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  • 1
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    The production of trace gases by photochemistry and lightning in the early atmosphere (1986)
    In:  CASI
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    Publication Date: 2006-02-14
    Description: Recent atmospheric calculation suggest that the prebiological atmosphere was most probably composed of nitrogen, carbon dioxide, and water vapor, resulting from volatile outgassing, as opposed to the older view of a strongly reducing early atmosphere composed of methane, ammonia, and hydrogen. Photochemical calculations indicate that methane would have been readily destroyed via reaction with the hydroxyl radical produced from water vapor and that ammonia would have been readily lost via photolysis and rainout. The rapid loss of methane and ammonia, coupled with the absence of a significant source of these gases, suggest that atmospheric methane and ammonia were very short lived, if they were present at all. An early atmosphere of N2, CO2, and H2O is stable and leads to the chemical production of a number of atmospheric species of biological significance, including oxygen, ozone, carbon monoxide, formaldehyde, and hydrogen cyanide. Using a photochemical model of the early atmosphere, the chemical productionof these species over a wide range of atmospheric parameters were investigated. These calculations indicate that early atmospheric levels of O3 were significantly below the levels needed to provide UV shielding. The fate of volcanically emitted sulfur species, e.g., sulfur dioxide and hydrogen sulfide, was investigated in the early atmosphere to assess their UV shielding properties. The photochemical calculations show that these species were of insufficient levels, due in part to their short photochemical lifetimes, to provide UV shielding.
    Keywords: GEOPHYSICS
    Type: NASA, Washington Second Symposium on Chemical Evolution and the Origin and Evolution of Life; p 47
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  • 2
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    Infrared measurements of HF and HCl total column abundances above Kitt Peak, 1977-1990 - Seasonal cycles, long-term increases, and comparisons with model calculations (1991)
    In:  Other Sources
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    Publication Date: 2011-08-19
    Description: The paper deals with hydrogen-chloride and hydrogen-fluoride total column measurements, their estimated long-term rates of increase, seasonal cycles, and variability, deduced from the analysis of a set of high-resolution infrared solar spectra recorded at Kitt Peak. The Kitt Peak observations and methods of analysis are described, the results are presented and compared with previously reported measurements and trends. The data is analyzed by using a multilayer nonlinear least-squares spectral fitting procedure and a consistent set of spectroscopic line parameters. Model-calculated hydrogen-chloride and hydrogen-fluoride total columns obtained with a two-dimensional model are discussed, and the model results are compared with the measured hydrogen-chloride and hydrogen-fluoride total columns, seasonal cycles, and trends. It is pointed out that the observed trends of both molecules are in satisfactory agreement with the model results calculated from emission histories and photooxidation rates for the source molecules.
    Keywords: GEOPHYSICS
    Type: Journal of Geophysical Research (ISSN 0148-0227); 96; 15
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  • 3
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    The nitrogen cycle: Atmosphere interactions (1984)
    In:  Other Sources
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    Publication Date: 2011-08-19
    Description: Atmospheric interactions involving the nitrogen species are varied and complex. These interactions include photochemical reactions, initiated by the absorption of solar photons and chemical kinetic reactions, which involve both homogeneous (gas-to-gas reactions) and heterogeneous (gas-to-particle) reactions. Another important atmospheric interaction is the production of nitrogen oxides by atmospheric lightning. The nitrogen cycle strongly couples the biosphere and atmosphere. Many nitrogen species are produced by biogenic processes. Once in the atmosphere nitrogen oxides are photochemically and chemically transformed to nitrates, which are returned to the biosphere via precipitation, dry deposition and aerosols to close the biosphere-atmosphere nitrogen cycle. The sources, sinks and photochemistry/chemistry of the nitrogen species; atmospheric nitrogen species; souces and sinks of nitrous oxide; sources; sinks and photochemistry/chemistry of ammonia; seasonal variation of the vertical distribution of ammonia in the troposphere; surface and atmospheric sources of the nitrogen species, and seasonal variation of ground level ammonia are summarized.
    Keywords: GEOPHYSICS
    Type: JPL The interaction of Global Biochemical Cycles; p 179-208
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  • 4
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    Aircraft measurements of ammonia and nitric acid in the lower troposphere (1985)
    In:  Other Sources
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    Publication Date: 2011-08-19
    Description: The first simultaneous measurements of ammonia and nitric acid in the troposphere have been made from an aircraft using a tungsten oxide denuder system. Vertical profiles of NH3 and HNO3 taken over coastal Virginia and Maryland in March and September, 1983, at altitudes from 150 m to 3000 m, show mixing ratios that decrease with altitude. Ammonia profiles show substantial seasonal variation, while nitric acid profiles do not. Using the measured profiles and a one-dimensional photochemical model, lifetimes due to heterogeneous loss of one day for HNO3 and ten days for NH3 are calculated. In contrast, NH3 profiles up to 5300 m over the North Atlantic Ocean during August 1982 show mixing ratios that increase slightly with altitude. These data represent the first ammonia profiles measured over the ocean. It is suggested that the increase in NH3 with altitude is a result of an ammonia-rich continental air mass advected over the ocean, followed by the dissolution of NH3 in the marine boundary layer on water-covered sea salt particles.
    Keywords: GEOPHYSICS
    Type: Geophysical Research Letters (ISSN 0094-8276); 12; 401-404
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  • 5
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    Water and the photochemistry of the troposphere (1984)
    In:  Other Sources
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    Publication Date: 2011-08-19
    Description: A discussion is presented concerning the role of water in its liquid and gaseous states in the chemistry and photochemistry of the earth's troposphere, with attention to the formation of the hydroxyl radical, oxidation chains involving the gases methane, carbon monoxide and ammonia, the atmospheric chemistry of the sulfur, hydrogen, halogen and nitrogen species, and the function of lightning as a source of tropospheric species. The phenomena of 'rainout', 'washout', and the aqueous chemistry of cloud an rain droplets and of water-covered aerosols, are noted. A section is devoted to the past and anticipated impact of anthropogenic activities on the chemistry and composition of the earth's atmosphere.
    Keywords: GEOPHYSICS
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  • 6
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    Tropospheric sources of NO(x) - Lightning and biology (1984)
    In:  Other Sources
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    Publication Date: 2011-08-19
    Description: Laboratory tests were performed to quantify the expected NO(x) production by lightning and biological processes. Attention was focused on energy deposition by lightning and the oxygen partial pressure of soil, and one-dimensional photochemical models were defined for the tropospheric distributions of NO and HNO3 for various NO source strengths. The Lightning Facility data were compared with air samples of N2O production gathered during over 2 yr of flights through storms. Soil NO(x) productions were studied in terms of nitrification processes involving Nitrosomonas europaea and Alcaligenes faecalis bacteria, which change ammonium to nitrite and release NO and N2O as byproducts. The results indicate that atmospheric NO(x) is generated at two tropospheric levels, with lightning and soil bacteria being significant contributors.
    Keywords: GEOPHYSICS
    Type: Atmospheric Environment (ISSN 0004-6981); 18; 9, 19
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  • 7
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    Simultaneous measurements of NO/x/, NO, and O3 production in a laboratory discharge - Atmospheric implications (1981)
    In:  Other Sources
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    Publication Date: 2011-08-18
    Description: Simultaneous measurements of NO(x) (NO + NO2), NO, and O3 production in a laboratory discharge show that within the uncertainties of the experiment, all of the NO(x) produced was NO, and no detectable enhancement of O3 after the discharge was observed. The laboratory experiments described gave an NO production rate of 5 + or - 2 x 10 to the 16th molecules/joule mole for a 100,000-1,000,000 joules/m spark. Assuming that the global dissipation of lightning energy is about 10 to the -8th joules/sq cm per sec (Dawson, 1980; and Hill et al., 1980), the NO production rate results in a global source of NO due to lightning of about 1.8 Mt(N)/yr, which is considerably lower than earlier estimates. This lower value for NO(x) production by lightning suggests that NO(x) emissions from anthropogenic sources, estimated to be at least 20 MT(N)/yr, may be the dominant source of NO(x) to the global troposphere. Furthermore, since most of the anthropogenic sources of NO(x) are located in the Northern Hemisphere, this new interpretation of the relative source strengths of this species favors a highly skewed asymmetric distribution of NO(x).
    Keywords: GEOPHYSICS
    Type: Geophysical Research Letters; 8; Apr. 198
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  • 8
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    Ozone, ultraviolet flux and temperature of the paleoatmosphere (1980)
    In:  Other Sources
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    Publication Date: 2011-08-17
    Description: The development of surface and atmospheric levels of paleoatmospheric ozone is calculated by means of a detailed photochemical model and used to determine the levels of ultraviolet flux to the surface and the surface and atmospheric temperatures of the primitive earth. The model takes into account the chemistry of oxygen, nitrogen and hydrogen species and the effects of vertical transport in an atmosphere originally composed of as much N2, H2O and CO2 as the present atmosphere to which O2 is added to calculate the vertical profiles of O3 and nitrogen oxides as a function of O2 content. Calculations show that as oxygen content increases from 0.0001 to 1 times its present value, the height of the ozone peak moves from 5 to 25 km, and that maximum ozone densities are achieved for an O2 level of 0.1 times the present. Calculations of solar UV absorption by atmospheric species indicate the presence of a UV window between 200 and 220 nm that closed only when O2 reached 0.01 times its present level. Finally, calculations made using a radiative-convective model reveal that O3 levels corresponding to an O2 level of 0.1 times the present result in a globally averaged surface temperature increase of about 4.5 K for the present solar constant.
    Keywords: GEOPHYSICS
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  • 9
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    The photochemistry of the paleoatmosphere (1982)
    In:  Other Sources
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    Publication Date: 2011-08-18
    Description: Recent progress in the understanding of the chemistry and photochemistry of the paleoatmosphere is reviewed with emphasis on the application of photochemical models to the investigation of the evolution of the atmosphere. Photochemical calculations are presented which show that a primordial highly reducing atmosphere composed of methane and ammonia, if it formed at all, would be short-lived in the presence of solar ultraviolet radiation, giving way rapidly to a more mildly reducing atmosphere of carbon dioxide and nitrogen. Estimations of O2 produced from the photolysis of water vapor prior to the emergence of photosynthesis range from less than 10 to the -14th to 0.1 times the present atmospheric level, indicating the need for further research. A series of photochemical models of increasing complexity has been developed to study the evolution of atmospheric ozone taking into account reactions with O atoms, hydrogen oxides, nitrogen oxides, and chlorine as well as vertical transport, temperature and tropospheric chemistry so that the total content and vertical distribution of O3 may be determined for a specified level of paleoatmospheric O2.
    Keywords: GEOPHYSICS
    Type: Journal of Molecular Evolution; 18; May 1
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  • 10
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    Oxygen and ozone in the early earth's atmosphere (1983)
    In:  Other Sources
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    Publication Date: 2011-08-18
    Description: The precise amount of O2 and O3 in the earth's prebiological paleoatmosphere has been a topic of considerable discussion in the past. Since the photolysis of H2O and CO2, the prebiological mechanisms to produce O2, depends on the ultraviolet flux from the Sun, a reliable quantification of the problem requires detailed knowledge of such flux. Using the most recent astronomical observation of young stars from the International Ultraviolet Explorer, as well as a detailed photochemical model of the paleoatmosphere, it is found that the amount of O2 in the prebiological paleoatmosphere may have been as much as a million times greater than previously estimated. Some of the implications of this new value are discussed.
    Keywords: GEOPHYSICS
    Type: Precambrian Research (ISSN 0301-9268); 20; 1983
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