carried to the Earth by the giant meteorite thought to have impacted at the end of the Cretaceous, some puzzling questions are raised: why weren't the amino acids incinerated in the impact, and why are they not present in the boundary clay itself? Here we suggest that the amino acids were actually deposited with the dust from a giant comet trapped in the inner Solar System, a fragment of which comprised the K/T impactor. Amino acids or their precursors in the comet dust would have been swept up by the Earth both before and after the impact, but any conveyed by the impactor itself would have been destroyed. The observed amino acid layers would thus have been deposited without an impact.

Aldehydes↗
PubMed1991

Positive holes in magnesium oxide. Correlation between magnetic, electric, and dielectric anomalies.

Magnetic susceptibility measurements of high purity MgO single crystals (<50-wt. ppm transition metals) by means of a vibrating-sample magnetometer shows an anomaly at 800 K. At the same temperature the electric conductivity increases anomalously, the static dielectric constant epsilon increases from 9 to approximately 150, a pronounced positive surface charge appears, and Fe2+ in the MgO matrix oxidizes to Fe3+. The data are consistent with O2(2-) (peroxy) defects, representing self-trapped, spin-paired positive holes at Mg2+ vacancy sites. Diamagnetic at low temperatures, the holes start to decouple their spins > 600 K, probably forming at first V0 centers (two O- at an Mg2+ vacancy), then V- centers (single O- at an Mg2+ vacancy), and releasing mobile O- states. These O- represent itinerant charge carriers on acceptor levels near the O 2p-dominated valence band and conduct by O- /O2- valency fluctuations. The O- concentration is of the order of 8 X 10(19) cm-3.

Crystallization↗
PubMed1991

Effect of void-size distribution on the Hugoniot state at low shock pressures.

In most theoretical and experimental investigations into the shock response of underdense solid media, the influence of the medium's mesostructure on the resulting pressure and degree of compaction has not been taken into account. In typical cases examined, shock pressures are well in excess of 1 GPa and this approach is clearly justified. However, at low pressures, calculations show that the distribution of void sizes can affect the final state achieved upon shocking the medium from a given initial porosity. This paper analyzes the response of porous aluminum to low pressure shocking and demonstrates a dependence of the final shocked state on the distribution of void sizes.

Aluminum↗
PubMed1990

Association reactions at low pressure. III. The C2H2+/C2H2 system.

The association reactions, C4H2(+) + C2H2 and C4H3(+) + C2H2 have been examined at pressures between 8 x 10(-8) and 1 x 10(-4) Torr at 298 K in an ion cyclotron resonance mass spectrometer. Association occurred via two different mechanisms. At pressures below approximately 2 x 10(-6) Torr, the association was bimolecular having rate coefficients k2 = 2.7 x 10(-10) cm3 s-1 and 2.0 x 10(-10) cm3 s-1 for C4H2+ and C4H3+, respectively. At pressures above approximately 2 x 10(-6) Torr, termolecular association was observed with rate coefficients, k3 = 5.7 x 10(-23) cm6 s-1 and 1.3 x 10(-23) cm6 s-1 for C4H2+ and C4H3+, respectively, when M = C2H2. The termolecular rate constants with N2, Ar, Ne, and He as the third body, M, are also reported. We propose that the low pressure bimolecular association process was the result of radiative stabilization of the complex and the termolecular association process was the result of collisional stabilization. Elementary rate coefficients were obtained and the lifetime of the collision complex was > or = 57 microseconds for (C6H4+)* and > or = 18 microseconds for (C6H5+)*. At pressures below 1 x 10(-6) Torr, approximately 11% of the (C6H4+)* were stabilized by photon emission and the remaining approximately 89% reverted back to reactants, while approximately 24% of the (C6H5+)* were stabilized by photon emission and the remaining approximately 76% reverted back to reactants. The ionic products of the C2H2(+) + C2H2 reaction, C4H2+ and C4H3+, were found to be formed with enough internal energy that they did not react by the radiative association channel until relaxed by several nonreactive collisions with the bath gas.

Acetylene↗
PubMed1991

Molecular dynamics of phenol at the liquid-vapor interface of water.

Molecular dynamics results are presented for phenol at the water liquid-vapor interface at 300 K. The calculated excess free energy of phenol at the interface is -2.8 +/- 0.4 kcal/mol, in good agreement with the recent experimental results of Eisenthal and co-workers. The most probable orientation of the phenol molecule at the surface is such that the aromatic ring is perpendicular to the interface and the OH group is fully immersed in water. The hydroxyl substituent has a preferred orientation which is similar to the orientation of OH bonds of water at the pure water liquid-vapor interface. The transition between interfacial and bulk-like behavior of phenol is abrupt and occurs when the center of mass of the solute is located about 6 angstroms from the Gibbs surface of water. In this region the para carbon atom of the hydrophobic benzene ring can reach the interface and become partially dehydrated. This result suggests that the width of the interfacial region in which the behavior of a simple amphiphilic solute in water is influenced by the presence of the surface depends primarily on the size of its hydrophobic part. The role of the OH substituent was investigated by comparing phenol at the interface with two model systems: benzene with and without partial charges on carbon and hydrogen atoms. It is shown that in the absence of the hydrophilic substituent the solute is located further away from the liquid phase and is more likely to be oriented parallel to the interface. However, when the center of mass of the solute is moved into the interfacial region where the density of water approaches that of the bulk solvent, all three molecules become oriented perpendicularly to the surface. In this orientation the work of cavity formation needed to accommodate the hydrophobic ring in aqueous solvent is minimized.

Algorithms↗
PubMed1991

Interaction of monovalent ions with the water liquid-vapor interface: a molecular dynamics study.

Results of molecular dynamics studies on the ions Na+, F-, and Cl- near the water liquid-vapor interface are reported. The free energies required to move the ions to the interface are presented and shown to depend on the sign of the ionic charge, and not the size of the ion. F- and Cl- can approach to within 2 molecular layers of the interface without incurring a significant change in free energy, while it costs about 2.5 kcal/mole to move Na+ this same distance. The free energy differences between the cation and the anions arise from the interaction of the ions with the water molecules in the interfacial region. These water molecules are oriented with a slight preference for their molecular dipoles to point toward the liquid. Thus, the anions approaching the interface disrupt the water structure less than does the cation. The calculated free energy curves are compared with predictions of simple dielectric models. It is shown that these models do not provide a good description of ions at the water surface. The ions are found to retain their first solvation shells at the interface. The anions also retain part of their second solvation shells, while Na+ does not. As a result, a larger bulge in the water surface is observed above the anions than above Na+. The lateral mobilities of the ions increase at the interface, in qualitative agreement with predictions of hydrodynamic models.

Chemical Phenomena↗