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Sample records for atmospheric chemistry project

  1. Integrated Global Observation Strategy - Ozone and Atmospheric Chemistry Project

    NASA Technical Reports Server (NTRS)

    Hilsenrath, Ernest; Readings, C. J.; Kaye, J.; Mohnen, V.; Einaudi, Franco (Technical Monitor)

    2000-01-01

    The "Long Term Continuity of Stratospheric Ozone Measurements and Atmospheric Chemistry" project was one of six established by the Committee on Earth Observing Satellites (CEOS) in response to the Integrated Global Observing Strategy (IGOS) initiative. IGOS links satellite and ground based systems for global environmental observations. The strategy of this project is to develop a consensus of user requirements including the scientific (SPARC, IGAC, WCRP) and the applications community (WMO, UNEP) and to develop a long-term international plan for ozone and atmospheric chemistry measurements. The major components of the observing system include operational and research (meeting certain criteria) satellite platforms planned by the space faring nations which are integrated with a well supported and sustained ground, aircraft, and balloon measurements program for directed observations as well satellite validation. Highly integrated and continuous measurements of ozone, validation, and reanalysis efforts are essential to meet the international scientific and applications goals. In order to understand ozone trends, climate change, and air quality, it is essential to conduct long term measurements of certain other atmospheric species. These species include key source, radical, and reservoir constituents.

  2. Integrated Global Observation Strategy - Ozone and Atmospheric Chemistry Project

    NASA Technical Reports Server (NTRS)

    Hilsenrath, Ernest; Readings, C. J.; Kaye, J.; Mohnen, V.; Einaudi, Franco (Technical Monitor)

    2000-01-01

    The "Long Term Continuity of Stratospheric Ozone Measurements and Atmospheric Chemistry" project was one of six established by the Committee on Earth Observing Satellites (CEOS) in response to the Integrated Global Observing Strategy (IGOS) initiative. IGOS links satellite and ground based systems for global environmental observations. The strategy of this project is to develop a consensus of user requirements including the scientific (SPARC, IGAC, WCRP) and the applications community (WMO, UNEP) and to develop a long-term international plan for ozone and atmospheric chemistry measurements. The major components of the observing system include operational and research (meeting certain criteria) satellite platforms planned by the space faring nations which are integrated with a well supported and sustained ground, aircraft, and balloon measurements program for directed observations as well satellite validation. Highly integrated and continuous measurements of ozone, validation, and reanalysis efforts are essential to meet the international scientific and applications goals. In order to understand ozone trends, climate change, and air quality, it is essential to conduct long term measurements of certain other atmospheric species. These species include key source, radical, and reservoir constituents.

  3. Atmospheric chemistry

    SciTech Connect

    Sloane, C.S. ); Tesche, T.W. )

    1991-01-01

    This book covers the predictive strength of atmospheric models. The book covers all of the major important atmospheric areas, including large scale models for ozone depletion and global warming, regional scale models for urban smog (ozone and visibility impairment) and acid rain, as well as accompanying models of cloud processes and biofeedbacks.

  4. Compilation and analyses of emissions inventories for the NOAA atmospheric chemistry project. Progress report, August 1997

    SciTech Connect

    Benkovitz, C.M.

    1997-09-01

    Global inventories of anthropogenic emissions of oxides of nitrogen for circa 1985 and 1990 and non-methane volatile organic compounds (NMVOCs) for circa 1990 have been compiled by this project. Work on the inventories has been carried out under the umbrella of the Global Emissions Inventory Activity of the International Global Atmospheric Chemistry program. Global emissions of NOx for 1985 are estimated to be 21 Tg N/yr, with approximately 84% originating in the Northern Hemisphere. The global emissions for 1990 are 31 Tg N/yr for NOx and 173 Gg NMVOC/yr. Ongoing research activities for this project continue to address emissions of both NOx and NMVOCs. Future tasks include: evaluation of more detailed regional emissions estimates and update of the default 1990 inventories with the appropriate estimates; derivation of quantitative uncertainty estimates for the emission values; and development of emissions estimates for 1995.

  5. Atmospheric Chemistry and Greenhouse Gases

    SciTech Connect

    Ehhalt, D.; Prather, M.; Dentener, F.; Derwent, R.; Dlugokencky, Edward J.; Holland, E.; Isaksen, I.; Katima, J.; Kirchhoff, V.; Matson, P.; Midgley, P.; Wang, M.; Berntsen, T.; Bey, I.; Brasseur, G.; Buja, L.; Collins, W. J.; Daniel, J. S.; DeMore, W. B.; Derek, N.; Dickerson, R.; Etheridge, D.; Feichter, J.; Fraser, P.; Friedl, R.; Fuglestvedt, J.; Gauss, M.; Grenfell, L.; Grubler, Arnulf; Harris, N.; Hauglustaine, D.; Horowitz, L.; Jackman, C.; Jacob, D.; Jaegle, L.; Jain, Atul K.; Kanakidou, M.; Karlsdottir, S.; Ko, M.; Kurylo, M.; Lawrence, M.; Logan, J. A.; Manning, M.; Mauzerall, D.; McConnell, J.; Mickley, L. J.; Montzka, S.; Muller, J. F.; Olivier, J.; Pickering, K.; Pitari, G.; Roelofs, G.-J.; Rogers, H.; Rognerud, B.; Smith, Steven J.; Solomon, S.; Staehelin, J.; Steele, P.; Stevenson, D. S.; Sundet, J.; Thompson, A.; van Weele, M.; von Kuhlmann, R.; Wang, Y.; Weisenstein, D. K.; Wigley, T. M.; Wild, O.; Wuebbles, D.J.; Yantosca, R.; Joos, Fortunat; McFarland, M.

    2001-10-01

    Chapter 4 of the IPCC Third Assessment Report Climate Change 2001: The Scientific Basis. Sections include: Executive Summary 2414.1 Introduction 2434.2 Trace Gases: Current Observations, Trends and Budgets 2484.3 Projections of Future Emissions 2664.4 Projections of Atmospheric Composition for the 21st Century 2674.5 Open Questions 2774.6 Overall Impact of Global Atmospheric Chemistry Change 279

  6. Observational constraints on ozone radiative forcing from the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Bowman, K.; Shindell, D.; Worden, H.; Lamarque, J. F.; Young, P. J.; Stevenson, D.; Qu, Z.; de la Torre, M.; Bergmann, D.; Cameron-Smith, P.; Collins, W. J.; Doherty, R.; Dalsøren, S.; Faluvegi, G.; Folberth, G.; Horowitz, L. W.; Josse, B.; Lee, Y. H.; MacKenzie, I.; Myhre, G.; Nagashima, T.; Naik, V.; Plummer, D.; Rumbold, S.; Skeie, R.; Strode, S.; Sudo, K.; Szopa, S.; Voulgarakis, A.; Zeng, G.; Kulawik, S.; Worden, J.

    2012-09-01

    We use simultaneous observations of ozone and outgoing longwave radiation (OLR) from the Tropospheric Emission Spectrometer (TES) to evaluate ozone distributions and radiative forcing simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5-20 ppb) in the Southern Hemisphere (SH) and modest high bias (5-10 ppb) in the Northern Hemisphere (NH) relative to TES for 2005-2010. These biases lead to substantial differences in ozone instantaneous radiative forcing between TES and the ACCMIP simulations. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean has a low bias in the SH tropics of up to 100 m W m-2 locally and a global low bias of 35 ± 44 m W m-2 relative to TES. Combining ACCMIP preindustrial ozone and the TES present-day ozone, we calculate an observationally constrained estimate of tropospheric ozone radiative forcing (RF) of 399 ± 70 m W m-2, which is about 7% higher than using the ACCMIP models alone but with the same standard deviation (Stevenson et al., 2012). In addition, we explore an alternate approach to constraining radiative forcing estimates by choosing a subset of models that best match TES ozone, which leads to an ozone RF of 369 ± 42 m W m-2. This estimate is closer to the ACCMIP ensemble mean RF but about a 40% reduction in standard deviation. These results point towards a profitable direction of combining observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

  7. Chemistry of atmospheres.

    NASA Astrophysics Data System (ADS)

    Wayne, R. P.

    Atmospheric chemistry has been the focus of much research activity in recent years. Like its predecessor, this new edition lays down the principles of atmospheric chemistry and provides the necessary background for more detailed study. New developments are covered, including the startling discovery of the "Antarctic ozone hole", and the increasingly rapid changes in the composition of the Earth's atmosphere, apparently a result of man's activities. Information gathered by the Voyager 2 and other space missions, which have provided a new understanding of the atmospheres of planets other than our own, is also discussed.

  8. Biomass burning studies and the International Global Atmospheric Chemistry (IGAC) project

    NASA Technical Reports Server (NTRS)

    Prinn, Ronald G.

    1991-01-01

    IGAC is an ambitious, decade-long and global research initiative concerned with major research challenges in the field of atmospheric chemistry; its chemists and ecosystem biologists are addressing the problems associated with global biomass burning (BMB). Among IGAC's goals is the achievement of a fundamental understanding of the natural and anthropogenic processes determining changes in atmospheric composition and chemistry, in order to allow century-long predictions. IGAC's studies have been organized into 'foci', encompassing the marine, tropical, polar, boreal, and midlatitude areas, as well as their global composite interactions. Attention is to be given to the effects of BMB on biogeochemical cycles.

  9. Biomass burning studies and the International Global Atmospheric Chemistry (IGAC) project

    NASA Technical Reports Server (NTRS)

    Prinn, Ronald G.

    1991-01-01

    IGAC is an ambitious, decade-long and global research initiative concerned with major research challenges in the field of atmospheric chemistry; its chemists and ecosystem biologists are addressing the problems associated with global biomass burning (BMB). Among IGAC's goals is the achievement of a fundamental understanding of the natural and anthropogenic processes determining changes in atmospheric composition and chemistry, in order to allow century-long predictions. IGAC's studies have been organized into 'foci', encompassing the marine, tropical, polar, boreal, and midlatitude areas, as well as their global composite interactions. Attention is to be given to the effects of BMB on biogeochemical cycles.

  10. (Chemistry of the global atmosphere)

    SciTech Connect

    Marland, G.

    1990-09-27

    The traveler attended the conference The Chemistry of the Global Atmosphere,'' and presented a paper on the anthropogenic emission of carbon dioxide (CO{sub 2}) to the atmosphere. The conference included meetings of the International Global Atmospheric Chemistry (IGAC) programme, a core project of the International Geosphere/Biosphere Programme (IGBP) and the traveler participated in meetings on the IGAC project Development of Global Emissions Inventories'' and agreed to coordinate the working group on CO{sub 2}. Papers presented at the conference focused on the latest developments in analytical methods, modeling and understanding of atmospheric CO{sub 2}, CO, CH{sub 4}, N{sub 2}O, SO{sub 2}, NO{sub x}, NMHCs, CFCs, and aerosols.

  11. Heterogeneous atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Schryer, D. R.

    1982-01-01

    The present conference on heterogeneous atmospheric chemistry considers such topics concerning clusters, particles and microparticles as common problems in nucleation and growth, chemical kinetics, and catalysis, chemical reactions with aerosols, electron beam studies of natural and anthropogenic microparticles, and structural studies employing molecular beam techniques, as well as such gas-solid interaction topics as photoassisted reactions, catalyzed photolysis, and heterogeneous catalysis. Also discussed are sulfur dioxide absorption, oxidation, and oxidation inhibition in falling drops, sulfur dioxide/water equilibria, the evidence for heterogeneous catalysis in the atmosphere, the importance of heterogeneous processes to tropospheric chemistry, soot-catalyzed atmospheric reactions, and the concentrations and mechanisms of formation of sulfate in the atmospheric boundary layer.

  12. Heterogeneous atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Schryer, D. R.

    1982-01-01

    The present conference on heterogeneous atmospheric chemistry considers such topics concerning clusters, particles and microparticles as common problems in nucleation and growth, chemical kinetics, and catalysis, chemical reactions with aerosols, electron beam studies of natural and anthropogenic microparticles, and structural studies employing molecular beam techniques, as well as such gas-solid interaction topics as photoassisted reactions, catalyzed photolysis, and heterogeneous catalysis. Also discussed are sulfur dioxide absorption, oxidation, and oxidation inhibition in falling drops, sulfur dioxide/water equilibria, the evidence for heterogeneous catalysis in the atmosphere, the importance of heterogeneous processes to tropospheric chemistry, soot-catalyzed atmospheric reactions, and the concentrations and mechanisms of formation of sulfate in the atmospheric boundary layer.

  13. Atmospheric Chemistry Data Products

    NASA Technical Reports Server (NTRS)

    2003-01-01

    This presentation poster covers data products from the Distributed Active Archive Center (DAAC) of the Goddard Earth Sciences (GES) Data and Information Services Center (DISC). Total Ozone Mapping Spectrometer products (TOMS) introduced in the presentation include TOMS Version 8 as well as Aura, which provides 25 years of TOMS and Upper Atmosphere Research Satellite (UARS) data. The presentation lists a number of atmospheric chemistry and dynamics data sets at DAAC.

  14. COMPILATION AND ANALYSES OF EMISSIONS INVENTORIES FOR THE NOAA ATMOSPHERIC CHEMISTRY PROJECT. PROGRESS REPORT, AUGUST 1997.

    SciTech Connect

    BENKOVITZ,C.M.

    1997-09-01

    Global inventories of anthropogenic emissions of oxides of nitrogen (NO{sub x}) for circa 1985 and 1990 and Non-Methane Volatile Organic Compounds (NMVOCs) for circa 1990 have been compiled by this project. Work on the inventories has been carried out under the umbrella of the Global Emissions Inventory Activity (GEIA) of the International Global Atmospheric Chemistry (IGAC) Program. The 1985 NO{sub x} inventory was compiled using default data sets of global emissions that were refined via the use of more detailed regional data sets; this inventory is being distributed to the scientific community at large as the GEIA Version 1A inventory. Global emissions of NO{sub x} for 1985 are estimated to be 21 Tg N y{sup -1}, with approximately 84% originating in the Northern Hemisphere. The 1990 inventories of NO{sub x} and NMVOCs were compiled using unified methodologies and data sets in collaboration with the Netherlands National Institute of Public Health and Environmental Protection (Rijksinstituut Voor Volksgezondheid en Milieuhygiene, RIVM) and the Division of Technology for Society of the Netherlands Organization for Applied Scientific Research, (IMW-TNO); these emissions will be used as the default estimates to be updated with more accurate regional data. The NMVOC inventory was gridded and speciated into 23 chemical categories. The resulting global emissions for 1990 are 31 Tg N yr{sup -1} for NO{sub x} and 173 Gg NMVOC yr{sup -1}. Emissions of NO{sub x} are highest in the populated and industrialized areas of eastern North America and across Europe, and in biomass burning areas of South America, Africa, and Asia. Emissions of NMVOCs are highest in biomass burning areas of South America, Africa, and Asia. The 1990 NO{sub x} emissions were gridded to 1{sup o} resolution using surrogate data, and were given seasonal, two-vertical-level resolution and speciated into NO and NO{sub 2} based on proportions derived from the 1985 GEIA Version 1B inventory. Global NMVOC

  15. The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Overview and Description of Models, Simulations and Climate Diagnostics

    NASA Technical Reports Server (NTRS)

    Lamarque, J.-F.; Shindell, D. T.; Naik, V.; Plummer, D.; Josse, B.; Righi, M.; Rumbold, S. T.; Schulz, M.; Skeie, R. B.; Strode, S.; hide

    2013-01-01

    The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to- model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.

  16. The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Overview and Description of Models, Simulations and Climate Diagnostics

    NASA Technical Reports Server (NTRS)

    Lamarque, J.-F.; Shindell, D. T.; Naik, V.; Plummer, D.; Josse, B.; Righi, M.; Rumbold, S. T.; Schulz, M.; Skeie, R. B.; Strode, S.; Young, P. J.; Cionni, I.; Dalsoren, S.; Eyring, V.; Bergmann, D.; Cameron-Smith, P.; Collins, W. J.; Doherty, R.; Faluvegi, G.; Folberth, G.; Ghan, S. J.; Horowitz, L. W.; Lee, Y. H.; MacKenzie, I. A.; Nagashima, T.

    2013-01-01

    The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to- model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.

  17. Atmospheric Pseudohalogen Chemistry

    NASA Technical Reports Server (NTRS)

    Lary, David John

    2004-01-01

    Hydrogen cyanide is not usually considered in atmospheric chemical models. The paper presents three reasons why hydrogen cyanide is likely to be significant for atmospheric chemistry. Firstly, HCN is a product and marker of biomass burning. Secondly, it is also likely that lightning is producing HCN, and as HCN is sparingly soluble it could be a useful long-lived "smoking gun" marker of lightning activity. Thirdly, the chemical decomposition of HCN leads to the production of small amounts of the cyanide (CN) and NCO radicals. The NCO radical can be photolyzed in the visible portion of the spectrum yielding nitrogen atoms (N). The production of nitrogen atoms is significant as it leads to the titration of total nitrogen from the atmosphere via N+N->N2, where N2 is molecular nitrogen.

  18. Partial support for the International Global Atmospheric Chemistry Core Project Office

    SciTech Connect

    Prinn, Ronald G.

    2001-05-04

    IGAC provides an international framework for the planning, coordination, and execution of atmospheric--biospheric research with emphasis on projects which require resources beyond the capabilities of any single nation. The development of chemical emission inventories by IGAC scientists, the development and intercomparison under IGAC leadership of existing chemical transport models, the analysis of data gathered during IGAC-sponsored field campaigns, etc., has provided new scientific information essential to the development of the discipline.

  19. Evaluation of Present-day Aerosols over China Simulated from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Liao, H.; Chang, W.

    2014-12-01

    High concentrations of aerosols over China lead to strong radiative forcing that is important for both regional and global climate. To understand the representation of aerosols in China in current global climate models, we evaluate extensively the simulated present-day aerosol concentrations and aerosol optical depth (AOD) over China from the 12 models that participated in Atmospheric Chemistry & Climate Model Intercomparison Project (ACCMIP), by using ground-based measurements and satellite remote sensing. Ground-based measurements of aerosol concentrations used in this work include those from the China Meteorological Administration (CMA) Atmosphere Watch Network (CAWNET) and the observed fine-mode aerosol concentrations collected from the literature. The ground-based measurements of AOD in China are taken from the AErosol RObotic NETwork (AERONET), the sites with CIMEL sun photometer operated by Institute of Atmospheric Physics, Chinese Academy of Sciences, and from Chinese Sun Hazemeter Network (CSHNET). We find that the ACCMIP models generally underestimate concentrations of all major aerosol species in China. On an annual mean basis, the multi-model mean concentrations of sulfate, nitrate, ammonium, black carbon, and organic carbon are underestimated by 63%, 73%, 54%, 53%, and 59%, respectively. The multi-model mean AOD values show low biases of 20-40% at studied sites in China. The ACCMIP models can reproduce seasonal variation of nitrate but cannot capture well the seasonal variations of other aerosol species. Our analyses indicate that current global models generally underestimate the role of aerosols in China in climate simulations.

  20. Study of the atmospheric chemistry of radon progeny in laboratory and real indoor atmospheres. Final project report

    SciTech Connect

    Hopke, P.K.

    1996-09-01

    This report completes Clarkson University`s study of the chemical and physical behavior of the {sup 218}Po atom immediately following its formation by the alpha decay of radon. Because small changes in size for activity in the sub-10 nm size range result in large changes in the delivered dose per unit exposure, this behavior must be understood if the exposure to radon progeny and it dose to the cells in the respiratory tract are to be fully assessed. In order to pursue this general goal, two areas of radon progeny behavior are being pursued; laboratory studies under controlled conditions to better understand the fundamental physical and chemical processes that affect the progeny`s atmospheric behavior and studies in actual indoor environments to develop a better assessment of the exposure of the occupants of that space to the size and concentration of the indoor radioactive aerosol. Thus, two sets of specific goals have been established for this project. The specific tasks of the controlled laboratory studies are (1) Determine the formation rates of {circ}OH radicals formed by the radiolysis of air following radon decay; (2) Examine the formation of particles by the radiolytic oxidation of substances like SO{sub 2}, ethylene, and H{sub 2}S to lower vapor pressure compounds and determine the role of gas phase additives such as H{sub 2}O and NH{sub 3} in determining the particle size; (3) Measure the rate of ion-induced nucleation using a thermal diffusion cloud chamber, and (4) Measure the neutralization rate of {sup 218}PoO{sub x}{sup +} in O{sub 2} at low radon concentrations.

  1. Tropospheric Ozone Changes, Radiative Forcing and Attribution to Emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Technical Reports Server (NTRS)

    Stevenson, D.S.; Young, P.J.; Naik, V.; Lamarque, J.-F.; Shindell, D. T.; Voulgarakis, A.; Skeie, R. B.; Dalsoren, S. B.; Myhre, G.; Berntsen, T. K.; hide

    2013-01-01

    Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m-2. The model range of pre-industrial to present-day changes in O3 produces a spread (+/-1 standard deviation) in RFs of +/-17%. Three different radiation schemes were used - we find differences in RFs between schemes (for the same ozone fields) of +/-10 percent. Applying two different tropopause definitions gives differences in RFs of +/-3 percent. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of +/-30 percent for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44+/-12 percent), nitrogen oxides (31 +/- 9 percent), carbon monoxide (15 +/- 3 percent) and non-methane volatile organic compounds (9 +/- 2 percent); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m(-2) DU(-1), a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m(-2); relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some

  2. The chemistry of planetary atmospheres

    NASA Technical Reports Server (NTRS)

    Huntress, W. T., Jr.

    1976-01-01

    Present knowledge concerning the chemistry of planetary atmospheres is reviewed along with the theories which attempt to explain observational data. The known gross atmospheric compositions of the terrestrial and giant planets are listed, differences between the atmospheres of earth and Venus are discussed, and the atmospheres of the giant planets are described. The origin and evolution of the atmospheres of earth, Venus, Mars, Jupiter, Saturn, and Uranus are outlined, and chemical processes in the atmospheres are examined, particularly cloud formation. The question of organic synthesis and evolution in the reducing atmospheres of the giant planets is considered. It is noted that laboratory work on the individual chemical processes and reactions involved in the evolution of organic compounds in planetary atmospheres, comets, and interstellar space points to the inevitability of organic-compound synthesis in all these situations and to the pervasiveness of organic chemistry throughout the universe.

  3. The chemistry of planetary atmospheres

    NASA Technical Reports Server (NTRS)

    Huntress, W. T., Jr.

    1976-01-01

    Present knowledge concerning the chemistry of planetary atmospheres is reviewed along with the theories which attempt to explain observational data. The known gross atmospheric compositions of the terrestrial and giant planets are listed, differences between the atmospheres of earth and Venus are discussed, and the atmospheres of the giant planets are described. The origin and evolution of the atmospheres of earth, Venus, Mars, Jupiter, Saturn, and Uranus are outlined, and chemical processes in the atmospheres are examined, particularly cloud formation. The question of organic synthesis and evolution in the reducing atmospheres of the giant planets is considered. It is noted that laboratory work on the individual chemical processes and reactions involved in the evolution of organic compounds in planetary atmospheres, comets, and interstellar space points to the inevitability of organic-compound synthesis in all these situations and to the pervasiveness of organic chemistry throughout the universe.

  4. Organic chemistry of the atmosphere

    SciTech Connect

    Hansen, L.D. . Dept. of Chemistry)

    1991-01-01

    This book reviews the information currently available regarding the chemistry of organic compounds in the atmosphere. Topics discussed include methods for collecting organic compounds from the atmosphere, the influence of organic compounds on indoor and outdoor air quality, the chemistry of polycyclic aromatic hydrocarbons, environmental tobacco smoke, organic compounds in rainwater, organic oxysulfur compounds, and the effect of organic compounds on visibility. Many of these topics presented have never been reviewed or have never appeared together in a single volume.

  5. Land cover change impacts on atmospheric chemistry: simulating projected large-scale tree mortality in the United States

    NASA Astrophysics Data System (ADS)

    Geddes, Jeffrey A.; Heald, Colette L.; Silva, Sam J.; Martin, Randall V.

    2016-02-01

    Land use and land cover changes impact climate and air quality by altering the exchange of trace gases between the Earth's surface and atmosphere. Large-scale tree mortality that is projected to occur across the United States as a result of insect and disease may therefore have unexplored consequences for tropospheric chemistry. We develop a land use module for the GEOS-Chem global chemical transport model to facilitate simulations involving changes to the land surface, and to improve consistency across land-atmosphere exchange processes. The model is used to test the impact of projected national-scale tree mortality risk through 2027 estimated by the 2012 USDA Forest Service National Insect and Disease Risk Assessment. Changes in biogenic emissions alone decrease monthly mean O3 by up to 0.4 ppb, but reductions in deposition velocity compensate or exceed the effects of emissions yielding a net increase in O3 of more than 1 ppb in some areas. The O3 response to the projected change in emissions is affected by the ratio of baseline NOx : VOC concentrations, suggesting that in addition to the degree of land cover change, tree mortality impacts depend on whether a region is NOx-limited or NOx-saturated. Consequently, air quality (as diagnosed by the number of days that 8 h average O3 exceeds 70 ppb) improves in polluted environments where changes in emissions are more important than changes to dry deposition, but worsens in clean environments where changes to dry deposition are the more important term. The influence of changes in dry deposition demonstrated here underscores the need to evaluate treatments of this physical process in models. Biogenic secondary organic aerosol loadings are significantly affected across the US, decreasing by 5-10 % across many regions, and by more than 25 % locally. Tree mortality could therefore impact background aerosol loadings by between 0.5 and 2 µg m-3. Changes to reactive nitrogen oxide abundance and partitioning are also locally

  6. Organic chemistry in Titan's atmosphere

    NASA Technical Reports Server (NTRS)

    Scattergood, T.

    1982-01-01

    Laboratory photochemical simulations and other types of chemical simulations are discussed. The chemistry of methane, which is the major known constituent of Titan's atmosphere was examined with stress on what can be learned from photochemistry and particle irradiation. The composition of dust that comprises the haze layer was determined. Isotope fractionation in planetary atmospheres is also discussed.

  7. Organic chemistry in Titan's atmosphere

    NASA Technical Reports Server (NTRS)

    Scattergood, T.

    1982-01-01

    Laboratory photochemical simulations and other types of chemical simulations are discussed. The chemistry of methane, which is the major known constituent of Titan's atmosphere was examined with stress on what can be learned from photochemistry and particle irradiation. The composition of dust that comprises the haze layer was determined. Isotope fractionation in planetary atmospheres is also discussed.

  8. Land cover change impacts on atmospheric chemistry: simulating projected large-scale tree mortality in the United States

    NASA Astrophysics Data System (ADS)

    Geddes, J. A.; Heald, C. L.; Silva, S. J.; Martin, R. V.

    2015-10-01

    Land use and land cover changes impact climate and air quality by altering the exchange of trace gases between the Earth's surface and atmosphere. Large-scale tree mortality that is projected to occur across the United States as a result of insect and disease may therefore have unexplored consequences for tropospheric chemistry. We develop a land use module for the GEOS-Chem global chemical transport model to facilitate simulations involving changes to the land surface, and to improve consistency across land-atmosphere exchange processes. The model is used to test the impact of projected national-scale tree mortality risk through 2027 estimated by the 2012 USDA Forest Service National Insect and Disease Risk Assessment. Changes in biogenic emissions alone decrease monthly mean O3 by up to 0.4 ppb, but reductions in deposition velocity compensate or exceed the effects of emissions yielding a net increase in O3 of more than 1 ppb in some areas. The O3 response to emissions is controlled by the ratio of baseline NOx : VOC concentrations, suggesting that in addition to the degree of land cover change, tree mortality impacts depend on whether a region is NOx-limited or NOx-saturated. Consequently, air quality (as diagnosed by the number of days that average 8 h O3 exceeds 65 ppb) improves in polluted environments where changes in emissions are more important than changes to dry deposition, but worsens in clean environments where changes to dry deposition are the more important term. Biogenic secondary organic aerosol loadings are significantly affected across the US, decreasing by 5-10 % across many regions, and by more than 25 % locally. Tree mortality could therefore impact background aerosol loadings by between 0.5 to 2 μg m-3. Changes to reactive nitrogen oxide abundance and partitioning are also locally important. These simulations suggest that changes in biosphere-atmosphere exchange must be considered when predicting future air quality and climate. We point to

  9. Compilation and analyses of emissions inventories for NOAA`s atmospheric chemistry project. Progress report, August 1997

    SciTech Connect

    Benkovitz, C.M.; Mubaraki, M.A.

    1997-09-01

    Global inventories of anthropogenic emissions of oxides of nitrogen (NO{sub x}) for circa 1985 and 1990 and Non-Methane Volatile Organic Compounds (NMVOCs) for circa 1990 have been compiled by this project. Work on the inventories has been carried out under the umbrella of the Global Emissions Inventory Activity (GEIA) of the International Global Atmospheric Chemistry (IGAC) Program. The 1985 NO{sub x} inventory was compiled using default data sets of global emissions that were refined via the use of more detailed regional data sets; this inventory is being distributed to the scientific community at large as the GEIA Version 1A inventory. Global emissions of NO{sub x} for 1985 are estimated to be 21 Tg N y{sup -1}, with approximately 84% originating in the Northern Hemisphere. The 1990 inventories of NO{sub x} and NMVOCs were compiled using unified methodologies and data sets in collaboration with the Netherlands National Institute of Public Health and Environmental Protection (Rijksinstituut Voor Volksgezondheid en Milieuhygiene, RIVM) and the Division of Technology for Society of the Netherlands Organization for Applied Scientific Research, (IMW-TNO); these emissions will be used as the default estimates to be updated with more accurate regional data. The NMVOC inventory was gridded and speciated into 23 chemical categories.

  10. Heterogeneous Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Schryer, David R.

    In the past few years it has become increasingly clear that heterogeneous, or multiphase, processes play an important role in the atmosphere. Unfortunately the literature on the subject, although now fairly extensive, is still rather dispersed. Furthermore, much of the expertise regarding heterogeneous processes lies in fields not directly related to atmospheric science. Therefore, it seemed desirable to bring together for an exchange of ideas, information, and methodologies the various atmospheric scientists who are actively studying heterogeneous processes as well as other researchers studying similar processes in the context of other fields.

  11. Chemistry Of Atmospheric Brown Carbon

    SciTech Connect

    Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey

    2015-05-27

    Organic carbon (OC) accounts for a large fraction of atmospheric aerosol and has profound effects on air quality, atmospheric chemistry and climate forcing. Molecular composition of the OC and its evolution during common processes of atmospheric aging have been a subject of extensive research over the last decade (see reviews of Ervens et al.,1 Hallquist et al.,2 Herckes et al.,3 Carlton et al.,4 Kroll and Seinfeld,5 Rudich et al.,6 and Kanakidou et al.7). Even though many fundamental advances have been reported in these studies, our understanding of the climate-related properties of atmospheric OC is still incomplete and the specific ways in which OC impacts atmospheric environment and climate forcing are just beginning to be understood. This review covers one topic of particular interest in this area –environmental chemistry of light-absorbing aerosol OC and its impact on radiative forcing.

  12. Computational solution of atmospheric chemistry problems

    NASA Technical Reports Server (NTRS)

    Jafri, J.; Ake, R. L.

    1986-01-01

    Extensive studies were performed on problems of interest in atmospheric chemistry. In addition to several minor projects, four major projects were performed and described (theoretical studies of ground and low-lying excited states of ClO2; ground and excited state potential energy surfaces of the methyl peroxy radical; electronic states ot the FO radical; and theoretical studies S02 (H2O) (sub n)).

  13. Multi-model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation of Historical and Projected Future Changes

    SciTech Connect

    Lamarque, Jean-Francois; Dentener, Frank; McConnell, J.R.; Ro, C-U; Shaw, Mark; Vet, Robert; Bergmann, D.; Cameron-Smith, Philip; Dalsoren, S.; Doherty, R.; Faluvegi, G.; Ghan, Steven J.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Plummer, David; Shindell, Drew; Skeie, R. B.; Stevenson, D. S.; Strode, S.; Zeng, G.; Curran, M.; Dahl-Jensen, D.; Das, S.; Fritzsche, D.; Nolan, M.

    2013-08-20

    We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice-core measurements. We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present-day (year 2000 ACCMIP time-slice), the ACCMIP results perform similarly to previously published multi-model assessments. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States, but less so over Europe. This difference points towards misrepresentation of 1980 NH3 emissions over North America. Based on ice-core records, the 1850 deposition fluxes agree well with Greenland ice cores but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double 2000 in some scenarios and reaching >1300 mgN/m2/yr averaged over regional to continental scale regions in RCP 2.6 and 8.5, ~30-50% larger than the values in any region currently (2000). Despite known issues, the new ACCMIP deposition dataset provides novel, consistent and evaluated global gridded deposition fields for use in a wide range of climate and ecological studies.

  14. Multi-model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation Historical and Projected Changes

    NASA Technical Reports Server (NTRS)

    Lamarque, J.-F.; Dentener, F.; McConnell, J.; Ro, C.-U.; Shaw, M.; Vet, R.; Bergmann, D.; Cameron-Smith, P.; Doherty, R.; Faluvegi, G.; hide

    2013-01-01

    We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice-core measurements. We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present-day (year 2000 ACCMIP time-slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multi-model mean deposition of 50 Tg(N) yr1 from nitrogen oxide emissions, 60 Tg(N) yr1 from ammonia emissions, and 83 Tg(S) yr1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards misrepresentation of 1980 NH3 emissions over North America. Based on ice-core records, the 1850 deposition fluxes agree well with Greenland ice cores but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double 2000 in some scenarios and reaching 1300 mg(N) m2 yr1 averaged over regional to continental scale regions in RCP 2.6 and 8.5, 3050 larger than the values in any region currently (2000). The new ACCMIP deposition dataset provides novel, consistent and evaluated global gridded deposition fields for use in a wide range of climate and ecological studies.

  15. Atmospheric chemistry over southern Africa

    NASA Astrophysics Data System (ADS)

    Gatebe, Charles K.; Levy, Robert C.; Thompson, Anne M.

    2012-03-01

    Changing Chemistry in a Changing Climate: Human and Natural Impacts Over Southern Africa (C4-SAR); Midrand, South Africa, 31 May to 3 June 2011 During the southern African dry season, regional haze from mixed industrial pollution, biomass burning aerosol and gases from domestic and grassland fires, and biogenic sources from plants and soils is worsened by a semipermanent atmospheric gyre over the subcontinent. These factors were a driver of several major international field campaigns in the 1990s and early 2000s and attracted many scientists to the region. Some researchers were interested in understanding fundamental processes governing chemistry of the atmosphere and interaction with climate change. Others found favorable conditions for evaluating satellite- derived measurements of atmospheric properties and a changing land surface. With that background in mind a workshop on atmospheric chemistry was held in South Africa. Sponsored by the International Commission on Atmospheric Chemistry and Global Pollution (ICACGP; http://www.icacgp.org/), the workshop received generous support from Eskom, the South African power utility; and the Climatology Research Group of the University of the Witwatersrand, Johannesburg, South Africa.

  16. Atmospheric Chemistry Over Southern Africa

    NASA Technical Reports Server (NTRS)

    Gatebe, Charles K.; Levy, Robert C.; Thompson, Anne M.

    2011-01-01

    During the southern African dry season, regional haze from mixed industrial pollution, biomass burning aerosol and gases from domestic and grassland fires, and biogenic sources from plants and soils is worsened by a semi-permanent atmosphere gyre over the subcontinent. These factors were a driver of several major international field campaigns in the 1990s and early 2000s, and attracted many scientists to the region. Some researchers were interested in understanding fundamental processes governing chemistry of the atmosphere and interaction with climate change. Others found favorable conditions for evaluating satellite-derived measurements of atmospheric properties and a changing land surface. With that background in mind a workshop on atmospheric chemistry was held in South Africa. Sponsored by the International Commission for Atmospheric Chemistry and Global Pollution (ICACGP; http://www.icacgp.org/), the workshop received generous support from the South African power utility, Eskom, and the Climatology Research Group of the University of the Witwatersrand, Johannesburg, South Africa. The purpose of the workshop was to review some earlier findings as well as more recent findings on southern African climate vulnerability, chemical changes due to urbanization, land-use modification, and how these factors interact. Originally proposed by John Burrows, president of ICACGP, the workshop was the first ICACGP regional workshop to study the interaction of air pollution with global chemical and climate change. Organized locally by the University of the Witwatersrand, the workshop attracted more than 60 delegates from South Africa, Mozambique, Botswana, Zimbabwe, France, Germany, Canada, and the United States. More than 30 presentations were given, exploring both retrospective and prospective aspects of the science. In several talks, attention was focused on southern African chemistry, atmospheric pollution monitoring, and climate processes as they were studied in the field

  17. Atmospheric chemistry and air pollution.

    PubMed

    Gaffney, Jeffrey S; Marley, Nancy A

    2003-04-07

    Atmospheric chemistry is an important discipline for understanding air pollution and its impacts. This mini-review gives a brief history of air pollution and presents an overview of some of the basic photochemistry involved in the production of ozone and other oxidants in the atmosphere. Urban air quality issues are reviewed with a specific focus on ozone and other oxidants, primary and secondary aerosols, alternative fuels, and the potential for chlorine releases to amplify oxidant chemistry in industrial areas. Regional air pollution issues such as acid rain, long-range transport of aerosols and visibility loss, and the connections of aerosols to ozone and peroxyacetyl nitrate chemistry are examined. Finally, the potential impacts of air pollutants on the global-scale radiative balances of gases and aerosols are discussed briefly.

  18. Atmospheric Chemistry and Air Pollution

    DOE PAGES

    Gaffney, Jeffrey S.; Marley, Nancy A.

    2003-01-01

    Atmospheric chemistry is an important discipline for understanding air pollution and its impacts. This mini-review gives a brief history of air pollution and presents an overview of some of the basic photochemistry involved in the production of ozone and other oxidants in the atmosphere. Urban air quality issues are reviewed with a specific focus on ozone and other oxidants, primary and secondary aerosols, alternative fuels, and the potential for chlorine releases to amplify oxidant chemistry in industrial areas. Regional air pollution issues such as acid rain, long-range transport of aerosols and visibility loss, and the connections of aerosols to ozonemore » and peroxyacetyl nitrate chemistry are examined. Finally, the potential impacts of air pollutants on the global-scale radiative balances of gases and aerosols are discussed briefly.« less

  19. Coupling Processes Between Atmospheric Chemistry and Climate

    NASA Technical Reports Server (NTRS)

    Ko, Malcolm K. W.; Weisenstein, Debra; Shia, Run-Lie; Sze, N. D.

    1998-01-01

    The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling tools for this work are the AER 2-dimensional chemistry-transport model, the AER 2-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry. We will continue developing our three-wave model so that we can help NASA determine the strength and weakness of the next generation assessment models.

  20. Coupling Processes Between Atmospheric Chemistry and Climate

    NASA Technical Reports Server (NTRS)

    Ko, M. K. W.; Weisenstein, Debra; Shia, Run-Lie; Sze, N. D.

    1998-01-01

    The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling tools for this work are the AER two-dimensional chemistry-transport model, the AER two-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry. We will continue developing our three-wave model so that we can help NASA determine the strength and weakness of the next generation assessment models.

  1. Coupling Processes between Atmospheric Chemistry and Climate

    NASA Technical Reports Server (NTRS)

    Ko, M. K. W.; Weisenstein, Debra; Shia, Run-Lie; Sze, N. D.

    1998-01-01

    This is the third semi-annual report for NAS5-97039, covering January through June 1998. The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling for this work are the AER 2-dimensional chemistry-transport model, the AER 2-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry. We will continue developing our three-wave model so that we can help NASA determine the strengths and weaknesses of the next generation assessment models.

  2. 1997 Atmospheric Chemistry Colloquium for Emerging Senior Scientists

    SciTech Connect

    Paul H. Wine

    1998-11-23

    DOE's Atmospheric Chemistry Program is providing partial funding for the Atmospheric Chemistry Colloquium for Emerging Senior Scientists (ACCESS) and FY 1997 Gordon Research Conference in Atmospheric Chemistry

  3. A critical evaluation of present-day and future surface ozone as simulated by global chemistry-climate models in the Atmospheric Chemistry & Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Schnell, J.; Prather, M. J.

    2014-12-01

    In evaluating a future scenario for air quality, one can identify four major causal factors: (1) global emissions that alter atmospheric composition and thence baseline levels of surface ozone (O3); (2) global changes in climate that also alter these baselines (e.g., temperature, water vapor); (3) climate-driven changes in the meteorological regimes of polluted regions that lead to air quality extreme (AQX) episodes; and (4) changes in the efficacy of local emissions to produce pollution within a governance region. While these factors are all part of a coupled system, a model that combines all would be difficult to verify. Thus an assessment approach would be to evaluate each factor separately using observations and an ensemble of models. In this study, we focus on factor (3), evaluating the ability of the models in the Atmospheric Chemistry & Climate Model Intercomparison Project (ACCMIP) to reproduce the observed present-day climatology (e.g. diurnal/seasonal cycles, AQX episode size) of surface O3 in North America (NA) and Europe (EU). We then characterize future changes within these domains as well as south Asia (SA) for two experiments of RCP8.5 climate, one with O3 precursor emissions representative of the 2100s (RCP8.5) and one representative of the 2000s (Cl2100Em2000). We find that most models simulate the observed climatology well, albeit biased high over the range of each domain's probability distribution (Fig. 1). For RCP8.5, the ensemble mean shows an increase of ~10% in the mean annual maximum daily 8-h average (MDA8) over all domains, with the largest changes in winter months. For Cl2100Em2000, NA shows a small increase (+1%) in annual mean MDA8 while EU and SA show small decreases (-2% and -3%, respectively). Also for RCP8.5, most models show decreases in the mean size (S) and mean duration (D) of AQX episodes in EU (S = -28%, D = -17%) and increases in SA (+54%, +15%). The ensemble mean shows decreases in D (-7%) and increases in S (+21%) in NA

  4. Atmospheric chemistry of hydrogen fluoride

    DOE PAGES

    Cheng, Meng -Dawn

    2017-04-11

    In this study, the atmospheric chemistry, emissions, and surface boundary layer transport of hydrogen fluoride (HF) is summarized. Although HF is known to be chemically reactive and highly soluble, both factors affect transport and removal in the atmosphere, we suggest that the chemistry can be ignored when the HF concentration is at a sufficiently low level (e.g., 10 ppmv). At a low concentration, the capability for HF to react in the atmosphere is diminished and therefore the species can be mathematically treated as inert during the transport. At a sufficiently high concentration of HF (e.g., kg/s release rate and thousandsmore » of ppm), however, HF can go through a series of rigorous chemical reactions including polymerization, depolymerization, and reaction with water to form molecular complex. As such, the HF species cannot be considered as inert because the reactions could intimately influence the plume s thermodynamic properties affecting the changes in plume temperature and density. The atmospheric residence time of HF was found to be less than four (4) days, and deposition (i.e., atmosphere to surface transport) is the dominant mechanism that controls the removal of HF and its oligomers from the atmosphere. The literature data on HF dry deposition velocity was relatively high compared to many commonly found atmospheric species such as ozone, sulfur dioxide, nitrogen oxides, etc. The global average of wet deposition velocity of HF was found to be zero based on one literature source. Uptake of HF by rain drops is limited by the acidity of the rain drops, and atmospheric particulate matter contributes negligibly to HF uptake. Finally, given that the reactivity of HF at a high release rate and elevated mole concentration cannot be ignored, it is important to incorporate the reaction chemistry in the near-field dispersion close to the proximity of the release source, and to incorporate the deposition mechanism in the far-field dispersion away from the

  5. Atmospheric chemistry in volcanic plumes

    PubMed Central

    von Glasow, Roland

    2010-01-01

    Recent field observations have shown that the atmospheric plumes of quiescently degassing volcanoes are chemically very active, pointing to the role of chemical cycles involving halogen species and heterogeneous reactions on aerosol particles that have previously been unexplored for this type of volcanic plumes. Key features of these measurements can be reproduced by numerical models such as the one employed in this study. The model shows sustained high levels of reactive bromine in the plume, leading to extensive ozone destruction, that, depending on plume dispersal, can be maintained for several days. The very high concentrations of sulfur dioxide in the volcanic plume reduces the lifetime of the OH radical drastically, so that it is virtually absent in the volcanic plume. This would imply an increased lifetime of methane in volcanic plumes, unless reactive chlorine chemistry in the plume is strong enough to offset the lack of OH chemistry. A further effect of bromine chemistry in addition to ozone destruction shown by the model studies presented here, is the oxidation of mercury. This relates to mercury that has been coemitted with bromine from the volcano but also to background atmospheric mercury. The rapid oxidation of mercury implies a drastically reduced atmospheric lifetime of mercury so that the contribution of volcanic mercury to the atmospheric background might be less than previously thought. However, the implications, especially health and environmental effects due to deposition, might be substantial and warrant further studies, especially field measurements to test this hypothesis. PMID:20368458

  6. Atmospheric chemistry in volcanic plumes.

    PubMed

    von Glasow, Roland

    2010-04-13

    Recent field observations have shown that the atmospheric plumes of quiescently degassing volcanoes are chemically very active, pointing to the role of chemical cycles involving halogen species and heterogeneous reactions on aerosol particles that have previously been unexplored for this type of volcanic plumes. Key features of these measurements can be reproduced by numerical models such as the one employed in this study. The model shows sustained high levels of reactive bromine in the plume, leading to extensive ozone destruction, that, depending on plume dispersal, can be maintained for several days. The very high concentrations of sulfur dioxide in the volcanic plume reduces the lifetime of the OH radical drastically, so that it is virtually absent in the volcanic plume. This would imply an increased lifetime of methane in volcanic plumes, unless reactive chlorine chemistry in the plume is strong enough to offset the lack of OH chemistry. A further effect of bromine chemistry in addition to ozone destruction shown by the model studies presented here, is the oxidation of mercury. This relates to mercury that has been coemitted with bromine from the volcano but also to background atmospheric mercury. The rapid oxidation of mercury implies a drastically reduced atmospheric lifetime of mercury so that the contribution of volcanic mercury to the atmospheric background might be less than previously thought. However, the implications, especially health and environmental effects due to deposition, might be substantial and warrant further studies, especially field measurements to test this hypothesis.

  7. Coupling Processes Between Atmospheric Chemistry and Climate

    NASA Technical Reports Server (NTRS)

    Ko, M. K. W.; Weisenstein, Debra; Shia, Run-Li; Sze, N. D.

    1997-01-01

    This is the first semi-annual report for NAS5-97039 summarizing work performed for January 1997 through June 1997. Work in this project is related to NAS1-20666, also funded by NASA ACMAP. The work funded in this project also benefits from work at AER associated with the AER three-dimensional isentropic transport model funded by NASA AEAP and the AER two-dimensional climate-chemistry model (co-funded by Department of Energy). The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling tools for this work are the AER two-dimensional chemistry-transport model, the AER two-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry.

  8. The Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Project: Overview and results from ten years of ACE operations

    NASA Astrophysics Data System (ADS)

    Walker, Kaley; Strong, Kimberly

    2014-05-01

    As of February 2014, the Canadian-led Atmospheric Chemistry Experiment (ACE) satellite mission has been making measurements of the Earth's atmosphere for ten years. As ACE operations have extended beyond the initial two-year mission, there is a continuing need to validate the trace gas data products from the ACE-Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instruments. Ground-based measurements provide critical data for the validation of satellite retrievals of trace gases and for the assessment of long-term stability of these measurements. In particular, validation comparisons are needed for ACE during Arctic springtime to understand better the measurements of species involved in stratospheric ozone chemistry. To this end, eleven Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns have been conducted during the spring period (February - April in 2004 - 2014) at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut (80°N, 86°W). This period coincides with the most chemically active time of year in the Arctic, as well as a significant number of satellite overpasses. A suite of as many as 12 ground-based instruments, as well as frequent balloon-borne ozonesonde and radiosonde launches, have been used in each campaign. These instruments include: a ground-based version of the ACE-FTS (PARIS - Portable Atmospheric Research Interferometric Spectrometer), a terrestrial version of the ACE-MAESTRO, a SunPhotoSpectrometer, two zenith-viewing UV-visible grating spectrometers, a Bomem DA8 Fourier transform spectrometer, a Bruker 125HR Fourier transform spectrometer, a Systeme d'Analyse par Observations Zenithales (SAOZ) instrument, and several Brewer spectrophotometers. In the past several years, these results have been used to validate the measurements by the ACE-FTS and ACE-MAESTRO instruments on SCISAT as well

  9. Coupling Processes between Atmospheric Chemistry and Climate

    NASA Technical Reports Server (NTRS)

    Ko, Malcolm K. W.; Weisenstein, Debra K.; Shia, Run-Lie; Scott, Courtney J.; Sze, Nien Dak

    1998-01-01

    This is the fourth semi-annual report for NAS5-97039, covering the time period July through December 1998. The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling tools for this work are the Atmospheric and Environmental Research (AER) two-dimensional chemistry-transport model, the AER two-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry. For this six month period, we report on a modeling study of new rate constant which modify the NOx/NOy ratio in the lower stratosphere; sensitivity to changes in stratospheric water vapor in the future atmosphere; a study of N2O and CH4 observations which has allowed us to adjust diffusion in the 2-D CTM in order to obtain appropriate polar vortex isolation; a study of SF6 and age of air with comparisons of models and measurements; and a report on the Models and Measurements II effort.

  10. Pre-industrial to end 21st century projections of tropospheric ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Young, P. J.; Archibald, A. T.; Bowman, K. W.; Lamarque, J.-F.; Naik, V.; Stevenson, D. S.; Tilmes, S.; Voulgarakis, A.; Wild, O.; Bergmann, D.; Cameron-Smith, P.; Cionni, I.; Collins, W. J.; Dalsøren, S. B.; Doherty, R. M.; Eyring, V.; Faluvegi, G.; Horowitz, L. W.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Nagashima, T.; Plummer, D. A.; Righi, M.; Rumbold, S. T.; Skeie, R. B.; Shindell, D. T.; Strode, S. A.; Sudo, K.; Szopa, S.; Zeng, G.

    2012-08-01

    Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The multi-model mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75%) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, although there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere. Compared to the present day multi-model mean tropospheric ozone burden of 337 Tg, the multi-model mean burden for 1850 time slice is ~ 30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes for the tropospheric ozone burden in 2030 (2100) for the different RCPs are: -5% (-22%) for RCP2.6, 3% (-8%) for RCP4.5, 0% (-9%) for RCP6.0, and 5% (15%) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a larger stratospheric influx increase ozone. Models with high ozone abundances for the present day also have high ozone levels for the other time slices, but there are no models consistently predicting large or small changes. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

  11. Nighttime atmospheric chemistry of iodine

    NASA Astrophysics Data System (ADS)

    Saiz-Lopez, Alfonso; Plane, John M. C.; Cuevas, Carlos A.; Mahajan, Anoop S.; Lamarque, Jean-François; Kinnison, Douglas E.

    2017-04-01

    Little attention has so far been paid to the nighttime atmospheric chemistry of iodine species. Atmospheric models predict a buildup of HOI and I2 during the night that leads to a spike of IO at sunrise, which is not observed by measurements. In this work, electronic structure calculations are used to survey possible reactions that HOI and I2 could undergo at night in the lower troposphere, and hence reduce their nighttime accumulation. The new reaction NO3 + HOI → IO + HNO3 is proposed and included in two atmospheric models, along with the known reaction between I2 and NO3, to explore a new nocturnal iodine radical activation mechanism. Our results show that this iodine scheme leads to a considerable reduction of nighttime HOI and I2, which results in the enhancement of more than 25% of nighttime ocean emissions of HOI + I2 and the removal of the anomalous spike of IO at sunrise. That active nighttime iodine could also have a considerable, so far unrecognized, impact on the reduction of the NO3 radical levels in the marine boundary layer (MBL) and hence upon the nocturnal oxidizing capacity of the marine atmosphere. The effect of this is exemplified by the indirect effect on dimethyl sulfide (DMS) oxidation.

  12. Pre-industrial to End 21st Century Projections of Tropospheric Ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Technical Reports Server (NTRS)

    Young, P. J.; Archibald, A. T.; Bowman, K. W.; Lamarque, J.-F.; Naik, V.; Stevenson, D. S.; Tilmes, S.; Voulgarakis, A.; Wild, O.; Bergmann, D.; hide

    2013-01-01

    Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337+/-23 Tg, the ensemble mean burden for 1850 time slice is approx. 30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: -4% (-16 %) for RCP2.6, 2% (-7%) for RCP4.5, 1% (-9%) for RCP6.0, and 7% (18 %) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations

  13. Pre-industrial to end 21st century projections of tropospheric ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Young, P. J.; Archibald, A. T.; Bowman, K. W.; Lamarque, J.-F.; Naik, V.; Stevenson, D. S.; Tilmes, S.; Voulgarakis, A.; Wild, O.; Bergmann, D.; Cameron-Smith, P.; Cionni, I.; Collins, W. J.; Dalsøren, S. B.; Doherty, R. M.; Eyring, V.; Faluvegi, G.; Horowitz, L. W.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Nagashima, T.; Plummer, D. A.; Righi, M.; Rumbold, S. T.; Skeie, R. B.; Shindell, D. T.; Strode, S. A.; Sudo, K.; Szopa, S.; Zeng, G.

    2013-02-01

    Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337 ± 23 Tg, the ensemble mean burden for 1850 time slice is ~30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: -4% (-16%) for RCP2.6, 2% (-7%) for RCP4.5, 1% (-9%) for RCP6.0, and 7% (18%) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A

  14. The Atmospheric Chemistry Experiment (ACE)

    NASA Astrophysics Data System (ADS)

    Bernath, P. F.

    2017-01-01

    The Atmospheric Chemistry Experiment (ACE), also called SCISAT, is a Canadian-led small satellite mission for remote sensing of the Earth's atmosphere. ACE was launched into a low Earth circular orbit by NASA on August 12, 2003 and it continues to function nominally. The ACE instruments are a high spectral resolution (0.02 cm-1) Fourier Transform Spectrometer (FTS) operating from 2.2 to 13.3 μm (750-4400 cm-1), a spectrophotometer known as Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (MAESTRO) with wavelength coverage of 285-1020 nm and two filtered detector arrays to image the Sun at 0.525 and 1.02 μm. ACE operates in solar occultation mode to provide altitude profiles of temperature, pressure, atmospheric extinction and the volume mixing ratios (VMRs) for several dozen molecules and related isotopologues. This paper presents a mission overview and a summary of selected scientific results.

  15. Nighttime atmospheric chemistry of iodine

    DOE PAGES

    Saiz-Lopez, Alfonso; Plane, John M. C.; Cuevas, Carlos A.; ...

    2016-12-19

    Little attention has so far been paid to the nighttime atmospheric chemistry of iodine species. Current atmospheric models predict a buildup of HOI and I2 during the night that leads to a spike of IO at sunrise, which is not observed by measurements. In this work, electronic structure calculations are used to survey possible reactions that HOI and I2 could undergo at night in the lower troposphere, and hence reduce their nighttime accumulation. The new reaction NO3+ HOI → IO + HNO3 is proposed, with a rate coefficient calculated from statistical rate theory over the temperature range 260–300 K andmore » at a pressure of 1000 hPa to be k(T) = 2.7 × 10-12 (300 K/T)2.66 cm3 molecule-1 s-1. This reaction is included in two atmospheric models, along with the known reaction between I2 and NO3, to explore a new nocturnal iodine radical activation mechanism. The results show that this iodine scheme leads to a considerable reduction of nighttime HOI and I2, which results in the enhancement of more than 25 % of nighttime ocean emissions of HOI + I2 and the removal of the anomalous spike of IO at sunrise. We suggest that active nighttime iodine can also have a considerable, so far unrecognized, impact on the reduction of the NO3 radical levels in the marine boundary layer (MBL) and hence upon the nocturnal oxidizing capacity of the marine atmosphere. In conclusion, the effect of this is exemplified by the indirect effect on dimethyl sulfide (DMS) oxidation.« less

  16. Nighttime atmospheric chemistry of iodine

    NASA Astrophysics Data System (ADS)

    Saiz-Lopez, Alfonso; Plane, John M. C.; Cuevas, Carlos A.; Mahajan, Anoop S.; Lamarque, Jean-François; Kinnison, Douglas E.

    2016-12-01

    Little attention has so far been paid to the nighttime atmospheric chemistry of iodine species. Current atmospheric models predict a buildup of HOI and I2 during the night that leads to a spike of IO at sunrise, which is not observed by measurements. In this work, electronic structure calculations are used to survey possible reactions that HOI and I2 could undergo at night in the lower troposphere, and hence reduce their nighttime accumulation. The new reaction NO3+ HOI → IO + HNO3 is proposed, with a rate coefficient calculated from statistical rate theory over the temperature range 260-300 K and at a pressure of 1000 hPa to be k(T) = 2.7 × 10-12 (300 K/T)2.66 cm3 molecule-1 s-1. This reaction is included in two atmospheric models, along with the known reaction between I2 and NO3, to explore a new nocturnal iodine radical activation mechanism. The results show that this iodine scheme leads to a considerable reduction of nighttime HOI and I2, which results in the enhancement of more than 25 % of nighttime ocean emissions of HOI + I2 and the removal of the anomalous spike of IO at sunrise. We suggest that active nighttime iodine can also have a considerable, so far unrecognized, impact on the reduction of the NO3 radical levels in the marine boundary layer (MBL) and hence upon the nocturnal oxidizing capacity of the marine atmosphere. The effect of this is exemplified by the indirect effect on dimethyl sulfide (DMS) oxidation.

  17. Nighttime atmospheric chemistry of iodine

    SciTech Connect

    Saiz-Lopez, Alfonso; Plane, John M. C.; Cuevas, Carlos A.; Mahajan, Anoop S.; Lamarque, Jean -Francois; Kinnison, Douglas E.

    2016-12-19

    Little attention has so far been paid to the nighttime atmospheric chemistry of iodine species. Current atmospheric models predict a buildup of HOI and I2 during the night that leads to a spike of IO at sunrise, which is not observed by measurements. In this work, electronic structure calculations are used to survey possible reactions that HOI and I2 could undergo at night in the lower troposphere, and hence reduce their nighttime accumulation. The new reaction NO3+ HOI → IO + HNO3 is proposed, with a rate coefficient calculated from statistical rate theory over the temperature range 260–300 K and at a pressure of 1000 hPa to be k(T) = 2.7 × 10-12 (300 K/T)2.66 cm3 molecule-1 s-1. This reaction is included in two atmospheric models, along with the known reaction between I2 and NO3, to explore a new nocturnal iodine radical activation mechanism. The results show that this iodine scheme leads to a considerable reduction of nighttime HOI and I2, which results in the enhancement of more than 25 % of nighttime ocean emissions of HOI + I2 and the removal of the anomalous spike of IO at sunrise. We suggest that active nighttime iodine can also have a considerable, so far unrecognized, impact on the reduction of the NO3 radical levels in the marine boundary layer (MBL) and hence upon the nocturnal oxidizing capacity of the marine atmosphere. In conclusion, the effect of this is exemplified by the indirect effect on dimethyl sulfide (DMS) oxidation.

  18. The chemistry of Venus' atmosphere

    NASA Technical Reports Server (NTRS)

    Sze, N. D.; Smith, W. H.

    1978-01-01

    A model for the Venus atmosphere involving photochemistry of oxygen, hydrogen, chlorine and sulfur species is presented. Sulfur reaction schemes and hydrogen and chlorine reaction schemes were included. The impact of sulfur on the oxygen budget and the subsequent production of H2SO4 molecules for the Venus cloud deck were explored. A major new reaction scheme for production of H2SO4 molecules involving sulfur and oxygen chemistry was established shown to dominate over the odd hydrogen scheme proposed earlier. The efficiency of the scheme in formation of H2SO4 is only about 50%, with the remaining sulfur residing in SO2 molecules. The calculated downward flux of H2SO4 may be sufficient to maintain a steady state sulfuric acid cloud if the resident time of H2SO4 droplets in the cloud is as long as a few years. If however, the resident time is half a year or shorter, additional chemistry capable of more efficient conversion of SO2 to SO3 is required.

  19. Atmospheric Composition Change: Climate-Chemistry Interactions

    NASA Technical Reports Server (NTRS)

    Isaksen, I.S.A.; Granier, C.; Myhre, G.; Bernsten, T. K.; Dalsoren, S. B.; Gauss, S.; Klimont, Z.; Benestad, R.; Bousquet, P.; Collins, W.; hide

    2011-01-01

    Chemically active climate compounds are either primary compounds such as methane (CH4), removed by oxidation in the atmosphere, or secondary compounds such as ozone (O3), sulfate and organic aerosols, formed and removed in the atmosphere. Man-induced climate-chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate-chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds such as O3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds such as O3, and of particles inducing both direct and indirect effects. Through EU projects such as ACCENT, QUANTIFY, and the AEROCOM project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric-tropospheric exchange of ozone, more frequent periods with stable conditions favouring pollution build up over industrial areas, enhanced temperature-induced biogenic emissions, methane releases from permafrost thawing, and enhanced

  20. Updated operational protocols for the U.S. Geological Survey Precipitation Chemistry Quality Assurance Project in support of the National Atmospheric Deposition Program

    USGS Publications Warehouse

    Wetherbee, Gregory A.; Martin, RoseAnn

    2017-02-06

    The U.S. Geological Survey Branch of Quality Systems operates the Precipitation Chemistry Quality Assurance Project (PCQA) for the National Atmospheric Deposition Program/National Trends Network (NADP/NTN) and National Atmospheric Deposition Program/Mercury Deposition Network (NADP/MDN). Since 1978, various programs have been implemented by the PCQA to estimate data variability and bias contributed by changing protocols, equipment, and sample submission schemes within NADP networks. These programs independently measure the field and laboratory components which contribute to the overall variability of NADP wet-deposition chemistry and precipitation depth measurements. The PCQA evaluates the quality of analyte-specific chemical analyses from the two, currently (2016) contracted NADP laboratories, Central Analytical Laboratory and Mercury Analytical Laboratory, by comparing laboratory performance among participating national and international laboratories. Sample contamination and stability are evaluated for NTN and MDN by using externally field-processed blank samples provided by the Branch of Quality Systems. A colocated sampler program evaluates the overall variability of NTN measurements and bias between dissimilar precipitation gages and sample collectors.This report documents historical PCQA operations and general procedures for each of the external quality-assurance programs from 2007 to 2016.

  1. Coupling Processes Between Atmospheric Chemistry and Climate

    NASA Technical Reports Server (NTRS)

    Ko, Malcolm K. W.; Weisenstein, Debra; Rodriguez, Jose; Danilin, Michael; Scott, Courtney; Shia, Run-Lie; Eluszkiewicz, Junusz; Sze, Nien-Dak

    1999-01-01

    This is the final report. The overall objective of this project is to improve the understanding of coupling processes among atmospheric chemistry, aerosol and climate, all important for quantitative assessments of global change. Among our priority are changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The work emphasizes two important aspects: (1) AER's continued participation in preparation of, and providing scientific input for, various scientific reports connected with assessment of stratospheric ozone and climate. These include participation in various model intercomparison exercises as well as preparation of national and international reports. and (2) Continued development of the AER three-wave interactive model to address how the transport circulation will change as ozone and the thermal properties of the atmosphere change, and assess how these new findings will affect our confidence in the ozone assessment results.

  2. Ether and the atmospheric chemistry data assimilation

    NASA Astrophysics Data System (ADS)

    Ricaud, P.; Phulpin, T.; Girod, F.; Boonne, C.

    The French atmospheric chemistry data base Ether has been developed and funded by the French Space Agency (CNES) and the Institut National des Sciences de l'Univers (INSU/CNRS) for about 6 years. The role of Ether is to assist French atmospheric researchers, European scientists, as long as they are involved in co-operation agreements with French scientists, to locate, access and interpret atmospheric data. This centre gathers data from satellite, balloon campaigns linked to satellite validation, aircraft and model results for stratospheric and tropospheric purposes and from different levels of production (raw data, physical data, interpolated or assimilated data). All Ether data are available on-line through a World Web interface (http://ether.ipsl.jussieu.fr). Software and added-value services are provided to assist in the manipulation of the data or to generate higher levels standard data products. Extensive information is also provided on the data collection procedures, formats, contact names and references to scientific papers. In addition to data support activities, a major goal of Ether is to promote the creation of different expertise networks on varying atmospheric chemistry topics. The first working group has been created on data assimilation. It consists in gathering expertises in different themes (satellites, assimilation techniques, modelling, real-time processing) in order to optimally develop a tool able to answer different scientific questions relative to the evolution of the Earth atmosphere in terms of chemistry and dynamics. Based on the PALM tool able to interconnect different codes, it will be able to process different satellite data using two atmospheric models and assimilation schemes within the French Ether data base. Ether will focus on the handling and on the development of added-value services of data for which the French community is directly or indirectly involved. For these projects Ether will provide all the data needed, and will

  3. Mars Atmospheric Chemistry and Astrobiology Workshop Summary

    NASA Astrophysics Data System (ADS)

    Allen, M.; Wennberg, P.

    2002-09-01

    The Mars Atmospheric Chemistry and Astrobiology (MACA) Workshop was held on the California Institute of Technology campus December 17-18, 2001. The prime objective of the workshop was to consider whether extant life beneath the surface, if it exists, would be in contact with the atmosphere and introduce a detectable signature in the atmosphere. To answer this question, the workshop also explored how well we understood the abiotic chemistry of the current atmosphere and other drivers of atmospheric composition (volcanoes, surface-atmosphere interactions, escape). The conclusions from this workshop will be presented.

  4. Atmospheric Aerosol Chemistry Analyzer: Demonstration of feasibility

    SciTech Connect

    Mroz, E.J.; Olivares, J.; Kok, G.

    1996-04-01

    This is the final report of a three-year, Laboratory-Directed Research and Development (LDRD) project at the Los Alamos National Laboratory (LANL). The project objective was to demonstrate the technical feasibility of an Atmospheric Aerosol Chemistry Analyzer (AACA) that will provide a continuous, real-time analysis of the elemental (major, minor and trace) composition of atmospheric aerosols. The AACA concept is based on sampling the atmospheric aerosol through a wet cyclone scrubber that produces an aqueous suspension of the particles. This suspension can then be analyzed for elemental composition by ICP/MS or collected for subsequent analysis by other methods. The key technical challenge was to develop a wet cyclone aerosol sampler suitable for respirable particles found in ambient aerosols. We adapted an ultrasonic nebulizer to a conventional, commercially available, cyclone aerosol sampler and completed collection efficiency tests for the unit, which was shown to efficiently collect particles as small as 0.2 microns. We have completed the necessary basic research and have demonstrated the feasibility of the AACA concept.

  5. Collaborative Physical Chemistry Projects Involving Computational Chemistry

    NASA Astrophysics Data System (ADS)

    Whisnant, David M.; Howe, Jerry J.; Lever, Lisa S.

    2000-02-01

    The physical chemistry classes from three colleges have collaborated on two computational chemistry projects using Quantum CAChe 3.0 and Gaussian 94W running on Pentium II PCs. Online communication by email and the World Wide Web was an important part of the collaboration. In the first project, students used molecular modeling to predict benzene derivatives that might be possible hair dyes. They used PM3 and ZINDO calculations to predict the electronic spectra of the molecules and tested the predicted spectra by comparing some with experimental measurements. They also did literature searches for real hair dyes and possible health effects. In the final phase of the project they proposed a synthetic pathway for one compound. In the second project the students were asked to predict which isomer of a small carbon cluster (C3, C4, or C5) was responsible for a series of IR lines observed in the spectrum of a carbon star. After preliminary PM3 calculations, they used ab initio calculations at the HF/6-31G(d) and MP2/6-31G(d) level to model the molecules and predict their vibrational frequencies and rotational constants. A comparison of the predictions with the experimental spectra suggested that the linear isomer of the C5 molecule was responsible for the lines.

  6. Modeling the atmospheric chemistry of TICs

    NASA Astrophysics Data System (ADS)

    Henley, Michael V.; Burns, Douglas S.; Chynwat, Veeradej; Moore, William; Plitz, Angela; Rottmann, Shawn; Hearn, John

    2009-05-01

    An atmospheric chemistry model that describes the behavior and disposition of environmentally hazardous compounds discharged into the atmosphere was coupled with the transport and diffusion model, SCIPUFF. The atmospheric chemistry model was developed by reducing a detailed atmospheric chemistry mechanism to a simple empirical effective degradation rate term (keff) that is a function of important meteorological parameters such as solar flux, temperature, and cloud cover. Empirically derived keff functions that describe the degradation of target toxic industrial chemicals (TICs) were derived by statistically analyzing data generated from the detailed chemistry mechanism run over a wide range of (typical) atmospheric conditions. To assess and identify areas to improve the developed atmospheric chemistry model, sensitivity and uncertainty analyses were performed to (1) quantify the sensitivity of the model output (TIC concentrations) with respect to changes in the input parameters and (2) improve, where necessary, the quality of the input data based on sensitivity results. The model predictions were evaluated against experimental data. Chamber data were used to remove the complexities of dispersion in the atmosphere.

  7. Energy, atmospheric chemistry, and global climate

    NASA Technical Reports Server (NTRS)

    Levine, Joel S.

    1991-01-01

    Global atmospheric changes due to ozone destruction and the greenhouse effect are discussed. The work of the Intergovernmental Panel on Climate Change is reviewed, including its judgements regarding global warming and its recommendations for improving predictive capability. The chemistry of ozone destruction and the global atmospheric budget of nitrous oxide are reviewed, and the global sources of nitrous oxide are described.

  8. The PHOCUS Project: Atmospheric Composition

    NASA Astrophysics Data System (ADS)

    Hedin, J.; Gumbel, J.; Khaplanov, M.

    2012-12-01

    On the morning of July 21, 2011, the PHOCUS sounding rocket was launched from Esrange, Sweden, into strong noctilucent clouds (NLC) and polar mesosphere summer echoes (PMSE). The aim of the PHOCUS project (Particles, Hydrogen and Oxygen Chemistry in the Upper Summer mesosphere) is to study mesospheric particles (ice and meteoric smoke) and their interaction with their neutral and charged environment. Interactions of interest comprise the charging and nucleation of particles, the relationship between meteoric smoke and ice, and the influence of these particles on gas-phase chemistry. Here we will describe the optical measurements of the atmospheric composition and present first results including comparison to the other simultaneous measurements. The atmospheric composition was probed by a set of optical instruments from Stockholm University. The idea behind the instrument setup was to combine the advantages of the sensitive resonance fluorescence with well-calibrated airglow photometry. The set of instruments consisted of two resonance fluorescence probes (each containing a lamp and a detector), one for atomic oxygen and one for atomic hydrogen, and two IR photometers for O2 and OH dayglow emissions in the near IR. The O2 IR Atmospheric system at 1.27 μm is related to the photolysis of O3, which during the day is in steady state with O and a retrieval of O is possible. The OH Meinel emission is produced by the reaction between mesospheric O3 and H, and H concentrations can be deduced by combining information from both photometers. Unfortunately, some of these measurements were corrupted by instrument problems or payload glow. O3 and O profiles will be presented and compared to the simultaneous measurements of ice and meteoric smoke particles, water vapour and the state of the background neutral and charged atmosphere.

  9. Carbon Monoxide Affecting Planetary Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    He, Chao; Hörst, Sarah M.; Riemer, Sydney; Sebree, Joshua A.; Pauley, Nicholas; Vuitton, Véronique

    2017-06-01

    CO is an important component in many {{{N}}}2/{{CH}}4 atmospheres, including Titan, Triton, and Pluto, and has also been detected in the atmosphere of a number of exoplanets. Numerous experimental simulations have been carried out in the laboratory to understand the chemistry in {{{N}}}2/{{CH}}4 atmospheres, but very few simulations have included CO in the initial gas mixtures. The effect of CO on the chemistry occurring in these atmospheres is still poorly understood. We have investigated the effect of CO on both gas and solid phase chemistry in a series of planetary atmosphere simulation experiments using gas mixtures of CO, {{CH}}4, and {{{N}}}2 with a range of CO mixing ratios from 0.05% to 5% at low temperature (˜100 K). We find that CO affects the gas phase chemistry, the density, and the composition of the solids. Specifically, with the increase of CO in the initial gases, there is less {{{H}}}2 but more {{{H}}}2{{O}}, HCN, {{{C}}}2{{{H}}}5{{N}}/{HCNO}, and {{CO}}2 produced in the gas phase, while the density, oxygen content, and degree of unsaturation of the solids increase. The results indicate that CO has an important impact on the chemistry occurring in our experiments and accordingly in planetary atmospheres.

  10. Coupling Processes Between Atmospheric Chemistry and Climate

    NASA Technical Reports Server (NTRS)

    Ko, Malcolm; Weisenstein, Debra; Rodriquez, Jose; Danilin, Michael; Scott, Courtney; Shia, Run-Lie; Eluszkiewicz, Janusz; Sze, Nien-Dak; Stewart, Richard W. (Technical Monitor)

    1999-01-01

    This is the final report for NAS5-97039 for work performed between December 1996 and November 1999. The overall objective of this project is to improve the understanding of coupling processes among atmospheric chemistry, aerosol and climate, all important for quantitative assessments of global change. Among our priority are changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The work emphasizes two important aspects: (1) AER's continued participation in preparation of, and providing scientific input for, various scientific reports connected with assessment of stratospheric ozone and climate. These include participation in various model intercomparison exercises as well as preparation of national and international reports. (2) Continued development of the AER three-wave interactive model to address how the transport circulation will change as ozone and the thermal properties of the atmosphere change, and assess how these new findings will affect our confidence in the ozone assessment results.

  11. Nitrogen Chemistry in Titan's Upper Atmosphere

    NASA Technical Reports Server (NTRS)

    McKay, Christopher P.; Cuzzi, Jeffrey (Technical Monitor)

    1996-01-01

    In Titan's upper atmosphere N2 is dissociated to N by solar UV and high energy electrons. This flux of N provides for interesting organic chemistry in the lower atmosphere of Titan. Previously the main pathway for the loss of this N was thought to be the formation of HCN, followed by diffusion of this HCN to lower altitudes leading ultimately to condensation. However, recent laboratory simulations of organic chemistry in Titan's atmosphere suggest that formation of the organic haze may be an important sink for atmospheric N. Because estimates of the eddy diffusion profile on Titan have been based on the HCN profile, inclusion of this additional sink for N will affect estimates for all transport processes in Titan's atmosphere. This and other implications of this sink for the N balance on Titan are considered.

  12. Nitrogen Chemistry in Titan's Upper Atmosphere

    NASA Technical Reports Server (NTRS)

    McKay, Christopher P.; Cuzzi, Jeffrey (Technical Monitor)

    1996-01-01

    In Titan's upper atmosphere N2 is dissociated to N by solar UV and high energy electrons. This flux of N provides for interesting organic chemistry in the lower atmosphere of Titan. Previously the main pathway for the loss of this N was thought to be the formation of HCN, followed by diffusion of this HCN to lower altitudes leading ultimately to condensation. However, recent laboratory simulations of organic chemistry in Titan's atmosphere suggest that formation of the organic haze may be an important sink for atmospheric N. Because estimates of the eddy diffusion profile on Titan have been based on the HCN profile, inclusion of this additional sink for N will affect estimates for all transport processes in Titan's atmosphere. This and other implications of this sink for the N balance on Titan are considered.

  13. Parallel computing in atmospheric chemistry models

    SciTech Connect

    Rotman, D.

    1996-02-01

    Studies of atmospheric chemistry are of high scientific interest, involve computations that are complex and intense, and require enormous amounts of I/O. Current supercomputer computational capabilities are limiting the studies of stratospheric and tropospheric chemistry and will certainly not be able to handle the upcoming coupled chemistry/climate models. To enable such calculations, the authors have developed a computing framework that allows computations on a wide range of computational platforms, including massively parallel machines. Because of the fast paced changes in this field, the modeling framework and scientific modules have been developed to be highly portable and efficient. Here, the authors present the important features of the framework and focus on the atmospheric chemistry module, named IMPACT, and its capabilities. Applications of IMPACT to aircraft studies will be presented.

  14. Perspective: Water cluster mediated atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Vaida, Veronica

    2011-07-01

    The importance of water in atmospheric and environmental chemistry initiated recent studies with results documenting catalysis, suppression and anti-catalysis of thermal and photochemical reactions due to hydrogen bonding of reagents with water. Water, even one water molecule in binary complexes, has been shown by quantum chemistry to stabilize the transition state and lower its energy. However, new results underscore the need to evaluate the relative competing rates between reaction and dissipation to elucidate the role of water in chemistry. Water clusters have been used successfully as models for reactions in gas-phase, in aqueous condensed phases and at aqueous surfaces. Opportunities for experimental and theoretical chemical physics to make fundamental new discoveries abound. Work in this field is timely given the importance of water in atmospheric and environmental chemistry.

  15. Perspective: Water cluster mediated atmospheric chemistry

    SciTech Connect

    Vaida, Veronica

    2011-07-14

    The importance of water in atmospheric and environmental chemistry initiated recent studies with results documenting catalysis, suppression and anti-catalysis of thermal and photochemical reactions due to hydrogen bonding of reagents with water. Water, even one water molecule in binary complexes, has been shown by quantum chemistry to stabilize the transition state and lower its energy. However, new results underscore the need to evaluate the relative competing rates between reaction and dissipation to elucidate the role of water in chemistry. Water clusters have been used successfully as models for reactions in gas-phase, in aqueous condensed phases and at aqueous surfaces. Opportunities for experimental and theoretical chemical physics to make fundamental new discoveries abound. Work in this field is timely given the importance of water in atmospheric and environmental chemistry.

  16. Atmospheric Chemistry: Nature's plasticized aerosols

    NASA Astrophysics Data System (ADS)

    Ziemann, Paul J.

    2016-01-01

    The structure of atmospheric aerosol particles affects their reactivity and growth rates. Measurements of aerosol properties over the Amazon rainforest indicate that organic particles above tropical rainforests are simple liquid drops.

  17. Atmospheric Chemistry: Fundamentals and Experimental Techniques

    NASA Astrophysics Data System (ADS)

    Ronneau, C.

    This book by B. J. Finlayson-Pitts and J. N. Pitts appears at a time when atmospheric chemistry has reached a remarkable achievement. This relatively new discipline was given its first impetus in the 1950s, when Haagen-Smit and his coworkers published their nowclassical papers about the Los Angeles photochemical smog. In less than 3 decades, atmospheric chemistry has matured and is now able to cope with the major challenges of air pollution. It has grown into an elaborate science, covering a broad range of experimental and theoretical approaches.

  18. Chemistry of Planetary Atmospheres: Insights and Prospects

    NASA Astrophysics Data System (ADS)

    Yung, Yuk

    2015-11-01

    Using observations from the Mariners, Pioneers, Vikings, Voyagers, Pioneer Venus, Galileo, Venus Express, Curiosity, Cassini, New Horizons, and numerous observatories both in orbit of Earth and on the ground, I will give a survey of the major chemical processes that control the composition of planetary atmospheres. For the first time since the beginning of the space age, we understand the chemistry of planetary atmospheres ranging from the primitive atmospheres of the giant planets to the highly evolved atmospheres of terrestrial planets and small bodies. Our understanding can be distilled into three important ideas: (1) The stability of planetary atmospheres against escape of their constituents to space, (2) the role of equilibrium chemistry in determining the partitioning of chemical species, and (3) the role of disequilibrium chemistry, which produces drastic departures from equilibrium chemistry. To these three ideas we must also add a fourth: the role of biochemistry at Earth's surface, which makes its atmospheric chemistry unique in the cosmochemical environment. Only in the Earth's atmosphere do strong reducing and oxidizing species coexist to such a degree. For example, nitrogen species in the Earth's atmosphere span eight oxidation states from ammonia to nitric acid. Much of the Earth's atmospheric chemistry consists of reactions initiated by the degradation of biologically produced molecules. Life uses solar energy to drive chemical reactions that would otherwise not occur; it represents a kind of photochemistry that is special to Earth, at least within the Solar System. It remains to be seen how many worlds like Earth there are beyond the Solar System, especially as we are now exploring the exoplanets using Kepler, TESS, HST, Spitzer, soon to be launched missions such as JWST and WFIRST, and ground-based telescopes. The atmospheres of the Solar System provide a benchmark for studying exoplanets, which in turn serve to test and extend our current

  19. Organic chemistry in the atmosphere. [laboratory modeling of Titan atmosphere

    NASA Technical Reports Server (NTRS)

    Sagan, C.

    1974-01-01

    The existence of an at least moderately complex organic chemistry on Titan is stipulated based on clear evidence of methane, and at least presumptive evidence of hydrogen in its atmosphere. The ratio of methane to hydrogen is the highest of any atmosphere in the solar system. Irradiation of hydrogen/methane mixtures produces aromatic and aliphatic hydrocarbons. A very reasonable hypothesis assumes that the red cloud cover of Titan is made of organic chemicals. Two-carbon hydrocarbons experimentally produced from irradiated mixtures of methane, ammonia, water, and hydrogen bear out the possible organic chemistry of the Titanian environment.

  20. PNNL's 'PEGASUS' Advances Atmospheric Chemistry

    SciTech Connect

    Berkowitz, Carl M.; Eades, Robert A.

    2001-04-16

    Presented an overview of software design to maximize computational efficiency on a massively parallel computing system. Also gave highlights of scientific results from this code, focusing primarily on how we can distinguish between stratospheric ozone in remote atmospheres and ozone generated from NOx/VOC chemical mechanisms.

  1. 1999 Gordon Research Conference on Atmospheric Chemistry

    SciTech Connect

    Storm, C.

    2000-08-01

    The Gordon Research Conference (GRC) on Atmospheric Chemistry was held at Salve Regina University in Newport, Rhode Island, June 13-18, 1999. The conference was well attended with 151 participants. The attendees represented the spectrum of endeavor in this field coming from academia, industry, and government laboratories, both US and foreign scientists, senior researchers, young investigators, and students.

  2. Evaluation of Preindustrial to Present-day Black Carbon and its Albedo Forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    SciTech Connect

    Lee, Y. H.; Lamarque, J.-F.; Flanner, M. G.; Jiao, C.; Shindell, Drew; Berntsen, T.; Bisiauxs, M.; Cao, J.; Collins, W. J.; Curran, M.; Edwards, R.; Faluvegi, G.; Ghan, Steven J.; Horowitz, L.; McConnell, J.R.; Ming, J.; Myhre, G.; Nagashima, T.; Naik, Vaishali; Rumbold, S.; Skeie, R. B.; Sudo, K.; Takemura, T.; Thevenon, F.; Xu, B.; Yoon, Jin-Ho

    2013-03-05

    As a part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against the observations including 12 ice core records, a long-term surface mass concentrations and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using the NCAR Community Land and Sea-Ice model 4 with prescribed meteorology from 1996-2000, which includes the SNICAR BC-snow model. We evaluated the vertical profile of BC snow concentrations from these offline simulations to using recent BC snowpack measurements. Despite using the same BC emissions, global BC burden differs by approximately a factor of 3 among models due to the differences in aerosol removal parameterizations and simulated meteorology among models; 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However,models agree well on 2.5~3 times increase in the global BC burden from preindustrial to present-day, which matches with the 2.5 times increase in BC emissions. We find a large model diversity at both NH and SH high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC mass concentrations well in Europe and North America except at Jungfrauch and Ispra. However, the models fail to capture the Arctic BC seasonality due tosevere underestimations during winter and spring. Compared to recent snowpack measurements, the simulated vertically resolved BC snow concentrations are, on average, within a factor of 2-3 of observations except for Greenland and Arctic Ocean. However, model and observation differ widely due to missing interannual variations in emissions and possibly due to the choice of the prescribed meteorology period (i.e., 1996-2000).

  3. Measurement and modelling of air pollution and atmospheric chemistry in the U.K. West Midlands conurbation: overview of the PUMA Consortium project.

    PubMed

    Harrison, R M; Yin, J; Tilling, R M; Cai, X; Seakins, P W; Hopkins, J R; Lansley, D L; Lewis, A C; Hunter, M C; Heard, D E; Carpenter, L J; Creasey, D J; Lee, J D; Pilling, M J; Carslaw, N; Emmerson, K M; Redington, A; Derwent, R G; Ryall, D; Mills, G; Penkett, S A

    2006-05-01

    The PUMA (Pollution of the Urban Midlands Atmosphere) Consortium project involved intensive measurement campaigns in the Summer of 1999 and Winter of 1999/2000, respectively, in which a wide variety of air pollutants were measured in the UK West Midlands conurbation including detailed speciation of VOCs and major component analysis of aerosol. Measurements of the OH and HO2 free radicals by the FAGE technique demonstrated that winter concentrations of OH were approximately half of those measured during the summer despite a factor of 15 reduction in production through the photolysis of ozone. Detailed box modelling of the fast reaction chemistry revealed the decomposition of Criegee intermediates formed from ozone-alkene reactions to be responsible for the majority of the formation of hydroxyl in both the summer and winter campaigns, in contrast to earlier rural measurements in which ozone photolysis was predominant. The main sinks for hydroxyl are reactions with NO2, alkenes and oxygenates. Concentrations of the more stable hydrocarbons were found to be relatively invariant across the conurbation, but the impacts of photochemistry were evident through analyses of formaldehyde which showed the majority to be photochemical in origin as opposed to emitted from road traffic. Measurements on the upwind and downwind boundaries of the conurbation revealed substantial enhancements in NOx as a result of emissions within the conurbation, especially during westerly winds which carried relatively clean air. Using calcium as a tracer for crustal particles, it proved possible to reconstruct aerosol mass from the major chemical components with a fairly high degree of success. The organic to elemental carbon ratios showed a far greater influence of photochemistry in summer than winter, presumably resulting mainly from the greater availability of biogenic precursors during the summer campaign. Two urban airshed models were developed and applied to the conurbation, one Eulerian, the

  4. Introductory lecture: atmospheric chemistry in the Anthropocene.

    PubMed

    Finlayson-Pitts, Barbara J

    2017-08-24

    The term "Anthropocene" was coined by Professor Paul Crutzen in 2000 to describe an unprecedented era in which anthropogenic activities are impacting planet Earth on a global scale. Greatly increased emissions into the atmosphere, reflecting the advent of the Industrial Revolution, have caused significant changes in both the lower and upper atmosphere. Atmospheric reactions of the anthropogenic emissions and of those with biogenic compounds have significant impacts on human health, visibility, climate and weather. Two activities that have had particularly large impacts on the troposphere are fossil fuel combustion and agriculture, both associated with a burgeoning population. Emissions are also changing due to alterations in land use. This paper describes some of the tropospheric chemistry associated with the Anthropocene, with emphasis on areas having large uncertainties. These include heterogeneous chemistry such as those of oxides of nitrogen and the neonicotinoid pesticides, reactions at liquid interfaces, organic oxidations and particle formation, the role of sulfur compounds in the Anthropocene and biogenic-anthropogenic interactions. A clear and quantitative understanding of the connections between emissions, reactions, deposition and atmospheric composition is central to developing appropriate cost-effective strategies for minimizing the impacts of anthropogenic activities. The evolving nature of emissions in the Anthropocene places atmospheric chemistry at the fulcrum of determining human health and welfare in the future.

  5. Photodissociation dynamics and atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Wayne, R. P.

    1993-07-01

    The paper uses data from the literature to explore photodissociation dynamics of molecules possessing three, four, and five atoms, as represented by O3 and CO2, NH3 and C2H2, and CH4, respectively. The results yield many details, even in regard to the disposal of energy into rotation, which have applications to atmospheric problems. For instance, experiments probing the translational energies of the O and the vibrational and rotational distributions in the CO suggest that a spin-forbidden channel operates as it does in ozone photolysis. The data for both O3 and CO2 suggest a relationship between the structure of the parent molecule and the dynamics of dissociation.

  6. Is microbiolgy an alternative route to photochemistry in atmospheric chemistry?

    NASA Astrophysics Data System (ADS)

    Vaitilingom, M.; Parazols, M.; Sancelme, M.; Deguillaume, L.; Mailhot, G.; Delort, A.-M.

    2009-04-01

    Until very recently scientists from atmospheric sciences focussed their studies on physical and chemical phenomena taking place in cloud water phase neglecting the presence of active microorganisms in this medium. For instance, considering atmospheric chemistry, solar light is considered as the predominant catalyser for chemical reactions occurring in the atmosphere. However recent studies show that living and active microorganisms, including bacteria, yeasts and fungi, are present in the atmospheric water phase and could play an active role in chemistry of clouds. Indeed living microorganisms are clearly biocatalysts which could transform organic compounds as an alternative route to photochemistry. The objective of our project is to bring answers to this new scientific question by a multidisciplinary approach involving atmospheric physicists, photochemists and microbiologists. Microorganisms have been isolated and identified in cloud water sampled at the puy de Dôme summit which is an atmospheric observatory and a European referenced site. Laboratory experiments were carried out to evaluate the potential of organic species (carboxylic acids) degradation by the photochemical or microbiological ways. The project was centred on few carboxylic acids among them succinic, acetic, formic and oxalic acids (the most important organic acids in cloud water sampled at Puy de Dôme). Degradation rates were measured during biodegradation alone (Pseudomonas syringae), photochemistry alone (hydrogen peroxide + light) and combing both processed using artificial reconstituted cloud water. Our first results show that the obtained degradation rates are in the range of order.

  7. New insights into martian atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Boxe, C. S.; Francisco, J. S.; Shia, R.-L.; Yung, Y. L.; Nair, H.; Liang, M.-C.; Saiz-Lopez, A.

    2014-11-01

    HOx radicals are produced in the martian atmosphere by the photolysis of water vapor and subsequently participate in catalytic cycles that recycle carbon dioxide (CO2) from its photolysis product carbon monoxide (CO), providing a qualitative explanation for the stability of its atmosphere. Balancing CO2 production and loss based on our current understanding of martian gas-phase chemistry has, however, proven to be difficult. The photolysis of O3 produces O(1D), while oxidation of CO produces HOCO radicals, a new member of the HOx family. The O(1D) quantum yield has recently been updated, which quantifies nonzero quantum yields in the Huggins bands. In Earth's atmosphere HOCO is considered to be unimportant since it is quickly removed by abundant oxygen molecules. The smaller amount of O2 in the Mars' atmosphere causes HOCO's lifetime to be longer in Mars' atmosphere than Earth's (3 × 10-5 s to 1.2 days from Mars's surface to 240 km, respectively). Limited kinetic data on reactions involving HOCO prevented consideration of its reactions directly in atmospheric models. Therefore, the impact of HOCO reactions on martian chemistry is currently unknown. Here, we incorporate new literature rate constants for HOCO chemistry and an updated representation of the O(1D) quantum yield in the Caltech/JPL 1-D photochemical model for Mars' atmosphere. Our simulations exemplify perturbations to NOy, HOx, and COx species, ranging from 5% to 50%. The modified O(1D) quantum yield and new HOCO chemistry cause a 10% decrease and a 50% increase in OH and H2O2 total column abundances, respectively. At low altitudes, HOCO production contributes 5% towards CO2 production. Given recent experimentally-obtained branching ratios for the oxidation of CO, HOCO may contribute up to 70% toward the production of NOy, where HOx and NOy species are enhanced up to a factor 3, which has implications for rethinking the fundamental understanding of NOy, HOx, and CO/CO2 cycling on Mars. Two new reaction

  8. Local Atmospheric Chemistry and Ozone Model (LACOM)

    NASA Astrophysics Data System (ADS)

    Pirjola, Liisa

    2000-12-01

    LACOM (Local Atmospheric Chemistry and Ozone Model) is a chemistry box model that can be applied to teaching and learning atmospheric chemistry at high schools, especially GLOBE (Global Learning and Observations to Benefit the Environment) schools, and at universities. The program code is written in Fortran and can be run on a PC under Microsoft Windows 95 or Windows NT, in MS-DOS prompt or using MS-Excel 97. Commercial graphic programs are used for data analysis. Using LACOM as a tool, students learn about the chemical complexity of the troposphere, the importance of solar radiation and photochemistry, the significant influence of emissions and depositions of gases, and the impact of meteorological parameters. Special attention is paid to tropospheric ozone. LACOM is appropriate for (i) simulating main features of a particular day, (ii) understanding the coupling between individual parameters, and (iii) predicting impacts of environmental problems such as increased pollution and ozone depletion in the lower atmosphere. As input the program needs meteorological data and information about local emissions. For the days simulated students can make environmental observations (e.g., daily minimum and maximum temperatures, and temperature, relative humidity, and cloudiness at noon) as GLOBE schools do continuously and use these data in the simulations.

  9. Preindustrial to present day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Naik, V.; Voulgarakis, A.; Fiore, A. M.; Horowitz, L. W.; Lamarque, J.-F.; Lin, M.; Prather, M. J.; Young, P. J.; Bergmann, D.; Cameron-Smith, P. J.; Cionni, I.; Collins, W. J.; Dalsøren, S. B.; Doherty, R.; Eyring, V.; Faluvegi, G.; Folberth, G. A.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Nagashima, T.; van Noije, T. P. C.; Plummer, D. A.; Righi, M.; Rumbold, S. T.; Skeie, R.; Shindell, D. T.; Stevenson, D. S.; Strode, S.; Sudo, K.; Szopa, S.; Zeng, G.

    2012-11-01

    We have analysed results from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore trends in hydroxyl radical concentration (OH) and methane (CH4) lifetime since preindustrial times (1850) and gain a better understanding of their key drivers. For the present day (2000), the models tend to simulate higher OH abundances in the Northern Hemisphere versus Southern Hemisphere. Evaluation of simulated carbon monoxide concentrations, the primary sink for OH, against observations suggests low biases in the Northern Hemisphere that may contribute to the high north-south OH asymmetry in the models. A comparison of modelled and observed methyl chloroform lifetime suggests that the present day global multi-model mean OH concentration is slightly overestimated. Despite large regional changes, the modelled global mean OH concentration is roughly constant over the past 150 yr, due to concurrent increases in OH sources (humidity, tropospheric ozone, and NOx emissions), together with decreases in stratospheric ozone and increase in tropospheric temperature, compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large intermodel diversity in the sign and magnitude of OH and methane lifetime changes over this period reflects differences in the relative importance of chemical and physical drivers of OH within each model. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH leads to a 4.3 ± 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present day climate change decreased the methane lifetime by about 4 months, representing a negative feedback on the climate system. Further, using a subset of the models, we find that global mean OH increased by 46.4 ± 12.2% in response to preindustrial to present day anthropogenic

  10. Chemistry and evolution of Titan's atmosphere

    NASA Technical Reports Server (NTRS)

    Strobel, D. F.

    1982-01-01

    The chemistry and evolution of Titan's atmosphere are reviewed, in light of the scientific findings from the Voyager mission. It is argued that the present N2 atmosphere may be Titan's initial atmosphere, rather than one photochemically derived from an original NH3 atmosphere. The escape rate of hydrogen from Titan is controlled by photochemical production from hydrocarbons. CH4 is irreversibly converted to less hydrogen-rich hydrocarbons, which over geologic time accumulate on the surface to a layer thickness of about 0.5 km. Magnetospheric electrons interacting with Titan's exosphere may dissociate enough N2 into hot, escaping N atoms to remove about 0.2 of Titan's present atmosphere over geologic time. The energy dissipation of magnetospheric electrons exceeds solar EUV energy deposition in Titan's atmosphere by an order of magnitude, and is the principal driver of nitrogen photochemistry. The environmental conditions in Titan's upper atmosphere are favorable to building up complex molecules, particularly in the north polar cap region.

  11. Chemistry and evolution of Titan's atmosphere

    NASA Technical Reports Server (NTRS)

    Strobel, D. F.

    1982-01-01

    The chemistry and evolution of Titan's atmosphere are reviewed, in light of the scientific findings from the Voyager mission. It is argued that the present N2 atmosphere may be Titan's initial atmosphere, rather than one photochemically derived from an original NH3 atmosphere. The escape rate of hydrogen from Titan is controlled by photochemical production from hydrocarbons. CH4 is irreversibly converted to less hydrogen-rich hydrocarbons, which over geologic time accumulate on the surface to a layer thickness of about 0.5 km. Magnetospheric electrons interacting with Titan's exosphere may dissociate enough N2 into hot, escaping N atoms to remove about 0.2 of Titan's present atmosphere over geologic time. The energy dissipation of magnetospheric electrons exceeds solar EUV energy deposition in Titan's atmosphere by an order of magnitude, and is the principal driver of nitrogen photochemistry. The environmental conditions in Titan's upper atmosphere are favorable to building up complex molecules, particularly in the north polar cap region.

  12. Preindustrial to Present-Day Changes in Tropospheric Hydroxyl Radical and Methane Lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Technical Reports Server (NTRS)

    Naik, V.; Voulgarakis, A.; Fiore, A. M.; Horowitz, L. W.; Lamarque, J.-F.; Lin, M.; Prather, M. J.; Young, P. J.; Bergmann, D.; Cameron-Smith, P. J.; hide

    2013-01-01

    We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the

  13. Preindustrial to present-day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Naik, V.; Voulgarakis, A.; Fiore, A. M.; Horowitz, L. W.; Lamarque, J.-F.; Lin, M.; Prather, M. J.; Young, P. J.; Bergmann, D.; Cameron-Smith, P. J.; Cionni, I.; Collins, W. J.; Dalsøren, S. B.; Doherty, R.; Eyring, V.; Faluvegi, G.; Folberth, G. A.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Nagashima, T.; van Noije, T. P. C.; Plummer, D. A.; Righi, M.; Rumbold, S. T.; Skeie, R.; Shindell, D. T.; Stevenson, D. S.; Strode, S.; Sudo, K.; Szopa, S.; Zeng, G.

    2013-05-01

    We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north-south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change

  14. Atmospheric Prebiotic Chemistry and Organic Hazes

    PubMed Central

    Trainer, Melissa G.

    2013-01-01

    Earth’s atmospheric composition at the time of the origin of life is not known, but it has often been suggested that chemical transformation of reactive species in the atmosphere was a significant source of prebiotic organic molecules. Experimental and theoretical studies over the past half century have shown that atmospheric synthesis can yield molecules such as amino acids and nucleobases, but these processes are very sensitive to gas composition and energy source. Abiotic synthesis of organic molecules is more productive in reduced atmospheres, yet the primitive Earth may not have been as reducing as earlier workers assumed, and recent research has reflected this shift in thinking. This work provides a survey of the range of chemical products that can be produced given a set of atmospheric conditions, with a particular focus on recent reports. Intertwined with the discussion of atmospheric synthesis is the consideration of an organic haze layer, which has been suggested as a possible ultraviolet shield on the anoxic early Earth. Since such a haze layer – if formed – would serve as a reservoir for organic molecules, the chemical composition of the aerosol should be closely examined. The results highlighted here show that a variety of products can be formed in mildly reducing or even neutral atmospheres, demonstrating that contributions of atmospheric synthesis to the organic inventory on early Earth should not be discounted. This review intends to bridge current knowledge of the range of possible atmospheric conditions in the prebiotic environment and pathways for synthesis under such conditions by examining the possible products of organic chemistry in the early atmosphere. PMID:24143126

  15. Atmospheric Prebiotic Chemistry and Organic Hazes

    NASA Technical Reports Server (NTRS)

    Trainer, Melissa G.

    2012-01-01

    Earth's atmospheric composition at the time of the origin of life is not known, but it has often been suggested that chemical transformation of reactive species in the atmosphere was a significant source of pre biotic organic molecules. Experimental and theoretical studies over the past half century have shown that atmospheric synthesis can yield molecules such as amino acids and nucleobases, but these processes are very sensitive to gas composition and energy source. Abiotic synthesis of organic molecules is more productive in reduced atmospheres, yet the primitive Earth may not have been as reducing as earlier workers assumed, and recent research has reflected this shift in thinking. This work provides a survey of the range of chemical products that can be produced given a set of atmospheric conditions, with a particular focus on recent reports. Intertwined with the discussion of atmospheric synthesis is the consideration of an organic haze layer, which has been suggested as a possible ultraviolet shield on the anoxic early Earth. Since such a haze layer - if formed - would serve as a reservoir for organic molecules, the chemical composition of the aerosol should be closely examined. The results highlighted here show that a variety of products can be formed in mildly reducing or even neutral atmospheres, demonstrating that contributions of atmospheric synthesis to the organic inventory on early Earth should not be discounted. This review intends to bridge current knowledge of the range of possible atmospheric conditions in the prebiotic environment and pathways for synthesis under such conditions by examining the possible products of organic chemistry in the early atmosphere.

  16. Atmospheric Prebiotic Chemistry and Organic Hazes.

    PubMed

    Trainer, Melissa G

    2013-08-01

    Earth's atmospheric composition at the time of the origin of life is not known, but it has often been suggested that chemical transformation of reactive species in the atmosphere was a significant source of prebiotic organic molecules. Experimental and theoretical studies over the past half century have shown that atmospheric synthesis can yield molecules such as amino acids and nucleobases, but these processes are very sensitive to gas composition and energy source. Abiotic synthesis of organic molecules is more productive in reduced atmospheres, yet the primitive Earth may not have been as reducing as earlier workers assumed, and recent research has reflected this shift in thinking. This work provides a survey of the range of chemical products that can be produced given a set of atmospheric conditions, with a particular focus on recent reports. Intertwined with the discussion of atmospheric synthesis is the consideration of an organic haze layer, which has been suggested as a possible ultraviolet shield on the anoxic early Earth. Since such a haze layer - if formed - would serve as a reservoir for organic molecules, the chemical composition of the aerosol should be closely examined. The results highlighted here show that a variety of products can be formed in mildly reducing or even neutral atmospheres, demonstrating that contributions of atmospheric synthesis to the organic inventory on early Earth should not be discounted. This review intends to bridge current knowledge of the range of possible atmospheric conditions in the prebiotic environment and pathways for synthesis under such conditions by examining the possible products of organic chemistry in the early atmosphere.

  17. Submillimeter Planetary Atmospheric Chemistry Exploration Sounder

    NASA Technical Reports Server (NTRS)

    Schlecht, Erich T.; Allen, Mark A.; Gill, John J.; Choonsup, Lee; Lin, Robert H.; Sin, Seth; Mehdi, Imran; Siegel, Peter H.; Maestrini, Alain

    2013-01-01

    Planetary Atmospheric Chemistry Exploration Sounder (SPACES), a high-sensitivity laboratory breadboard for a spectrometer targeted at orbital planetary atmospheric analysis. The frequency range is 520 to 590 GHz, with a target noise temperature sensitivity of 2,500 K for detecting water, sulfur compounds, carbon compounds, and other atmospheric constituents. SPACES is a prototype for a powerful tool for the exploration of the chemistry and dynamics of any planetary atmosphere. It is fundamentally a single-pixel receiver for spectral signals emitted by the relevant constituents, intended to be fed by a fixed or movable telescope/antenna. Its front-end sensor translates the received signal down to the 100-MHz range where it can be digitized and the data transferred to a spectrum analyzer for processing, spectrum generation, and accumulation. The individual microwave and submillimeter wave components (mixers, LO high-powered amplifiers, and multipliers) of SPACES were developed in cooperation with other programs, although with this type of instrument in mind. Compared to previous planetary and Earth science instruments, its broad bandwidth (approx. =.13%) and rapid tunability (approx. =.10 ms) are new developments only made possible recently by the advancement in submillimeter circuit design and processing at JPL.

  18. Chemistry and spectroscopy of the Jovian atmosphere

    NASA Technical Reports Server (NTRS)

    Prinn, R. G.; Owen, T.

    1976-01-01

    A comprehensive review is given of the chemistry and spectroscopic studies of the Jovian atmosphere. Thermochemical equilibrium models for determining atmospheric composition are considered along with possible disequilibrating processes, and studies of the photochemistry of H2, CH4, NH3, H2S, and PH3 using the modeling methods are summarized. It is shown that photodissociation and advection are the major disequilibrating processes in Jupiter's atmosphere, that lightning and charged-particle bombardment are relatively minor factors in the planet's bulk chemistry, and that the existence of living organisms on the planet is highly improbable. Spectroscopic investigations of Jupiter are discussed, emphasizing recent observations of absorption bands due to CH4, NH3, H2, He, and D. Spectroscopic abundance determinations are examined for H2, HD, CH4, CH3D, NH3, C2H6, C2H2, and PH3. Upper limits are given for the abundances of several unobserved gases in the visible atmosphere, including H2S, HCl, SiH4, benzene, purines, pyrimidines, and their derivatives.

  19. Chemistry and spectroscopy of the Jovian atmosphere

    NASA Technical Reports Server (NTRS)

    Prinn, R. G.; Owen, T.

    1976-01-01

    A comprehensive review is given of the chemistry and spectroscopic studies of the Jovian atmosphere. Thermochemical equilibrium models for determining atmospheric composition are considered along with possible disequilibrating processes, and studies of the photochemistry of H2, CH4, NH3, H2S, and PH3 using the modeling methods are summarized. It is shown that photodissociation and advection are the major disequilibrating processes in Jupiter's atmosphere, that lightning and charged-particle bombardment are relatively minor factors in the planet's bulk chemistry, and that the existence of living organisms on the planet is highly improbable. Spectroscopic investigations of Jupiter are discussed, emphasizing recent observations of absorption bands due to CH4, NH3, H2, He, and D. Spectroscopic abundance determinations are examined for H2, HD, CH4, CH3D, NH3, C2H6, C2H2, and PH3. Upper limits are given for the abundances of several unobserved gases in the visible atmosphere, including H2S, HCl, SiH4, benzene, purines, pyrimidines, and their derivatives.

  20. Carbon Monoxide Affecting Planetary Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    He, Chao; Horst, Sarah

    2016-10-01

    Atmospheric hazes are present in a range of solar system and extrasolar planetary atmospheres, and organic hazes, such as that in Titan's atmosphere, could be a source of prebiotic molecules.1 However, the chemistry occurring in planetary atmospheres and the resulting chemical structures are still not clear. Numerous experimental simulations2 have been carried out in the laboratory to understand the chemistry in N2/CH4 atmospheres, but very few simulations4 have included CO in their initial gas mixtures, which is an important component in many N2/CH4 atmospheres including Titan, Triton, and Pluto.3 Here we have conducted a series of atmosphere simulation experiments using AC glow discharge (cold plasma) as energy source to irradiate reactions in gas mixtures of CO, CH4, and N2 with a range of CO mixing ratios (from 0, 0.05%, 0.2%, 0.5%, 1%, 2.5%, to 5%) at low temperature (~100 K). Gas phase products are monitored during the reaction by quadrupole mass spectrometer (MS), and solid phase products are analyzed by solution-state nuclear magnetic resonance spectroscopy (NMR). MS results show that with the increase of CO in the initial gases, the production of nitrogenous organic molecules increases while the production of hydrogen molecules decreases in the gas phase. NMR measurements of the solid phase products show that with the increase of CO, hydrogen atoms bonded to nitrogen or oxygen in unsaturated structures increase while those bonded to saturated carbon decrease, which means more unsaturated species and less saturated species formed with the addition of CO. MS and NMR results demonstrate that the inclusion of CO affects the compositions of both gas and solid phase products, indicating that CO has an important impact on the chemistry occurring in our experiments and probably in planetary atmospheres.1. Hörst, S. M., et al. 2012, AsBio, 12, 8092. Cable, M. L., et al. 2012, Chem. Rev., 112, 18823. Lutz, B. L., et al. 1983, Sci, 220, 1374; Greaves, J. S., et al

  1. Atmospheric Chemistry of Micrometeoritic Organic Compounds

    NASA Technical Reports Server (NTRS)

    Kress, M. E.; Belle, C. L.; Pevyhouse, A. R.; Iraci, L. T.

    2011-01-01

    Micrometeorites approx.100 m in diameter deliver most of the Earth s annual accumulation of extraterrestrial material. These small particles are so strongly heated upon atmospheric entry that most of their volatile content is vaporized. Here we present preliminary results from two sets of experiments to investigate the fate of the organic fraction of micrometeorites. In the first set of experiments, 300 m particles of a CM carbonaceous chondrite were subject to flash pyrolysis, simulating atmospheric entry. In addition to CO and CO2, many organic compounds were released, including functionalized benzenes, hydrocarbons, and small polycyclic aromatic hydrocarbons. In the second set of experiments, we subjected two of these compounds to conditions that simulate the heterogeneous chemistry of Earth s upper atmosphere. We find evidence that meteor-derived compounds can follow reaction pathways leading to the formation of more complex organic compounds.

  2. On the chemistry of Jupiter's upper atmosphere

    USGS Publications Warehouse

    Saslaw, W.C.; Wildey, R.L.

    1967-01-01

    We conduct a first investigation into the ion-molecule chemistry of the upper Jovian atmosphere. Experimental results show that intense ultraviolet radiation reacts with the constituents of the Jovian atmosphere to produce C2H4, C2H6, C3H8, and higher polymers. The general procedure for calculating both equilibrium and nonequilibrium abundances of these products is formulated and applied to the case of the surface passage of a satellite shadow. A specific example is made of ethylene, for which an analytical approximation gives 1010 molecules in an atmospheric column of 1 cm2 cross section after a very rapid rise to equilibrium. Such a concentration of ethylene does not substantially affect the infrared radiation in the shadow. ?? 1967.

  3. Atmospheric Aerosols: Clouds, Chemistry, and Climate.

    PubMed

    McNeill, V Faye

    2017-06-07

    Although too small to be seen with the human eye, atmospheric particulate matter has major impacts on the world around us, from our health to global climate. Understanding the sources, properties, and transformations of these particles in the atmosphere is among the major challenges in air quality and climate research today. Significant progress has been made over the past two decades in understanding atmospheric aerosol chemistry and its connections to climate. Advances in technology for characterizing aerosol chemical composition and physical properties have enabled rapid discovery in this area. This article reviews fundamental concepts and recent developments surrounding ambient aerosols, their chemical composition and sources, light-absorbing aerosols, aerosols and cloud formation, and aerosol-based solar radiation management (also known as solar geoengineering).

  4. Trace Element Chemistry in Urban Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Farhana, B.; Husain, L.

    2006-12-01

    Unlike in the United States, the concentration of trace elements in urban air is still high enough in South Asian cities to study the impact of trace elements on climate and human health. Hence, continuous sampling of PM2.5 (particulate matter of <2.5 μm aerodynamic diameter)was carried out using low volume sampler in winter (2005-2006) in Lahore, the second largest city of Pakistan, which is highly impacted by urban and agricultural emissions and has remained unexplored in terms of atmospheric chemistry. Aerosols collected on this campaign are likely to carry the signatures of emissions from Afghanistan, North and Central Pakistan, North India in addition to the local pollution sources. During sampling from December 2005 to January 2006, it was possible to collect several samples during brief fog episodes. Samples were analyzed for 25 elements (Be, Na, Mg, Al, K, Ca, Ti, V, Cr, Mn, Fe, Co, Ni, Zn, As, Se, Sr, Mo, Ag, Cd, Sn, Sb, Ba, Tl and Pb) using inductively coupled plasma mass spectrometry. High pollutant concentrations were observed throughout the study, for instance, Cr concentrations up to 1.4 μgm-3, As, 135 ngm-3, Cd, 93 ngm-3, Sn, 988 ngm-3 and Sb, 157 ngm-3. Pb and Zn concentrations respectively up to 12 and 48 μgm-3 were observed. Calculation of enrichment factor and crustal correction illustrate the attribution of Cr, Co, Ni, Zn, As, Se, Mo, Ag Cd, Sn, Sb, Tl and Pb to non-crustal sources. Air parcel back trajectories, interelemental relationships and meteorological observations have been used to explain the sources and the impacts of fog chemistry and mixing heights on atmospheric processing of trace elements in PM2.5. Atmospheric stagnation appeared to be one of factors causing episodic high concentrations. Crustal correction and interelemental relationships apparently suggest the emissions from coal and oil combustion, industrial processes, building construction sites and biomass burning as the prime role players in the atmospheric pollution in

  5. Global atmospheric chemistry - which air matters

    NASA Astrophysics Data System (ADS)

    Prather, Michael J.; Zhu, Xin; Flynn, Clare M.; Strode, Sarah A.; Rodriguez, Jose M.; Steenrod, Stephen D.; Liu, Junhua; Lamarque, Jean-Francois; Fiore, Arlene M.; Horowitz, Larry W.; Mao, Jingqiu; Murray, Lee T.; Shindell, Drew T.; Wofsy, Steven C.

    2017-07-01

    An approach for analysis and modeling of global atmospheric chemistry is developed for application to measurements that provide a tropospheric climatology of those heterogeneously distributed, reactive species that control the loss of methane and the production and loss of ozone. We identify key species (e.g., O3, NOx, HNO3, HNO4, C2H3NO5, H2O, HOOH, CH3OOH, HCHO, CO, CH4, C2H6, acetaldehyde, acetone) and presume that they can be measured simultaneously in air parcels on the scale of a few km horizontally and a few tenths of a km vertically. As a first step, six global models have prepared such climatologies sampled at the modeled resolution for August with emphasis on the vast central Pacific Ocean basin. Objectives of this paper are to identify and characterize differences in model-generated reactivities as well as species covariances that could readily be discriminated with an unbiased climatology. A primary tool is comparison of multidimensional probability densities of key species weighted by the mass of such parcels or frequency of occurrence as well as by the reactivity of the parcels with respect to methane and ozone. The reactivity-weighted probabilities tell us which parcels matter in this case, and this method shows skill in differentiating among the models' chemistry. Testing 100 km scale models with 2 km measurements using these tools also addresses a core question about model resolution and whether fine-scale atmospheric structures matter to the overall ozone and methane budget. A new method enabling these six global chemistry-climate models to ingest an externally sourced climatology and then compute air parcel reactivity is demonstrated. Such an objective climatology containing these key species is anticipated from the NASA Atmospheric Tomography (ATom) aircraft mission (2015-2020), executing profiles over the Pacific and Atlantic Ocean basins. This modeling study addresses a core part of the design of ATom.

  6. Nonlinear Kalman filters for atmospheric chemistry models

    NASA Astrophysics Data System (ADS)

    Segers, Arjo; Heemink, Arnold; Verlaan, Martin; van Loon, Maarten

    Four non linear Kaiman filter implementations are applied to an atmospheric chemistry model. The type of non linear dynamics present in such a model complicates an accurate forecast of the state of the system. Therefore, different non linear forecast methods are applied as part of the Reduced Rank Square Root formulation of the Kaiman filter, either based on ensemble statistics or on linearizations. A filter based on minimal exact sampling proves to produce an accurate forecast of state and covariance, using only a few model evaluations. Ensemble statistics are able to produce even more accurate results, but with the cost of at least a double amount of computation time.

  7. Atmospheric chemistry - Response to human influence

    NASA Technical Reports Server (NTRS)

    Logan, J. A.; Prather, M. J.; Wofsy, S. G.; Mcelroy, M. B.

    1978-01-01

    Global atmospheric chemistry is surveyed, and the agreement of models with observed distribution of gases is considered. The influence of human perturbations due to combustion, agriculture, and chloro-carbon releases is examined with emphasis on ozone. Effects of combustion-related releases of CO on the abundances of other gases as well as possible effects of CO on tropospheric ozone are discussed. Other topics include the contribution of the chlorocarbon industry to stratospheric chloride and the recombination of nitrogen fixed by agriculture and combustion.

  8. THE ADVANCED CHEMISTRY BASINS PROJECT

    SciTech Connect

    William Goddard; Peter Meulbroek; Yongchun Tang; Lawrence Cathles III

    2004-04-05

    In the next decades, oil exploration by majors and independents will increasingly be in remote, inaccessible areas, or in areas where there has been extensive shallow exploration but deeper exploration potential may remain; areas where the collection of data is expensive, difficult, or even impossible, and where the most efficient use of existing data can drive the economics of the target. The ability to read hydrocarbon chemistry in terms of subsurface migration processes by relating it to the evolution of the basin and fluid migration is perhaps the single technological capability that could most improve our ability to explore effectively because it would allow us to use a vast store of existing or easily collected chemical data to determine the major migration pathways in a basin and to determine if there is deep exploration potential. To this end a the DOE funded a joint effort between California Institute of Technology, Cornell University, and GeoGroup Inc. to assemble a representative set of maturity and maturation kinetic models and develop an advanced basin model able to predict the chemistry of hydrocarbons in a basin from this input data. The four year project is now completed and has produced set of public domain maturity indicator and maturation kinetic data set, an oil chemistry and flash calculation tool operable under Excel, and a user friendly, graphically intuitive basin model that uses this data and flash tool, operates on a PC, and simulates hydrocarbon generation and migration and the chemical changes that can occur during migration (such as phase separation and gas washing). The DOE Advanced Chemistry Basin Model includes a number of new methods that represent advances over current technology. The model is built around the concept of handling arbitrarily detailed chemical composition of fluids in a robust finite-element 2-D grid. There are three themes on which the model focuses: chemical kinetic and equilibrium reaction parameters, chemical

  9. Composition and chemistry of Saturn's atmosphere

    NASA Technical Reports Server (NTRS)

    Prinn, R. G.; Larson, H. P.; Caldwell, J. J.; Gautier, D.

    1984-01-01

    A comprehensive discussion and review is presented of the chemistry and composition of Saturn as determined by earth-based, earth-orbital, and Voyager 1 and 2 spectroscopic observations. The observations imply that there are important differences between the actual composition of Saturn's atmosphere and that predicted for a homogeneous solar-composition planet. The H2, He, Ch4, NH3, and PH3 volume mixing ratios differ from the expected solar composition ratios, implying that during its formation Saturn accreted a significant amount of ice and rock. The depletion of He in the visible atmosphere suggests that this element has preferentially differentiated toward the center of the planet. The D to H ratio is similar to that on Jupiter and has important cosmological implications. Volume mixing ratios for C2H6 and C2H2 are consistent with the theoretically expected photochemical sources for these gases.

  10. Composition and chemistry of Saturn's atmosphere

    NASA Technical Reports Server (NTRS)

    Prinn, R. G.; Larson, H. P.; Caldwell, J. J.; Gautier, D.

    1984-01-01

    A comprehensive discussion and review is presented of the chemistry and composition of Saturn as determined by earth-based, earth-orbital, and Voyager 1 and 2 spectroscopic observations. The observations imply that there are important differences between the actual composition of Saturn's atmosphere and that predicted for a homogeneous solar-composition planet. The H2, He, Ch4, NH3, and PH3 volume mixing ratios differ from the expected solar composition ratios, implying that during its formation Saturn accreted a significant amount of ice and rock. The depletion of He in the visible atmosphere suggests that this element has preferentially differentiated toward the center of the planet. The D to H ratio is similar to that on Jupiter and has important cosmological implications. Volume mixing ratios for C2H6 and C2H2 are consistent with the theoretically expected photochemical sources for these gases.

  11. Chapter 15 Elementary Processes in Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Maciel, Glauciete S.; Cappelletti, David; Grossi, Gaia; Pirani, Fernando; Aquilanti, Vincenzo

    The present article provides an account of recent progress in the use of quantum mechanical tools for understanding structure and processes for systems of relevance in atmospheric chemistry. The focus is on problems triggered by experimental activity in this laboratory on investigations of intermolecular interactions by molecular beam scattering. Regarding the major components of the atmosphere, results are summarized on dimers (N2-N2, O2-O2, N2-O2) where experimental and phenomenogically derived potential energy surfaces have been used to compute quantum mechanically the intermolecular clusters dynamics. Rovibrational levels and wave functions are obtained, for perspective use in atmospheric modelling, specifically of radiative absorption of weakly bound complexes. Further work has involved interactions of paramount importance, those of water, for which state-of-the-art quantum chemical calculations for its complexes with rare gases yield complementary information on the interaction (specifically the anisotropies) with respect to molecular beam scattering experiments that measure essentially the isotropic forces. Similar approaches and results have been pursued and obtained for H2S. Stimulated in part by the interesting problem of large amplitude vibrations, such as the chirality change transitions associated with the torsional motions around OO and SS bonds, a systematic series of quantum chemical studies has been undertaken on systems that play also roles in the photochemistry of the minor components of the atmosphere. They are H2O2, H2S2 and several molecules obtained by substitutions of the hydrogens by alkyl groups or halogens. Quantum chemistry is shown to have reached the stage of resolving many previously controversial features regarding these series of molecules (dipole moment, equilibrium geometries, heights of barriers for torsion), which are crucial for intramolecular dynamics. Quantum dynamics calculations are also performed to compute torsional

  12. Evaluation of preindustrial to present-day black carbon and its albedo forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Technical Reports Server (NTRS)

    Lee, Y. H.; Lamarque, J.-F.; Flanner, M. G.; Jiao, C.; Shindell, D. T.; Bernsten, T.; Bisiaux, M. M.; Cao, J.; Collins, W. J.; Curran, M.; hide

    2013-01-01

    As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations, and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996-2000. We evaluate the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5-3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period.We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2-3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. For the ice core evaluation, models tend to adequately capture both the observed temporal trends and the magnitudes at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores

  13. Evaluation of preindustrial to present-day black carbon and its albedo forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Lamarque, J.-F.; Flanner, M. G.; Jiao, C.; Shindell, D. T.; Berntsen, T.; Bisiaux, M. M.; Cao, J.; Collins, W. J.; Curran, M.; Edwards, R.; Faluvegi, G.; Ghan, S.; Horowitz, L. W.; McConnell, J. R.; Ming, J.; Myhre, G.; Nagashima, T.; Naik, V.; Rumbold, S. T.; Skeie, R. B.; Sudo, K.; Takemura, T.; Thevenon, F.; Xu, B.; Yoon, J.-H.

    2013-03-01

    As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations, and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996-2000. We evaluate the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5-3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period. We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2-3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. For the ice core evaluation, models tend to adequately capture both the observed temporal trends and the magnitudes at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores

  14. Evaluation of preindustrial to present-day black carbon and its albedo forcing from ACCMIP (Atmospheric Chemistry and Climate Model Intercomparison Project)

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Lamarque, J.-F.; Flanner, M. G.; Jiao, C.; Shindell, D. T.; Berntsen, T.; Bisiaux, M. M.; Cao, J.; Collins, W. J.; Curran, M.; Edwards, R.; Faluvegi, G.; Ghan, S.; Horowitz, L. W.; McConnell, J. R.; Myhre, G.; Nagashima, T.; Naik, V.; Rumbold, S. T.; Skeie, R. B.; Sudo, K.; Takemura, T.; Thevenon, F.

    2012-08-01

    As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996-2000. We evaluated the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5-3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period. We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Jungfraujoch and Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2-3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. For the ice core evaluation, models tend to capture both the observed temporal trends and the magnitudes well at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice-core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice

  15. Spectroscopic Studies of Atmospheric Aerosol Chemistry

    NASA Astrophysics Data System (ADS)

    Wamsley, R.; Leather, K.; Horn, A. B.; Percival, C.

    2008-12-01

    Particles are ubiquitous in the troposphere and are involved in chemical and physical processes affecting the composition of the atmosphere, climate, cloud albedo and human health (Finlayson-Pitts and Pitts, 2000). Organic species, such as alcohols, carboxylic acids, ketones, aldehydes, aromatics, alkenes and alkanes, originate both from anthropogenic and natural sources and comprise a large component of atmospheric particles. Gas-phase species, such as ozone, can oxidize these organics, changing the particle's oxygen-to carbon ratio and potentially altering its hygroscopicity, viscosity, morphology and reactivity. One reaction in particular, that between ozone and oleic acid, has been the focus of several recent studies and extensively researched by Ziemann (2005). Oleic acid reacts readily with ozone and has a low vapor pressure making this reaction convenient to study in the laboratory and has become the benchmark for studying heterogeneous reactions representing the oxidative processing of atmospheric organic aerosols. A critical source of uncertainty in reactivity estimates is a lack of understanding of the mechanism through which some VOCs are oxidized. This knowledge gap is especially critical for aromatic compounds. Because the intermediate reaction steps and products of aromatics oxidation are unknown, chemical mechanisms incorporate parameters estimated from environmental chamber experiments to represent their overall contribution to ozone formation, e.g. Volkamer et al. ( 2006). Previous studies of uncertainties in incremental reactivity estimates for VOCs found that the representation of aromatics chemistry contributed significantly to the estimated 40 - 50% uncertainties in the incremental reactivities of common aromatic compounds Carter et al. (2002). This study shows development of an effective IR method that can monitor the reaction and hence obtain the kinetics of the ozonolysis of an aromatic compound in the aerosol phase. The development of such

  16. Coupled Atmospheric Chemistry Schemes for Modeling Regional and Global Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Saunders, E.; Stockwell, W. R.

    2016-12-01

    Atmospheric chemistry models require chemical reaction mechanisms to simulate the production of air pollution. GACM (Global Atmospheric Chemistry Mechanism) is intended for use in global scale atmospheric chemistry models to provide chemical boundary conditions for regional scale simulations by models such as CMAQ. GACM includes additional chemistry for marine environments while reducing its treatment of the chemistry needed for highly polluted urban regions. This keeps GACM's size small enough to allow it to be used efficiently in global models. GACM's chemistry of volatile organic compounds (VOC) is highly compatible with the VOC chemistry in RACM2 allowing a global model with GACM to provide VOC boundary conditions to a regional scale model with RACM2 with reduced error. The GACM-RACM2 system of mechanisms should yield more accurate forecasts by regional air quality models such as CMAQ. Chemical box models coupled with the regional and global atmospheric chemistry mechanisms (RACM2 & GACM) will be used to make simulations of tropospheric ozone, nitric oxides, and volatile organic compounds that are produced in regional and global domains. The simulations will focus on the Los Angeles' South Coast Air Basin (SoCAB) where the Pacific Ocean meets a highly polluted urban area. These two mechanisms will be compared on the basis of simulated ozone concentrations over this marine-urban region. Simulations made with the more established RACM2 will be compared with simulations made with the newer GACM. In addition WRF-Chem will be used to simulate how RACM2 will produce regional simulations of tropospheric ozone and NOx, which can be further, analyzed for air quality impacts. Both the regional and global model in WRF-Chem will be used to predict how the concentrations of ozone and nitrogen oxides change over land and ocean. The air quality model simulation results will be applied to EPA's BenMAP-CE (Environmental Benefits Mapping & Analysis Program-Community Edition

  17. Ion Chemistry in Atmospheric and Astrophysical Plasmas

    NASA Technical Reports Server (NTRS)

    Dalgarno, A.; Fox, J. L.

    1994-01-01

    There are many differences and also remarkable similarities between the ion chemistry and physics of planetary ionospheres and the ion chemistry and physics of astronomical environments beyond the solar system. In the early Universe, an expanded cooling gas of hydrogen and helium was embedded in the cosmic background radiation field and ionized by it. As the Universe cooled by adiabatic expansion, recombination occurred and molecular formation was driven by catalytic reactions involving the relict electrons and protons. Similar chemical processes are effective in the ionized zones of gaseous and planetary nebulae and in stellar winds where the ionization is due to radiation from the central stars, in the envelopes of supernovae where the ionization is initiated by the deposition of gamma-rays, in dissociative shocks where the ionization arises from electron impacts in a hot gas and in quasar broad-line region clouds where the quasar is responsible for the ionization. At high altitudes in the atmospheres of the Jovian planets, the main constituents are hydrogen and helium and the ion chemistry and physics is determined by the same processes, the source of the ionization being solar ultraviolet radiation and cosmic rays. After the collapse of the first distinct astronomical entities to emerge from the uniform flow, heavy elements were created by nuclear burning in the cores of the collapsed objects and distributed throughout the Universe by winds and explosions. The chemistry and physics became more complicated. Over 90 distinct molecular species have been identified in interstellar clouds where they are ionized globally by cosmic ray impacts and locally by radiation and shocks associated with star formation and evolution. Complex molecules have also been found in circumstellar shells of evolved stars. At intermediate and low altitudes in the Jovian atmospheres, the ion chemistry is complicated by the increasing abundance of heavy elements such as carbon, and an

  18. Steam Atmosphere — Magma Ocean Chemistry on the Early Earth

    NASA Astrophysics Data System (ADS)

    Fegley, B.; Lodders, K.

    2016-08-01

    We use experimental data from the literature to calculate chemistry of the steam atmosphere — magma ocean system on the early Earth. Our results show partitioning of rocky elements into the steam atmosphere.

  19. Chamber studies of atmospheric iodine chemistry

    NASA Astrophysics Data System (ADS)

    Buxmann, J.; Nájera, J.; Schmitt, S.; Bleicher, S.; Pöhler, D.; Horbanski, M.; Platt, U.; Zetzsch, C.; Bloss, W. J.

    2012-12-01

    Iodine chemistry has been shown to occur through much of the marine boundary layer (MBL). It leads to significant impacts upon atmospheric oxidising capacity, ozone levels and particle number concentration; however, there are major uncertainties in our knowledge of the iodine chemical reaction system, which limit our ability to accurately quantify these impacts using atmospheric models. In this work we report the results of novel atmospheric simulation chamber experiments, to study aspects of the fast gas-phase inorganic iodine oxide chemistry. We consider two specific issues here: First, in the presence of moderate levels of NO2, most current models predict that most active iodine should exist as INO3 (whose lifetime is controlled primarily by photolysis) and that levels of IO and OIO should be minimal. This is in contrast to observations from recent field measurements from semi-polluted coastal MBL locations which find significant levels of IO in the presence of NOx. Explanations include possible reactions of INO3 with I or O3 regenerating IO, or errors in the INO3 photochemical parameters. Second, while ozone loss is almost universally cited as a reason to study atmospheric iodine chemistry, calculations of the actual ozone destruction rate which results from a given iodine source term are rather uncertain - as we do not have quantitative understanding of the fate of the many potential iodine oxide species formed. This limits our ability to predict the steady state IO levels which will exist in equilibrium with a given iodine source term, and the resulting ozone loss rate. Recent field measurements in the MBL struggle to reconcile the observed IO with the measured iodine sources - indicating that additional sources exist, or alternatively that the model representation of the gas-phase iodine sink via higher iodine oxides is incorrect. We report the results from experiments performed in a 3.5 m3 indoor PTFE atmospheric simulation chamber located at Bay

  20. Technique for atmospheric rate chemistry calculations. [of SST exhaust

    NASA Technical Reports Server (NTRS)

    Matloff, G. L.

    1976-01-01

    The possibility that predictions of atmospheric photochemistry/transport models are sensitive to uncertainties in reaction rates and other inputs stresses the need for rapid numerical integration schemes in rate photochemistry problems. Reducing the computational burden has a major merit in facilitating sensitivity studies to assess the effect of uncertainties on predicted ozone diminutions from NOx (NO + NO2) in the exhaust plume of SST engines. The paper discusses the validity of an algorithmic approach to integration of rate chemistry problems in combustion, developed by Rubel and Baronti for an approximate calculation of the production rate of the i-th chemical species involved. An analysis of two projected SST engines confirms the validity of the proposed algorithm. Because of the relative arithmetical simplicity, it may be easier to treat diffusion rate chemistry calculations using the Rubel and Baronti approximation than would be possible by other approaches.

  1. Atmospheric chemistry of methylglyoxal. Final report

    SciTech Connect

    Orlando, J.; Tyndall, G.; Staffelbach, T.; Cantrell, C.; Shetter, R.

    1993-06-01

    The purpose of the study is to determine, through a set of laboratory experiments, the fate of methylglyoxal (CH3COCHO) in the troposphere, Methylglyoxal is an oxidation product of numerous non-methane hydrocarbons (NMHCs), including isoprene and toluene. Hence, the determination of the contribution of these NMHCs to regional ozone production requires a quantitative knowledge of the fate of methylglyoxal. Although it is generally accepted that the two main loss processes for methylglyoxal are photolysis and reaction with OH, large discrepancies or gaps existed in the data base regarding the rate and mechanism of these two processes. The measurements reported here resolve quantitative discrepancies that existed in the literature regarding the UV/visible absorption cross section of methylglyoxal and the rate constant for its reaction with OH, and should provide the necessary kinetic and mechanistic information required to accurately model its atmospheric chemistry.

  2. Atmospheric Chemistry Experiment (ACE) Measurements of Tropospheric and Stratospheric Chemistry and Long-Term Trends

    NASA Technical Reports Server (NTRS)

    Rinsland, Curtis P.; Bernath, Peter; Boone, Chris; Nassar, Ray

    2007-01-01

    We highlight chemistry and trend measurement results from the Atmospheric Chemistry Experiment (ACE) which is providing precise middle troposphere to the lower thermosphere measurements with a 0.02/cm resolution Fourier transform spectrometer covering 750-4400/cm

  3. Atmospheric chemistry of an Antarctic volcanic plume

    NASA Astrophysics Data System (ADS)

    Oppenheimer, Clive; Kyle, Philip; Eisele, Fred; Crawford, Jim; Huey, Greg; Tanner, David; Kim, Saewung; Mauldin, Lee; Blake, Don; Beyersdorf, Andreas; Buhr, Martin; Davis, Doug

    2010-01-01

    We report measurements of the atmospheric plume emitted by Erebus volcano, Antarctica, renowned for its persistent lava lake. The observations were made in December 2005 both at source, with an infrared spectrometer sited on the crater rim, and up to 56 km downwind, using a Twin Otter aircraft; with the two different measurement platforms, plume ages were sampled ranging from <1 min to as long as 9 h. Three species (CO, carbonyl sulfide (OCS), and SO2) were measured from both air and ground. While CO and OCS were conserved in the plume, consistent with their long atmospheric lifetimes, the downwind measurements indicate a SO2/CO ratio about 20% of that observed at the crater rim, suggesting rapid chemical conversion of SO2. The aircraft measurements also identify volcanogenic H2SO4, HNO3 and, recognized for the first time in a volcanic plume, HO2NO2. We did not find NOx in the downwind plume despite previous detection of NO2 above the crater. This suggests that near-source NOx was quickly oxidized to HNO3 and HO2NO2, and probably NO32-(aq), possibly in tandem with the conversion of SO2 to sulfate. These fast processes may have been facilitated by "cloud processing" in the dense plume immediately downwind from the crater. A further striking observation was O3 depletion of up to ˜35% in parts of the downwind plume. This is likely to be due to the presence of reactive halogens (BrO and ClO) formed through heterogeneous processes in the young plume. Our analysis adds to the growing evidence for the tropospheric reactivity of volcanic plumes and shows that Erebus volcano has a significant impact on Antarctic atmospheric chemistry, at least locally in the Southern Ross Sea area.

  4. Atmospheric Chemistry of Acenaphthalene and Acenaphthylene

    NASA Astrophysics Data System (ADS)

    Zhou, S.; Wenger, J. C.

    2009-04-01

    Polycyclic aromatic hydrocarbons (PAHs) are released into the atmosphere as a by-product of combustion processes and have been detected in ambient air at urban locations around the world. In the atmosphere, PAHs containing two and three rings are found predominantly in the gas-phase, whilst those containing six or more rings principally adsorb to particles. PAHs with four or five rings are found in both phases. The gas-phase PAHs can be chemically transformed in the lower troposphere via reaction with hydroxyl (OH) and nitrate (NO3) radicals and ozone. These reactions lead to the formation of a range of oxidation products including phenols, nitro-PAHs and carbonyls, in addition to other pollutants such as ozone and secondary organic aerosol (SOA). Despite their importance, relatively little is known about the atmospheric chemistry of the PAHs, mainly because of the difficulty of working with these compounds and also the variety and complexity of the reaction products formed. Up to now only one kinetic study on the reaction of acenaphthalene and acenaphthylene with OH, NO3 and ozone has been reported in the peer-reviewed literature. In this study, we have determined rate coefficients for the gas-phase reactions of acenaphthalene and acenaphthylene with OH, NO3 and ozone using the relative rate method. The results are compared with previous measurements and used to provide estimates of the tropospheric lifetimes of these compounds. A recently developed denuder-filter sampling technique was used to investigate the gas and particle phase products arising from the photooxidation of the PAHs. Chemical analysis was performed using gas chromatography - mass spectrometry using O-(2,3,4,5,6- pentafluorobenzyl)-hydroxylamine (PFBHA) and pentafluorobenzyl bromide (PFBBr) as derivatizing agents for carbonyls and phenols respectively. The results provide new data on the gas-particle partitioning behavior of the oxidation products and useful information on the products likely to

  5. The Atmospheric Chemistry of Methyl Chavicol (Estragole)

    NASA Astrophysics Data System (ADS)

    Bloss, W. J.; Alam, M. S.; Rickard, A. R.; Hamilton, J. F.; Pereira, K. F.; Camredon, M.; Munoz, A.; Vazquez, M.; Alacreu, P.; Rodenas, M.; Vera, T.

    2012-12-01

    The oxidation of volatile organic compounds (VOCs) leads to formation of ozone and secondary organic aerosols (SOA), with consequences for health, air quality, crop yields, atmospheric chemistry and radiative transfer. It is estimated that ca. 90 % of VOC emissions to the atmosphere originate from biogenic sources (BVOC); such emissions may increase under future climates. Recent field observations have identified Methyl Chavicol ("MC" hereafter, also known as Estragole; 1-allyl-4-methoxybenzene, C10H12O) as a major BVOC above pine forests in the USA [Bouvier-Brown et al., 2009], and within an oil palm plantation in Malaysian Borneo, where it was found that MC could represent the highest single floral contribution of reactive carbon to the atmosphere [Misztal et al., 2010]. Palm oil cultivation, and hence emissions of MC, may be expected to increase with societal food and biofuel demand. We present the results of a series of simulation chamber experiments to assess the atmospheric fate of MC. Experiments were performed in the EUPHORE (European Photoreactor) facility in Valencia, Spain (200 m3 outdoor smog chamber), investigating the degradation of MC by reaction with OH, O3 and NO3. An extensive range of measurement instrumentation was used to monitor precursor and product formation, including stable species (FTIR, PTR-MS, GC-FID and GC-MS), radical intermediates (LIF), inorganic components (NOx, O3, HONO (LOPAP and aerosol production (SMPS) and composition (PILS and filters; analysed offline by LC-MS and FTICR-MS). Experiments were conducted at a range of NOx:VOC ratios, and in the presence and absence of radical (OH) scavenger compounds. This chamber dataset is used to determine the rate constants for reaction of MC with OH, O3 and NO3, the ozonolysis radical yields, and identify the primary degradation products for each initiation route, alongside the aerosol mass yields. Aerosol composition measurements are analysed to identify markers for MC contributions to

  6. Parametric Analyses of Potential Effects on Stratospheric and Tropospheric Ozone Chemistry by a Fleet of Supersonic Business Jets Projected in a 2020 Atmosphere

    NASA Technical Reports Server (NTRS)

    Wey, Chowen (Technical Monitor); Dutta, M.; Patten, K.; Wuebbles, D.

    2004-01-01

    A class of new supersonic aircraft for business purposes is currently under consideration for use starting around 2015 to 2020. These aircraft, which can accommodate about 12 to 13 passengers, will fly at a speed of Mach 1.6 to 2 and are commonly termed as Supersonic Business Jets (SSBJs). A critical issue that needs to be addressed during the conception phase of such aircraft is the potential impact of emissions from such aircraft on the atmosphere especially on stratospheric ozone. Although these SSBJs will be much smaller in size and will have smaller engines than the hypothetical fleets of commercial passenger High Speed Civil Transport (HSCT) aircraft that we have studied previously, they will still emit nitrogen oxides (NOx = NO + NO2), carbon dioxide (CO2), water vapor (H2O) and sulfur, the latter if it is still in the fuel. Thus, it is important to design these SSBJs in a manner so that a projected fleet of these aircraft will not have a significant effect on ozone or on climate. This report analyzes the potential impact of a fleet of SSBJs in a set of parametric analyses that examine the envelope of potential effects on ozone over a range of total fuel burns, emission indices of nitrogen oxides (E.I.(NOx)), and cruise altitudes, using the current version of the UIUC zonally-averaged two-dimensional model of the global atmosphere.

  7. The Atmospheric Chemistry Experiment (ACE): MLT Results

    NASA Astrophysics Data System (ADS)

    Bernath, Peter

    2010-05-01

    ACE (also known as SCISAT) is making a comprehensive set of simultaneous measurements of numerous trace gases, thin clouds, aerosols and temperature by solar occultation from a satellite in low earth orbit. A high inclination (74 degrees) low earth orbit (650 km) gives ACE coverage of tropical, mid-latitudes and polar regions. The primary instrument is a high-resolution (0.02 cm-1) infrared Fourier Transform Spectrometer (FTS) operating from 2 to 13 microns (750-4400 cm-1). ACE was launched by NASA on 12 August 2003 for a nominal 2-year mission; after 6 years on orbit the ACE-FTS performance is still excellent. The first results of ACE have been presented in a special issue of Geophysics Research Letters (http://www.agu.org/journals/ss/ACECHEM1/) in 2005 and recently a special issue on ACE validation has been prepared for Atmospheric Chemistry and Physics (http://www.atmos-chem-phys.net/special_issue114.html) by K. Walker and K. Strong; more information can be found at http://www.ace.uwaterloo.ca. The ACE mission goals were initially focussed mainly on polar ozone chemistry, and more recently have shifted more to the troposphere where organic pollutants such as methanol and formaldehyde have been detected. ACE makes limb observations from about 5 km (cloud free scenes) up to nearly 150 km in the lower thermosphere, where CO2 absorption is still weakly detectable. This talk will review ACE-FTS results in the mesosphere and lower thermosphere. Topics covered will include the mesospheric descent of NOx in the polar winter, spectra of polar mesospheric clouds, concentration profiles of CO2 (which do not match model predictions), and combined Odin-Osiris/ACE-FTS observations.

  8. The Atmospheric Chemistry Experiment (ACE): Mission Overview

    NASA Astrophysics Data System (ADS)

    Bernath, P. F.; Boone, C.; Walker, K.; McLeod, S.; Nassar, R.

    2003-12-01

    The ACE mission goals are: (1) to measure and to understand the chemical and dynamical processes that control the distribution of ozone in the upper troposphere and stratosphere, with a particular emphasis on the Arctic region; (2) to explore the relationship between atmospheric chemistry and climate change; (3) to study the effects of biomass burning in the free troposphere; (4) to measure aerosol number density, size distribution and composition in order to reduce the uncertainties in their effects on the global energy balance. ACE will make a comprehensive set of simultaneous measurements of trace gases, thin clouds, aerosols, and temperature by solar occultation from a satellite in low earth orbit. A high inclination (74 degrees) low earth orbit (650 km) gives ACE coverage of tropical, mid-latitudes and polar regions. The solar occultation advantages are high sensitivity and self-calibration. A high-resolution (0.02 cm-1) infrared Fourier Transform Spectrometer (FTS) operating from 2 to 13 microns (750-4100 cm-1) will measure the vertical distribution of trace gases, and the meteorological variables of temperature and pressure. The ACE concept is derived from the now-retired ATMOS FTS instrument, which flew on the Space Shuttle in 1985, 1992, 1993, 1994. Climate-chemistry coupling may lead to the formation of an Arctic ozone hole. ACE will provide high quality data to confront these model predictions and will monitor polar chemistry as chlorine levels decline. The ACE-FTS can measure water vapor and HDO in the tropical tropopause region to study dehydration and strat-trop exchange. The molecular signatures of massive forest fires will evident in the ACE infrared spectra. The CO2 in our spectra can be used to either retrieve atmospheric pressure or (if the instrument pointing knowledge proves to be satisfactory) for an independent retrieval of a CO2 profile for carbon cycle science. Aerosols and clouds will be monitored using the extinction of solar radiation at

  9. The Atmospheric Chemistry Experiment (ACE): Mission Overview

    NASA Astrophysics Data System (ADS)

    Bernath, P.

    2003-04-01

    The ACE mission goals are: (1) to measure and to understand the chemical and dynamical processes that control the distribution of ozone in the upper troposphere and stratosphere, with a particular emphasis on the Arctic region; (2) to explore the relationship between atmospheric chemistry and climate change; (3) to study the effects of biomass burning in the free troposphere; (4) to measure aerosol number density, size distribution and composition in order to reduce the uncertainties in their effects on the global energy balance. ACE will make a comprehensive set of simultaneous measurements of trace gases, thin clouds, aerosols, and temperature by solar occultation from a satellite in low earth orbit. A high inclination (74 degrees) low earth orbit (650 km) will give ACE coverage of tropical, mid-latitudes and polar regions. The solar occultation advantages are high sensitivity and self-calibration. A high-resolution (0.02 cm-1) infrared Fourier Transform Spectrometer (FTS) operating from 2 to 13 microns (750-4100 cm-1) will measure the vertical distribution of trace gases, and the meteorological variables of temperature and pressure. The ACE concept is derived from the now-retired ATMOS FTS instrument, which flew on the Space Shuttle in 1985, 1992, 1993, 1994. Climate-chemistry coupling may lead to the formation of an Arctic ozone hole. ACE will provide high quality data to confront these model predictions and will monitor polar chemistry as chlorine levels decline. The ACE-FTS can measure water vapor and HDO in the tropical tropopause region to study dehydration and strat-trop exchange. The molecular signatures of massive forest fires will evident in the ACE infrared spectra. The CO_2 in our spectra can be used to either retrieve atmospheric pressure or (if the instrument pointing knowledge proves to be satisfactory) for an independent retrieval of a CO_2 profile for carbon cycle science. Aerosols and clouds will be monitored using the extinction of solar

  10. Negative ion chemistry in Titan's upper atmosphere

    NASA Astrophysics Data System (ADS)

    Vuitton, V.; Lavvas, P.; Yelle, R. V.; Wellbrock, A.; Lewis, G. R.; Coates, A.; Thissen, R.; Dutuit, O.

    2008-09-01

    In the upper part of atmospheres lies the ionosphere, a region of particular interest for planetary science, because it provides the link between the neutral atmosphere, and the ionizing processes from outer space. On Titan, it is created by the interaction of solar ultraviolet radiation and magnetospheric electrons with the main atmospheric constituents, N2 and CH4. Cassini has revealed that an extremely complex chemistry occurs in Titan's ionosphere. The INMS mass spectrometer detected positively charged hydrocarbons and nitrogen-bearing species with a charge-to-mass ratio (m/z) up to 100 amu [1]. In 2007, the Electron Spectrometer (ELS), one of the sensors making up the Cassini Plasma Spectrometer (CAPS) revealed the existence of numerous negative ions in Titan's upper atmosphere [2]. The data showed evidence for negatively charged ions with m/z up to 10,000 amu and at lower m/z for two distinct peaks below 50 amu, corresponding to a total density of ~200 cm-3, giving an anion to cation ratio of ~0.1. This detection happened almost simultaneously with the surprising discovery of four negative ions in the interstellar medium: C4H-, C6H-, C8H- and C3N- [3; 4; 5; 6; 7]. The possible presence of negative ions in Titan's upper atmosphere had only been briefly discussed before the Cassini-Huygens mission. Three-body electron attachment to radicals or collisional charging of aerosols had been suggested as a source of negatively charged species. Because the first process is negligible at high altitude (neutral densities lower than 1015 cm-3) and because aerosols were not expected above ~500 km, ionospheric models considered the presence of negatively charged species to be highly unlikely. However, the observations clearly show that Titan has the most complex ionosphere of the Solar System with an intense chemistry, leading to an increase of molecular size. By analyzing the optical properties of the detached haze layer observed at 520 km in Titan's mesosphere, Lavvas et

  11. Do airborne microbes matter for atmospheric chemistry and cloud formation?

    PubMed

    Konstantinidis, Konstantinos T

    2014-06-01

    The role of airborne microbial cells in the chemistry of the atmosphere and cloud formation remains essentially speculative. Recent studies have indicated that microbes might be more important than previously anticipated for atmospheric processes. However, more work and direct communication between microbiologists and atmospheric scientists and modellers are necessary to better understand and model bioaerosol-cloud-precipitation-climate interactions.

  12. [Global Atmospheric Chemistry/Transport Modeling and Data-Analysis

    NASA Technical Reports Server (NTRS)

    Prinn, Ronald G.

    1999-01-01

    This grant supported a global atmospheric chemistry/transport modeling and data- analysis project devoted to: (a) development, testing, and refining of inverse methods for determining regional and global transient source and sink strengths for trace gases; (b) utilization of these inverse methods which use either the Model for Atmospheric Chemistry and Transport (MATCH) which is based on analyzed observed winds or back- trajectories calculated from these same winds for determining regional and global source and sink strengths for long-lived trace gases important in ozone depletion and the greenhouse effect; (c) determination of global (and perhaps regional) average hydroxyl radical concentrations using inverse methods with multiple "titrating" gases; and (d) computation of the lifetimes and spatially resolved destruction rates of trace gases using 3D models. Important ultimate goals included determination of regional source strengths of important biogenic/anthropogenic trace gases and also of halocarbons restricted by the Montreal Protocol and its follow-on agreements, and hydrohalocarbons now used as alternatives to the above restricted halocarbons.

  13. National Chemistry Week 2003: Earth's Atmosphere and Beyond. JCE Resources for Chemistry and the Atmosphere

    NASA Astrophysics Data System (ADS)

    Jacobsen, Erica K.

    2003-10-01

    This annotated bibliography collects the best that past issues of the Journal of Chemical Education have to offer for use with this year's National Chemistry Week theme: Earth's Atmosphere and Beyond. Each article has been characterized as a demonstration, experiment, activity, informational, or software/video item; several fit in more than one classification. The most recent articles are listed first. Also included is an evaluation as to which levels the article may serve. Articles that appeared adaptable to other levels, but are not designed explicitly for those levels, are labeled "poss. h.s." "poss. elem.", and so forth.

  14. Aerosols and chemistry in the planetary atmospheres

    NASA Astrophysics Data System (ADS)

    Zhang, Xi

    This dissertation is devoted to studying aerosols and their roles in regulating chemistry, radiation, and dynamics of planetary atmospheres. In chapter I, we provided a fundamental mathematical basis for the quasi-equilibrium growth assumption, a well-accepted approach to representing formation of secondary organic aerosols (SOAs) in microphysical simulations in the Earth's atmosphere. Our analytical work not only explains the quasi-equilibrium growth, which emerges as a limiting case in our theory, but also predicts the other types of condensational growth, confirmed by the recent laboratory and field experiments. In chapter II, we presented a new photochemical mechanism in which the evaporation of the aerosols composed of sulfuric acid or polysulfur on the nightside of Venus could provide a sulfur source above 90 km. Our model results imply the enhancements of sulfur oxides such as SO, SO2, and SO3. This is inconsistent with the previous model results but in agreement with the recent ground-based and spacecraft observations. In chapters III and IV, we developed a nonlinear optimization approach to retrieve the aerosol and cloud structure on Jupiter from the visible and ultraviolet images acquired by the Cassini spacecraft, combined with the ground-based near-infrared observations. We produced the first realistic spatial distribution of Jovian stratospheric aerosols in latitudes and altitudes. We also retrieved the stratospheric temperature and hydrocarbon species based on the mid-infrared spectra from the Cassini and Voyager spacecrafts. Based on the above information, the accurate and detailed maps of the instantaneous radiative forcing in Jovian stratosphere are obtained, revealing a significant heating effect from the polar dark aerosols in the high latitude region and therefore a strong modulation on the global meridional circulation in the stratosphere of Jupiter. In chapter V, we study the transport of passive tracers, such as aerosols, acetylene (C2H 2

  15. The Atmospheric Chemistry Experiment (ACE): Latest Results

    NASA Astrophysics Data System (ADS)

    Bernath, P.

    2008-12-01

    ACE (also known as SCISAT) is making a comprehensive set of simultaneous measurements of numerous trace gases, thin clouds, aerosols and temperature by solar occultation from a satellite in low earth orbit. A high inclination (74 degrees) low earth orbit (650 km) gives ACE coverage of tropical, mid-latitudes and polar regions. A high-resolution (0.02 cm-1) infrared Fourier Transform Spectrometer (FTS) operating from 2 to 13 microns (750-4400 cm-1) is measuring the vertical distribution of trace gases, and the meteorological variables of temperature and pressure. Aerosols and clouds are being monitored using the extinction of solar radiation at 0.525 and 1.02 microns as measured by two filtered imagers as well as by their infrared spectra. A dual spectrograph called MAESTRO extends the wavelength coverage to the 400-1000 nm spectral region. The principal investigator for MAESTRO is T. McElroy of the Meteorological Service of Canada. The FTS and imagers have been built by ABB-Bomem in Quebec City, while the satellite bus has been made by Bristol Aerospace in Winnipeg. ACE is part of the Canadian Space Agency's small satellite program, and was launched by NASA on 12 August 2003 for a nominal 2-year mission. The first results of ACE have been presented in a special issue of Geophysics Research Letters (http://www.agu.org/journals/ss/ACECHEM1/) in 2005 and recently a special issue on ACE validation has been prepared for Atmospheric Chemistry and Physics by K. Walker and K. Strong. A mission overview and status report will be presented. Science results for a few selected topics including the detection of organic molecules such as methanol and formaldehyde in the troposphere will be discussed.

  16. Gridded global surface ozone metrics for atmospheric chemistry model evaluation

    NASA Astrophysics Data System (ADS)

    Sofen, E. D.; Bowdalo, D.; Evans, M. J.; Apadula, F.; Bonasoni, P.; Cupeiro, M.; Ellul, R.; Galbally, I. E.; Girgzdiene, R.; Luppo, S.; Mimouni, M.; Nahas, A. C.; Saliba, M.; Tørseth, K.; Wmo Gaw, Epa Aqs, Epa Castnet, Capmon, Naps, Airbase, Emep, Eanet Ozone Datasets, All Other Contributors To

    2015-07-01

    The concentration of ozone at the Earth's surface is measured at many locations across the globe for the purposes of air quality monitoring and atmospheric chemistry research. We have brought together all publicly available surface ozone observations from online databases from the modern era to build a consistent dataset for the evaluation of chemical transport and chemistry-climate (Earth System) models for projects such as the Chemistry-Climate Model Initiative and Aer-Chem-MIP. From a total dataset of approximately 6600 sites and 500 million hourly observations from 1971-2015, approximately 2200 sites and 200 million hourly observations pass screening as high-quality sites in regional background locations that are appropriate for use in global model evaluation. There is generally good data volume since the start of air quality monitoring networks in 1990 through 2013. Ozone observations are biased heavily toward North America and Europe with sparse coverage over the rest of the globe. This dataset is made available for the purposes of model evaluation as a set of gridded metrics intended to describe the distribution of ozone concentrations on monthly and annual timescales. Metrics include the moments of the distribution, percentiles, maximum daily eight-hour average (MDA8), SOMO35, AOT40, and metrics related to air quality regulatory thresholds. Gridded datasets are stored as netCDF-4 files and are available to download from the British Atmospheric Data Centre (doi:10.5285/08fbe63d-fa6d-4a7a-b952-5932e3ab0452). We provide recommendations to the ozone measurement community regarding improving metadata reporting to simplify ongoing and future efforts in working with ozone data from disparate networks in a consistent manner.

  17. Gridded global surface ozone metrics for atmospheric chemistry model evaluation

    NASA Astrophysics Data System (ADS)

    Sofen, E. D.; Bowdalo, D.; Evans, M. J.; Apadula, F.; Bonasoni, P.; Cupeiro, M.; Ellul, R.; Galbally, I. E.; Girgzdiene, R.; Luppo, S.; Mimouni, M.; Nahas, A. C.; Saliba, M.; Tørseth, K.

    2016-02-01

    The concentration of ozone at the Earth's surface is measured at many locations across the globe for the purposes of air quality monitoring and atmospheric chemistry research. We have brought together all publicly available surface ozone observations from online databases from the modern era to build a consistent data set for the evaluation of chemical transport and chemistry-climate (Earth System) models for projects such as the Chemistry-Climate Model Initiative and Aer-Chem-MIP. From a total data set of approximately 6600 sites and 500 million hourly observations from 1971-2015, approximately 2200 sites and 200 million hourly observations pass screening as high-quality sites in regionally representative locations that are appropriate for use in global model evaluation. There is generally good data volume since the start of air quality monitoring networks in 1990 through 2013. Ozone observations are biased heavily toward North America and Europe with sparse coverage over the rest of the globe. This data set is made available for the purposes of model evaluation as a set of gridded metrics intended to describe the distribution of ozone concentrations on monthly and annual timescales. Metrics include the moments of the distribution, percentiles, maximum daily 8-hour average (MDA8), sum of means over 35 ppb (daily maximum 8-h; SOMO35), accumulated ozone exposure above a threshold of 40 ppbv (AOT40), and metrics related to air quality regulatory thresholds. Gridded data sets are stored as netCDF-4 files and are available to download from the British Atmospheric Data Centre (doi: 10.5285/08fbe63d-fa6d-4a7a-b952-5932e3ab0452). We provide recommendations to the ozone measurement community regarding improving metadata reporting to simplify ongoing and future efforts in working with ozone data from disparate networks in a consistent manner.

  18. Collaborative Research. Atmospheric Pressure Microplasma Chemistry-Photon Synergies

    SciTech Connect

    Park, Sung-Jin; Eden, James Gary

    2015-12-01

    Combining the effects of low temperature, atmospheric pressure microplasmas and microplasma photon sources offers the promise of greatly expanding the range of applications for each of them. The plasma sources create active chemical species and these can be activated further by the addition of photons and the associated photochemistry. There are many ways to combine the effects of plasma chemistry and photochemistry, especially if there are multiple phases present. This project combined the construction of appropriate test experimental systems, various spectroscopic diagnostics and mathematical modeling. Through a continuous discussion and co-design process with the UC-Berkeley Team, we have successfully completed the fabrication and testing of all components for a microplasma array-assisted system designed for photon-activated plasma chemistry research. Microcavity plasma lamps capable of generating more than 20 mW/cm2 at 172 nm (Xe dimer) were fabricated with a custom form factor to mate to the plasma chemistry setup, and a lamp was current being installed by the Berkeley team so as to investigate plasma chemistry-photon synergies at a higher photon energy (~7.2 eV) as compared to the UVA treatment that is afforded by UV LEDs operating at 365 nm. In particular, motivated by the promising results from the Berkeley team with UVA treatment, we also produced the first generation of lamps that can generate photons in the 300-370 nm wavelength range. Another set of experiments, conducted under the auspices of this grant, involved the use of plasma microjet arrays. The combination of the photons and excited radicals produced by the plasma column resulted in broad area deactivation of bacteria.

  19. Session on coupled atmospheric/chemistry coupled models

    NASA Technical Reports Server (NTRS)

    Thompson, Anne

    1993-01-01

    The session on coupled atmospheric/chemistry coupled models is reviewed. Current model limitations, current issues and critical unknowns, and modeling activity are addressed. Specific recommendations and experimental strategies on the following are given: multiscale surface layer - planetary boundary layer - chemical flux measurements; Eulerian budget study; and Langrangian experiment. Nonprecipitating cloud studies, organized convective systems, and aerosols - heterogenous chemistry are also discussed.

  20. Sulfur Chemistry in the Early and Present Atmosphere of Mars

    NASA Technical Reports Server (NTRS)

    Levine, Joel S.; Summers, M. E.

    2011-01-01

    Atmospheric sulfur species resulting from volcanic emissions impact the composition and chemistry of the atmosphere, impact the climate, and hence, the habitability of Mars and impact the mineralogy and composition of the surface of Mars. The geochemical/ photochemical cycling of sulfur species between the interior (via volcanism), the atmosphere (atmospheric photochemical and chemical processes) and the deposition of sulfuric acid on the surface of Mars is an important, but as yet poorly understood geochemical/ photochemical cycle on Mars. There is no observational evidence to indicate that Mars is volcanically active at the present time, however, there is strong evidence that volcanism was an important and widespread process on early Mars. The chemistry and photochemistry of sulfur species in the early and present atmosphere of Mars will be assessed using a one-dimensional photochemical model. Since it is generally assumed that the atmosphere of early Mars was significantly denser than the present 6-millibar atmosphere, photochemical calculations were performed for the present atmosphere and for the atmosphere of early Mars with assumed surface pressures of 60 and 350-millibars, where higher surface pressure resulted from enhanced atmospheric concentrations of carbon dioxide (CO2). The following sections include the results of earlier modeling studies, a summary of the one-dimensional photochemical model used in this study, a summary of the photochemistry and chemistry of sulfur species in the atmosphere of Mars and some of the results of the calculations.

  1. A comparison of atmospheric composition using the Carbon Bond and Regional Atmospheric Chemistry MechanismsChemistry Mechanisms

    EPA Science Inventory

    We incorporate the recently developed Regional Atmospheric Chemistry Mechanism (version 2, RACM2) into the Community Multiscale Air Quality modeling system for comparison with the existing 2005 Carbon Bond mechanism with updated toluene chemistry (CB05TU). Compared to CB05TU, RAC...

  2. A comparison of atmospheric composition using the Carbon Bond and Regional Atmospheric Chemistry MechanismsChemistry Mechanisms

    EPA Science Inventory

    We incorporate the recently developed Regional Atmospheric Chemistry Mechanism (version 2, RACM2) into the Community Multiscale Air Quality modeling system for comparison with the existing 2005 Carbon Bond mechanism with updated toluene chemistry (CB05TU). Compared to CB05TU, RAC...

  3. Chemistry [Sahuarita High School Career Curriculum Project].

    ERIC Educational Resources Information Center

    Lane, Robert

    This course entitled "Chemistry" is one of a series of instructional guides prepared by teachers for the Sahuarita High School (Arizona) Career Curriculum Project. It consists of three packages, the first dealing with solids, liquids and solutions, the second with acids, bases and anions, and the third with cation analysis. These packages are…

  4. Concluding remarks: Faraday Discussion on chemistry in the urban atmosphere.

    PubMed

    Jimenez, Jose L

    2016-07-18

    This article summarises the Concluding remarks from the Faraday Discussion on Chemistry in the Urban Atmosphere. The following themes are addressed: (a) new results that inform our understanding of the evolving sources and composition of the urban atmosphere ("News"); (b) results that identify gaps in our understanding that necessitate further work ("Gaps");

  5. Joint analysis of deposition fluxes and atmospheric concentrations of inorganic nitrogen and sulphur compounds predicted by six chemistry transport models in the frame of the EURODELTAIII project

    NASA Astrophysics Data System (ADS)

    Vivanco, M. G.; Bessagnet, B.; Cuvelier, C.; Theobald, M. R.; Tsyro, S.; Pirovano, G.; Aulinger, A.; Bieser, J.; Calori, G.; Ciarelli, G.; Manders, A.; Mircea, M.; Aksoyoglu, S.; Briganti, G.; Cappelletti, A.; Colette, A.; Couvidat, F.; D'Isidoro, M.; Kranenburg, R.; Meleux, F.; Menut, L.; Pay, M. T.; Rouïl, L.; Silibello, C.; Thunis, P.; Ung, A.

    2017-02-01

    In the framework of the UNECE Task Force on Measurement and Modelling (TFMM) under the Convention on Long-range Transboundary Air Pollution (LRTAP), the EURODELTAIII project is evaluating how well air quality models are able to reproduce observed pollutant air concentrations and deposition fluxes in Europe. In this paper the sulphur and nitrogen deposition estimates of six state-of-the-art regional models (CAMx, CHIMERE, EMEP MSC-W, LOTOS-EUROS, MINNI and CMAQ) are evaluated and compared for four intensive EMEP measurement periods (25 Feb-26 Mar 2009; 17 Sep-15 Oct 2008; 8 Jan-4 Feb 2007 and 1-30 Jun 2006). For sulphur, this study shows the importance of including sea salt sulphate emissions for obtaining better model results; CMAQ, the only model considering these emissions in its formulation, was the only model able to reproduce the high measured values of wet deposition of sulphur at coastal sites. MINNI and LOTOS-EUROS underestimate sulphate wet deposition for all periods and have low wet deposition efficiency for sulphur. For reduced nitrogen, all the models underestimate both wet deposition and total air concentrations (ammonia plus ammonium) in the summer campaign, highlighting a potential lack of emissions (or incoming fluxes) in this period. In the rest of campaigns there is a general underestimation of wet deposition by all models (MINNI and CMAQ with the highest negative bias), with the exception of EMEP, which underestimates the least and even overestimates deposition in two campaigns. This model has higher scavenging deposition efficiency for the aerosol component, which seems to partly explain the different behaviour of the models. For oxidized nitrogen, CMAQ, CAMx and MINNI predict the lowest wet deposition and the highest total air concentrations (nitric acid plus nitrates). Comparison with observations indicates a general underestimation of wet oxidized nitrogen deposition by these models, as well as an overestimation of total air concentration for

  6. COMPUTATIONAL CHEMISTRY: AN EMERGING TECHNOLOGY FOR SOLVING PROBLEMS IN ATMOSPHERIC CHEMISTRY

    EPA Science Inventory

    Over the past three decades, atmospheric chemistry has served as an important component in developing strategies for reducing ambient concentrations of air pollutants. Laboratory studies are carried out to investigate the key chemical reactions that determine the fates and lif...

  7. COMPUTATIONAL CHEMISTRY: AN EMERGING TECHNOLOGY FOR SOLVING PROBLEMS IN ATMOSPHERIC CHEMISTRY

    EPA Science Inventory

    Over the past three decades, atmospheric chemistry has served as an important component in developing strategies for reducing ambient concentrations of air pollutants. Laboratory studies are carried out to investigate the key chemical reactions that determine the fates and lif...

  8. Atmospheric Chemistry in a Changing World

    NASA Astrophysics Data System (ADS)

    Brune, William H.

    The world is changing,and the atmosphere's composition is changing with it. Human activity is responsible for much of this. Global population growth and migration to urban centers, extensive biomass burning, the spread of fertilizer-intensive agribusiness, globalization of business and industry, rising standards of living in the developing world, and increased energy use fuels atmospheric change. If current practices continue, atmospheric increases are likely for the greenhouse gases carbon dioxide, methane, nitrous oxide; and for the chemically active gases nitric oxide, sulfur dioxide,and ammonia. Increases in global tropospheric ozone and aerosols are a distinct possibility.

  9. The Essential Role for Laboratory Studies in Atmospheric Chemistry.

    PubMed

    Burkholder, James B; Abbatt, Jonathan P D; Barnes, Ian; Roberts, James M; Melamed, Megan L; Ammann, Markus; Bertram, Allan K; Cappa, Christopher D; Carlton, Annmarie G; Carpenter, Lucy J; Crowley, John N; Dubowski, Yael; George, Christian; Heard, Dwayne E; Herrmann, Hartmut; Keutsch, Frank N; Kroll, Jesse H; McNeill, V Faye; Ng, Nga Lee; Nizkorodov, Sergey A; Orlando, John J; Percival, Carl J; Picquet-Varrault, Bénédicte; Rudich, Yinon; Seakins, Paul W; Surratt, Jason D; Tanimoto, Hiroshi; Thornton, Joel A; Tong, Zhu; Tyndall, Geoffrey S; Wahner, Andreas; Weschler, Charles J; Wilson, Kevin R; Ziemann, Paul J

    2017-03-07

    Laboratory studies of atmospheric chemistry characterize the nature of atmospherically relevant processes down to the molecular level, providing fundamental information used to assess how human activities drive environmental phenomena such as climate change, urban air pollution, ecosystem health, indoor air quality, and stratospheric ozone depletion. Laboratory studies have a central role in addressing the incomplete fundamental knowledge of atmospheric chemistry. This article highlights the evolving science needs for this community and emphasizes how our knowledge is far from complete, hindering our ability to predict the future state of our atmosphere and to respond to emerging global environmental change issues. Laboratory studies provide rich opportunities to expand our understanding of the atmosphere via collaborative research with the modeling and field measurement communities, and with neighboring disciplines.

  10. Lookup tables to compute high energy cosmic ray induced atmospheric ionization and changes in atmospheric chemistry

    SciTech Connect

    Atri, Dimitra; Melott, Adrian L.; Thomas, Brian C. E-mail: melott@ku.edu

    2010-05-01

    A variety of events such as gamma-ray bursts and supernovae may expose the Earth to an increased flux of high-energy cosmic rays, with potentially important effects on the biosphere. Existing atmospheric chemistry software does not have the capability of incorporating the effects of substantial cosmic ray flux above 10 GeV. An atmospheric code, the NASA-Goddard Space Flight Center two-dimensional (latitude, altitude) time-dependent atmospheric model (NGSFC), is used to study atmospheric chemistry changes. Using CORSIKA, we have created tables that can be used to compute high energy cosmic ray (10 GeV–1 PeV) induced atmospheric ionization and also, with the use of the NGSFC code, can be used to simulate the resulting atmospheric chemistry changes. We discuss the tables, their uses, weaknesses, and strengths.

  11. Atmospheric chemistry: The return of ethane

    NASA Astrophysics Data System (ADS)

    Hakola, Hannele; Hellén, Heidi

    2016-07-01

    Ethane emissions can lead to ozone pollution. Measurements at 49 sites show that long-declining atmospheric ethane concentrations started rising in 2010 in the Northern Hemisphere, largely due to greater oil and gas production in the USA.

  12. Hydrogen chemistry - Perspective on experiment and theory. [atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Kaufman, F.

    1975-01-01

    A review is presented of the advantages and limitations of various experimental methods for the investigation of the kinetics of hydrogen chemistry, including classic thermal and photochemical methods and the crossed molecular beam method. Special attention is given to the flash photolysis-resonance fluorescence apparatus developed by Braun et al, in which repetitive vacuum UV flashes result in the photolytic generation of the desired species, and to the discharge-flow technique. The use of various theoretical methods for the selection or elimination of kinetic data is considered in a brief discussion of the rate theory of two-body encounters and recombination-dissociation processes in neutral reactions. Recent kinetic studies of a series of OH reactions and of a major loss process for odd H in the stratosphere are summarized.

  13. Hydrogen chemistry - Perspective on experiment and theory. [atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Kaufman, F.

    1975-01-01

    A review is presented of the advantages and limitations of various experimental methods for the investigation of the kinetics of hydrogen chemistry, including classic thermal and photochemical methods and the crossed molecular beam method. Special attention is given to the flash photolysis-resonance fluorescence apparatus developed by Braun et al, in which repetitive vacuum UV flashes result in the photolytic generation of the desired species, and to the discharge-flow technique. The use of various theoretical methods for the selection or elimination of kinetic data is considered in a brief discussion of the rate theory of two-body encounters and recombination-dissociation processes in neutral reactions. Recent kinetic studies of a series of OH reactions and of a major loss process for odd H in the stratosphere are summarized.

  14. Response of lightning NOx emissions and ozone production to climate change: Insights from the Atmospheric Chemistry and Climate Model Intercomparison Project

    NASA Astrophysics Data System (ADS)

    Finney, D. L.; Doherty, R. M.; Wild, O.; Young, P. J.; Butler, A.

    2016-05-01

    Results from an ensemble of models are used to investigate the response of lightning nitrogen oxide emissions to climate change and the consequent impacts on ozone production. Most models generate lightning using a parameterization based on cloud top height. With this approach and a present-day global emission of 5 TgN, we estimate a linear response with respect to changes in global surface temperature of +0.44 ± 0.05 TgN K-1. However, two models using alternative approaches give +0.14 and -0.55 TgN K-1 suggesting that the simulated response is highly dependent on lightning parameterization. Lightning NOx is found to have an ozone production efficiency of 6.5 ± 4.7 times that of surface NOx sources. This wide range of efficiencies across models is partly due to the assumed vertical distribution of the lightning source and partly to the treatment of nonmethane volatile organic compound (NMVOC) chemistry. Careful consideration of the vertical distribution of emissions is needed, given its large influence on ozone production.

  15. Impact of Plasma Chemistry on Io's Atmosphere

    NASA Astrophysics Data System (ADS)

    Moore, Chris H.; Deng, H.; Goldstein, D. B.; Levin, D.; Varghese, P. L.; Trafton, L. M.; Walker, A. C.; Stewart, B. D.

    2010-10-01

    We present results of an investigation of the jovian plasma torus’ interaction with Io's sublimation atmosphere using the direct simulation Monte Carlo (DSMC) method which is appropriate for solving rarefied flows such as Io's atmosphere. Accurate simulation of Io's atmosphere is critical for modeling the supply of material to the torus and understanding the morphology and intensity of the electron excited aurora on Io. The plasma sweeps past Io at 57 km/s and the resultant energetic collisions with Io's neutral atmosphere create an inflated, mixed atmosphere of SO2 and its daughter products. In the present work, the plasma interaction is modeled by a flux of ions and electrons which flow around and through Io's atmosphere along pre-computed perturbed magnetic field lines. Since the Debye length is everywhere much less than the size of the DSMC computational cells (which scale with the neutral mean free path), we assume the plasma is quasi-neutral. A two time-step method is used in which the neutrals move and then are stationary while the ions and electrons move with a much smaller time-step. Ions can undergo non-reactive collisions and charge exchange collisions with the neutral species. Fast neutrals produced via charge exchange have sufficient energy to dissociate the neutral molecular species; these interaction cross sections have been computed using MD/QCT simulations. The electron interactions with the neutral species are functions of the collision energy and are based on measured reaction cross sections (elastic, excitation, ionization, and dissociation). The effect of the plasma on the circumplanetary winds, the escape rate of neutrals from Io, and the composition and structure of Io's atmosphere is investigated and compared with previous continuum simulations by Smyth and Wong. Future work will investigate the resultant auroral emissions and their implications on volcanic activity and the upstream electron temperature.

  16. Multiple oscillations in Neoarchaean atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Izon, Gareth; Zerkle, Aubrey L.; Zhelezinskaia, Iadviga; Farquhar, James; Newton, Robert J.; Poulton, Simon W.; Eigenbrode, Jennifer L.; Claire, Mark W.

    2015-12-01

    The Great Oxidation Event (GOE) represents a crucial juncture in Earth history, signifying the rise in atmospheric oxygen from parts per million to percent levels at ∼2.45-2.32 billion-years-ago (Ga). Although planetary oxygenation undoubtedly led to the inception of the contemporary Earth system, the trigger(s) and mechanism(s) controlling this chemical reorganisation remain elusive. Quantitative estimates of the atmosphere's composition in the prelude to the GOE are central to understanding this oxygenation event. Previous analyses of 2.65-2.5 Ga sediments from the Griqualand Basin (South Africa) invoke a tantalising picture of an unusual Earth environment, alluding to an atmosphere periodically dominated by a layer of organic particles ("haze") formed from methane photolysis. However, as yet this hypothesis has remained untested. Here we present four new coupled carbon and quadruple sulphur isotope records from distal, time equivalent (2.7-2.5 Ga), sedimentary successions from South Africa and Western Australia. These extended records reveal similar chemostratigraphic trends, supporting a dynamic terminal-Neoarchaean atmosphere, oscillating between a hazy state at elevated methane concentrations, and a haze-free anoxic background state. We suggest these atmospheric aberrations were related to heightened biogenic methane fluxes fuelled by enhanced nutrient delivery from climatically or weathering induced feedbacks. These data question the canonical view of a simple, unidirectional planetary oxygenation and signify that the overture to the GOE was governed by complex feedbacks within the Earth-biosphere system.

  17. Global atmospheric chemistry of CFC-123

    NASA Technical Reports Server (NTRS)

    Prinn, Ronald G.; Golombek, Amram

    1990-01-01

    The compound 1,1-dichloro--2,2,2-trifluoroethane (CFC-123) has been proposed as an industrial substitute for trichlorofluoromethane (CFC-11). The chemical destruction rates of CFC-123 by various processes is calculated here using a three-dimensional global model of the atmosphere, and it is confirmed that the chief sink of CFC-123 is destruction by OH radicals below 12 km, accounting for 88 percent of its loss. The calculated destruction rate is greatest in the equatorial region below 2 km. The calculated steady-state lifetime of CFC-123 is 1.5 years, much shorter than that of CFC-11, the destruction of which is largely confined to the stratosphere. For equal rates of CFC-123 and CFC-11 emission to the atmosphere, the molar content in the atmosphere and the injection rate of chlorine into the stratosphere are, respectively, 48 and 14 times greater for CFC-11 than for CFC-123 in steady state.

  18. Night-time atmospheric chemistry of methacrylates.

    PubMed

    Salgado, M Sagrario; Gallego-Iniesta, M Paz; Martín, M Pilar; Tapia, Araceli; Cabañas, Beatriz

    2011-07-01

    Methacrylates are α, β-unsaturated esters that are widely used in the polymer plastics and resins production. Kinetic information of NO(3) radical reactions is especially scarce and a good understanding of all the atmospheric oxidation processes of these compounds is necessary in order to determine lifetimes in the atmosphere and to evaluate the impact of these reactions on the formation of ozone and other photooxidants. The experiments have been carried out using the relative technique in a static Teflon reactor at room temperature and atmospheric pressure (N(2) as bath gas) using gas chromatography (GC)-flame ionization detection (FID) as detection system. Products were analyzed using solid phase microextraction (SPME)-GC-mass spectrometry (MS) technique and Fourier transform infrared spectroscopy (FTIR) using air as bath gas. The following rate coefficients were obtained (in cm(3) molecule(-1) s(-1)): methyl methacrylate + NO(3) = (3.55 ± 0.62) × 10(-15), ethyl methacrylate + NO(3) = (5.42 ± 1.90) × 10(-15), butyl methacrylate + NO(3) = (7.87 ± 3.86) × 10(-15). Methylpyruvate, ethylpyruvate, and butylpyruvate/butanol were identified as main degradation products respectively in the GC-MS analysis. Nitrates compounds were also identified in the FTIR study. The reactivity increases with the substitution and with the chain of the alkyl group in -C(O)OR. An electrophilic addition mechanism is proposed as dominant degradation process. Estimations of the atmospheric lifetimes clearly indicate that the dominant atmospheric loss process for methacrylate esters is their daytime reaction with the hydroxyl radical. NO(3) and ozone are the main oxidants at night time. A detailed products analysis including quantification could elucidate the mechanism for butanol generation for butyl methacrylate reaction.

  19. Nitrogen Chemistry in Titan's Upper Atmosphere

    NASA Astrophysics Data System (ADS)

    Kammer, J. A.; Shemansky, D. E.; Zhang, X.; Yung, Y. L.

    2012-04-01

    Titan’s atmosphere has evolved over time into its current state through complex photochemical processes (Yung et al. 1984), involving nitrogen (N2), the dominant molecular species in the atmosphere, as well as methane (CH4). It has been proposed that this composition may be analogous to the early Earth’s, as it certainly provides an abundance of hydrocarbons the like from which early life may have arisen (Coustenis & Taylor 1999; Lunine 2005). Recent results from the Cassini spacecraft have greatly improved our knowledge of the current state of Titan’s atmosphere, and measurements made by the Ultraviolet Imaging Spectrograph (UVIS) in particular are able to probe the region of interest from 400 km to 1500 km in altitude where much of the photochemistry on Titan occurs (Shemansky et al. 2005, Koskinen et al. 2011). This photochemistry in part converts nitrogen from stable N2 molecules and incorporates it into detectable hydrocarbon products such as HCN, HC3N, and other heavier compounds. Therefore the nitrogen story is of particular interest, and we examine UVIS occultation observations in both the EUV and FUV regions of the spectrum in order to directly retrieve the vertical profiles of N2 in addition to its related hydrocarbon derivatives. Constraints from UVIS on temperature profiles of the upper atmosphere are also examined and compared to current results from the Ion and Neutral Mass Spectrometer (INMS), which probes a region above 1000 km altitude in Titan’s atmosphere (Westlake et al. 2011). References: Coustenis, A., and F. Taylor: “Titan: The Earth-Like Moon”. Singapore: World Scientific, 1999. Koskinen, T. T., et al.: “The mesosphere and thermosphere of Titan revealed by Cassini/UVIS stellar occultations”. Icarus, Vol. 216, pp. 507-534, 2011. Lunine, J. I.: “Astrobiology: A Multidisciplinary Approach”. San Francisco, CA: Pearson Addison Wesley, 2005. Shemansky, D. E., et al.: “The Cassini UVIS stellar probe of the Titan atmosphere

  20. Parallel processing of atmospheric chemistry calculations: Preliminary considerations

    SciTech Connect

    Elliott, S.; Jones, P.

    1995-01-01

    Global climate calculations are already saturating the class modern vector supercomputers with only a few central processing units. Increased resolution and inclusion of routines to deal with biogeochemical portions of the terrestrial climate system will soon demand massively parallel approaches. The atmospheric photochemistry ensemble is intimately linked to climate through the trace greenhouse gases ozone and methane and modules for representing it are being attached to global three dimensional transport and GCM frameworks. Atmospheric kinetics involve dozens of highly interactive tracers and so will accentuate the need for parallel processing of earth system simulations. In the present text we lay some of the groundwork for addition of atmospheric kinetics packages to GCM and global scale atmospheric models on multiply parallel computers. The discussion is tailored for consumption by the photochemical modelling community. After a review of numerical atmospheric chemistry methods, we examine how kinetics can be implemented on a parallel computer. We concentrate especially on data layout and flexibility and how these can be implemented in various programming models. We conclude that chemistry can be implemented rather easily within existing frameworks of several parallel atmospheric models. However, memory limitations may preclude high resolution studies of global chemistry.

  1. Atmospheric Composition and Chemistry Discoveries from Space

    NASA Astrophysics Data System (ADS)

    Douglass, A. R.; Stolarski, R. S.

    2005-12-01

    Satellite observations have given scientists a global perspective on the photochemical and dynamical processes that control the atmospheric evolution of constituents like ozone. The satellites and their instruments are often designed to address specific questions and sometimes vastly exceed their developer's expectations. The Total Ozone Mapping Spectrometer (TOMS) was designed to simply map the variability of the ozone column due to atmospheric waves. The instruments on the Upper Atmosphere Research Satellite (UARS) were designed to measure upper stratospheric ozone and quantities important to ozone including solar flux, winds and constituents that contribute to ozone destruction. The scientific payoff from UARS and TOMS vastly exceeded these modest goals. Total ozone measurements from TOMS revealed the extent and variability of the Antarctic ozone hole. UARS instruments showed the spatial structures of the conversion of chlorine species from reservoirs to radicals and back to reservoirs during the seasonal development and disappearance of the ozone hole. UARS investigators discovered previously unknown features of the atmospheric circulation. For example, long-lived tracer measurements showed unmixed descent of mesospheric air into the polar lower stratosphere as the winter vortex was formed. Observations of water vapor in the tropical stratosphere showed that air parcels carry the memory of the tropical tropopause temperature for years as they ascend through the stratosphere (the tropical "tape recorder"). The persistence of this signature places constraints on mass flux into the stratosphere and the mixing between tropical and middle latitudes. Satellite data have yielded unexpected bonuses. Improvements in the understanding of the TOMS retrieval algorithm allowed for the removal of drifts in instrument performance to produce a stable climate-quality data set for trend analysis. Apparent noise in the retrievals was eventually understood to be due to aerosols

  2. Atmospheric and combustion chemistry of dimethyl ether

    SciTech Connect

    Nielsen, O.J.; Egsgaard, H.; Larsen, E.; Sehested, J.; Wallington, T.J.

    1997-12-31

    It has been demonstrated that dimethyl ether (DME) is an ideal diesel fuel alternative. DME, CH{sub 3}OCH{sub 3}, combines good fuel properties with low exhaust emissions and low combustion noise. Large scale production of this fuel can take place using a single step catalytic process converting CH{sub 4} to DME. The fate of DME in the atmosphere has previously been studied. The atmospheric degradation is initiated by the reaction with hydroxyl radicals, which is also a common feature of combustion processes. Spectrokinetic investigations and product analysis were used to demonstrate that the intermediate oxy radical, CH{sub 3}OCH{sub 2}O, exhibits a novel reaction pathway of hydrogen atom ejection. The application of tandem mass spectrometry to chemi-ions based on supersonic molecular beam sampling has recently been demonstrated. The highly reactive ionic intermediates are sampled directly from the flame and identified by collision activation mass spectrometry and ion-molecule reactions. The mass spectrum reflects the distribution of the intermediates in the flame. The atmospheric degradation of DME as well as the unique fuel properties of a oxygen containing compound will be discussed.

  3. Chemistry in the near-surface atmosphere at Ganymede

    NASA Astrophysics Data System (ADS)

    Shematovich, V. I.

    2013-09-01

    Theoretical predictions of the composition and chemical evolution of near-surface atmospheres of the icy satellites in the Jovian and Kronian systems are of great importance for assessing the biological potential of these satellites. Depending on the satellite mass the formation of the rarefied exosphere with the relatively dense near-surface layer is possible as, for example, in the case of the relatively heavy Galilean satellites Europa and Ganymede in the Jovian system [1-3]. Ganymede is of special interest, because observations indicate that Ganymede has a significant O2 near - surface atmosphere, probably subsurface ocean, and is the only satellite with its own magnetosphere. Processes of formation of the rarefied gaseous envelope of Ganymede and chemical exchange between atmosphere and icy surface will be considered. The water vapour is usually the domin ant parent species in such gaseous envelope because of the ejection from the satellite icy surface due to the thermal outgassing, non-thermal photolysis and radiolysis and other active processes at work on the surface. The photochemis try of water vapour in the near - surface atmospheric layer [4] and the radiolysis of icy regolith [5] result in the supplement of the atmosphere by an admixture of H2, O2, OH and O. Returning molecules have species-dependent behaviour on contact with icy surface of the satellite and non-thermal energy distributions for the chemical radicals. The H2 and O2 molecules stick with very low efficiency and are immediately desorbed thermally, but returning H2O, OH, H and O stick to the grains in the icy regolith with unit efficiency. The suprathermal radicals OH, H, and O entering the regolith can drive the surface chemistry. The numerical kinetic model to investigate on the molecular level the chemistry of the atmosphere - surface interface of the rarefied Н2О-dominant gaseous envelope at Ganymede was developed. Such numerical model simulates the gas-phase and diffusive surface

  4. Chemistry of atmospheric ions reacting with fully fluorinated compounds

    SciTech Connect

    Morris, R.A.; Paulson, J.F.; Viggiano, A.A.; Arnold, S.T.

    1995-12-31

    Fully fluorinated (perfluorinated) compounds are a class of chemicals with large global warming potentials (GWPs) resulting from a combination of strong infrared absorption and very long atmospheric lifetimes, i.e. millennia. In this paper, the authors describe the detailed findings of the laboratory measurements of the atmospheric ion chemistry involved. Some of the studied reactions are also of importance in plasma processing of microcircuits and thus in the chemical modeling thereof. The authors have previously reported kinetics results for a large number of reactions between ions and halocarbons; this article extends the work and includes atmospheric ions.

  5. Effects of Deep Convection on Atmospheric Chemistry

    NASA Technical Reports Server (NTRS)

    Pickering, Kenneth E.

    2007-01-01

    This presentation will trace the important research developments of the last 20+ years in defining the roles of deep convection in tropospheric chemistry. The role of deep convection in vertically redistributing trace gases was first verified through field experiments conducted in 1985. The consequences of deep convection have been noted in many other field programs conducted in subsequent years. Modeling efforts predicted that deep convection occurring over polluted continental regions would cause downstream enhancements in photochemical ozone production in the middle and upper troposphere due to the vertical redistribution of ozone precursors. Particularly large post-convective enhancements of ozone production were estimated for convection occurring over regions of pollution from biomass burning and urban areas. These estimates were verified by measurements taken downstream of biomass burning regions of South America. Models also indicate that convective transport of pristine marine boundary layer air causes decreases in ozone production rates in the upper troposphere and that convective downdrafts bring ozone into the boundary layer where it can be destroyed more rapidly. Additional consequences of deep convection are perturbation of photolysis rates, effective wet scavenging of soluble species, nucleation of new particles in convective outflow, and the potential fix stratosphere-troposphere exchange in thunderstorm anvils. The remainder of the talk will focus on production of NO by lightning, its subsequent transport within convective clouds . and its effects on downwind ozone production. Recent applications of cloud/chemistry model simulations combined with anvil NO and lightning flash observations in estimating NO Introduction per flash will be described. These cloud-resolving case-study simulations of convective transport and lightning NO production in different environments have yielded results which are directly applicable to the design of lightning

  6. Effects of Deep Convection on Atmospheric Chemistry

    NASA Technical Reports Server (NTRS)

    Pickering, Kenneth E.

    2007-01-01

    This presentation will trace the important research developments of the last 20+ years in defining the roles of deep convection in tropospheric chemistry. The role of deep convection in vertically redistributing trace gases was first verified through field experiments conducted in 1985. The consequences of deep convection have been noted in many other field programs conducted in subsequent years. Modeling efforts predicted that deep convection occurring over polluted continental regions would cause downstream enhancements in photochemical ozone production in the middle and upper troposphere due to the vertical redistribution of ozone precursors. Particularly large post-convective enhancements of ozone production were estimated for convection occurring over regions of pollution from biomass burning and urban areas. These estimates were verified by measurements taken downstream of biomass burning regions of South America. Models also indicate that convective transport of pristine marine boundary layer air causes decreases in ozone production rates in the upper troposphere and that convective downdrafts bring ozone into the boundary layer where it can be destroyed more rapidly. Additional consequences of deep convection are perturbation of photolysis rates, effective wet scavenging of soluble species, nucleation of new particles in convective outflow, and the potential fix stratosphere-troposphere exchange in thunderstorm anvils. The remainder of the talk will focus on production of NO by lightning, its subsequent transport within convective clouds . and its effects on downwind ozone production. Recent applications of cloud/chemistry model simulations combined with anvil NO and lightning flash observations in estimating NO Introduction per flash will be described. These cloud-resolving case-study simulations of convective transport and lightning NO production in different environments have yielded results which are directly applicable to the design of lightning

  7. Exoplanetary Atmospheres-Chemistry, Formation Conditions, and Habitability.

    PubMed

    Madhusudhan, Nikku; Agúndez, Marcelino; Moses, Julianne I; Hu, Yongyun

    2016-12-01

    Characterizing the atmospheres of extrasolar planets is the new frontier in exoplanetary science. The last two decades of exoplanet discoveries have revealed that exoplanets are very common and extremely diverse in their orbital and bulk properties. We now enter a new era as we begin to investigate the chemical diversity of exoplanets, their atmospheric and interior processes, and their formation conditions. Recent developments in the field have led to unprecedented advancements in our understanding of atmospheric chemistry of exoplanets and the implications for their formation conditions. We review these developments in the present work. We review in detail the theory of atmospheric chemistry in all classes of exoplanets discovered to date, from highly irradiated gas giants, ice giants, and super-Earths, to directly imaged giant planets at large orbital separations. We then review the observational detections of chemical species in exoplanetary atmospheres of these various types using different methods, including transit spectroscopy, Doppler spectroscopy, and direct imaging. In addition to chemical detections, we discuss the advances in determining chemical abundances in these atmospheres and how such abundances are being used to constrain exoplanetary formation conditions and migration mechanisms. Finally, we review recent theoretical work on the atmospheres of habitable exoplanets, followed by a discussion of future outlook of the field.

  8. Ozone Depletion, UVB and Atmospheric Chemistry

    NASA Technical Reports Server (NTRS)

    Stolarski, Richard S.

    1999-01-01

    The primary constituents of the Earth's atmosphere are molecular nitrogen and molecular oxygen. Ozone is created when ultraviolet light from the sun photodissociates molecular oxygen into two oxygen atoms. The oxygen atoms undergo many collisions but eventually combine with a molecular oxygen to form ozone (O3). The ozone molecules absorb ultraviolet solar radiation, primarily in the wavelength region between 200 and 300 nanometers, resulting in the dissociation of ozone back into atomic oxygen and molecular oxygen. The oxygen atom reattaches to an O2 molecule, reforming ozone which can then absorb another ultraviolet photon. This sequence goes back and forth between atomic oxygen and ozone, each time absorbing a uv photon, until the oxygen atom collides with and ozone molecule to reform two oxygen molecules.

  9. Atmospheric chemistry of 1-methyl-2-pyrrolidinone

    NASA Astrophysics Data System (ADS)

    Aschmann, Sara M.; Atkinson, Roger

    Rate constants for the atmospheric reactions of 1-methyl-2-pyrrolidinone with OH radicals, NO 3 radicals and O 3 have been measured at 296±2 K and atmospheric pressure of air, and the products of the OH radical and NO 3 radical reactions investigated. Using relative rate techniques, rate constants for the gas-phase reactions of OH and NO 3 radicals with 1-methyl-2-pyrrolidinone of (2.15±0.36)×10 -11 cm 3 molecule -1 s -1 and (1.26±0.40)×10 -13 cm 3 molecule -1 s -1, respectively, were measured, where the indicated errors include the estimated overall uncertainties in the rate constants for the reference compounds. An upper limit to the rate constant for the O 3 reaction of <1×10 -19 cm 3 molecule -1 s -1 was also determined. These kinetic data lead to a calculated tropospheric lifetime of 1-methyl-2-pyrrolidinone of a few hours, with both the daytime OH radical reaction and the nighttime NO 3 radical reaction being important loss processes. Products of the OH radical and NO 3 radical reactions were analyzed by gas chromatography with flame ionization detection and combined gas chromatography-mass spectrometry. N-methylsuccinimide and (tentatively) 1-formyl-2-pyrrolidinone were identified as products of both of these reactions. The measured formation yields of N-methylsuccinimide and 1-formyl-2-pyrrolidinone were 44±12% and 41±12%, respectively, from the OH radical reaction and 59±16% and ˜4%, respectively, from the NO 3 radical reaction. Reaction mechanisms consistent with formation of these products are presented.

  10. Atmospheric chemistry of i-butanol.

    PubMed

    Andersen, V F; Wallington, T J; Nielsen, O J

    2010-12-02

    Smog chamber/FTIR techniques were used to determine rate constants of k(Cl + i-butanol) = (2.06 ± 0.40) × 10(-10), k(Cl + i-butyraldehyde) = (1.37 ± 0.08) × 10(-10), and k(OH + i-butanol) = (1.14 ± 0.17) × 10(-11) cm(3) molecule(-1) s(-1) in 700 Torr of N(2)/O(2) diluent at 296 ± 2K. The UV irradiation of i-butanol/Cl(2)/N(2) mixtures gave i-butyraldehyde in a molar yield of 53 ± 3%. The chlorine atom initiated oxidation of i-butanol in the absence of NO gave i-butyraldehyde in a molar yield of 48 ± 3%. The chlorine atom initiated oxidation of i-butanol in the presence of NO gave (molar yields): i-butyraldehyde (46 ± 3%), acetone (35 ± 3%), and formaldehyde (49 ± 3%). The OH radical initiated oxidation of i-butanol in the presence of NO gave acetone in a yield of 61 ± 4%. The reaction of chlorine atoms with i-butanol proceeds 51 ± 5% via attack on the α-position to give an α-hydroxy alkyl radical that reacts with O(2) to give i-butyraldehyde. The atmospheric fate of (CH(3))(2)C(O)CH(2)OH alkoxy radicals is decomposition to acetone and CH(2)OH radicals. The atmospheric fate of OCH(2)(CH(3))CHCH(2)OH alkoxy radicals is decomposition to formaldehyde and CH(3)CHCH(2)OH radicals. The results are consistent with, and serve to validate, the mechanism that has been assumed in the estimation of the photochemical ozone creation potential of i-butanol.

  11. Chemistry of Atmospheres: An Introduction to the Chemistry of the Atmospheres of Earth, the Planets and Their Satellites

    NASA Astrophysics Data System (ADS)

    Beebe, Reta; Barnet, Chris

    The author of this book states that he has attempted to produce a text that will be “intelligible to readers approaching atmospheric chemistry from any scientific discipline.” He proposes to provide the links between atmospheric chemistry and the traditional approaches to physics, chemistry, and biology. Within this context, he has presented a very readable general discussion at a level slightly higher than the popular level.Wayne has chosen not to interrupt the text with direct references but rather to group them at the back of each chapter. Although this sometimes raises a question concerning the basis of a specific statement, the references are in general adequate and extend through 1984. The manner in which the material is presented is not intimidating, and the book would be a good vehicle for introducing students to the subject and providing a starting point for individual research papers.

  12. Multiple steady states in atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Stewart, Richard W.

    1993-01-01

    The equations describing the distributions and concentrations of trace species are nonlinear and may thus possess more than one solution. This paper develops methods for searching for multiple physical solutions to chemical continuity equations and applies these to subsets of equations describing tropospheric chemistry. The calculations are carried out with a box model and use two basic strategies. The first strategy is a 'search' method. This involves fixing model parameters at specified values, choosing a wide range of initial guesses at a solution, and using a Newton-Raphson technique to determine if different initial points converge to different solutions. The second strategy involves a set of techniques known as homotopy methods. These do not require an initial guess, are globally convergent, and are guaranteed, in principle, to find all solutions of the continuity equations. The first method is efficient but essentially 'hit or miss' in the sense that it cannot guarantee that all solutions which may exist will be found. The second method is computationally burdensome but can, in principle, determine all the solutions of a photochemical system. Multiple solutions have been found for models that contain a basic complement of photochemical reactions involving O(x), HO(x), NO(x), and CH4. In the present calculations, transitions occur between stable branches of a multiple solution set as a control parameter is varied. These transitions are manifestations of hysteresis phenomena in the photochemical system and may be triggered by increasing the NO flux or decreasing the CH4 flux from current mean tropospheric levels.

  13. Multiple steady states in atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Stewart, Richard W.

    1993-01-01

    The equations describing the distributions and concentrations of trace species are nonlinear and may thus possess more than one solution. This paper develops methods for searching for multiple physical solutions to chemical continuity equations and applies these to subsets of equations describing tropospheric chemistry. The calculations are carried out with a box model and use two basic strategies. The first strategy is a 'search' method. This involves fixing model parameters at specified values, choosing a wide range of initial guesses at a solution, and using a Newton-Raphson technique to determine if different initial points converge to different solutions. The second strategy involves a set of techniques known as homotopy methods. These do not require an initial guess, are globally convergent, and are guaranteed, in principle, to find all solutions of the continuity equations. The first method is efficient but essentially 'hit or miss' in the sense that it cannot guarantee that all solutions which may exist will be found. The second method is computationally burdensome but can, in principle, determine all the solutions of a photochemical system. Multiple solutions have been found for models that contain a basic complement of photochemical reactions involving O(x), HO(x), NO(x), and CH4. In the present calculations, transitions occur between stable branches of a multiple solution set as a control parameter is varied. These transitions are manifestations of hysteresis phenomena in the photochemical system and may be triggered by increasing the NO flux or decreasing the CH4 flux from current mean tropospheric levels.

  14. NASA's Upper Atmosphere Research Program (UARP) and Atmospheric Chemistry Modeling and Analysis Program (ACMAP): Research Summaries 1997-1999

    NASA Technical Reports Server (NTRS)

    Kurylo, M. J.; DeCola, P. L.; Kaye, J. A.

    2000-01-01

    Under the mandate contained in the FY 1976 NASA Authorization Act, the National Aeronautics and Space Administration (NASA) has developed and is implementing a comprehensive program of research, technology development, and monitoring of the Earth's upper atmosphere, with emphasis on the upper troposphere and stratosphere. This program aims at expanding our chemical and physical understanding to permit both the quantitative analysis of current perturbations as well as the assessment of possible future changes in this important region of our environment. It is carried out jointly by the Upper Atmosphere Research Program (UARP) and the Atmospheric Chemistry Modeling and Analysis Program (ACMAP), both managed within the Research Division in the Office of Earth Science at NASA. Significant contributions to this effort have also been provided by the Atmospheric Effects of Aviation Project (AEAP) of NASA's Office of Aero-Space Technology. The long-term objectives of the present program are to perform research to: understand the physics, chemistry, and transport processes of the upper troposphere and the stratosphere and their control on the distribution of atmospheric chemical species such as ozone; assess possible perturbations to the composition of the atmosphere caused by human activities and natural phenomena (with a specific emphasis on trace gas geographical distributions, sources, and sinks and the role of trace gases in defining the chemical composition of the upper atmosphere); understand the processes affecting the distributions of radiatively active species in the atmosphere, and the importance of chemical-radiative-dynamical feedbacks on the meteorology and climatology of the stratosphere and troposphere; and understand ozone production, loss, and recovery in an atmosphere with increasing abundances of greenhouse gases. The current report is composed of two parts. Part 1 summarizes the objectives, status, and accomplishments of the research tasks supported

  15. Understanding atmospheric peroxyformic acid chemistry: observation, modeling and implication

    NASA Astrophysics Data System (ADS)

    Liang, H.; Chen, Z. M.; Huang, D.; Wu, Q. Q.; Huang, L. B.

    2015-01-01

    The existence and importance of peroxyformic acid (PFA) in the atmosphere has been under controversy. We present here, for the first time, the observation data for PFA from four field measurements carried out in China. These data provided powerful evidence that PFA can stay in the atmosphere, typically in dozens of pptv level. The relationship between PFA and other detected peroxides was examined. The results showed that PFA had a strong positive correlation with its homolog, peroxyacetic acid, due to their similar sources and sinks. Through an evaluation of PFA production and removal rates, we proposed that the reactions between peroxyformyl radical (HC(O)O2) and formaldehyde or the hydroperoxyl radical (HO2) were likely to be the major source and degradation into formic acid (FA) was likely to be the major sink for PFA. Based on a box model evaluation, we proposed that the HC(O)O2 and PFA chemistry was a major source for FA under low NOx conditions. Furthermore, it is found that the impact of the HC(O)O2 and PFA chemistry on radical cycling was dependent on the yield of HC(O)O2 radical from HC(O) + O2 reaction. When this yield exceeded 50%, the HC(O)O2 and PFA chemistry should not be neglected for calculating the radical budget. To make clear the exact importance of HC(O)O2 and PFA chemistry in the atmosphere, further kinetic, field and modeling studies are required.

  16. THE ATMOSPHERIC CHEMISTRY OF GJ 1214b: PHOTOCHEMISTRY AND CLOUDS

    SciTech Connect

    Miller-Ricci Kempton, Eliza; Fortney, Jonathan J.; Zahnle, Kevin

    2012-01-20

    Recent observations of the transiting super-Earth GJ 1214b reveal that its atmosphere may be hydrogen-rich or water-rich in nature, with clouds or hazes potentially affecting its transmission spectrum in the optical and very-near-IR. Here, we further examine the possibility that GJ 1214b does indeed possess a hydrogen-dominated atmosphere, which is the hypothesis that is favored by models of the bulk composition of the planet. We study the effects of non-equilibrium chemistry (photochemistry, thermal chemistry, and mixing) on the planet's transmission spectrum. We furthermore examine the possibility that clouds could play a significant role in attenuating GJ 1214b's transmission spectrum at short wavelengths. We find that non-equilibrium chemistry can have a large effect on the overall chemical composition of GJ 1214b's atmosphere, however these changes mostly take place above the height in the atmosphere that is probed by transmission spectroscopy. The effects of non-equilibrium chemistry on GJ 1214b's transmission spectrum are therefore minimal, with the largest effects taking place if the planet's atmosphere has super-solar metallicity and a low rate of vertical mixing. Interestingly, we find that the best fit to the observations of GJ 1214b's atmosphere in transmission occurs if the planet's atmosphere is deficient in CH{sub 4}, and possesses a cloud layer at a pressure of {approx}200 mbar. This is consistent with a picture of efficient methane photolysis, accompanied by formation of organic haze that obscures the lower atmosphere of GJ 1214b at optical wavelengths. However, for methane to be absent from GJ 1214b's transmission spectrum, UV photolysis of this molecule must be efficient at pressures of greater than {approx}1 mbar, whereas we find that methane only photolyzes to pressures less than 0.1 mbar, even under the most optimistic assumptions. An alternative explanation of the observations of GJ 1214b is that the atmosphere is water-rich, although this

  17. The atmospheric chemistry of Po-218

    SciTech Connect

    Hopke, P.K.

    1990-09-30

    The chemical and physical properties of {sup 218}Po immediately following its formation from {sup 222}Rn decay are important in determining its behavior in indoor atmospheres and plays a major part in determining its potential health effects. In 88% of the decays, a singly charged positive ion of {sup 218}Po is obtained at the end of its recoil path. The neutralization rates for Po-218 by the small ion recombination, electron transfer or electron scavenging mechanisms were previously reported. We have measured the small ion recombination rate in high purity gases to determine the negative small ion production rate as a function of the ionization potential of the gas. Our previous studies have also shown that radiolysis of water vapor by the recoiling Po ion produces high local concentrations of hydroxyl ({center dot}OH) radicals. These radicals can lead to oxidation of reactive trace gases and the neutral polonium molecule can become incorporated in ultrafine particles formed by the nucleation of low vapor pressure compounds produced by this radical oxidation process. The hydroxyl radical production rate and the production of particles are currently being studied. 12 refs., 1 fig.

  18. Modelling trace gas chemistry in the Martian atmosphere

    NASA Astrophysics Data System (ADS)

    Duffy, M. K. D.; Lewis, S. R.; Mason, N. J.

    2012-09-01

    Dust-bourne heterogeneous reactions have been modelled using the UK Mars Global Circulation Model (MGCM) coupled with physics and chemistry schemes used in the Laboratoire de Météorologie Dynamique (LMD) MGCM. The seasonal ozone column abundance has been calculated using a number of different dust scenarios. Reactions involving volcanically interesting species such as water vapour, SO2 and HCl have been included and tracer release experiments have been conducted to mimic short and long-term volcanic outgassing. The effect of these new reactions on the bulk chemistry of the Martian atmosphere has been quantified.

  19. The THS experiment: probing Titan's atmospheric chemistry at low temperature

    NASA Astrophysics Data System (ADS)

    Sciamma-O'Brien, Ella; Upton, Kathleen; Beauchamp, Jack L; Salama, Farid

    2014-06-01

    In Titan’s atmosphere, a complex chemistry between N2 and CH4 occurs at temperatures lower than 200K and leads to the production of heavy molecules and subsequently solid aerosols that form the haze surrounding Titan. The Titan Haze Simulation (THS) experiment has been developed at the NASA Ames COSmIC facility to study Titan’s atmospheric chemistry at low temperature in order to help interpret Cassini’s observational data. In the THS, the chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas is jet-cooled to Titan-like temperature 150K) before inducing the chemistry by plasma, and remains at low temperature in the plasma discharge 200K). Different N2-CH4-based gas mixtures can be injected in the plasma, with or without the addition of heavier precursors present as trace elements on Titan. Both the gas phase and solid phase products resulting from the plasma-induced chemistry can be monitored and analyzed using a combination of complementary in situ and ex situ diagnostics.Here we present the complementary results of two studies of the gas and solid phase. A Mass spectrometry analysis of the gas phase has demonstrated that the THS experiment is a unique tool to probe the first and intermediate steps as well as specific chemical pathways of Titan’s atmospheric chemistry at Titan-like temperature. The more complex chemistry, observed in the gas phase when adding trace elements to the initial N2-CH4 mixture, has also been confirmed by an extensive study of the solid phase products: Scanning Electron Microscopy images have shown that aggregates produced in N2-CH4-C2H2-C6H6 mixtures (up to 5 μm in diameter) are much larger than those produced in N2-CH4 mixtures (0.1-0.5 μm), and Nuclear Magnetic Resonance results support a growth evolution of the chemistry when adding acetylene to the N2-CH4 mixture, resulting in the production of more complex hydrogen bonds than with a simple N2-CH4 mixture

  20. New observational constraints on hydrocarbon chemistry in Saturn's upper atmosphere

    NASA Astrophysics Data System (ADS)

    Koskinen, Tommi; Moses, Julianne I.; West, Robert; Guerlet, Sandrine; Jouchoux, Alain

    2016-10-01

    Until now there have been only a few observations of hydrocarbons and photochemical haze in the region where they are produced in Saturn's upper atmosphere. We present new results on hydrocarbon abundances and atmospheric structure based on more than 40 stellar occultations observed by the Cassini/UVIS instrument that we have combined with results from Cassini/CIRS to generate full atmosphere structure models. In addition to detecting CH4, C2H2, C2H4 and C2H6, we detect benzene (C6H6) in UVIS occultations that probe different latitudes and present the first vertical abundance profiles for this species in its production region. Benzene is the simplest ring polyaromatic hydrocarbon (PAH) and a stepping stone to the formation of more complex molecules that are believed to form stratospheric haze. Our calculations show that the observed abundances of benzene can be explained by solar-driven ion chemistry that is enhanced by high-latitude auroral production at least in the northern spring hemisphere. Condensation of benzene and heavier hydrocarbons is possible in the cold polar night of the southern winter where we detect evidence for high altitude haze. We also report on substantial variability in the CH4 profiles that arise from dynamics and affects the minor hydrocarbon abundances. Our results demonstrate the importance of hydrocarbon ion chemistry and coupled models of chemistry and dynamics for future studies of Saturn's upper atmosphere.

  1. The DaVinci Project: Multimedia in Art and Chemistry.

    ERIC Educational Resources Information Center

    Simonson, Michael; Schlosser, Charles

    1998-01-01

    Provides an overview of the DaVinci Project, a collaboration of students, teachers, and researchers in chemistry and art to develop multimedia materials for grades 3-12 visualizing basic concepts in chemistry and visual art. Topics addressed include standards in art and science; the conceptual framework for the project; and project goals,…

  2. The DaVinci Project: Multimedia in Art and Chemistry.

    ERIC Educational Resources Information Center

    Simonson, Michael; Schlosser, Charles

    1998-01-01

    Provides an overview of the DaVinci Project, a collaboration of students, teachers, and researchers in chemistry and art to develop multimedia materials for grades 3-12 visualizing basic concepts in chemistry and visual art. Topics addressed include standards in art and science; the conceptual framework for the project; and project goals,…

  3. Studies of Arctic Middle Atmosphere Chemistry using Infrared Absorption Spectroscopy

    NASA Astrophysics Data System (ADS)

    Lindenmaier, Rodica

    The objective of this Ph.D. project is to investigate Arctic middle atmosphere chemistry using solar infrared absorption spectroscopy. These measurements were made at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Nunavut, which is operated by the Canadian Network for the Detection of Atmospheric Change (CANDAC). This research is part of the CANDAC/PEARL Arctic Middle Atmosphere Chemistry theme and aims to improve our understanding of the processes controlling the stratospheric ozone budget using measurements of the concentrations of stratospheric constituents. The instrument, a Bruker IFS 125HR Fourier transform infrared (FTIR) spectrometer, has been specifically designed for high-resolution measurements over a broad spectral range and has been used to measure reactive species, source gases, reservoirs, and dynamical tracers at PEARL since August 2006. The first part of this research focuses on the optimization of ozone retrievals, for which 22 microwindows were studied and compared. The spectral region from 1000 to 1005 cm-1 was found to be the most sensitive in both the stratosphere and troposphere, giving the highest number of independent pieces of information and the smallest total error for retrievals at Eureka. Similar studies were performed in coordination with the Network for the Detection of Atmospheric Composition Change for nine other species, with the goal of improving and harmonizing the retrieval parameters among all Infrared Working Group sites. Previous satellite validation exercises have identified the highly variable polar conditions of the spring period to be a challenge. In this work, comparisons between the 125HR and ACE-FTS (Atmospheric Chemistry Experiment-Fourier transform spectrometer) from 2007 to 2010 have been used to develop strict criteria that allow the ground and satellite-based instruments to be confidently compared. After applying these criteria, the differences between the two instruments were generally

  4. What makes urban atmospheric chemistry different and special?

    NASA Astrophysics Data System (ADS)

    Harrison, Roy M.

    2016-04-01

    There has been a tendency in the atmospheric chemistry community to regard urban atmospheric chemistry as no different to global processes and to differentiate only in terms of the emissions density in models. Such an approach may be suitable for assessing the impact of urban emissions upon regional and global processes but is unsuited to generating a clear understanding of processes within the urban atmosphere itself. The urban atmosphere differentiates itself from the global atmosphere in terms of its density of emissions and relatively short timescales for chemical reaction processes, a consequence of which is that the key processes in the urban atmosphere are often different from those in the regional and remote atmosphere. This lecture will give relevant examples. One of the key aspects of both urban and rural/remote atmospheres is the oxidation of primary pollutants and the formation of secondary species. Such processes may differ markedly between urban and non-urban environments as there are major differences in the behaviour of key oxidants such as ozone, hydroxyl and NO3 radical. In the remote atmosphere the key production process for hydroxyl is through the photolysis of ozone to form excited state oxygen atoms which react with water vapour to form OH. In the urban atmosphere, concentrations of ozone are typically depressed relative to the rural atmosphere and hence this source of OH is less favourable. There are likely to be much higher concentrations of both nitrous acid and formaldehyde in the urban atmosphere whose photolysis is probably the major source of OH. Additionally, there is far more possibility for nocturnal formation of OH in the urban atmosphere from reactions of Criegee intermediates resulting from the oxidation of alkenes. As a consequence, it has been shown that winter to summer ratios of hydroxyl radical concentrations are much higher in the urban atmosphere than is typical of rural atmospheres in northern mid-latitudes. In rural

  5. Research for the advancement of green chemistry practice: Studies in atmospheric and educational chemistry

    NASA Astrophysics Data System (ADS)

    Cullipher, Steven Gene

    Green chemistry is a philosophy of chemistry that emphasizes a decreasing dependence on limited non-renewable resources and an increasing focus on preventing pollution byproducts of the chemical industry. In short, it is the discipline of chemistry practiced through the lens of environmental stewardship. In an effort to advance the practice of green chemistry, three studies will be described that have ramifications for the practice. The first study examines the atmospheric oxidation of a hydrofluorinated ether, a third-generation CFC replacement compound with primarily unknown atmospheric degradation products. Determination of these products has the potential to impact decisions on refrigerant usage in the future. The second study examines chemistry students' development of understanding benefits-costs-risks analysis when presented with two real-world scenarios: refrigerant choice and fuel choice. By studying how benefits-costs-risks thinking develops, curricular materials and instructional approaches can be designed to better foster the development of an ability that is both necessary for green chemists and important in daily decision-making for non-chemists. The final study uses eye tracking technology to examine students' abilities to interpret molecular properties from structural information in the context of global warming. Such abilities are fundamental if chemists are to appropriately assess risks and hazards of chemistry practice.

  6. Chemistry of the surface and lower atmosphere of Venus

    NASA Technical Reports Server (NTRS)

    Fegley, B., Jr.; Treiman, A.

    1992-01-01

    A comprehensive overview of the chemical interactions between the atmosphere and surface of Venus is presented. Earth-based, earth-orbital, and spacecraft data on the composition of the atmosphere and surface of Venus are presented and applied to quantitative evaluations of the chemical interactions between carbon, hydrogen, sulfur, chlorine, fluorine, and nitrogen-containing gases and possible minerals on the Venus surface. The calculation results are used to predict stable minerals and mineral assemblages on the Venus surface to determine which, if any, atmospheric gases are buffered by mineral assemblages on the surface, and to critically review and assess prior work on atmosphere-surface chemistry on Venus. It is concluded that the CO2 pressure on Venus is comparable to the CO2 equilibrium partial pressure developed by the calcite + wollastonite + quartz assemblage at the mean Venus surface temperature of 740 K.

  7. Chemistry of the surface and lower atmosphere of Venus

    NASA Technical Reports Server (NTRS)

    Fegley, B., Jr.; Treiman, A.

    1992-01-01

    A comprehensive overview of the chemical interactions between the atmosphere and surface of Venus is presented. Earth-based, earth-orbital, and spacecraft data on the composition of the atmosphere and surface of Venus are presented and applied to quantitative evaluations of the chemical interactions between carbon, hydrogen, sulfur, chlorine, fluorine, and nitrogen-containing gases and possible minerals on the Venus surface. The calculation results are used to predict stable minerals and mineral assemblages on the Venus surface to determine which, if any, atmospheric gases are buffered by mineral assemblages on the surface, and to critically review and assess prior work on atmosphere-surface chemistry on Venus. It is concluded that the CO2 pressure on Venus is comparable to the CO2 equilibrium partial pressure developed by the calcite + wollastonite + quartz assemblage at the mean Venus surface temperature of 740 K.

  8. Relationships Between Atmospheric Aerosols and Snow Chemistry at Denali, Alaska

    NASA Astrophysics Data System (ADS)

    Burzynski, A. M.; Osterberg, E. C.; Kreutz, K. J.; Wake, C. P.; Campbell, S. W.

    2013-12-01

    Ice cores are important tools in paleoclimate studies as they provide long-term, high-resolution archives of atmospheric composition beyond the scope of modern instrumental records. To use ice core chemical records to reconstruct past climate and atmospheric composition, it is necessary to understand how snow chemistry relates to air chemistry and to identify the source regions of air masses influencing the ice core sites. Air-snow chemistry transfer functions are not fully understood and these relationships tend to be site-specific. For example, results found on ice sheets may not apply to mountainous regions because of differences in aerosol deposition mechanisms, proximity to source regions, and seasonality of precipitation and melt. Here we show that significant correlations between ice core chemistry and regionally sampled atmospheric aerosols are highly element specific in Denali, a central Alaskan mountainous region. Ice core chemistry records from Mount Hunter (62.938 -151.083, 3900m elev.) and Kahiltna Pass (63.075 -151.173, 3000m elev.) were compared to aerosol monitoring stations at Denali Headquarters (63.7233 -148.9675, 658m elev.) over the years 2000-2009. Significant correlations (p<.05) are shown between Mount Hunter ice core chemistry and the IMPROVE aerosol records at Denali Headquarters at annual resolution for Al, As, Ca, Cr, Fe, Pb, Mn, K, Sr, S, Ti and at seasonal resolution for Al, Ca, Fe Mn, Sr, S, and Ti. Some elements are particularly sensitive to sample timing, as illustrated by Mg and Na sampled by IMPROVE and CASTNET at Denali Headquarters over 2001-2004. Spatial and elevation variation are also factors in this region. Cu, Zn, As, V SO4 and NO3 sampled by IMPROVE at Denali Headquarters and Trapper Creek (62.3153 -150.3156,155m elev.) show spatial variability over 2001-2004. HYSPLIT atmospheric back-trajectory model analysis characterizes the air mass source regions at the ice core sites and lower elevation aerosol sampling sites

  9. The coupled atmosphere-chemistry-ocean model SOCOL-MPIOM

    NASA Astrophysics Data System (ADS)

    Muthers, S.; Anet, J. G.; Stenke, A.; Raible, C. C.; Rozanov, E.; Brönnimann, S.; Peter, T.; Arfeuille, F. X.; Shapiro, A. I.; Beer, J.; Steinhilber, F.; Brugnara, Y.; Schmutz, W.

    2014-09-01

    The newly developed atmosphere-ocean-chemistry-climate model SOCOL-MPIOM is presented by demonstrating the influence of chemistry-climate interactions on the climate state and the variability. Therefore, we compare pre-industrial control simulations with (CHEM) and without (NOCHEM) interactive chemistry. In general, the influence of the chemistry on the mean state and the variability is small and mainly restricted to the stratosphere and mesosphere. The atmospheric dynamics mainly differ in polar regions, with slightly stronger polar vortices in the austral and boreal winter, respectively. The strengthening of the vortex is related to larger stratospheric temperature gradients, which are attributed to a parameterisation of the absorption of ozone and oxygen in different wavelength intervals, which is considered in the version with interactive chemistry only. A second reason for the temperature differences between CHEM and NOCHEM is related to diurnal variations in the ozone concentrations in the higher atmosphere, which are missing in NOCHEM. Furthermore, stratospheric water vapour concentrations substantially differ between the two experiments, but their effect on temperature is small. In both setups, the simulated intensity and variability of the northern polar vortex is inside the range of present-day observations. Additionally, the performance of SOCOL-MPIOM under changing external forcings is assessed for the period 1600-2000 using an ensemble of simulations. In the industrial period from 1850 onward SOCOL-MPIOM overestimates the global mean surface air temperature increase in comparison to observational data sets. Sensitivity simulations show that this overestimation can be attributed to a combination of factors: the solar forcing reconstruction, the simulated ozone changes, and incomplete aerosol effects and land use changes.

  10. The Role of Chemistry in Atmosphere-Forest Exchange (Invited)

    NASA Astrophysics Data System (ADS)

    Thornton, J. A.; Wolfe, G. M.; Bouvier-Brown, N. C.; Goldstein, A. H.; Park, J.; McKay, M.; Matross, D. M.; Mao, J.; Brune, W. H.; Lafranchi, B. W.; Browne, E. C.; Min, K.; Wooldridge, P. J.; Cohen, R. C.; Crounse, J.; Faloona, I. C.; Gilman, J. B.; Kuster, W. C.; de Gouw, J. A.; Huisman, A. J.; Keutsch, F. N.

    2010-12-01

    Forest-atmosphere exchange of hydrocarbons, ozone, oxidized nitrogen and other reactive species impacts both atmospheric composition and ecosystem productivity, with broad implications for air quality and climate. Recent interpretations of measured ozone and acyl peroxy nitrate fluxes have inferred that intra-canopy chemistry plays an important role in governing both the sign and magnitude of the atmosphere-forest flux of these compounds. I review these observational insights and present results from a recently constructed 1-D vertically-resolved chemical transport model (CAFE) developed for analysis and interpretation of observations made during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX). The model incorporates a fully resolved forest canopy; emissions from which are parameterized, in many cases, to match leaf-level and top-of-canopy fluxes measured at the ponderosa pine plantation. Model chemistry is based on the Master Chemical Mechanism (MCM), with several additions to simulate the oxidation of monoterpenes and sesquiterpenes not in the current MCM. The base model underestimates measured noontime OH concentrations by a factor of six. As a result we invoke enhanced OH-recycling from first generation isoprene and 2-methyl-3-buten-2-ol peroxy radicals to reconcile model and observed HOx components. Noting a few other aspects of model performance, I will focus on the model predictions of chemistry-induced fluxes. The model qualitatively reproduces the inferred sensitivity to intra-canopy chemistry for both ozone and acyl peroxy nitrates. In both cases, however, the model underestimates the observed exchange velocity suggesting non-stomatal losses (depositional or chemical) remain underestimated in the canopy. As an example of the potential importance of intra-canopy chemistry, the meteorological and structural characteristics of the forest are varied within the model. An intriguing result is that acyl peroxy nitrate (e.g., PAN) fluxes

  11. Evaluated kinetic and photochemical data for atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Baulch, D. L.; Cox, R. A.; Hampson, R. F., Jr.; Kerr, J. A.; Troe, J.; Watson, R. T.

    1980-01-01

    This paper contains a critical evaluation of the kinetics and photochemistry of gas phase chemical reactions of neutral species involved in middle atmosphere chemistry (10-55 km altitude). Data sheets have been prepared for 148 thermal and photochemical reactions, containing summaries of the available experimental data with notes giving details of the experimental procedures. For each reaction a preferred value of the rate coefficient at 298 K is given together with a temperature dependency where possible. The selection of the preferred value is discussed, and estimates of the accuracies of the rate coefficients and temperature coefficients have been made for each reaction. The data sheets are intended to provide the basic physical chemical data needed as input for calculations which model atmospheric chemistry. A table summarizing the preferred rate data is provided, together with an appendix listing the available data on enthalpies of formation of the reactant and product species.

  12. Vibrational Spectroscopy of Photoreactive Molecules in Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Vaida, Veronica

    2010-06-01

    Vibrational overtone spectra of oxidized atmospheric chromophores are presented and analyzed to energies where chemistry through vibrational overtone pumping is possible. Experimental near infrared and visible spectra complemented by dynamical theory are presented to elucidate the light initiated reaction dynamics of pyruvic and of glyoxilic acid photo-decarboxylation. The role of water is investigated by making use of vibrational spectra of hydrates of the title compounds. Consequences of water and sunlight mediated chemistry to formation of secondary organic aerosol in the atmosphere will be discussed. K. L. Plath, J. L. Axson, G. C. Nelson, K. Takahashi, R. T. Skodje and V. Vaida -- React. Kineti. Catal. Lett. 96, 209 (2009) V. Vaida J. Phys. Chem. A 113, 5 (2009) K. Takahashi, K. L. Plath, R. T. Skodje and V. Vaida J. Phys. Chem A 112 7321 (2008)

  13. An Overview of Atmospheric Chemistry and Air Quality Modeling

    NASA Technical Reports Server (NTRS)

    Johnson, Matthew S.

    2017-01-01

    This presentation will include my personal research experience and an overview of atmospheric chemistry and air quality modeling to the participants of the NASA Student Airborne Research Program (SARP 2017). The presentation will also provide examples on ways to apply airborne observations for chemical transport (CTM) and air quality (AQ) model evaluation. CTM and AQ models are important tools in understanding tropospheric-stratospheric composition, atmospheric chemistry processes, meteorology, and air quality. This presentation will focus on how NASA scientist currently apply CTM and AQ models to better understand these topics. Finally, the importance of airborne observation in evaluating these topics and how in situ and remote sensing observations can be used to evaluate and improve CTM and AQ model predictions will be highlighted.

  14. Evaluated kinetic and photochemical data for atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Baulch, D. L.; Cox, R. A.; Hampson, R. F., Jr.; Kerr, J. A.; Troe, J.; Watson, R. T.

    1980-01-01

    This paper contains a critical evaluation of the kinetics and photochemistry of gas phase chemical reactions of neutral species involved in middle atmosphere chemistry (10-55 km altitude). Data sheets have been prepared for 148 thermal and photochemical reactions, containing summaries of the available experimental data with notes giving details of the experimental procedures. For each reaction a preferred value of the rate coefficient at 298 K is given together with a temperature dependency where possible. The selection of the preferred value is discussed, and estimates of the accuracies of the rate coefficients and temperature coefficients have been made for each reaction. The data sheets are intended to provide the basic physical chemical data needed as input for calculations which model atmospheric chemistry. A table summarizing the preferred rate data is provided, together with an appendix listing the available data on enthalpies of formation of the reactant and product species.

  15. Recent Discoveries and Future Challenges in Atmospheric Organic Chemistry.

    PubMed

    Glasius, Marianne; Goldstein, Allen H

    2016-03-15

    Earth's atmosphere contains a multitude of organic compounds, which differ by orders of magnitude regarding fundamental properties such as volatility, reactivity, and propensity to form cloud droplets, affecting their impact on global climate and human health. Despite recent major research efforts and advances, there are still substantial gaps in understanding of atmospheric organic chemistry, hampering efforts to understand, model, and mitigate environmental problems such as aerosol formation in both polluted urban and more pristine regions. The analytical toolbox available for chemists to study atmospheric organic components has expanded considerably during the past decade, opening new windows into speciation, time resolution and detection of reactive and semivolatile compounds at low concentrations. This has provided unprecedented opportunities, but also unveiled new scientific challenges. Specific groundbreaking examples include the role of epoxides in aerosol formation especially from isoprene, the importance of highly oxidized, reactive organics in air-surface processes (whether atmosphere-biosphere exchange or aerosols), as well as the extent of interactions of anthropogenic and biogenic emissions and the resulting impact on atmospheric organic chemistry.

  16. Isotopic evidence for Mesoarchaean anoxia and changing atmospheric sulphur chemistry.

    PubMed

    Farquhar, James; Peters, Marc; Johnston, David T; Strauss, Harald; Masterson, Andrew; Wiechert, Uwe; Kaufman, Alan J

    2007-10-11

    The evolution of the Earth's atmosphere is marked by a transition from an early atmosphere with very low oxygen content to one with an oxygen content within a few per cent of the present atmospheric level. Placing time constraints on this transition is of interest because it identifies the time when oxidative weathering became efficient, when ocean chemistry was transformed by delivery of oxygen and sulphate, and when a large part of Earth's ecology changed from anaerobic to aerobic. The observation of non-mass-dependent sulphur isotope ratios in sedimentary rocks more than approximately 2.45 billion years (2.45 Gyr) old and the disappearance of this signal in younger sediments is taken as one of the strongest lines of evidence for the transition from an anoxic to an oxic atmosphere around 2.45 Gyr ago. Detailed examination of the sulphur isotope record before 2.45 Gyr ago also reveals early and late periods of large amplitude non-mass-dependent signals bracketing an intervening period when the signal was attenuated. Until recently, this record has been too sparse to allow interpretation, but collection of new data has prompted some workers to argue that the Mesoarchaean interval (3.2-2.8 Gyr ago) lacks a non-mass-dependent signal, and records the effects of earlier and possibly permanent oxygenation of the Earth's atmosphere. Here we focus on the Mesoarchaean interval, and demonstrate preservation of a non-mass-dependent signal that differs from that of preceding and following periods in the Archaean. Our findings point to the persistence of an anoxic early atmosphere, and identify variability within the isotope record that suggests changes in pre-2.45-Gyr-ago atmospheric pathways for non-mass-dependent chemistry and in the ultraviolet transparency of an evolving early atmosphere.

  17. Role of Double Hydrogen Atom Transfer Reactions in Atmospheric Chemistry.

    PubMed

    Kumar, Manoj; Sinha, Amitabha; Francisco, Joseph S

    2016-05-17

    Hydrogen atom transfer (HAT) reactions are ubiquitous and play a crucial role in chemistries occurring in the atmosphere, biology, and industry. In the atmosphere, the most common and traditional HAT reaction is that associated with the OH radical abstracting a hydrogen atom from the plethora of organic molecules in the troposphere via R-H + OH → R + H2O. This reaction motif involves a single hydrogen transfer. More recently, in the literature, there is an emerging framework for a new class of HAT reactions that involves double hydrogen transfers. These reactions are broadly classified into four categories: (i) addition, (ii) elimination, (iii) substitution, and (iv) rearrangement. Hydration and dehydration are classic examples of addition and elimination reactions, respectively whereas tautomerization or isomerization belongs to a class of rearrangement reactions. Atmospheric acids and water typically mediate these reactions. Organic and inorganic acids are present in appreciable levels in the atmosphere and are capable of facilitating two-point hydrogen bonding interactions with oxygenates possessing an hydroxyl and/or carbonyl-type functionality. As a result, acids influence the reactivity of oxygenates and, thus, the energetics and kinetics of their HAT-based chemistries. The steric and electronic effects of acids play an important role in determining the efficacy of acid catalysis. Acids that reduce the steric strain of 1:1 substrate···acid complex are generally better catalysts. Among a family of monocarboxylic acids, the electronic effects become important; barrier to the catalyzed reaction correlates strongly with the pKa of the acid. Under acid catalysis, the hydration of carbonyl compounds leads to the barrierless formation of diols, which can serve as seed particles for atmospheric aerosol growth. The hydration of sulfur trioxide, which is the principle mechanism for atmospheric sulfuric acid formation, also becomes barrierless under acid catalysis

  18. Cassini atmospheric chemistry mapper. Volume 1. Investigation and technical plan

    NASA Technical Reports Server (NTRS)

    Smith, William Hayden; Baines, Kevin Hays; Drossart, Pierre; Fegley, Bruce; Orton, Glenn; Noll, Keith; Reitsema, Harold; Bjoraker, Gordon L.

    1990-01-01

    The Cassini Atmospheric Chemistry Mapper (ACM) enables a broad range of atmospheric science investigations for Saturn and Titan by providing high spectral and spatial resolution mapping and occultation capabilities at 3 and 5 microns. ACM can directly address the major atmospheric science objectives for Saturn and for Titan, as defined by the Announcement of Opportunity, with pivotal diagnostic measurements not accessible to any other proposed Cassini instrument. ACM determines mixing ratios for atmospheric molecules from spectral line profiles for an important and extensive volume of the atmosphere of Saturn (and Jupiter). Spatial and vertical profiles of disequilibrium species abundances define Saturn's deep atmosphere, its chemistry, and its vertical transport phenomena. ACM spectral maps provide a unique means to interpret atmospheric conditions in the deep (approximately 1000 bar) atmosphere of Saturn. Deep chemistry and vertical transport is inferred from the vertical and horizontal distribution of a series of disequilibrium species. Solar occultations provide a method to bridge the altitude range in Saturn's (and Titan's) atmosphere that is not accessible to radio science, thermal infrared, and UV spectroscopy with temperature measurements to plus or minus 2K from the analysis of molecular line ratios and to attain an high sensitivity for low-abundance chemical species in the very large column densities that may be achieved during occultations for Saturn. For Titan, ACM solar occultations yield very well resolved (1/6 scale height) vertical mixing ratios column abundances for atmospheric molecular constituents. Occultations also provide for detecting abundant species very high in the upper atmosphere, while at greater depths, detecting the isotopes of C and O, constraining the production mechanisms, and/or sources for the above species. ACM measures the vertical and horizontal distribution of aerosols via their opacity at 3 microns and, particularly, at 5

  19. Portsmouth Atmospheric Science School (PASS) Project

    NASA Technical Reports Server (NTRS)

    Coleman, Clarence D.; Hathaway, Roger (Technical Monitor)

    2002-01-01

    The Portsmouth Atmospheric Science School Project (PASS) Project was granted a one-year no cost extension for 2001-2002. In year three of the project, objectives and strategies were modified based on the previous year-end evaluation. The recommendations were incorporated and the program was replicated within most of the remaining elementary schools in Portsmouth, Virginia and continued in the four middle schools. The Portsmouth Atmospheric Science School Project is a partnership, which includes Norfolk State University, Cooperating Hampton Roads Organizations for Minorities in Engineering (CHROME), NASA Langley Research Center, and the City of Portsmouth, Virginia Public Schools. The project seeks to strengthen the knowledge of Portsmouth Public Schools students in the field of atmospheric sciences and enhance teacher awareness of hands on activities in the atmospheric sciences. The project specifically seeks to: 1) increase the interest and participation of elementary and middle school students in science and mathematics; 2) strengthen existing science programs; and 3) facilitate greater achievement in core subjects, which are necessary for math, science, and technical careers. Emphasis was placed on providing training activities, materials and resources for elementary students (grades 3 - 5) and middle school students (grades 6 - 8), and teachers through a CHROME club structure. The first year of the project focused on introducing elementary students to concepts and activities in atmospheric science. Year two of the project built on the first year's activities and utilizes advanced topics and activities appropriate for middle school students. During the third year of the project, in addition to the approaches used in years one and two, emphasis was placed on activities that enhanced the Virginia Standards of Learning (SOL).

  20. Particle precipitation: How the spectrum fit impacts atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Wissing, J. M.; Nieder, H.; Yakovchouk, O. S.; Sinnhuber, M.

    2016-11-01

    Particle precipitation causes atmospheric ionization. Modeled ionization rates are widely used in atmospheric chemistry/climate simulations of the upper atmosphere. As ionization rates are based on particle measurements some assumptions concerning the energy spectrum are required. While detectors measure particles binned into certain energy ranges only, the calculation of a ionization profile needs a fit for the whole energy spectrum. Therefore the following assumptions are needed: (a) fit function (e.g. power-law or Maxwellian), (b) energy range, (c) amount of segments in the spectral fit, (d) fixed or variable positions of intersections between these segments. The aim of this paper is to quantify the impact of different assumptions on ionization rates as well as their consequences for atmospheric chemistry modeling. As the assumptions about the particle spectrum are independent from the ionization model itself the results of this paper are not restricted to a single ionization model, even though the Atmospheric Ionization Module OSnabrück (AIMOS, Wissing and Kallenrode, 2009) is used here. We include protons only as this allows us to trace changes in the chemistry model directly back to the different assumptions without the need to interpret superposed ionization profiles. However, since every particle species requires a particle spectrum fit with the mentioned assumptions the results are generally applicable to all precipitating particles. The reader may argue that the selection of assumptions of the particle fit is of minor interest, but we would like to emphasize on this topic as it is a major, if not the main, source of discrepancies between different ionization models (and reality). Depending on the assumptions single ionization profiles may vary by a factor of 5, long-term calculations may show systematic over- or underestimation in specific altitudes and even for ideal setups the definition of the energy-range involves an intrinsic 25% uncertainty for the

  1. An Atmospheric Instrument Development Outreach Project

    NASA Astrophysics Data System (ADS)

    Guerra, David; Cordella, Nick; Bracy, Sue

    2002-04-01

    In an effort to cultivate the interest in atmospheric science of middle school students, we have established a long-term outreach program in which students become active participants in an instrument development study. This project was motivated by the low cost, $20.00, hand-held haze detector (HHHD) developed by Forrest Mims III and the capabilities of the instruments located 5 miles away as part of the Saint Anselm Atmospheric Sensing Experiment (SAASE). The focus of the project, for the past two academic years, has been the development and data collected with two different HHHDs, operated by eighth graders from Mountain View Middle School (MVMS). This data is then compared to the solar irradiance measurements made with SAASE's automated multifilter shadow band radiometer (MFSBR). This type of outreach project not only teaches students about the atmosphere but also the process of instrument development and the creative aspects of science.

  2. IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry

    SciTech Connect

    Atkinson, R.; Baulch, D.L.; Cox, R.A.; Hampson, R.F. Jr.; Kerr, J.A.; Rossi, M.J.; Troe, J.

    1997-11-01

    This paper updates and extends part of the previous data base of critical evaluations of the kinetics and photochemistry of gas-phase chemical reactions of neutral species involved in atmospheric chemistry [J. Phys. Chem. Ref. Data {bold 9}, 295 (1980); {bold 11}, 327 (1982); {bold 13}, 1259 (1984); {bold 18}, 881 (1989); {bold 21}, 1125 (1992); {bold 26}, 521 (1997)]. The present evaluation is limited to the following families of atmospherically important reactions: O{sub x}, HO{sub x}, NO{sub x}, and SO{sub x}. The work has been carried out by the authors under the auspices of the IUPAC Subcommittee on Gas Phase Kinetic Data Evaluation for Atmospheric Chemistry. Data sheets have been prepared for 151 thermal and photochemical reactions, containing summaries of the available experimental data with notes giving details of the experimental procedures. For each thermal reaction, a preferred value of the rate coefficient at 298 K is given together with a temperature dependence where possible. The selection of the preferred value is discussed and estimates of the accuracies of the rate coefficients and temperature coefficients have been made for each reaction. For each photochemical reaction the data sheets list the preferred values of the photoabsorption cross-sections and the quantum yields of the photochemical reactions together with comments on how they were selected. The data sheets are intended to provide the basic physical chemical data needed as input for calculations which model atmospheric chemistry. A table summarizing the preferred rate data is provided, together with an appendix listing the available data on enthalpies of formation of the reactant and product species. {copyright} {ital 1997 American Institute of Physics and American Chemical Society.}

  3. Putting a Human Face on Chemistry: A Project for Liberal Arts Chemistry.

    ERIC Educational Resources Information Center

    Kriz, George; Popejoy, Kate

    A collaborative project in liberal arts chemistry, involving faculty in chemistry and science education, is described. The project includes various components: an introductory test (DAST) to examine students' perceptions of scientists, a group library research exercise, oral and written presentation of the results of the library research, a…

  4. Post-Cassini Investigations of Titan Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Hörst, Sarah M.

    chemistry occurring in Titan's upper atmosphere may be capable of forming incredibly complex organic molecules, which may have implications for the origin of life on Earth and elsewhere in the universe. %K Atmosphere, Cassini, Chemistry, Tholins, Titan

  5. Systematic evaluation of atmospheric chemistry-transport model CHIMERE

    NASA Astrophysics Data System (ADS)

    Khvorostyanov, Dmitry; Menut, Laurent; Mailler, Sylvain; Siour, Guillaume; Couvidat, Florian; Bessagnet, Bertrand; Turquety, Solene

    2017-04-01

    Regional-scale atmospheric chemistry-transport models (CTM) are used to develop air quality regulatory measures, to support environmentally sensitive decisions in the industry, and to address variety of scientific questions involving the atmospheric composition. Model performance evaluation with measurement data is critical to understand their limits and the degree of confidence in model results. CHIMERE CTM (http://www.lmd.polytechnique.fr/chimere/) is a French national tool for operational forecast and decision support and is widely used in the international research community in various areas of atmospheric chemistry and physics, climate, and environment (http://www.lmd.polytechnique.fr/chimere/CW-articles.php). This work presents the model evaluation framework applied systematically to the new CHIMERE CTM versions in the course of the continuous model development. The framework uses three of the four CTM evaluation types identified by the Environmental Protection Agency (EPA) and the American Meteorological Society (AMS): operational, diagnostic, and dynamic. It allows to compare the overall model performance in subsequent model versions (operational evaluation), identify specific processes and/or model inputs that could be improved (diagnostic evaluation), and test the model sensitivity to the changes in air quality, such as emission reductions and meteorological events (dynamic evaluation). The observation datasets currently used for the evaluation are: EMEP (surface concentrations), AERONET (optical depths), and WOUDC (ozone sounding profiles). The framework is implemented as an automated processing chain and allows interactive exploration of the results via a web interface.

  6. Stability of the Martian atmosphere: Possible role of heterogeneous chemistry

    SciTech Connect

    Atreya, S.K. ); Blamont, J.E. )

    1990-03-01

    A new hypothesis is proposed for recycling Martian CO to CO{sub 2}. The same hypothesis can satisfactorily explain the recently observed depletion in CO in the middle atmosphere of Mars. The mechanism involves oxidation of carbon monoxide through heterogeneous chemistry in the presence of aerosols. It is further suggested that H{sub 2}O ice aerosols in the atmosphere of Mars are particularly effective in this process. The thrust for suggesting this mechanism came from the extensive presence of aerosols in the Martian atmosphere detected by the Auguste-Spectrophotometer Interferometer experiment on the Phobos spacecraft, combined with similar results from earlier missions, the detection of relatively low CO mixing ratios in the low to middle atmosphere by the Infrared Spectrometer experiment on the Phobos spacecraft, and the fact that earlier proposed mechanisms for recycling CO{sub 2} require either unacceptably high values of the eddy diffusion coefficient or a high water vapor abundance in the middle atmosphere of Mars. The mechanism proposed in this paper might have an analog in the Antarctic ozone hole problem, and it points out a need for laboratory measurements of appropriate sticking coefficients and rate constants.

  7. Spectroscopy and chemistry of the atmosphere of Uranus

    NASA Technical Reports Server (NTRS)

    Fegley, Bruce, Jr.; Gautier, Daniel; Owen, Tobias; Prinn, Ronald G.

    1991-01-01

    A comprehensive review of the chemistry and spectroscopy of the Uranian atmosphere is presented by means of earth-based, earth-orbital, and Voyager 2 observations covering the UV, visible, infrared, and radio wavelength regions. It is inferred from these observations, in concert with the average density of about 1.3 g/cu cm, that the Uranian atmosphere is enriched in heavy elements relative to solar composition. Pre-Voyager earth-based observations of CH4 bands in the visible region and Voyager radio occultation data imply a CH4/H2 volume mixing ratio of about 2 percent corresponding to an enrichment of approximately 24 times the solar value of 0.000835. In contrast to CH4, microwave observations indicate an apparent depletion of NH3 in the 155-to-200-K region of the atmosphere by 100 to 200 times relative to the solar NH3/H2 mixing ratio of -0.000174. It is suggested that the temporal and latitudinal variations deduced for the NH3/H2 mixing ratio in this region of the Uranian atmosphere are due to atmospheric circulation effects.

  8. Spectroscopy and chemistry of the atmosphere of Uranus

    NASA Technical Reports Server (NTRS)

    Fegley, Bruce, Jr.; Gautier, Daniel; Owen, Tobias; Prinn, Ronald G.

    1991-01-01

    A comprehensive review of the chemistry and spectroscopy of the Uranian atmosphere is presented by means of earth-based, earth-orbital, and Voyager 2 observations covering the UV, visible, infrared, and radio wavelength regions. It is inferred from these observations, in concert with the average density of about 1.3 g/cu cm, that the Uranian atmosphere is enriched in heavy elements relative to solar composition. Pre-Voyager earth-based observations of CH4 bands in the visible region and Voyager radio occultation data imply a CH4/H2 volume mixing ratio of about 2 percent corresponding to an enrichment of approximately 24 times the solar value of 0.000835. In contrast to CH4, microwave observations indicate an apparent depletion of NH3 in the 155-to-200-K region of the atmosphere by 100 to 200 times relative to the solar NH3/H2 mixing ratio of -0.000174. It is suggested that the temporal and latitudinal variations deduced for the NH3/H2 mixing ratio in this region of the Uranian atmosphere are due to atmospheric circulation effects.

  9. The coupled atmosphere-chemistry-ocean model SOCOL-MPIOM

    NASA Astrophysics Data System (ADS)

    Muthers, S.; Anet, J. G.; Stenke, A.; Raible, C. C.; Rozanov, E.; Brönnimann, S.; Peter, T.; Arfeuille, F. X.; Shapiro, A. I.; Beer, J.; Steinhilber, F.; Brugnara, Y.; Schmutz, W.

    2014-05-01

    The newly developed atmosphere-ocean-chemistry-climate model SOCOL-MPIOM is presented by demonstrating the influence of the interactive chemistry module on the climate state and the variability. Therefore, we compare pre-industrial control simulations with (CHEM) and without (NOCHEM) interactive chemistry. In general, the influence of the chemistry on the mean state and the variability is small and mainly restricted to the stratosphere and mesosphere. The largest differences are found for the atmospheric dynamics in the polar regions, with slightly stronger northern and southern winter polar vortices in CHEM. The strengthening of the vortex is related to larger stratospheric temperature gradients, which are attributed to a parametrization of the absorption of ozone and oxygen in the Lyman-alpha, Schumann-Runge, Hartley, and Higgins bands. This effect is parametrized in the version with interactive chemistry only. A second reason for the temperature differences between CHEM and NOCHEM is related to diurnal variations in the ozone concentrations in the higher atmosphere, which are missing in NOCHEM. Furthermore, stratospheric water vapour concentrations differ substantially between the two experiments, but their effect on the temperatures is small. In both setups, the simulated intensity and variability of the northern polar vortex is inside the range of present day observations. Sudden stratospheric warming events are well reproduced in terms of their frequency, but the distribution amongst the winter months is too uniform. Additionally, the performance of SOCOL-MPIOM under changing external forcings is assessed for the period 1600-2000 using an ensemble of simulations driven by a spectral solar forcing reconstruction. The amplitude of the reconstruction is large in comparison to other state-of-the-art reconstructions, providing an upper limit for the importance of the solar signal. In the pre-industrial period (1600-1850) the simulated surface temperature trends

  10. Composition and Chemistry of the Neutral Atmosphere of Venus

    NASA Astrophysics Data System (ADS)

    Marcq, E.; Millis, F.; Sandor, B.; Vandaele, A. C.

    2014-04-01

    With the pending ending of the ESA Venus Express mission after 8 years of scientific success, a new page in the in situ exploration of the inner solar system is on the verge of being turned. Considering how much our vision of Venus has been updated and refined thanks to it, the scientific community has decided to summarize our new picture of Venus in a dedicated book. This talk aims at presenting the structure and some contents of the Composition and Chemistry of the Neutral Atmosphere chapter.

  11. STREAMWATER ACID-BASED CHEMISTRY AND CRITICAL LOADS OF ATMOSPHERIC SULFUR DEPOSITION IN SHENANDOAH NATIONAL PARK, VIRGINIA

    EPA Science Inventory

    A modeling study was conducted to evaluate the acid-base chemistry of streams within Shenandoah National Park, Virginia and to project future responses to sulfur (S) and nitrogen (N) atmospheric emissions controls. Many of the major stream systems in the Park have acid neutraliz...

  12. STREAMWATER ACID-BASED CHEMISTRY AND CRITICAL LOADS OF ATMOSPHERIC SULFUR DEPOSITION IN SHENANDOAH NATIONAL PARK, VIRGINIA

    EPA Science Inventory

    A modeling study was conducted to evaluate the acid-base chemistry of streams within Shenandoah National Park, Virginia and to project future responses to sulfur (S) and nitrogen (N) atmospheric emissions controls. Many of the major stream systems in the Park have acid neutraliz...

  13. Global phosgene observations from the Atmospheric Chemistry Experiment (ACE) mission

    NASA Astrophysics Data System (ADS)

    Fu, Dejian; Boone, Chris D.; Bernath, Peter F.; Walker, Kaley A.; Nassar, Ray; Manney, Gloria L.; McLeod, Sean D.

    2007-09-01

    The first study of the global distribution of atmospheric phosgene (COCl2) has been performed using solar occultation measurements from the Atmospheric Chemistry Experiment (ACE) satellite mission. A total of 5614 measured profiles spanning the period February 2004 through May 2006 were used in the study. The phosgene concentrations display a zonally symmetric pattern with the maximum concentration located approximately over the equator at about 25 km in altitude and the concentration decreases towards the poles. A layer of enhanced concentration of phosgene spans the lower stratosphere over all latitudes, with volume mixing ratios of 20-60 pptv. The ACE observations show lower phosgene concentrations in the stratosphere than were obtained from previous observations in the 1980s and 1990s. This has been attributed to a significant decrease in its source species, particularly two major sources CH3CCl3 and CCl4, since the introduction of restrictions required by the Montreal Protocol and its amendments.

  14. EDITORIAL: Ice in the environment: connections to atmospheric chemistry Ice in the environment: connections to atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    McNeill, V. Faye; Hastings, Meredith G.

    2008-12-01

    Ice in the environment, whether in the form of ice particles in clouds or sea ice and snow at the Earth's surface, has a profound influence on atmospheric composition and climate. The interaction of trace atmospheric gases with snow and sea ice surfaces largely controls atmospheric composition in polar regions. The heterogeneous chemistry of ice particles in clouds also plays critical roles in polar stratospheric ozone depletion and in tropospheric chemistry. A quantitative physical understanding of the interactions of snow and ice with trace gases is critical for predicting the effects of climate change on atmospheric composition, for the interpretation of ice core chemical records, and for modeling atmospheric chemistry. The motivation behind this focus issue of Environmental Research Letters (ERL), and the special session at the Fall 2007 meeting of the American Geophysical Union that generated it, was to enhance communication and interactions among field and laboratory scientists and modelers working in this area. Members of these three groups are each working toward a mutual goal of understanding and quantifying the connections between the chemistry of snow and ice in the environment and atmospheric composition, and communication and collaboration across these traditional disciplinary boundaries pose a challenge for the community. We are pleased to present new work from several current leaders in the field and laboratory communities in this focus issue. Topics include the interaction of organics and mercury with snow and ice surfaces, halogen activation from halide ice, and the emissions of reactive nitrogen oxides from snow. Novel experimental techniques are presented that make progress towards overcoming the experimental challenges of quantifying the chemistry of realistic snow samples and ice chemistry at temperatures relevant to the polar boundary layer. Several of the papers in this issue also touch on one of the significant gaps in our current

  15. Evaluation of Chemistry Climate Model Projections for Ozone Recovery using Network for Detection of Atmospheric Composition Change (NDACC) Column Measurements of Chlorine Reservoirs HCl and ClONO2

    NASA Astrophysics Data System (ADS)

    Douglass, A. R.; Strahan, S. E.; Stolarski, R. S.

    2012-12-01

    Nearly identical conceptual models of the stratospheric processes underlie the group of chemistry climate models that participated in CCMVal-2 and the Scientific Assessment of Ozone Depletion: 2010. However, there are differences in the future simulations of the evolution of ozone as chlorofluorcarbons decrease and the stratosphere cools due to increases in greenhouse gases. Column ozone decreases in every CCM as chlorine increases, and in the absence of climate change would return to 1980 levels when chlorine compounds returned to 1980 levels as specified by boundary conditions. Climate change also affects stratospheric ozone: a) ozone increases throughout the upper stratosphere due to cooling; b) acceleration of the Brewer Dobson circulation decreases tropical ozone, but increases ozone in the middle and high latitudes due to increased downwelling. The overall simulated impact of climate change on stratospheric ozone is positive, thus the computed 60S - 60N average returns to 1980 values years before chlorine levels reach 1980 values. Although all models show the same qualitative results, they differ in their quantification of the chemistry-climate interaction. In an effort to understand model differences in chemistry-climate interactions, we compare computed columns for reservoir gases ground-based measurements of HCl and ClONO2 columns obtained by various stations in the Network for Detection of Atmospheric Composition Change (NDAAC). We note that both the maximum value of inorganic chlorine and partitioning vary among models but timeseries from CCMs with good performance on CCMVal transport tests compare remarkably well with observations. The lower stratospheric ClONO2 columns are shown to be linearly related to the simulated sensitivity to chlorine. Variation in the rate of change of upwelling as well as differences in the pattern of enhanced downwelling contribute substantially to the variation in the return year. We also show that the annual cycle obtained

  16. The global change research center atmospheric chemistry model

    SciTech Connect

    Moraes, Jr., Francis Perry

    1995-01-01

    This work outlines the development of a new model of the chemistry of the natural atmosphere. The model is 2.5-dimensional, having spatial coordinates height, latitude, and, the half-dimension, land and ocean. The model spans both the troposphere and stratosphere, although the troposphere is emphasized and the stratosphere is simple and incomplete. The chemistry in the model includes the Ox, HOx, NOx, and methane cycles in a highly modular fashion which allows model users great flexibility in selecting simulation parameters. A detailed modeled sensitivity analysis is also presented. A key aspect of the model is its inclusion of clouds. The model uses current understanding of the distribution and optical thickness of clouds to determine the true radiation distribution in the atmosphere. As a result, detailed studies of the radiative effects of clouds on the distribution of both oxidant concentrations and trace gas removal are possible. This work presents a beginning of this study with model results and discussion of cloud effects on the hydroxyl radical.

  17. Chemistry of Atmospheric Aerosols at Pacifichem 2015 Congress

    SciTech Connect

    Nizkorodov, Sergey

    2016-12-28

    This grant was used to provide participant support for a symposium entitled “Chemistry of Atmospheric Aerosols” at the 2015 International Chemical Congress of Pacific Basin Societies (Pacifichem) that took place in Honolulu, Hawaii, USA, on December 15-20, 2015. The objective was to help attract both distinguished scientists as well as more junior researchers, including graduate students, to this international symposium by reducing the financial barrier for its attendance. It was the second time a symposium devoted to Atmospheric Aerosols was part of the Pacifichem program. This symposium provided a unique opportunity for the scientists from different countries to gather in one place and discuss the cutting edge advances in the cross-disciplinary areas of aerosol research. To achieve the highest possible impact, the PI and the symposium co-organizers actively advertised the symposium by e-mail and by announcements at other conferences. A number of people responded, and the end result was a very busy program with about 100 oral and poster presentation described in the attached PDF file. Presentations by invited speakers occupied approximately 30% of time in each of the sessions. In addition to the invited speakers, each session also had contributed presentations, including those by graduate students and postdoctoral researchers. This symposium gathered established aerosol chemists from a number of countries including United States, Canada, China, Japan, Korea, Australia, Brazil, Hongkong, Switzerland, France, and Germany. There were plenty of time for the attendees to discuss new ideas and potential collaborations both during the oral sessions and at the poster sessions of the symposium. The symposium was very beneficial to graduate student researchers, postdoctoral fellows, and junior researchers whose prior exposure to international aerosol chemistry science had been limited. The symposium provided junior researchers with a much broader perspective of aerosol

  18. "The Chemicals Project": Connecting General Chemistry to Students' Lives

    NASA Astrophysics Data System (ADS)

    Stout, Roland

    2000-10-01

    "The Chemicals Project" described here strives to bring freshman chemistry alive for students by emphasizing its connection to the real world and to their own lives and experiences. Its major assignments deal with chemical phobias, recognizing the chemicals found in everyday life and chemical hazards (using Material Data Safety Sheets). The project is described in a cooperative learning format, employs portfolio grading, and includes a significant writing component. Ways of linking this project with the course lecture and student evaluations of the project are described. The bottom line: pre- and post-testing shows that it works. The Chemicals Project brings chemistry alive for students.

  19. The 1-way on-line coupled atmospheric chemistry model system MECO(n) - Part 1: The limited-area atmospheric chemistry model COSMO/MESSy

    NASA Astrophysics Data System (ADS)

    Kerkweg, A.; Jöckel, P.

    2011-06-01

    The numerical weather prediction model of the Consortium for Small Scale Modelling (COSMO), maintained by the German weather service (DWD), is connected with the Modular Earth Submodel System (MESSy). This effort is undertaken in preparation of a~new, limited-area atmospheric chemistry model. This model is as consistent as possible, with respect to atmospheric chemistry and related processes, with a previously developed global atmospheric chemistry general circulation model: the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. The combined system constitutes a new research tool, bridging the global to the meso-γ scale for atmospheric chemistry research. MESSy provides the infrastructure and includes, among others, the process and diagnostic submodels for atmospheric chemistry simulations. Furthermore, MESSy is highly flexible allowing model setups with tailor made complexity, depending on the scientific question. Here, the connection of the MESSy infrastructure to the COSMO model is documented. Previously published prototype submodels for simplified tracer studies are generalised to be plugged-in and used in the global and the limited-area model. They are used to evaluate the tracer transport characteristics of the new COSMO/MESSy model system, an important prerequisite for future atmospheric chemistry applications. A supplementary document with further details on the technical implementation of the MESSy interface into COSMO with a complete list of modifications to the COSMO code is provided.

  20. Chemistry of atmospheres - An introduction to the chemistry of the atmospheres of earth, the planets, and their satellites (2nd revised and enlarged edition)

    NASA Astrophysics Data System (ADS)

    Wayne, Richard P.

    An introduction to the chemistry of the atmospheres of the earth, the planets, and their satellites is presented, with particular attention given to the application of photochemistry and kinetics to atmospheres, ozone in the earth's stratosphere, the earth's troposphere, ions in the atmosphere, the airglow, and evolution and change in atmospheres and climates. This book presents the principles of atmospheric chemistry and provides the necessary background for more detailed study. New developments are covered, including the discovery of the Antarctic ozone hole. Information gathered by the Voyager 2 and other space missions is also discussed.

  1. Pilot Project for Chemistry Teaching in Asia.

    ERIC Educational Resources Information Center

    United Nations Educational, Scientific, and Cultural Organization, Bangkok (Thailand).

    The major portion of this publication is devoted to the presentation of 20 chemistry experiments dealing with corrosion of metals. The experiments are intended for high school level students or for chemistry teachers for demonstration purposes. Diagrams and illustrations accompany the written directions. Also included in this publication are…

  2. AEROCE - 10 Years of Atmospheric Chemistry at Bermuda

    NASA Astrophysics Data System (ADS)

    Savoie, D. L.

    2001-12-01

    The Atmosphere/Ocean Chemistry Experiment (AEROCE) was a comprehensive multi-disciplinary and multi-institutional research program that focused on a number of aspects of the atmospheric chemistry over the North Atlantic Ocean (NAO). These included: ozone and the oxidizing capacity of the atmosphere; aerosol physical and chemical properties (especially for sulfur and nitrogen species and mineral aerosol) and related precipitation chemistry; the role of aerosols in climate; and chemical air/sea exchange. Two major themes of AEROCE research were designed to (1) understand the role of anthropogenic emissions and natural processes in the ozone budget and oxidizing capacity of the troposphere over the North Atlantic Ocean (NAO) and (2) characterize the physical and chemical properties of aerosols that are important to the radiative properties of the atmosphere and to climate; to study the processes that affect these properties; and to assess the relative importance of natural and human sources. AEROCE focused on the atmosphere over the NAO because it is the ocean region that is most likely to be affected by atmospheric transport from the continents. The AEROCE station at Bermuda was an extremely important part of this program. Bermuda is the recipient of relatively clean marine air from the central North Atlantic as well as pollutants and natural continental materials from North America, Europe, and Africa. Seasonally, the highest ozone concentrations occur during the spring and are associated with transport off the North American continent. The highest daily ozone values occur under conditions of large-scale subsidence from the mid-troposphere in association with the passage of cold fronts across Bermuda. During the 1996 spring intensive field experiment, AEROCE researchers found that these high ozone concentrations resulted from a combination of downmixing from the stratosphere and production from precursors associated with North American pollution. The highest

  3. A Chemistry Laboratory Project to Develop Thinking and Writing Skills.

    ERIC Educational Resources Information Center

    Goodman, W. Daniel; Bean, John C.

    1983-01-01

    Describes a method for conducting a sophomore organic chemistry laboratory which included integrating projects with a writing task involving peer group interaction. Also includes background/theory, chemistry tasks, writing tasks, and evaluation. Included in appendices are an analytic worksheet and grading scale. (JN)

  4. Reactive greenhouse gas scenarios: Systematic exploration of uncertainties and the role of atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Prather, Michael J.; Holmes, Christopher D.; Hsu, Juno

    2012-05-01

    Knowledge of the atmospheric chemistry of reactive greenhouse gases is needed to accurately quantify the relationship between human activities and climate, and to incorporate uncertainty in our projections of greenhouse gas abundances. We present a method for estimating the fraction of greenhouse gases attributable to human activities, both currently and for future scenarios. Key variables used to calculate the atmospheric chemistry and budgets of major non-CO2 greenhouse gases are codified along with their uncertainties, and then used to project budgets and abundances under the new climate-change scenarios. This new approach uses our knowledge of changing abundances and lifetimes to estimate current total anthropogenic emissions, independently and possibly more accurately than inventory-based scenarios. We derive a present-day atmospheric lifetime for methane (CH4) of 9.1 ± 0.9 y and anthropogenic emissions of 352 ± 45 Tg/y (64% of total emissions). For N2O, corresponding values are 131 ± 10 y and 6.5 ± 1.3 TgN/y (41% of total); and for HFC-134a, the lifetime is 14.2 ± 1.5 y.

  5. Laboratory studies of low temperature rate coefficients: The atmospheric chemistry of the outer planets

    NASA Technical Reports Server (NTRS)

    Leone, Stephen R.

    1992-01-01

    The purpose of the project is to perform laboratory measurements of reaction rate coefficients at low temperature. The reactions and temperatures of interest are those that are important in the chemistry of the hydrocarbon rich atmospheres of the outer planets and their satellites. In this stage of the study we are investigating reactions of ethynyl radicals, C2H, with acetylene (C2H2), methane (CH4), and hydrogen (H2). In the previous status report from 24 Jan. 1992, we reported on the development of the experimental apparatus and the first, preliminary data for the C2H + C2H2 reaction.

  6. The Unsolved Mysteries of Atmospheric Chemistry for High School Students and Teachers

    NASA Astrophysics Data System (ADS)

    Simonich, S. L.

    2011-12-01

    The grant "CAREER: New Molecular Markers of Asian Air Emissions - Anthropogenic Semi-Volatile Organic Compounds" (ATM-0239823) was funded by NSF from 2003-2008. The CAREER proposal described the integration of research and outreach education activities in the field of atmospheric chemistry, specifically atmospheric measurements and atmospheric transport. The primary objective of the research was to identify anthropogenic semi-volatile organic compounds (SOCs) that could be used as molecular markers for Asian air emissions and trans-Pacific atmospheric transport. The outreach education activity was integrated with the research by developing curriculum to introduce underrepresented minority high school students, and their teachers, to atmospheric chemistry and atmospheric measurements through Oregon State University's National Institute of Environmental Health Sciences funded Hydroville Curriculum Project (http://www.hydroville.org/iaq_resources). A curriculum was developed to allow students to assume the role of "Air Quality Scientist" and measure air temperature, air flow, relative humidity, CO, CO2, O3, and volatile organic compounds in out-door and in-door air. The students gained an understanding of atmospheric transport and compared measured concentrations to recommended guidelines. In addition, the outreach education activities included the development of the "Unsolved Mysteries of Human Health" website (http://www.unsolvedmysteries.oregonstate.edu/), including a specific module on the research conducted under the CAREER grant (http://www.unsolvedmysteries.oregonstate.edu /Gas-Chromatography-Mass-Spectrometry-Overview). The PI of the CAREER proposal, Dr. Staci Massey Simonich, is now a full professor at Oregon State University. To date, she has published over 50 peer-review journal articles, as well as mentored 9 undergraduate students, 20 graduate students, 3 post-doctoral scholars, and 3 international visiting scientists in her laboratory.

  7. The Bio-atmospheric N Cycle: A Story of Multiple Element Interactions, N, C, S, Atmospheric Chemistry and the Climate System

    NASA Astrophysics Data System (ADS)

    Holland, E. A.

    2003-12-01

    The bio-atmospheric N plays a key role in the climate system through regulation of atmospheric greenhouse concentrations, including nitrous oxide, carbon dioxide, methane, and tropospheric ozone, as well as impacting aerosol abundance. I will examine the evidence for including the full bio-atmospheric nitrogen cycle into earth system models. The most obvious is the impact of the bio-atmospheric nitrogen cycle on nitrous and nitric oxide emissions. Nitrogen deposition significantly impacts terrestrial carbon dioxide uptake, as well as influencing leaf level nitrogen concentrations that in turn impact stomatal conductance. The importance of this interaction has been recognized by the atmospheric chemistry community and a modeling project is underway to quantify and compare global estimates of N deposition, including ammonia(um) and NOy and its impact on the carbon cycle. Ammonia impacts sulfate aerosol abundance as well as reacting with nitrate form aerosols that act as cloud condensation nuclei to he potential to significantly impact the water cycle. The SRES emission projections and an accumulating body of evidence suggest that sulfur dioxide emissions will decline over the next century, while carbon and nitrogen emissions, carbon dioxide, methane, carbon monoxide, and VOCs, and NOx are all projected to continue to increase. The long-term goal is an Earth System model that allows examination of the complex interactions of biology, climate, atmospheric chemistry and humans.

  8. The effects of atmospheric chemistry on radiation budget in the Community Earth Systems Model

    NASA Astrophysics Data System (ADS)

    Choi, Y.; Czader, B.; Diao, L.; Rodriguez, J.; Jeong, G.

    2013-12-01

    The Community Earth Systems Model (CESM)-Whole Atmosphere Community Climate Model (WACCM) simulations were performed to study the impact of atmospheric chemistry on the radiation budget over the surface within a weather prediction time scale. The secondary goal is to get a simplified and optimized chemistry module for the short time period. Three different chemistry modules were utilized to represent tropospheric and stratospheric chemistry, which differ in how their reactions and species are represented: (1) simplified tropospheric and stratospheric chemistry (approximately 30 species), (2) simplified tropospheric chemistry and comprehensive stratospheric chemistry from the Model of Ozone and Related Chemical Tracers, version 3 (MOZART-3, approximately 60 species), and (3) comprehensive tropospheric and stratospheric chemistry (MOZART-4, approximately 120 species). Our results indicate the different details in chemistry treatment from these model components affect the surface temperature and impact the radiation budget.

  9. Chemistry of atmospheric nucleation: on the recent advances on precursor characterization and atmospheric cluster composition in connection with atmospheric new particle formation.

    PubMed

    Kulmala, M; Petäjä, T; Ehn, M; Thornton, J; Sipilä, M; Worsnop, D R; Kerminen, V-M

    2014-01-01

    The recent development in measurement techniques and theoretical understanding has enabled us to study atmospheric vapor, cluster and nanoparticle concentrations, dynamics, and their connection to atmospheric nucleation. Here we present a summary of the chemistry of atmospheric clustering, growing nanoparticles, and their precursors. In this work, we focus particularly on atmospheric gas-to-particle conversion and recent progress in its understanding.

  10. Hydrogen atom initiated chemistry. [chemical evolution in planetary atmospheres

    NASA Technical Reports Server (NTRS)

    Hong, J. H.; Becker, R. S.

    1979-01-01

    H Atoms have been created by the photolysis of H2S. These then initiated reactions in mixtures involving acetylene-ammonia-water and ethylene-ammonia-water. In the case of the acetylene system, the products consisted of two amino acids, ethylene and a group of primarily cyclic thio-compounds, but no free sulfur. In the case of the ethylene systems, seven amino acids, including an aromatic one, ethane, free sulfur, and a group of solely linear thio-compounds were produced. Total quantum yields for the production of amino acids were about 3 x 10 to the -5th and about 2 x 10 to the -4th with ethylene and acetylene respectively as carbon substrates. Consideration is given of the mechanism for the formation of some of the products and implications regarding planetary atmosphere chemistry, particularly that of Jupiter, are explored.

  11. Hydrogen atom initiated chemistry. [chemical evolution in planetary atmospheres

    NASA Technical Reports Server (NTRS)

    Hong, J. H.; Becker, R. S.

    1979-01-01

    H Atoms have been created by the photolysis of H2S. These then initiated reactions in mixtures involving acetylene-ammonia-water and ethylene-ammonia-water. In the case of the acetylene system, the products consisted of two amino acids, ethylene and a group of primarily cyclic thio-compounds, but no free sulfur. In the case of the ethylene systems, seven amino acids, including an aromatic one, ethane, free sulfur, and a group of solely linear thio-compounds were produced. Total quantum yields for the production of amino acids were about 3 x 10 to the -5th and about 2 x 10 to the -4th with ethylene and acetylene respectively as carbon substrates. Consideration is given of the mechanism for the formation of some of the products and implications regarding planetary atmosphere chemistry, particularly that of Jupiter, are explored.

  12. TROPOLITE, on the path of atmospheric chemistry made simple

    NASA Astrophysics Data System (ADS)

    Maresi, Luca; Van Der Meulen, Wencke; Vink, Rob

    2014-10-01

    Accurate, reliable and stable long term measurements of Earth's Atmospheric Chemistry from Space are currently done by complex instruments, whose mass is in excess of 100 Kg. TROPOMI is the more recent instrument being developed jointly by ESA and NSO and due for launch in 2015. TROPOMI, consisting of four spectrometers ranging from UV to SWIR, is paving the way to the development of high performance spectrometers that will compose the backbone of the European Copernicus system. The objective of TROPOMI is to measure trace gases with an accuracy one order of magnitude better of what is currently done from Space. While teams of engineers are still busy finalizing TROPOMI, ESA, NSO, and TNO have launched an initiative along a different development axis: to explore the possibility of a lighter version of TROPOMI, to address a market valuing a cost effective instrument for Atmospheric Chemistry. TROPOLITE, as it is dubbed, leverages on all the technology developments and the lessons learnt from TROPOMI, but with the clear objective of a design to cost solution. Furthermore, mass and power of the instrument shall be within the envelope of a payload of a small satellite, namely 20kg and 30W and possibly within a volume of 20 x 20 x 40 cm3. The scope of TROPOLITE is to address a larger user base that is interested in an affordable instrument to perform from a small satellite some specific tasks relevant to Air Quality and/or Climate. The paper, after a short overview of the TROPOMI design and current status, presents the design philosophy of TROPOLITE, and shows what are the technologies and processes stemming from the experience gained with TROPOMI that make possible a simplified, but still very performing, version of TROPOMI. A comparison in terms of performance and functionalities of the two instruments is discussed. Finally, the development plan from the current development status of TROPOLITE up to Qualification Model is presented.

  13. A review of atmospheric chemistry observations at mountain sites

    NASA Astrophysics Data System (ADS)

    Okamoto, Sachiko; Tanimoto, Hiroshi

    2016-12-01

    Located far from anthropogenic emission sources, high-altitude mountain stations are considered to be ideal sites for monitoring climatic and environmentally important baseline changes in free tropospheric trace gases and aerosols. In addition, the observations taken at these stations are often used to study the long-range transport of dust as well as anthropogenic and biomass burning pollutants from source regions and to evaluate the performance of global and regional models. In this paper, we summarize the results from past and ongoing field measurements of atmospheric constituents at high-altitude stations across the globe, with particular emphasis on reactive trace species including tropospheric ozone, along with its precursors such as carbon monoxide, nitrogen oxides, total reactive nitrogen, and nonmethane hydrocarbons. Over the past decades, our understanding of the temporal variability and meteorological mechanisms of long-range transport has advanced in tandem with progress in instrumentation and modeling. Finally, the future needs of atmospheric chemistry observations at mountain sites are addressed.

  14. Incorporating Student-Designed Research Projects in the Chemistry Curriculum

    ERIC Educational Resources Information Center

    Iimoto, Devin S.; Frederick, Kimberley A.

    2011-01-01

    Although many chemistry students at small liberal arts colleges participate in undergraduate research projects with faculty members, they do not get much experience framing their own research questions and designing their own projects, which is an important part of science. We have implemented a developmental process to help students design and…

  15. Incorporating Student-Designed Research Projects in the Chemistry Curriculum

    ERIC Educational Resources Information Center

    Iimoto, Devin S.; Frederick, Kimberley A.

    2011-01-01

    Although many chemistry students at small liberal arts colleges participate in undergraduate research projects with faculty members, they do not get much experience framing their own research questions and designing their own projects, which is an important part of science. We have implemented a developmental process to help students design and…

  16. The 1-way on-line coupled atmospheric chemistry model system MECO(n) - Part 1: Description of the limited-area atmospheric chemistry model COSMO/MESSy

    NASA Astrophysics Data System (ADS)

    Kerkweg, A.; Jöckel, P.

    2012-01-01

    The numerical weather prediction model of the Consortium for Small Scale Modelling (COSMO), maintained by the German weather service (DWD), is connected with the Modular Earth Submodel System (MESSy). This effort is undertaken in preparation of a new, limited-area atmospheric chemistry model. Limited-area models require lateral boundary conditions for all prognostic variables. Therefore the quality of a regional chemistry model is expected to improve, if boundary conditions for the chemical constituents are provided by the driving model in consistence with the meteorological boundary conditions. The new developed model is as consistent as possible, with respect to atmospheric chemistry and related processes, with a previously developed global atmospheric chemistry general circulation model: the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. The combined system constitutes a new research tool, bridging the global to the meso-γ scale for atmospheric chemistry research. MESSy provides the infrastructure and includes, among others, the process and diagnostic submodels for atmospheric chemistry simulations. Furthermore, MESSy is highly flexible allowing model setups with tailor made complexity, depending on the scientific question. Here, the connection of the MESSy infrastructure to the COSMO model is documented and also the code changes required for the generalisation of regular MESSy submodels. Moreover, previously published prototype submodels for simplified tracer studies are generalised to be plugged-in and used in the global and the limited-area model. They are used to evaluate the TRACER interface implementation in the new COSMO/MESSy model system and the tracer transport characteristics, an important prerequisite for future atmospheric chemistry applications. A supplementary document with further details on the technical implementation of the MESSy interface into COSMO with a complete list of modifications to the COSMO code is provided.

  17. Chemistry, The Nuffield Foundation Science Teaching Project.

    ERIC Educational Resources Information Center

    Nuffield Foundation, London (England).

    A description of the Nuffield approach to Chemistry for students 11-16 years of age, a discussion of the possible entry points to the materials provided for the five years of British secondary schools before the "O"-Level examination, an account of the type of examination to be expected, and estimates of the cost of introducing the…

  18. Solar Energy Project, Activities: Chemistry & Physics.

    ERIC Educational Resources Information Center

    Tullock, Bruce, Ed.; And Others

    This guide contains lesson plans and outlines of science activities which present concepts of solar energy in the context of chemistry and physics experiments. Each unit presents an introduction to the unit; objectives; required skills and knowledge; materials; method; questions; recommendations for further work; and a teacher information sheet.…

  19. Implementing a Student-Designed Green Chemistry Laboratory Project in Organic Chemistry

    ERIC Educational Resources Information Center

    Graham, Kate J.; Jones, T. Nicholas; Schaller, Chris P.; McIntee, Edward J.

    2014-01-01

    A multiweek organic chemistry laboratory project is described that emphasizes sustainable practices in experimental design. An emphasis on student-driven development of the project is meant to mirror the independent nature of research. Students propose environmentally friendly modifications of several reactions. With instructor feedback, students…

  20. Implementing a Student-Designed Green Chemistry Laboratory Project in Organic Chemistry

    ERIC Educational Resources Information Center

    Graham, Kate J.; Jones, T. Nicholas; Schaller, Chris P.; McIntee, Edward J.

    2014-01-01

    A multiweek organic chemistry laboratory project is described that emphasizes sustainable practices in experimental design. An emphasis on student-driven development of the project is meant to mirror the independent nature of research. Students propose environmentally friendly modifications of several reactions. With instructor feedback, students…

  1. Street Canyon Atmospheric Composition: Coupling Dynamics and Chemistry

    NASA Astrophysics Data System (ADS)

    Bright, V.; Bloss, W. J.; Cai, X.

    2010-12-01

    Atmospheric composition within the urban environment, particularly within street canyons (formed by a road running between two rows of buildings), has a direct effect on the air quality of an environment in which a large majority of people live and work. The composition of air within a street canyon is determined by the composition of background air mixed in from above, advection of air into and out of the canyon, vehicle exhaust and other emissions from within the street, together with the mixing and chemical processing of pollutants within the canyon. This occurs on a timescale of a few seconds to minutes and as a result, within-canyon atmospheric processes can have a significant effect on atmospheric composition on such timescales. This paper outlines a modelling study of street canyon atmospheric composition, integrating the combined effects of emissions, dynamics and chemistry. This work builds upon an existing dynamical model of canyon atmospheric motion (Large Eddy Simulation (LES) model) by adding a detailed chemical reaction scheme. Previous studies have considered basic NOx-O3 cycles with only a small number of chemical reactions included. Initially, a zero-dimensional box model was used to develop and assess the accuracy of a suitable reduced chemical scheme to be included within the LES. The reduced chemical scheme, based upon a subset of the Master Chemical Mechanism (MCM), includes 51 chemical species and 136 reactions. Vehicle emissions taken from the UK National Atmospheric Emissions Inventory (NAEI) were subsequently added to the box model. These elements were then combined with the canyon dynamics simulated by the Large Eddy Simulation (LES) model. Results demonstrate that the enhanced model is a suitable tool to be used to further investigate the combined effects of mixing and chemical processing upon air quality within the street canyon. Subsequently, a number of key questions relating to urban atmospheric composition are addressed using the

  2. First Global Observations of Atmospheric COCIF from the Atmospheric Chemistry Experiment Mission

    NASA Technical Reports Server (NTRS)

    Fu, Dejian; Boone, Chris D.; Bernath, Peter F.; Weisenstein, Debra K.; Rinsland, Curtis P.; Manney, Gloria L.; Walker, Kaley A.

    2010-01-01

    Carbonyl chlorofluoride (COCIF) is an important reservoir of chlorine and fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COCIF, obtained by the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong source region for COCIF in the tropical stratosphere near 27 km. A layer of enhanced COCIF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts per trillion by volume, largest in the tropics and decreasing toward the poles. The COCIF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3 F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

  3. Appendix C: First Global Observations of Atmospheric COClF from the Atmospheric Chemistry Experiment Mission

    NASA Technical Reports Server (NTRS)

    Fu, Djian; Boone, Chris D.; Bernath, Peter F.; Walker, Kaley A.; Rinsland, Curtis P.; Weisenstein, Debra K.; Manney, Gloria L.

    2009-01-01

    Carbonyl chlorofluoride (COCIF) is an important reservoir of chlorine and Fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COCIF, obtained by Received in revised form the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong Accepted 18 February 2009 source region for COCIF in the tropical stratosphere near 27 km. A layer of enhanced COCIF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts Per trillion by volume, largest in the tropics and decreasing toward the poles. The COCIF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

  4. Microwave Studies of Chemistry of the Middle Atmosphere

    NASA Astrophysics Data System (ADS)

    Sandor, Brad J.

    The purpose of this study has been to investigate O_3 chemistry in Earth's middle atmosphere. The NRAO 12-meter radio telescope at Kitt Peak, AZ was used to observe lambda = 1 mm emission spectra of trace species at altitudes 50 -70 km. Brightness of the emission lines was used to determine abundance of the emitting species, and shapes of the pressure broadened lines were used to obtain altitude resolution of these abundances. Observations of ^{18}O^{16}O, CO, and O_3 were used to establish a calibration appropriate for atmospheric observations with a telescope primarily used for astronomical work. Diurnal variation of O_2(^1 Delta_{g}) was observed and compared with photochemical model results. Observed O_2(^1Delta_ {g}) abundances were 20% higher than model abundances, and model results can be brought into agreement with observations by reducing the rate coefficient for O_2(^1Delta_ {g}) quenching by 20% below the accepted value. The behavior of O_2(^1Delta _{g}) through the afternoon and evening was observed to agree with model calculations. Symmetric and asymmetric isotopomers of ^{50}O_3 were observed. Previous workers have found large, highly variable, and unexplained enhancements of ^{50}O _3 in the stratosphere. We extend the range of observations to the mesosphere. Significant variability in the abundance of the asymmetric isotopomer was observed. Diurnal variations of HO_2 were observed in conjunction with H_2O and O_3. Comparisons were made with photochemical model results. At mid-day HO _2 abundances were observed to be ~40% higher than model predictions. Model results for this time period can be brought into agreement with observations by reducing the rate coefficient for rm HO_2 + O--> OH + O _2 by 40%. Observed HO_2 altitude profiles in the early morning, late afternoon, and early evening are very different from model predictions.

  5. Urban Climate Effects on Air Pollution and Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Rasoul, Tara; Bloss, William; Pope, Francis

    2016-04-01

    Tropospheric ozone, adversely affects the environment and human health. The presence of chlorine nitrate (ClNO2) in the troposphere can enhance ozone (O3) formation as it undergoes photolysis, releasing chlorine reactive atoms (Cl) and nitrogen dioxide (NO2), both of which enhance tropospheric ozone formation. The importance of new sources of tropospheric ClNO2 via heterogeneous processes has recently been highlighted. This study employed a box model, using the Master Chemical Mechanism (MCM version 3.2) to assess the effect of ClNO2 on air quality in urban areas within the UK. The model updated to include ClNO2 production, photolysis, a comprehensive parameterisation of dinitrogen pentoxide (N2O5) uptake, and ClNO2 production calculated from bulk aerosol composition. The model simulation revealed the presence of ClNO2 enhances the formation of NO2, organic peroxy radical (CH3O2), O3, and hydroxyl radicals (OH) when compared with simulations excluding ClNO2. In addition, the study examined the effect of temperature variation upon ClNO2 formation. The response of ClNO2 to temperature was analysed to identify the underlying drivers, of particular importance when assessing the response of atmospheric chemistry processes under potential future climates.

  6. Molecular identification of organic compounds in atmospheric complex mixtures and relationship to atmospheric chemistry and sources.

    PubMed Central

    Mazurek, Monica A

    2002-01-01

    This article describes a chemical characterization approach for complex organic compound mixtures associated with fine atmospheric particles of diameters less than 2.5 m (PM2.5). It relates molecular- and bulk-level chemical characteristics of the complex mixture to atmospheric chemistry and to emission sources. Overall, the analytical approach describes the organic complex mixtures in terms of a chemical mass balance (CMB). Here, the complex mixture is related to a bulk elemental measurement (total carbon) and is broken down systematically into functional groups and molecular compositions. The CMB and molecular-level information can be used to understand the sources of the atmospheric fine particles through conversion of chromatographic data and by incorporation into receptor-based CMB models. Once described and quantified within a mass balance framework, the chemical profiles for aerosol organic matter can be applied to existing air quality issues. Examples include understanding health effects of PM2.5 and defining and controlling key sources of anthropogenic fine particles. Overall, the organic aerosol compositional data provide chemical information needed for effective PM2.5 management. PMID:12634131

  7. NASA's Atmospheric Effects of Aviation Project

    NASA Technical Reports Server (NTRS)

    Cofer, W. Randy, III; Anderson, Bruce E.; Connors, V. S.; Wey, C. C.; Sanders, T.; Winstead, E. L.; Pui, C.; Chen, Da-ren; Hagen, D. E.; Whitefield, P.

    2001-01-01

    During August 1-14, 1999, NASA's Atmospheric Effects of Aviation Project (AEAP) convened a workshop at the NASA Langley Research Center to try to determine why such a wide variation in aerosol emissions indices and chemical and physical properties has been reported by various independent AEAP-supported research teams trying to characterize the exhaust emissions of subsonic commercial aircraft. This workshop was divided into two phases, a laboratory phase and a field phase. The laboratory phase consisted of supplying known particle number densities (concentrations) and particle size distributions to a common manifold for the participating research teams to sample and analyze. The field phase was conducted on an aircraft run-up pad. Participating teams actually sampled aircraft exhaust generated by a Langley T-38 Talon aircraft at 1 and 9 m behind the engine at engine powers ranging from 48 to 100 percent. Results from the laboratory phase of this intercomparison workshop are reported in this paper.

  8. Nucla circulating atmospheric fluidized bed demonstration project

    SciTech Connect

    Keith, Raymond E.

    1991-10-01

    Colorado-Ute Electric Association began a study to evaluate options for upgrading and extending the life of its Nucla power station in 1982. Located in southwestern Colorado near the town of Nucla, this station was commissioned in 1959 with a local bituminous coal as its design fuel for three identical stoker-fired units, each rated at 12.6 MW(e). Poor station efficiency, high fuel costs, and spiraling boiler maintenance costs forced the Nucla Station into low priority in the CUEA dispatch order as early as 1981. Among the options CUEA considered was to serve as a host utility to demonstrate Atmospheric Fluidized Bed Combustion (AFBC) technology. The anticipated environmental benefits and apparent attractive economics of a circulating AFBC led to Colorado-Ute's decision to proceed with the design and construction of a demonstration project in 1984 at the Nucla facility.

  9. Some Tests For Adaptative Observations In Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Quélo, D.; Michelangeli, P.-A.; Sportisse, B.

    Air pollution forecast requires the coupling of models with data through data assimi- lation. A key question is related to the choice of observations (apart from technical require- ments). One wants to choose in a judicious way the species to observe, in which loca- tions and at which moments. The appropriate strategies are related to the techniques of "targeting" and "adaptative observations". We will investigate these techniques on a simplified model. The first part reports the influence of the slow-fast behaviour of atmospheric chem- istry. The second part presents the use of singular vectors and second-order adjoint techniques in order to determine the "optimal" choice of observations. This project is led in the framework of the INRIA Cooperative Research Action CO- MODE (COupling MOdels and Data in Environment).

  10. Atmospheric Ionizing Radiation (AIR) Project Review

    NASA Technical Reports Server (NTRS)

    Singleterry, R. C., Jr.; Wilson, J. W.; Whitehead, A. H.; Goldhagen, P. E.

    1999-01-01

    The National Council on Radiation Protection and Measurement (NCRP) and the National Academy of Science (NAS) established that the uncertainty in the data and models associated with the high-altitude radiation environment could and should be reduced. In response, the National Aeronautics and Space Administration (NASA) and the U.S. Department of Energy Environmental Measurements Laboratory (EML) created the Atmospheric Ionizing Radiation (AIR) Project under the auspices of the High Speed Research (HSR) Program Office at the Langley Research Center. NASA's HSR Program was developed to address the potential of a second-generation supersonic transport. A critical element focussed on the environmental issues, including the threat to crew and passengers posed by atmospheric radiation. Various international investigators were solicited to contribute instruments to fly on an ER-2 aircraft at altitudes similar to those proposed for the High Speed Civil Transport (HSCT). A list of participating investigators, their institutions, and instruments with quantities measured is presented. The flight series took place at solar minimum (radiation maximum) with northern, southern, and east/west flights. The investigators analyzed their data and presented preliminary results at the AIR Workshop in March, 1998. A review of these results are included.

  11. Chemistry-Materials Laboratory Project Book, 1979-80.

    ERIC Educational Resources Information Center

    Connecticut State Dept. of Education, Hartford. Bureau of Vocational-Technical Schools.

    This Chemistry-Materials Laboratory Project Book, assembled through a survey of science instructors in vocational-technical schools in Connecticut, is intended to meet a variety of needs. It can serve as an idea book, with the instructor taking from it as needed and adding or substituting material related to class interests; as a guide book for…

  12. Building Bridges between Science Courses Using Honors Organic Chemistry Projects

    ERIC Educational Resources Information Center

    Hickey, Timothy; Pontrello, Jason

    2016-01-01

    Introductory undergraduate science courses are traditionally offered as distinct units without formalized student interaction between classes. To bridge science courses, the authors used three Honors Organic Chemistry projects paired with other science courses. The honors students delivered presentations to mainstream organic course students and…

  13. Final-Year Education Projects for Undergraduate Chemistry Students

    ERIC Educational Resources Information Center

    Page, Elizabeth

    2011-01-01

    The Undergraduate Ambassadors Scheme provides an opportunity for students in their final year of the chemistry degree course at the University of Reading to choose an educational project as an alternative to practical research. The undergraduates work in schools where they can be regarded as role models and offer one way of inspiring pupils to…

  14. Building Bridges between Science Courses Using Honors Organic Chemistry Projects

    ERIC Educational Resources Information Center

    Hickey, Timothy; Pontrello, Jason

    2016-01-01

    Introductory undergraduate science courses are traditionally offered as distinct units without formalized student interaction between classes. To bridge science courses, the authors used three Honors Organic Chemistry projects paired with other science courses. The honors students delivered presentations to mainstream organic course students and…

  15. An Integrated Biology-Chemistry Freshman Laboratory Project in Biotechnology.

    ERIC Educational Resources Information Center

    Schendel, Marilyn Shimizu

    1999-01-01

    Describes a freshman biology laboratory project that uses the polymerase chain reaction to introduce students to the interrelationship between biology and chemistry. Students must develop their own experimental protocol, perform calculations introduced in freshman classes, and evaluate group dynamics. (Author/WRM)

  16. Chemistry-Materials Laboratory Project Book, 1979-80.

    ERIC Educational Resources Information Center

    Connecticut State Dept. of Education, Hartford. Bureau of Vocational-Technical Schools.

    This Chemistry-Materials Laboratory Project Book, assembled through a survey of science instructors in vocational-technical schools in Connecticut, is intended to meet a variety of needs. It can serve as an idea book, with the instructor taking from it as needed and adding or substituting material related to class interests; as a guide book for…

  17. An Integrated Biology-Chemistry Freshman Laboratory Project in Biotechnology.

    ERIC Educational Resources Information Center

    Schendel, Marilyn Shimizu

    1999-01-01

    Describes a freshman biology laboratory project that uses the polymerase chain reaction to introduce students to the interrelationship between biology and chemistry. Students must develop their own experimental protocol, perform calculations introduced in freshman classes, and evaluate group dynamics. (Author/WRM)

  18. Stereoscopic Projection in the Chemistry Classroom

    ERIC Educational Resources Information Center

    McGrew, LeRoy A.

    1972-01-01

    Describes the development of a three-dimensional projection system used to present structural principles by means of slides. Polarization of images from two planar projectors and viewing through polarized lenses gives stereo results. Techniques used in producing the slides and constructing the equipment are given. (TS)

  19. Atmospheric OCS measurements on Project Gametag

    NASA Astrophysics Data System (ADS)

    Torres, A. L.; Maroulis, P. J.; Goldberg, A. B.; Bandy, A. R.

    1980-12-01

    In the spring of 1978, carbonyl sulfide measurements were made at Drexel University in Philadelphia, Pennsylvania, and on Project Gametag (Global Atmospheric Measurements Experiment of Tropospheric Aerosols and Gases). At Drexel University, measurements were made on 7 days in mid-March, using a dual-channel sampling system. These data had a mean concentration and standard deviation of 544±27 pptv on channel 1 and 522±27 pptv on channel 2. In project Gametag, 346 measurements of the tropospheric concentration of OCS were made over a latitude range 57°S to 70°N. Samples were obtained over the central and southern Pacific Ocean and the western sections of the United States and Canada. Overall OCS levels averaged 512 pptv with a standard deviation of 65 pptv and a standard error of the mean of 4 pptv. Carbonyl sulfide levels were statistically the same in the free troposphere and the boundary layer and over continental and marine areas. The apparent north-south gradient seen in the Gametag data set was attributed to a change in the calibration system as a function of time during the experiment.

  20. Composition and chemistry of the Venusian atmosphere after Venus Express

    NASA Astrophysics Data System (ADS)

    Marcq, Emmanuel

    The ESA/Venus Express orbiter mission is expected to end before the end of this year (2014), and time has come to summarize its results and examine how they changed our view of this planet. Venus Express instruments (especially the spectrometers VIRTIS and SPICAV/SOIR) have been addressing numerous scientific issues since 2006, among which remote sensing of many minor species from the lower troposphere up to the mesosphere at various latitudes and local solar time, often evidencing spatial or temporal variability. In preparation of a new synthesis of our current knowledge about Venusian atmospheric chemistry and composition to be included in the Venus III book (expected to be published in 2015), we shall present an overview of the most significant updates in this domain. A non-exhaustive list of the sub-topics we would like to address is; (1) Lower tropospheric measurements: Venus Express has been able to study in detail most of the thermal infrared windows, yielding extensive night side measurements of some key minor species (CO, OCS, H_2O, HDO, SO_2) (2) Profiles at an unparalleled vertical resolution of many minor species in the lower mesosphere thanks to stellar and solar occultation techniques. (3) Spatial and temporal variability of minor species at various scales, the most striking example being SO_2 above cloud top. (4) New theoretical understanding and modeling of the interplay between the various chemical cycles (carbon, sulfur, halogens) and the condensed phase particulate matter from the clouds and hazes, based on the newest available observational constraints from Venus Express and ground-based telescopes.

  1. A fast stratospheric chemistry solver: the E4CHEM submodel for the atmospheric chemistry global circulation model EMAC

    NASA Astrophysics Data System (ADS)

    Baumgaertner, A. J. G.; Jöckel, P.; Steil, B.; Tost, H.; Sander, R.

    2010-06-01

    The atmospheric chemistry general circulation model ECHAM5/MESSy (EMAC) and the atmospheric chemistry box model CAABA are extended by a computationally very efficient submodel for atmospheric chemistry, E4CHEM. It focuses on stratospheric chemistry but also includes background tropospheric chemistry. It is based on the chemistry of MAECHAM4-CHEM and is intended to serve as a simple and fast alternative to the flexible but also computationally more demanding submodel MECCA. In a model setup with E4CHEM, EMAC is now also suitable for simulations of longer time scales. The reaction mechanism contains basic O3, CH4, CO, HOx, NOx, and ClOx gas phase chemistry. In addition, E4CHEM includes optional fast routines for heterogeneous reactions on sulphate aerosols and polar stratospheric clouds (substituting the existing submodels PSC and HETCHEM), and scavenging (substituting the existing submodel SCAV). We describe the implementation of E4CHEM into the MESSy structure of CAABA and EMAC. For some species the steady state in the box model differs by up to 100% when compared to results from CAABA/MECCA due to different reaction rates. After an update of the reaction rates in E4CHEM the mixing ratios in both boxmodel and 3-D model simulations are in satisfactory agreement with the results from a simulation where MECCA with a similar chemistry scheme was employed. Finally, a comparison against a simulation with a more complex and already evaluated chemical mechanism is presented in order to discuss shortcomings associated with the simplification of the chemical mechanism.

  2. A fast stratospheric chemistry solver: the E4CHEM submodel for the atmospheric chemistry global circulation model EMAC

    NASA Astrophysics Data System (ADS)

    Baumgaertner, A. J. G.; Jöckel, P.; Steil, B.; Tost, H.; Sander, R.

    2010-02-01

    The atmospheric chemistry general circulation model ECHAM5/MESSy (EMAC) and the atmospheric chemistry box model CAABA are extended by a computationally very efficient submodel for atmospheric chemistry, E4CHEM. It focuses on stratospheric chemistry but also includes background tropospheric chemistry. It is based on the chemistry of MAECHAM4-CHEM and is intended to serve as a simple and fast alternative to the flexible but also computationally more demanding submodel MECCA. In a model setup with E4CHEM, EMAC is now also suitable for simulations of longer time scales. The reaction mechanism contains basic O3, CH4, CO, HOx, NOx and ClOx gas phase chemistry. In addition, E4CHEM includes optional fast routines for heterogeneous reactions on sulphate aerosols and polar stratospheric clouds (substituting the existing submodels PSC and HETCHEM), and scavenging (substituting the existing submodel SCAV). We describe the implementation of E4CHEM into the MESSy structure of CAABA and EMAC. For some species the steady state in the box model differs by up to 100% when compared to results from CAABA/MECCA due to different reaction rates. After an update of the reaction rates in E4CHEM the mixing ratios in both boxmodel and 3-D model simulations are in satisfactory agreement with the results from a simulation where MECCA with a similar chemistry scheme was employed. Finally, a comparison against a simulation with a more complex and already evaluated chemical mechanism is presented in order to discuss shortcomings associated with the simplification of the chemical mechanism.

  3. he Impact of Primary Marine Aerosol on Atmospheric Chemistry, Radiation and Climate: A CCSM Model Development Study

    SciTech Connect

    Keene, William C.; Long, Michael S.

    2013-05-20

    This project examined the potential large-scale influence of marine aerosol cycling on atmospheric chemistry, physics and radiative transfer. Measurements indicate that the size-dependent generation of marine aerosols by wind waves at the ocean surface and the subsequent production and cycling of halogen-radicals are important but poorly constrained processes that influence climate regionally and globally. A reliable capacity to examine the role of marine aerosol in the global-scale atmospheric system requires that the important size-resolved chemical processes be treated explicitly. But the treatment of multiphase chemistry across the breadth of chemical scenarios encountered throughout the atmosphere is sensitive to the initial conditions and the precision of the solution method. This study examined this sensitivity, constrained it using high-resolution laboratory and field measurements, and deployed it in a coupled chemical-microphysical 3-D atmosphere model. First, laboratory measurements of fresh, unreacted marine aerosol were used to formulate a sea-state based marine aerosol source parameterization that captured the initial organic, inorganic, and physical conditions of the aerosol population. Second, a multiphase chemical mechanism, solved using the Max Planck Institute for Chemistry's MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) system, was benchmarked across a broad set of observed chemical and physical conditions in the marine atmosphere. Using these results, the mechanism was systematically reduced to maximize computational speed. Finally, the mechanism was coupled to the 3-mode modal aerosol version of the NCAR Community Atmosphere Model (CAM v3.6.33). Decadal-scale simulations with CAM v.3.6.33, were run both with and without reactive-halogen chemistry and with and without explicit treatment of particulate organic carbon in the marine aerosol source function. Simulated results were interpreted (1) to evaluate influences of

  4. First Global Observations of Atmospheric COClF from the Atmospheric Chemistry Experiment Mission

    NASA Technical Reports Server (NTRS)

    Fu, Dejian; Boone, Chris D.; Bernath, Peter F.; Weisenstein, Debra K.; Rinsland, Curtis P.; Manney, Gloria L.; Walker, Kaley A.

    2009-01-01

    Carbonyl chlorofluoride (COClF) is an important reservoir of chlorine and fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COClF, obtained by the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong source region for COClF in the tropical stratosphere near 27 km. A layer of enhanced COClF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts per trillion by volume, largest in the tropics and decreasing toward the poles. The COClF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

  5. NASA's Upper Atmosphere Research Program UARP and Atmospheric Chemistry Modeling and Analysis Program (ACMAP): Research Summaries 1994 - 1996. Report to Congress and the Environmental Protection Agency

    NASA Technical Reports Server (NTRS)

    Kendall, Rose (Compiler); Wolfe, Kathy (Compiler)

    1997-01-01

    Under the mandate contained in the FY 1976 NASA Authorization Act, the National Aeronautics and Space Administration (NASA) has developed and is implementing a comprehensive program of research, technology, and monitoring of the Earth's upper atmosphere, with emphasis on the stratosphere. This program aims at expanding our understanding to permit both the quantitative analysis of current perturbations as well as the assessment of possible future changes in this important region of our environment. It is carried out jointly by the Upper Atmosphere Research Program (UARP) and the Atmospheric Chemistry Modeling and Analysis Program (ACMAP), both managed within the Science Division in the Office of Mission to Planet Earth at NASA. Significant contributions to this effort are also provided by the Atmospheric Effects of Aviation Project (AEAP) of NASA's Office of Aeronautics. The long-term objectives of the present program are to perform research to: understand the physics, chemistry, and transport processes of the upper atmosphere and their effect on the distribution of chemical species in the stratosphere, such as ozone; understand the relationship of the trace constituent composition of the lower stratosphere and the lower troposphere to the radiative balance and temperature distribution of the Earth's atmosphere; and accurately assess possible perturbations of the upper atmosphere caused by human activities as well as by natural phenomena. In compliance with the Clean Air Act Amendments of 1990, Public Law 101-549, NASA has prepared a report on the state of our knowledge of the Earth's upper atmosphere, particularly the stratosphere, and on the progress of UARP and ACMAP. The report for the year 1996 is composed of two parts. Part 1 summarizes the objectives, status, and accomplishments of the research tasks supported under NASA UARP and ACMAP in a document entitled, Research Summary 1994-1996. Part 2 is entitled Present State of Knowledge of the Upper Atmosphere

  6. Simulating the impacts of large scale insect- and disease-driven tree mortality on atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Geddes, J.; Heald, C. L.; Silva, S. J.; Martin, R.

    2015-12-01

    Land-use and land-cover change (LUC) is an important driver of global change through the alteration of local energy, moisture, and carbon exchanges. LUC can also directly impact the emission and deposition of important reactive trace gases, altering the oxidative chemistry of the atmosphere and subsequently air quality and climate. Large-scale tree mortality as a result of insects and disease may therefore have unexplored feedbacks on atmospheric chemistry. Between 2013 and 2027, over 80 million acres of treed land in the United States is predicted to experience basal area mortality rates exceeding 25%. We harmonized the description of land cover across the relevant surface-atmosphere exchange processes in the GEOS-Chem chemical transport model to facilitate LUC simulations, and used this adapted model to test the impact of projected tree mortality according to the 2012 USDA National Insect and Disease Risk Assessment. Nation-wide biogenic VOC emissions were reduced by 5%, with local impacts approaching 50% in some regions. By themselves, these emission reductions resulted in lower surface-level O3 mixing ratios, but this was counteracted by decreases in the O3 deposition velocity (by up to 10%) due to the reduction in vegetation density. Organic aerosol mass concentrations were also significantly affected across the United States, decreasing by 5-10% across the eastern U.S. and the northwest, with local impacts exceeding 25% in some regions. We discuss the general impacts on air quality in clean and polluted regions of the US, and point to developments needed for a more robust understanding of land cover change feedbacks.

  7. Long-term atmospheric effects of medium-energy electron precipitation from chemistry-climate modelling

    NASA Astrophysics Data System (ADS)

    Andersson, M. E.; Verronen, P. T.; Marsh, D. R.; Seppälä, A.; Kalakoski, N.

    2016-12-01

    Medium energy electrons (MEE) from the Earth's outer radiation belt continuously affects the chemical composition of the mesosphere. In particular, ionisation caused by MEE leads to the production of odd hydrogen and odd nitrogen species that affects ozone chemistry. By absorbing a great part of UV radiation, ozone plays an important role in the energy budget and dynamics of the middle atmosphere. During strong precipitation events lasting days, ozone has been observed to decrease by tens of percent in the wintertime polar region. Such ozone perturbation causes zonal wind anomalies through wave-mean flow interaction which propagate to lower altitudes during the polar winter and affect stratospheric temperature. However, understanding the long term effects from MEE and its potential role in the polar climate variability is a difficult task due to the limitations of the satellite measurements. Here we use the Whole Atmosphere Community Climate Model (WACCM) together with MEE flux characterised using a precipitation model driven by the magnetic Ap index to simulate the effects of MEE on the solar cycles time scale. We will present results from free running simulations for the period of time 1955-2005. We will contrast our results with those from the fifth phase of the Coupled Model Intercomparison Project (CMIP5) in order to assess the role of MEE and its significance to the atmospheric dynamics and climate variability in the polar regions.

  8. Advanced Placement Chemistry: Project Advance and the Advanced Placement Program: A Comparison of Students' Performance on the AP Chemistry Examination.

    ERIC Educational Resources Information Center

    Mercurio, Joseph; And Others

    1984-01-01

    Compared performance of Syracuse University Project Advance (PA) chemistry students (N=35) with advanced placement (AP) candidates on the AP chemistry examination. PA students scored slightly above the national average on the examination, and students who performed well (B or better) in AP chemistry also did well on the examination. (JN)

  9. Evaluated Kinetic, Photochemical and Heterogeneous Data for Atmospheric Chemistry: Supplement V, IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry

    SciTech Connect

    Atkinson, R.; Baulch, D.L.; Cox, R.A.; Hampson, R.F. Jr.; Kerr, J.A. Chairman; Rossi, M.J.; Troe, J.

    1997-05-01

    This paper updates and extends previous critical evaluations of the kinetics and photochemistry of gas-phase chemical reactions of neutral species involved in atmospheric chemistry [J. Phys. Chem. Ref. Data {bold 9}, 295 (1980); {bold 11}, 327 (1982); {bold 13}, 1259 (1984); {bold 18}, 881 (1989); {bold 21}, 1125 (1992)]. The work has been carried out by the authors under the auspices of the IUPAC Subcommittee on Gas Phase Kinetic Data Evaluation for Atmospheric Chemistry. Data sheets have been prepared for 658 thermal and photochemical reactions, containing summaries of the available experimental data with notes giving details of the experimental procedures. For each reaction, a preferred value of the rate coefficient at 298 K is given together with a temperature dependence where possible. The selection of the preferred value is discussed and estimates of the accuracies of the rate coefficients and temperature coefficients have been made for each reaction. The data sheets are intended to provide the basic physical chemical data needed as input for calculations which model atmospheric chemistry. A table summarizing the preferred rate data is provided, together with an appendix listing the available data on enthalpies of formation of the reactant and product species. We have also included for the first time in this series of evaluations a section on heterogeneous reactions of importance in atmospheric chemistry. {ital Key words:} air pollution; atmospheric chemistry; chemical kinetics; data evaluation; gas phase; heterogeneous atmospheric reactions; photoabsorption cross-section, photochemistry; quantum yield; rate coefficient.{copyright} {ital 1997 American Institute of Physics and American Chemical Society.}

  10. Understanding Heterogeneous Chemistry at the Molecular-Level using Broadband Nonlinear Technologies: Application to Atmospheric Aerosol Growth and Chemistry

    NASA Astrophysics Data System (ADS)

    Allen, H. C.

    2001-12-01

    Surface reactions on liquid and solid particles can significantly impact tropospheric chemistry since many reactions that are slow to occur in the gas phase may in fact be favored on these atmospheric particles. Currently, we are investigating the surface structure of a variety of solid and liquid surfaces in order to understand particle growth and chemistry in the troposphere. The structure of a surface is different than the bulk media and consequently, the chemistry occurring at a surface is often unique. Surface vibrational sum frequency generation is the primary tool used in these studies because of its surface and molecular selectivity. New advances in our lab using broadband technology and ultra-fast laser sources for probing reactions taking place on surfaces on short timescales and at atmospheric pressures will be presented. Surface structures and adsorption of gas-phase water at the surface of various organic solutions (e.g. ethylene glycol and methylnapthalene) will be discussed.

  11. Alternative Solvents through Green Chemistry Project

    NASA Technical Reports Server (NTRS)

    Hintze, Paul E.; Quinn, Jacqueline

    2014-01-01

    Components in the aerospace industry must perform with accuracy and precision under extreme conditions, and surface contamination can be detrimental to the desired performance, especially in cases when the components come into contact with strong oxidizers such as liquid oxygen. Therefore, precision cleaning is an important part of a components preparation prior to utilization in aerospace applications. Current cleaning technologies employ a variety of cleaning agents, many of which are halogenated solvents that are either toxic or cause environmental damage. Thus, this project seeks to identify alternative precision cleaning solvents and technologies, including use of less harmful cleaning solvents, ultrasonic and megasonic agitation, low-pressure plasma cleaning techniques, and supercritical carbon dioxide extraction. Please review all data content found in the Public Data tab located at: https:techport.nasa.govview11697public

  12. Atmosphere aerosol satellite project Aerosol-UA

    NASA Astrophysics Data System (ADS)

    Milinevsky, Gennadi; Yatskiv, Yaroslav; Syniavskyi, Ivan; Bovchaliuk, Andrii; Degtyaryov, Oleksandr; Sosonkin, Mikhail; Mishchenko, Michael; Danylevsky, Vassyl; Ivanov, Yury; Oberemok, Yevgeny; Masley, Volodymyr; Rosenbush, Vera; Moskalev, Sergii

    2017-04-01

    The experiment Aerosol-UA is Ukrainian space mission aimed to the terrestrial atmospheric aerosol spatial distribution and microphysics investigations. The experiment concept is based on idea of Glory/APS mission of precise orbital measurements of polarization and intensity of the sunlight scattered by the atmosphere, aerosol and the surface the multichannel Scanning Polarimeter (ScanPol) with narrow field-of-view. ScanPol measurements will be accompanied by the wide-angle MultiSpectral Imager-Polarimeter (MSIP). The ScanPol is designed to measure Stokes parameters I, Q, U within the spectral range from the UV to the SWIR in a wide range of phase angles along satellite ground path. Expected ScanPol polarimetric accuracy is 0.15%. A high accuracy measurement of the degree of linear polarization is provided by on-board calibration of the ScanPol polarimeter. On-board calibration is performed for each scan of the mirror scanning system. A set of calibrators is viewed during the part of the scan range when the ScanPol polarimeter looks in the direction opposite to the Earth's surface. These reference assemblies provide calibration of the zero of the polarimetric scale (unpolarized reference assembly) and the scale factor for the polarimetric scale (polarized reference assembly). The zero of the radiometric scale is provided by the dark reference assembly.The spectral channels of the ScanPol are used to estimate the tropospheric aerosol absorption, the aerosol over the ocean and the land surface, the signals from cirrus clouds, stratospheric aerosols caused by major volcanic eruptions, and the contribution of the Earth's surface. The imager-polarimeter MSIP will collect 60°x60° field-of-view images on the state of the atmosphere and surface in the area, where the ScanPol polarimeter will measure, to retrieve aerosol optical depth and polarization properties of aerosol by registration of three Stokes parameters simultaneously in three spectral channels. The two more

  13. The Skylab concentrated atmospheric radiation project

    NASA Technical Reports Server (NTRS)

    Kuhn, P. M.; Marlatt, W. E.; Whitehead, V. S. (Principal Investigator)

    1975-01-01

    The author has identified the following significant results. Comparison of several existing infrared radiative transfer models under somewhat controlled conditions and with atmospheric observations of Skylab's S191 and S192 radiometers illustrated that the models tend to over-compute atmospheric attenuation in the window region of the atmospheric infrared spectra.

  14. Using high-frequency sampling to detect effects of atmospheric pollutants on stream chemistry

    Treesearch

    Stephen D. Sebestyen; James B. Shanley; Elizabeth W. Boyer

    2009-01-01

    We combined information from long-term (weekly over many years) and short-term (high-frequency during rainfall and snowmelt events) stream water sampling efforts to understand how atmospheric deposition affects stream chemistry. Water samples were collected at the Sleepers River Research Watershed, VT, a temperate upland forest site that receives elevated atmospheric...

  15. Atmospheric chemistry and environmental impact of the use of amines in carbon capture and storage (CCS).

    PubMed

    Nielsen, Claus J; Herrmann, Hartmut; Weller, Christian

    2012-10-07

    This critical review addresses the atmospheric gas phase and aqueous phase amine chemistry that is relevant to potential emissions from amine-based carbon capture and storage (CCS). The focus is on amine, nitrosamine and nitramine degradation, and nitrosamine and nitramine formation processes. A comparison between the relative importance of the various atmospheric sinks for amines, nitrosamines and nitramines is presented.

  16. Project-based learning in the secondary chemistry classroom

    NASA Astrophysics Data System (ADS)

    Crane, Elizabeth L.

    This study investigated the use of project-based learning (PBL) in a high school chemistry classroom. PBL encourages the use of projects, which promote continual learning, rather than a summative project at the end of a unit after the learning has already been done. Along with implementing PBL, the study also incorporated many of the strategies included in the broader strategy known as Assessment for Learning (AfL), which stresses developing assessments that are part of the learning process rather than simply a measurement of the amount of learning that has occurred upon completion of a unit. The hypothesis of this research was that PBL would increase student comprehension and motivation as measured through pre and post-test data and a student survey. The new project-based unit required students to research and present the properties and structures of elements and how we use them. The expectation was that this approach would engage students with the material, the computer modeling would allow for more concrete visualization of structures and the project-based format would allow students to become more invested in their own learning. This study provided evidence to support the hypothesis that the implementation of project-based learning, supported by formative assessment and other assessment for learning strategies, will improve student comprehension and motivation in the secondary chemistry classroom.

  17. Investigating Titan's Atmospheric Chemistry at Low Temperature in Support of the NASA Cassini Mission

    NASA Technical Reports Server (NTRS)

    Sciamma-O'Brien, Ella; Salama, Farid

    2013-01-01

    Titan's atmosphere, composed mainly of N2 and CH4, is the siege of a complex chemistry induced by solar UV radiation and electron bombardment from Saturn's magnetosphere. This organic chemistry occurs at temperatures lower than 200 K and leads to the production of heavy molecules and subsequently solid aerosols that form the orange haze surrounding Titan. The Titan Haze Simulation (THS) experiment has been developed on the COSMIC simulation chamber at NASA Ames in order to study the different steps of Titan's atmospheric chemistry at low temperature and to provide laboratory data in support for Cassini data analysis. The chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas mixture is adiabatically cooled to Titan-like temperature (approx. 150 K) before inducing the chemistry by plasma discharge. Different gas mixtures containing N2, CH4, and the first products of the N2,-CH4 chemistry (C2H2, C2H4, C6H6...) but also heavier molecules such as PAHs or nitrogen containing PAHs can be injected. Both the gas phase and solid phase products resulting from the plasma-induced chemistry can be monitored and analyzed. Here we present the results of recent gas phase and solid phase studies that highlight the chemical growth evolution when injecting heavier hydrocarbon trace elements in the initial N2-CH4 mixture. Due to the short residence time of the gas in the plasma discharge, only the first steps of the chemistry have time to occur in a N2-CH4 discharge. However by adding acetylene and benzene to the initial N2-CH4 mixture, we can study the intermediate steps of Titan's atmospheric chemistry as well as specific chemical pathways. These results show the uniqueness of the THS experiment to help understand the first and intermediate steps of Titan fs atmospheric chemistry as well as specific chemical pathways leading to Titan fs haze formation.

  18. News from Online: In a Planet, Not a Test Tube: Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Michalovic, Mark

    2003-04-01

    Atmospheric chemistry covers many topics including the gas laws, chemical reactions, kinetics, and catalysis. The article reviews some of the materials available online for teaching chemistry through exploration of the atmosphere. Included are web sites dealing with ozone depletion caused by chlorofluorocarbons and the green house effect and global warming related to the presence of naturally-occurring and human-made compounds in the air. Also covered are materials dealing with the extraterrestrial chemistry in the atmospheres of other worlds, including Venus with its choking, high-pressure carbon dioxide and sulfuric acid atmosphere and Saturn's moon Titan, whose dense nitrogen blanket harbors hydrocarbons and other compounds thought necessary for life to develop.

  19. Remote sensing of atmospheric chemistry; Proceedings of the Meeting, Orlando, FL, Apr. 1-3, 1991

    NASA Technical Reports Server (NTRS)

    Mcelroy, James L. (Editor); Mcneal, Robert J. (Editor)

    1991-01-01

    The present volume on remote sensing of atmospheric chemistry discusses special remote sensing space observations and field experiments to study chemical change in the atmosphere, network monitoring for detection of stratospheric chemical change, stratospheric chemistry studies, and the combining of model, in situ, and remote sensing in atmospheric chemistry. Attention is given to the measurement of tropospheric carbon monoxide using gas filter radiometers, long-path differential absorption measurements of tropospheric molecules, air quality monitoring with the differential optical absorption spectrometer, and a characterization of tropospheric methane through space-based remote sensing. Topics addressed include microwave limb sounder experiments for UARS and EOS, an overview of the spectroscopy of the atmosphere using an FIR emission experiment, the detection of stratospheric ozone trends by ground-based microwave observations, and a FIR Fabry-Perot spectrometer for OH measurements.

  20. CHEMISTRY OF SILICATE ATMOSPHERES OF EVAPORATING SUPER-EARTHS

    SciTech Connect

    Schaefer, Laura; Fegley, Bruce E-mail: bfegley@levee.wustl.ed

    2009-10-01

    We model the formation of silicate atmospheres on hot volatile-free super-Earths. Our calculations assume that all volatile elements such as H, C, N, S, and Cl have been lost from the planet. We find that the atmospheres are composed primarily of Na, O{sub 2}, O, and SiO gas, in order of decreasing abundance. The atmospheric composition may be altered by fractional vaporization, cloud condensation, photoionization, and reaction with any residual volatile elements remaining in the atmosphere. Cloud condensation reduces the abundance of all elements in the atmosphere except Na and K. We speculate that large Na and K clouds such as those observed around Mercury and Io may surround hot super-Earths. These clouds would occult much larger fractions of the parent star than a closely bound atmosphere, and may be observable through currently available methods.

  1. Atmospheric Halogen Chemistry of Volcanic Plumes in WRF-Chem

    NASA Astrophysics Data System (ADS)

    Surl, Luke; Donohoue, Deanna; von Glasow, Roland

    2015-04-01

    Volcanic eruptions are known to be a strong and concentrated source of reactive halogen species. The chemistry that these species are known to take part in include ozone-destruction cycles. Despite the potentially large perturbation to the chemistry of the troposphere that eruptions may cause, the magnitude of such impacts on global and regional scales is largely unknown. We used WRF-Chem to investigate the influence of Mount Etna on the tropospheric chemistry of the Mediterranean region. The chemistry of bromine, chlorine and mercury has been added to the chemical mechanism CBMZ and we have coupled WRF-Chem with the emissions program PrepChem. We developed a simple parameterisation of the key multiphase reaction cycles involving halogens. Comparison with published field data shows that the model is able to reproduce the bromine explosion phenomenon seen in spectroscopic investigations of volcanic plumes. From the model results we are able to determine a detailed picture of the chemistry of a volcanic plume; results are presented which show in detail how the character of the volcanic plume evolves as it is advected downwind and we identify which parts of the chemical cycle are most likely to be the limiting factors for the speed of the processing. Additionally, these modelled results are supplemented with, and compared against, measurements of ozone depletion that we made within the plume at the summit of Mount Etna.

  2. The Titan Haze Simulation experiment on COSmIC: Probing Titan's atmospheric chemistry at low temperature

    NASA Astrophysics Data System (ADS)

    Sciamma-O'Brien, Ella; Ricketts, Claire L.; Salama, Farid

    2014-11-01

    The aim of the Titan Haze Simulation (THS) experiment is to contribute to a better understanding of aerosol formation in Titan's atmosphere through the study of the chemical formation pathways that link the simpler gas phase molecules resulting from the first steps of the N2-CH4 chemistry, to the more complex gas phase precursors of aerosols; and more specifically, to investigate the role of polycyclic aromatic hydrocarbons (PAHs) and nitrogenated polycyclic aromatic hydrocarbons (PANHs), among other hydrocarbons, in this process. In the THS experiment developed at the NASA Ames Cosmic simulation facility (COSmIC), Titan's atmospheric chemistry is simulated by a pulsed plasma jet expansion at temperature conditions (∼150 K) close to those found in Titan's atmosphere in regions where aerosols are formed. In addition, because of the very short residence time of the gas in the plasma discharge, only the initial steps of the chemistry occur, making the COSmIC/THS a unique tool to study the first and intermediate (when adding heavier precursors to the initial N2-CH4 mixture) steps of Titan's atmospheric chemistry at low temperature as shown in the study presented here. We further illustrate the potential of COSmIC/THS for the simulation of Titan's atmospheric chemistry by presenting very promising results from a preliminary comparison of the laboratory data to data from the Cassini Plasma Spectrometer-Ion Beam Spectrometer (CAPS-IBS) instrument.

  3. Experimental and Theoretical Studies of Atmosphereic Inorganic Chlorine Chemistry

    NASA Technical Reports Server (NTRS)

    Sander, Stanley P.; Friedl, Randall R.

    1993-01-01

    Over the last five years substantial progress has been made in defining the realm of new chlorine chemistry in the polar stratosphere. Application of existing experimental techniques to potentially important chlorine-containing compounds has yielded quantitative kinetic and spectroscopic data as well as qualitative mechanistic insights into the relevant reactions.

  4. Experimental and Theoretical Studies of Atmosphereic Inorganic Chlorine Chemistry

    NASA Technical Reports Server (NTRS)

    Sander, Stanley P.; Friedl, Randall R.

    1993-01-01

    Over the last five years substantial progress has been made in defining the realm of new chlorine chemistry in the polar stratosphere. Application of existing experimental techniques to potentially important chlorine-containing compounds has yielded quantitative kinetic and spectroscopic data as well as qualitative mechanistic insights into the relevant reactions.

  5. Vesper - Venus Chemistry and Dynamics Orbiter - A NASA Discovery Mission Proposal: Submillimeter Investigation of Atmospheric Chemistry and Dynamics

    NASA Technical Reports Server (NTRS)

    Chin, Gordon

    2011-01-01

    Vesper conducts a focused investigation of the chemistry and dynamics of the middle atmosphere of our sister planet- from the base of the global cloud cover to the lower thermosphere. The middle atmosphere controls the stability of the Venus climate system. Vesper determines what processes maintain the atmospheric chemical stability, cause observed variability of chemical composition, control the escape of water, and drive the extreme super-rotation. The Vesper science investigation provides a unique perspective on the Earth environment due to the similarities in the middle atmosphere processes of both Venus and the Earth. Understanding key distinctions and similarities between Venus and Earth will increase our knowledge of how terrestrial planets evolve along different paths from nearly identical initial conditions.

  6. Atmospheric Chemistry of Volcanic Plumes in WRF-Chem

    NASA Astrophysics Data System (ADS)

    Surl, L.; Donohoue, D.; von Glasow, R.

    2014-12-01

    Volcanic eruptions are known to be a strong and concentrated source of reactive halogen species. The chemistry that these species are known to take part in include ozone-destruction cycles. Despite the potentially large perturbation to the chemistry of the troposphere that eruptions may cause the magnitude of such impacts on global and regional scales is largely unknown. We used WRF-Chem to investigate the influence of Mount Etna on the tropospheric chemistry of the Mediterranean region. The chemistry of bromine, chlorine and mercury has been added to the chemical mechanism CBMZ and we have coupled WRF-Chem with the emissions program PrepChem. We developed a simple parameterisation of the key multiphase reaction cycles involving halogens. Comparison with published field data shows that the model is able to reproduce the bromine explosion phenomenon seen in spectroscopic investigations of volcanic plumes. From the model results we are able to determine a detailed picture of the chemistry of a volcanic plume; results are presented which show how the character of the volcanic plume evolves as it is advected downwind. We determine the magnitude of Mt. Etna's regional influence under typical conditions. We also present results which show how the variation in volcanic output, as well as meteorological variation within the region, can influence the extent of Mt. Etna's regional impact. As WRF-Chem is very flexible, we also performed model runs fir other volcanoes.. The model results are compared to satellite measurements of BrO and SO2 to improve our understanding of chemical processes in tropospheric volcanic plumes.

  7. Atmospheric Chemistry from Space: Present Status and Future Plans

    NASA Technical Reports Server (NTRS)

    Schoeberl, Mark R.; Einaudi, Franco (Technical Monitor)

    2001-01-01

    One of the unqualified successes of the earth observation program is NASA's continuing monitoring of the ozone layer from space. This activity began in the early 70's with research instruments and continues to this day with the TOMS instrument series and the Upper Atmosphere Research Satellite. In the near future, NASA will be launching the EOS Aura spacecraft (launch mid-2003) which will continue our study of the chemical processes that produce stratospheric ozone depletion. In addition, Aura will begin the first global study of lower atmospheric air pollution including urban ozone, aerosols, nitrogen oxides and carbon monoxide. Atmospheric air pollution measurements from earth orbit involve the development of very high precision spectrometer technologies that have never been flown in space. Farther into the future, lower atmospheric ozone and aerosols may be monitored by space based lidars in low earth orbit, by sensors in geostationary orbit and by continuous limb observations instrument from the Lagrange point L2.

  8. The THS experiment: Simulating Titan's atmospheric chemistry at low temperature (200 K)

    NASA Astrophysics Data System (ADS)

    Sciamma-O'Brien, Ella; Upton, Kathleen T.; Beauchamp, Jack L.; Salama, Farid

    2016-10-01

    In the Titan Haze Simulation (THS) experiment, Titan's atmospheric chemistry is simulated by plasma discharge in the stream of a supersonic expansion, i.e. at low Titan-like temperature (150 K). Here, we present complementary gas and solid phase analyses of four N2-CH4-based gas mixtures that demonstrate the unique capability of the THS to monitor the chemical growth evolution in order to better understand Titan's chemistry and the origin of aerosol formation.

  9. Potential changes in atmospheric chemistry in the decades ahead: Climate and biosphere interactions and feedbacks

    SciTech Connect

    Gaffney, J.S.; Marley, N.A.

    1991-10-01

    Atmospheric chemistry is a challenging area of research where much knowledge is needed if we are to continue to survive as a species. This paper outlines research needs in the decades ahead in this key area of scientific endeavor. Highlighted are areas of research that are likely to lead to climatic and biospheric impacts and have been given little attention in the past. In particular, the possible organic transformation chemistries that may lead to chemical and physical changes in tropospheric cloud chemistries are highlighted and emphasized as an area where research is needed in the future. 22 refs.

  10. Non-Equilibrium Thermodynamic Chemistry and the Composition of the Atmosphere of Mars

    NASA Technical Reports Server (NTRS)

    Levine, J. S.; Summers, M. E.

    2003-01-01

    A high priority objective of the Mars Exploration Program is to Determine if life exists today (MEPAG Goal I, Objective A). The measurement of gases of biogenic origin may be an approach to detect the presence of microbial life on the surface or subsurface of Mars. Chemical thermodynamic calculations indicate that on both Earth and Mars, certain gases should exist in extremely low concentrations, if at all. Microbial metabolic activity is an important non-equilibrium chemistry process on Earth, and if microbial life exists on Mars, may be an important nonequilibrium chemistry process on Mars. The non-equilibrium chemistry of the atmosphere of Mars is discussed in this paper.

  11. Non-Equilibrium Thermodynamic Chemistry and the Composition of the Atmosphere of Mars

    NASA Technical Reports Server (NTRS)

    Levine, J. S.; Summers, M. E.

    2003-01-01

    A high priority objective of the Mars Exploration Program is to Determine if life exists today (MEPAG Goal I, Objective A). The measurement of gases of biogenic origin may be an approach to detect the presence of microbial life on the surface or subsurface of Mars. Chemical thermodynamic calculations indicate that on both Earth and Mars, certain gases should exist in extremely low concentrations, if at all. Microbial metabolic activity is an important non-equilibrium chemistry process on Earth, and if microbial life exists on Mars, may be an important nonequilibrium chemistry process on Mars. The non-equilibrium chemistry of the atmosphere of Mars is discussed in this paper.

  12. The role of computational chemistry in the science and measurements of the atmosphere

    NASA Technical Reports Server (NTRS)

    Phillips, D. H.

    1978-01-01

    The role of computational chemistry in determining the stability, photochemistry, spectroscopic parameters, and parameters for estimating reaction rates of atmospheric constituents is discussed. Examples dealing with the photolysis cross sections of HOCl and (1 Delta g) O2 and with the stability of gaseous NH4Cl and asymmetric ClO3 are presented. It is concluded that computational chemistry can play an important role in the study of atmospheric constituents, particularly reactive and short-lived species which are difficult to investigate experimentally.

  13. Strong atmospheric chemistry feedback to climate warming from Arctic methane emissions

    USGS Publications Warehouse

    Isaksen, Ivar S.A.; Gauss, Michael; Myhre, Gunnar; Walter Anthony, Katey M.; Ruppel, Carolyn

    2011-01-01

    The magnitude and feedbacks of future methane release from the Arctic region are unknown. Despite limited documentation of potential future releases associated with thawing permafrost and degassing methane hydrates, the large potential for future methane releases calls for improved understanding of the interaction of a changing climate with processes in the Arctic and chemical feedbacks in the atmosphere. Here we apply a “state of the art” atmospheric chemistry transport model to show that large emissions of CH4 would likely have an unexpectedly large impact on the chemical composition of the atmosphere and on radiative forcing (RF). The indirect contribution to RF of additional methane emission is particularly important. It is shown that if global methane emissions were to increase by factors of 2.5 and 5.2 above current emissions, the indirect contributions to RF would be about 250% and 400%, respectively, of the RF that can be attributed to directly emitted methane alone. Assuming several hypothetical scenarios of CH4 release associated with permafrost thaw, shallow marine hydrate degassing, and submarine landslides, we find a strong positive feedback on RF through atmospheric chemistry. In particular, the impact of CH4 is enhanced through increase of its lifetime, and of atmospheric abundances of ozone, stratospheric water vapor, and CO2 as a result of atmospheric chemical processes. Despite uncertainties in emission scenarios, our results provide a better understanding of the feedbacks in the atmospheric chemistry that would amplify climate warming.

  14. Coordinating interdisciplinary and international research through CATCH (The Cryosphere and ATmospheric CHemistry)

    NASA Astrophysics Data System (ADS)

    Thomas, Jennie L.; Murphy, Jennifer; Bartels-Rausch, Thorsten; Frey, Markus; McNeill, V. Faye; Shepson, Paul; Pratt, Kerri; Douglas, Tom; Willis, Megan; Abbatt, Jon; Jones, Anna; Anastasio, Cort; Matrai, Patricia; Nomura, Daiki; Kim, Kitae; Melamed, Megan L.

    2017-04-01

    CATCH is a new international activity co-sponsored by IGAC (International Global Atmospheric Chemistry) and SOLAS (Surface Ocean - Lower Atmosphere Study). As an emerging international activity established in 2016, the CATCH mission is to facilitate atmospheric chemistry research within the international community, with a focus on natural processes specific to cold regions of the Earth. Cryospheric processes are known to be important for atmospheric chemistry in the Polar regions as well as other cold regions, such as continental snowpack. These processes are strongly linked to global and local environmental change, for example, through changes in snow and sea ice cover and aerosol processing in cold regions. CATCH aims to coordinate and encourage international/interdisciplinary cooperation between scientists in order to better understand and predict: - The impacts of physical, chemical, biological, and ecological changes in sea ice and snow on atmospheric chemistry; - Aerosol formation and processing in cold regions; - Changes in the cryosphere that alter feedbacks between climate change and atmospheric chemistry; - Ice core records of global environmental change; - Cold region aerosols as cloud condensation nuclei and their impacts on cloud properties; - Impacts of microbiology on the biogeochemical cycling of elements in cold environments; and - Changes in cold region atmospheric gases and aerosols due to industrialization and climate change. In this presentation, the ways for linking modeling and measurements including observations in the Arctic through CATCH in the future will be explored. CATCH is seeking participation and guidance and engagement from the community, including how to best link to existing efforts, to meet these objectives and to define future directions.

  15. Chemistry of atmosphere-surface interactions on Venus and Mars

    NASA Technical Reports Server (NTRS)

    Fegley, Bruce, Jr.; Treiman, Allan H.

    1992-01-01

    Earth-based, earth-orbital, and spacecraft observational data are used in the present evaluation of Venus atmosphere-surface interactions to quantitatively characterize the reactions between C, H, S, Cl, F, and N gases and plausible surface minerals. Calculation results are used to predict stable minerals and mineral assemblages on the Venus surface, in order to ascertain which (if any) of the atmospheric gases are buffeted by mineral assemblages. Chemical equilibrium calculations using extant thermodynamic data on scapolite minerals predict that carbonate-bearing scapolite and sulfate meionite are unstable on the surface of Venus, while chloride-bearing scapolite is stable.

  16. The Validity of Stirling's Approximation: A Physical Chemistry Project

    NASA Astrophysics Data System (ADS)

    Wallner, A. S.; Brandt, K. A.

    1999-10-01

    Often in physical chemistry courses, the direct proof of Stirling's approximation is omitted owing to the complexity of the mathematics involved. We present an accessible proof of this result that requires only an understanding of first-year calculus. We also present an undergraduate project dealing with the validity of Stirling's approximation. This assignment asks students to study the validity of the formula using mathematical tools such as programmable calculators, commercially available computer software such as Derive, and basic computer programming. Examples of students' solutions are provided.

  17. Size resolved fog water chemistry and its atmospheric implications

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida; Ervens, Barbara; Bhattu, Deepika

    2015-04-01

    Fog is a natural meteorological phenomenon that occurs throughout the world. It usually contains substantial quantity of liquid water and results in severe visibility reduction leading to disruption of normal life. Fog is generally seen as a natural cleansing agent but it also has the potential to form Secondary Organic Aerosol (SOA) via aqueous processing of ambient aerosols. Size- resolved fog water chemistry for inorganics were reported in previous studies but processing of organics inside the fog water and quantification of aqSOA remained a challenge. To assess the organics processing via fog aqueous processing, size resolved fog water samples were collected in two consecutive winter seasons (2012-13, 2013-14) at Kanpur, a heavily polluted urban area of India. Caltech 3 stage fog collector was used to collect the fog droplets in 3 size fraction; coarse (droplet diameter > 22 µm), medium (22> droplet diameter >16 µm) and fine (16> droplet diameter >4 µm). Collected samples were atomized into various instruments such as Aerosol Mass Spectrometer (AMS), Cloud Condensation Nucleus Counter (CCNc), Total Organic Carbon (TOC) and a thermo denuder (TD) for the physico-chemical characterization of soluble constituents. Fine droplets are found to be more enriched with different aerosol species and interestingly contain more aged and less volatile organics compared to other coarser sizes. Organics inside fine droplets have an average O/C = 0.87 compared to O/C of 0.67 and 0.74 of coarse and medium droplets. Metal chemistry and higher residence time of fine droplets are seemed to be the two most likely reasons for this outcome from as the results of a comprehensive modeling carried out on the observed data indicate. CCN activities of the aerosols from fine droplets are also much higher than that of coarse or medium droplets. Fine droplets also contain light absorbing material as was obvious from their 'yellowish' solution. Source apportionment of fog water organics via

  18. Seasonal variations in atmospheric chemistry in the Adirondacks

    SciTech Connect

    Kelly, T.J.; Tanner, R.L.; McLaren, S.E.; DuBois, M.V.

    1985-03-01

    The results of continuous real-time measurements of aerosol composition, HNO/sub 3/, and SO/sub 2/, performed at the summit of Whiteface Mountain, New York, during 1984 are reported. The purpose was to shed light on the seasonal variation in atmospheric acidity in this ecologically sensitive area. 13 refs., 5 figs. (ACR)

  19. Electrostatic activation of prebiotic chemistry in substellar atmospheres

    NASA Astrophysics Data System (ADS)

    Stark, C. R.; Helling, Ch.; Diver, D. A.; Rimmer, P. B.

    2014-04-01

    Charged dust grains in the atmospheres of exoplanets may play a key role in the formation of prebiotic molecules, necessary to the origin of life. Dust grains submerged in an atmospheric plasma become negatively charged and attract a flux of ions that are accelerated from the plasma. The energy of the ions upon reaching the grain surface may be sufficient to overcome the activation energy of particular chemical reactions that would be unattainable via ion and neutral bombardment from classical, thermal excitation. As a result, prebiotic molecules or their precursors could be synthesized on the surface of dust grains that form clouds in exoplanetary atmospheres. This paper investigates the energization of the plasma ions, and the dependence on the plasma electron temperature, in the atmospheres of substellar objects such as gas giant planets. Calculations show that modest electron temperatures of ~1 eV (~104 K) are enough to accelerate ions to sufficient energies that exceed the activation energies required for the formation of formaldehyde, ammonia, hydrogen cyanide and the amino acid glycine.

  20. Biological regulation of atmospheric chemistry en route to planetary oxygenation

    NASA Astrophysics Data System (ADS)

    Izon, Gareth; Zerkle, Aubrey L.; Williford, Kenneth H.; Farquhar, James; Poulton, Simon W.; Claire, Mark W.

    2017-03-01

    Emerging evidence suggests that atmospheric oxygen may have varied before rising irreversibly ˜2.4 billion years ago, during the Great Oxidation Event (GOE). Significantly, however, pre-GOE atmospheric aberrations toward more reducing conditions—featuring a methane-derived organic-haze—have recently been suggested, yet their occurrence, causes, and significance remain underexplored. To examine the role of haze formation in Earth’s history, we targeted an episode of inferred haze development. Our redox-controlled (Fe-speciation) carbon- and sulfur-isotope record reveals sustained systematic stratigraphic covariance, precluding nonatmospheric explanations. Photochemical models corroborate this inference, showing Δ36S/Δ33S ratios are sensitive to the presence of haze. Exploiting existing age constraints, we estimate that organic haze developed rapidly, stabilizing within ˜0.3 ± 0.1 million years (Myr), and persisted for upward of ˜1.4 ± 0.4 Myr. Given these temporal constraints, and the elevated atmospheric CO2 concentrations in the Archean, the sustained methane fluxes necessary for haze formation can only be reconciled with a biological source. Correlative δ13COrg and total organic carbon measurements support the interpretation that atmospheric haze was a transient response of the biosphere to increased nutrient availability, with methane fluxes controlled by the relative availability of organic carbon and sulfate. Elevated atmospheric methane concentrations during haze episodes would have expedited planetary hydrogen loss, with a single episode of haze development providing up to 2.6-18 × 1018 moles of O2 equivalents to the Earth system. Our findings suggest the Neoarchean likely represented a unique state of the Earth system where haze development played a pivotal role in planetary oxidation, hastening the contingent biological innovations that followed.

  1. Biological regulation of atmospheric chemistry en route to planetary oxygenation

    PubMed Central

    Farquhar, James; Poulton, Simon W.

    2017-01-01

    Emerging evidence suggests that atmospheric oxygen may have varied before rising irreversibly ∼2.4 billion years ago, during the Great Oxidation Event (GOE). Significantly, however, pre-GOE atmospheric aberrations toward more reducing conditions—featuring a methane-derived organic-haze—have recently been suggested, yet their occurrence, causes, and significance remain underexplored. To examine the role of haze formation in Earth’s history, we targeted an episode of inferred haze development. Our redox-controlled (Fe-speciation) carbon- and sulfur-isotope record reveals sustained systematic stratigraphic covariance, precluding nonatmospheric explanations. Photochemical models corroborate this inference, showing Δ36S/Δ33S ratios are sensitive to the presence of haze. Exploiting existing age constraints, we estimate that organic haze developed rapidly, stabilizing within ∼0.3 ± 0.1 million years (Myr), and persisted for upward of ∼1.4 ± 0.4 Myr. Given these temporal constraints, and the elevated atmospheric CO2 concentrations in the Archean, the sustained methane fluxes necessary for haze formation can only be reconciled with a biological source. Correlative δ13COrg and total organic carbon measurements support the interpretation that atmospheric haze was a transient response of the biosphere to increased nutrient availability, with methane fluxes controlled by the relative availability of organic carbon and sulfate. Elevated atmospheric methane concentrations during haze episodes would have expedited planetary hydrogen loss, with a single episode of haze development providing up to 2.6–18 × 1018 moles of O2 equivalents to the Earth system. Our findings suggest the Neoarchean likely represented a unique state of the Earth system where haze development played a pivotal role in planetary oxidation, hastening the contingent biological innovations that followed. PMID:28289223

  2. Biological regulation of atmospheric chemistry en route to planetary oxygenation.

    PubMed

    Izon, Gareth; Zerkle, Aubrey L; Williford, Kenneth H; Farquhar, James; Poulton, Simon W; Claire, Mark W

    2017-03-28

    Emerging evidence suggests that atmospheric oxygen may have varied before rising irreversibly ∼2.4 billion years ago, during the Great Oxidation Event (GOE). Significantly, however, pre-GOE atmospheric aberrations toward more reducing conditions-featuring a methane-derived organic-haze-have recently been suggested, yet their occurrence, causes, and significance remain underexplored. To examine the role of haze formation in Earth's history, we targeted an episode of inferred haze development. Our redox-controlled (Fe-speciation) carbon- and sulfur-isotope record reveals sustained systematic stratigraphic covariance, precluding nonatmospheric explanations. Photochemical models corroborate this inference, showing Δ(36)S/Δ(33)S ratios are sensitive to the presence of haze. Exploiting existing age constraints, we estimate that organic haze developed rapidly, stabilizing within ∼0.3 ± 0.1 million years (Myr), and persisted for upward of ∼1.4 ± 0.4 Myr. Given these temporal constraints, and the elevated atmospheric CO2 concentrations in the Archean, the sustained methane fluxes necessary for haze formation can only be reconciled with a biological source. Correlative δ(13)COrg and total organic carbon measurements support the interpretation that atmospheric haze was a transient response of the biosphere to increased nutrient availability, with methane fluxes controlled by the relative availability of organic carbon and sulfate. Elevated atmospheric methane concentrations during haze episodes would have expedited planetary hydrogen loss, with a single episode of haze development providing up to 2.6-18 × 10(18) moles of O2 equivalents to the Earth system. Our findings suggest the Neoarchean likely represented a unique state of the Earth system where haze development played a pivotal role in planetary oxidation, hastening the contingent biological innovations that followed.

  3. The Exchange of Soil Nitrite and Atmospheric HONO: a Missing Process in the Nitrogen Cycle and Atmospheric Chemistry

    NASA Astrophysics Data System (ADS)

    Cheng, Yafang; Su, Hang; Oswald, Robert; Behrendt, Thomas; Trebs, Ivonne; Meixner, Franz X.; Andreae, Meinrat O.; Pöschl, Ulrich

    2013-04-01

    Hydroxyl radicals (OH) are a key species in atmospheric photochemistry. In the lower atmosphere, up to ~30% of the primary OH radical production is attributed to the photolysis of nitrous acid (HONO), and field observations suggest a large missing source of HONO. The dominant sources of N(III) in soil, however, are biological nitrification and denitrification processes, which produce nitrite ions from ammonium (by nitrifying microbes) as well as from nitrate (by denitrifying microbes). We show that soil nitrite can release HONO and explain the reported strength and diurnal variation of the missing source. We also show that the soil-atmosphere exchange of N(III), though not considered in the N cycle, might result in significant amount of reactive nitrogen emission (comparable to soil NO emissions). Fertilized soils with low pH appear to be particularly strong sources of HONO and OH. Thus, agricultural activities and land-use changes may strongly influence the oxidizing capacity of the atmosphere. Because of the widespread occurrence of nitrite-producing microbes and increasing N and acid deposition, the release of HONO from soil may also be important in natural environments, including forests and boreal regions. In view of the potentially large impact on atmospheric chemistry and global environmental change, we recommend further studies of HONO release from soil nitrite and related processes in the biogeochemical cycling of N in both agricultural and natural environments. Reference: Su, H., Cheng, Y., et al., Soil Nitrite as a Source of Atmospheric HONO and OH Radicals, Science, 333, 1616-1618, 10.1126/science.1207687, 2011. Su, H., et al., The Exchange of Soil Nitrite and Atmospheric HONO: A Missing Process in the Nitrogen Cycle and Atmospheric Chemistry, NATO Science for Peace and Security Series C: Environmental Security, Springer Netherlands, 93-99, 2013.

  4. NASA atmospheric effects of aviation projects: Status and plans

    NASA Technical Reports Server (NTRS)

    Wesoky, Howard L.; Thompson, Anne M.; Stolarski, Richard S.

    1994-01-01

    NASA's Atmospheric Effects of Aviation Project is developing a scientific basis for assessment of the atmospheric impact of subsonic and supersonic aviation. Issues addressed include predicted ozone changes and climatic impact, and related uncertainties. A primary goal is to assist assessments of United Nations scientific organizations and, hence, consideration of emission standards by the International Civil Aviation Organization. Project focus is on simulation of atmospheric processes by computer models, but studies of aircraft operations, laboratory studies, and remote and in situ observations of chemical, dynamic, and radiative processes are also included.

  5. Advances in atmospheric chemistry modeling: the LLNL impact tropospheric/stratospheric chemistry model

    SciTech Connect

    Rotman, D A; Atherton, C

    1999-10-07

    We present a unique modeling capability to understand the global distribution of trace gases and aerosols throughout both the troposphere and stratosphere. It includes the ability to simulate tropospheric chemistry that occurs both in the gas phase as well as on the surfaces of solid particles. We have used this capability to analyze observations from particular flight campaigns as well as averaged observed data. Results show the model to accurately simulate the complex chemistry occurring near the tropopause and throughout the troposphere and stratosphere.

  6. Precipitation chemistry - Atmospheric loadings to the surface waters of the Indian River lagoon basin by rainfall

    NASA Technical Reports Server (NTRS)

    Dreschel, Thomas W.; Madsen, Brooks C.; Maull, Lee A.; Hinkle, C. R.; Knott, William M., III

    1990-01-01

    Rain volume and chemistry monitoring as part of the Kennedy Space Center Long Term Environmental Monitoring Program included the years 1984-1987 as part of the National Atmospheric Deposition Program. Atmospheric deposition in rainfall consisted primarily of sea salt and hydrogen ion, sulfate, nitrate, and ammonium ions. The deposition of nitrogen (a principal plant nutrient) was on the order of 200-300 metric tons per year to the surface waters.

  7. Projects in the Physcial Chemistry Laboratory: Letting the Students Choose

    NASA Astrophysics Data System (ADS)

    Buckley, Paul D.; Jolley, Kenneth W.; Watson, Ian D.

    1997-05-01

    In a twelve week Physical Chemistry laboratory course half the time is spent on a standard set of rotation experiments and half on a project of the students own choosing. The students are told that they must only use equipment available within the department and chemicals that are either in the department or which can be ordered on a strictly limited budget. These restriction provide valuable experience in planning research work using limited resources. Initially the projects are based on an article in the literature or on an experiment in a Laboratory Manual and only after successfully repeating the published procedure is the project extended into new areas. Each student gives a short talk outlining the planned experiments before the experimental work begins and/or one presenting the results at the end. A positive attitude to problem solving is encouraged. Successful problem solving is identified through regular review by the class of progress in each project. Students report finding the project a rewarding and challenging experience. The laboratory course is now a more satisfying experience for both staff and students.

  8. Martian atmospheric chemistry during the time of low water abundance

    NASA Technical Reports Server (NTRS)

    Nair, Hari; Allen, Mark; Yung, Yuk L.; Clancy, R. Todd

    1992-01-01

    The importance of odd hydrogen (or HO(x)) radicals in the catalytic recombination of carbon monoxide and oxygen in the Martian atmosphere is a well known fact. The inclusion of recent chemical kinetics data, specifically temperature-dependent CO2 absorption cross sections, into our one dimensional photochemical model shows that HO(x) is too efficient in this regard. The absorption cross sections of CO2 are smaller than previously assumed; this leads to a reduction in the photolysis rate of CO2 while the photolysis rate of H2O has increased. As a consequence the predicted mixing ratio of CO in our models is substantially less than the observed value of 6.5(10)(exp -4). Simultaneous measurements of water, ozone, and carbon monoxide were obtained in the Martian atmosphere in early Dec. 1990 (L(sub s) for Mars was 344 deg.).

  9. Martian atmospheric chemistry during the time of low water abundance

    NASA Technical Reports Server (NTRS)

    Nair, Hari; Allen, Mark; Yung, Yuk L.; Clancy, R. Todd

    1992-01-01

    The importance of odd hydrogen (or HO(x)) radicals in the catalytic recombination of carbon monoxide and oxygen in the Martian atmosphere is a well known fact. The inclusion of recent chemical kinetics data, specifically temperature-dependent CO2 absorption cross sections, into our one dimensional photochemical model shows that HO(x) is too efficient in this regard. The absorption cross sections of CO2 are smaller than previously assumed; this leads to a reduction in the photolysis rate of CO2 while the photolysis rate of H2O has increased. As a consequence the predicted mixing ratio of CO in our models is substantially less than the observed value of 6.5(10)(exp -4). Simultaneous measurements of water, ozone, and carbon monoxide were obtained in the Martian atmosphere in early Dec. 1990 (L(sub s) for Mars was 344 deg.).

  10. The contribution of hydrogen peroxide to atmospheric liquid phase chemistry

    SciTech Connect

    Klockow, D.; Jacob, P.; Bambauer, A.

    1986-04-01

    The most frequently investigated and best understood atmospheric liquid phase process is the oxidation of dissolved sulfur dioxide. The relevant reactions are controlled either by restricted solubilities of the respective species or by high activation energies. The most favorable properties as an oxidant for SO/sub 2/ (aq) under atmospheric conditions are exhibited by hydrogen peroxide: It is highly soluble in water and reacts fast with dissolved sulfur dioxide even at low pH values. In this talk new methodology for determination of hydrogen peroxide in liquid and gas phase is presented. Furthermore results of measurement of hydrogen peroxide in condensed phases (rain, snow, polar ice) as well as in the gas phase are discussed. Finally laboratory and field studies related to formation of hydrogen peroxide in the liquid phase and its reaction with dissolved reduced species ((HSO/sub 3/, NO/sub 2/) under the influence of light are described.

  11. Atmospheric Chemistry of Neonicotinoids Used in Urban Areas

    NASA Astrophysics Data System (ADS)

    Finlayson-Pitts, B. J.; Aregahegn, K.; Shemesh, D.; Gerber, R. B.

    2016-12-01

    Neonicotinoid (NN) pesticides are used extensively in both urban and agricultural settings to control sucking pests such as aphids, as well as for flea control for domestic pets. As a result, they are commonly found on surfaces that are exposed to the atmosphere. Imidacloprid (IMD) is one of the major NNs in pest control formulations. While there have been a number of studies of IMD reactions in solution, there are relatively few surface reactions that are relevant to atmospheric exposures. We report here laboratory studies of the photochemistry of IMD on surfaces in which quantum yields are measured and combined with absorption cross sections to estimate tropospheric lifetimes with respect to photolysis. Products identified using a combination of ATR-FTIR, DART-MS and ESI-MS include the desnitro and urea derivatives in the solid, and N2O in the gas phase. Quantum chemical calculations suggest a mechanism for the photolysis and production of these products. The implications for altering toxicity through atmospheric reactions will be discussed.

  12. Theory of planetary atmospheres: an introduction to their physics and chemistry /2nd revised and enlarged edition/

    SciTech Connect

    Chamberlain, J.W.; Hunten, D.M.

    1987-01-01

    Theoretical models of planetary atmospheres are characterized in an introductory text intended for graduate physics students and practicing scientists. Chapters are devoted to the vertical structure of an atmosphere; atmospheric hydrodynamics; the chemistry and dynamics of the earth stratosphere; planetary astronomy; ionospheres; airglows, auroras, and aeronomy; and the stability of planetary atmospheres. Extensive graphs, diagrams, and tables of numerical data are provided.

  13. Acid deposition and atmospheric chemistry at Allegheny Mountain

    SciTech Connect

    Pierson, W.R.; Brachaczek, W.W.; Gorse, R.A. Jr.; Japar, S.M.; Norbeck, J.M.; Keeler, G.J.

    1986-04-01

    In August, 1983 members of the Research Staff of Ford Motor Company carried out a field experiment at two rural sites in southwestern Pennsylvania involving various aspects of the acid deposition phenomenon. This presentation focuses on the wet (rain) deposition during the experiment, as well as the relative importance of wet and dry deposition processes for nitrate and sulfate at the sites. Other aspects of the experiment have been discussed elsewhere: the chemistry of dew and its role in acid deposition (1), the dry deposition of HNO/sub 3/ and SO/sub 2/ to surrogate surfaces (2), and the role of elemental carbon in light absorption and of light absorption in degradation of visibility (3).

  14. Investigating Titan's Atmospheric Chemistry at Low Temperature in Support of the NASA Cassini Mission

    NASA Astrophysics Data System (ADS)

    Sciamma-O'Brien, Ella; Salama, F.

    2013-06-01

    Titan’s atmosphere, composed mainly of N2 and CH4, is the siege of a complex chemistry induced by solar UV radiation and electron bombardment from Saturn’s magnetosphere. This organic chemistry occurs at temperatures lower than 200 K and leads to the production of heavy molecules and subsequently solid aerosols that form the orange haze surrounding Titan. The Titan Haze Simulation (THS) experiment has been developed on the COSmIC simulation chamber at NASA Ames in order to study the different steps of Titan’s atmospheric chemistry at low temperature and to provide laboratory data in support for Cassini data analysis. The chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas mixture is adiabatically cooled to Titan-like temperature 150 K) before inducing the chemistry by plasma discharge. Different gas mixtures containing N2, CH4, and the first products of the N2-CH4 chemistry (C2H2, C2H4, C6H6…) but also heavier molecules such as PAHs or nitrogen containing PAHs can be injected. Both the gas phase and solid phase products resulting from the plasma-induced chemistry can be monitored and analyzed. Here we present the results of recent gas phase and solid phase studies that highlight the chemical growth evolution when injecting heavier hydrocarbon trace elements in the initial N2-CH4 mixture. Due to the short residence time of the gas in the plasma discharge, only the first steps of the chemistry have time to occur in a N2-CH4 discharge. However by adding acetylene and benzene to the initial N2-CH4 mixture, we can study the intermediate steps of Titan’s atmospheric chemistry as well as specific chemical pathways. These results show the uniqueness of the THS experiment to help understand the first and intermediate steps of Titan’s atmospheric chemistry as well as specific chemical pathways leading to Titan’s haze formation. Aknowledgements: This research is supported by NASA SMD (PATM). E

  15. "Holes" in Student Understanding: Addressing Prevalent Misconceptions regarding Atmospheric Environmental Chemistry

    ERIC Educational Resources Information Center

    Kerr, Sara C.; Walz, Kenneth A.

    2007-01-01

    There is a misconception among undergraduate students that global warming is caused by holes in the ozone layer. In this study, we evaluated the presence of this and other misconceptions surrounding atmospheric chemistry that are responsible for the entanglement of the greenhouse effect and the ozone hole in students' conceptual frameworks. We…

  16. "Holes" in Student Understanding: Addressing Prevalent Misconceptions regarding Atmospheric Environmental Chemistry

    ERIC Educational Resources Information Center

    Kerr, Sara C.; Walz, Kenneth A.

    2007-01-01

    There is a misconception among undergraduate students that global warming is caused by holes in the ozone layer. In this study, we evaluated the presence of this and other misconceptions surrounding atmospheric chemistry that are responsible for the entanglement of the greenhouse effect and the ozone hole in students' conceptual frameworks. We…

  17. Ion chemistry and N-containing molecules in Titan's upper atmosphere

    NASA Astrophysics Data System (ADS)

    Vuitton, V.; Yelle, R. V.; McEwan, M. J.

    2007-11-01

    High-energy photons, electrons, and ions initiate ion-neutral chemistry in Titan's upper atmosphere by ionizing the major neutral species (nitrogen and methane). The Ion and Neutral Mass Spectrometer (INMS) onboard the Cassini spacecraft performed the first composition measurements of Titan's ionosphere. INMS revealed that Titan has the most compositionally complex ionosphere in the Solar System, with roughly 50 ions at or above the detection threshold. Modeling of the ionospheric composition constrains the density of minor neutral constituents, most of which cannot be measured with any other technique. The species identified with this approach include the most complex molecules identified so far on Titan. This confirms the long-thought idea that a very rich chemistry is actually taking place in this atmosphere. However, it appears that much of the interesting chemistry occurs in the upper atmosphere rather than at lower altitudes. The species observed by INMS are probably the first intermediates in the formation of even larger molecules. As a consequence, they affect the composition of the bulk atmosphere, the composition and optical properties of the aerosols and the flux of condensable material to the surface. In this paper, we discuss the production and loss reactions for the ions and how this affects the neutral densities. We compare our results to neutral densities measured in the stratosphere by other instruments, to production yields obtained in laboratory experiments simulating Titan's chemistry and to predictions of photochemical models. We suggest neutral formation mechanisms and highlight needs for new experimental and theoretical data.

  18. A Controlled-Environment Chamber for Atmospheric Chemistry Studies Using FT-IR Spectroscopy

    DTIC Science & Technology

    1990-06-01

    A one-meter diameter, Teflon coated, stainless steel sph ere has been constructed as a tool for conducting studies of the atmospheric chemistry of...port to determine their effects on gases under study . The chamber is equipped with an in situ, multipass optical system which allows infrared path

  19. [Relationship between atmospheric particles and rain water chemistry character].

    PubMed

    Huo, Ming-Qun; Sun, Qian; Xie, Peng; Bai, Yu-Hua; Liu, Zhao-Rong; Li, Ji-Long; Lu, Si-Hua

    2009-11-01

    Rain and atmospheric particle samples were collected in the rural area of Taian and Shenzhen in 2007, respectively. Rain sampling was carried out during the precipitation process and several samples were got from the beginning of one precipitation to the end. The chemical character changes during precipitation and the changes of concentration of particles before and after rain were studied in this research to understand the contribution of particles on the rain chemical character and the rain-out effect for particles. The volume-weighted mean pH of rainwater in Taian was 5.97 and the total concentration of ions was 1 187.96 microeq x L(-1). The mass concentration of PM10 in Taian was 131.76 microg/m3 and that of PM2.5 was 103.84 microg/m3. The volume-weighted mean pH of rainwater in Shenzhen was 4.72 and the total concentration of ions was 175.89 microeq x L(-1). The mass concentration of PM10 in Shenzhen was 56.66 microg/m3 and that of PM2.5 was 41.52 microg/m3. During precipitation process pH and ion concentration of rain decrease and it is shown the neutralizing effect happens. The difference between rainwater of Taian and Shenzhen is due to cloud water acidity, atmospheric particles character and atmospheric acid-basic gases concentration. The clean-up effect of Na+ and Ca2+ by rain is high and which of NH4+ and NO3- is low. The clean-up effect for mass concentration, ions concentration and element concentration of particles by rain are significant.

  20. Atmospheric Chemistry of Toxic Industrial Chemicals (Briefing Slides)

    DTIC Science & Technology

    2007-01-11

    22 days≥ 188 days≥ 400 days14 daysAcetylene ~4 days35 min36 min4.3 hourstrans- 2 - Butene 5 days205 days≥ 1300 yr5 daysn-Butane Cl [1 x 104 cm- 3 ...REPORT DATE (DD-MM-YYYY) 2 . REPORT TYPE 3 . DATES COVERED (From - To) 4. TITLE AND SUBTITLE 5a. CONTRACT NUMBER 5b. GRANT NUMBER 5c. PROGRAM...identical except that the lower right is accounting for the reactivity of 2 - methyl propene in the atmosphere. I’ve placed two arrows on the map to help

  1. The atmospheric chemistry box model CAABA/MECCA-3.0gmdd

    NASA Astrophysics Data System (ADS)

    Sander, R.; Baumgaertner, A.; Gromov, S.; Harder, H.; Jöckel, P.; Kerkweg, A.; Kubistin, D.; Regelin, E.; Riede, H.; Sandu, A.; Taraborrelli, D.; Tost, H.; Xie, Z.-Q.

    2011-01-01

    We present version 3.0gmdd of the atmospheric chemistry box model CAABA/MECCA. In addition to a complete update of the rate coefficients to the most recent recommendations, a number of new features have been added: chemistry in multiple aerosol size bins; automatic multiple simulations reaching steady-state conditions; Monte-Carlo simulations with randomly varied rate coefficients within their experimental uncertainties; calculations along Lagrangian trajectories; mercury chemistry; more detailed isoprene chemistry; tagging of isotopically labeled species. Further changes have been implemented to make the code more user-friendly and to facilitate the analysis of the model results. Like earlier versions, CAABA/MECCA-3.0gmdd is a community model published under the GNU General Public License (GPL).

  2. The atmospheric chemistry box model CAABA/MECCA-3.0

    NASA Astrophysics Data System (ADS)

    Sander, R.; Baumgaertner, A.; Gromov, S.; Harder, H.; Jöckel, P.; Kerkweg, A.; Kubistin, D.; Regelin, E.; Riede, H.; Sandu, A.; Taraborrelli, D.; Tost, H.; Xie, Z.-Q.

    2011-05-01

    We present version 3.0 of the atmospheric chemistry box model CAABA/MECCA. In addition to a complete update of the rate coefficients to the most recent recommendations, a number of new features have been added: chemistry in multiple aerosol size bins; automatic multiple simulations reaching steady-state conditions; Monte-Carlo simulations with randomly varied rate coefficients within their experimental uncertainties; calculations along Lagrangian trajectories; mercury chemistry; more detailed isoprene chemistry; tagging of isotopically labeled species. Further changes have been implemented to make the code more user-friendly and to facilitate the analysis of the model results. Like earlier versions, CAABA/MECCA-3.0 is a community model published under the GNU General Public License.

  3. State-of-the-art chamber facility for studying atmospheric aerosol chemistry.

    PubMed

    Cocker, D R; Flagan, R C; Seinfeld, J H

    2001-06-15

    A state-of-the-art chamber facility is described for investigation of atmospheric aerosol chemistry. Dual 28 m3 FEP Teflon film chambers are used to simulate atmospheric conditions in which aerosol formation may occur. This facility provides the flexibility to investigate dark, single oxidant reactions as well as full photochemical simulations. This paper discusses the environmental control implemented as well as the gas-phase and aerosol-phase instrumentation used to monitor atmospheric aerosol formation and growth. Physical processes occurring in the chamber and procedures for estimating secondary organic aerosol formation during reaction are described. Aerosol formation and evolution protocols at varying relative humidity conditions are presented.

  4. Sentinel-5 Precursor: First Copernicus Atmospheric Chemistry Mission ready for Launch

    NASA Astrophysics Data System (ADS)

    McMullan, Kevin; Nett, Herbert

    2017-04-01

    Sentinel-5 Precursor (S-5P) will be the first of a series of atmospheric chemistry missions to be launched within the European Commission's Copernicus (former GMES) Programme. With the current launch window of June 2017 and a nominal lifetime of 7 years, S-5P is expected to provide continuity in the availability of global atmospheric data products between its predecessor missions SCIAMACHY (Envisat) and OMI (AURA) and the future Sentinel-4 and -5 series. S-5P will deliver unique data regarding the sources and sinks of trace gases with a focus on the lower Troposphere including the planet boundary layer due to its enhanced spatial, temporal and spectral sampling capabilities as compared to its predecessors. The S-5P satellite will carry a single payload, TROPOMI (TROPOspheric Monitoring Instrument) which is jointly developed by The Netherlands and ESA. Covering spectral channels in the UV, visible, near- and short-wave infrared, it will measure various key species including tropospheric/stratospheric ozone, NO2, SO2, CO, CH4, CH2O as well as cloud and aerosol parameters. The S-5P Project successfully passed the Ground Segment Acceptance Review (GS-AR) and the satellite-level Qualification Acceptance Review (QAR) in March and April 2016, respectively. Remaining pre-launch tasks focus on the detailed planning of Phase E1 activities and the training of the operations teams. The paper includes descriptions of the S-5p spacecraft, the TROPOMI instrument, data products and applications, Level-1b and Level-2 processing, Ground Segment, launch preparation, launch and in-orbit commissioning and in-flight calibration and validation.

  5. Fundamental surface processes in heterogeneous atmospheric chemistry: Applications to sea-salt (NaCl) and oxide particulate chemistry

    NASA Astrophysics Data System (ADS)

    Allen, Heather Cecile

    1997-10-01

    Although heterogeneous phenomena are important in many atmospheric processes, these complex systems have been difficult to study at the fundamental level. Surface- sensitive techniques are currently being utilized to probe the chemistry of heterogeneous atmospheric systems. In addition to presenting fundamental surface chemistry of several systems, this dissertation shows that surface- sensitive and electron microscopy technology can provide substantial insight into heterogeneous atmospheric processes. Transmission electron microscopy and energy dispersive spectroscopy (TEM-EDS) were used to better understand fundamental mechanisms of the reaction of sodium chloride with nitric acid vapor (and reaction with nitrogen dioxide) followed by water vapor. Results show for the first time that exposures to water vapor can lead to major reconstruction and concurrent recrystallization of the surface after reaction of NaCl(s) with HNO3(g). This has significant implications for tropospheric chemistry in polluted urban regions. The entire volume of airborne sea-salt (i.e. NaCl) particles is available for reaction due to the water-induced reorganization of the surface. Additional studies presented here include: (1) Laser induced desorption-Fourier transform mass spectrometry (LID-FTMS) studies of the reactivity of thin films of aluminum oxide (γ- Al2O3/NiAl(100)) after exposure to molecules relevant to tropospheric and stratospheric particulate chemistry, (2) TEM-EDS studies of stratospheric particles, and (3) Thermal desorption spectroscopy (TDS) of CO/NiAl(100). TDS and LID-FTMS studies reveal that non-hydroxylated γ- Al2O3/NiAl(100) is inert toward the adsorption of CF2Cl2 and HCF2Cl. LID-FTMS results show that 1,3-butadiene desorbs intact from non- hydroxylated γ- Al2O3/NiAl(100) at ~200 K. The TEM-EDS studies of stratospheric particles reveal that submicron alumina spheres are amorphous. Previous studies of submicron alumina spheres showed that γ-alumina was the

  6. Equilibrium Chemistry of the Atmospheres of Scorched Rocky Exoplanets

    NASA Astrophysics Data System (ADS)

    Schaefer, Laura; Lodders, K.; Fegley, B., Jr.

    2011-01-01

    The Kepler and COROT missions and Earth-based observations detected putative rocky exoplanets. Some of the planets are exposed to extreme temperatures as they orbit close to their host stars, e.g., CoRot-7b. Such planets can develop atmospheres through (partial) vaporization of their exterior crusts or even mantle silicates. We investigated the chemical equilibrium composition of such heated systems from 500 - 4000 K and total pressures from 10-6 to 10+2.5 bars. The major gas phase species formed by the volatile elements H, C, N, O, and S, and the lithophile elements Na, K, Fe, Si, Mg, Al, Ca, and Ti are H2O and CO2 at low temperatures, and Na, K, O2, SiO, and O at high temperatures. The effects on overall elemental composition of the evaporated systems will be discussed. The computational results will be useful in planning spectroscopic studies of the atmospheres of hot Earth-like exoplanets. This work was supported by the NSF Astronomy Program and the NASA Astrobiology Program.

  7. Atmospheric chemistry of CF3CF2OCH3

    NASA Astrophysics Data System (ADS)

    Østerstrøm, Freja F.; Nielsen, Ole John; Wallington, Timothy J.

    2016-06-01

    Smog chamber Fourier transform infrared techniques were used to investigate the kinetics of the reaction of CF3CF2OCH3 with Cl atoms and OH radicals: k(Cl + CF3CF2OCH3) = (1.09 ± 0.16) × 10-13 and k(OH + CF3CF2OCH3) = (1.28 ± 0.19) × 10-14 cm3 molecule-1 s-1 in 700 Torr total pressure of N2/O2 at 296 ± 2 K. The Cl-initiated oxidation of CF3CF2OCH3 gives CF3CF2OCHO in a yield indistinguishable from 100%. An estimate of k(Cl + CF3CF2OCHO) = (1.18 ± 0.34) × 10-14 cm3 molecule-1 s-1 is provided. Based on the OH reaction rate, the atmospheric lifetime of CF3CF2OCH3 is estimated to be 5.0 years. The 100-year time horizon global warming potential of CF3CF2OCH3 is estimated to be 585. The atmospheric impact of CF3CF2OCH3 is discussed.

  8. On the numerical treatment of problems in atmospheric chemistry

    SciTech Connect

    Aro, Colin J.

    1995-09-01

    Atmospheric chemical-radiative-transport (CRT) models are vital in performing research on atmospheric chemical change. Even with the enormous computing capability delivered by massively parallel systems, extended three dimensional CRT simulations are still not computationally feasible. The major obstacle in a CRT model is the nonlinear ODE system describing the chemical kinetics in the model. These ODE systems are usually very stiff and account for anywhere from 75% to 90% of the CPU time required to run a CRT model. In this study, a simple explicit class of time stepping method is developed and demonstrated to be useful in treating chemical ODE systems without the use of a Jacobian matrix. These methods, called preconditioned time differencing methods, are tested on small mathematically idealized problems, box model problems, and full 2-D and 3-D CRT models. The methods are found to be both fast and memory efficient. Studies are performed on both vector and parallel systems. The preconditioned time differencing methods are established as a viable alternative to the more common backward differentiation formulas in terms of CPU speed across architectural platforms.

  9. Soil Moisture-Atmosphere Feedbacks on Atmospheric Tracers: The Effects of Soil Moisture on Precipitation and Near-Surface Chemistry

    NASA Astrophysics Data System (ADS)

    Tawfik, Ahmed B.

    The atmospheric component is described by rapid fluctuations in typical state variables, such as temperature and water vapor, on timescales of hours to days and the land component evolves on daily to yearly timescales. This dissertation examines the connection between soil moisture and atmospheric tracers under varying degrees of soil moisture-atmosphere coupling. Land-atmosphere coupling is defined over the United States using a regional climate model. A newly examined soil moisture-precipitation feedback is identified for winter months extending the previous summer feedback to colder temperature climates. This feedback is driven by the freezing and thawing of soil moisture, leading to coupled land-atmosphere conditions near the freezing line. Soil moisture can also affect the composition of the troposphere through modifying biogenic emissions of isoprene (C5H8). A novel first-order Taylor series decomposition indicates that isoprene emissions are jointly driven by temperature and soil moisture in models. These compounds are important precursors for ozone formation, an air pollutant and a short-lived forcing agent for climate. A mechanistic description of commonly observed relationships between ground-level ozone and meteorology is presented using the concept of soil moisture-temperature coupling regimes. The extent of surface drying was found to be a better predictor of ozone concentrations than temperature or humidity for the Eastern U.S. This relationship is evaluated in a coupled regional chemistry-climate model under several land-atmosphere coupling and isoprene emissions cases. The coupled chemistry-climate model can reproduce the observed soil moisture-temperature coupling pattern, yet modeled ozone is insensitive to changes in meteorology due to the balance between isoprene and the primary atmospheric oxidant, the hydroxyl radical (OH). Overall, this work highlights the importance of soil moisture-atmosphere coupling for previously neglected cold climate

  10. A simplified chemistry module for atmospheric transport and dispersion models: Proof-of-concept using SCIPUFF

    NASA Astrophysics Data System (ADS)

    Burns, Douglas S.; Rottmann, Shawn D.; Plitz, Angela B. L.; Wiseman, Floyd L.; Moore, William; Chynwat, Veeradej

    2012-09-01

    An atmospheric chemistry module was developed to predict the fate of environmentally hazardous compounds discharged into the atmosphere. The computationally efficient model captures the diurnal variation within the environment and in the degradation rates of the released compounds, follows the formation of toxic degradation products, runs rapidly, and in principle can be integrated with any atmospheric transport and dispersion model. To accomplish this, a detailed atmospheric chemistry mechanism for a target toxic industrial compound (TIC) was reduced to a simple empirical effective degradation rate term (keff). Empirically derived decay functions for keff were developed as a function of important meteorological parameters such as solar flux, temperature, humidity, and cloud cover for various land uses and locations by statistically analyzing data generated from a detailed chemistry mechanism run over a wide range of (typical) atmospheric conditions. 1-Butene and two degradation products (propanal and nitrooxybutanone) were used as representative chemicals in the algorithm development for this proof-of-concept demonstration of the capability of the model. The quality of the developed model was evaluated via comparison with experimental chamber data and the results (decay rates) compared favorably for ethene, propene, and 1-butene (within a factor of two 75% or more of the time).

  11. Photochemical Formation of Aerosol in Planetary Atmospheres: Photon and Water Mediated Chemistry of SO_2

    NASA Astrophysics Data System (ADS)

    Kroll, Jay A.; Donaldson, D. J.; Vaida, Veronica

    2016-06-01

    Sulfur compounds have been observed in a number of planetary atmospheres throughout our solar system. Our current understanding of sulfur chemistry explains much of what we observe in Earth's atmosphere. However, several discrepancies between modeling and observations of the Venusian atmosphere show there are still problems in our fundamental understanding of sulfur chemistry. This is of particular concern due to the important role sulfur compounds play in the formation of aerosols, which have a direct impact on planetary climates, including Earth's. We investigate the role of water complexes in the hydration of sulfur oxides and dehydration of sulfur acids and will present spectroscopic studies to document such effects. I will present recent work investigating mixtures of SO_2 and water that generate large quantities of aerosol when irradiated with solar UV light, even in the absence of traditional OH chemistry. I will discuss a proposed mechanism for the formation of sulfurous acid (H_2SO_3) and present recent experimental work that supports this proposed mechanism. Additionally, the implications that photon-induced hydration of SO_2 has for aerosol formation in the atmosphere of earth as well as other planetary atmospheres will be discussed.

  12. NUCLA Circulating Atmospheric Fluidized Bed Demonstration Project

    SciTech Connect

    Not Available

    1992-02-01

    The objective of this DOE Cooperative Agreement is to conduct a cost-shared clean coal technology project to demonstrate the feasibility of circulating fluidized bed combustion technology and to evaluate economic, environmental, and operational benefits of CFB steam generators on a utility scale. At the conclusion of the Phase 2 program, testing related to satisfying these objectives was completed. Data analysis and reporting are scheduled for completion by October 1991. (VC)

  13. Trends in Mesospheric Dynamics and Chemistry: Simulations With a Model of the Entire Atmosphere

    NASA Astrophysics Data System (ADS)

    Brasseur, G. P.

    2005-05-01

    The cooling resulting from infrared CO2 radiative transfer is a major contribution to the energy budget of the middle atmosphere and thermosphere. The rapid increase of the atmospheric CO2 concentration resulting from anthropogenic emissions is therefore expected to lead, in general, to a substantial cooling in this height range. This can potentially be counteracted by heating due to absorption of near infrared radiation by CO2. Changes in ozone as a consequence of increasing methane and water vapor may also have an impact on the energy budget as dynamical changes caused by increased tropospheric temperatures. By means of numerical simulations with a general circulation and chemistry model of the entire atmosphere we will address the following questions: 1.) Can state-of-the-art atmospheric modeling explain the mesospheric temperature trends observed during the last decades? 2.)Which part of the temperature changes resulting from an increase of atmospheric CO2 is caused by local changes in the radiative budget and which part is influenced by remote dynamical effects? The model used is the newly developed Hamburg Model of the Neutral and Ionized Atmosphere (HAMMONIA) that resolves the atmosphere from the Earth's surface up to about 250 km altitude, and is based on the 3-D dynamics from the ECHAM5 general circulation model and the chemistry scheme from MOZART-3. Results from different time slice experiment representative of years 1970 and 2000, and for a doubling of CO2 will be presented.

  14. Atmospheric cloud physics laboratory project study

    NASA Technical Reports Server (NTRS)

    Schultz, W. E.; Stephen, L. A.; Usher, L. H.

    1976-01-01

    Engineering studies were performed for the Zero-G Cloud Physics Experiment liquid cooling and air pressure control systems. A total of four concepts for the liquid cooling system was evaluated, two of which were found to closely approach the systems requirements. Thermal insulation requirements, system hardware, and control sensor locations were established. The reservoir sizes and initial temperatures were defined as well as system power requirements. In the study of the pressure control system, fluid analyses by the Atmospheric Cloud Physics Laboratory were performed to determine flow characteristics of various orifice sizes, vacuum pump adequacy, and control systems performance. System parameters predicted in these analyses as a function of time include the following for various orifice sizes: (1) chamber and vacuum pump mass flow rates, (2) the number of valve openings or closures, (3) the maximum cloud chamber pressure deviation from the allowable, and (4) cloud chamber and accumulator pressure.

  15. The chemistry of atmospheric bromine. [catalyst for ozone destruction

    NASA Technical Reports Server (NTRS)

    Wofsy, S. C.; Mcelroy, M. B.; Yung, Y. L.

    1975-01-01

    Bromine may act as a catalyst for recombination of ozone and could be more efficient than either nitric oxide or chlorine. The lower atmosphere contains small concentrations of gaseous bromine produced in part by marine activity and volatilization of particulate material released during the combustion of leaded gasoline, with an additional contribution due to the use of methyl bromide as an agricultural fumigant. Observations by Lazrus et al., (1975) indicate small concentrations of bromine, about 10 to the -11th power (v/v), in the contemporary stratosphere and appear to imply a reduction of approximately 0.3% in the global budget of O3. Estimates are given for future reductions in O3 which might occur if the use of CH3Br as an agricultural fumigant were to continue to grow at present rates.

  16. Heterogeneous chemistry of HOBR on surfaces characteristic of atmospheric aerosols

    SciTech Connect

    Abbatt, J.P.D.

    1995-12-31

    The heterogeneous interactions of HOBr, HBr and HCl with ice and supercooled sulfuric acid solutions have been studied in a low temperatures low pressure flow tube coupled to a mass spectrometer. The heterogeneous reactions HOBr + HCl {yields} BrCl + H{sub 2}O and HOBr + HBr {yields} Br{sub 2} + H{sub 2}O have been demonstrated to proceed readily on these surfaces, and it has been shown that both HOBr and HBr are more easily partitioned to the condensed phase than their chlorine analogues. These heterogeneous reactions represent routes for the activation of halogen species in the atmosphere. In particular, the implications of this research to the depletion of stratospheric ozone after the Mt. Pinatubo volcanic eruption and to the depletion of ozone in the springtime Arctic boundary layer will be discussed.

  17. Atmospheric chemistry: Laboratory studies of kinetics of important reactions

    NASA Astrophysics Data System (ADS)

    Smith, S. J.

    Experiments to measure the rate constants for some reactions of the atmospherically important nitrate radical (NO3) are described using the discharge-flow technique. The nitrate radical was monitored by optical absorption at lambda = 662 nm. The reactions of NO3 with some stable organic and inorganic substrates are reported. The temperature dependences of some of the rate constants were also determined (298 less than T less than 523 K). In most cases, computer simulation was used to extract the rate constant for the primary process because the time-dependent behavior of (NO3) was affected by secondary reactions of NO3 with products of the primary interaction. The Arrhenius parameter for the reactions of NO3 with CH3CH3, CH2CH2, CH3OH, CHCl3, and HCl were determined. The activation energies for the reactions studied between NO3 and some alkynes are presented along with the corresponding pre-exponential factors. Some reactions were studied at room temperature (298 plus or minus 2 K) only and the rate constants found (in units of cubic cm/molecule sec) are: buta-1,3-diene (1.8 x 10 (exp -13), isobutene (2.8 x 10 (exp -13), HBr (1.3 x 10 (exp -15) and hex-2-yne (3.0 x 10 (exp -14). Non-Arrhenius behavior was found in the reactions of NO3 with n-butane, isobutane and propene. The empirical variation of these rate constants with temperature is presented. The curvature of the Arrhenius plots is discussed in terms of (1) a temperature-dependent pre-exponential factor, and (2) the possibility that two competing channels, possessing differing activation energies, exist for each reaction. The atmospheric implications of these reactions are discussed with reference to the nighttime production of nitric acid and the importance of the these reactions as loss processes for NO3.

  18. The ChemViz Project: Using a Supercomputer To Illustrate Abstract Concepts in Chemistry.

    ERIC Educational Resources Information Center

    Beckwith, E. Kenneth; Nelson, Christopher

    1998-01-01

    Describes the Chemistry Visualization (ChemViz) Project, a Web venture maintained by the University of Illinois National Center for Supercomputing Applications (NCSA) that enables high school students to use computational chemistry as a technique for understanding abstract concepts. Discusses the evolution of computational chemistry and provides a…

  19. Making a Natural Product Chemistry Course Meaningful with a Mini Project Laboratory

    ERIC Educational Resources Information Center

    Hakim, Aliefman; Liliasari; Kadarohman, Asep; Syah, Yana Maolana

    2016-01-01

    This paper discusses laboratory activities that can improve the meaningfulness of natural product chemistry course. These laboratory activities can be useful for students from many different disciplines including chemistry, pharmacy, and medicine. Students at the third-year undergraduate level of chemistry education undertake the project to…

  20. The ChemViz Project: Using a Supercomputer To Illustrate Abstract Concepts in Chemistry.

    ERIC Educational Resources Information Center

    Beckwith, E. Kenneth; Nelson, Christopher

    1998-01-01

    Describes the Chemistry Visualization (ChemViz) Project, a Web venture maintained by the University of Illinois National Center for Supercomputing Applications (NCSA) that enables high school students to use computational chemistry as a technique for understanding abstract concepts. Discusses the evolution of computational chemistry and provides a…

  1. Making a Natural Product Chemistry Course Meaningful with a Mini Project Laboratory

    ERIC Educational Resources Information Center

    Hakim, Aliefman; Liliasari; Kadarohman, Asep; Syah, Yana Maolana

    2016-01-01

    This paper discusses laboratory activities that can improve the meaningfulness of natural product chemistry course. These laboratory activities can be useful for students from many different disciplines including chemistry, pharmacy, and medicine. Students at the third-year undergraduate level of chemistry education undertake the project to…

  2. Chemistry of dimethyl sulfide in the equatorial Pacific atmosphere

    SciTech Connect

    Bandy, A.R.; Thornton, D.C.; Blomquist, B.W.

    1996-04-01

    A field study of the chemistry of dimethyl sulfide (DMS) was conducted on the island of Kiritimati (Christmas Island) during July and August, 1994. This island is located at 2{degrees}N, 157{degrees}W approximately 2000km south of Hawaii. The authors obtained a very repeatable diurnal variation for both DMS and sulfur dioxide (SO{sub 2}) during two 5-day and one 2-day experiments. Near sunrise DMS was about 200pptv. It decreased to about 120 pptv by late afternoon. During the daytime SO{sub 2} increased from about 20 pptv to about 75 pptv. At night DMS increased and SO{sub 2} decreased almost linearly. About 62% of the DMS was converted to SO{sub 2}. DMS was emitted from the ocean at an average flux of 3.7 x 10{sup 13} molecules in m{sup {minus}2}s{sup {minus}1}. The average dry deposition velocity of SO{sub 2} was 6.8 mm sec{sup {minus}1} Most of the SO{sub 2} appeared to be lost to the ocean although a comparable but not significantly larger flux to aerosol cannot be ruled out. Dimethyl sulfoxide was in the range 10 to 50 pptv with a mean of about 25 pptv. Dimethyl sulfone was in the range 0 to 15 pptv with a mean of about 3 pptv. There was no diurnal trend in other species. A much smaller fraction of the DMS was converted to dimethyl sulfone than dimethyl sulfoxide. 27 refs., 2 fig., 2 tab.

  3. Acid rain and atmospheric chemistry at Allegheny Mountain

    SciTech Connect

    Pierson, W.R.; Brachaczek, W.W.; Gorse, R.A. Jr.; Japar, S.M.; Norbeck, J.M.; Keeler, G.J.

    1987-07-01

    Rain chemistry was measured in August 1983 on Allegheny Mountain and Larel Hill in southwester Pennsylvania. The average composition approximated an H/sub 2/SO/sub 5//HNO/sub 3/ mixture with a volume-weighted average pH of 3.5 and an SO/sub 4//sup 2 -//NO/sub 3//sup -/ mole ratio of 1.8. There was very little undissociated (weak) acidity and very little S(IV). The acidic rains were associated with air masses traversing SO/sub 2/ source regions west of the sites; stagnation and intervening precipitation were important influences. The geographic scale for a halving of rain SO/sub 4//sup 2 -/ concentration downwind of SO/sub 2/ sources was approx.440 km. Scavenging ratios were inferred for SO/sub 2/, aerosol SO/sub 4//sup 2 -/, and HNO/sub 3/. On average about half of the rain SO/sub 4//sup 2 -/ resulted from scavenging of SO/sub 2/, the rest from scavenging of SO/sub 4//sup 2 -/. The rain H/sup +/ was attributed about 25% to HNO/sub 3/, 55% to scavenging of SO/sub 2/, and 20% to scavenging of aerosol acid SO/sub 4//sup 2 -/. Cumulative deposition totals in rain were compared with deposition in fog and with dry deposition in the same experiment. A crude acid-deposition budget was calculated as follows: 47%, H/sub 2/SO/sub 4/ in rain; 23%, SO/sub 2/ dry deposition without dew; 16%, HNO/sub 3/ in rain; 11%, HNO/sub 3/ dry deposition without dew; 2%, HNO/sub 3/ and H/sub 2/SO/sub 4/ in fog and dew; 0.5%, aerosol dry deposition without dew. 86 references, 4 figures, 8 tables.

  4. Plant surface reactions: an ozone defence mechanism impacting atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Jud, W.; Fischer, L.; Canaval, E.; Wohlfahrt, G.; Tissier, A.; Hansel, A.

    2015-07-01

    Elevated tropospheric ozone concentrations are considered a toxic threat to plants, responsible for global crop losses with associated economic costs of several billion dollars per year. Plant injuries have been linked to the uptake of ozone through stomatal pores and oxidative damage of the internal leaf tissue. But a striking question remains: how much ozone effectively enters the plant through open stomata and how much is lost by chemical reactions at the plant surface? In this laboratory study we could show that semi-volatile organic compounds exuded by the glandular trichomes of different Nicotiana tabacum varieties are an efficient ozone sink at the plant surface. In our experiments, different diterpenoid compounds were responsible for a strongly variety dependent ozone uptake of plants under dark conditions, when stomatal pores are almost closed. Surface reactions of ozone were accompanied by prompt release of oxygenated volatile organic compounds, which could be linked to the corresponding precursor compounds: ozonolysis of cis-abienol (C20H34O) - a diterpenoid with two exocyclic double bonds - caused emissions of formaldehyde (HCHO) and methyl vinyl ketone (C4H6O). The ring-structured cembratrien-diols (C20H34O2) with three endocyclic double bonds need at least two ozonolysis steps to form volatile carbonyls such as 4-oxopentanal (C5H8O2), which we could observe in the gas phase, too. Fluid dynamic calculations were used to model ozone distribution in the diffusion limited leaf boundary layer under daylight conditions. In the case of an ozone-reactive leaf surface, ozone gradients in the vicinity of stomatal pores are changed in such a way, that ozone flux through the open stomata is strongly reduced. Our results show that unsaturated semi-volatile compounds at the plant surface should be considered as a source of oxygenated volatile organic compounds, impacting gas phase chemistry, as well as efficient ozone sink improving the ozone tolerance of plants.

  5. Evaluation of laboratory kinetics and photochemical data for atmospheric chemistry applications.

    PubMed

    Cox, R A

    2012-10-07

    This article deals with the evaluation of chemical kinetics and photochemical data for use in atmospheric modeling. Models used to calculate the temporal and spatial variation of atmospheric trace gas composition are based on chemical schemes which require chemical kinetics data for the elementary reactions involved. These data derive from careful experimentation under conditions relevant for the atmosphere, carried out in laboratories worldwide using ever improving technology over the past 50 years. The article contains an account of the background issues of atmospheric composition change which have stimulated this branch of atmospheric science; this is followed by a section on parameterisation and evaluation of kinetics data. A description of currently available on-line databases is provided. The final section contains a short description of some recent significant improvement in knowledge of rate constants for key reactions of interest in stratospheric and tropospheric chemistry.

  6. Science Project Ideas about Kitchen Chemistry. Revised Edition.

    ERIC Educational Resources Information Center

    Gardner, Robert

    This book presents science experiments that can be conducted in the kitchen. Contents include: (1) "Safety First"; (2) "Chemistry in and Near the Kitchen Sink"; (3) "Chemistry in the Refrigerator"; (4) "Chemistry on the Stove"; (5) "Chemistry on the Kitchen Counter"; and (6) "Further Reading and Internet Addresses." (YDS)

  7. Understanding differences in chemistry climate model projections of stratospheric ozone

    NASA Astrophysics Data System (ADS)

    Douglass, A. R.; Strahan, S. E.; Oman, L. D.; Stolarski, R. S.

    2014-04-01

    Chemistry climate models (CCMs) are used to project future evolution of stratospheric ozone as concentrations of ozone-depleting substances (ODSs) decrease and greenhouse gases increase, cooling the stratosphere. CCM projections exhibit not only many common features but also a broad range of values for quantities such as year of ozone return to 1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to ODS concentration change from that due to climate change. We show that the sensitivity of lower stratospheric ozone to chlorine change ΔO3/ΔCly is a near-linear function of partitioning of total inorganic chlorine (Cly) into its reservoirs; both Cly and its partitioning are largely controlled by lower stratospheric transport. CCMs with best performance on transport diagnostics agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035, differences in ΔO3/ΔCly contribute little to the spread in CCM projections as the anthropogenic contribution to Cly becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change ΔO3/ΔT due to different contributions from various ozone loss processes, each with its own temperature dependence. Ozone decrease in the tropical lower stratosphere caused by a projected speedup in the Brewer-Dobson circulation may or may not be balanced by ozone increases in the middle- and high-latitude lower stratosphere and upper troposphere. This balance, or lack thereof, contributes most to the spread in late 21st century projections.

  8. Understanding Differences in Chemistry Climate Model Projections of Stratospheric Ozone

    NASA Technical Reports Server (NTRS)

    Douglass, A. R.; Strahan, S. E.; Oman, L. D.; Stolarski, R. S.

    2014-01-01

    Chemistry climate models (CCMs) are used to project future evolution of stratospheric ozone as concentrations of ozone-depleting substances (ODSs) decrease and greenhouse gases increase, cooling the stratosphere. CCM projections exhibit not only many common features but also a broad range of values for quantities such as year of ozone return to 1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to ODS concentration change from that due to climate change. We show that the sensitivity of lower stratospheric ozone to chlorine change Delta Ozone/Delta inorganic chlorine is a near-linear function of partitioning of total inorganic chlorine into its reservoirs; both inorganic chlorine and its partitioning are largely controlled by lower stratospheric transport. CCMs with best performance on transport diagnostics agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035, differences in Delta Ozone/Delta inorganic chlorine contribute little to the spread in CCM projections as the anthropogenic contribution to inorganic chlorine becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change Delta Ozone/Delta T due to different contributions from various ozone loss processes, each with its own temperature dependence. Ozone decrease in the tropical lower stratosphere caused by a projected speedup in the Brewer-Dobson circulation may or may not be balanced by ozone increases in the middle- and high-latitude lower stratosphere and upper troposphere. This balance, or lack thereof, contributes most to the spread in late 21st century projections.

  9. Understanding Differences in Chemistry Climate Model Projections of Stratospheric Ozone

    NASA Technical Reports Server (NTRS)

    Douglass, A. R.; Strahan, S. E.; Oman, L. D.; Stolarski, R. S.

    2014-01-01

    Chemistry climate models (CCMs) are used to project future evolution of stratospheric ozone as concentrations of ozone-depleting substances (ODSs) decrease and greenhouse gases increase, cooling the stratosphere. CCM projections exhibit not only many common features but also a broad range of values for quantities such as year of ozone return to 1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to ODS concentration change from that due to climate change. We show that the sensitivity of lower stratospheric ozone to chlorine change Delta Ozone/Delta inorganic chlorine is a near-linear function of partitioning of total inorganic chlorine into its reservoirs; both inorganic chlorine and its partitioning are largely controlled by lower stratospheric transport. CCMs with best performance on transport diagnostics agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035, differences in Delta Ozone/Delta inorganic chlorine contribute little to the spread in CCM projections as the anthropogenic contribution to inorganic chlorine becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change Delta Ozone/Delta T due to different contributions from various ozone loss processes, each with its own temperature dependence. Ozone decrease in the tropical lower stratosphere caused by a projected speedup in the Brewer-Dobson circulation may or may not be balanced by ozone increases in the middle- and high-latitude lower stratosphere and upper troposphere. This balance, or lack thereof, contributes most to the spread in late 21st century projections.

  10. Variations in school playground and classroom atmospheric particulate chemistry

    NASA Astrophysics Data System (ADS)

    Moreno, Teresa; Rivas, Ioar; Bouso, Laura; Viana, Mar; Jones, Tim; Àlvarez-Pedrerol, Mar; Alastuey, Andrés; Sunyer, Jordi; Querol, Xavier

    2014-07-01

    The chemical analysis of 553 school playground and classroom PM2.5 filters collected during the BREATHE sampling campaign in Barcelona, Spain, reveals a remarkable degree of spatial and temporal variability in ambient PM composition. Classroom air quality shows average PM2.5 concentrations of 37 μg m-3 (28% higher than outdoors), with much of this mass comprising carbon (including abundant cotton fibres), blackboard chalk particles and silicates. Where sandy playgrounds are present these exert a major influence on inhalable PM2.5 concentrations both indoors and outdoors. Throughout the city there is widespread contamination by metalliferous traffic particles, especially at schools located close to major urban highways where outdoor EC levels can be an order of magnitude higher than in peripheral, green belt schools. Penetration into the classroom of outdoor EC, ammonium sulphate and anthropogenic metals such as Cu, Sn, Sb, Zn and V is pervasive, especially during warmer months. In contrast, levels of nitrate and ammonium are much higher outdoors than in the classroom, especially during winter. During their work and play, schoolchildren across the city respire in a diversity of chemically differing atmospheric microenvironments.

  11. Physical Chemistry of the Freezing Process of Atmospheric Aqueous Drops.

    PubMed

    Bogdan, Anatoli; Molina, Mario J

    2017-04-27

    In supercooled aqueous solutions, ice nucleation is the initial stage of the freezing process. In this paper, we present experimental results that indicate that during the freezing of aqueous solutions, freeze-induced phase separation (FIPS) into pure ice and a freeze-concentrated solution (FCS) takes place. Our observations involve the use of an optical cryo-microscope (OC-M) to record images and movies. The results visually indicate for the first time that there are two freezing processes for (NH4)3H(SO4)2/H2O solutions: (i) contact freezing, as is the case for pure water drops, and (ii) the Wegener-Bergeron-Findeisen process, which is the growth of frozen drops (ice) at the expense of liquid ones. We also present OC-M images of frozen micrometer-scaled H2SO4/H2O drops that support our previous finding that freezing of these solutions generates mixed-phase particles, namely an ice core coated with a FCS. These results are relevant for atmospheric as well as for pharmaceutical sciences.

  12. Carbon dioxide in the atmosphere. [and other research projects

    NASA Technical Reports Server (NTRS)

    Johnson, F. S.

    1974-01-01

    Research projects for the period ending September 15, 1973 are reported as follows: (1) the abundances of carbon dioxide in the atmosphere, and the processes by which it is released from carbonate deposits in the earth and then transferred to organic material by photosynthesis; the pathways for movement of carbon and oxygen through the atmosphere; (2) space science computation assistance by PDP computer; the performance characteristics and user instances; (3) OGO-6 data analysis studies of the variations of nighttime ion temperature in the upper atmosphere.

  13. Coupling non-linear optical spectroscopy and surface chemistry: Towards new insights in atmospheric chemistry and aerosols

    NASA Astrophysics Data System (ADS)

    Abdelmonem, Ahmed; Lützenkirchen, Johannes

    2017-04-01

    For decades, the observation of atmospheric processes in general and ice nucleation in particular bridged the scales from macroscopic to microscopic levels. They delivered a wide variety of results in cloud microphysics, particularly concerning the ice nucleation ability of atmospheric aerosol particles [1]. The surface properties of an ice-nucleating particle (INP) play a major role in its ice nucleation ability. This role is not well explored in terms of water/INP-surface molecular-level interactions. For example, we found recently that surface-charge induced templating hampers ice nucleation [2]. Aging of an INP in a cloud may change its surface properties and hence its ice nucleation efficiency. To improve our understanding of heterogeneous ice nucleation, we combine chemical and optical surface techniques to probe the change in surface properties of an INP and the corresponding water structuring on it, respectively. The presentation will show the different scenarios after aging of an INP in a cloud and the impact on its ice nucleation ability. References 1. Hoose, C. and O. Mohler, Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments. Atmospheric Chemistry and Physics, 2012. 12(20): p. 9817-9854. 2. Abdelmonem, A., et al., Surface charge-induced orientation of interfacial water suppresses heterogeneous ice nucleation on α-alumina (0001). Angewandte Chemie (Submitted), 2017.

  14. Development of an aerosol-chemistry transport model coupled to non-hydrostatic icosahedral atmospheric model (NICAM) through applying a stretched grid system to regional simulations around Japan

    NASA Astrophysics Data System (ADS)

    Goto, D.; Nakajima, T.; Masaki, S.

    2014-12-01

    Air pollution has a great impact on both climate change and human health. One effective way to tackle with these issues is a use of atmospheric aerosol-chemistry models with high-resolution in a global scale. For this purpose, we have developed an aerosol-chemistry model based on a global cloud-resolving model (GCRM), Nonhydrostatic Icosahedral Atmospheric Model (NICAM; Tomita and Satoh, Fluid. Dyn. Res. 2004; Satoh et al., J. Comput. Phys. 2008, PEPS, 2014) under MEXT/RECCA/SALSA project. In the present study, we have simulated aerosols and tropospheric ozone over Japan by our aerosol-chemistry model "NICAM-Chem" with a stretched-grid system of approximately 10 km resolution, for saving the computer resources. The aerosol and chemistry modules are based on Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS; Takemura et al., J. Geophys. Res., 2005) and Chemical AGCM for Study of Atmospheric Environment and Radiative Forcing (CHASER; Sudo et al., J. Geophys. Res., 2002). We found that our model can generally reproduce both aerosols and ozone, in terms of temporal variations (daily variations of aerosols and diurnal variations of ozone). Under MEXT/RECCA/SALSA project, we also have used these results obtained by NICAM-Chem for the assessment of their impact on human health.

  15. The ENVISAT Atmospheric Chemistry mission (GOMOS, MIPAS and SCIAMACHY) -Processing status and data availability

    NASA Astrophysics Data System (ADS)

    Dehn, Angelika; Brizzi, G.; Barrot, G.; Bovensmann, H.; Canela, M.; Fehr, T.; Laur, H.; Lichtenberg, G.; Niro, F.; Perron, G.; Raspollini, P.; Saavedra de Miguel, L.; Scarpino, G.; Vogel, P.

    The atmospheric chemistry instruments on board the ENVISAT platform (GOMOS, MIPAS and SCIAMACHY) provide a unique dataset of geophysical parameters (e.g.: trace gases, clouds, and aerosol) that allows a comprehensive characterization of the atmosphere's chemical and climatological processes [1]. These instruments started to provide significant science data shortly after the launch of the ENVISAT satellite (March 2002). At the time of writing this paper, these instruments and the whole payload modules are fully working and are well beyond the expected lifetime of 5 years. In addition the orbit control strategy of the platform will be modified starting from 2010, in order to extend the mission lifetime up to 2013 [2]. This means that if no instrument problems will appear, the ENVISAT atmospheric sensors will provide at the end of their life, three separated, but complementary datasets of the most important atmospheric state parameters, spanning a time interval of about 11 years. This represents an extraordinary source of information for the scientific user community, both for the completeness and quality of the data and for the extent of the dataset. The aim of this paper is to present the actual status of the ESA operational atmospheric chemistry dataset provided by the three ENVISAT atmospheric chemistry instruments and the future evolution. The processing and reprocessing status will be described in details for each instrument. The outcomes of the geophysical validation and the planned validation activities will be discussed. Finally the data availability and the source of information will be specified. [1] H. Nett, J. Frerick, T. Paulsen, and G. Levrini, "The atmospheric instruments and their applications: GOMOS, MIPAS and SCIAMACHY", ESA Bulletin (ISSN 0376-4265), No. 106, p. 77 -87 (2001) [2] J. Frerick, B. Duesmann, and M. Canela, "2010 and beyond -The ENVISAT mission extension", Proc. `Envisat Symposium 2007', Montreux, Switzerland, 23-27 April 2007 (ESA SP

  16. Non-OH chemistry in oxidation flow reactors for the study of atmospheric chemistry systematically examined by modeling

    NASA Astrophysics Data System (ADS)

    Peng, Z.; Day, D. A.; Ortega, A. M.; Palm, B. B.; Hu, W. W.; Stark, H.; Li, R.; Tsigaridis, K.; Brune, W. H.; Jimenez, J. L.

    2015-09-01

    Oxidation flow reactors (OFRs) using low-pressure Hg lamp emission at 185 and 254 nm produce OH radicals efficiently and are widely used in atmospheric chemistry and other fields. However, knowledge of detailed OFR chemistry is limited, allowing speculation in the literature about whether some non-OH reactants, including several not relevant for tropospheric chemistry, may play an important role in these OFRs. These non-OH reactants are UV radiation, O(1D), O(3P), and O3. In this study, we investigate the relative importance of other reactants to OH for the fate of reactant species in OFR under a wide range of conditions via box modeling. The relative importance of non-OH species is less sensitive to UV light intensity than to relative humidity (RH) and external OH reactivity (OHRext), as both non-OH reactants and OH scale roughly proportional to UV intensity. We show that for field studies in forested regions and also the urban area of Los Angeles, reactants of atmospheric interest are predominantly consumed by OH. We find that O(1D), O(3P), and O3 have relative contributions to VOC consumption that are similar or lower than in the troposphere. The impact of O atoms can be neglected under most conditions in both OFR and troposphere. Under "pathological OFR conditions" of low RH and/or high OHRext, the importance of non-OH reactants is enhanced because OH is suppressed. Some biogenics can have substantial destructions by O3, and photolysis at non-tropospheric wavelengths (185 and 254 nm) may also play a significant role in the degradation of some aromatics under pathological conditions. Working under low O2 with the OFR185 mode allows OH to completely dominate over O3 reactions even for the biogenic species most reactive with O3. Non-tropospheric VOC photolysis may have been a problem in some laboratory and source studies, but can be avoided or lessened in future studies by diluting source emissions and working at lower precursor concentrations in lab studies, and

  17. Non-OH Chemistry in Oxidation Flow Reactors for the Study of Atmospheric Chemistry Systematically Examined by Modeling

    NASA Technical Reports Server (NTRS)

    Peng, Zhe; Day, Douglas A.; Ortega, Amber M.; Palm, Brett B.; Hu, Weiwei; Stark, Harald; Li, Rui; Tsigaridis, Kostas; Brune, William H.; Jimenez, Jose L.

    2016-01-01

    Oxidation flow reactors (OFRs) using low-pressure Hg lamp emission at 185 and 254 nm produce OH radicals efficiently and are widely used in atmospheric chemistry and other fields. However, knowledge of detailed OFR chemistry is limited, allowing speculation in the literature about whether some non-OH reactants, including several not relevant for tropospheric chemistry, may play an important role in these OFRs. These non-OH reactants are UV radiation, O(1D), O(3P), and O3. In this study, we investigate the relative importance of other reactants to OH for the fate of reactant species in OFR under a wide range of conditions via box modeling. The relative importance of non-OH species is less sensitive to UV light intensity than to relative humidity (RH) and external OH reactivity (OHRext), as both non-OH reactants and OH scale roughly proportional to UV intensity. We show that for field studies in forested regions and also the urban area of Los Angeles, reactants of atmospheric interest are predominantly consumed by OH. We find that O(1D), O(3P), and O3 have relative contributions to VOC consumption that are similar or lower than in the troposphere. The impact of O atoms can be neglected under most conditions in both OFR and troposphere. Under pathological OFR conditions of low RH and/or high OHRext, the importance of non-OH reactants is enhanced because OH is suppressed. Some biogenics can have substantial destructions by O3, and photolysis at non-tropospheric wavelengths (185 and 254 nm) may also play a significant role in the degradation of some aromatics under pathological conditions. Working under low O2 with the OFR185 mode allows OH to completely dominate over O3 reactions even for the biogenic species most reactive with O3. Non-tropospheric VOC photolysis may have been a problem in some laboratory and source studies, but can be avoided or lessened in future studies by diluting source emissions and working at lower precursor concentrations in lab studies, and by

  18. Composition, Chemistry, and Climate of the Atmosphere. 2: Mean properties of the atmosphere

    NASA Technical Reports Server (NTRS)

    Singh, Hanwant B. (Editor); Salstein, David A.

    1994-01-01

    The atmosphere can be defined as the relatively thin gaseous envelope surrounding the entire planet Earth. It possesses a number of properties related to its physical state and chemical composition, and it undergoes a variety of internal processes and external interactions that can either maintain or alter these properties. Whereas descriptions of the atmosphere's chemical properties form much of the remaining chapters of this book, the present chapter will highlight the atmosphere's gases, and these define its temperature structure. In contrast, the larger-scale motions comprise the winds, the global organization of which is often referred to as the general circulation. The framework of the dynamical and thermodynamical laws, including the three principles of conversation of mass, momentum, and energy, are fundamental in describing both the internal processes of the atmosphere and its external interactions. The atmosphere is not a closed system, because it exchanges all three of these internally conservative quantities across the atmosphere's boundary below and receives input from regions outside it. Thus surface fluxes of moisture, momentum, and heat occur to and from the underlying ocean and land. The atmosphere exchanges very little mass and momentum with space, though it absorbs directly a portion of the solar radiational energy received from above.

  19. Atmospheric chemistry measurements from the 1992 ASTEX/MAGE Cruise, May 30, 1992 through July 21, 1992, Cruise Number 91-126. Data report

    SciTech Connect

    Carsey, T.P.; Farmer, M.L.; Fischer, C.J.; Mendez, A.; Pszenny, A.A.

    1994-10-01

    The report describes the results of the 1992 ASTEX/MAGE cruise aboard the NOAA R/V MALCOLM BALDRIGE. The cruise was designed to support research sponsored by the NOAA Climate and Global Change Program under: (1) the Marine Sulfur and Climate (MS&C) component of the Atmosphere and Land-Surface Processes Core Project, and (2) the Radiatively Important Trace Species (RITS) component of the Atmospheric Chemistry Core Project. Chemical and meteorological measurements obtained on the cruise include reduced sulfur gases, ozone, carbon monoxide, nitrogen oxides and peroxyacetyl nitrate, rawinsondes, aerosol chemistry, microwave radiometry, vertical wind profiles, heat and water momentum flux, non-methane hydrocarbons, trace metals, aerosol size distributions, aerosol physical properties, and surface water chlorophyll. The report contains a brief description of the experimental apparatus and procedures employed, plus graphic and tabular presentations of the data sets, for most of the data from AOML/OCD investigators.

  20. Atmospheric Chemistry: Laboratory Studies of Kinetics of Important Reactions.

    NASA Astrophysics Data System (ADS)

    Smith, S. J.

    Available from UMI in association with The British Library. Requires signed TDF. This thesis describes the experiments to measure the rate constants for some reactions of the atmospherically important nitrate radical (NO_3) using the discharge-flow technique. The nitrate radical was monitored by optical absorption at lambda = 662 nm. The reactions of NO_3 with some stable organic and inorganic substrates are reported. The temperature dependences of some of the rate constants have also been determined (298 < T < 523 K). In most cases, computer simulation was used to extract the rate constant for the primary process because the time-dependent behaviour of (NO_3) was affected by secondary reactions of NO_3 with products of the primary interaction. The Arrhenius parameter in parentheses (E _{rm a}/kJ mol^ {-1}, A/cm^3 molecule ^{-1}s^ {-1} respectively) for the following reactions have been determined: ethane (37, 6.7 times 10^{-12}), ethylene (25.8, 6.3 times 10^ {-12}), CH_3OH (21.3, 1.2 times 10^ {-12}), CHCiota_3 (23.4, 8.6 times 10 ^{-13}) and HCl (27.7, 4 times 10^{-12}). The activation energies for the reactions studied between NO_3 and some alkynes are represented well by the value 25 +/- 3 kJ mol^{-1} and the corresponding pre-exponential factors (expressed as ln(10 ^{13}A/cm^3 molecule^{-1}s ^{-1}) are as follows: C_2H_2 (1.6 +/- 1.4), C_3H _4 (5.0 +/- 1.4), 1-C_4H_6 (5.8 +/- 1.0), 1-C_5 H_8 (5.7 +/- 0.6) and 1-C_6H _{10} (4.5 +/- 0.4). Some reactions were studied at room temperature _3(298 +/- 2 K) only and the rate constants found (in units of cm ^3 molecule^{ -1}s^{-1}) are: buta-1,3-diene (1.8 times 10 ^{-13}), isobutene (2.8 times 10^{-13 }), HBr (1.3 times 10 ^{-15}) and hex-2-yne (3.0 times 10^{-14 }). Non-Arrhenius behaviour was found in the reactions of NO_3 with n-butane, isobutane and propene. The empirical variation of these rate constants with temperature is well represented by the three parameter expressions:. k(T) = 1.2 times 10 ^{-46}T^{11

  1. Impact of future land use and land cover changes on atmospheric chemistry-climate interactions

    NASA Astrophysics Data System (ADS)

    Ganzeveld, Laurens; Bouwman, Lex; Stehfest, Elke; van Vuuren, Detlef P.; Eickhout, Bas; Lelieveld, Jos

    2010-12-01

    To demonstrate potential future consequences of land cover and land use changes beyond those for physical climate and the carbon cycle, we present an analysis of large-scale impacts of land cover and land use changes on atmospheric chemistry using the chemistry-climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry) constrained with present-day and 2050 land cover, land use, and anthropogenic emissions scenarios. Future land use and land cover changes are expected to result in an increase in global annual soil NO emissions by ˜1.2 TgN yr-1 (9%), whereas isoprene emissions decrease by ˜50 TgC yr-1 (-12%). The analysis shows increases in simulated boundary layer ozone mixing ratios up to ˜9 ppbv and more than a doubling in hydroxyl radical concentrations over deforested areas in Africa. Small changes in global atmosphere-biosphere fluxes of NOx and ozone point to compensating effects. Decreases in soil NO emissions in deforested regions are counteracted by a larger canopy release of NOx caused by reduced foliage uptake. Despite this decrease in foliage uptake, the ozone deposition flux does not decrease since surface layer mixing ratios increase because of a reduced oxidation of isoprene by ozone. Our study indicates that the simulated impact of land cover and land use changes on atmospheric chemistry depends on a consistent representation of emissions, deposition, and canopy interactions and their dependence on meteorological, hydrological, and biological drivers to account for these compensating effects. It results in negligible changes in the atmospheric oxidizing capacity and, consequently, in the lifetime of methane. Conversely, we expect a pronounced increase in oxidizing capacity as a consequence of anthropogenic emission increases.

  2. Interconnection of reactive oxygen species chemistry across the interfaces of atmospheric, environmental, and biological processes.

    PubMed

    Anglada, Josep M; Martins-Costa, Marilia; Francisco, Joseph S; Ruiz-López, Manuel F

    2015-03-17

    Oxidation reactions are ubiquitous and play key roles in the chemistry of the atmosphere, in water treatment processes, and in aerobic organisms. Ozone (O3), hydrogen peroxide (H2O2), hydrogen polyoxides (H2Ox, x > 2), associated hydroxyl and hydroperoxyl radicals (HOx = OH and HO2), and superoxide and ozonide anions (O2(-) and O3(-), respectively) are the primary oxidants in these systems. They are commonly classified as reactive oxygen species (ROS). Atmospheric chemistry is driven by a complex system of chain reactions of species, including nitrogen oxides, hydroxyl and hydroperoxide radicals, alkoxy and peroxy radicals, and ozone. HOx radicals contribute to keeping air clean, but in polluted areas, the ozone concentration increases and creates a negative impact on plants and animals. Indeed, ozone concentration is used to assess air quality worldwide. Clouds have a direct effect on the chemical composition of the atmosphere. On one hand, cloud droplets absorb many trace atmospheric gases, which can be scavenged by rain and fog. On the other hand, ionic species can form in this medium, which makes the chemistry of the atmosphere richer and more complex. Furthermore, recent studies have suggested that air-cloud interfaces might have a significant impact on the overall chemistry of the troposphere. Despite the large differences in molecular composition, concentration, and thermodynamic conditions among atmospheric, environmental, and biological systems, the underlying chemistry involving ROS has many similarities. In this Account, we examine ROS and discuss the chemical characteristics common to all of these systems. In water treatment, ROS are key components of an important subset of advanced oxidation processes. Ozonation, peroxone chemistry, and Fenton reactions play important roles in generating sufficient amounts of hydroxyl radicals to purify wastewater. Biochemical processes within living organisms also involve ROS. These species can come from pollutants in

  3. The "Chemistry Is in the News" Project: Can a Workshop Induce a Pedagogical Change?

    ERIC Educational Resources Information Center

    Barak, Miri; Carson, Kathleen M.; Zoller, Uri

    2007-01-01

    Chemistry Is in the News (CIITN) is an innovative project aimed at enhancing higher-order cognitive skills (HOCS) via connecting university-level chemistry to everyday life and real-world issues. The CIITN project and its related Web tools were presented in a workshop to illustrate their conceptual framework, educational potential, and…

  4. A New Project-Based Lab for Undergraduate Environmental and Analytical Chemistry

    ERIC Educational Resources Information Center

    Adami, Gianpiero

    2006-01-01

    A new project-based lab was developed for third year undergraduate chemistry students based on real world applications. The experience suggests that the total analytical procedure (TAP) project offers a stimulating alternative for delivering science skills and developing a greater interest for analytical chemistry and environmental sciences and…

  5. Computer Series, 101: Accurate Equations of State in Computational Chemistry Projects.

    ERIC Educational Resources Information Center

    Albee, David; Jones, Edward

    1989-01-01

    Discusses the use of computers in chemistry courses at the United States Military Academy. Provides two examples of computer projects: (1) equations of state, and (2) solving for molar volume. Presents BASIC and PASCAL listings for the second project. Lists 10 applications for physical chemistry. (MVL)

  6. The Effect of Web-Based Project Applications on Students' Attitudes towards Chemistry

    ERIC Educational Resources Information Center

    Morgil, Inci; Gungor Seyhan, Hatice; Ural Alsan, Evrim; Temel, Senar

    2008-01-01

    Students perform intensive web-based applications during their education. One of these is project-based application. In this study, the effect of web based project applications on students' attitudes towards chemistry has been investigated. 42 students attending Hacettepe University, Faculty of Education, and Department of Chemistry Education have…

  7. Atmospheric chemistry of carboxylic acids: microbial implication versus photochemistry

    NASA Astrophysics Data System (ADS)

    Vaïtilingom, M.; Charbouillot, T.; Deguillaume, L.; Maisonobe, R.; Parazols, M.; Amato, P.; Sancelme, M.; Delort, A.-M.

    2011-02-01

    Clouds are multiphasic atmospheric systems in which the dissolved organic compounds, dominated by carboxylic acids, are subject to multiple chemical transformations in the aqueous phase. Among them, solar radiation, by generating hydroxyl radicals (•OH), is considered as the main catalyzer of the reactivity of organic species in clouds. We investigated to which extent the active biomass existing in cloud water represents an alternative route to the chemical reactivity of carboxylic acids. Pure cultures of seventeen bacterial strains (Arthrobacter, Bacillus, Clavibacter, Frigoribacterium, Pseudomonas, Sphingomonas and Rhodococcus), previously isolated from cloud water and representative of the viable community of clouds were first individually incubated in two artificial bulk cloud water solutions at 17 °C and 5 °C. These solutions mimicked the chemical composition of cloud water from "marine" and "continental" air masses, and contained the major carboxylic acids existing in the cloud water (i.e. acetate, formate, succinate and oxalate). The concentrations of these carboxylic compounds were monitored over time and biodegradation rates were determined. In average, they ranged from 2 ×10-19 for succinate to 1 × 10-18 mol cell-1 s-1 for formate at 17 °C and from 4 × 10-20 for succinate to 6 × 10-19 mol cell-1 s-1 for formate at 5 °C, with no significant difference between "marine" and "continental" media. In parallel, irradiation experiments were also conducted in these two artificial media to compare biodegradation and photodegradation of carboxylic compounds. To complete this comparison, the photodegradation rates of carboxylic acids by •OH radicals were calculated from literature data. Inferred estimations suggested a significant participation of microbes to the transformation of carboxylic acids in cloud water, particularly for acetate and succinate (up to 90%). Furthermore, a natural cloud water sample was incubated (including its indigenous microflora

  8. Ammonia in the atmosphere: a review on emission sources, atmospheric chemistry and deposition on terrestrial bodies.

    PubMed

    Behera, Sailesh N; Sharma, Mukesh; Aneja, Viney P; Balasubramanian, Rajasekhar

    2013-11-01

    Gaseous ammonia (NH3) is the most abundant alkaline gas in the atmosphere. In addition, it is a major component of total reactive nitrogen. The largest source of NH3 emissions is agriculture, including animal husbandry and NH3-based fertilizer applications. Other sources of NH3 include industrial processes, vehicular emissions and volatilization from soils and oceans. Recent studies have indicated that NH3 emissions have been increasing over the last few decades on a global scale. This is a concern because NH3 plays a significant role in the formation of atmospheric particulate matter, visibility degradation and atmospheric deposition of nitrogen to sensitive ecosystems. Thus, the increase in NH3 emissions negatively influences environmental and public health as well as climate change. For these reasons, it is important to have a clear understanding of the sources, deposition and atmospheric behaviour of NH3. Over the last two decades, a number of research papers have addressed pertinent issues related to NH3 emissions into the atmosphere at global, regional and local scales. This review article integrates the knowledge available on atmospheric NH3 from the literature in a systematic manner, describes the environmental implications of unabated NH3 emissions and provides a scientific basis for developing effective control strategies for NH3.

  9. Management of the Atmosphere Resource Recovery and Environmental Monitoring Project

    NASA Technical Reports Server (NTRS)

    Roman, Monsi; Perry, Jay; Howard, David

    2013-01-01

    The Advanced Exploration Systems Program's Atmosphere Resource Recovery and Environmental Monitoring (ARREM) project is working to further optimize atmosphere revitalization and environmental monitoring system architectures. This paper discusses project management strategies that tap into skill sets across multiple engineering disciplines, projects, field centers, and industry to achieve the project success. It is the project's objective to contribute to system advances that will enable sustained exploration missions beyond Lower Earth Orbit (LEO) and improve affordability by focusing on the primary goals of achieving high reliability, improving efficiency, and reducing dependence on ground-based logistics resupply. Technology demonstrations are achieved by infusing new technologies and concepts with existing developmental hardware and operating in a controlled environment simulating various crewed habitat scenarios. The ARREM project's strengths include access to a vast array of existing developmental hardware that perform all the vital atmosphere revitalization functions, exceptional test facilities to fully evaluate system performance, and a well-coordinated partnering effort among the NASA field centers and industry partners to provide the innovative expertise necessary to succeed.

  10. Atmospheric chemistry on Venus, Earth, and Mars: Main features and comparison

    NASA Astrophysics Data System (ADS)

    Krasnopolsky, Vladimir A.

    2011-08-01

    This paper deals with two common problems and then considers major aspects of chemistry in the atmospheres of Mars and Venus. (1) The atmospheres of the terrestrial planets have similar origins but different evolutionary pathways because of the different masses and distances to the Sun. Venus lost its water by hydrodynamic escape, Earth lost CO 2 that formed carbonates and is strongly affected by life, Mars lost water in the reaction with iron and then most of the atmosphere by the intense meteorite impacts. (2) In spite of the higher solar radiation on Venus, its thermospheric temperatures are similar to those on Mars because of the greater gravity acceleration and the higher production of O by photolysis of CO 2. O stimulates cooling by the emission at 15 μm in the collisions with CO 2. (3) There is a great progress in the observations of photochemical tracers and minor constituents on Mars in the current decade. This progress is supported by progress in photochemical modeling, especially by photochemical GCMs. Main results in these areas are briefly discussed. The problem of methane presents the controversial aspects of its variations and origin. The reported variations of methane cannot be explained by the existing data on gas-phase and heterogeneous chemistry. The lack of current volcanism, SO 2, and warm spots on Mars favor the biological origin of methane. (4) Venus' chemistry is rich and covers a wide range of temperatures and pressures and many species. Photochemical models for the middle atmosphere (58-112 km), for the nighttime atmosphere and night airglow at 80-130 km, and the kinetic model for the lower atmosphere are briefly discussed.

  11. Investigating Titan's Atmospheric Chemistry at Low Temperature with the Titan Haze Simulation Experiment

    NASA Astrophysics Data System (ADS)

    Sciamma-O'Brien, E. M.; Salama, F.

    2012-12-01

    Titan, Saturn's largest satellite, possesses a dense atmosphere (1.5 bar at the surface) composed mainly of N2 and CH4. The solar radiation and electron bombardment from Saturn's magnetosphere induces a complex organic chemistry between these two constituents leading to the production of more complex molecules and subsequently to solid aerosols. These aerosols in suspension in the atmosphere form the haze layers giving Titan its characteristic orange color. Since 2004, the instruments onboard the Cassini orbiter have produced large amounts of observational data, unraveling a chemistry much more complex than what was first expected, particularly in Titan's upper atmosphere. Neutral, positively and negatively charged heavy molecules have been detected in the ionosphere of Titan, including benzene (C6H6) and toluene (C6H5CH3). The presence of these critical precursors of polycyclic aromatic hydrocarbon (PAH) compounds suggests that PAHs might play a role in the production of Titan's aerosols. The aim of the Titan Haze Simulation (THS) experiment, developed at the NASA Ames COSmIC facility, is to study the chemical pathways that link the simple molecules resulting from the first steps of the N2-CH4 chemistry to benzene, and to PAHs and nitrogen-containing PAHs (PANHs) as precursors to the production of solid aerosols. In the THS experiment, Titan's atmospheric chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas mixture is cooled to Titan-like temperature (~150K) before inducing the chemistry by plasma discharge. Due to the short residence time of the gas in the plasma discharge, the THS experiment can be used to probe the first and intermediate steps of Titan's chemistry by injecting different gas mixtures in the plasma. The products of the chemistry are detected and studied using two complementary techniques: Cavity Ring Down Spectroscopy and Time-Of-Flight Mass Spectrometry. Thin tholin deposits are also produced

  12. MIR station atmospheric chemistry investigations: numerical simulation of the future space experiments

    NASA Astrophysics Data System (ADS)

    Timofeyev, Yuriy M.

    1995-12-01

    Regular, long-term, g1obalscale measurements of atmospheric minor gaseous and aerosol composition (MGAC) by means ofdifferent instruments (PHOENIX, OZONE-MIR, ISTOK-1, DOPI) are planned on board the SPECTR and PRIRODA modules of the Space Station MIR during 1995-1998. The main characteristics of these devices are given. The principal goals of the space experiments are: investigations of the spatial and temporal MGAC variations, comparisons of different space-borne atmospheric chemistry sensors and their intercalibration, validation of the space MGAC measurements using different ground-based station and aircraft data, and studies of the molecular absorption in the atmosphere aimed to enhance an accuracy of radiative transfer atmospheric models. Special attention is . devoted to radiative transfer model (line-mixing, line-shift, line-narrowing, Non-LTE effects). The numerical estimations of the errors of the MGAC vertical profile retrievals using different device data are carried out.

  13. The impact of atmospheric aerosols on trace metal chemistry in open ocean surface seawater. 3. Lead

    NASA Astrophysics Data System (ADS)

    Maring, H. B.; Duce, R. A.

    1990-04-01

    Atmospheric aerosols collected at Enewetak Atoll in the tropical North Pacific were exposed to seawater in laboratory experiments to assess the impact of atmospheric aerosols on lead chemistry in surface seawater. The net atmospheric flux of soluble lead to the ocean is between 16 and 32 pmol cm-2 yr-1 at Enewetak. The stable lead isotopic composition of soluble aerosol lead indicates that it is of anthropogenic origin. Anthropogenic aerosol lead from Central and North America appears to be less soluble and/or to dissolve less rapidly than that from Asia. Dissolved organic matter and possibly lower pH appear to increase the nonaluminosilicate aerosol lead solubility and/or dissolution rate. The isotopic composition of lead in air, seawater and dry deposition suggests that after deposition in the ocean, nonaluminosilicate paniculate lead can be reinjected into the atmosphere during sea salt aerosol production.

  14. The THS Experiment: Simulating Titans Atmospheric Chemistry at Low Temperature (200K)

    NASA Technical Reports Server (NTRS)

    Sciamma-O'Brien, Ella; Upton, Kathleen; Beauchamp, Jack L.; Salama, Farid; Contreras, Cesar Sanchez; Bejaoui, Salma; Foing, Bernard; Pascale, Ehrenfreund

    2015-01-01

    In Titan's atmosphere, composed mainly of N2 (95-98%) and CH4 (2-5%), a complex chemistry occurs at low temperature, and leads to the production of heavy organic molecules and subsequently solid aerosols. Here, we used the Titan Haze Simulation (THS) experiment, an experimental setup developed at the NASA Ames COSmIC simulation facility to study Titan's atmospheric chemistry at low temperature. In the THS, the chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas is cooled to Titan-like temperature ( approximately 150K) before inducing the chemistry by plasma, and remains at low temperature in the plasma discharge (approximately 200K). Different N2-CH4-based gas mixtures can be injected in the plasma, with or without the addition of heavier precursors present as trace elements on Titan, in order to monitor the evolution of the chemical growth. Both the gas- and solid phase products resulting from the plasma-induced chemistry can be monitored and analyzed using a combination of complementary in situ and ex situ diagnostics. A recent mass spectrometry[1] study of the gas phase has demonstrated that the THS is a unique tool to probe the first and intermediate steps of Titan's atmospheric chemistry at Titan-like temperature. In particular, the mass spectra obtained in a N2-CH4-C2H2-C6H6 mixture are relevant for comparison to Cassini's CAPS-IBS instrument. The results of a complementary study of the solid phase are consistent with the chemical growth evolution observed in the gas phase. Grains and aggregates form in the gas phase and can be jet deposited on various substrates for ex situ analysis. Scanning Electron Microscopy images show that more complex mixtures produce larger aggregates. A mass spectrometry analysis of the solid phase has detected the presence of aminoacetonitrile, a precursor of glycine, in the THS aerosols. X-ray Absorption Near Edge Structure (XANES) measurements also show the presence of imine

  15. The THS: Simulating Titan’s atmospheric chemistry at low temperature

    NASA Astrophysics Data System (ADS)

    Sciamma-O'Brien, Ella; Upton, Kathleen T.; Beauchamp, Jack L.; Salama, Farid

    2015-08-01

    In Titan’s atmosphere, composed mainly of N2 (95-98%) and CH4 (2-5%), a complex chemistry occurs at low temperature, and leads to the production of heavy organic molecules and subsequently solid aerosols. Here, we used the Titan Haze Simulation (THS) experiment, an experimental setup developed at the NASA Ames COSmIC simulation facility to study Titan’s atmospheric chemistry at low temperature. In the THS, the chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas is cooled to Titan-like temperature (~150K) before inducing the chemistry by plasma, and remains at low temperature in the plasma discharge (~200K). Different N2-CH4-based gas mixtures can be injected in the plasma, with or without the addition of heavier precursors present as trace elements on Titan, in order to monitor the evolution of the chemical growth. Both the gas- and solid phase products resulting from the plasma-induced chemistry can be monitored and analyzed using a combination of complementary in situ and ex situ diagnostics.A recent mass spectrometry study of the gas phase has demonstrated that the THS is a unique tool to probe the first and intermediate steps of Titan’s atmospheric chemistry at Titan-like temperature. In particular, the mass spectra obtained in a N2-CH4-C2H2-C6H6 mixture are relevant for comparison to Cassini’s CAPS-IBS instrument. The results of a complementary study of the solid phase are consistent with the chemical growth evolution observed in the gas phase. Grains and aggregates form in the gas phase and can be jet deposited on various substrates for ex situ analysis. Scanning Electron Microscopy images show that more complex mixtures produce larger aggregates. A DART mass spectrometry analysis of the solid phase has detected the presence of aminoacetonitrile, a precursor of glycine, in the THS aerosols. X-ray Absorption Near Edge Structure (XANES) measurements also show the presence of imine and nitrile

  16. An Extended View of Ozone and Chemistry in the Atmosphere of Mars

    NASA Technical Reports Server (NTRS)

    Smith, Ramsey L.; Fast, Kelly E.; Kostiuk, T.; Lefevre, Frank; Hewagama, Tilak; Livengood, Timothy A.

    2011-01-01

    We present an ongoing effort to characterize chemistry in Mars' atmosphere in multiple seasons on timescales longer than spaceflight missions through coordinated efforts by GSFC's HIPWAC spectrometer and Mars Express SPICAM, archival measurements, and tests/application of photochemical models. The trace species ozone (03) is an effective probe of Mars' atmospheric chemistry because it is destroyed by odd-hydrogen species (HOx, from water vapor photolysis). Observed ozone is a critical test for specific predictions by 3-D photochemical models (spatial, diurnal, seasonal). Coordinated measurements by HIPWAC and SPICAM quantitatively linked mission data to the 23-year GSFC ozone data record and also revealed unanticipated inter-decadal variability of same-season ozone abundances, a possible indicator of changing cloud activity (heterogeneous sink for HOx). A detailed study of long-term conditions is critical to characterizing the predictability of Mars' seasonal chemical behavior, particularly in light of the implications of and the lack of explanation for reported methane behavior.

  17. Global tropospheric experiment at the Hong Kong Atmosphere Chemistry Measurement Station

    NASA Technical Reports Server (NTRS)

    Carroll, Mary Ann; Wang, Tao

    1995-01-01

    The major activities of the Global Tropospheric Experiment at the Hong Kong Atmospheric Chemistry Measurement Station are presented for the period 1 January - 31 December 1995. Activities included data analysis, reduction, and archiving of atmospheric measurements and sampling. Sampling included O3, CO, SO2, NO, TSP, RSP, and ozone column density. A data archive was created for the surface meteorological data. Exploratory data analysis was performed, including examination of time series, frequency distributions, diurnal variations and correlation. The major results have been or will be published in scientific journals as well as presented at conferences/workshops. Abstracts are attached.

  18. Quantifying the Perturbation of Atmospheric Chemistry from Medium-Size Asteroid Impacts in the Ocean

    NASA Astrophysics Data System (ADS)

    Pierazzo, E.; Garcia, R. R.; Kinnison, D. E.; Marsh, D. R.

    2009-12-01

    The continuous monitoring of space in the Earth’s neighborhood by the Spaceguard program has reassured us that there are currently no asteroids capable of causing mass extinctions threatening Earth. Although it is believed that about 80% of all Near-Earth Objects (NEOs) larger than 1 km in diameter have been discovered and catalogued, there is still a large number of undiscovered NEOs between 300m and 1km in diameter that are looming in our neighborhood. The consequences of a collision of a NEO in this size range with the Earth have never been explored in detail. If headed on a collision course with Earth, such NEOs will be more likely to hit the Earth’s oceans than continental areas. Using a 3D shock physics code SOVA, we estimated the amount of water vapor injected in the atmosphere by the impact of an asteroid 500m in diameter (with an average asteroidal impact velocity of 18km/s and impact angle of 45° from the surface) into a 4 km deep region of the ocean. While the ocean floor is hardly affected by the impact, large amounts of water are ejected in the atmosphere. We found that, overall, about 5×1012 kg of water was ejected in the middle atmosphere (above about 12 km). Liquid water is removed on a short timescale, but about 1×1012 kg of water vapor is entrained in the middle atmosphere where it can produce a sizeable perturbation to atmospheric chemistry. This is an important, yet largely unexplored, environmental effect of oceanic impacts. The localized distribution of water vapor from the impact simulation is introduced into the Whole Atmosphere Community Climate Model (WACCM) a 3D Chemistry-Climate Model whose vertical domain extends to about 140km. WACCM has a fully interactive Chemistry package that can track the chemical consequences of water vapor into the middle atmosphere. We will report on initial WACCM calculations of the perturbation to the atmospheric chemistry from the injected water vapor. Oceanic water contains significant amounts of

  19. Atmospheric Chemistry Effects of the 20 January 2005 Solar Proton Event

    NASA Astrophysics Data System (ADS)

    Klekociuk, A. R.; Bombardieri, D. J.; Duldig, M. L.; Michael, K. J.

    2009-03-01

    Atmospheric ionization during Solar Proton Events (SPE) has traditionally been modeled using top-of-atmosphere (TOA) particle fluxes measured by near-Earth spacecraft, and as a consequence the modeling has been restricted to particle energies below 500 MeV. However, as inferred from measurements by Earth-based muon telescopes and neutron monitors during Ground Level Enhancement (GLE) events, protons accompanying the most energetic SPEs can have significant short-term (<1 day duration) fluxes at energies up to at least 20GeV. Here, we examine atmospheric chemistry changes in the polar atmosphere during the large GLE of 20 January 2005. We use TOA particle spectra derived from satellite measurements augmented with proton spectra inferred from ground-based neutron monitor data to drive NOy and OH production in the SOCRATES two-dimensional atmospheric chemistry model. We show that the energetic particles of the January 20 event and associated particle enhancements during the preceding 5 days produced sufficient short timescale ionization in the lower stratosphere for measurable effects on HNO3 and O3 concentrations in the polar regions of both hemispheres. We also show that the detailed consideration of the most energetic particles that contributed to this GLE is of low importance for modeling ionization in the lower stratosphere, at least on a daily average timescale.

  20. Kinetic and photochemical data for atmospheric chemistry reactions of the nitrogen oxides

    NASA Technical Reports Server (NTRS)

    Hampson, R. F., Jr.

    1980-01-01

    Data sheets for thermal and photochemical reactions of importance in the atmospheric chemistry of the nitrogen oxides are presented. For each reaction the available experimental data are summarized and critically evaluated, and a preferred value of the rate coefficient is given. The selection of the preferred value is discussed and an estimate of its accuracy is given. For the photochemical process, the data are summarized, and preferred for the photoabsorption cross section and primary quantum yields are given.

  1. The Skylab concentrated atmospheric radiation project. [Arizona and New Mexico

    NASA Technical Reports Server (NTRS)

    Kuhn, P. M.; Whitehead, V. S.; Marlatt, W. E.

    1975-01-01

    The Skylab field phase in June, August and September of 1973 for the Skylab concentrated atmospheric radiation project provided an opportunity to conduct infrared and solar observations and subsequent calculations beneath the orbiting space vehicle during EREP overpasses. Infrared and solar transmission and absorption properties observed within the atmosphere were compared with EREP experiments, notably the S-191 and S-192. These same observations were later employed in the development and comparison of various atmospheric infrared and solar radiative transfer approximations. Solar radiation observations and calculations in the scattering atmosphere included the 0.4 to 1.1 microns spectral range while infrared observations and calculations covered the spectral band and portions thereof within the 5.0 to 40.0 microns region. Principal conclusions drawn from the solar radiation research and the infrared radiation research are discussed.

  2. Atmospheric chemistry of toxic contaminants. 1. Reaction rates and atmospheric persistence

    SciTech Connect

    Grosjean, D. )

    1990-10-01

    Using structure-reactivity relationships between reaction rate constants and ionization potentials for structural homologues, estimates are presented for the rate constants of the reactions of ozone, the hydroxyl radical, and the nitrate radical with forty toxic air contaminants for which no or little data are available. These rate constants are in turn used to estimate the atmospheric persistence of saturated aliphatics, unsaturated aliphatics, and aromatic toxic organics. The corresponding atmospheric half-lives for removal by chemical reactions range from a few hours for the most reactive toxics (chloroprene, hexachlorocyclo-pentadiene, cresols, nitrosamines, maleic anhydride) to several months for the least reactive compounds (nitrobenzene, methyl bromide, phosgene).

  3. Chemistry and Climate in Asia - An Earth System Modeling Project

    NASA Astrophysics Data System (ADS)

    Barth, M. C.; Emmons, L. K.; Massie, S. T.; Pfister, G.; Romero Lankao, P.; Lamarque, J.; Carmichael, G. R.

    2011-12-01

    Asia is one of the most highly populated and economically dynamic regions in the world, with much of the population located in growing mega-cities. It is a region with significant emissions of greenhouse gases, aerosols and other pollutants, which pose high health risks to urban populations. Emissions of these aerosols and gases increased drastically over the last decade due to economic growth and urbanization and are expected to rise further in the near future. As such, the continent plays a role in influencing climate change via its effluent of aerosols and gaseous pollutants. Asia is also susceptible to adverse climate change through interactions between aerosols and clouds, which potentially can have serious implications for freshwater resources. We are developing an integrated inter-disciplinary program to focus on Asia, its climate, air quality, and impact on humans that will include connections with hydrology, ecosystems, extreme weather events, and human health. The primary goal of this project is to create a team to identify key scientific questions and establish networks of specialists to create a plan for future studies to address these questions. A second goal is to establish research facilities and a framework for investigating chemistry and climate over Asia. These facilities include producing high resolution Earth System Model simulations that have been evaluated with meteorological and chemical measurements, producing high-resolution emission inventories, analyzing satellite data, and analyzing the vulnerability of humans to air quality and extreme natural events. In this presentation we will describe in more detail these activities and discuss a future workshop on the impact of chemistry in climate on air quality and human health.

  4. Addition of a Project-Based Component to a Conventional Expository Physical Chemistry Laboratory

    ERIC Educational Resources Information Center

    Tsaparlis, Georgios; Gorezi, Marianna

    2007-01-01

    Students should enjoy their laboratory classes and for this purpose a project-based activity is added to a conventional physical chemistry laboratory. Students were given project work instead of conventional experiment and then they had to make progress in the project according to instructions and then carry out experiments related to the project.

  5. Addition of a Project-Based Component to a Conventional Expository Physical Chemistry Laboratory

    ERIC Educational Resources Information Center

    Tsaparlis, Georgios; Gorezi, Marianna

    2007-01-01

    Students should enjoy their laboratory classes and for this purpose a project-based activity is added to a conventional physical chemistry laboratory. Students were given project work instead of conventional experiment and then they had to make progress in the project according to instructions and then carry out experiments related to the project.

  6. Variational data assimilation schemes for transport and transformation models of atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Penenko, Alexey; Penenko, Vladimir; Tsvetova, Elena; Antokhin, Pavel

    2016-04-01

    The work is devoted to data assimilation algorithm for atmospheric chemistry transport and transformation models. In the work a control function is introduced into the model source term (emission rate) to provide flexibility to adjust to data. This function is evaluated as the constrained minimum of the target functional combining a control function norm with a norm of the misfit between measured data and its model-simulated analog. Transport and transformation processes model is acting as a constraint. The constrained minimization problem is solved with Euler-Lagrange variational principle [1] which allows reducing it to a system of direct, adjoint and control function estimate relations. This provides a physically-plausible structure of the resulting analysis without model error covariance matrices that are sought within conventional approaches to data assimilation. High dimensionality of the atmospheric chemistry models and a real-time mode of operation demand for computational efficiency of the data assimilation algorithms. Computational issues with complicated models can be solved by using a splitting technique. Within this approach a complex model is split to a set of relatively independent simpler models equipped with a coupling procedure. In a fine-grained approach data assimilation is carried out quasi-independently on the separate splitting stages with shared measurement data [2]. In integrated schemes data assimilation is carried out with respect to the split model as a whole. We compare the two approaches both theoretically and numerically. Data assimilation on the transport stage is carried out with a direct algorithm without iterations. Different algorithms to assimilate data on nonlinear transformation stage are compared. In the work we compare data assimilation results for both artificial and real measurement data. With these data we study the impact of transformation processes and data assimilation to the performance of the modeling system [3]. The

  7. Studies in photochemical smog chemistry. 1. Atmospheric chemistry of toulene. 2. Analysis of chemical reaction mechanisms for photochemical smog

    SciTech Connect

    Leone, J.A.

    1985-01-01

    This study focuses on two related topics in the gas phase organic chemistry of importance in urban air pollution. An experimental effort aimed at developing a new explicit reaction mechanism for the atmospheric photooxidation of toluene is described. This mechanism is tested using experimental data from both indoor and outdoor smog chamber facilities. The predictions of the new reaction mechanism are found to be in good agreement with both sets of experimental data. Additional simulations performed with the new mechanism are used to investigate various mechanistic paths. A theoretical analysis of lumped chemical reaction mechanisms for photochemical smog is presented. Included is a description of a new counter species analysis technique which can be used to analyze any complex chemical reaction mechanism. When applied to mechanisms for photochemical smog, this analysis is shown capable of providing answers to previously inaccessible questions such as the relative contributions of individual organics to photochemical ozone formation.

  8. Novel and Improved Nanomaterials, Chemistries and Apparatus for Nanobiotechnology: the NACBO project.

    PubMed

    Bruce, Ian James

    2011-02-01

    This article outlines the nature and activities of the recently completed EU Framework Programme 6 Integrated Project, Novel and Improved Nanomaterials, Chemistries and Apparatus for Nanobiotechnology (NACBO). This project was designed to yield new nanomaterials, surface activation and synthetic nucleic acid chemistries, procedures and hardware for applications in forensics and diagnostics. It provides details on the project's structure and partnership along with its principal objectives and successes in terms of publications and commercial exploitation.

  9. Heterogeneous chemistry and reaction dynamics of the atmospheric oxidants, O3, NO3, and OH, on organic surfaces.

    PubMed

    Chapleski, Robert C; Zhang, Yafen; Troya, Diego; Morris, John R

    2016-07-07

    Heterogeneous chemistry of the most important atmospheric oxidants, O3, NO3, and OH, plays a central role in regulating atmospheric gas concentrations, processing aerosols, and aging materials. Recent experimental and computational studies have begun to reveal the detailed reaction mechanisms and kinetics for gas-phase O3, NO3, and OH when they impinge on organic surfaces. Through new research approaches that merge the fields of traditional surface science with atmospheric chemistry, researchers are developing an understanding for how surface structure and functionality affect interfacial chemistry with this class of highly oxidizing pollutants. Together with future research initiatives, these studies will provide a more complete description of atmospheric chemistry and help others more accurately predict the properties of aerosols, the environmental impact of interfacial oxidation, and the concentrations of tropospheric gases.

  10. Perchlorate formation on Mars through surface radiolysis-initiated atmospheric chemistry: A potential mechanism.

    PubMed

    Wilson, Eric H; Atreya, Sushil K; Kaiser, Ralf I; Mahaffy, Paul R

    2016-08-01

    Recent observations of the Martian surface by the Phoenix lander and the Sample Analysis at Mars indicate the presence of perchlorate (ClO4(-)). The abundance and isotopic composition of these perchlorates suggest that the mechanisms responsible for their formation in the Martian environment may be unique in our solar system. With this in mind, we propose a potential mechanism for the production of Martian perchlorate: the radiolysis of the Martian surface by galactic cosmic rays, followed by the sublimation of chlorine oxides into the atmosphere and their subsequent synthesis to form perchloric acid (HClO4) in the atmosphere, and the surface deposition and subsequent mineralization of HClO4 in the regolith to form surface perchlorates. To evaluate the viability of this mechanism, we employ a one-dimensional chemical model, examining chlorine chemistry in the context of Martian atmospheric chemistry. Considering the chlorine oxide, OClO, we find that an OClO flux as low as 3.2 × 10(7) molecules cm(-2) s(-1) sublimated into the atmosphere from the surface could produce sufficient HClO4 to explain the perchlorate concentration on Mars, assuming an accumulation depth of 30 cm and integrated over the Amazonian period. Radiolysis provides an efficient pathway for the oxidation of chlorine, bypassing the efficient Cl/HCl recycling mechanism that characterizes HClO4 formation mechanisms proposed for the Earth but not Mars.

  11. Patterns of Soil and Streamwater Chemistry Relative to Atmospheric Deposition in Acadia National Park, Maine, USA

    NASA Astrophysics Data System (ADS)

    Ewing, H. A.; Weathers, K. C.; Hollister, C. C.; Steele, B.

    2006-12-01

    Atmospheric deposition is the source of many nutrients and pollutants to ecosystems, yet estimates of total deposition to complex landscapes are rare, thus limiting our understanding of the linkages between atmospheric deposition and ecosystem processes. Using a new model of atmospheric deposition to Acadia National Park, we have quantified deposition across elevational gradients and on a watershed basis, and here relate deposition to soil and streamwater chemistry. Soil samples collected across two elevational gradients varied three-fold in modeled deposition and four-fold in percent base saturation. Despite large variations in base saturation across sites and between surface and subsurface soil horizons, the relationship between deposition and Ca:Al ratios was weak. In the surface soil organic horizon, some trace metal concentrations (e.g., Pb) were strongly correlated with modeled deposition, but concentrations of other metals such as Cu and Zn were either unrelated or negatively correlated with modeled deposition. In general, the more biologically mobile trace metals were less well correlated with modeled deposition than those elements with lesser biological activity. At the watershed scale, deposition varied by a factor of two. Sulfate in streamwater was strongly correlated with modeled sulfur deposition to the watershed, suggesting that sulfur export may be strongly influenced by atmospheric inputs. Streamwater pH and ANC were variable among watersheds, however their patterns were weakly predicted by both deposition and landscape variables, suggesting that chemical and biological processing in the watershed may be more important than deposition in controlling these aspects of streamwater chemistry.

  12. Perchlorate Formation on Mars Through Surface Radiolysis-Initiated Atmospheric Chemistry: A Potential Mechanism

    NASA Technical Reports Server (NTRS)

    Wilson, Eric H.; Atreya, Sushil K.; Kaiser, Ralf I.; Mahaffy, Paul R.

    2016-01-01

    Recent observations of the Martian surface by the Phoenix lander and the Sample Analysis at Mars indicate the presence of perchlorate (ClO4). The abundance and isotopic composition of these perchlorates suggest that the mechanisms responsible for their formation in the Martian environment may be unique in our solar system. With this in mind, we propose a potential mechanism for the production of Martian perchlorate: the radiolysis of the Martian surface by galactic cosmic rays, followed by the sublimation of chlorine oxides into the atmosphere and their subsequent synthesis to form perchloric acid (HClO4) in the atmosphere, and the surface deposition and subsequent mineralization of HClO4 in the regolith to form surface perchlorates. To evaluate the viability of this mechanism, we employ a one-dimensional chemical model, examining chlorine chemistry in the context of Martian atmospheric chemistry. Considering the chlorine oxide, OClO, we find that an OClO flux as low as 3.2 x 10(exp 7) molecules/sq cm/s sublimated into the atmosphere from the surface could produce sufficient HClO4 to explain the perchlorate concentration on Mars, assuming an accumulation depth of 30 cm and integrated over the Amazonian period. Radiolysis provides an efficient pathway for the oxidation of chlorine, bypassing the efficient Cl/HCl recycling mechanism that characterizes HClO4 formation mechanisms proposed for the Earth but not Mars.

  13. Perchlorate formation on Mars through surface radiolysis-initiated atmospheric chemistry: A potential mechanism

    NASA Astrophysics Data System (ADS)

    Wilson, Eric H.; Atreya, Sushil K.; Kaiser, Ralf I.; Mahaffy, Paul R.

    2016-08-01

    Recent observations of the Martian surface by the Phoenix lander and the Sample Analysis at Mars indicate the presence of perchlorate (ClO4-). The abundance and isotopic composition of these perchlorates suggest that the mechanisms responsible for their formation in the Martian environment may be unique in our solar system. With this in mind, we propose a potential mechanism for the production of Martian perchlorate: the radiolysis of the Martian surface by galactic cosmic rays, followed by the sublimation of chlorine oxides into the atmosphere and their subsequent synthesis to form perchloric acid (HClO4) in the atmosphere, and the surface deposition and subsequent mineralization of HClO4 in the regolith to form surface perchlorates. To evaluate the viability of this mechanism, we employ a one-dimensional chemical model, examining chlorine chemistry in the context of Martian atmospheric chemistry. Considering the chlorine oxide, OClO, we find that an OClO flux as low as 3.2 × 107 molecules cm-2 s-1 sublimated into the atmosphere from the surface could produce sufficient HClO4 to explain the perchlorate concentration on Mars, assuming an accumulation depth of 30 cm and integrated over the Amazonian period. Radiolysis provides an efficient pathway for the oxidation of chlorine, bypassing the efficient Cl/HCl recycling mechanism that characterizes HClO4 formation mechanisms proposed for the Earth but not Mars.

  14. A comprehensive NMR structural study of Titan aerosol analogs: Implications for Titan's atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    He, Chao; Smith, Mark A.

    2014-11-01

    Titan has a thick atmosphere composed primarily of nitrogen and methane. Complex organic chemistry induced by solar ultraviolet radiation and energetic particles, takes place in Titan's upper atmosphere, producing an optically thick reddish brown carbon based haze encircling this moon. The chemistry in Titan's atmosphere and its resulting chemical structures are still not fully understood in spite of a great many efforts being made. In our previous work, we have investigated the structure of the 13C and 15N labeled, simulated Titan haze aerosols (tholin) by NMR and identified several dominant small molecules in the tholin. Here we report our expanded structural investigation of the bulk of the tholin by more comprehensive NMR study. The NMR results show that the tholin materials are dominated by heavily nitrogenated compounds, in which the macromolecular structures are highly branched polymeric or oligomeric compounds terminated in methyl, amine, and nitrile groups. The structural characteristic suggest that the tholin materials are formed via different copolymerization or incorporation mechanisms of small precursors, such as HCN, CH2dbnd NH, NH3 and C2H2. This study helps to understand the formation process of nitrogenated organic aerosols in Titan's atmosphere and their prebiotic implications.

  15. Coupling between the atmosphere, the ionosphere and the magnetosphere : Project of microsatellite Taranis

    NASA Astrophysics Data System (ADS)

    Blanc, E.; Taranis Team

    2003-04-01

    Strong interactions between the middle and upper regions of the atmosphere and ionosphere are manifested by light emission in the middle and upper atmosphere, known as sprites and elves, gamma radiation of atmospheric origin, electromagnetic emissions recently observed above atmospheric storms. This direct coupling between active storm cells, the thermosphere and the ionosphere - and the considerable energies involved - gives rise to processes unsuspected until now regarding space plasmas as well as the chemistry and dynamics of the middle atmosphere. The electromagnetic and particle emissions could derive from the run away relativistic electrons initiated by the impact of cosmic rays on storm cells. These processes can have a significant effect on the Earth's magnetosphere, in particular by modifying the source terms and loss of the radiation belts. The microsatellite Taranis (Tool for the Analysis of RAdiations from lightNIngs and Sprites) proposes to study the coupling between atmosphere, ionosphere and magnetosphere during atmospheric storms. This has to be carried on a local and global scale in order to understand the physical mechanisms responsible for the impulsive transfers of energy between the neutral atmosphere and plasmas of the ionosphere and magnetosphere. The final goal is to establish the impact of these processes on the Earth's environment. The purpose of this presentation is to describe in a first part the project Taranis, his scientific objectives, the mission and the scientific payload. In a second part the first results of the experiment LSO (Lightning and Sprite Observations), on board of the International Space Station, will be presented. LSO is composed of two micro-cameras, fixed on a ISS window for observations at the horizon or at the nadir. One camera is equipped with a filter and measures the emissions from earth in a specific spectral window, the second works in the visible. The measurements allow the identification of sprites and

  16. Atmospheric chemistry

    Treesearch

    Andrzej Bytnerowicz; Mark Fenn; Edith B. Allen; Ricardo Cisneros

    2016-01-01

    At present, negative impacts of air pollution on California ecosystems are caused mainly by elevated levels of ozone and nitrogen deposition. Generally, ozone air pollution in California has been improving significantly since the 1970s; however, it still causes serious ecological and human health effects. The most serious ecological effects occur in mixed conifer...

  17. The NOx dependence of bromine chemistry in the Arctic atmospheric boundary layer

    NASA Astrophysics Data System (ADS)

    Custard, K. D.; Thompson, C. R.; Pratt, K. A.; Shepson, P. B.; Liao, J.; Huey, L. G.; Orlando, J. J.; Weinheimer, A. J.; Apel, E.; Hall, S. R.; Flocke, F.; Mauldin, L.; Hornbrook, R. S.; Pöhler, D.; General, S.; Zielcke, J.; Simpson, W. R.; Platt, U.; Fried, A.; Weibring, P.; Sive, B. C.; Ullmann, K.; Cantrell, C.; Knapp, D. J.; Montzka, D. D.

    2015-03-01

    Arctic boundary layer nitrogen oxides (NOx = NO2 + NO) are naturally produced in and released from the sunlit snowpack and range between 10 to 100 pptv in the remote background surface layer air. These nitrogen oxides have significant effects on the partitioning and cycling of reactive radicals such as halogens and HOx (OH + HO2). However, little is known about the impacts of local anthropogenic NOx emission sources on gas-phase halogen chemistry in the Arctic, and this is important because these emissions can induce large variability in ambient NOx and thus local chemistry. In this study, a zero-dimensional photochemical kinetics model was used to investigate the influence of NOx on the unique springtime halogen and HOx chemistry in the Arctic. Trace gas measurements obtained during the 2009 OASIS (Ocean-Atmosphere-Sea Ice-Snowpack) field campaign at Barrow, AK were used to constrain many model inputs. We find that elevated NOx significantly impedes gas-phase radical chemistry, through the production of a variety of reservoir species, including HNO3, HO2NO2, peroxyacetyl nitrate (PAN), BrNO2, ClNO2 and reductions in BrO and HOBr, with a concomitant, decreased net O3 loss rate. The effective removal of BrO by anthropogenic NOx was directly observed from measurements conducted near Prudhoe Bay, AK during the 2012 Bromine, Ozone, and Mercury Experiment (BROMEX). Thus, while changes in snow-covered sea ice attributable to climate change may alter the availability of molecular halogens for ozone and Hg depletion, predicting the impact of climate change on polar atmospheric chemistry is complex and must take into account the simultaneous impact of changes in the distribution and intensity of anthropogenic combustion sources. This is especially true for the Arctic, where NOx emissions are expected to increase because of increasing oil and gas extraction and shipping activities.

  18. Final Report for LDRD Project 05-ERD-050: "Developing a Reactive Chemistry Capability for the NARAC Operational Model (LODI)"

    SciTech Connect

    Cameron-Smith, P; Grant, K; Connell, P

    2008-02-11

    In support of the National Security efforts of LLNL, this project addressed the existing imbalance between dispersion and chemical capabilities of LODI (Lagrangian Operational Dispersion Integrator--the NARAC operational dispersion model). We have demonstrated potentially large effects of atmospheric chemistry on the impact of chemical releases (e.g., industrial chemicals and nerve agents). Prior to our work, LODI could only handle chains of first-order losses (exponential decays) that were independent of time and space, limiting NARAC's capability to respond when reactive chemistry is important. We significantly upgraded the chemistry and aerosol capability of LODI to handle (1) arbitrary networks of chemical reactions, (2) mixing and reactions with ambient species, (3) evaporation and condensation of aerosols, and (4) heat liberated from chemical reactions and aerosol condensation (which can cause a cold and dense plume hugging the ground to rise into the atmosphere, then descend to the ground again as droplets). When this is made operational, it will significantly improve NARAC's ability to respond to terrorist attacks and industrial accidents that involve reactive chemistry, including many chemical agents and toxic industrial chemicals (TICS). As a dual-use, the resulting model also has the potential to be a state-of-the-art air-quality model. Chemical releases are the most common type of airborne hazardous release and many operational applications involve such scenarios. The new capability we developed is therefore relevant to the needs of the Department of Energy (DOE), Department of Homeland Security (DHS) and Department of Defense (DoD).

  19. Effects of numerical tolerance levels on an atmospheric chemistry model for mercury

    SciTech Connect

    Ferris, D.C.; Burns, D.S.; Shuford, J.

    1996-12-31

    A Box Model was developed to investigate the atmospheric oxidation processes of mercury in the environment. Previous results indicated the most important influences on the atmospheric concentration of HgO(g) are (i) the flux of HgO(g) volatilization, which is related to the surface medium, extent of contamination, and temperature, and (ii) the presence of Cl{sub 2} in the atmosphere. The numerical solver which has been incorporated into the ORganic CHemistry Integrated Dispersion (ORCHID) model uses the Livermore Solver of Ordinary Differential Equations (LSODE). In the solution of the ODE`s, LSODE uses numerical tolerances. The tolerances effect computer run time, the relative accuracy of ODE calculated species concentrations and whether or not LSODE converges to a solution using this system of equations. The effects of varying these tolerances on the solution of the box model and the ORCHID model will be discussed.

  20. Aqueous organic chemistry in the atmosphere: sources and chemical processing of organic aerosols.

    PubMed

    McNeill, V Faye

    2015-02-03

    Over the past decade, it has become clear that aqueous chemical processes occurring in cloud droplets and wet atmospheric particles are an important source of organic atmospheric particulate matter. Reactions of water-soluble volatile (or semivolatile) organic gases (VOCs or SVOCs) in these aqueous media lead to the formation of highly oxidized organic particulate matter (secondary organic aerosol; SOA) and key tracer species, such as organosulfates. These processes are often driven by a combination of anthropogenic and biogenic emissions, and therefore their accurate representation in models is important for effective air quality management. Despite considerable progress, mechanistic understanding of some key aqueous processes is still lacking, and these pathways are incompletely represented in 3D atmospheric chemistry and air quality models. In this article, the concepts, historical context, and current state of the science of aqueous pathways of SOA formation are discussed.

  1. An algorithm for variational data assimilation of contact concentration measurements for atmospheric chemistry models

    NASA Astrophysics Data System (ADS)

    Penenko, Alexey; Penenko, Vladimir

    2014-05-01

    Contact concentration measurement data assimilation problem is considered for convection-diffusion-reaction models originating from the atmospheric chemistry study. High dimensionality of models imposes strict requirements on the computational efficiency of the algorithms. Data assimilation is carried out within the variation approach on a single time step of the approximated model. A control function is introduced into the source term of the model to provide flexibility for data assimilation. This function is evaluated as the minimum of the target functional that connects its norm to a misfit between measured and model-simulated data. In the case mathematical model acts as a natural Tikhonov regularizer for the ill-posed measurement data inversion problem. This provides flow-dependent and physically-plausible structure of the resulting analysis and reduces a need to calculate model error covariance matrices that are sought within conventional approach to data assimilation. The advantage comes at the cost of the adjoint problem solution. This issue is solved within the frameworks of splitting-based realization of the basic convection-diffusion-reaction model. The model is split with respect to physical processes and spatial variables. A contact measurement data is assimilated on each one-dimensional convection-diffusion splitting stage. In this case a computationally-efficient direct scheme for both direct and adjoint problem solution can be constructed based on the matrix sweep method. Data assimilation (or regularization) parameter that regulates ratio between model and data in the resulting analysis is obtained with Morozov discrepancy principle. For the proper performance the algorithm takes measurement noise estimation. In the case of Gaussian errors the probability that the used Chi-squared-based estimate is the upper one acts as the assimilation parameter. A solution obtained can be used as the initial guess for data assimilation algorithms that assimilate

  2. Ozone productivity of atmospheric organics, coordinating research council project A-10. Final report

    SciTech Connect

    Seinfeld, J.H.; Bowman, F.M.

    1996-02-06

    This project addresses elucidating the fundamental chemical basis of incremental reactivities. The value of the incremental reactivity of a particular compound, given its atmospheric oxidation mechanism, depends on the VOC/NOx mixture in which the compound is imbedded. The dependence of incremental reactivity on the base VOC/NOx mixture has been an issue of concern since the introduction of the incremental reactivity as a regulatory concept. This project answers the basic question: how and why does the incremental reactivity of a compound change as the base VOC/NOx mixture is changed, both with respect to the individual VOC combustion and with respect to the overall VOC/NOx ratio. This paper is composed of several papers which describe the methodology used to examine incremental reactivities, indicate to what factors the incremental changes in ozone can be attributed, and explain the incremental reactivities of fuel oxygenates based on their reaction chemistry.

  3. On the use of plant emitted volatile organic compounds for atmospheric chemistry simulation experiments

    NASA Astrophysics Data System (ADS)

    Kiendler-Scharr, A.; Hohaus, T.; Yu, Z.; Tillmann, R.; Kuhn, U.; Andres, S.; Kaminski, M.; Wegener, R.; Novelli, A.; Fuchs, H.; Wahner, A.

    2015-12-01

    Biogenic volatile organic compounds (BVOC) contribute to about 90% of the emitted VOC globally with isoprene being one of the most abundant BVOC (Guenther 2002). Intensive efforts in studying and understanding the impact of BVOC on atmospheric chemistry were undertaken in the recent years. However many uncertainties remain, e.g. field studies have shown that in wooded areas measured OH reactivity can often not be explained by measured BVOC and their oxidation products (e.g. Noelscher et al. 2012). This discrepancy may be explained by either a lack of understanding of BVOC sources or insufficient understanding of BVOC oxidation mechanisms. Plants emit a complex VOC mixture containing likely many compounds which have not yet been measured or identified (Goldstein and Galbally 2007). A lack of understanding BVOC sources limits bottom-up estimates of secondary products of BVOC oxidation such as SOA. Similarly, the widespread oversimplification of atmospheric chemistry in simulation experiments, using single compound or simple BVOC mixtures to study atmospheric chemistry processes limit our ability to assess air quality and climate impacts of BVOC. We will present applications of the new extension PLUS (PLant chamber Unit for Simulation) to our atmosphere simulation chamber SAPHIR. PLUS is used to produce representative BVOC mixtures from direct plant emissions. We will report on the performance and characterization of the newly developed chamber. As an exemplary application, trees typical of a Boreal forest environment were used to compare OH reactivity as directly measured by LIF to the OH reactivity calculated from BVOC measured by GC-MS and PTRMS. The comparison was performed for both, primary emissions of trees without any influence of oxidizing agents and using different oxidation schemes. For the monoterpene emitters investigated here, we show that discrepancies between measured and calculated total OH reactivity increase with increasing degree of oxidation

  4. New parameterization of dust emissions in the global atmospheric chemistry-climate model EMAC

    NASA Astrophysics Data System (ADS)

    Astitha, M.; Lelieveld, J.; Abdel Kader, M.; Pozzer, A.; de Meij, A.

    2012-05-01

    Airborne desert dust influences radiative transfer, atmospheric chemistry and dynamics, as well as nutrient transport and deposition. It directly and indirectly affects climate on regional and global scales. We present two versions of a parameterization scheme to compute desert dust emissions, incorporated into the atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy2.41 Atmospheric Chemistry). One uses a globally uniform soil particle size distribution, whereas the other explicitly accounts for different soil textures worldwide. We have tested these schemes and investigated the sensitivity to input parameters, using remote sensing data from the Aerosol Robotic Network (AERONET) and dust concentrations and deposition measurements from the AeroCom dust benchmark database (and others). The two schemes are shown to produce similar atmospheric dust loads in the N-African region, while they deviate in the Asian, Middle Eastern and S-American regions. The dust outflow from Africa over the Atlantic Ocean is accurately simulated by both schemes, in magnitude, location and seasonality. The modelled dust concentrations and deposition fluxes compare well with observations at (island) stations in the Atlantic Ocean and Asia, and are underestimated in the Pacific Ocean where annual means are relatively low (<1 μg m-3). The two schemes perform similarly well, even though the total annual source differs by ~50%, indicating the importance of transport and deposition processes (being the same for the two schemes). Our results emphasize the need to represent arid regions individually and explicitly in global models according to their unique land characteristics and meteorological conditions.

  5. A new Geoengineering Model Intercomparison Project (GeoMIP) experiment designed for climate and chemistry models

    SciTech Connect

    Tilmes, S.; Mills, Mike; Niemeier, Ulrike; Schmidt, Hauke; Robock, Alan; Kravitz, Benjamin S.; Lamarque, J. F.; Pitari, G.; English, J. M.

    2015-01-15

    A new Geoengineering Model Intercomparison Project (GeoMIP) experiment "G4 specified stratospheric aerosols" (short name: G4SSA) is proposed to investigate the impact of stratospheric aerosol geoengineering on atmosphere, chemistry, dynamics, climate, and the environment. In contrast to the earlier G4 GeoMIP experiment, which requires an emission of sulfur dioxide (SO₂) into the model, a prescribed aerosol forcing file is provided to the community, to be consistently applied to future model experiments between 2020 and 2100. This stratospheric aerosol distribution, with a total burden of about 2 Tg S has been derived using the ECHAM5-HAM microphysical model, based on a continuous annual tropical emission of 8 Tg SO₂ yr⁻¹. A ramp-up of geoengineering in 2020 and a ramp-down in 2070 over a period of 2 years are included in the distribution, while a background aerosol burden should be used for the last 3 decades of the experiment. The performance of this experiment using climate and chemistry models in a multi-model comparison framework will allow us to better understand the impact of geoengineering and its abrupt termination after 50 years in a changing environment. The zonal and monthly mean stratospheric aerosol input data set is available at https://www2.acd.ucar.edu/gcm/geomip-g4-specified-stratospheric-aerosol-data-set.

  6. A new Geoengineering Model Intercomparison Project (GeoMIP) experiment designed for climate and chemistry models

    DOE PAGES

    Tilmes, S.; Mills, Mike; Niemeier, Ulrike; ...

    2015-01-15

    A new Geoengineering Model Intercomparison Project (GeoMIP) experiment "G4 specified stratospheric aerosols" (short name: G4SSA) is proposed to investigate the impact of stratospheric aerosol geoengineering on atmosphere, chemistry, dynamics, climate, and the environment. In contrast to the earlier G4 GeoMIP experiment, which requires an emission of sulfur dioxide (SO₂) into the model, a prescribed aerosol forcing file is provided to the community, to be consistently applied to future model experiments between 2020 and 2100. This stratospheric aerosol distribution, with a total burden of about 2 Tg S has been derived using the ECHAM5-HAM microphysical model, based on a continuous annualmore » tropical emission of 8 Tg SO₂ yr⁻¹. A ramp-up of geoengineering in 2020 and a ramp-down in 2070 over a period of 2 years are included in the distribution, while a background aerosol burden should be used for the last 3 decades of the experiment. The performance of this experiment using climate and chemistry models in a multi-model comparison framework will allow us to better understand the impact of geoengineering and its abrupt termination after 50 years in a changing environment. The zonal and monthly mean stratospheric aerosol input data set is available at https://www2.acd.ucar.edu/gcm/geomip-g4-specified-stratospheric-aerosol-data-set.« less

  7. Laboratory Simulations Of Titan’s Atmospheric Chemistry With The NASA Ames Titan Haze Simulation Experiment

    NASA Astrophysics Data System (ADS)

    Sciamma-O'Brien, Ella; Contreras, C. S.; Ricketts, C. L.; Salama, F.

    2012-05-01

    Solar UV radiation and electron bombardment from Saturn’s magnetosphere dissociate nitrogen and methane in Titan’s atmosphere, leading to the production of heavier molecules and solid organic aerosols that contribute to the haze layers giving Titan its characteristic orange color. The detection of benzene and toluene, critical precursors of polycyclic aromatic hydrocarbon (PAH), in Titan’s ionosphere, by the Cassini INMS suggests that PAHs might play a role in the production of Titan’s aerosols. The Titan Haze Simulation (THS) experiment has been developed at NASA Ames’ Cosmic Simulation facility (COSmIC) to study the chemical pathways that link the simple molecules resulting from the first steps of the N2-CH4 chemistry (C2H2, C2H4, HCN..) to benzene, and to PAHs and nitrogen-containing PAHs (PANHs) as precursors to the production of solid aerosols. In the THS experiment, Titan’s atmospheric chemistry is simulated by plasma in the stream of a supersonic jet expansion. With this unique design, the gas mixture is cooled to Titan-like temperature ( 150K) before inducing the chemistry by plasma discharge. Different gas mixtures containing the first products of Titan’s N2-CH4 chemistry, but also much heavier molecules like PAHs or PANHs can be injected to study specific chemical reactions. The products of the chemistry are detected and studied using Cavity Ring Down Spectroscopy and Time-Of-Flight Mass Spectrometry. Thin tholin (Titan aerosol analogs) deposits are also produced in the THS experiment and can be analyzed by Gas Chromatography-Mass Spectrometry (GC-MS) and Scanning Electron Microscopy (SEM). We present the results of mass spectrometry studies using different gas mixtures, and discuss their relevance for the study of specific pathways in Titan’s atmospheric chemistry. Acknowledgements: This research is supported by NASA PATM. E.S.O., C.S.C. and C.L.R acknowledge the support of the NASA Postdoctoral Program. The authors acknowledge the

  8. Model projections of atmospheric steering of Sandy-like superstorms.

    PubMed

    Barnes, Elizabeth A; Polvani, Lorenzo M; Sobel, Adam H

    2013-09-17

    Superstorm Sandy ravaged the eastern seaboard of the United States, costing a great number of lives and billions of dollars in damage. Whether events like Sandy will become more frequent as anthropogenic greenhouse gases continue to increase remains an open and complex question. Here we consider whether the persistent large-scale atmospheric patterns that steered Sandy onto the coast will become more frequent in the coming decades. Using the Coupled Model Intercomparison Project, phase 5 multimodel ensemble, we demonstrate that climate models consistently project a decrease in the frequency and persistence of the westward flow that led to Sandy's unprecedented track, implying that future atmospheric conditions are less likely than at present to propel storms westward into the coast.

  9. Model projections of atmospheric steering of Sandy-like superstorms

    PubMed Central

    Barnes, Elizabeth A.; Polvani, Lorenzo M.; Sobel, Adam H.

    2013-01-01

    Superstorm Sandy ravaged the eastern seaboard of the United States, costing a great number of lives and billions of dollars in damage. Whether events like Sandy will become more frequent as anthropogenic greenhouse gases continue to increase remains an open and complex question. Here we consider whether the persistent large-scale atmospheric patterns that steered Sandy onto the coast will become more frequent in the coming decades. Using the Coupled Model Intercomparison Project, phase 5 multimodel ensemble, we demonstrate that climate models consistently project a decrease in the frequency and persistence of the westward flow that led to Sandy’s unprecedented track, implying that future atmospheric conditions are less likely than at present to propel storms westward into the coast. PMID:24003129

  10. Response of the AMOC to reduced solar radiation - the modulating role of atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Muthers, Stefan; Raible, Christoph C.; Rozanov, Eugene; Stocker, Thomas F.

    2016-11-01

    The influence of reduced solar forcing (grand solar minimum or geoengineering scenarios like solar radiation management) on the Atlantic Meridional Overturning Circulation (AMOC) is assessed in an ensemble of atmosphere-ocean-chemistry-climate model simulations. Ensemble sensitivity simulations are performed with and without interactive chemistry. In both experiments the AMOC is intensified in the course of the solar radiation reduction, which is attributed to the thermal effect of the solar forcing: reduced sea surface temperatures and enhanced sea ice formation increase the density of the upper ocean in the North Atlantic and intensify the deepwater formation. Furthermore, a second, dynamical effect on the AMOC is identified driven by the stratospheric cooling in response to the reduced solar forcing. The cooling is strongest in the tropics and leads to a weakening of the northern polar vortex. By stratosphere-troposphere interactions, the stratospheric circulation anomalies induce a negative phase of the Arctic Oscillation in the troposphere which is found to weaken the AMOC through wind stress and heat flux anomalies in the North Atlantic. The dynamic mechanism is present in both ensemble experiments. In the experiment with interactive chemistry, however, it is strongly amplified by stratospheric ozone changes. In the coupled system, both effects counteract and weaken the response of the AMOC to the solar forcing reduction. Neglecting chemistry-climate interactions in model simulations may therefore lead to an overestimation of the AMOC response to solar forcing.

  11. Coupled Surface-Atmosphere Chemistry of the Martian Peroxide and Perchlorate Oxidants

    NASA Astrophysics Data System (ADS)

    Atreya, Sushil K.; Wilson, Eric; Encrenaz, Thérèse; Kaiser, Ralf; Mahaffy, Paul

    2017-04-01

    Oxidants play a significant role in planetary habitability. On Mars, while they can be a source of nutrients, they can also destroy surface organics. They may also impact the atmospheric trace gas chemistry. Hydrogen peroxide was first detected in the martian atmosphere in 2003 [1,2], and perchlorates were detected in the surface in 2008 in the polar region [3] and 2012 in the equatorial region [4,5]. Global and seasonal maps of hydrogen peroxide have been generated from regular observations since 2003 [6], while all indications are that perchlorates are ubiquitous on Mars. Homogeneous gas phase chemistry can generally explain the observed atmospheric hydrogen peroxide, but the magnitude of seasonal variation poses a challenge. Heterogeneous chemistry involving airborne dust lifted from the surface and triboelectric processes [6,7] may play a role. Perchlorate formation on Mars is poorly understood, but one thing is clear that the same atmospheric process that works reasonably well for terrestrial perchlorates fails at Mars. An alternative proposal to perchlorate formation in an ancient aqueous environment is an initiation throughout the history of Mars in the surface by radiolysis to source gaseous ClO2 to the atmosphere with subsequent further oxidation [8]. This talk will discuss the current status of oxidant chemistry on Mars in the above context and provide directions for future laboratory and modeling studies. References: [1] Encrenaz, T., et al. (2004) Icarus 170, 424. [2] Clancy, R.T., et al. (2004) Icarus 168, 116. [3] Hecht, M.H., et al. (2009) Science, 325(5936), 64, doi:10.1126/science.1172466. [4] Glavin, D.P., et al. (2013) JGR Planets 118, 1955, doi:10.1002/jgre.20144. [5] Ming, D.W., et al. (2014) Science, 343(6169), doi:10.1126/science.1245267. [6] Encrenaz, T., et al. (2015) A&A. 578, A127 (12pp), DOI: 10.1051/0004-6361/201425448. [7] Atreya, S.K., et al. (2006) Astrobiology 6 (no. 3), 439. [8] Wilson, E.H. et al., (2016) JGR Planets, doi: 10

  12. Study of the atmospheric chemistry of radon progeny in laboratory and real indoor atmospheres

    SciTech Connect

    Hopke, P.K.

    1992-07-01

    This report covers the second year of the 28 month grant current grant to Clarkson University to study the chemical and physical behavior of the polonium 218 atom immediately following its formation by the alpha decay of radon. Because small changes in size for activity result in large changes in the delivered dose per unit exposure, this behavior must be understood if the exposure to radon progeny and it dose to the cells in the respiratory tract are to be fully assessed. Two areas of radon progeny behavior are being pursued; laboratory studies under controlled conditions to better understand the fundamental physical and chemical process that affect the progeny's atmospheric behavior and studies in actual indoor environments to develop a better assessment of the exposure of the occupants of that space to the size and concentration of the indoor radioactive aerosol. This report describes the progress toward achieving these objectives.

  13. Human "Footprints" in the Atmosphere: Anthropogenic Evidence in MOPITT and TES Atmospheric Chemistry Data

    NASA Astrophysics Data System (ADS)

    Hunt, L. A.

    2005-05-01

    The Measurements Of Pollution In The Troposphere (MOPITT) experiment was launched on board the NASA Earth Observing System (EOS) Terra Satellite in December 1999 and has accumulated more than five years of global carbon monoxide measurements. Available MOPITT data products include Level 1 radiances and Level 2 derived CO total column and mixing ratio profiles at a horizontal resolution of about 22 km at nadir and a vertical resolution of about 4 km. The primary sources of CO are biomass burning and industrial pollution, making CO an indicator of the anthropogenic influence on the atmosphere. MOPITT is the first instrument to make long-term global measurements of this species and is providing a better understanding of its transport, sources and sinks. A number of visual results will be included in this presentation. The Tropospheric Emission Spectrometer (TES) instrument is a high-resolution imaging infrared Fourier-transform spectrometer that operates in both nadir and limb-sounding modes. TES is flying aboard Aura, the third of NASA's EOS satellites, which was launched in July 2004. Tropospheric ozone is a pollutant and a greenhouse gas. It has both natural and anthropogenic sources. TES makes global 3-D measurements of ozone and other chemical species involved in its formation and destruction, including water vapor, methane, carbon monoxide, nitrogen dioxide, and nitric acid. The spatial resolution is 0.5 x 5 km in the nadir and 2.3 x 23 km in the limb. Level 1B spectral radiance data are currently available, and the Level 2 species data products will be publicly available in Summer 2005. Preliminary visual results will be shown. These data are available free of charge from the NASA Langley Atmospheric Sciences Data Center. Additional information can be found at http://eosweb.larc.nasa.gov.

  14. Role of water in alkali halide heterogeneous chemistry relevant to the atmosphere: A surface science study

    NASA Astrophysics Data System (ADS)

    Ghosal, Sutapa

    2001-05-01

    Water is a ubiquitous atmospheric constituent. The interaction of water in its various forms (vapor, liquid, ice) with other atmospheric constituents has a significant impact on the chemistry of the atmosphere. Another class of compounds that are of considerable importance in atmospheric chemistry are alkali halide salts such as sea salt particles. Heterogeneous reactions of alkali halides with gas phase pollutants are believed to be an important source of halogens in the troposphere. There is an increasing amount of evidence that the presence of water plays an important role in the heterogeneous chemistry of alkali halide particles. It is the goal of this dissertation to contribute to the understanding of the interaction of water with alkali halide surfaces and its atmospheric implications. Surface processes are of fundamental importance in heterogeneous atmospheric chemistry, but they are often difficult to study because of their inherent complexity. As this dissertation shows, the use of modern surface science techniques offer valuable insights into these complex processes and as such offer complementary alternatives to the traditional atmospheric chemistry experiments. The surface science techniques used in this dissertation are X-ray photoelectron spectroscopy (XPS), scanning polarization force microscopy (SPFM) and scanning electron microscopy (SEM). Presented here are the results of the XPS and SEM studies undertaken to determine the nature and content of surface adsorbed water on NaCl as a function of surface defects. The details of HNO3 uptake on NaCl and the effect of surface adsorbed water on this uptake are also discussed. Our results show that the amount of ``strongly adsorbed water'' (SAW) on the surface of NaCl particles depends on the particle size and hence, on the concentration of surface defects. Unlike the (100) single crystal the more defective surfaces show dissociative water uptake at room temperature upon exposure to water vapor well below

  15. CAM-chem: description and evaluation of interactive atmospheric chemistry in the Community Earth System Model

    SciTech Connect

    Lamarque, J.-F.; Emmons, L.; Hess, Peter; Kinnison, Douglas E.; Tilmes, S.; Vitt, Francis; Heald, C. L.; Holland, Elisabeth A.; Lauritzen, P. H.; Neu, J.; Orlando, J. J.; Rasch, Philip J.; Tyndall, G. S.

    2012-03-27

    We discuss and evaluate the representation of atmospheric chemistry in the global Community Atmosphere Model (CAM) version 4, the atmospheric component of the Community Earth System Model (CESM). We present a variety of configurations for the representation of tropospheric and stratospheric chemistry, wet removal, and online and offline meteorology. Results from simulations illustrating these configurations are compared with surface, aircraft and satellite observations. Major biases include a negative bias in the high-latitude CO distribution, a positive bias in upper-tropospheric/lower-stratospheric ozone, and a positive bias in summertime surface ozone (over the United States and Europe). The tropospheric net chemical ozone production varies significantly between configurations, partly related to variations in stratosphere-troposphere exchange. Aerosol optical depth tends to be underestimated over most regions, while comparison with aerosol surface measurements over the United States indicate reasonable results for sulfate, especially in the online simulation. Other aerosol species exhibit significant biases. Overall, the model-data comparison indicates that the offline simulation driven by GEOS5 meteorological analyses provides the best simulation, possibly due in part to the increased vertical resolution (52 levels instead of 26 for online dynamics). The CAM-chem code as described in this paper, along with all the necessary datasets needed to perform the simulations described here, are available for download at www.cesm.ucar.edu.

  16. Simulation chamber studies on the NO3 chemistry of atmospheric aldehydes

    NASA Astrophysics Data System (ADS)

    Bossmeyer, J.; Brauers, T.; Richter, C.; Rohrer, F.; Wegener, R.; Wahner, A.

    2006-09-01

    Absolute reaction rate studies of NO3 radicals with 4 aldehydes were performed in the atmosphere simulation chamber SAPHIR at the Research Center Jülich. Rate coefficients (ethanal: 2.6 +/- 0.5, propanal: 5.8 +/- 1.0, butanal: 11.9 +/- 1.4, benzaldehyde: 2.2 +/- 0.6; in 10-15 cm3 s-1 at 300 K) were determined from measured concentration-time profiles of aldehydes and NO3 at near ambient conditions. The values for the aliphatic aldehydes are in good agreement with the most recent recommendations (IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry: Evaluated kinetic and photochemical data for atmospheric chemistry, 2005, available at http://www.iupac-kinetic.ch.cam.ac.uk). The measured concentration-time profiles of precursor aldehydes, NO3, NO2, and of product aldehydes were compared to model calculations based on the MCM v3 (Jenkin et al., 2003; Saunders et al., 2003). Differences between measurements and model are attributed to a major interference of the GC system to peroxyacyl nitrates. In addition modifications to the rate constants in the MCM are suggested.

  17. Study of the diurnal variability of atmospheric chemistry with respect to boundary layer dynamics during DOMINO

    NASA Astrophysics Data System (ADS)

    van Stratum, B. J. H.; Vilà-Guerau de Arellano, J.; Ouwersloot, H. G.; van den Dries, K.; van Laar, T. W.; Martinez, M.; Lelieveld, J.; Diesch, J.-M.; Drewnick, F.; Fischer, H.; Hosaynali Beygi, Z.; Harder, H.; Regelin, E.; Sinha, V.; Adame, J. A.; Sörgel, M.; Sander, R.; Bozem, H.; Song, W.; Williams, J.; Yassaa, N.

    2012-03-01

    We study the interactions between atmospheric boundary layer (ABL) dynamics and atmospheric chemistry using a mixed-layer model (MXLCH) coupled to chemical reaction schemes. Guided by both atmospheric and chemical measurements obtained during the DOMINO campaign (2008), numerical experiments are performed to study the role of ABL dynamics and the accuracy of chemical schemes with different complexity: MOZART-4 and a reduced mechanism of this chemical system. Both schemes produce satisfactory results, indicating that the reduced scheme is capable of reproducing the O3-NOx-VOC-HOx diurnal cycle during conditions characterised by a low NOx regime and small O3 tendencies (less than 1 ppb per hour). By focussing on the budget equations of chemical species in the mixed-layer model, we show that for species like O3, NO and NO2, the influence of entrainment and boundary layer growth is of the same order as chemical production/loss. This indicates that an accurate representation of ABL processes is crucial in understanding the daily cycle of chemical species. By comparing the time scales of chemical reactive species with the mixing time scale of turbulence, we propose a classification based on the Damköhler number to further determine the importance of dynamics on chemistry during field campaigns. Our findings advocate an integrated approach, simultaneously solving the ABL dynamics and chemical reactions, in order to obtain a better understanding of chemical pathways and processes and the interpretation of the results obtained during measurement campaigns.

  18. Oxidation of a new Biogenic VOC: Chamber Studies of the Atmospheric Chemistry of Methyl Chavicol

    NASA Astrophysics Data System (ADS)

    Bloss, William; Alam, Mohammed; Adbul Raheem, Modinah; Rickard, Andrew; Hamilton, Jacqui; Pereira, Kelly; Camredon, Marie; Munoz, Amalia; Vazquez, Monica; Vera, Teresa; Rodenas, Mila

    2013-04-01

    The oxidation of volatile organic compounds (VOCs) leads to formation of ozone and SOA, with consequences for air quality, health, crop yields, atmospheric chemistry and radiative transfer. Recent observations have identified Methyl Chavicol ("MC": Estragole; 1-allyl-4-methoxybenzene, C10H12O) as a major BVOC above pine forests in the USA, and oil palm plantations in Malaysian Borneo. Palm oil cultivation, and hence MC emissions, may be expected to increase with societal food and bio fuel demand. We present the results of a series of simulation chamber experiments to assess the atmospheric fate of MC. Experiments were performed in the EUPHORE facility, monitoring stable product species, radical intermediates, and aerosol production and composition. We determine rate constants for reaction of MC with OH and O3, and ozonolysis radical yields. Stable product measurements (FTIR, PTRMS, GC-SPME) are used to determine the yields of stable products formed from OH- and O3- initiated oxidation, and to develop an understanding of the initial stages of the MC degradation chemistry. A surrogate mechanism approach is used to simulate MC degradation within the MCM, evaluated in terms of ozone production measured in the chamber experiments, and applied to quantify the role of MC in the real atmosphere.

  19. Analytical Models of Exoplanetary Atmospheres. III. Gaseous C-H-O-N Chemistry with Nine Molecules

    NASA Astrophysics Data System (ADS)

    Heng, Kevin; Tsai, Shang-Min

    2016-10-01

    We present novel, analytical, equilibrium-chemistry formulae for the abundances of molecules in hot exoplanetary atmospheres that include the carbon, oxygen, and nitrogen networks. Our hydrogen-dominated solutions involve acetylene (C2H2), ammonia (NH3), carbon dioxide (CO2), carbon monoxide (CO), ethylene (C2H4), hydrogen cyanide (HCN), methane (CH4), molecular nitrogen (N2), and water (H2O). By considering only the gas phase, we prove that the mixing ratio of carbon monoxide is governed by a decic equation (polynomial equation of 10 degrees). We validate our solutions against numerical calculations of equilibrium chemistry that perform Gibbs free energy minimization and demonstrate that they are accurate at the ˜ 1 % level for temperatures from 500 to 3000 K. In hydrogen-dominated atmospheres, the ratio of abundances of HCN to CH4 is nearly constant across a wide range of carbon-to-oxygen ratios, which makes it a robust diagnostic of the metallicity in the gas phase. Our validated formulae allow for the convenient benchmarking of chemical kinetics codes and provide an efficient way of enforcing chemical equilibrium in atmospheric retrieval calculations.

  20. Bimineralic ooids as a record of Late Paleozoic changes in atmospheric and oceanic chemistry

    SciTech Connect

    Watson, B.A.; Algeo, T.J. . Dept. of Geology)

    1994-03-01

    Mineralogic variation in modern ooids is thought to be controlled mainly by short-term changes in the chemistry of the precipitating fluid. Other research documents large fluctuations in atmospheric pCO2 and changes in the mineralogy of tropical-marine carbonate sediments in relation to Pleistocene glacial/interglacial cycles. Glacio-eustatic control is generally inferred for transgressive/regressive carbonate cycles of Late Pennsylvanian age. The authors are investigating changes in ooid mineralogy in Late Pennsylvanian carbonates of the Midcontinent area that may provide a record of changing atmospheric and oceanic chemistry at this time. This study employs petrographic and geochemical techniques for inferring original carbonate mineralogy to document dominant primary mineralogies of ooids in transgressive and regressive limestone in the Missourian Series in southeastern Kansas. Enrichment of strontium in aragonite relative to calcite provides a trace-elemental indicator of primary mineralogies. Microprobe analyses of ooids with tangential fabrics show enrichment in strontium while strontium in ooids with radial fabrics is at lower levels. Investigation thus far suggests that originally aragonitic ooids having a tangential fabric are commonly associated with regressive units whereas originally calcitic ooids with radial fabric are more common in transgressive units. Changes in ooid mineralogy within and between transgressive/regressive limestones may allow semi-quantitative interpretation of changes in paleo-atmospheric and paleo-oceanic CO2 levels based on mineralogy.

  1. A numerical method for parameterization of atmospheric chemistry - Computation of tropospheric OH

    NASA Technical Reports Server (NTRS)

    Spivakovsky, C. M.; Wofsy, S. C.; Prather, M. J.

    1990-01-01

    An efficient and stable computational scheme for parameterization of atmospheric chemistry is described. The 24-hour-average concentration of OH is represented as a set of high-order polynomials in variables such as temperature, densities of H2O, CO, O3, and NO(t) (defined as NO + NO2 + NO3 + 2N2O5 + HNO2 + HNO4) as well as variables determining solar irradiance: cloud cover, density of the overhead ozone column, surface albedo, latitude, and solar declination. This parameterization of OH chemistry was used in the three-dimensional study of global distribution of CH3CCl3. The proposed computational scheme can be used for parameterization of rates of chemical production and loss or of any other output of a full chemical model.

  2. Independent Learning Project for Advanced Chemistry (ILPAC). Teachers' and Technicians' Notes for First Year Units.

    ERIC Educational Resources Information Center

    Inner London Education Authority (England).

    The Independent Learning Project for Advanced Chemistry (ILPAC) has produced units of study for students in A-level chemistry. Students completing ILPAC units assume a greater responsibility for their own learning and can work, to some extent, at their own pace. By providing guidance, and detailed solutions to exercises in the units, supported by…

  3. Chemistry Teaching through the Student's World: A High School Project in Mexico.

    ERIC Educational Resources Information Center

    Garritz, Andoni; Chamizo, Jose A.

    1994-01-01

    Describes a project to revise high school chemistry courses in Mexico in the face of decreasing student selection of chemistry careers and the increasing social importance of chemical literacy. Changes include recognizing pedagogical advances and going beyond traditional subjects to teach chemical language, method, and quantitativeness. The new…

  4. Independent Learning Project for Advanced Chemistry (ILPAC). Teachers' and Technicians' Notes for First Year Units.

    ERIC Educational Resources Information Center

    Inner London Education Authority (England).

    The Independent Learning Project for Advanced Chemistry (ILPAC) has produced units of study for students in A-level chemistry. Students completing ILPAC units assume a greater responsibility for their own learning and can work, to some extent, at their own pace. By providing guidance, and detailed solutions to exercises in the units, supported by…

  5. Untangling the Chemical Evolution of Titan's Atmosphere and Surface -- From Homogeneous to Heterogeneous Chemistry

    SciTech Connect

    Kaiser, Ralf I.; Maksyutenko, Pavlo; Ennis, Courtney; Zhang, Fangtong; Gu, Xibin; Krishtal, Sergey P.; Mebel, Alexander M.; Kostko, Oleg; Ahmed, Musahid

    2010-03-16

    The arrival of the Cassini-Huygens probe at Saturn's moon Titan - the only Solar System body besides Earth and Venus with a solid surface and a thick atmosphere with a pressure of 1.4 atm at surface level - in 2004 opened up a new chapter in the history of Solar System exploration. The mission revealed Titan as a world with striking Earth-like landscapes involving hydrocarbon lakes and seas as well as sand dunes and lava-like features interspersed with craters and icy mountains of hitherto unknown chemical composition. The discovery of a dynamic atmosphere and active weather system illustrates further the similarities between Titan and Earth. The aerosol-based haze layers, which give Titan its orange-brownish color, are not only Titan's most prominent optically visible features, but also play a crucial role in determining Titan's thermal structure and chemistry. These smog-like haze layers are thought to be very similar to those that were present in Earth's atmosphere before life developed more than 3.8 billion years ago, absorbing the destructive ultraviolet radiation from the Sun, thus acting as 'prebiotic ozone' to preserve astrobiologically important molecules on Titan. Compared to Earth, Titan's low surface temperature of 94 K and the absence of liquid water preclude the evolution of biological chemistry as we know it. Exactly because of these low temperatures, Titan provides us with a unique prebiotic 'atmospheric laboratory' yielding vital clues - at the frozen stage - on the likely chemical composition of the atmosphere of the primitive Earth. However, the underlying chemical processes, which initiate the haze formation from simple molecules, have been not understood well to date.

  6. Atmospheric chemistry, sources and sinks of carbon suboxide, C3O2

    NASA Astrophysics Data System (ADS)

    Keßel, Stephan; Cabrera-Perez, David; Horowitz, Abraham; Veres, Patrick R.; Sander, Rolf; Taraborrelli, Domenico; Tucceri, Maria; Crowley, John N.; Pozzer, Andrea; Stönner, Christof; Vereecken, Luc; Lelieveld, Jos; Williams, Jonathan

    2017-07-01

    Carbon suboxide, O = C = C = C = O, has been detected in ambient air samples and has the potential to be a noxious pollutant and oxidant precursor; however, its lifetime and fate in the atmosphere are largely unknown. In this work, we collect an extensive set of studies on the atmospheric chemistry of C3O2. Rate coefficients for the reactions of C3O2 with OH radicals and ozone were determined as kOH = (2.6 ± 0.5) × 10-12 cm3 molecule-1 s-1 at 295 K (independent of pressure between ˜ 25 and 1000 mbar) and kO3 < 1.5 × 10-21 cm3 molecule-1 s-1 at 295 K. A theoretical study on the mechanisms of these reactions indicates that the sole products are CO and CO2, as observed experimentally. The UV absorption spectrum and the interaction of C3O2 with water (Henry's law solubility and hydrolysis rate constant) were also investigated, enabling its photodissociation lifetime and hydrolysis rates, respectively, to be assessed. The role of C3O2 in the atmosphere was examined using in situ measurements, an analysis of the atmospheric sources and sinks and simulation with the EMAC atmospheric chemistry-general circulation model. The results indicate sub-pptv levels at the Earth's surface, up to about 10 pptv in regions with relatively strong sources, e.g. influenced by biomass burning, and a mean lifetime of ˜ 3.2 days. These predictions carry considerable uncertainty, as more measurement data are needed to determine ambient concentrations and constrain the source strengths.

  7. A Collaborative, Wiki-Based Organic Chemistry Project Incorporating Free Chemistry Software on the Web

    ERIC Educational Resources Information Center

    Evans, Michael J.; Moore, Jeffrey S.

    2011-01-01

    In recent years, postsecondary instructors have recognized the potential of wikis to transform the way students learn in a collaborative environment. However, few instructors have embraced in-depth student use of chemistry software for the creation of interactive chemistry content on the Web. Using currently available software, students are able…

  8. A Collaborative, Wiki-Based Organic Chemistry Project Incorporating Free Chemistry Software on the Web

    ERIC Educational Resources Information Center

    Evans, Michael J.; Moore, Jeffrey S.

    2011-01-01

    In recent years, postsecondary instructors have recognized the potential of wikis to transform the way students learn in a collaborative environment. However, few instructors have embraced in-depth student use of chemistry software for the creation of interactive chemistry content on the Web. Using currently available software, students are able…

  9. The NOx dependence of bromine chemistry in the Arctic atmospheric boundary layer

    NASA Astrophysics Data System (ADS)

    Custard, K. D.; Thompson, C. R.; Pratt, K. A.; Shepson, P. B.; Liao, J.; Huey, L. G.; Orlando, J. J.; Weinheimer, A. J.; Apel, E.; Hall, S. R.; Flocke, F.; Mauldin, L.; Hornbrook, R. S.; Pöhler, D.; S., General; Zielcke, J.; Simpson, W. R.; Platt, U.; Fried, A.; Weibring, P.; Sive, B. C.; Ullmann, K.; Cantrell, C.; Knapp, D. J.; Montzka, D. D.

    2015-09-01

    Arctic boundary layer nitrogen oxides (NOx = NO2 + NO) are naturally produced in and released from the sunlit snowpack and range between 10 to 100 pptv in the remote background surface layer air. These nitrogen oxides have significant effects on the partitioning and cycling of reactive radicals such as halogens and HOx (OH + HO2). However, little is known about the impacts of local anthropogenic NOx emission sources on gas-phase halogen chemistry in the Arctic, and this is important because these emissions can induce large variability in ambient NOx and thus local chemistry. In this study, a zero-dimensional photochemical kinetics model was used to investigate the influence of NOx on the unique springtime halogen and HOx chemistry in the Arctic. Trace gas measurements obtained during the 2009 OASIS (Ocean - Atmosphere - Sea Ice - Snowpack) field campaign at Barrow, AK were used to constrain many model inputs. We find that elevated NOx significantly impedes gas-phase halogen radical-based depletion of ozone, through the production of a variety of reservoir species, including HNO3, HO2NO2, peroxyacetyl nitrate (PAN), BrNO2, ClNO2 and reductions in BrO and HOBr. The effective removal of BrO by anthropogenic NOx was directly observed from measurements conducted near Prudhoe Bay, AK during the 2012 Bromine, Ozone, and Mercury Experiment (BROMEX). Thus, while changes in snow-covered sea ice attributable to climate change may alter the availability of molecular halogens for ozone and Hg depletion, predicting the impact of climate change on polar atmospheric chemistry is complex and must take into account the simultaneous impact of changes in the distribution and intensity of anthropogenic combustion sources. This is especially true for the Arctic, where NOx emissions are expected to increase because of increasing oil and gas extraction and shipping activities.

  10. Lessons Learned from the Bay Region Atmospheric Chemistry Experiment (BRACE) and Implications for Nitrogen Management of Tampa Bay

    EPA Science Inventory

    Results from air quality modeling and field measurements made as part of the Bay Region Atmospheric Chemistry Experiment (BRACE) along with related scientific literature were reviewed to provide an improved estimate of atmospheric reactive nitrogen (N) deposition to Tampa Bay, to...

  11. Lessons Learned from the Bay Region Atmospheric Chemistry Experiment (BRACE) and Implications for Nitrogen Management of Tampa Bay

    EPA Science Inventory

    Results from air quality modeling and field measurements made as part of the Bay Region Atmospheric Chemistry Experiment (BRACE) along with related scientific literature were reviewed to provide an improved estimate of atmospheric reactive nitrogen (N) deposition to Tampa Bay, to...

  12. Chemistry and aerosol model development for the Copernicus Atmosphere Monitoring Service at ECWMF

    NASA Astrophysics Data System (ADS)

    Flemming, Johannes; Huijnen, Vincent; Remy, Samuel; Kipling, Zak

    2017-04-01

    The global forecast and data assimilation system for atmospheric composition of the Copernicus Atmosphere Monitoring Service (CAMS) is part of ECMWF's integrated forecasting system (IFS). The CAMS system is run on a lower resolution (40 km) than the operational Numerical Weather Prediction (NWP) suite (9km), but it uses the same meteorological model for both configurations in order to maintain a seamless approach to earth-system forecasting. The IFS with the modules for atmospheric composition is referred to as C-IFS. Although developments of the chemistry and aerosol modules are by far the most important reasons for changes in the simulation of atmospheric composition with C-IFS, the impact of continuous developments of the meteorological part of C-IFS also introduces changes to the operational composition forecast. The development of the IFS is predominantly driven by the improvements in weather predication scores at high resolution. IFS model upgrades occur several times a year. In the presentation we will address the opportunities and challenges to improve the quality of the CAMS operational composition forecasts as part of a steadily changing operational NWP system. We will discuss examples on how changes in the IFS model impact the composition simulation such as changes to the convection scheme, lightning activity and surface processes. We will also provide a detailed break down of the additional computational cost of the atmospheric composition simulation.

  13. Observations of atmospheric and snowpack chemistry in the summer on the Juneau Icefield

    NASA Astrophysics Data System (ADS)

    Berry, J.; Thompson, C. R.; Pratt, K.

    2014-12-01

    Cryospheric environments, such as ice sheets and glaciers, are particularly sensitive to perturbations in radiative forcing due to climate change. In recent decades, research in Arctic regions has revealed unique local-scale chemistry related to the greenhouse gas ozone and chemical interactions with snow and ice surfaces. Additionally, these remote regions are often impacted by long range transport events that bring atmospheric pollutants, including both gases and atmospheric particles, from anthropogenic sources and biomass burning; these pollutants can reduce visibility, change absorption and/or scattering of solar radiation, and lead to reductions in snow albedo (e.g., through deposition of black carbon). Both ozone and black carbon particles have consequences on radiative forcing and can lead to increased snow ablation and glacier recession. The Juneau Icefield is a temperate tidewater glacier network located east of Juneau, Alaska. In July 2014, as part of the Juneau Icefield Research Program, we conducted a pilot study including measurements of ozone, size-resolved atmospheric particles, and atmospheric black carbon, in conjunction with snowpack black carbon, inorganic ion, and albedo measurements. Here, we present the initial findings from this study and discuss local-scale atmospheric composition and impacts of long-range transport on snow albedo.

  14. Active Upper-atmosphere Chemistry and Dynamics from Polar Circulation Reversal on Titan

    NASA Technical Reports Server (NTRS)

    Teanby, Nicholas A.; Irwin, Patrick Gerard Joseph; Nixon, Conor A.; DeKok, Remco; Vinatier, Sandrine; Coustenis, Athena; Sefton-Nash, Elliot; Calcutt, Simon B.; Flasar, Michael F.

    2012-01-01

    Saturn's moon Titan has a nitrogen atmosphere comparable to Earth's, with a surface pressure of 1.4 bar. Numerical models reproduce the tropospheric conditions very well but have trouble explaining the observed middle-atmosphere temperatures, composition and winds. The top of the middle-atmosphere circulation has been thought to lie at an altitude of 450 to 500 kilometres, where there is a layer of haze that appears to be separated from the main haze deck. This 'detached' haze was previously explained as being due to the colocation of peak haze production and the limit of dynamical transport by the circulation's upper branch. Herewe report a build-up of trace gases over the south pole approximately two years after observing the 2009 post-equinox circulation reversal, from which we conclude that middle-atmosphere circulation must extend to an altitude of at least 600 kilometres. The primary drivers of this circulation are summer-hemisphere heating of haze by absorption of solar radiation and winter-hemisphere cooling due to infrared emission by haze and trace gases; our results therefore imply that these effects are important well into the thermosphere (altitudes higher than 500 kilometres). This requires both active upper-atmosphere chemistry, consistent with the detection of high-complexity molecules and ions at altitudes greater than 950 kilometres, and an alternative explanation for the detached haze, such as a transition in haze particle growth from monomers to fractal structures.

  15. Prebiotic Chemistry and Atmospheric Warming of Early Earth by an Active Young Sun

    NASA Technical Reports Server (NTRS)

    Airapetian, V. S.; Glocer, A.; Gronoff, G.; Hebrard, E.; Danchi, W.

    2016-01-01

    Nitrogen is a critical ingredient of complex biological molecules. Molecular nitrogen, however, which was outgassed Into the Earth's early atmosphere, is relatively chemically inert and nitrogen fixation into more chemically reactive compounds requires high temperatures. Possible mechanisms of nitrogen fixation include lightning, atmospheric shock heating by meteorites, and solar ultraviolet radiation. Here we show that nitrogen fixation in the early terrestrial atmosphere can be explained by frequent and powerful coronal mass ejection events from the young Sun -- so-called superflares. Using magnetohydrodynamic simulations constrained by Kepler Space Telescope observations, we find that successive superflare ejections produce shocks that accelerate energetic particles, which would have compressed the early Earth's magnetosphere. The resulting extended polar cap openings provide pathways for energetic particles to penetrate into the atmosphere and, according to our atmospheric chemistry simulations, initiate reactions converting molecular nitrogen, carbon dioxide and methane to the potent greenhouse gas nitrous oxide as well as hydrogen cyanide, an essential compound for life. Furthermore, the destruction of N2, C02 and CH, suggests that these greenhouse gases cannot explain the stability of liquid water on the early Earth. Instead, we propose that the efficient formation of nitrous oxide could explain a warm early Earth.

  16. Active upper-atmosphere chemistry and dynamics from polar circulation reversal on Titan.

    PubMed

    Teanby, Nicholas A; Irwin, Patrick G J; Nixon, Conor A; de Kok, Remco; Vinatier, Sandrine; Coustenis, Athena; Sefton-Nash, Elliot; Calcutt, Simon B; Flasar, F Michael

    2012-11-29

    Saturn's moon Titan has a nitrogen atmosphere comparable to Earth's, with a surface pressure of 1.4 bar. Numerical models reproduce the tropospheric conditions very well but have trouble explaining the observed middle-atmosphere temperatures, composition and winds. The top of the middle-atmosphere circulation has been thought to lie at an altitude of 450 to 500 kilometres, where there is a layer of haze that appears to be separated from the main haze deck. This 'detached' haze was previously explained as being due to the co-location of peak haze production and the limit of dynamical transport by the circulation's upper branch. Here we report a build-up of trace gases over the south pole approximately two years after observing the 2009 post-equinox circulation reversal, from which we conclude that middle-atmosphere circulation must extend to an altitude of at least 600 kilometres. The primary drivers of this circulation are summer-hemisphere heating of haze by absorption of solar radiation and winter-hemisphere cooling due to infrared emission by haze and trace gases; our results therefore imply that these effects are important well into the thermosphere (altitudes higher than 500 kilometres). This requires both active upper-atmosphere chemistry, consistent with the detection of high-complexity molecules and ions at altitudes greater than 950 kilometres, and an alternative explanation for the detached haze, such as a transition in haze particle growth from monomers to fractal structures.

  17. Prebiotic chemistry and atmospheric warming of early Earth by an active young Sun

    NASA Astrophysics Data System (ADS)

    Airapetian, V. S.; Glocer, A.; Gronoff, G.; Hébrard, E.; Danchi, W.

    2016-06-01

    Nitrogen is a critical ingredient of complex biological molecules. Molecular nitrogen, however, which was outgassed into the Earth’s early atmosphere, is relatively chemically inert and nitrogen fixation into more chemically reactive compounds requires high temperatures. Possible mechanisms of nitrogen fixation include lightning, atmospheric shock heating by meteorites, and solar ultraviolet radiation. Here we show that nitrogen fixation in the early terrestrial atmosphere can be explained by frequent and powerful coronal mass ejection events from the young Sun--so-called superflares. Using magnetohydrodynamic simulations constrained by Kepler Space Telescope observations, we find that successive superflare ejections produce shocks that accelerate energetic particles, which would have compressed the early Earth’s magnetosphere. The resulting extended polar cap openings provide pathways for energetic particles to penetrate into the atmosphere and, according to our atmospheric chemistry simulations, initiate reactions converting molecular nitrogen, carbon dioxide and methane to the potent greenhouse gas nitrous oxide as well as hydrogen cyanide, an essential compound for life. Furthermore, the destruction of N2, CO2 and CH4 suggests that these greenhouse gases cannot explain the stability of liquid water on the early Earth. Instead, we propose that the efficient formation of nitrous oxide could explain a warm early Earth.

  18. The Right Chemistry. Lawn Care Project Brings Science down to Earth.

    ERIC Educational Resources Information Center

    Dollar, David

    1992-01-01

    At Southwest High School in Fort Worth, Texas, an applied learning project enables chemistry students to determine the most effective, economical, and environmentally safe fertilizer for the lawns of schools in the district. (SK)

  19. The Right Chemistry. Lawn Care Project Brings Science down to Earth.

    ERIC Educational Resources Information Center

    Dollar, David

    1992-01-01

    At Southwest High School in Fort Worth, Texas, an applied learning project enables chemistry students to determine the most effective, economical, and environmentally safe fertilizer for the lawns of schools in the district. (SK)

  20. Specification of Biogenic VOC Emission Data in the Coupled System of Regional Climate and Atmospheric Chemistry/Aerosols Model

    NASA Astrophysics Data System (ADS)

    Zemankova, K.; Huszar, P.

    2009-12-01

    Coupling of regional climate model RegCM (Pal et al., 2007) and atmospheric chemistry/aerosols model CAMx (Environ, 2006) is being developed at our department under the CECILIA project (EC 6th FP) with the aim to study climate forcing due to atmospheric chemistry/aerosols on regional scale. Regional climate model RegCM with the resolution of 10 km drives transport, chemistry and dry/wet deposition of the CAMx model being operated on the Central and Eastern European domain and consequently the radiative active agents from the CAMx model enter the radiative transfer schemes for the calculation of heating rate changes in the regional climate model. In order to increase the accuracy of land cover data in this model system, a new input dataset has been prepared and used for the calculation of emissions of volatile organic compounds (VOCs) from natural sources. This dataset is mainly based on the single tree species database from the european project of JRC in Ispra - Agriculture, Forestry, and Other Land Uses in Europe (AFOLU) which covers most of the model domain. For the locations where AFOLU data were not available, i.e. basically non-EU areas, the USGS Eurasia land cover database has been used. Both databases are available in 1 km resolution. Emission factors for new land cover categories were obtained either from the laboratory measurements or from the literature. The Guenther et al. (1995) model algorithm has been used for the calculation of biogenic VOC (BVOC) emission fluxes. Effects of new land cover and BVOC emission data on the CAMx model simulations of low level ozone in the year 2000 have been studied. Improvement of model results when compared with the measured data may be seen, especially in the simulation of extreme values such as ozone summer maxima. References: - ENVIRON Corp., 2006. CAMx User’s Guide, version 4.40 - Guenther A., Hewitt N., Erickson D., Fall R., Geron Ch., Graedel T., Harley P., Klinger L., Lerdau M., McKay W. A., Pierce T., Scholes

  1. Upper atmosphere research satellite program. [to study the chemistry energetics, and dynamics

    NASA Technical Reports Server (NTRS)

    Huntress, W. T., Jr.

    1978-01-01

    A satellite program to conduct research on the chemistry, energetics, and dynamics of the upper atmosphere was developed. The scientific goals of the Upper Atmospheric Research Program, the program requirements, and the approach toward meeting those requirements are outlined. An initial series of two overlapping spacecraft missions is described. Both spacecraft are launched and recovered by the STS, one in the winter of 1983 at a 56 deg inclination, and the other a year later at a 70 deg inclination. The duration of each mission is 18 months, and each carries instruments to make global measurements of the temperature, winds, composition, irradation, and radiance in the stratosphere, mesosphere, and lower thermosphere between the tropopause and 120 km altitude. The program requires a dedicated ground-based data system and a science team organization that leads to a strong interaction between the experiments and theory. The program includes supportive observations from other platforms such as rockets, balloons, and the Spacelab.

  2. Diphosphine is an intermediate in the photolysis of phosphine to phosphorus and hydrogen. [Jupiter atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Ferris, J. P.; Benson, R.

    1980-01-01

    The photolysis of phosphine to red phosphorus (P4) and hydrogen is investigated in light of the potential significance of the reaction in the atmospheric chemistry of Jupiter. It is reported that the photolysis of PH3 at room temperature by a 206.2-nm light source gave rise to a product identified by its UV and IR spectra and gas chromatographic retention time as P2H4, the yield of which is found to increase to a maximum and then decrease to 20% of the maximum value with illumination time. A mechanism for phosphine photolysis including diphosphine formation as an intermediate step is proposed, and it is concluded that P2H4 is a likely constituent of the atmospheres of the Jovian planets.

  3. Diphosphine is an intermediate in the photolysis of phosphine to phosphorus and hydrogen. [Jupiter atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Ferris, J. P.; Benson, R.

    1980-01-01

    The photolysis of phosphine to red phosphorus (P4) and hydrogen is investigated in light of the potential significance of the reaction in the atmospheric chemistry of Jupiter. It is reported that the photolysis of PH3 at room temperature by a 206.2-nm light source gave rise to a product identified by its UV and IR spectra and gas chromatographic retention time as P2H4, the yield of which is found to increase to a maximum and then decrease to 20% of the maximum value with illumination time. A mechanism for phosphine photolysis including diphosphine formation as an intermediate step is proposed, and it is concluded that P2H4 is a likely constituent of the atmospheres of the Jovian planets.

  4. Contrail: A Module from Physical Chemistry On-Line Project

    ERIC Educational Resources Information Center

    Chen, Franklin; Zielinski, Theresa Julia; Long, George

    2007-01-01

    The impact of contrails on Earth's climate is researched to understand the active area. It is suggested that the process of contrail formation involves combustion, cooling and ice formation, which are good comprehensive learning exercise for physical chemistry students.

  5. Contrail: A Module from Physical Chemistry On-Line Project

    ERIC Educational Resources Information Center

    Chen, Franklin; Zielinski, Theresa Julia; Long, George

    2007-01-01

    The impact of contrails on Earth's climate is researched to understand the active area. It is suggested that the process of contrail formation involves combustion, cooling and ice formation, which are good comprehensive learning exercise for physical chemistry students.

  6. Do Chemistry-Climate Models Project the Same Greenhouse Gas Chemistry if Initialized with Observations of the Trace Gases: A Pre-ATom Test

    NASA Astrophysics Data System (ADS)

    Flynn, C. M.; Prather, M. J.; Zhu, X.; Strode, S. A.; Steenrod, S. D.; Strahan, S. E.; Lamarque, J. F.; Fiore, A. M.; Horowitz, L. W.; Mao, J.; Murray, L. T.; Shindell, D. T.

    2016-12-01

    Experience with climate and chemistry model intercomparison projects (MIPs) has demonstrated a diversity in model projections for the chemical greenhouse gases CH4 and O3, even when forced by the same emissions. In general, the MIPs show that models diverge in the distribution of the many key trace species that control the reactivity of the troposphere (defined here as the loss of CH4 and the production and loss of O3). Two possible sources of model differences are the chemistry-transport coupling that creates the pattern of the essential precursor species, and the calculation of reactivity. Suppose that observations, such as those planned by NASA's Atmospheric Tomography (ATom) mission, provide us with enough of a chemical climatology to constrain the modeled distribution of the essential chemical species for the current epoch. Would the models calculate the same reactivity? ATom uses the DC-8 to make in situ measurements slicing through the middle of the Pacific and Atlantic Ocean basins each season and measuring the essential trace species. Unfortunately, ATom measurements will not be available until mid-2017. Here we take the baseline chemistry from one model version (as pseudo-observations) and use it to initialize 6 other global chemistry models. In this pre-ATom MIP, we take the full chemical composition for meridional slices centered on the Dateline (UC Irvine Chemistry-Transport Model, 0.6 deg resolution, 30 layers in the troposphere). We use grid cells between 0.5 and 12 km from 60 S to 60 N to initialize grid cells in the other six models (GEOS-Chem, GFDL-AM3, GISS ModelE2, GSFC GMI, NCAR, UCI CTM). The models are then integrated for 1 day and the key chemical rates (CH4, O3) are saved. These simulations assume that the initialized parcels remain unmixed over the 24 hours, and, hence, model-to-model variations will be due to differences in photochemistry, including clouds. In addition, we assess the relative importance of the precursor species by running

  7. Fingerprint of the atmospheric deposition on the biogeochemical functioning in the Mediterranean Sea - Evolution since the preindustrial era and projections

    NASA Astrophysics Data System (ADS)

    Christodoulaki, Sylvia; Petihakis, George; Mihalopoulos, Nikolaos; Tsiaras, Kostas; Triantafyllou, George; Kanakidou, Maria

    2017-04-01

    The atmospheric deposition of trace elements in the marine environment plays a major role in low-nutrient low-chlorophyll (LNLC) regions, such as the Mediterranean Sea. Particularly the deposition of nitrogen (mainly nitrate and ammonium) and phosphorous (phosphate) represents an important source of essential nutrients for the growth of phytoplankton and bacteria, enhancing the marine productivity in these oligotrophic areas. In this study we investigate how the increase in atmospheric deposition of N over the past 1.5 century, together with a smaller increase in atmospheric P deposition onto the surface seawater, affected the nutrient stoichiometry and the marine ecosystem in the Eastern Mediterranean Sea and how this impact will change in the near future. To this end, and in order to understand the atmospheric and marine processes that regulate the effects of atmospheric deposition in the marine ecosystem and the N/P ratio as well as its temporal evolution in the Eastern Mediterranean, a 1-D coupled physical- biogeochemical model is used. The model is forced by observations of atmospheric deposition fluxes at Crete, while for the hindcast (1860) and forecast (2030) simulations, the changes in atmospheric deposition calculated by global chemistry- transport models are applied to the present-day observed fluxes. Then, a coupled 3-D hydrodynamic/biogeochemical model that is currently operational within the POSEIDON forecast system, forced by the TM4-ECPL global atmospheric chemistry transport model, is implemented at Mediterranean basin scale. Both the 1D and the 3D models show that the atmospheric deposition of N and P is capable of explaining the observed west-to-east gradient of N/P ratio in the sea. Impacts of atmospheric deposition of N and P on the marine carbon and nutrients cycles are investigated and discussed. This work has been supported by Thales - ADAMANT project (ESF - NSRF 2007- 2013).

  8. Development and application of the High resolution VOC Atmospheric Chemistry in Canopies (Hi-VACC) model

    NASA Astrophysics Data System (ADS)

    Kenny, W.; Bohrer, G.; Chatziefstratiou, E.

    2013-12-01

    We have been working to develop a new post-processing model - High resolution VOC Atmospheric Chemistry in Canopies (Hi-VACC) - which will be able to resolve the dispersion and chemistry of reacting chemical species given their emission rates from the vegetation and soil, driven by high resolution meteorological forcing and wind fields from various high resolution atmospheric regional and large-eddy simulations. Hi-VACC reads in fields of pressure, temperature, humidity, air density, short-wave radiation, wind (3-D u, v and w components) and sub-grid-scale turbulence that were simulated by a high resolution atmospheric model. This meteorological forcing data is provided as snapshots of 3-D fields. Presently, the advection-diffusion portion of the model is fully developed, and we have tested it using a number of RAMS-based Forest Large Eddy Simulation (RAFLES) runs. Here, we present results from utilizing Hi-VACC in a few different contexts where it performs smoke and particle dispersion well. These include simulations of smoke dispersion from a theoretical forest fire in a domain in The Pine Barrens in New Jersey, as well as simulations to test the effects of heat flux on a scalar plume dispersing over a vegetative windbreak in an agricultural setting. Additional, we show initial results from testing the coupled chemistry component of Hi-VACC. One of the primary benefits of Hi-VACC is that users of other models can utilize this tool with only minimal work on their part -- processing their output fields into the appropriate HI-VACC input format. We have developed our model such that for whatever atmospheric model is being used with it, a MATLAB function must be written to extract the necessary information from the output files of that model and shape it into the proper format. This is the only model-specific work required. As such, this sort of smoke dispersion modeling performed by Hi-VACC - as well as its other capabilities - can be easily performed in other

  9. UARS Measurements and their Relationship to Atmospheric Chemistry and Climate Issues

    NASA Astrophysics Data System (ADS)

    Russell, J. M.; Jackman, C. H.; Anderson, J.

    2001-12-01

    The Upper Atmosphere Research Satellite (UARS) was launched by the Space Shuttle Discovery at 7:11:04 on September 12, 1991 and after boosting, finally reaching a 585 km, 57o inclined orbit. The satellite hosts ten experiments focused on a range of atmospheric phenomena including chemistry, dynamics, solar coupling with the atmosphere and energetic particle effects. The satellite provided an explosion of new information about the middle atmosphere and began the process of characterizing the low stratosphere and the mid to upper troposphere; both regions being vital to climate research studies. UARS experiments confirmed the role of CFCs in O3 depletion, clarified chemical process responsible for the Antarctic ozone hole, identified chemical O3 destruction in the Arctic region and shed new light on the role of dynamics as it affects latitude regions equaterward of the polar vortex. It also provided the first global measurements of HCl, HF, ClO, ClONO2 and N2O5 simultaneous with other key constituents including O3 itself, H2O, CH4, NO, NO2, HNO3, N2O, CF2Cl3, CFCl3, CO, aerosols and Polar Mesospheric Clouds. The long life of the mission has provided extended time series of key constituents and yielded remarkable and provocative results that leave many unanswered questions regarding atmospheric phenomena. We discuss some of the chemistry and climate issues addressed by UARS in this paper and summarize findings. The ten-year chlorine record shows increases on altitude surfaces since the beginning of 2000 that are not understood; but on CH4 surfaces a clear leveling off of the pre-Montreal Protocol increase in accord with protocol predictions has occurred. The long-term fluorine record is consistent with the protocol on an altitude surface. UARS also provided important data on mid to upper troposphere H2O both in the form of vertical profiles and in altitude regions clearly showing the effect of the El Niño and correlations with sea surface temperature. We will

  10. Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere

    NASA Astrophysics Data System (ADS)

    Kroll, Jesse H.; Seinfeld, John H.

    2008-05-01

    Secondary organic aerosol (SOA), particulate matter composed of compounds formed from the atmospheric transformation of organic species, accounts for a substantial fraction of tropospheric aerosol. The formation of low-volatility (semivolatile and possibly nonvolatile) compounds that make up SOA is governed by a complex series of reactions of a large number of organic species, so the experimental characterization and theoretical description of SOA formation presents a substantial challenge. In this review we outline what is known about the chemistry of formation and continuing transformation of low-volatility species in the atmosphere. The primary focus is chemical processes that can change the volatility of organic compounds: (1) oxidation reactions in the gas phase, (2) reactions in the particle phase, and (3) continuing chemistry (in either phase) over several generations. Gas-phase oxidation reactions can reduce volatility by the addition of polar functional groups or increase it by the cleavage of carbon-carbon bonds; key branch points that control volatility are the initial attack of the oxidant, reactions of alkylperoxy (RO2) radicals, and reactions of alkoxy (RO) radicals. Reactions in the particle phase include oxidation reactions as well as accretion reactions, non-oxidative processes leading to the formation of high-molecular-weight species. Organic carbon in the atmosphere is continually subject to reactions in the gas and particle phases throughout its atmospheric lifetime (until lost by physical deposition or oxidized to CO or CO2), implying continual changes in volatility over the timescales of several days. The volatility changes arising from these chemical reactions must be parameterized and included in models in order to gain a quantitative and predictive understanding of SOA formation.

  11. Analysis of atmospheric methane from Siberian tower observation using chemistry transport model

    NASA Astrophysics Data System (ADS)

    Ishijima, K.; Sasakawa, M.; Machida, T.; Patra, P. K.; Ito, A.; Ghosh, A.; Morimoto, S.; Aoki, S.; Nakazawa, T.

    2014-12-01

    Atmospheric methane (CH4) is the second greenhouse gas, which is originally a natural atmospheric component, but the amount in the atmosphere has been dramatically increased due to addition of various anthropogenic sources especially after industrialization triggered in 18th century. Such coexistence of both natural and anthropogenic sources at the present make it difficult to quantitatively understand CH4 cycles on the globe. For example, CH4 concentration was increasing in 1990s, became stable in 2000s, and began to increase again from 2007, but discussions on what caused such intriguing long-term variations remain inconclusive. On the other hand, it is well known that wetlands is the largest natural source of CH4. Of them, wetlands in Arctic regions have been recently receiving remarkable attention, because high-latitude regions are more sensitive to global warming than low-latitudes, possibly enhancing CH4 emissions there. In West Siberia, there are large wetland areas significantly contributing to the global CH4 budget. In order to monitor atmospheric CH4 variability, which strongly reflects CH4 emissions from surrounding wetlands, continuous measurements of CH4 concentration from an expanding network of towers (JR-STATION: Japan-Russia Siberian Tall Tower Inland Observation Network) have been conducted mainly in West Siberia since 2004. A previous study on the measurements has revealed that CH4 concentration has large diurnal and seasonal variability, which are driven by seasonally varying wetland and fossil fuel emissions as well as by significant diurnal and seasonal variations of planetary boundary layer height (PBLH). While chemistry transport model can be a useful tool to understand atmospheric CH4 variations in many cases, model simulation for the JR-STATION seems to be slightly challenging, since it is well known that present transport models' capability to reproduce PBLH is not enough. In this study, we validate model transport of the CCSR

  12. Studies in photochemical smog chemistry. I. Atmospheric chemistry of toluene. II. Analysis of chemical reaction mechanisms for photochemical smog

    SciTech Connect

    Leone, J.A.

    1985-01-01

    This study focuses on two related topics in the gas phase organic chemistry of importance in urban air pollution. Part I describes an experimental and modeling effort aimed at developing a new explicit reaction mechanism for the atmospheric photooxidation of toluene. This mechanism is tested using experimental data from both indoor and outdoor smog chamber facilities. The predictions of the new reaction mechanism are found to be in good agreement with both sets of experimental data. Additional simulations performed with the new mechanism are used to investigate various mechanistic paths, and to gain insight into areas where the understanding is not complete. The outdoor experimental facility, which was built to provide the second set of experimental data, consists of a 65 cubic meter teflon smog chamber together with full instrumentation capable of measuring ozone, nitrogen dioxide, nitric oxide, peroxyacetyl nitrate (PAN), carbon monoxide, relative humidity, temperature, aerosol size distributions, and of course toluene and its photooxidation products. In Part II, a theoretical analysis of lumped chemical reaction mechanisms for photochemical smog is presented. Included is a description of a new counter species analysis technique which can be used to analyze any complex chemical reaction mechanism. Finally, a new lumped mechanism for photochemical smog is developed and tested against experimental data from two smog chamber facilities. Advantages of this mechanism relative to the existing lumped mechanisms are discussed.

  13. Non-OH chemistry in oxidation flow reactors for the study of atmospheric chemistry systematically examined by modeling

    NASA Astrophysics Data System (ADS)

    Peng, Zhe; Day, Douglas A.; Ortega, Amber M.; Palm, Brett B.; Hu, Weiwei; Stark, Harald; Li, Rui; Tsigaridis, Kostas; Brune, William H.; Jimenez, Jose L.

    2016-04-01

    Oxidation flow reactors (OFRs) using low-pressure Hg lamp emission at 185 and 254 nm produce OH radicals efficiently and are widely used in atmospheric chemistry and other fields. However, knowledge of detailed OFR chemistry is limited, allowing speculation in the literature about whether some non-OH reactants, including several not relevant for tropospheric chemistry, may play an important role in these OFRs. These non-OH reactants are UV radiation, O(1D), O(3P), and O3. In this study, we investigate the relative importance of other reactants to OH for the fate of reactant species in OFR under a wide range of conditions via box modeling. The relative importance of non-OH species is less sensitive to UV light intensity than to water vapor mixing ratio (H2O) and external OH reactivity (OHRext), as both non-OH reactants and OH scale roughly proportionally to UV intensity. We show that for field studies in forested regions and also the urban area of Los Angeles, reactants of atmospheric interest are predominantly consumed by OH. We find that O(1D), O(3P), and O3 have relative contributions to volatile organic compound (VOC) consumption that are similar or lower than in the troposphere. The impact of O atoms can be neglected under most conditions in both OFR and troposphere. We define "riskier OFR conditions" as those with either low H2O (< 0.1 %) or high OHRext ( ≥ 100 s-1 in OFR185 and > 200 s-1 in OFR254). We strongly suggest avoiding such conditions as the importance of non-OH reactants can be substantial for the most sensitive species, although OH may still dominate under some riskier conditions, depending on the species present. Photolysis at non-tropospheric wavelengths (185 and 254 nm) may play a significant (> 20 %) role in the degradation of some aromatics, as well as some oxidation intermediates, under riskier reactor conditions, if the quantum yields are high. Under riskier conditions, some biogenics can have substantial destructions by O3, similarly to

  14. Non-OH chemistry in oxidation flow reactors for the study of atmospheric chemistry systematically examined by modeling

    DOE PAGES

    Peng, Zhe; Day, Douglas A.; Ortega, Amber M.; ...

    2016-04-06

    Oxidation flow reactors (OFRs) using low-pressure Hg lamp emission at 185 and 254 nm produce OH radicals efficiently and are widely used in atmospheric chemistry and other fields. However, knowledge of detailed OFR chemistry is limited, allowing speculation in the literature about whether some non-OH reactants, including several not relevant for tropospheric chemistry, may play an important role in these OFRs. These non-OH reactants are UV radiation, O(1D), O(3P), and O3. In this study, we investigate the relative importance of other reactants to OH for the fate of reactant species in OFR under a wide range of conditions via box modeling.more » The relative importance of non-OH species is less sensitive to UV light intensity than to water vapor mixing ratio (H2O) and external OH reactivity (OHRext), as both non-OH reactants and OH scale roughly proportionally to UV intensity. We show that for field studies in forested regions and also the urban area of Los Angeles, reactants of atmospheric interest are predominantly consumed by OH. We find that O(1D), O(3P), and O3 have relative contributions to volatile organic compound (VOC) consumption that are similar or lower than in the troposphere. The impact of O atoms can be neglected under most conditions in both OFR and troposphere. We define “riskier OFR conditions” as those with either low H2O (< 0.1%) or high OHRext (≥ 100s–1 in OFR185 and > 200s–1 in OFR254). We strongly suggest avoiding such conditions as the importance of non-OH reactants can be substantial for the most sensitive species, although OH may still dominate under some riskier conditions, depending on the species present. Photolysis at non-tropospheric wavelengths (185 and 254 nm) may play a significant (> 20%) role in the degradation of some aromatics, as well as some oxidation intermediates, under riskier reactor conditions, if the quantum yields are high. Under riskier conditions, some biogenics can have substantial destructions by O3

  15. SIOUX project: a simultaneous multiband camera for exoplanet atmospheres studies

    NASA Astrophysics Data System (ADS)

    Christille, Jean Marc; Bonomo, Aldo Stefano; Borsa, Francesco; Busonero, Deborah; Calcidese, Paolo; Claudi, Riccardo; Damasso, Mario; Giacobbe, Paolo; Molinari, Emilio; Pace, Emanuele; Riva, Alberto; Sozzetti, Alesandro; Toso, Giorgio; Tresoldi, Daniela

    2016-08-01

    The exoplanet revolution is well underway. The last decade has seen order-of-magnitude increases in the number of known planets beyond the Solar system. Detailed characterization of exoplanetary atmospheres provide the best means for distinguishing the makeup of their outer layers, and the only hope for understanding the interplay between initial composition chemistry, temperature-pressure atmospheric profiles, dynamics and circulation. While pioneering work on the observational side has produced the first important detections of atmospheric molecules for the class of transiting exoplanets, important limitations are still present due to the lack of systematic, repeated measurements with optimized instrumentation at both visible (VIS) and near-infrared (NIR) wavelengths. It is thus of fundamental importance to explore quantitatively possible avenues for improvements. In this paper we report initial results of a feasibility study for the prototype of a versatile multi-band imaging system for very high-precision differential photometry that exploits the choice of specifically selected narrow-band filters and novel ideas for the execution of simultaneous VIS and NIR measurements. Starting from the fundamental system requirements driven by the science case at hand, we describe a set of three opto-mechanical solutions for the instrument prototype: 1) a radial distribution of the optical flux using dichroic filters for the wavelength separation and narrow-band filters or liquid crystal filters for the observations; 2) a tree distribution of the optical flux (implying 2 separate foci), with the same technique used for the beam separation and filtering; 3) an 'exotic' solution consisting of the study of a complete optical system (i.e. a brand new telescope) that exploits the chromatic errors of a reflecting surface for directing the different wavelengths at different foci. In this paper we present the first results of the study phase for the three solutions, as well as the

  16. Isotopic links between atmospheric chemistry and the deep sulphur cycle on Mars.

    PubMed

    Franz, Heather B; Kim, Sang-Tae; Farquhar, James; Day, James M D; Economos, Rita C; McKeegan, Kevin D; Schmitt, Axel K; Irving, Anthony J; Hoek, Joost; Dottin, James

    2014-04-17

    The geochemistry of Martian meteorites provides a wealth of information about the solid planet and the surface and atmospheric processes that occurred on Mars. The degree to which Martian magmas may have assimilated crustal material, thus altering the geochemical signatures acquired from their mantle sources, is unclear. This issue features prominently in efforts to understand whether the source of light rare-earth elements in enriched shergottites lies in crustal material incorporated into melts or in mixing between enriched and depleted mantle reservoirs. Sulphur isotope systematics offer insight into some aspects of crustal assimilation. The presence of igneous sulphides in Martian meteorites with sulphur isotope signatures indicative of mass-independent fractionation suggests the assimilation of sulphur both during passage of magmas through the crust of Mars and at sites of emplacement. Here we report isotopic analyses of 40 Martian meteorites that represent more than half of the distinct known Martian meteorites, including 30 shergottites (28 plus 2 pairs, where pairs are separate fragments of a single meteorite), 8 nakhlites (5 plus 3 pairs), Allan Hills 84001 and Chassigny. Our data provide strong evidence that assimilation of sulphur into Martian magmas was a common occurrence throughout much of the planet's history. The signature of mass-independent fractionation observed also indicates that the atmospheric imprint of photochemical processing preserved in Martian meteoritic sulphide and sulphate is distinct from that observed in terrestrial analogues, suggesting fundamental differences between the dominant sulphur chemistry in the atmosphere of Mars and that in the atmosphere of Earth.

  17. Maillard Chemistry in Clouds and Aqueous Aerosol As a Source of Atmospheric Humic-Like Substances.

    PubMed

    Hawkins, Lelia N; Lemire, Amanda N; Galloway, Melissa M; Corrigan, Ashley L; Turley, Jacob J; Espelien, Brenna M; De Haan, David O

    2016-07-19

    The reported optical, physical, and chemical properties of aqueous Maillard reaction mixtures of small aldehydes (glyoxal, methylglyoxal, and glycolaldehyde) with ammonium sulfate and amines are compared with those of aqueous extracts of ambient aerosol (water-soluble organic carbon, WSOC) and the humic-like substances (HULIS) fraction of WSOC. Using a combination of new and previously published measurements, we examine fluorescence, X-ray absorbance, UV/vis, and IR spectra, complex refractive indices, (1)H and (13)C NMR spectra, thermograms, aerosol and electrospray ionization mass spectra, surface activity, and hygroscopicity. Atmospheric WSOC and HULIS encompass a range of properties, but in almost every case aqueous aldehyde-amine reaction mixtures are squarely within this range. Notable exceptions are the higher UV/visible absorbance wavelength dependence (Angström coefficients) observed for methylglyoxal reaction mixtures, the lack of surface activity of glyoxal reaction mixtures, and the higher N/C ratios of aldehyde-amine reaction products relative to atmospheric WSOC and HULIS extracts. The overall optical, physical, and chemical similarities are consistent with, but not demonstrative of, Maillard chemistry being a significant secondary source of atmospheric HULIS. However, the higher N/C ratios of aldehyde-amine reaction products limits the source strength to ≤50% of atmospheric HULIS, assuming that other sources of HULIS incorporate only negligible quantities of nitrogen.

  18. Lumping, testing, tuning: The invention of an artificial chemistry in atmospheric transport modeling

    NASA Astrophysics Data System (ADS)

    Heymann, Matthias

    Since the late 1950s computer simulation has been used to investigate the transport of pollutants in the atmosphere. About 20 years later also the chemical transformation of atmospheric pollutants was included in computer models of photochemical smog formation. Due to limited knowledge of atmospheric chemistry and due to limited computer capacity, chemical processes in the atmosphere were modeled with the help of simplified chemical models. In these models chemical substances are lumped together forming artificial virtual compounds with virtual characteristics. The paper aims at studying the practices developed in chemical model building and the creation of confidence in these models. Core of the paper will be the analysis of the Urban Airshed Model (UAM) for the Los Angeles region, a pioneering development in the early 1970s. The construction of the UAM involved the "lumping" of chemical processes and extensive testing and tuning. These practices led to a consistent model representation, in which diverse pieces of information fitted and were mutually stabilized. The pragmatic achievement of consistency created confidence, even though empirical tests of the models remained ambiguous and problematic.

  19. Investigating the Chemical Pathways to PAH- and PANH-Based Aerosols in Titan's Atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Sciamma-O'Brien, Ella Marion; Contreras, Cesar; Ricketts, Claire Louise; Salama, Farid

    2011-01-01

    A complex organic chemistry between Titan's two main constituents, N2 and CH4, leads to the production of more complex molecules and subsequently to solid organic aerosols. These aerosols are at the origin of the haze layers giving Titan its characteristic orange color. In situ measurements by the Ion Neutral Mass Spectrometer (INMS) and Cassini Plasma Spectrometer (CAPS) instruments onboard Cassini have revealed the presence of large amounts of neutral, positively and negatively charged heavy molecules in the ionosphere of Titan. In particular, benzene (C6H6) and toluene (C6H5CH3), which are critical precursors of polycyclic aromatic hydrocarbon (PAH) compounds, have been detected, suggesting that PAHs might play a role in the production of Titan s aerosols. Moreover, results from numerical models as well as laboratory simulations of Titan s atmospheric chemistry are also suggesting chemical pathways that link the simple precursor molecules resulting from the first steps of the N2-CH4 chemistry (C2H2, C2H4, HCN ...) to benzene, and to PAHs and nitrogen-containing PAHs (or PANHs) as precursors to the production of solid aerosols.

  20. Geochemical cycles of atmospheric gases

    NASA Technical Reports Server (NTRS)

    Walker, J. C. G.; Drever, J. I.

    1988-01-01

    The processes that control the atmosphere and atmospheric changes are reviewed. The geochemical cycles of water vapor, nitrogen, carbon dioxide, oxygen, and minor atmospheric constituents are examined. Changes in atmospheric chemistry with time are discussed using evidence from the rock record and analysis of the present atmosphere. The role of biological evolution in the history of the atmosphere and projected changes in the future atmosphere are considered.

  1. Geochemical cycles of atmospheric gases

    NASA Technical Reports Server (NTRS)

    Walker, J. C. G.; Drever, J. I.

    1988-01-01

    The processes that control the atmosphere and atmospheric changes are reviewed. The geochemical cycles of water vapor, nitrogen, carbon dioxide, oxygen, and minor atmospheric constituents are examined. Changes in atmospheric chemistry with time are discussed using evidence from the rock record and analysis of the present atmosphere. The role of biological evolution in the history of the atmosphere and projected changes in the future atmosphere are considered.

  2. Comparative Experimental Investigation of Titan's Atmospheric Chemistry Driven by Solar EUV Radiation and Energetic Electron Precipitation

    NASA Astrophysics Data System (ADS)

    Imanaka, Hiroshi; Lavvas, P.; Yelle, R. V.; Smith, M. A.

    2010-10-01

    The observations by the Cassini Ion Neutral Mass Spectrometer (INMS) and the Cassini Plasma Spectrometer (CAPS) clearly demonstrate the importance of complex organic chemistry in the upper atmosphere of Titan; a complex coupling of neutral and ion chemistry for organic aerosol generation induced by EUV photons and Saturn's magnetospheric charged particles. To understand the dominant energy source for aerosol formation and its formation chemistry, we comparatively investigate the chemical mechanism in N2/CH4 gas mixtures resulting from EUV-VUV synchrotron radiation (50-150 nm) and tunable mono-energetic electron beam irradiation (5 eV - 2000 eV). These excitation energy sources cover the dominant energy source available in Titan's upper atmosphere. Our previous study of the EUV-VUV photolysis of N2/CH4 gas mixtures revealed the unique role of nitrogen photoionization in the catalytic formation of complex hydrocarbons and in the major nitrogen fixation process in Titan's upper atmosphere (Imanaka and Smith, 2007, 2009, 2010). However, relative roles of ion-molecule reactions and radical/neutral reactions in such complex chemistry remain to be determined. We characterized the electron energy distribution by conducting the Langmuir probe measurements. Degradation of the primary photoelectron from N2 photoionization at 20.6 eV photons is clearly observed, and the electron density rapidly decreases down to 109-10 cm-3, which suggests the complex coupling of ion-molecular reactions and dissociative ion-electron recombination reactions for the observed development of complex organic molecules. The electron beam irradiation experiments at energy larger than 200 eV shows distinct gaseous product distribution with nitrogenated gaseous species from those with EUV irradiation products. The generation of secondary electrons and multiple inelastic collisions of fast electrons might increases the nitrogen fixation efficiency. The much less stringent spin selection rules could

  3. Constraining the Sources and Sinks of Atmospheric Methane Using Stable Isotope Observations and Chemistry Climate Modeling

    NASA Astrophysics Data System (ADS)

    Feinberg, A.; Coulon, A.; Stenke, A.; Peter, T.

    2015-12-01

    Methane acts as both a greenhouse gas and a driver of atmospheric chemistry. There is a lack of consensus for the explanation behind the atmospheric methane trend in recent years (1980-2010). High uncertainties are associated with the magnitudes of individual methane source and sink processes. Methane isotopes have the potential to distinguish between the different methane fluxes, as each flux is characterized by an isotopic signature. Methane emissions from each source category are expressed explicitly in a chemistry climate model SOCOL, including wetlands, rice paddies, biomass burning, industry, etc. The model includes 48 methane tracers based on source type and geographical origin in order to track methane after it has been emitted. SOCOL simulations for the years 1980-2010 are performed in "nudged mode", so that model dynamics reflect observed meteorology. Available database estimates of the various surface emission fluxes are inputted into SOCOL. The model diagnostic methane tracers are compared to methane isotope observations from measurement networks. Inconsistencies between the model results and observations point to deficiencies in the available emission estimates or model sink processes. Because of their dependence on the OH sink, deuterated methane observations and methyl chloroform tracers are used to investigate the variability of OH mixing ratios in the model and the real world. The analysis examines the validity of the methane source and sink category estimates over the last 30 years.

  4. Atmospheric Chemistry of the Carbon Capture Solvent Monoethanolamine (MEA): A Theoretical Study

    NASA Astrophysics Data System (ADS)

    da Silva, G.

    2012-12-01

    The development of amine solvent technology for carbon capture and storage has the potential to create large new sources of amines to the atmosphere. The atmospheric chemistry of amines generally, and carbon capture solvents in particular, is not well understood. We have used quantum chemistry and master equation modelling to investigate the OH radical initiated oxidation of monoethanolamine (NH2CH2CH2OH), or MEA, the archetypal carbon capture solvent. The OH radical can abstract H atoms from either carbon atom in MEA, with negative reaction barriers. Treating these reactions with a two transition state model can reliably reproduce experimental rate constants and their temperature dependence. The products of the MEA + OH reaction, the NH2CHCH2OH and NH2CH2CHOH radicals, undergo subsequent reaction with O2, which has also been studied. In both cases chemically activated reactions that bypass peroxyl radical intermediates dominate, producing 2-iminoethanol + HO2 (from NH2CHCH2OH) or aminoacetaldehyde + HO2 (from NH2CH2CHOH), making the process HOx-neutral. The operation of chemically activated reaction mechanisms has implications for the ozone forming potential of MEA. The products of MEA photo-oxidation are proposed as important species in the formation of both organic and inorganic secondary aerosols, particularly through uptake of the imine 2-iminoethanol and subsequent hydrolysis to ammonia and glycolaldehyde.

  5. ASIS v1.0: an adaptive solver for the simulation of atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Cariolle, Daniel; Moinat, Philippe; Teyssèdre, Hubert; Giraud, Luc; Josse, Béatrice; Lefèvre, Franck

    2017-04-01

    This article reports on the development and tests of the adaptive semi-implicit scheme (ASIS) solver for the simulation of atmospheric chemistry. To solve the ordinary differential equation systems associated with the time evolution of the species concentrations, ASIS adopts a one-step linearized implicit scheme with specific treatments of the Jacobian of the chemical fluxes. It conserves mass and has a time-stepping module to control the accuracy of the numerical solution. In idealized box-model simulations, ASIS gives results similar to the higher-order implicit schemes derived from the Rosenbrock's and Gear's methods and requires less computation and run time at the moderate precision required for atmospheric applications. When implemented in the MOCAGE chemical transport model and the Laboratoire de Météorologie Dynamique Mars general circulation model, the ASIS solver performs well and reveals weaknesses and limitations of the original semi-implicit solvers used by these two models. ASIS can be easily adapted to various chemical schemes and further developments are foreseen to increase its computational efficiency, and to include the computation of the concentrations of the species in aqueous-phase in addition to gas-phase chemistry.

  6. Upper Atmosphere Sounding Rocket Projects at Esrange Space Center

    NASA Astrophysics Data System (ADS)

    Lockowandt, Christian; Kemi, Stig; Sjolander, Krister; Abrahamsson, Mattias

    Swedish Space Corporation, SSC has a long tradition of developing and launching scientific sounding rockets from Esrange Space Center with the aim to study the different layers of the atmosphere and near space. Now a new era has started with an initiative from the Swedish National Space Board, SNSB. The sounding rocket and atmospheric balloon activities will be vitalised with a national program offering the scientific community yearly rocket launches and balloon flights. The three upcoming sounding rocket missions that have recently started are: O-STATES O STATES (Oxygen transformation in the thermosphere) is a research project at the Meteorological Institute of Stockholm University with Prof. Jörg Gumbel, as responsible researcher. The payload comprises two instrument modules with totally 7 instruments for studying oxygen in its various forms. The payload will be launched twice on two sounding rockets at the same launch campaign, in different atmospheric conditions. This provides a cost-effective mission with a large research exchange. The launches from Esrange Space Center are preliminary scheduled to take place in August 2014 with an apogee of approximately 250 km. SPIDER SPIDER (Small Payloads for Investigation of Disturbances in Electrojet by Rockets) is a research project at Space and Plasma Physics, Royal Institute of Technology, Stockholm with Nicholay Ivchenko as responsible researcher. The mission includes up to 10 subsidiary payloads ejected from the main payload to measure the structure of the electrostatic turbulence in the ionosphere. The measurements take place entirely in the subsidiary payloads, which are completely autonomous and recovered individually after the flight. The launch from Esrange Space Center is preliminary scheduled to take place in March 2015 with a desired apogee of approximately 140 km. LEEWAVES LEEWAVES (Local Excitation and Effects of Waves on Atmospheric Vertical Structure) is a research project at the Meteorological

  7. Project of the URAN array for registration of atmospheric neutrons

    NASA Astrophysics Data System (ADS)

    Gromushkin, D. M.; Barbashina, N. S.; Bogdanov, F. A.; Kokoulin, R. P.; Ovchinnikov, V. V.; Petrukhin, A. A.; Stenkin, Yu V.; Khokhlov, S. S.; Shulzhenko, I. A.; Yashin, I. I.

    2016-02-01

    The project of a new setup is directed at the registration of atmospheric neutrons (URAN) generated by hadronic component of extensive air showers (EAS). The setup includes 72 en-detector which simultaneously register two major EAS components: electromagnetic by the group passage of charged particles and hadron component by the thermal neutrons. The neutrons and charged particles are detected using a specialized scintillation composition made of granulated alloy of crystals based on the ZnS(Ag) powder with an admixture of B2O3.

  8. Poster 6: Influence of traces elements in the organic chemistry of upper atmosphere of Titan

    NASA Astrophysics Data System (ADS)

    Mathe, Christophe; Carrasco, Nathalie; Trainer, Melissa G.; Gautier, Thomas; Gavilan, Lisseth; Dubois, David; Li, Xiang

    2016-06-01

    In the upper atmosphere of Titan, complex chemistry leads to the formation of organic aerosols. Since the work of Khare et al. in 1984, several experiments investigated the formation of Titan aerosols, so called tholins, in the laboratory. It has been suggested that nitrogen-containing compounds may contribute significantly to the aerosols formation process. In this study, we focused on the influence of pyridine, the simplest nitrogenous aromatic hydrocarbon, on the chemistry of Titan's atmosphere and on aerosol formation. To assess the effect of pyridine on aerosol formation chemistry, we used two different experimental setups : a capacitively coupled radio-frequency (electronic impact), and a VUV Deuterium lamp (photochemistry) in a collaboration between LATMOS (Guyancourt) and NASA-GSFC (Greenbelt), respectively. Aerosols produced with both setups were first analyzed using a FTIR-ATR (Fourier Transform Infrared spectroscopy - Attenuated Total Reflection) with a spectral range of 4000-800 cm-1 to characterize their optical properties. Next the samples were analysed using a Bruker Autoflex Speed MALDI mass spectrometer with a m/z range up to 2000 Da in order to infer their composition. Infrared spectroscopy analysis showed that tholins produced with a nitrogen-methane gas mixture (95:5) and nitrogenpyridine gas mixture (99:250ppm) present very similar spectra features. Tholins produced with a mixture of nitrogenmethane-pyridine (99:1:250ppm) do not present aliphatic CH2 or CH3 vibrational signatures. This could indicate a cyclic polymerization by a pyridine skeleton. Mass spectrometry is still in progress to confirm this.

  9. On the one-dimensional chemistry-diffusion model in planetary atmospheres

    NASA Astrophysics Data System (ADS)

    Zhang, Xi; Showman, Adam

    Most of the current atmospheric chemistry models for planets (e.g., Krasnopolsky & Parshev 1981; Yung et al., 1984; Lavvas et al., 2008) and exo-planets (e.g., Moses et al., 2011; Line et al., 2011; Hu et al., 2012) adopt a one-dimensional (1D) chemistry-diffusion approach in the vertical coordinate such as pressure or altitude. Although only a crude approximation, these 1D models have succeeded in explaining the global-averaged vertical profiles of many chemical species in observations. One of the important assumptions of these models is that, all chemical species are transported via the same eddy diffusion profile. Here we show that, as also noticed in the Earth community (e.g., Holton 1986), in the presence of horizontal transport driven by eddies in the middle atmospheres such as the stratospheres on Earth and Titan, this “homogenous eddy diffusion” assumption generally breaks down. Instead, the eddy diffusion should depend both on the horizontal eddy mixing and the chemical lifetime of the species. It implies that the long-lived species and short-lived species could have significantly different eddy diffusion profiles. We show analytically why this new approach is more physically based. We also show numerically why the old approach fails compared with the globally averaged results from a more realistic two-dimensional (2D) simulation using the state-of-art Caltech/JPL 2D chemistry-diffusion-advection model (Zhang et al., 2013), and discuss the possible consequences. This research was supported by the Bisgrove Scholar Program in the University of Arizona.

  10. Laboratory studies on N(2D) reactions of relevance to the chemistry of planetary atmospheres

    NASA Astrophysics Data System (ADS)

    Balucani, N.; Casavecchia, P.

    Molecular nitrogen is a very stable molecule, practically inert from a chemical point of view. For a nitrogen chemistry to occur in the planetary atmospheres which contain N2 , it is necessary to transform it into an active form, such as atoms or ions. As far as the production of atomic nitrogen in the upper atmospheres of planets (like Mars) or moons (like Titan) is concerned, several processes - as N2 dissociation induced by electron impact, EUV photolysis (λ <80 nm) and dissociative photoionization, or galactic cosmic ray absorption and N+ dissociative recombination all 2 lead to atomic nitrogen, notably in the ground, 4 S3/2 , and first electronically excited, 2 D3/2,5/2 , states with comparable yields. The radiative lifetimes of the metastable states 2 D3/2 and 2 D5/2 are quite long (12.3 and 48 hours, respectively), because the transition from a doublet to a quartet state is strongly forbidden. In addition, the physical quenching of N(2 D) is often a slow process and in some important cases the main fate of N(2 D) is chemical reaction with other constituents of the planetary atmospheres. The production of N atoms in the 2 D state is an important fact, because N(4 S) atoms exhibit very low reactivity with closed-shell molecules and the probability of collision with an open-shell radical is small. Unfortunately laboratory experiments on the gas-phase reactions of N(2 D) have been lacking until recently, because of serious experimental difficulties in studying these reactive systems. Accurate kinetic data on the reactions of N(2 D) with the some molecules of relevance to the chemistry of planetary atmospheres have finally become available in the late 90's, but a better knowledge of the reactive behavior requires a dynamical investigation of N(2 D) reactions. The capability of generating intense continuous beams of N(2 D) achieved in our laboratory some years ago has opened up the possibility of studying the reactive scattering of this species under single

  11. Update of the Black Dog atmospheric fluidized bed combustion project

    SciTech Connect

    Osthus, D.; Larva, J.; Rens, D. )

    1988-01-01

    Northern States Power Co. converted its Black Dog Unit 2, a pulverized coal-fired 100 MW unit that was built in 1954, to an atmospheric fluidized bed (bubbling bed) configuration, in order to commercially demonstrate AFBC technology as a cost-effective way to reduce SO2 emissions. As part of the AFBC conversion, the unit was upgraded to 130 MW capacity. Unit 2 burns Western coal, is equipped with electrostatic precipitators, and cycles on and off line daily. The innovative nature of this project contributed to a protracted encountered. These problems are discussed. Many of the problems have been solved, and the unit is now meeting most of the goals set for the project.

  12. The Middle Atmosphere Program: A special project for the Antarctic Middle Atmosphere (AMA)

    NASA Astrophysics Data System (ADS)

    Hirasawa, T.

    1982-04-01

    Areas of concern are: dynamics, structure, and atmospheric composition of the middle atmosphere in Antarctica; particle precipitation and interaction of the middle atmosphere with the lower ionosphere; atmospheric pollution; and the difference between the northern and southern polar middle atmosphere.

  13. The Middle Atmosphere Program: A special project for the Antarctic Middle Atmosphere (AMA)

    NASA Technical Reports Server (NTRS)

    Hirasawa, T.

    1982-01-01

    Areas of concern are: dynamics, structure, and atmospheric composition of the middle atmosphere in Antarctica; particle precipitation and interaction of the middle atmosphere with the lower ionosphere; atmospheric pollution; and the difference between the northern and southern polar middle atmosphere.

  14. Projections of atmospheric mercury levels and their effect on air quality in the United States

    NASA Astrophysics Data System (ADS)

    Lei, H.; Wuebbles, D. J.; Liang, X.-Z.; Tao, Z.; Olsen, S.; Artz, R.; Ren, X.; Cohen, M.

    2014-01-01

    The individual and combined effects of global climate change and emissions changes from 2000 to 2050 on atmospheric mercury levels in the United States are investigated by using the global climate-chemistry model, CAM-Chem, coupled with a mercury chemistry-physics mechanism (CAM-Chem/Hg). Three future pathways from the Intergovernmental Panel on Climate Change (IPCC) Special Report on Emissions Scenarios (SRES) are considered, with the A1FI, A1B and B1 scenarios representing the upper, middle and lower bounds of potential climate warming, respectively. The anthropogenic and biomass burning emissions of mercury are projected from the energy use assumptions in the IPCC SRES report. Natural emissions from both land and ocean sources are projected by using dynamic schemes. TGM concentration increases are greater in the low latitudes than they are in the high latitudes, indicative of a larger meridional gradient than in the present day. In the A1FI scenario, TGM concentrations in 2050 are projected to increase by 2.1-4.0 ng m-3 for the eastern US and 1.4-3.0 ng m-3 for the western US. This spatial difference corresponds to potential increases in wet deposition of 10-14 μg m-2 for the eastern US and 2-4 μg m-2 for the western US. The increase in Hg(II) emissions tends to enhance wet deposition and hence increase the risk of higher mercury entering the hydrological cycle and ecosystem. In the B1 scenario, mercury concentrations in 2050 are similar to present level concentrations; this finding indicates that the domestic reduction in mercury emissions is essentially counteracted by the effects of climate warming and emissions increases in other regions. The sensitivity analyses show that changes in anthropogenic emissions contribute 32-53% of projected changes in mercury air concentration, while the independent contribution by climate change and its induced natural emissions change accounts for 47-68%.

  15. Fire risk, atmospheric chemistry and radiative forcing assessment of wildfires in eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Athanasopoulou, E.; Rieger, D.; Walter, C.; Vogel, H.; Karali, A.; Hatzaki, M.; Gerasopoulos, E.; Vogel, B.; Giannakopoulos, C.; Gratsea, M.; Roussos, A.

    2014-10-01

    The current research study aims at investigating the atmospheric implications of a major fire event in the Mediterranean area. For this purpose, a regional aerosol model coupled online with meteorology (COSMO-ART) is applied over Greece during late summer 2007. Fire risk model results proved to be adequate in reproducing the highly destructive event, which supports further applications for national meteorological forecasts and early warning systems for fire prevention. Columnar aerosol loading field predictions are consistent with satellite maps, which further allows for the correlation of this wildfire event to the atmospheric chemistry and the radiative forcing. Gaseous chemistry resembles that in urban environments and led to nitrogen dioxide and ozone exceedances in several cities in proximity to and downwind the fire spots, respectively. Influence in Athens is found significant from the Euboean plume (45% of total surface PM10) and small (5%) from the fires in Peloponnese. Fire events are indicated by sharp increases in organic to elemental carbon (6), together with sharp decreases in secondary to total organic components (0.1), in comparison to their values during the pre- and post-fire period over Athens (1 and 0.6, respectively). The change in the radiative budget induced by the fire plume is found negative (3-day-average value up to -10 W m-2). Direct heat input is found negligible, thus the net temperature effect is also negative over land (-0.5 K). Nevertheless, positive temperature changes are found overseas (hourly value up to +2 K), due to the amplified radiation absorption by aged soot, coupled to the intense stabilization of the atmosphere above the sea surface.

  16. Evaluation of the atmospheric chemistry general circulation model ECHAM5/MESSy1

    NASA Astrophysics Data System (ADS)

    Joeckel, P.; Tost, H.; Pozzer, A.; Bruehl, C.; Buchholz, J.; Ganzeveld, L.; Hoor, P.; Kerkweg, A.; Lawrence, M. G.; Metzger, S.; Sander, R.; Steil, B.; Stiller, G.; Tanarhte, M.; Taraborrelli, D.; van Aardenne, J.; Lelieveld, J.

    2006-12-01

    We present the new Modular Earth Submodel System (MESSy) coupled to the 5th generation European Centre Hamburg GCM, ECHAM5. MESSy describes atmospheric chemistry and meteorological processes in a modular framework, following strict coding standards. This approach is chosen to face the challenges associated with increasing model complexity. The resulting model system is portable, user-friendly and easily expandable. The system enables the testing of different modules of the same processes (e.g. convection) under otherwise identical numerical conditions. In a first model evaluation simulation we apply a 90-layer model setup up to 0.01 hPa at T42 spectral resolution to simulate the dynamics and chemistry, both coupled via radiation, of the lower and middle atmosphere. A Newtonian relaxation technique was applied in the troposphere to weakly nudge the model towards the analysed (ECMWF) meteorology during the period 1998-2005. This technique allows a direct comparison of model results with observations. It is shown that the tropospheric wave forcing of the stratosphere in the model suffices to reproduce the Quasi- Biennial Oscillation and major stratospheric warming events leading e.g. to the vortex split over Antarctica in 2002. The model realistically simulates stratosphere-troposphere exchange processes as shown by comparisons with satellite and in situ measurements. The main characteristics of the trace gas distributions are reproduced well. In summary, the model consistently simulates the state of the atmosphere from the surface to the mesosphere without the need to prescribe artifical boundary conditions, e.g., such as ozone at the tropopause.

  17. Observed variations of methane on Mars unexplained by known atmospheric chemistry and physics.

    PubMed

    Lefèvre, Franck; Forget, François

    2009-08-06

    The detection of methane on Mars has revived the possibility of past or extant life on this planet, despite the fact that an abiogenic origin is thought to be equally plausible. An intriguing aspect of the recent observations of methane on Mars is that methane concentrations appear to be locally enhanced and change with the seasons. However, methane has a photochemical lifetime of several centuries, and is therefore expected to have a spatially uniform distribution on the planet. Here we use a global climate model of Mars with coupled chemistry to examine the implications of the recently observed variations of Martian methane for our understanding of the chemistry of methane. We find that photochemistry as currently understood does not produce measurable variations in methane concentrations, even in the case of a current, local and episodic methane release. In contrast, we find that the condensation-sublimation cycle of Mars' carbon dioxide atmosphere can generate large-scale methane variations differing from those observed. In order to reproduce local methane enhancements similar to those recently reported, we show that an atmospheric lifetime of less than 200 days is necessary, even if a local source of methane is only active around the time of the observation itself. This implies an unidentified methane loss process that is 600 times faster than predicted by standard photochemistry. The existence of such a fast loss in the Martian atmosphere is difficult to reconcile with the observed distribution of other trace gas species. In the case of a destruction mechanism only active at the surface of Mars, destruction of methane must occur with an even shorter timescale of the order of approximately 1 hour to explain the observations. If recent observations of spatial and temporal variations of methane are confirmed, this would suggest an extraordinarily harsh environment for the survival of organics on the planet.

  18. National Atmospheric Deposition Program (NADP) Networks: Data on the chemistry of precipitation

    DOE Data Explorer

    The National Atmospheric Deposition Program/National Trends Network (NADP/NTN) is a nationwide network of sites collecting data on the chemistry of precipitation for monitoring of geographical and temporal long