WorldWideScience

Sample records for atmospheric chemistry

  1. Atmospheric chemistry and climate

    OpenAIRE

    Satheesh, SK

    2012-01-01

    Atmospheric chemistry is a branch of atmospheric science where major focus is the composition of the Earth's atmosphere. Knowledge of atmospheric composition is essential due to its interaction with (solar and terrestrial) radiation and interactions of atmospheric species (gaseous and particulate matter) with living organisms. Since atmospheric chemistry covers a vast range of topics, in this article the focus is on the chemistry of atmospheric aerosols with special emphasis on the Indian reg...

  2. Atmosphere physics and chemistry

    International Nuclear Information System (INIS)

    Delmas, R.; Megie, G.; Peuch, V.H.

    2005-10-01

    Since the 1970's, the awareness about the atmospheric pollution threat has led to a spectacular development of the researches on the complex interactions between the chemical composition of the atmosphere and the climate. This book makes a synthesis of the state-of-the-art in this very active domain of research. Content: introduction, atmosphere dynamics and transport, matter-radiation interaction and radiant transfer, physico-chemical processes, atmospheric aerosol and heterogenous chemistry, anthropic and natural emissions and deposition, stratospheric chemical system, tropospheric chemical system, polluted boundary layer, paleo-environments and ice archives, role of atmospheric chemistry in global changes, measurement principles and instruments, numerical modeling, experimental strategy, regulation and management of the atmospheric environment, index. (J.S.)

  3. Modeling the atmospheric chemistry of TICs

    Science.gov (United States)

    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.

  4. 1997 Atmospheric Chemistry Colloquium for Emerging Senior Scientists

    Energy Technology Data Exchange (ETDEWEB)

    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

  5. Atmospheric Chemistry Over Southern Africa

    Science.gov (United States)

    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

  6. Quantifying atmospheric transport, chemistry, and mixing using a new trajectory-box model and a global atmospheric-chemistry GCM

    Directory of Open Access Journals (Sweden)

    H. Riede

    2009-12-01

    Full Text Available We present a novel method for the quantification of transport, chemistry, and mixing along atmospheric trajectories based on a consistent model hierarchy. The hierarchy consists of the new atmospheric-chemistry trajectory-box model CAABA/MJT and the three-dimensional (3-D global ECHAM/MESSy atmospheric-chemistry (EMAC general circulation model. CAABA/MJT employs the atmospheric box model CAABA in a configuration using the atmospheric-chemistry submodel MECCA (M, the photochemistry submodel JVAL (J, and the new trajectory submodel TRAJECT (T, to simulate chemistry along atmospheric trajectories, which are provided offline. With the same chemistry submodels coupled to the 3-D EMAC model and consistent initial conditions and physical parameters, a unique consistency between the two models is achieved. Since only mixing processes within the 3-D model are excluded from the model consistency, comparisons of results from the two models allow to separate and quantify contributions of transport, chemistry, and mixing along the trajectory pathways. Consistency of transport between the trajectory-box model CAABA/MJT and the 3-D EMAC model is achieved via calculation of kinematic trajectories based on 3-D wind fields from EMAC using the trajectory model LAGRANTO. The combination of the trajectory-box model CAABA/MJT and the trajectory model LAGRANTO can be considered as a Lagrangian chemistry-transport model (CTM moving isolated air parcels. The procedure for obtaining the necessary statistical basis for the quantification method is described as well as the comprehensive diagnostics with respect to chemistry.

    The quantification method presented here allows to investigate the characteristics of transport, chemistry, and mixing in a grid-based 3-D model. The analysis of chemical processes within the trajectory-box model CAABA/MJT is easily extendable to include, for example, the impact of different transport pathways or of mixing processes onto

  7. (Chemistry of the global atmosphere)

    Energy Technology Data Exchange (ETDEWEB)

    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.

  8. Atmospheric Chemistry and Air Pollution

    Directory of Open Access Journals (Sweden)

    Jeffrey S. Gaffney

    2003-01-01

    Full Text Available 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.

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

    Science.gov (United States)

    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...

  10. Atmospheric chemistry and physics from air pollution to climate change

    CERN Document Server

    Seinfeld, John H

    2016-01-01

    Expanded and updated with new findings and new features Since the second edition of Seinfeld and Pandis’ classic textbook, significant progress has taken place in the field of atmospheric chemistry and physics, particularly in the areas of tropospheric chemistry, aerosols, and the science of climate change. A new edition of this comprehensive work has been developed by the renowned author team. Atmospheric Chemistry and Physics, 3rd Edition, as the previous two editions have done, provides a rigorous and comprehensive treatment of the chemistry and physics of the atmosphere – including the chemistry of the stratosphere and troposphere, aerosol physics and chemistry, atmospheric new particle formation, physical meteorology, cloud physics, global climate, statistical analysis of data, and mathematical chemical/transport models of the atmosphere. Each of these topics is covered in detail and in each area the central results are developed from first principles. In this way the reader gains a significant un...

  11. Organic chemistry in Titan's atmosphere

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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.

  13. Impact of Amazonian deforestation on atmospheric chemistry

    NARCIS (Netherlands)

    Ganzeveld, L.N.; Lelieveld, J.

    2004-01-01

    A single-column chemistry and climate model has been used to study the impact of deforestation in the Amazon Basin on atmospheric chemistry. Over deforested areas, daytime ozone deposition generally decreases strongly except when surface wetness decreases through reduced precipitation, whereas

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

    Directory of Open Access Journals (Sweden)

    A. Kerkweg

    2012-01-01

    Full Text Available 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.

  15. Data assimilation in atmospheric chemistry models: current status and future prospects for coupled chemistry meteorology models

    OpenAIRE

    M. Bocquet; H. Elbern; H. Eskes; M. Hirtl; R. Žabkar; G. R. Carmichael; J. Flemming; A. Inness; M. Pagowski; J. L. Pérez Camaño; P. E. Saide; R. San Jose; M. Sofiev; J. Vira; A. Baklanov

    2015-01-01

    Data assimilation is used in atmospheric chemistry models to improve air quality forecasts, construct re-analyses of three-dimensional chemical (including aerosol) concentrations and perform inverse modeling of input variables or model parameters (e.g., emissions). Coupled chemistry meteorology models (CCMM) are atmospheric chemistry models that simulate meteorological processes and chemical transformations jointly. They offer the possibility to assimilate both meteorologica...

  16. Recent Advances in Atmospheric Chemistry of Mercury

    Directory of Open Access Journals (Sweden)

    Lin Si

    2018-02-01

    Full Text Available Mercury is one of the most toxic metals and has global importance due to the biomagnification and bioaccumulation of organomercury via the aquatic food web. The physical and chemical transformations of various mercury species in the atmosphere strongly influence their composition, phase, transport characteristics and deposition rate back to the ground. Modeling efforts to assess global cycling of mercury require an accurate understanding of atmospheric mercury chemistry. Yet, there are several key uncertainties precluding accurate modeling of physical and chemical transformations. We focus this article on recent studies (since 2015 on improving our understanding of the atmospheric chemistry of mercury. We discuss recent advances in determining the dominant atmospheric oxidant of elemental mercury (Hg0 and understanding the oxidation reactions of Hg0 by halogen atoms and by nitrate radical (NO3—in the aqueous reduction of oxidized mercury compounds (HgII as well as in the heterogeneous reactions of Hg on atmospheric-relevant surfaces. The need for future research to improve understanding of the fate and transformation of mercury in the atmosphere is also discussed.

  17. Evaluated kinetic and photochemical data for atmospheric chemistry: Supplement VIII, halogen species evaluation for atmospheric chemistry

    International Nuclear Information System (INIS)

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

    2000-01-01

    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 9, 295 (1980); 11, 327 (1982); 13, 1259 (1984); 18, 881 (1989); 21, 1125 (1992); 26, 521 (1997); 26, 1329 (1997); 28, 191 (1999)]. The present evaluation is limited to the inorganic halogen family of atmospherically important reactions. 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 102 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 that model atmospheric chemistry. A table summarizing the preferred rate data is provided, together with an appendix listing the available values of enthalpies of formation of the reactant and product species

  18. Atmospheric chemistry: Description of the area of performance and a working plan

    Science.gov (United States)

    Kirchhoff, Volker W. J. H.

    1986-11-01

    INPE's program in Atmospheric Chemistry Research is described. Research in this area is concerned with atmospheric gases and their chemical reactions, production and loss rates, and their interactions with the biosphere. Atmospheric chemistry includes concepts in Physics, Chemistry, Meteorology, and Biology, which gives it a strong interdisciplinary character. The interaction of some of the atmospheric gases with the biosphere, such as ozone, is very strong and direct. Studying atmospheric chemistry is, therefore, of direct interest to man and the quality of life. Details are described to define the objectives of study, in particular those of our research program at INPE. A working plan is proposed in order to reach the defined goals. Owing to the large anthropogenic interference in the balance of the natural atmosphere it is anticipated that a better understanding of Atmospheric Chemistry will be the great scientific challenge of the next decade.

  19. Biomass burning studies and the International Global Atmospheric Chemistry (IGAC) Project

    International Nuclear Information System (INIS)

    Prinn, R.G.

    1991-01-01

    The perturbations to local and regional atmospheric chemistry caused by biomass burning also have global significance. The International Global Atmospheric Chemistry (IGAC) Project was created by scientists from over twenty countries in response to the growing interest concern about atmospheric chemical changes and their potential impact on mankind. The goal of the IGAC is to develop a fundamental understanding of the natural and anthropogenic processes that determine the chemical composition of the atmosphere and the interactions between atmospheric composition and biospheric and climatic processes. A specific objective is to accurately predict changes over the next century in the composition and chemistry of the global atmosphere. Current activities, leaders and scientists involved are presented in this chapter

  20. Atmospheric and aerosol chemistry

    International Nuclear Information System (INIS)

    McNeill, V. Faye; Ariya, Parisa A.; McGill Univ. Montreal, QC

    2014-01-01

    This series presents critical reviews of the present position and future trends in modern chemical research. Short and concise reports on chemistry, each written by the world renowned experts. Still valid and useful after 5 or 10 years. More information as well as the electronic version of the whole content available at: springerlink.com. Christian George, Barbara D'Anna, Hartmut Herrmann, Christian Weller, Veronica Vaida, D. J. Donaldson, Thorsten Bartels-Rausch, Markus Ammann Emerging Areas in Atmospheric Photochemistry. Lisa Whalley, Daniel Stone, Dwayne Heard New Insights into the Tropospheric Oxidation of Isoprene: Combining Field Measurements, Laboratory Studies, Chemical Modelling and Quantum Theory. Neil M. Donahue, Allen L. Robinson, Erica R. Trump, Ilona Riipinen, Jesse H. Kroll Volatility and Aging of Atmospheric Organic Aerosol. P. A. Ariya, G. Kos, R. Mortazavi, E. D. Hudson, V. Kanthasamy, N. Eltouny, J. Sun, C. Wilde Bio-Organic Materials in the Atmosphere and Snow: Measurement and Characterization V. Faye McNeill, Neha Sareen, Allison N. Schwier Surface-Active Organics in Atmospheric Aerosols.

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

    Science.gov (United States)

    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.

  2. Atmospheric and aerosol chemistry

    Energy Technology Data Exchange (ETDEWEB)

    McNeill, V. Faye [Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Ariya, Parisa A. (ed.) [McGill Univ. Montreal, QC (Canada). Dept. of Chemistry; McGill Univ. Montreal, QC (Canada). Dept. of Atmospheric and Oceanic Sciences

    2014-09-01

    This series presents critical reviews of the present position and future trends in modern chemical research. Short and concise reports on chemistry, each written by the world renowned experts. Still valid and useful after 5 or 10 years. More information as well as the electronic version of the whole content available at: springerlink.com. Christian George, Barbara D'Anna, Hartmut Herrmann, Christian Weller, Veronica Vaida, D. J. Donaldson, Thorsten Bartels-Rausch, Markus Ammann Emerging Areas in Atmospheric Photochemistry. Lisa Whalley, Daniel Stone, Dwayne Heard New Insights into the Tropospheric Oxidation of Isoprene: Combining Field Measurements, Laboratory Studies, Chemical Modelling and Quantum Theory. Neil M. Donahue, Allen L. Robinson, Erica R. Trump, Ilona Riipinen, Jesse H. Kroll Volatility and Aging of Atmospheric Organic Aerosol. P. A. Ariya, G. Kos, R. Mortazavi, E. D. Hudson, V. Kanthasamy, N. Eltouny, J. Sun, C. Wilde Bio-Organic Materials in the Atmosphere and Snow: Measurement and Characterization V. Faye McNeill, Neha Sareen, Allison N. Schwier Surface-Active Organics in Atmospheric Aerosols.

  3. Chemistry and evolution of Titan's atmosphere

    International Nuclear Information System (INIS)

    Strobel, D.F.

    1982-01-01

    The chemistry and evolution of Titan's atmosphere is reviewed in the light of the scientific findings from the Voyager mission. It is argued that the present N 2 atmosphere may be Titan's initial atmosphere rather than photochemically derived from an original NH 3 atmosphere. The escape rate of hydrogen from Titan is controlled by photochemical production from hydrocarbons. CH 4 is irreversibly converted to less hydrogen rich hydrocarbons, which over geologic time accumulate on the surface to a layer thickness of approximately 0.5 km. Magnetospheric electrons interacting with Titan's exosphere may dissociate enough N 2 into hot, escaping N atoms to remove approximately 0.2 of Titan's present atmosphere over geologic time. The energy dissipation of magnetospheric electrons exceeds solar e.u.v. 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. (author)

  4. Impact of aircraft emissions on the atmospheric chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Dameris, M; Sausen, R; Grewe, V; Koehler, I; Ponater, M [Deutsche Forschungs- und Versuchsanstalt fuer Luft- und Raumfahrt e.V., Oberpfaffenhofen (Germany). Inst. fuer Physik der Atmosphaere; Steil, B [Max-Planck-Inst. fuer Meteorologie, Hamburg (Germany); Bruehl, Ch [Max-Planck-Inst. fuer Chemie (Otto-Hahn-Institut), Mainz (Germany)

    1998-12-31

    A hierarchy of models of different complexity has been applied to estimate the impact of aircraft NO{sub x} emissions on atmospheric chemistry. The global circulation model ECHAM3 has been coupled with two types of chemistry modules. The first of these describes only a simplified (linear) NO{sub x} and HNO{sub 3} chemistry while the second one is a comprehensive chemistry module (CHEM), describing tropospheric and stratospheric chemistry including photochemical reactions and heterogeneous reactions on sulphate aerosols and PSCs. The module CHEM has been coupled either off-line or with feedback via the ozone concentration. First results of multilayer integrations (over decades) are discussed. (author) 27 refs.

  5. Impact of aircraft emissions on the atmospheric chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Dameris, M.; Sausen, R.; Grewe, V.; Koehler, I.; Ponater, M. [Deutsche Forschungs- und Versuchsanstalt fuer Luft- und Raumfahrt e.V., Oberpfaffenhofen (Germany). Inst. fuer Physik der Atmosphaere; Steil, B. [Max-Planck-Inst. fuer Meteorologie, Hamburg (Germany); Bruehl, Ch. [Max-Planck-Inst. fuer Chemie (Otto-Hahn-Institut), Mainz (Germany)

    1997-12-31

    A hierarchy of models of different complexity has been applied to estimate the impact of aircraft NO{sub x} emissions on atmospheric chemistry. The global circulation model ECHAM3 has been coupled with two types of chemistry modules. The first of these describes only a simplified (linear) NO{sub x} and HNO{sub 3} chemistry while the second one is a comprehensive chemistry module (CHEM), describing tropospheric and stratospheric chemistry including photochemical reactions and heterogeneous reactions on sulphate aerosols and PSCs. The module CHEM has been coupled either off-line or with feedback via the ozone concentration. First results of multilayer integrations (over decades) are discussed. (author) 27 refs.

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

    Science.gov (United States)

    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.

  7. Report to the International Global Atmospheric Chemistry Project

    Energy Technology Data Exchange (ETDEWEB)

    Reisdorf, Jill [University Corporation for Atmospheric Research (UCAR/CPAESS), Boulder, CO (United States); Wiedinmyer, Christine [National Center for Atmospheric Research (NCAR/ACOM), Boulder, CO (United States)

    2017-04-21

    IGAC’s mission is to facilitate atmospheric chemistry research towards a sustainable world. This is achieved through IGAC’s three focal activities: fostering community, building capacity, and providing leadership. A key component to achieving IGAC’s mission is its developing early career program. These scientists join an international network early in their career that puts the cogs in motion to further facilitate atmospheric chemistry research at an international level for years to come. IGAC’s Science Conference is a primary mechanism for IGAC to build cooperation and disseminate scientific information across its international community. The first IGAC Science Conference was held in 1993 in Eilat, Israel. Since then, IGAC has successfully held fourteen science conferences, consistently becoming a biennial conference starting in 2002. The biennial IGAC Science Conference is regarded as THE international conference on atmospheric chemistry and participation in the conference is typically in the range of 350-650 participants. Since 2004, IGAC has included an Early Career Scientists Program as part of the conference to foster the next generation of scientists. IGAC believes, and has seen, that by allowing scientists to form an international network of colleagues early in their career that future international collaborations in atmospheric chemistry are enhanced. The 2016 IGAC Science Conference Early Career Program consisted of numerous events throughout the week giving these scientists the opportunity to not only create a community amongst themselves, but to also engage and build relationships with senior scientists. In order to support the Early Career Scientists Program, IGAC sought funding from international, regional and local organizations to provide Travel Grants to the conference based on an assessment of both need and merit. This conference summary reports on outcomes of the 2016 IGAC Science Conference and the Early Career Program, which included

  8. Atmospheric Composition Change: Climate-Chemistry Interactions

    Science.gov (United States)

    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

  9. Atmospheric Boundary Layer, Integrating Air Chemistry and Land Interactions

    NARCIS (Netherlands)

    Vilà-Guerau De Arellano, J.; Heerwaarden, van C.C.; Stratum, van B.J.H.; Dries, van den C.L.A.M.

    2015-01-01

    This textbook provides an introduction to the interactions between the atmosphere and the land for advanced undergraduate and graduate students and a reference text for researchers in atmospheric physics and chemistry, hydrology, and plant physiology. The combination of the book, which provides the

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

    Science.gov (United States)

    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.

  11. 2017 Atmospheric Chemistry Gordon Research Conference

    Science.gov (United States)

    2017-11-13

    am - 10:45 am Discussion 10:45 am - 11:05 am Coffee Break 11:05 am - 11:35 am Allison Steiner (University of Michigan, USA) "The Atmospheric Life ...34Progress and Prospects: The Quest to Understand the Impacts of Multiphase Chemistry on a Wet Planet " 11:35 am - 11:50 am Discussion 11:50 am - 12:00

  12. IceBridge Atmospheric Chemistry L1B Data

    Data.gov (United States)

    National Aeronautics and Space Administration — The IceBridge Atmospheric Chemistry L1B Data set (ICHEM1B) contains measurements acquired over Antarctica using the AVOCET differential Non-Dispersive Infrared...

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

    Science.gov (United States)

    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

  14. Atmospheric Chemistry of Micrometeoritic Organic Compounds

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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.

  16. Atmospheric Prebiotic Chemistry and Organic Hazes

    Science.gov (United States)

    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.

  17. Atmospheric Chemistry of (CF3)2CF-C≡N

    DEFF Research Database (Denmark)

    Andersen, Mads Peter Sulbæk; Kyte, Mildrid; Thirstrup Andersen, Simone

    2017-01-01

    FTIR/smog chamber experiments and ab initio quantum calculations were performed to investigate the atmospheric chemistry of (CF3)2CFCN, a proposed replacement compound for the industrially important sulfur hexafluoride, SF6. The present study determined k(Cl + (CF3)2CFCN) = (2.33 ± 0.87) × 10–17, k......(OH + (CF3)2CFCN) = (1.45 ± 0.25) × 10–15, and k(O3 + (CF3)2CFCN) ≤ 6 × 10–24 cm3 molecule–1 s–1, respectively, in 700 Torr of N2 or air diluent at 296 ± 2 K. The main atmospheric sink for (CF3)2CFCN was determined to be reaction with OH radicals. Quantum chemistry calculations, supported by experimental...

  18. Organic chemistry in a CO2 rich early Earth atmosphere

    Science.gov (United States)

    Fleury, Benjamin; Carrasco, Nathalie; Millan, Maëva; Vettier, Ludovic; Szopa, Cyril

    2017-12-01

    The emergence of life on the Earth has required a prior organic chemistry leading to the formation of prebiotic molecules. The origin and the evolution of the organic matter on the early Earth is not yet firmly understood. Several hypothesis, possibly complementary, are considered. They can be divided in two categories: endogenous and exogenous sources. In this work we investigate the contribution of a specific endogenous source: the organic chemistry occurring in the ionosphere of the early Earth where the significant VUV contribution of the young Sun involved an efficient formation of reactive species. We address the issue whether this chemistry can lead to the formation of complex organic compounds with CO2 as only source of carbon in an early atmosphere made of N2, CO2 and H2, by mimicking experimentally this type of chemistry using a low pressure plasma reactor. By analyzing the gaseous phase composition, we strictly identified the formation of H2O, NH3, N2O and C2N2. The formation of a solid organic phase is also observed, confirming the possibility to trigger organic chemistry in the upper atmosphere of the early Earth. The identification of Nitrogen-bearing chemical functions in the solid highlights the possibility for an efficient ionospheric chemistry to provide prebiotic material on the early Earth.

  19. The Department of Energy's Atmospheric Chemistry Program: A critical review

    International Nuclear Information System (INIS)

    1991-01-01

    In response to a request from the Department of Energy's (DOE) Office of Health and Environmental Research (OHER), the Committee on Atmospheric Chemistry has reviewed OHER's Atmospheric Chemistry Program (ACP). This report contains the committee's evaluation and critique arising from that review. The review process included a two-day symposium held at the National Academy of Sciences on September 25 and 26, 1990, that focused on presenting the ACP's current components, recent scientific accomplishments, and scientific plans. Following the symposium, committee members met in a one-day executive session to formulate and outline this report. In undertaking this review, OHER and ACP management requested that the committee attempt to answer several specific questions involving the program's technical capability and productivity, its leadership and organization, and its future direction. These questions are given in the Appendix. This report represents the committee's response to the questions posed in the Appendix. Chapter I explores the committee's view of the role that atmospheric chemistry could and should assume within the DOE and its prospective National Energy Strategy. Chapter 2 assesses the current ACP, Chapter 3 presents recommendations for revising and strengthening it, and Chapter 4 restates the committee's conclusions and recommendations

  20. Problems in global atmospheric chemistry

    Science.gov (United States)

    Crutzen, Paul J.

    1993-02-01

    The chemistry of the atmosphere is substantially influenced by a wide range of chemical processes which are primarily driven by the action of ultraviolet radiation of wavelengths shorter than 320 nm (UV-B) on ozone and water vapor. This leads to the formation of hydroxyl (OH) radicals which, despite very low tropospheric concentrations, remove most gases that are emitted into the atmosphere by natural and anthropogenic processes. Therefore, although only about 10% of all atmospheric ozone is located in the troposphere, through the formation of OH, it determines the oxidation efficiency of the atmosphere and is, therefore, of the utmost importance for maintaining its chemical composition. Due to a variety of human activities, especially through increasing emissions of CH4, CO, and NOx, the concentrations of tropospheric ozone and hydroxyl are expected to be increasing in polluted and decreasing in clean tropospheric environments. Altogether, this may be leading to an overall decrease in the oxidation efficiency of the atmosphere, contributing to a gradual buildup of several longlived trace gases that are primarily removed by reaction with OH. In the stratosphere, especially due to catalytic reactions of chlorine-containing gases of industrial origin, ozone is being depleted, most drastically noted during the early spring months over Antarctica. Because ozone is the only atmospheric constituent that can significantly absorb solar radiation in the wavelength region 240 - 320 nm, this loss of ozone enhances the penetration of biologically harmful UV-B radiation to the earth's surface with ensuing negative consequences for the biosphere. Several of the aforementioned chemically active trace gases with growing trends in the atmosphere are also efficient greenhouse gases. Together they can exert a warming effect on the earth's climate about equal to that of carbon dioxide.

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

    Science.gov (United States)

    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. © 2014 Society for Applied Microbiology and John Wiley & Sons Ltd.

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

    Science.gov (United States)

    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.

  3. Results of an interactively coupled atmospheric chemistry – general circulation model: Comparison with observations

    Directory of Open Access Journals (Sweden)

    R. Hein

    Full Text Available The coupled climate-chemistry model ECHAM4.L39(DLR/CHEM is presented which enables a simultaneous treatment of meteorology and atmospheric chemistry and their feedbacks. This is the first model which interactively combines a general circulation model with a chemical model, employing most of the important reactions and species necessary to describe the stratospheric and upper tropospheric ozone chemistry, and which is computationally fast enough to allow long-term integrations with currently available computer resources. This is possible as the model time-step used for the chemistry can be chosen as large as the integration time-step for the dynamics. Vertically the atmosphere is discretized by 39 levels from the surface up to the top layer which is centred at 10 hPa, with a relatively high vertical resolution of approximately 700 m near the extra-tropical tropopause. We present the results of a control simulation representing recent conditions (1990 and compare it to available observations. The focus is on investigations of stratospheric dynamics and chemistry relevant to describe the stratospheric ozone layer. ECHAM4.L39(DLR/CHEM reproduces main features of stratospheric dynamics in the arctic vortex region, including stratospheric warming events. This constitutes a major improvement compared to earlier model versions. However, apparent shortcomings in Antarctic circulation and temperatures persist. The seasonal and interannual variability of the ozone layer is simulated in accordance with observations. Activation and deactivation of chlorine in the polar stratospheric vortices and their inter-hemispheric differences are reproduced. Considering methane oxidation as part of the dynamic-chemistry feedback results in an improved representation of the spatial distribution of stratospheric water vapour concentrations. The current model constitutes a powerful tool to investigate, for instance, the combined direct and indirect effects of anthropogenic

  4. The global change research center atmospheric chemistry model

    Energy Technology Data Exchange (ETDEWEB)

    Moraes, Jr., Francis Perry [Oregon Graduate Inst. of Science and Technology, Portland, OR (United States)

    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.

  5. Parameterization of dust emissions in the global atmospheric chemistry-climate model EMAC: impact of nudging and soil properties

    OpenAIRE

    Astitha, M.; Lelieveld, J.; Kader, M. Abdel; Pozzer, A.; de Meij, A.

    2012-01-01

    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. Two versions of a parameterization scheme to compute desert dust emissions are incorporated into the atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy2.41 Atmospheric Chemistry). One uses a global...

  6. Nighttime atmospheric chemistry of iodine

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    McElroy, James L.; McNeal, Robert J.

    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. (For individual items see A93-31377 to A93-31412)

  9. Frontiers in Atmospheric Chemistry Modelling

    Science.gov (United States)

    Colette, Augustin; Bessagnet, Bertrand; Meleux, Frederik; Rouïl, Laurence

    2013-04-01

    The first pan-European kilometre-scale atmospheric chemistry simulation is introduced. The continental-scale air pollution episode of January 2009 is modelled with the CHIMERE offline chemistry-transport model with a massive grid of 2 million horizontal points, performed on 2000 CPU of a high performance computing system hosted by the Research and Technology Computing Center at the French Alternative Energies and Atomic Energy Commission (CCRT/CEA). Besides the technical challenge, which demonstrated the robustness of the selected air quality model, we discuss the added value in terms of air pollution modelling and decision support. The comparison with in-situ observations shows that model biases are significantly improved despite some spurious added spatial variability attributed to shortcomings in the emission downscaling process and coarse resolution of the meteorological fields. The increased spatial resolution is clearly beneficial for the detection of exceedances and exposure modelling. We reveal small scale air pollution patterns that highlight the contribution of city plumes to background air pollution levels. Up to a factor 5 underestimation of the fraction of population exposed to detrimental levels of pollution can be obtained with a coarse simulation if subgrid scale correction such as urban increments are ignored. This experiment opens new perspectives for environmental decision making. After two decades of efforts to reduce air pollutant emissions across Europe, the challenge is now to find the optimal trade-off between national and local air quality management strategies. While the first approach is based on sectoral strategies and energy policies, the later builds upon new alternatives such as urban development. The strategies, the decision pathways and the involvement of individual citizen differ, and a compromise based on cost and efficiency must be found. We illustrated how high performance computing in atmospheric science can contribute to this

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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

  12. Some current problems in atmospheric ozone chemistry; role of chemical kinetics

    Energy Technology Data Exchange (ETDEWEB)

    Cox, R.A.

    1987-03-01

    A review is given on selected aspects of the reaction mechanisms of current interest in the chemistry of atmospheric ozone. Atmospheric ozone is produced and removed by a complex series of elementary gas-phase photochemical reactions involving O/sub x/, HO/sub x/, NO/sub x/, CIO/sub x/ and hydrocarbon species. At the present time there is a good knowledge of the basic processes involved in ozone chemistry in the stratosphere and the troposphere and the kinetics of most of the key reactions are well defined. There are a number of difficulties in the theoretical descriptions of observed ozone behaviour which may be due to uncertainties in the chemistry. Examples are the failure to predict present day ozone in the photochemically controlled region above 35 Km altitude and the large reductions in the ozone column in the Antartic Spring which has been observed in recent years. In the troposphere there is growing evidence that ozone and other trace gases have changed appreciably from pre-industrial concentrations, due to chemical reactions involving man-made pollutants. Quantitative investigation of the mechanisms by which these changes may occur requires a sound laboratory kinetics data base.

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

    Science.gov (United States)

    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...

  14. Characterization of a boreal convective boundary layer and its impact on atmospheric chemistry during HUMPPA-COPEC-2010

    Directory of Open Access Journals (Sweden)

    H. G. Ouwersloot

    2012-10-01

    Full Text Available We studied the atmospheric boundary layer (ABL dynamics and the impact on atmospheric chemistry during the HUMPPA-COPEC-2010 campaign. We used vertical profiles of potential temperature and specific moisture, obtained from 132 radio soundings, to determine the main boundary layer characteristics during the campaign. We propose a classification according to several main ABL prototypes. Further, we performed a case study of a single day, focusing on the convective boundary layer, to analyse the influence of the dynamics on the chemical evolution of the ABL. We used a mixed layer model, initialized and constrained by observations. In particular, we investigated the role of large scale atmospheric dynamics (subsidence and advection on the ABL development and the evolution of chemical species concentrations. We find that, if the large scale forcings are taken into account, the ABL dynamics are represented satisfactorily. Subsequently, we studied the impact of mixing with a residual layer aloft during the morning transition on atmospheric chemistry. The time evolution of NOx and O3 concentrations, including morning peaks, can be explained and accurately simulated by incorporating the transition of the ABL dynamics from night to day. We demonstrate the importance of the ABL height evolution for the representation of atmospheric chemistry. Our findings underscore the need to couple the dynamics and chemistry at different spatial scales (from turbulence to mesoscale in chemistry-transport models and in the interpretation of observational data.

  15. Variational data assimilation schemes for transport and transformation models of atmospheric chemistry

    Science.gov (United States)

    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

  16. Global atmospheric chemistry – which air matters

    Directory of Open Access Journals (Sweden)

    M. J. Prather

    2017-07-01

    Full Text Available 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.

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

    Science.gov (United States)

    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"); (c) the emerging instrumentation revolution and some of the challenges that it brings; (d) the structural issues of insufficient support for the analysis of field campaigns; and (e) some important areas that were missing from this Faraday Discussion and that should receive an increasing focus in the future.

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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

  1. Modelling iodide – iodate speciation in atmospheric aerosol: Contributions of inorganic and organic iodine chemistry

    Directory of Open Access Journals (Sweden)

    S. Pechtl

    2007-01-01

    Full Text Available The speciation of iodine in atmospheric aerosol is currently poorly understood. Models predict negligible iodide concentrations but accumulation of iodate in aerosol, both of which is not confirmed by recent measurements. We present an updated aqueous phase iodine chemistry scheme for use in atmospheric chemistry models and discuss sensitivity studies with the marine boundary layer model MISTRA. These studies show that iodate can be reduced in acidic aerosol by inorganic reactions, i.e., iodate does not necessarily accumulate in particles. Furthermore, the transformation of particulate iodide to volatile iodine species likely has been overestimated in previous model studies due to negligence of collision-induced upper limits for the reaction rates. However, inorganic reaction cycles still do not seem to be sufficient to reproduce the observed range of iodide – iodate speciation in atmospheric aerosol. Therefore, we also investigate the effects of the recently suggested reaction of HOI with dissolved organic matter to produce iodide. If this reaction is fast enough to compete with the inorganic mechanism, it would not only directly lead to enhanced iodide concentrations but, indirectly via speed-up of the inorganic iodate reduction cycles, also to a decrease in iodate concentrations. Hence, according to our model studies, organic iodine chemistry, combined with inorganic reaction cycles, is able to reproduce observations. The presented chemistry cycles are highly dependent on pH and thus offer an explanation for the large observed variability of the iodide – iodate speciation in atmospheric aerosol.

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

    Science.gov (United States)

    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

  3. Tracer chemistry in the laboratory and the atmosphere

    International Nuclear Information System (INIS)

    Rowland, F.S.

    1994-01-01

    The steady bombardment of the Earth's atmosphere by cosmic radiation induces numerous radioactive species in the atmosphere of which the best known are 14 C and T. Others of interest include 7 Be, 10 Be, and several isotopes of chlorine. The eventual formation of 14 CO 2 and its subsequent significance for archaeological dating were brilliantly established by Willard Libby in the 1940s. However, the initial reactions of nascent 14 C in a mixture of N 2 and O 2 produce 14 CO, as shown first in the lab. and then in the atmosphere. Because cosmic ray production rates are essentially constant in a given location, the observed concentration of 14 CO provides an excellent tool for studying the removal process, oxidation by HO to form 14 CO 2 . Because 14 CO 2 becomes incorporated into all living biological species, other molecules become labeled with 14 C as well, including 14 CH 4 . Measurement of the 14 C radioactivity of such molecules in the atmosphere allows apportionment of sources between biological and fossil fuel origins. Tritium atoms are also formed by cosmic radiation, and can subsequently be incorporated into the chemical forms HT and HTO. Although most T atoms from cosmic radiation are found as HTO, the much higher specific radioactivity of HT provides interesting insights into atmospheric processes. Lab. studies furnish important clues for understanding the atmospheric routes. The differences in radioactive half-lives cause the terrestrial locations of cosmic ray induced 7 Be and 10 Be to be primarily the atmosphere and the oceans, respectively. In a comparable manner, the chemistry of atmospheric radiochlorine divides between the very long-lived 36 Cl and three isotopes with half-lives less than an hour, 34m Cl, 38 Cl and 39 Cl

  4. The impact of Future Land Use and Land Cover Changes on Atmospheric Chemistry-Climate Interactions

    NARCIS (Netherlands)

    Ganzeveld, L.N.; Bouwman, L.

    2010-01-01

    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

  5. Chemistry of Atmospheric Aerosols at Pacifichem 2015 Congress

    Energy Technology Data Exchange (ETDEWEB)

    Nizkorodov, Sergey [Univ. of California, Irvine, CA (United States)

    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

  6. Atmospheric Chemistry of CH3CH2OCH3

    DEFF Research Database (Denmark)

    Andersen, Mads Peter Sulbæk; Bjørn Svendsen, Sissel; Østerstrøm, Freja From

    2017-01-01

    The atmospheric chemistry of methyl ethyl ether, CH3CH2OCH3, was examined using FT-IR/relative-rate methods. Hydroxyl radical and chlorine atom rate coefficients of k(CH3CH2OCH3+OH) = (7.53 ± 2.86) × 10−12 cm3 molecule−1 s−1 and k(CH3CH2OCH3+Cl) = (2.35 ± 0.43) × 10−10 cm3 molecule−1 s−1 were...

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

    Science.gov (United States)

    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…

  8. Iterative ensemble variational methods for nonlinear data assimilation: Application to transport and atmospheric chemistry

    International Nuclear Information System (INIS)

    Haussaire, Jean-Matthieu

    2017-01-01

    Data assimilation methods are constantly evolving to adapt to the various application domains. In atmospheric sciences, each new algorithm has first been implemented on numerical weather prediction models before being ported to atmospheric chemistry models. It has been the case for 4D variational methods and ensemble Kalman filters for instance. The new 4D ensemble variational methods (4D EnVar) are no exception. They were developed to take advantage of both variational and ensemble approaches and they are starting to be used in operational weather prediction centers, but have yet to be tested on operational atmospheric chemistry models. The validation of new data assimilation methods on these models is indeed difficult because of the complexity of such models. It is hence necessary to have at our disposal low-order models capable of synthetically reproducing key physical phenomena from operational models while limiting some of their hardships. Such a model, called L95-GRS, has therefore been developed. Il combines the simple meteorology from the Lorenz-95 model to a tropospheric ozone chemistry module with 7 chemical species. Even though it is of low dimension, it reproduces some of the physical and chemical phenomena observable in real situations. A data assimilation method, the iterative ensemble Kalman smoother (IEnKS), has been applied to this model. It is an iterative 4D EnVar method which solves the full non-linear variational problem. This application validates 4D EnVar methods in the context of non-linear atmospheric chemistry, but also raises the first limits of such methods, most noticeably when they are applied to weakly coupled stable models. After this experiment, results have been extended to a realistic atmospheric pollution prediction model. 4D EnVar methods, via the IEnKS, have once again shown their potential to take into account the non-linearity of the chemistry model in a controlled environment, with synthetic observations. However, the

  9. Atmospheric chemistry of CFCs and potential alternatives

    International Nuclear Information System (INIS)

    Watson, R.T.

    1990-01-01

    Since the discovery of the ozone hole, the knowledge of atmospheric chemistry related to ozone depletion and chlorofluorocarbons has increased significantly. Factors that result in large losses in ozone during the Antarctic spring are present in the Arctic, although a hole has not been observed. The latest science is discussed as it pertains to the Arctic and Antarctic regions. The ozone depletion potentials (ODP) and global warming potentials (GWP) of the most likely alternatives are presented and related to their environmental acceptability. NASA, NSF, NOAA, EPA and the industry sponsored AFEAS program are coordinating efforts to provide further scientific information to more fully understand the potential environmental effects of alternatives. A progress report is given

  10. Bunsen conference 1999. Atmospheric physical chemistry; Bunsentagung 1999. Physikalische Chemie der Atmosphaere

    Energy Technology Data Exchange (ETDEWEB)

    Crutzen, P.J.; Zellner, R. [comps.

    2000-07-01

    The main subject of the 1999 Bunsen conference was atmospheric physical chemistry. There were lectures and posters on measurement and distribution of atmospheric trace gases, photochemical reactions in the different parts of the atmosphere, natural and anthropogenic emissions resulting from biomass combustion, thermodynamics and microphysics of aerosol, and air pollution abatement. [German] Die Bunsentagung 1999 beschaeftigte sich mit dem Thema Physikalische Chemie der Atmosphaere. Themen der Vortraege und Poster waren u.a. die Messung und Verteilung von Spurengasen in der Atmosphaere, photochemische Reaktionen in den verschiedenen Schichten der Atmosphaere, natuerliche und anthropogene Emissionen durch Verbrennung von Biomasse, Thermodynamik und Microphysik von Aerosolen und Klimaschutz.

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

    Energy Technology Data Exchange (ETDEWEB)

    Keene, William C. [University of Virginia; Long, Michael S. [University of Virginia

    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

  12. Atmospheric Photooxidation Products and Chemistry of Current-use Pesticides

    Science.gov (United States)

    Murschell, T.; Farmer, D.

    2017-12-01

    Pesticides are widely used in agricultural, commercial, and residential applications across the United States. Pesticides can volatilize off targets and travel long distances, with atmospheric lifetimes determined by both physical and chemical loss processes. In particular, oxidation by the hydroxyl radical (OH) can reduce the lifetime and thus atmospheric transport of pesticides, though the rates and oxidation products of atmospheric pesticide oxidation are poorly understood. Here, we investigate reactions of current-use pesticides with OH. MCPA, triclopyr, and fluroxypyr are herbicides that are often formulated together to target broadleaf weeds. We detect these species in the gas-phase using real-time high resolution chemical ionization mass spectrometry (CIMS) with both acetate and iodide reagent ions. We used an Oxidative Flow Reactor to explore OH radical oxidation and photolysis of these compounds, simulating up to 5 equivalent days of atmospheric aging by OH. Use of two ionization schemes allowed for the more complete representation of the OH radical oxidation of the three pesticides. The high resolution mass spectra allows us to deduce structures of the oxidation products and identify multi-generational chemistry. In addition, we observe nitrogen oxides, as well as isocyanic acid (HNCO), from some nitrogen-containing pesticides. We present yields of species of atmospheric importance, including NOx and halogen species and consider their impact on air quality following pesticide application.

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

    Energy Technology Data Exchange (ETDEWEB)

    Park, Sung-Jin [Univ. of Illinois, Urbana, IL (United States); Eden, James Gary [Univ. of Illinois, Urbana, IL (United States)

    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.

  14. The role of ammonia in the chemistry of atmospheric aerosols

    International Nuclear Information System (INIS)

    Brosset, C.

    1979-01-01

    Data is presented on the concentrations of hydrogen and ammonium ions in aerosol samples taken under various meteorological conditions in different areas of Sweden, and implications for the atmospheric chemistry of aerosols are discussed. Particle compositions at coastal and inland stations were determined during situations when particle concentrations increased as much as a hundred times due to atmospheric transport from Europe or air movements from the east or west. Analysis of particle compositions during both types of particle episodes reveals variations in the H(+)/NH4(+) ratio which indicate that particles present over agricultural areas take up ammonia from the ground and release it over a forest district with acid lakes. The ratio is found to be dependent on the atmospheric partial pressure of ammonia at equilibrium, with the flow of ammonia to or from the ground and transport conditions also likely to influence the ratio

  15. Atmospheric chemistry, sources and sinks of carbon suboxide, C3O2

    Science.gov (United States)

    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 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.

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

    Science.gov (United States)

    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

  17. Variational methods for direct/inverse problems of atmospheric dynamics and chemistry

    Science.gov (United States)

    Penenko, Vladimir; Penenko, Alexey; Tsvetova, Elena

    2013-04-01

    We present a variational approach for solving direct and inverse problems of atmospheric hydrodynamics and chemistry. It is important that the accurate matching of numerical schemes has to be provided in the chain of objects: direct/adjoint problems - sensitivity relations - inverse problems, including assimilation of all available measurement data. To solve the problems we have developed a new enhanced set of cost-effective algorithms. The matched description of the multi-scale processes is provided by a specific choice of the variational principle functionals for the whole set of integrated models. Then all functionals of variational principle are approximated in space and time by splitting and decomposition methods. Such approach allows us to separately consider, for example, the space-time problems of atmospheric chemistry in the frames of decomposition schemes for the integral identity sum analogs of the variational principle at each time step and in each of 3D finite-volumes. To enhance the realization efficiency, the set of chemical reactions is divided on the subsets related to the operators of production and destruction. Then the idea of the Euler's integrating factors is applied in the frames of the local adjoint problem technique [1]-[3]. The analytical solutions of such adjoint problems play the role of integrating factors for differential equations describing atmospheric chemistry. With their help, the system of differential equations is transformed to the equivalent system of integral equations. As a result we avoid the construction and inversion of preconditioning operators containing the Jacobi matrixes which arise in traditional implicit schemes for ODE solution. This is the main advantage of our schemes. At the same time step but on the different stages of the "global" splitting scheme, the system of atmospheric dynamic equations is solved. For convection - diffusion equations for all state functions in the integrated models we have developed the

  18. Collaborative Research: Atmospheric Pressure Microplasma Chemistry-Photon Synergies Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Graves, David [Univ. of California, Berkeley, CA (United States)

    2017-02-07

    Combining the effects of low temperature, atmospheric pressure microplasmas and microplasma photon sources shows greatly expanded range of applications of each of them. The plasma sources create active chemical species and these can be activated further by addition of photons and associated photochemistry. There are many ways to combine the effects of plasma chemistry and photochemistry, especially if there are multiple phases present. The project combines construction of appropriate test experimental systems, various spectroscopic diagnostics and mathematical modeling.

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

    Science.gov (United States)

    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

  20. The role of human activity and land use change in atmospheric chemistry and air quality

    International Nuclear Information System (INIS)

    Penner, J.E.

    1992-07-01

    In the this paper, I review the importance of a mineral of fossil fuel emissions atmospheric chemistry, air quality, and climate. I then review current estimates of the sources for each specie, deriving the fraction of each source that is due to specific land use practices or land cover categories. Understanding the current trends of those species with known increasing abundances and projecting increases into the future is possible if the estimated sources from human activity and land use change can be projected and if the known atmospheric sinks and the interactions in atmospheric chemistry and climate change are appropriately taken into account. Regional trends in the short-lived species can be projected as well, assuming the estimated sources and sinks are correct. However, significant uncertainties continue to surround the estimated budgets for most of these species. Uncertainties and the estimated ranges in different source strength estimates for each are also discussed

  1. Characterization of a boreal convective boundary layer and its impact on atmospheric chemistry during HUMPPA-COPEC-2010

    NARCIS (Netherlands)

    Ouwersloot, H.G.; Vilà-Guerau de Arellano, J.; Nölscher, A.C.; Krol, M.C.; Ganzeveld, L.N.; Breitenberger, C.; Mammarella, I.; Williams, J.; Lelieveld, J.

    2012-01-01

    We studied the atmospheric boundary layer (ABL) dynamics and the impact on atmospheric chemistry during the HUMPPA-COPEC-2010 campaign. We used vertical profiles of potential temperature and specific moisture, obtained from 132 radio soundings, to determine the main boundary layer characteristics

  2. Clays as mineral dust aerosol: An integrated approach to studying climate, atmospheric chemistry, and biogeochemical effects of atmospheric clay minerals in an undergraduate research laboratory

    Science.gov (United States)

    Hatch, C. D.; Crane, C. C.; Harris, K. J.; Thompson, C. E.; Miles, M. K.; Weingold, R. M.; Bucuti, T.

    2011-12-01

    Entrained mineral dust aerosol accounts for 45% of the global annual atmospheric aerosol load and can have a significant influence on important environmental issues, including climate, atmospheric chemistry, cloud formation, biogeochemical processes, visibility, and human health. 70% of all mineral aerosol mass originating from Africa consists of layered aluminosilicates, including illite, kaolinite, and montmorillonite clays. Clay minerals are a largely neglected component of mineral aerosol, yet they have unique physiochemical properties, including a high reactive surface area, large cation exchange capacities, small particle sizes, and a relatively large capacity to take up adsorbed water, resulting in expansion of clay layers (and a larger reactive surface area for heterogeneous interactions) in some cases. An integrated laboratory research approach has been implemented at Hendrix College, a Primarily Undergraduate Institution, in which undergraduate students are involved in independent and interdisciplinary research projects that relate the chemical aging processes (heterogeneous chemistry) of clay minerals as a major component of mineral aerosol to their effects on climate (water adsorption), atmospheric chemistry (trace gas uptake), and biogeochemistry (iron dissolution and phytoplankton biomarker studies). Preliminary results and future directions will be reported.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  4. ALMA observations of Titan's atmospheric chemistry and seasonal variation

    Science.gov (United States)

    Cordiner, Martin

    2017-04-01

    Titan is the largest moon of Saturn, with a thick (1.45 bar) atmosphere composed primarily of molecular nitrogen and methane. Photochemistry in Titan's upper atmosphere results in the production of a wide range of organic molecules, including hydrocarbons, nitriles and aromatics, some of which could be of pre-biotic relevance. Thus, we obtain insights into the possible molecular inventories of primitive (reducing) planetary atmospheres. Titan's atmosphere also provides a unique laboratory for testing our understanding of fundamental processes involving the chemistry and spectroscopy of complex organic molecules. In this talk, results will be presented from our studies using the Atacama Large Millimeter/submillimeter Array (ALMA) during the period 2012-2015, focussing in particular on the detection and mapping of emission from various nitrile species. By combining data from multiple ALMA observations, our spectra have reached an unprecedented sensitivity level, enabling the first spectroscopic detection and mapping of C2H3CN (vinyl cyanide) on Titan. Liquid-phase simulations of Titan's seas indicate that vinyl cyanide molecules could combine to form vesicle membranes (similar to the cells of terrestrial biology), and the astrobiological implications of this discovery will be discussed. Furthermore, ALMA observations provide instantaneous snapshot mapping of Titan's entire Earth-facing hemisphere, for gases inaccessible to previous instruments. Combined with complementary data obtained from the Cassini Saturn orbiter, as well as theoretical models and laboratory studies, our observed, seasonally variable, spatially resolved abundance patterns are capable of providing new insights into photochemical production and transport in primitive planetary atmospheres in the Solar System and beyond.

  5. Laboratory studies of nitrate radical chemistry - application to atmospheric processes

    Energy Technology Data Exchange (ETDEWEB)

    Noremsaune, Ingse

    1997-12-31

    This thesis studies atmospheric chemistry and tries in particular to fill gaps in the data base of atmospheric reactions. It studies the nitrate radical reactions with chloroethenes and with but-2-yne (2-butyne). The mechanisms and rate coefficients for the NO{sub 3}-initiated degradation of the chloroethenes and 2-butyne were investigated by means of the static reaction chamber and the fast flow-discharge technique. The reactions between the nitrate radical and the chloroethenes were studied at atmospheric pressure in a reaction chamber with synthetic air as bath gas. FTIR (Fourier Transform InfraRed spectroscopy) spectroscopy was used to follow the reactions and to identify the products. Products were observed for the reactions with (E)-1,2-dichloroethene and tetrachloroethene, although the absorption bands are weak. The alkyl peroxynitrate and nitrate compounds form very strong and characteristic absorption bands. The rate coefficients for the reactions between NO{sub 3} and the chloroethenes were investigated at room temperature by three different methods. The results are given in tables. 132 refs., 44 figs., 21 tabs.

  6. On the use of plant emitted volatile organic compounds for atmospheric chemistry simulation experiments

    Science.gov (United States)

    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

  7. The Atmospheric Chemistry of Methyl Chavicol (Estragole)

    Science.gov (United States)

    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

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

    Science.gov (United States)

    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.

  9. Atmospheric Circulation, Chemistry, and Infrared Spectra of Titan-like Exoplanets around Different Stellar Types

    Science.gov (United States)

    Lora, Juan M.; Kataria, Tiffany; Gao, Peter

    2018-01-01

    With the discovery of ever smaller and colder exoplanets, terrestrial worlds with hazy atmospheres must be increasingly considered. Our solar system’s Titan is a prototypical hazy planet, whose atmosphere may be representative of a large number of planets in our Galaxy. As a step toward characterizing such worlds, we present simulations of exoplanets that resemble Titan but orbit three different stellar hosts: G, K, and M dwarf stars. We use general circulation and photochemistry models to explore the circulation and chemistry of these Titan-like planets under varying stellar spectra, in all cases assuming a Titan-like insolation. Due to the strong absorption of visible light by atmospheric haze, the redder radiation accompanying later stellar types produces more isothermal stratospheres, stronger meridional temperature gradients at mbar pressures, and deeper and stronger zonal winds. In all cases, the planets’ atmospheres are strongly superrotating, but meridional circulation cells are weaker aloft under redder starlight. The photochemistry of hydrocarbon and nitrile species varies with stellar spectra, with variations in the FUV/NUV flux ratio playing an important role. Our results tentatively suggest that column haze production rates could be similar under all three hosts, implying that planets around many different stars could have similar characteristics to Titan’s atmosphere. Lastly, we present theoretical emission spectra. Overall, our study indicates that, despite important and subtle differences, the circulation and chemistry of Titan-like exoplanets are relatively insensitive to differences in the host star. These findings may be further probed with future space-based facilities, like WFIRST, LUVOIR, HabEx, and OST.

  10. Atmospheric Constraints on the Surface UV Environment of Mars at 3.9 Ga Relevant to Prebiotic Chemistry

    Science.gov (United States)

    Ranjan, Sukrit; Wordsworth, Robin; Sasselov, Dimitar D.

    2017-08-01

    Recent findings suggest that Mars may have been a clement environment for the emergence of life and may even have compared favorably to Earth in this regard. These findings have revived interest in the hypothesis that prebiotically important molecules or even nascent life may have formed on Mars and been transferred to Earth. UV light plays a key role in prebiotic chemistry. Characterizing the early martian surface UV environment is key to understanding how Mars compares to Earth as a venue for prebiotic chemistry. Here, we present two-stream, multilayer calculations of the UV surface radiance on Mars at 3.9 Ga to constrain the surface UV environment as a function of atmospheric state. We explore a wide range of atmospheric pressures, temperatures, and compositions that correspond to the diversity of martian atmospheric states consistent with available constraints. We include the effects of clouds and dust. We calculate dose rates to quantify the effect of different atmospheric states on UV-sensitive prebiotic chemistry. We find that, for normative clear-sky CO2-H2O atmospheres, the UV environment on young Mars is comparable to young Earth. This similarity is robust to moderate cloud cover; thick clouds (τcloud ≥ 100) are required to significantly affect the martian UV environment, because cloud absorption is degenerate with atmospheric CO2. On the other hand, absorption from SO2, H2S, and dust is nondegenerate with CO2, meaning that, if these constituents build up to significant levels, surface UV fluence can be suppressed. These absorbers have spectrally variable absorption, meaning that their presence affects prebiotic pathways in different ways. In particular, high SO2 environments may admit UV fluence that favors pathways conducive to abiogenesis over pathways unfavorable to it. However, better measurements of the spectral quantum yields of these pathways are required to evaluate this hypothesis definitively.

  11. The Chemistry of Atmosphere-Forest Exchange (CAFE Model – Part 2: Application to BEARPEX-2007 observations

    Directory of Open Access Journals (Sweden)

    G. M. Wolfe

    2011-02-01

    Full Text Available In a companion paper, we introduced the Chemistry of Atmosphere-Forest Exchange (CAFE model, a vertically-resolved 1-D chemical transport model designed to probe the details of near-surface reactive gas exchange. Here, we apply CAFE to noontime observations from the 2007 Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX-2007. In this work we evaluate the CAFE modeling approach, demonstrate the significance of in-canopy chemistry for forest-atmosphere exchange and identify key shortcomings in the current understanding of intra-canopy processes.

    CAFE generally reproduces BEARPEX-2007 observations but requires an enhanced radical recycling mechanism to overcome a factor of 6 underestimate of hydroxyl (OH concentrations observed during a warm (~29 °C period. Modeled fluxes of acyl peroxy nitrates (APN are quite sensitive to gradients in chemical production and loss, demonstrating that chemistry may perturb forest-atmosphere exchange even when the chemical timescale is long relative to the canopy mixing timescale. The model underestimates peroxy acetyl nitrate (PAN fluxes by 50% and the exchange velocity by nearly a factor of three under warmer conditions, suggesting that near-surface APN sinks are underestimated relative to the sources. Nitric acid typically dominates gross dry N deposition at this site, though other reactive nitrogen (NOy species can comprise up to 28% of the N deposition budget under cooler conditions. Upward NO2 fluxes cause the net above-canopy NOy flux to be ~30% lower than the gross depositional flux. CAFE under-predicts ozone fluxes and exchange velocities by ~20%. Large uncertainty in the parameterization of cuticular and ground deposition precludes conclusive attribution of non-stomatal fluxes to chemistry or surface uptake. Model-measurement comparisons of vertical concentration gradients for several emitted species suggests that the lower canopy airspace may be

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

    Science.gov (United States)

    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.

  13. The atmospheric chemistry of methyl salicylate - reactions with atomic chlorine and with ozone

    Energy Technology Data Exchange (ETDEWEB)

    Canosa-Mas, C.E.; Duffy, J.M.; Thompson, K.C.; Wayne, R.P. [Physical and Theoretical Chemical Lab., Oxford (United Kingdom); King, M.D. [King' s College, London (United Kingdom). Dept. of Chemistry

    2002-05-01

    Methyl salicylate is one of a number of semiochemicals, signal molecules, emitted by herbivore-infested plants. These signal molecules attract predators of the herbivore, and the chemicals thus act indirectly as part of the defence mechanism of the plant. Previous studies have shown that ozone damage to plants can also elicit the emission of signal molecules. The fate of these signal molecules in the atmosphere is not known. Preliminary studies have been undertaken to examine the atmospheric chemistry of methyl salicylate for the first time. Rate coefficients for the reaction of methyl salicylate with atomic chlorine and with ozone have been determined; the values are (2.8()+-(0.3)x10{sup -12} and )approx4x10{sup -21} cm{sup 3} molecule{sup -1} s{sup -1}. These results suggest that neither reaction with atomic chlorine nor reaction with ozone will provide important loss routes for methyl salicylate in the atmosphere. The possible importance of photolysis of methyl salicylate in the atmosphere is considered. (Author)

  14. The atmospheric chemistry of methyl salicylate—reactions with atomic chlorine and with ozone

    Science.gov (United States)

    Canosa-Mas, Carlos E.; Duffy, Justin M.; King, Martin D.; Thompson, Katherine C.; Wayne, Richard P.

    Methyl salicylate is one of a number of semiochemicals, signal molecules, emitted by herbivore-infested plants. These signal molecules attract predators of the herbivore, and the chemicals thus act indirectly as part of the defence mechanism of the plant. Previous studies have shown that ozone damage to plants can also elicit the emission of signal molecules. The fate of these signal molecules in the atmosphere is not known. Preliminary studies have been undertaken to examine the atmospheric chemistry of methyl salicylate for the first time. Rate coefficients for the reaction of methyl salicylate with atomic chlorine and with ozone have been determined; the values are (2.8±0.3)×10 -12 and ˜4×10 -21 cm 3 molecule -1 s -1. These results suggest that neither reaction with atomic chlorine nor reaction with ozone will provide important loss routes for methyl salicylate in the atmosphere. The possible importance of photolysis of methyl salicylate in the atmosphere is considered.

  15. A short overview of the microbial population in clouds: Potential roles in atmospheric chemistry and nucleation processes

    Science.gov (United States)

    Delort, Anne-Marie; Vaïtilingom, Mickael; Amato, Pierre; Sancelme, Martine; Parazols, Marius; Mailhot, Gilles; Laj, Paolo; Deguillaume, Laurent

    2010-11-01

    Recent studies showed that living microorganisms, including bacteria, fungi and yeasts, are present in the atmospheric water phase (fog and clouds) and their role in chemical processes may have been underestimated. At the interface between atmospheric science and microbiology, information about this field of science suffers from the fact that not all recent findings are efficiently conveyed to both scientific communities. The purpose of this paper is therefore to provide a short overview of recent work linked to living organisms in the atmospheric water phase, from their activation to cloud droplets and ice crystal, to their potential impact on atmospheric chemical processes. This paper is focused on the microorganisms present in clouds and on the role they could play in atmospheric chemistry and nucleation processes. First, the life cycle of microorganisms via the atmosphere is examined, including their aerosolization from sources, their integration into clouds and their wet deposition on the ground. Second, special attention is paid to the possible impacts of microorganisms on liquid and ice nucleation processes. Third, a short description of the microorganisms that have been found in clouds and their variability in numbers and diversity is presented, emphasizing some specific characteristics that could favour their occurrence in cloud droplets. In the last section, the potential role of microbial activity as an alternative route to photochemical reaction pathways in cloud chemistry is discussed.

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

    Directory of Open Access Journals (Sweden)

    G. Sarwar

    2013-10-01

    Full Text Available 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, RACM2 enhances the domain-wide monthly mean hydroxyl radical concentrations by 46% and nitric acid by 26%. However, it reduces hydrogen peroxide by 2%, peroxyacetic acid by 94%, methyl hydrogen peroxide by 19%, peroxyacetyl nitrate by 40%, and organic nitrate by 41%. RACM2 enhances ozone compared to CB05TU at all ambient levels. Although it exhibited greater overestimates at lower observed concentrations, it displayed an improved performance at higher observed concentrations. The RACM2 ozone predictions are also supported by increased ozone production efficiency that agrees better with observations. Compared to CB05TU, RACM2 enhances the domain-wide monthly mean sulfate by 10%, nitrate by 6%, ammonium by 10%, anthropogenic secondary organic aerosols by 42%, biogenic secondary organic aerosols by 5%, and in-cloud secondary organic aerosols by 7%. Increased inorganic and organic aerosols with RACM2 agree better with observed data. Any air pollution control strategies developed using the two mechanisms do not differ appreciably.

  17. Aqueous organic chemistry in the atmosphere: sources and chemical processing of organic aerosols.

    Science.gov (United States)

    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.

  18. The influence of small-scale variations in isoprene concentrations on atmospheric chemistry over a tropical rainforest

    Directory of Open Access Journals (Sweden)

    T. A. M. Pugh

    2011-05-01

    Full Text Available Biogenic volatile organic compounds (BVOCs such as isoprene constitute a large proportion of the global atmospheric oxidant sink. Their reactions in the atmosphere contribute to processes such as ozone production and secondary organic aerosol formation. However, over the tropical rainforest, where 50 % of the global emissions of BVOCs are believed to occur, atmospheric chemistry models have been unable to simulate concurrently the measured daytime concentration of isoprene and that of its principal oxidant, hydroxyl (OH. One reason for this model-measurement discrepancy may be incomplete mixing of isoprene within the convective boundary layer, leading to patchiness or segregation in isoprene and OH mixing ratios and average concentrations that appear to be incompatible with each other. One way of capturing this effect in models of atmospheric chemistry is to use a reduced effective rate constant for their reaction. Recent studies comparing atmospheric chemistry global/box models with field measurements have suggested that this effective rate reduction may be as large as 50 %; which is at the upper limit of that calculated using large eddy simulation models. To date there has only been one field campaign worldwide that has reported co-located measurements of isoprene and OH at the necessary temporal resolution to calculate the segregation of these compounds. However many campaigns have recorded sufficiently high resolution isoprene measurements to capture the small-scale fluctuations in its concentration. Assuming uniform distributions of other OH production and loss processes, we use a box model of atmospheric chemistry, constrained by the spectrum of isoprene concentrations measured, as a virtual instrument, to estimate the variability in OH at a point and hence, to estimate the segregation intensity of isoprene and OH from high-frequency isoprene time series. The method successfully reproduces the only directly observed segregation, using

  19. Oxidation of a new Biogenic VOC: Chamber Studies of the Atmospheric Chemistry of Methyl Chavicol

    Science.gov (United States)

    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.

  20. Development of a Grid-Independent Geos-Chem Chemical Transport Model (v9-02) as an Atmospheric Chemistry Module for Earth System Models

    Science.gov (United States)

    Long, M. S.; Yantosca, R.; Nielsen, J. E; Keller, C. A.; Da Silva, A.; Sulprizio, M. P.; Pawson, S.; Jacob, D. J.

    2015-01-01

    The GEOS-Chem global chemical transport model (CTM), used by a large atmospheric chemistry research community, has been re-engineered to also serve as an atmospheric chemistry module for Earth system models (ESMs). This was done using an Earth System Modeling Framework (ESMF) interface that operates independently of the GEOSChem scientific code, permitting the exact same GEOSChem code to be used as an ESM module or as a standalone CTM. In this manner, the continual stream of updates contributed by the CTM user community is automatically passed on to the ESM module, which remains state of science and referenced to the latest version of the standard GEOS-Chem CTM. A major step in this re-engineering was to make GEOS-Chem grid independent, i.e., capable of using any geophysical grid specified at run time. GEOS-Chem data sockets were also created for communication between modules and with external ESM code. The grid-independent, ESMF-compatible GEOS-Chem is now the standard version of the GEOS-Chem CTM. It has been implemented as an atmospheric chemistry module into the NASA GEOS- 5 ESM. The coupled GEOS-5-GEOS-Chem system was tested for scalability and performance with a tropospheric oxidant-aerosol simulation (120 coupled species, 66 transported tracers) using 48-240 cores and message-passing interface (MPI) distributed-memory parallelization. Numerical experiments demonstrate that the GEOS-Chem chemistry module scales efficiently for the number of cores tested, with no degradation as the number of cores increases. Although inclusion of atmospheric chemistry in ESMs is computationally expensive, the excellent scalability of the chemistry module means that the relative cost goes down with increasing number of cores in a massively parallel environment.

  1. CARBON-RICH GIANT PLANETS: ATMOSPHERIC CHEMISTRY, THERMAL INVERSIONS, SPECTRA, AND FORMATION CONDITIONS

    Energy Technology Data Exchange (ETDEWEB)

    Madhusudhan, Nikku [Department of Astrophysical Sciences, Princeton University, Princeton, NJ 08544 (United States); Mousis, Olivier [Institut UTINAM, CNRS-UMR 6213, Observatoire de Besancon, BP 1615, F-25010 Besancon Cedex (France); Johnson, Torrence V. [Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91109 (United States); Lunine, Jonathan I., E-mail: nmadhu@astro.princeton.edu [Department of Astronomy, Cornell University, Ithaca, NY 14853 (United States)

    2011-12-20

    The recent inference of a carbon-rich atmosphere, with C/O {>=} 1, in the hot Jupiter WASP-12b motivates the exotic new class of carbon-rich planets (CRPs). We report a detailed study of the atmospheric chemistry and spectroscopic signatures of carbon-rich giant (CRG) planets, the possibility of thermal inversions in their atmospheres, the compositions of icy planetesimals required for their formation via core accretion, and the apportionment of ices, rock, and volatiles in their envelopes. Our results show that CRG atmospheres probe a unique region in composition space, especially at high temperature (T). For atmospheres with C/O {>=} 1, and T {approx}> 1400 K in the observable atmosphere, most of the oxygen is bound up in CO, while H{sub 2}O is depleted and CH{sub 4} is enhanced by up to two or three orders of magnitude each, compared to equilibrium compositions with solar abundances (C/O = 0.54). These differences in the spectroscopically dominant species for the different C/O ratios cause equally distinct observable signatures in the spectra. As such, highly irradiated transiting giant exoplanets form ideal candidates to estimate atmospheric C/O ratios and to search for CRPs. We also find that the C/O ratio strongly affects the abundances of TiO and VO, which have been suggested to cause thermal inversions in highly irradiated hot Jupiter atmospheres. A C/O = 1 yields TiO and VO abundances of {approx}100 times lower than those obtained with equilibrium chemistry assuming solar abundances, at P {approx} 1 bar. Such a depletion is adequate to rule out thermal inversions due to TiO/VO even in the most highly irradiated hot Jupiters, such as WASP-12b. We estimate the compositions of the protoplanetary disk, the planetesimals, and the envelope of WASP-12b, and the mass of ices dissolved in the envelope, based on the observed atmospheric abundances. Adopting stellar abundances (C/O = 0.44) for the primordial disk composition and low-temperature formation conditions

  2. An evaluation of the Cray T3D programming paradigms in atmospheric chemistry/transport models

    NARCIS (Netherlands)

    J.G. Blom (Joke); C. Keßler (Carsten); J.G. Verwer (Jan)

    1996-01-01

    textabstractIn this paper we compare the different programming paradigms available on the Cray T3D for the implementation of a 3D prototype of an Atmospheric Chemistry/Transport Model. We discuss the amount of work needed to convert existing codes to the T3D and the portability of the resulting

  3. Trends in the chemistry of atmospheric deposition and surface waters in the Lake Maggiore catchment

    Directory of Open Access Journals (Sweden)

    M. Rogora

    2001-01-01

    Full Text Available The Lake Maggiore catchment is the area of Italy most affected by acid deposition. Trend analysis was performed on long-term (15-30 years series of chemical analyses of atmospheric deposition, four small rivers draining forested catchments and four high mountain lakes. An improvement in the quality of atmospheric deposition was detected, due to decreasing sulphate concentration and increasing pH. Similar trends were also found in high mountain lakes and in small rivers. Atmospheric deposition, however, is still providing a large and steady flux of nitrogen compounds (nitrate and ammonium which is causing increasing nitrogen saturation in forest ecosystems and increasing nitrate levels in rivers. Besides atmospheric deposition, an important factor controlling water acidification and recovery is the weathering of rocks and soils which may be influenced by climate warming. A further factor is the episodic deposition of Saharan calcareous dust which contributes significantly to base cation deposition. Keywords: trend, atmospheric deposition, nitrogen, stream water chemistry.

  4. Discharge physics and chemistry of a novel atmospheric pressure plasma source

    Energy Technology Data Exchange (ETDEWEB)

    Park, J.; Henins, I.; Hermann, J.W.; Selwyn, G.S.; Jeong, J.Y.; Hickis, R.

    1999-07-01

    The atmospheric pressure plasma jet (APPJ) is a unique plasma source operating at atmospheric pressure. The APPJ operates with RF power and produces a stable non-thermal discharge in capacitively-coupled configuration. The discharge is spatially and temporally homogeneous and provides a unique gas phase chemistry that is well suited for various applications including etching, film deposition, surface treatment and decontamination of chemical and biological warfare (CBW) agents. A theoretical model shows electron densities of 0.2--2 x 10{sup 11} cm{sup {minus}3} for a helium discharge at a power level of 3--30 W cm{sup {minus}3}. The APPJ also produces a large flux, equivalent of up to 10,000 monolayer s{sup {minus}1}, of chemically-active, atomic and metastable molecular species which can impinge surfaces several cm downstream of the confined source. In addition, the efforts are in progress to measure the electron density using microwave diagnostics and to benchmark the gas phase chemical model by using LIF and titration.

  5. Application of inorganic mass spectrometry to problems in atmospheric chemistry

    International Nuclear Information System (INIS)

    Kelly, W.R.

    1990-01-01

    The measurement of isotopes by thermal ionization mass spectrometry is a highly sensitive and accurate technique which can be used to determine the concentration of specific nuclides as well as the isotopic composition in environmental samples. The first application uses isotope dilution which makes possible the determination of all elements with two or more stable isotopes in all types of matrices. The second application is a very powerful and useful application in atmospheric chemistry because it permits the use of stable isotopes as definitive intentional tracers of emissions from high temperature combustion sources. The use of stable isotopes of S, Nd, Sm, and U in the study of visibility, deposition, and definitive tracing of emissions will be presented

  6. Chemistry-nuclear chemistry division. Progress report, October 1979-September 1980

    International Nuclear Information System (INIS)

    Ryan, R.R.

    1981-05-01

    This report presents the research and development programs pursued by the Chemistry-Nuclear Chemistry Division of the Los Alamos National Laboratory. Topics covered include advanced analytical methods, atmospheric chemistry and transport, biochemistry, biomedical research, element migration and fixation, inorganic chemistry, isotope separation and analysis, atomic and molecular collisions, molecular spectroscopy, muonic x rays, nuclear cosmochemistry, nuclear structure and reactions, radiochemical separations, theoretical chemistry, and unclassified weapons research

  7. Chemistry-nuclear chemistry division. Progress report, October 1979-September 1980

    Energy Technology Data Exchange (ETDEWEB)

    Ryan, R.R. (comp.)

    1981-05-01

    This report presents the research and development programs pursued by the Chemistry-Nuclear Chemistry Division of the Los Alamos National Laboratory. Topics covered include advanced analytical methods, atmospheric chemistry and transport, biochemistry, biomedical research, element migration and fixation, inorganic chemistry, isotope separation and analysis, atomic and molecular collisions, molecular spectroscopy, muonic x rays, nuclear cosmochemistry, nuclear structure and reactions, radiochemical separations, theoretical chemistry, and unclassified weapons research.

  8. Prebiotic chemistry and atmospheric warming of early Earth by an active young Sun

    Science.gov (United States)

    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.

  9. Prebiotic Chemistry and Atmospheric Warming of Early Earth by an Active Young Sun

    Science.gov (United States)

    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.

  10. Atmospheric chemistry of n-CxF2x+1CHO (x = 1, 2, 3, 4)

    DEFF Research Database (Denmark)

    Hurley, M. D.; Ball, J. C.; Wallington, T. J.

    2006-01-01

    Smog chamber/FTIR techniques were used to study the atmospheric fate of n-C(x)F(2)(x)(+1)C(O) (x = 1, 2, 3, 4) radicals in 700 Torr O(2)/N(2) diluent at 298 +/- 3 K. A competition is observed between reaction with O(2) to form n-C(x)()F(2)(x)()(+1)C(O)O(2) radicals and decomposition to form n-C(x...... to the atmospheric chemistry of n-C(x)F(2)(x)(+1)C(O) radicals and their possible role in contributing to the formation of perfluorocarboxylic acids in the environment....

  11. Results of an interactively coupled atmospheric chemistry - general circulation model. Comparison with observations

    Energy Technology Data Exchange (ETDEWEB)

    Hein, R.; Dameris, M.; Schnadt, C. [and others

    2000-01-01

    An interactively coupled climate-chemistry model which enables a simultaneous treatment of meteorology and atmospheric chemistry and their feedbacks is presented. This is the first model, which interactively combines a general circulation model based on primitive equations with a rather complex model of stratospheric and tropospheric chemistry, and which is computational efficient enough to allow long-term integrations with currently available computer resources. The applied model version extends from the Earth's surface up to 10 hPa with a relatively high number (39) of vertical levels. We present the results of a present-day (1990) simulation and compare it to available observations. We focus on stratospheric dynamics and chemistry relevant to describe the stratospheric ozone layer. The current model version ECHAM4.L39(DLR)/CHEM can realistically reproduce stratospheric dynamics in the Arctic vortex region, including stratospheric warming events. This constitutes a major improvement compared to formerly applied model versions. However, apparent shortcomings in Antarctic circulation and temperatures persist. The seasonal and interannual variability of the ozone layer is simulated in accordance with observations. Activation and deactivation of chlorine in the polar stratospheric vortices and their interhemispheric differences are reproduced. The consideration of the chemistry feedback on dynamics results in an improved representation of the spatial distribution of stratospheric water vapor concentrations, i.e., the simulated meriodional water vapor gradient in the stratosphere is realistic. The present model version constitutes a powerful tool to investigate, for instance, the combined direct and indirect effects of anthropogenic trace gas emissions, and the future evolution of the ozone layer. (orig.)

  12. Active Upper-atmosphere Chemistry and Dynamics from Polar Circulation Reversal on Titan

    Science.gov (United States)

    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.

  13. HIGH METALLICITY AND NON-EQUILIBRIUM CHEMISTRY IN THE DAYSIDE ATMOSPHERE OF HOT-NEPTUNE GJ 436b

    International Nuclear Information System (INIS)

    Madhusudhan, N.; Seager, S.

    2011-01-01

    We present a detailed analysis of the dayside atmosphere of the hot-Neptune GJ 436b, based on recent Spitzer observations. We report statistical constraints on the thermal and chemical properties of the planetary atmosphere, study correlations between the various molecular species, and discuss scenarios of equilibrium and non-equilibrium chemistry in GJ 436b. We model the atmosphere with a one-dimensional line-by-line radiative transfer code with parameterized molecular abundances and temperature structure. We explore the model parameter space with 10 6 models, using a Markov chain Monte Carlo scheme. Our results encompass previous findings, indicating a paucity of methane, an overabundance of CO and CO 2 , and a slight underabundance of H 2 O, as compared to equilibrium chemistry with solar metallicity. The concentrations of the species are highly correlated. Our best-fit, and most plausible, constraints require a CH 4 mixing ratio of 10 -7 to10 -6 , with CO ≥10 -3 , CO 2 ∼10 -6 to10 -4 , and H 2 O ≤10 -4 ; higher CH 4 would require much higher CO and CO 2 . Based on calculations of equilibrium and non-equilibrium chemistry, we find that the observed abundances can potentially be explained by a combination of high metallicity (∼10x solar) and vertical mixing with K zz ∼ 10 6 -10 7 cm 2 s -1 . The inferred metallicity is enhanced over that of the host star which is known to be consistent with solar metallicity. Our constraints rule out a dayside thermal inversion in GJ 436b. We emphasize that the constraints reported in this work depend crucially on the observations in the two Spitzer channels at 3.6 μm and 4.5 μm. Future observations with warm Spitzer and with the James Webb Space Telescope will be extremely important to improve upon the present constraints on the abundances of carbon species in the dayside atmosphere of GJ 436b.

  14. Response of lake chemistry to atmospheric deposition and climate in selected Class I wilderness areas in the western United States, 1993-2009

    Science.gov (United States)

    Mast, M. Alisa

    2011-01-01

    The U.S. Geological Survey, in cooperation with the U.S. Department of Agriculture Forest Service, Air Resource Management, conducted a study to evaluate long-term trends in lake-water chemistry for 64 high-elevation lakes in selected Class I wilderness areas in Colorado, Idaho, Utah, and Wyoming during 1993 to 2009. Understanding how and why lake chemistry is changing in mountain areas is essential for effectively managing and protecting high-elevation aquatic ecosystems. Trends in emissions, atmospheric deposition, and climate variables (air temperature and precipitation amount) were evaluated over a similar period of record. A main objective of the study was to determine if changes in atmospheric deposition of contaminants in the Rocky Mountain region have resulted in measurable changes in the chemistry of high-elevation lakes. A second objective was to investigate linkages between lake chemistry and air temperature and precipitation to improve understanding of the sensitivity of mountain lakes to climate variability.

  15. Implementation of the chemistry module MECCA (v2.5 in the modal aerosol version of the Community Atmosphere Model component (v3.6.33 of the Community Earth System Model

    Directory of Open Access Journals (Sweden)

    M. S. Long

    2013-02-01

    Full Text Available A coupled atmospheric chemistry and climate system model was developed using the modal aerosol version of the National Center for Atmospheric Research Community Atmosphere Model (modal-CAM; v3.6.33 and the Max Planck Institute for Chemistry's Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA; v2.5 to provide enhanced resolution of multiphase processes, particularly those involving inorganic halogens, and associated impacts on atmospheric composition and climate. Three Rosenbrock solvers (Ros-2, Ros-3, RODAS-3 were tested in conjunction with the basic load-balancing options available to modal-CAM (1 to establish an optimal configuration of the implicitly-solved multiphase chemistry module that maximizes both computational speed and repeatability of Ros-2 and RODAS-3 results versus Ros-3, and (2 to identify potential implementation strategies for future versions of this and similar coupled systems. RODAS-3 was faster than Ros-2 and Ros-3 with good reproduction of Ros-3 results, while Ros-2 was both slower and substantially less reproducible relative to Ros-3 results. Modal-CAM with MECCA chemistry was a factor of 15 slower than modal-CAM using standard chemistry. MECCA chemistry integration times demonstrated a systematic frequency distribution for all three solvers, and revealed that the change in run-time performance was due to a change in the frequency distribution of chemical integration times; the peak frequency was similar for all solvers. This suggests that efficient chemistry-focused load-balancing schemes can be developed that rely on the parameters of this frequency distribution.

  16. Evaluated kinetic and photochemical data for atmospheric chemistry: Volume V – heterogeneous reactions on solid substrates

    Directory of Open Access Journals (Sweden)

    J. N. Crowley

    2010-09-01

    Full Text Available This article, the fifth in the ACP journal series, presents data evaluated by the IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry. It covers the heterogeneous processes on surfaces of solid particles present in the atmosphere, for which uptake coefficients and adsorption parameters have been presented on the IUPAC website in 2010. The article consists of an introduction and guide to the evaluation, giving a unifying framework for parameterisation of atmospheric heterogeneous processes. We provide summary sheets containing the recommended uptake parameters for the evaluated processes. Four substantial appendices contain detailed data sheets for each process considered for ice, mineral dust, sulfuric acid hydrate and nitric acid hydrate surfaces, which provide information upon which the recommendations are made.

  17. Parameterization of dust emissions in the global atmospheric chemistry-climate model EMAC: impact of nudging and soil properties

    Science.gov (United States)

    Astitha, M.; Lelieveld, J.; Abdel Kader, M.; Pozzer, A.; de Meij, A.

    2012-11-01

    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. Two versions of a parameterization scheme to compute desert dust emissions are 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 two versions 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 versions 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. Approximately 70% of the modelled annual deposition data and 70-75% of the modelled monthly aerosol optical depth (AOD) in the Atlantic Ocean stations lay in the range 0.5 to 2 times the observations for all simulations. The two versions have similar performance, even though the total annual source differs by ~50%, which underscores the importance of transport and deposition processes (being the same for both versions). Even though the explicit soil particle size distribution is considered more realistic, the simpler scheme appears to perform better in several locations. This paper discusses the differences between the two versions of the dust emission scheme, focusing on their limitations and strengths in describing the global dust cycle and suggests possible future improvements.

  18. Parameterization of dust emissions in the global atmospheric chemistry-climate model EMAC: impact of nudging and soil properties

    Directory of Open Access Journals (Sweden)

    M. Astitha

    2012-11-01

    Full Text Available 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. Two versions of a parameterization scheme to compute desert dust emissions are 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 two versions 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 versions 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. Approximately 70% of the modelled annual deposition data and 70–75% of the modelled monthly aerosol optical depth (AOD in the Atlantic Ocean stations lay in the range 0.5 to 2 times the observations for all simulations. The two versions have similar performance, even though the total annual source differs by ~50%, which underscores the importance of transport and deposition processes (being the same for both versions. Even though the explicit soil particle size distribution is considered more realistic, the simpler scheme appears to perform better in several locations. This paper discusses the differences between the two versions of the dust emission scheme, focusing on their limitations and strengths in describing the global dust cycle and suggests possible future improvements.

  19. Upper atmosphere research satellite program. [to study the chemistry energetics, and dynamics

    Science.gov (United States)

    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.

  20. Preface to the Special Issue on Climate-Chemistry Interactions: Atmospheric Ozone, Aerosols, and Clouds over East Asia

    Directory of Open Access Journals (Sweden)

    Wei-Chyung Wang and Jen-Ping Chen

    2007-01-01

    Full Text Available Atmospheric radiatively-important chemical constituents (e.g., O3 and aerosols are important to maintain the radiation balance of the Earth-atmosphere climate system, and changes in their concentration due to both natural causes and anthropogenic activities will induce climate changes. The distribution of these constituents is sensitive to the state of the climate (e.g., temperature, moisture, wind, and clouds. Therefore, rises in atmospheric temperature and water vapor, and changes in circulation and clouds in global warming can directly affect atmospheric chemistry with subsequent implications for these constituents. Although many coupling mechanisms are identified, the net effect of all these impacts on climate change is not well understood. In particular, changes in water vapor and clouds associated with the hydrologic cycle contain significant uncertainties.

  1. Untangling the Chemical Evolution of Titan's Atmosphere and Surface -- From Homogeneous to Heterogeneous Chemistry

    Energy Technology Data Exchange (ETDEWEB)

    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.

  2. Poster 6: Influence of traces elements in the organic chemistry of upper atmosphere of Titan

    Science.gov (United States)

    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.

  3. Simulating atmospheric composition over a South-East Asian tropical rainforest: performance of a chemistry box model

    Directory of Open Access Journals (Sweden)

    T. A. M. Pugh

    2010-01-01

    Full Text Available Atmospheric composition and chemistry above tropical rainforests is currently not well established, particularly for south-east Asia. In order to examine our understanding of chemical processes in this region, the performance of a box model of atmospheric boundary layer chemistry is tested against measurements made at the top of the rainforest canopy near Danum Valley, Malaysian Borneo. Multi-variate optimisation against ambient concentration measurements was used to estimate average canopy-scale emissions for isoprene, total monoterpenes and nitric oxide. The excellent agreement between estimated values and measured fluxes of isoprene and total monoterpenes provides confidence in the overall modelling strategy, and suggests that this method may be applied where measured fluxes are not available, assuming that the local chemistry and mixing are adequately understood. The largest contributors to the optimisation cost function at the point of best-fit are OH (29%, NO (22% and total peroxy radicals (27%. Several factors affect the modelled VOC chemistry. In particular concentrations of methacrolein (MACR and methyl-vinyl ketone (MVK are substantially overestimated, and the hydroxyl radical (OH concentration is substantially underestimated; as has been seen before in tropical rainforest studies. It is shown that inclusion of dry deposition of MACR and MVK and wet deposition of species with high Henry's Law values substantially improves the fit of these oxidised species, whilst also substantially decreasing the OH sink. Increasing OH production arbitrarily, through a simple OH recycling mechanism , adversely affects the model fit for volatile organic compounds (VOCs. Given the constraints on isoprene flux provided by measurements, a substantial decrease in the rate of reaction of VOCs with OH is the only remaining option to explain the measurement/model discrepancy for OH. A reduction in the isoprene+OH rate constant of 50%, in conjunction with

  4. Chemical kinetics and modeling of planetary atmospheres

    Science.gov (United States)

    Yung, Yuk L.

    1990-01-01

    A unified overview is presented for chemical kinetics and chemical modeling in planetary atmospheres. The recent major advances in the understanding of the chemistry of the terrestrial atmosphere make the study of planets more interesting and relevant. A deeper understanding suggests that the important chemical cycles have a universal character that connects the different planets and ultimately link together the origin and evolution of the solar system. The completeness (or incompleteness) of the data base for chemical kinetics in planetary atmospheres will always be judged by comparison with that for the terrestrial atmosphere. In the latter case, the chemistry of H, O, N, and Cl species is well understood. S chemistry is poorly understood. In the atmospheres of Jovian planets and Titan, the C-H chemistry of simple species (containing 2 or less C atoms) is fairly well understood. The chemistry of higher hydrocarbons and the C-N, P-N chemistry is much less understood. In the atmosphere of Venus, the dominant chemistry is that of chlorine and sulfur, and very little is known about C1-S coupled chemistry. A new frontier for chemical kinetics both in the Earth and planetary atmospheres is the study of heterogeneous reactions. The formation of the ozone hole on Earth, the ubiquitous photochemical haze on Venus and in the Jovian planets and Titan all testify to the importance of heterogeneous reactions. It remains a challenge to connect the gas phase chemistry to the production of aerosols.

  5. Simulation of comprehensive chemistry and atmospheric methane lifetime in the LGM with EMAC

    Science.gov (United States)

    Gromov, Sergey; Steil, Benedikt

    2017-04-01

    Past records of atmospheric methane (CH4) abundance/isotope composition may provide a substantial insight on C exchanges in the Earth System (ES). When simulated in the climate models, CH4 helps to identify climate parameters transitions via triggering of its different (natural) sources, with a proviso that its sinks are adequately represented in the model. The latter are still a matter of large uncertainty in the studies focussing on the interpretation of CH4 evolution throughout Last Glacial Maximum (LGM), judging the conferred span of tropospheric CH4 lifetime (λ) of 3-16 yr [1-4]. In this study, we attempt to: (i) deliver the most adequate estimate of the LGM atmospheric sink of CH4 in the EMAC AC-GCM [5] equipped with the comprehensive representation of atmospheric chemistry [6], (ii) reveal the ES and CH4 emission parameters that are most influential for λ and (iii) based on these findings, suggest a parameterisation for λ that may be consistently used in climate models. In pursuing (i) we have tuned the EMAC model for simulating LGM atmospheric chemistry state, including careful revisiting of the trace gases emissions from the biosphere, biomass burning/lightning source, etc. The latter affect the key simulated component bound with λ, viz. the abundance and distribution of the hydroxyl radicals (OH) which, upon reacting with CH4, constitute its main tropospheric sink. Our preliminary findings suggest that OH is buffered in the atmosphere in a similar fashion to preindustrial climate, which in line with the recent studies employing comprehensive chemistry mechanisms (e.g., [3]). The analysis in (ii) suggests that tropospheric λ values may be qualitatively described as a convolution of values typical for zonal domain with high and low photolytic recycling rates (i.e. tropics and extra-tropics), as in the latter a dependence of the zonal average λ value on the CH4 emission strength exists. We further use the extensive diagnostic in EMAC to infer the

  6. Atmospheric pollution. From processes to modelling

    International Nuclear Information System (INIS)

    Sportisse, B.

    2008-01-01

    Air quality, greenhouse effect, ozone hole, chemical or nuclear accidents.. All these phenomena are tightly linked to the chemical composition of atmosphere and to the atmospheric dispersion of pollutants. This book aims at supplying the main elements of understanding of 'atmospheric pollutions': stakes, physical processes involved, role of scientific expertise in decision making. Content: 1 - classifications and scales: chemical composition of the atmosphere, vertical structure, time scales (transport, residence); 2 - matter/light interaction: notions of radiative transfer, application to the Earth's atmosphere; 3 - some elements about the atmospheric boundary layer: notion of scales in meteorology, atmospheric boundary layer (ABL), thermal stratification and stability, description of ABL turbulence, elements of atmospheric dynamics, some elements about the urban climate; 4 - notions of atmospheric chemistry: characteristics, ozone stratospheric chemistry, ozone tropospheric chemistry, brief introduction to indoor air quality; 5 - aerosols, clouds and rains: aerosols and particulates, aerosols and clouds, acid rains and leaching; 6 - towards numerical simulation: equation of reactive dispersion, numerical methods for chemistry-transport models, numerical resolution of the general equation of aerosols dynamics (GDE), modern simulation chains, perspectives. (J.S.)

  7. Investigating the Chemical Pathways to PAH- and PANH-Based Aerosols in Titan's Atmospheric chemistry

    Science.gov (United States)

    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.

  8. Jovian atmospheres

    International Nuclear Information System (INIS)

    Allison, M.; Travis, L.D.

    1986-10-01

    A conference on the atmosphere of Jupiter produced papers in the areas of thermal and ortho-para hydrogen structure, clouds and chemistry, atmospheric structure, global dynamics, synoptic features and processes, atmospheric dynamics, and future spaceflight opportunities. A session on the atmospheres of Uranus and Neptune was included, and the atmosphere of Saturn was discussed in several papers

  9. Chemistry-Nuclear Chemistry Division. Progress report, October 1980-September 1981

    International Nuclear Information System (INIS)

    Ryan, R.R.

    1982-05-01

    This report describes major progress in the research and development programs pursued by the Chemistry-Nuclear Chemistry Division of the Los Alamos National Laboratory during FY 1981. Topics covered include advanced analytical methods, atmospheric chemistry and transport, biochemistry, biomedical research, medical radioisotopes research, element migration and fixation, nuclear waste isolation research, inorganic and structural chemistry, isotope separation, analysis and applications, the newly established Nuclear Magnetic Resonance Center, atomic and molecular collisions, molecular spectroscopy, nuclear cosmochemistry, nuclear structure and reactions, pion charge exchange, radiochemical separations, theoretical chemistry, and unclassified weapons research

  10. Chemistry-Nuclear Chemistry Division. Progress report, October 1980-September 1981

    Energy Technology Data Exchange (ETDEWEB)

    Ryan, R.R. (comp.)

    1982-05-01

    This report describes major progress in the research and development programs pursued by the Chemistry-Nuclear Chemistry Division of the Los Alamos National Laboratory during FY 1981. Topics covered include advanced analytical methods, atmospheric chemistry and transport, biochemistry, biomedical research, medical radioisotopes research, element migration and fixation, nuclear waste isolation research, inorganic and structural chemistry, isotope separation, analysis and applications, the newly established Nuclear Magnetic Resonance Center, atomic and molecular collisions, molecular spectroscopy, nuclear cosmochemistry, nuclear structure and reactions, pion charge exchange, radiochemical separations, theoretical chemistry, and unclassified weapons research.

  11. Atmospheric chemistry of CF3O radicals: Reaction with H2O

    DEFF Research Database (Denmark)

    Wallington, T.J.; Hurley, M.D.; Schneider, W.F.

    1993-01-01

    Evidence is presented that CF3O radicals react with H2O in the gas phase at 296 K to give CF3OH and OH radicals. This reaction is calculated to be exothermic by 1.7 kcal mol-I implying a surprisingly strong CF3O-H bond energy of 120 +/- 3 kcal mol-1. Results from a relative rate experimental study...... suggest that the rate constant for the reaction of CF3O radicals with H2O lies in the range (0.2-4.0) X 10(-17) cm3 molecule-1 s-1. Implications for the atmospheric chemistry of CF3O radicals are discussed....

  12. Modeling emissions for three-dimensional atmospheric chemistry transport models.

    Science.gov (United States)

    Matthias, Volker; Arndt, Jan A; Aulinger, Armin; Bieser, Johannes; Denier Van Der Gon, Hugo; Kranenburg, Richard; Kuenen, Jeroen; Neumann, Daniel; Pouliot, George; Quante, Markus

    2018-01-24

    Poor air quality is still a threat for human health in many parts of the world. In order to assess measures for emission reductions and improved air quality, three-dimensional atmospheric chemistry transport modeling systems are used in numerous research institutions and public authorities. These models need accurate emission data in appropriate spatial and temporal resolution as input. This paper reviews the most widely used emission inventories on global and regional scale and looks into the methods used to make the inventory data model ready. Shortcomings of using standard temporal profiles for each emission sector are discussed and new methods to improve the spatio-temporal distribution of the emissions are presented. These methods are often neither top-down nor bottom-up approaches but can be seen as hybrid methods that use detailed information about the emission process to derive spatially varying temporal emission profiles. These profiles are subsequently used to distribute bulk emissions like national totals on appropriate grids. The wide area of natural emissions is also summarized and the calculation methods are described. Almost all types of natural emissions depend on meteorological information, which is why they are highly variable in time and space and frequently calculated within the chemistry transport models themselves. The paper closes with an outlook for new ways to improve model ready emission data, for example by using external databases about road traffic flow or satellite data to determine actual land use or leaf area. In a world where emission patterns change rapidly, it seems appropriate to use new types of statistical and observational data to create detailed emission data sets and keep emission inventories up-to-date. Emission data is probably the most important input for chemistry transport model (CTM) systems. It needs to be provided in high temporal and spatial resolution and on a grid that is in agreement with the CTM grid. Simple

  13. Nitrogen Fixation by Photochemistry in the Atmosphere of Titan and Implications for Prebiotic Chemistry

    Science.gov (United States)

    Balucani, Nadia

    The observation of N-containing organic molecules and the composition of the haze aerosols, as determined by the Aerosol Collector and Pyrolyser (ACP) on-board Huygens, are clear indications that some chemistry involving nitrogen active forms and hydrocarbons is operative in the upper atmosphere of Titan. Neutral-neutral reactions involving the first electronically excited state of atomic nitrogen, N(2D), and small hydrocarbons have the right prerequisites to be among the most significant pathways to formation of nitriles, imines and other simple N-containing organic molecules. The closed-shell products methanimine, ethanimine, ketenimine, 2H-azirine and the radical products CH3N, HCCN and CH2NCH can be the intermediate molecular species that, via addition reactions, polymerization and copolymerization form the N-rich organic aerosols of Titan as well as tholins in bulk reactors simulating Titan's atmosphere.

  14. Organic chemistry in Titan's upper atmosphere and its astrobiological consequences: I. Views towards Cassini plasma spectrometer (CAPS) and ion neutral mass spectrometer (INMS) experiments in space

    Science.gov (United States)

    Ali, A.; Sittler, E. C.; Chornay, D.; Rowe, B. R.; Puzzarini, C.

    2015-05-01

    The discovery of carbocations and carbanions by Ion Neutral Mass Spectrometer (INMS) and the Cassini Plasma Spectrometer (CAPS) instruments onboard the Cassini spacecraft in Titan's upper atmosphere is truly amazing for astrochemists and astrobiologists. In this paper we identify the reaction mechanisms for the growth of the complex macromolecules observed by the CAPS Ion Beam Spectrometer (IBS) and Electron Spectrometer (ELS). This identification is based on a recently published paper (Ali et al., 2013. Planet. Space Sci. 87, 96) which emphasizes the role of Olah's nonclassical carbonium ion chemistry in the synthesis of the organic molecules observed in Titan's thermosphere and ionosphere by INMS. The main conclusion of that work was the demonstration of the presence of the cyclopropenyl cation - the simplest Huckel's aromatic molecule - and its cyclic methyl derivatives in Titan's atmosphere at high altitudes. In this study, we present the transition from simple aromatic molecules to the complex ortho-bridged bi- and tri-cyclic hydrocarbons, e.g., CH2+ mono-substituted naphthalene and phenanthrene, as well as the ortho- and peri-bridged tri-cyclic aromatic ring, e.g., perinaphthenyl cation. These rings could further grow into tetra-cyclic and the higher order ring polymers in Titan's upper atmosphere. Contrary to the pre-Cassini observations, the nitrogen chemistry of Titan's upper atmosphere is found to be extremely rich. A variety of N-containing hydrocarbons including the N-heterocycles where a CH group in the polycyclic rings mentioned above is replaced by an N atom, e.g., CH2+ substituted derivative of quinoline (benzopyridine), are found to be dominant in Titan's upper atmosphere. The mechanisms for the formation of complex molecular anions are discussed as well. It is proposed that many closed-shell complex carbocations after their formation first, in Titan's upper atmosphere, undergo the kinetics of electron recombination to form open-shell neutral

  15. Atmospheric impact of the 1783–1784 Laki eruption: Part I Chemistry modelling

    Directory of Open Access Journals (Sweden)

    D. S. Stevenson

    2003-01-01

    Full Text Available Results from the first chemistry-transport model study of the impact of the 1783–1784 Laki fissure eruption (Iceland: 64°N, 17°W upon atmospheric composition are presented. The eruption released an estimated 61 Tg(S as SO2 into the troposphere and lower stratosphere. The model has a high resolution tropopause region, and detailed sulphur chemistry. The simulated SO2 plume spreads over much of the Northern Hemisphere, polewards of ~40°N. About 70% of the SO2 gas is directly deposited to the surface before it can be oxidised to sulphuric acid aerosol. The main SO2 oxidants, OH and H2O2, are depleted by up to 40% zonally, and the lifetime of SO2 consequently increases. Zonally averaged tropospheric SO2 concentrations over the first three months of the eruption exceed 20 ppbv, and sulphuric acid aerosol reaches ~2 ppbv. These compare to modelled pre-industrial/present-day values of 0.1/0.5 ppbv SO2 and 0.1/1.0 ppbv sulphate. A total sulphuric acid aerosol yield of 17–22 Tg(S is produced. The mean aerosol lifetime is 6–10 days, and the peak aerosol loading of the atmosphere is 1.4–1.7 Tg(S (equivalent to 5.9–7.1 Tg of hydrated sulphuric acid aerosol. These compare to modelled pre-industrial/present-day sulphate burdens of 0.28/0.81 Tg(S, and lifetimes of 6/5 days, respectively. Due to the relatively short atmospheric residence times of both SO2 and sulphate, the aerosol loading approximately mirrors the temporal evolution of emissions associated with the eruption. The model produces a reason-able simulation of the acid deposition found in Greenland ice cores. These results appear to be relatively insensitive to the vertical profile of emissions assumed, although if more of the emissions reached higher levels (>12 km, this would give longer lifetimes and larger aerosol yields. Introducing the emissions in episodes generates similar results to using monthly mean emissions, because the atmospheric lifetimes are similar to the repose periods

  16. The ENVISAT Atmospheric Chemistry mission (GOMOS, MIPAS and SCIAMACHY) -Instrument status and mission evolution

    Science.gov (United States)

    Dehn, Angelika

    The ENVISAT ESA's satellite was launched on a polar orbit on March 2002. It carries on-board three atmospheric chemistry instruments: GOMOS, MIPAS and SCIAMACHY [1]. At the present time, although the mission expected lifetime of 5 years has been already exceeded, all the payload modules are in good to excellent status. The only limiting factor is the available fuel that is used for orbit control manoeuvre. A new strategy was proposed [2] that will allow to save fuel and to extend the mission up to 2013. Following this strategy, the altitude of the orbit will be lowered by 17 km starting from end of 2010 and the inclination will be allowed to drift. The new orbit scenario will result in a new repeating cycle with a variation of the Mean Local Solar Time (MLST). This will have an impact on both the in-flight operations, on the science data and on the mission. The simulations carried out for the atmospheric chemistry instruments show that the new orbit strategy will neither have a significant impact in the instrument operations nor on the quality of the science data. Therefore we expect that the atmospheric mission will continue nominally until the end of the platform life time, providing to the scientist a unique dataset of the most important geophysical parameters (e.g., trace gases, clouds, and aerosol) spanning a time interval of about 11 years. The aim of this paper is to review the overall ENVISAT atmospheric mission status for the past, present and future. The evolution of the instrument performances since launch will be analyzed with focus on the life-limited items monitoring. The tuning of the instrument in-flight operations decided to cope with instrument degradation or scientific needs will be described. The lessons learned on how to operate and monitor the instruments will be highlighted. Finally the expected evolution of the instrument performances until the ENVISAT end-of-life will be discussed. [1] H. Nett, J. Frerick, T. Paulsen, and G. Levrini, "The

  17. The Chemistry of Atmosphere-Forest Exchange (CAFE Model – Part 1: Model description and characterization

    Directory of Open Access Journals (Sweden)

    G. M. Wolfe

    2011-01-01

    Full Text Available We present the Chemistry of Atmosphere-Forest Exchange (CAFE model, a vertically-resolved 1-D chemical transport model designed to probe the details of near-surface reactive gas exchange. CAFE integrates all key processes, including turbulent diffusion, emission, deposition and chemistry, throughout the forest canopy and mixed layer. CAFE utilizes the Master Chemical Mechanism (MCM and is the first model of its kind to incorporate a suite of reactions for the oxidation of monoterpenes and sesquiterpenes, providing a more comprehensive description of the oxidative chemistry occurring within and above the forest. We use CAFE to simulate a young Ponderosa pine forest in the Sierra Nevada, CA. Utilizing meteorological constraints from the BEARPEX-2007 field campaign, we assess the sensitivity of modeled fluxes to parameterizations of diffusion, laminar sublayer resistance and radiation extinction. To characterize the general chemical environment of this forest, we also present modeled mixing ratio profiles of biogenic hydrocarbons, hydrogen oxides and reactive nitrogen. The vertical profiles of these species demonstrate a range of structures and gradients that reflect the interplay of physical and chemical processes within the forest canopy, which can influence net exchange.

  18. 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

    Science.gov (United States)

    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

  19. Photochemistry of Planetary Atmospheres

    Science.gov (United States)

    Yung, Y. L.

    2005-12-01

    The Space Age started half a century ago. Today, with the completion of a fairly detailed study of the planets of the Solar System, we have begun studying exoplanets (or extrasolar planets). The overriding question in is to ask whether an exoplanet is habitable and harbors life, and if so, what the biosignatures ought to be. This forces us to confront the fundamental question of what controls the composition of an atmosphere. The composition of a planetary atmosphere reflects a balance between thermodynamic equilibrium chemistry (as in the interior of giant planets) and photochemistry (as in the atmosphere of Mars). The terrestrial atmosphere has additional influence from life (biochemistry). The bulk of photochemistry in planetary atmospheres is driven by UV radiation. Photosynthesis may be considered an extension of photochemistry by inventing a molecule (chlorophyll) that can harvest visible light. Perhaps the most remarkable feature of photochemistry is catalytic chemistry, the ability of trace amounts of gases to profoundly affect the composition of the atmosphere. Notable examples include HOx (H, OH and HO2) chemistry on Mars and chlorine chemistry on Earth and Venus. Another remarkable feature of photochemistry is organic synthesis in the outer solar system. The best example is the atmosphere of Titan. Photolysis of methane results in the synthesis of more complex hydrocarbons. The hydrocarbon chemistry inevitably leads to the formation of high molecular weight products, giving rise to aerosols when the ambient atmosphere is cool enough for them to condense. These results are supported by the findings of the recent Cassini mission. Lastly, photochemistry leaves a distinctive isotopic signature that can be used to trace back the evolutionary history of the atmosphere. Examples include nitrogen isotopes on Mars and sulfur isotopes on Earth. Returning to the question of biosignatures on an exoplanet, our Solar System experience tells us to look for speciation

  20. A two-dimensional atmospheric chemistry modeling investigation of Earth's Phanerozoic O3 and near-surface ultraviolet radiation history

    Science.gov (United States)

    Harfoot, Michael B. J.; Beerling, David J.; Lomax, Barry H.; Pyle, John A.

    2007-04-01

    We use the Cambridge two-dimensional (2-D) chemistry-radiation transport model to investigate the implications for column O3 and near-surface ultraviolet radiation (UV), of variations in atmospheric O2 content over the Phanerozoic (last 540 Myr). Model results confirm some earlier 1-D model investigations showing that global annual mean O3 column increases monotonically with atmospheric O2. Sensitivity studies indicate that changes in temperature and N2O exert a minor influence on O3 relative to O2. We reconstructed Earth's O3 history by interpolating the modeled relationship between O3 and O2 onto two Phanerozoic O2 histories. Our results indicate that the largest variation in Phanerozoic column O3 occurred between 400 and 200 Myr ago, corresponding to a rise in atmospheric O2 to ˜1.5 times the present atmospheric level (PAL) and subsequent fall to ˜0.5 PAL. The O3 response to this O2 decline shows latitudinal differences, thinning most at high latitudes (30-40 Dobson units (1 DU = 0.001 atm cm) at 66°N) and least at low latitudes (5-10 DU at 9°N) where a "self-healing" effect is evident. This O3 depletion coincides with significant increases in the near-surface biologically active UV radiation at high latitudes, +28% as weighted by the Thimijan spectral weighting function. O3 and UV changes were exacerbated when we incorporated a direct feedback of the terrestrial biosphere on atmospheric chemistry, through enhanced N2O production as the climate switched from an icehouse to a greenhouse mode. On the basis of a summary of field and laboratory experimental evidence, we suggest that these UV radiation increases may have exerted subtle rather than catastrophic effects on ecosystem processes.

  1. Titan: a laboratory for prebiological organic chemistry

    Science.gov (United States)

    Sagan, C.; Thompson, W. R.; Khare, B. N.

    1992-01-01

    When we examine the atmospheres of the Jovian planets (Jupiter, Saturn, Uranus, and Neptune), the satellites in the outer solar system, comets, and even--through microwave and infrared spectroscopy--the cold dilute gas and grains between the stars, we find a rich organic chemistry, presumably abiological, not only in most of the solar system but throughout the Milky Way galaxy. In part because the composition and surface pressure of the Earth's atmosphere 4 x 10(9) years ago are unknown, laboratory experiments on prebiological organic chemistry are at best suggestive; but we can test our understanding by looking more closely at the observed extraterrestrial organic chemistry. The present Account is restricted to atmospheric organic chemistry, primarily on the large moon of Saturn. Titan is a test of our understanding of the organic chemistry of planetary atmospheres. Its atmospheric bulk composition (N2/CH4) is intermediate between the highly reducing (H2/He/CH4/NH3/H2O) atmospheres of the Jovian planets and the more oxidized (N2/CO2/H2O) atmospheres of the terrestrial planets Mars and Venus. It has long been recognized that Titan's organic chemistry may have some relevance to the events that led to the origin of life on Earth. But with Titan surface temperatures approximately equal to 94 K and pressures approximately equal to 1.6 bar, the oceans of the early Earth have no ready analogue on Titan. Nevertheless, tectonic events in the water ice-rich interior or impact melting and slow re-freezing may lead to an episodic availability of liquid water. Indeed, the latter process is the equivalent of a approximately 10(3)-year-duration shallow aqueous sea over the entire surface of Titan.

  2. NATO Advanced Study Institute on Pollutants from Combustion Formation and Impact on Atmospheric Chemistry

    CERN Document Server

    2000-01-01

    This volume is based on the lectures presented at the NATO Advanced Study Institute: (ASI) «Pollutants Formation from Combustion. Formation Mechanisms and Impact on th th Atmospheric Chemistry» held in Maratea, Italy, from 13 to 26 september 1998. Preservation of the environment is of increasing concern in individual countries but also at continental or world scales. The structure of a NATO ASI which involve lecturers and participants of different nationalities was thought as especially well suited to address environmental issues. As combustion is known to substantially contribute to the damaging of the atmosphere, it was natural to concentrate the ASI program on reviewing the currently available knowledge of the formation mechanisms of the main pollutants liberated by combustion systems. In most situations, pollutants are present as trace components and their formation and removal is strongly conditioned by the chemical reactions initiated by fuel consumption. Therefore specific lectures were aimed at defi...

  3. Atmospheric and Geophysical Sciences Program report, 1990--1991

    International Nuclear Information System (INIS)

    MacCracken, M.C.; Albritton, J.R.; MacGregor, P.M.

    1992-06-01

    This report describes research programs from Lawrence Livermore Laboratory from 1990--1991 in atmospheric chemistry and geophysics. Programs such as mathematical modeling of atmospheric dispersions of pollutants and radionuclides,tropospheric chemistry, clouds, climate models, and the effects of atmospheric trace constiuents on ozone are described

  4. Chemistry and physics of fogwater collection. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Jaeschke, W.; Enderle, K.H. (eds.)

    1988-01-01

    Increasing interest in the problems of air pollution and source receptor relationships has led to a significant expansion of knowledge in the field of atmospheric chemistry. In recent years the multiphase atmospheric chemistry was given great scholarly attention, and slogans like acid precipitation, dirty cloud or killer fog indicated these phenomena. The report describes results of collection and chemical analysis of fog water with emphasis or fog microphysics, of the heterogeneous atmospheric chemistry project in the Po-valley, of the development of the Great Dun Fell project, of the mountain cloud chemistry project in eastern U.S., of the design of fog water collectors and of the numerical study of the radiation fog event on October 10/11, 1982 in Albany, N.Y.

  5. Middle atmosphere response to different descriptions of the 11-yr solar cycle in spectral irradiance in a chemistry-climate model

    Directory of Open Access Journals (Sweden)

    W. H. Swartz

    2012-07-01

    Full Text Available The 11-yr solar cycle in solar spectral irradiance (SSI inferred from measurements by the SOlar Radiation & Climate Experiment (SORCE suggests a much larger variation in the ultraviolet than previously accepted. We present middle atmosphere ozone and temperature responses to the solar cycles in SORCE SSI and the ubiquitous Naval Research Laboratory (NRL SSI reconstruction using the Goddard Earth Observing System chemistry-climate model (GEOSCCM. The results are largely consistent with other recent modeling studies. The modeled ozone response is positive throughout the stratosphere and lower mesosphere using the NRL SSI, while the SORCE SSI produces a response that is larger in the lower stratosphere but out of phase with respect to total solar irradiance above 45 km. The modeled responses in total ozone are similar to those derived from satellite and ground-based measurements, 3–6 Dobson Units per 100 units of 10.7-cm radio flux (F10.7 in the tropics. The peak zonal mean tropical temperature response using the SORCE SSI is nearly 2 K per 100 units F10.7 – 3 times larger than the simulation using the NRL SSI. The GEOSCCM and the Goddard Space Flight Center (GSFC 2-D coupled model are used to examine how the SSI solar cycle affects the atmosphere through direct solar heating and photolysis processes individually. Middle atmosphere ozone is affected almost entirely through photolysis, whereas the solar cycle in temperature is caused both through direct heating and photolysis feedbacks, processes that are mostly linearly separable. This is important in that it means that chemistry-transport models should simulate the solar cycle in ozone well, while general circulation models without coupled chemistry will underestimate the temperature response to the solar cycle significantly in the middle atmosphere. Further, the net ozone response results from the balance of ozone production at wavelengths less than 242 nm

  6. Atmospheric Chemistry in a Changing World

    Science.gov (United States)

    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.

  7. Do vibrationally excited OH molecules affect middle and upper atmospheric chemistry?

    Directory of Open Access Journals (Sweden)

    T. von Clarmann

    2010-10-01

    Full Text Available Except for a few reactions involving electronically excited molecular or atomic oxygen or nitrogen, atmospheric chemistry modelling usually assumes that the temperature dependence of reaction rates is characterized by Arrhenius' law involving kinetic temperatures. It is known, however, that in the upper atmosphere the vibrational temperatures may exceed the kinetic temperatures by several hundreds of Kelvins. This excess energy has an impact on the reaction rates. We have used upper atmospheric OH populations and reaction rate coefficients for OH(v=0...9+O3 and OH(v=0...9+O to estimate the effective (i.e. population weighted reaction rates for various atmospheric conditions. We have found that the effective rate coefficient for OH(v=0...9+O3 can be larger by a factor of up to 1470 than that involving OH in its vibrational ground state only. At altitudes where vibrationally excited states of OH are highly populated, the OH reaction is a minor sink of Ox and O3 compared to other reactions involving, e.g., atomic oxygen. Thus the impact of vibrationally excited OH on the ozone or Ox sink remains small. Among quiescent atmospheres under investigation, the largest while still small (less than 0.1% effect was found for the polar winter upper stratosphere and mesosphere. The contribution of the reaction of vibrationally excited OH with ozone to the OH sink is largest in the upper polar winter stratosphere (up to 4%, while its effect on the HO2 source is larger in the lower thermosphere (up to 1.5% for polar winter and 2.5% for midlatitude night conditions. For OH(v=0...9+O the effective rate coefficients are lower by up to 11% than those involving OH in its vibrational ground state. The effects on the odd oxygen sink are negative and can reach −3% (midlatitudinal nighttime lowermost thermosphere, i.e. neglecting vibrational excitation overestimates the odd

  8. Stream water chemistry in watersheds receiving different atmospheric inputs of H+, NH4+, NO3-, and SO42-1

    Science.gov (United States)

    Stottlemyer, R.

    1997-01-01

    Weekly precipitation and stream water samples were collected from small watersheds in Denali National Park, Alaska, the Fraser Experimental Forest, Colorado, Isle Royale National Park, Michigan, and the Calumet watershed on the south shore of Lake Superior, Michigan. The objective was to determine if stream water chemistry at the mouth and upstream stations reflected precipitation chemistry across a range of atmospheric inputs of H+, NH4+, NO3-, and SO42-. Volume-weighted precipitation H+, NH4+, NO3-, and SO42- concentrations varied 4 to 8 fold with concentrations highest at Calumet and lowest in Denali. Stream water chemistry varied among sites, but did not reflect precipitation chemistry. The Denali watershed, Rock Creek, had the lowest precipitation NO3- and SO42- concentrations, but the highest stream water NO3and SO42- concentrations. Among sites, the ratio of mean monthly upstream NO3- concentration to precipitation NO3- concentration declined (p 90 percent inputs) across inputs ranging from 0.12 to > 6 kg N ha-1 y-1. Factors possibly accounting for the weak or non-existent signal between stream water and precipitation ion concentrations include rapid modification of meltwater and precipitation chemistry by soil processes, and the presence of unfrozen soils which permits winter mineralization and nitrification to occur.

  9. Chemistry and climate change

    International Nuclear Information System (INIS)

    Bernier, Jean-Claude; Brasseur, Guy; Brechet, Yves; Candel, Sebastien; Cazenave, Anny; Courtillot, Vincent; Fontecave, Marc; Garnier, Emmanuel; Goebel, Philippe; Legrand, Jack; Legrand, Michel; Le Treut, Herve; Mauberger, Pascal; Dinh-Audouin, Minh-Thu; Olivier, Daniele; Rigny, Paul; Bigot, Bernard

    2016-01-01

    In its first part, this collective publication addresses the decennial and centuries-old variations of climate: perspectives and implications of climate change for the 21. century, questions remaining about the understanding of climate change from its sources to its modelling, extreme climate variations and societies during the last millennium. The contributions of the second part outline how chemistry is a tool to study climate change: ice chemistry as an archive of our past environment, observations and predictions on sea level rise, relationship between atmosphere chemistry and climate. The third set of contributions discusses the transformation of the energy system for a cleaner atmosphere and the management of the climate risk: the chemical processing of CO_2, actions of chemical companies to support the struggle against climate change, relationship between barrel price and renewable energies, relationship between grid complexity and green energy. The last part outlines the role chemistry can have to be able to do without fossil fuels: chemistry in front of challenges of transformation of the energy system, the use of micro-algae, the use of hydrogen as a vector of energy transition

  10. Reactions at surfaces in the atmosphere: integration of experiments and theory as necessary (but not necessarily sufficient) for predicting the physical chemistry of aerosols.

    Science.gov (United States)

    Finlayson-Pitts, Barbara J

    2009-09-28

    While particles have significant deleterious impacts on human health, visibility and climate, quantitative understanding of their formation, composition and fates remains problematic. Indeed, in many cases, even qualitative understanding is lacking. One area of particular uncertainty is the nature of particle surfaces and how this determines interactions with gases in the atmosphere, including water, which is important for cloud formation and properties. The focus in this Perspective article is on some chemistry relevant to airborne particles and especially to reactions occurring on their surfaces. The intent is not to provide a comprehensive review, but rather to highlight a few selected examples of interface chemistry involving inorganic and organic species that may be important in the lower atmosphere. This includes sea salt chemistry, nitrate and nitrite ion photochemistry, organics on surfaces and heterogeneous reactions of oxides of nitrogen on proxies for airborne mineral dust and boundary layer surfaces. Emphasis is on the molecular level understanding that can only be gained by fully integrating experiment and theory to elucidate these complex systems.

  11. Clouds and Chemistry in the Atmosphere of Extrasolar Planet HR8799b

    Energy Technology Data Exchange (ETDEWEB)

    Barman, T S; Macintosh, B A; Konopacky, Q M; Marois, C

    2011-03-21

    Using the integral field spectrograph OSIRIS, on the Keck II telescope, broad near-infrared H and K-band spectra of the young exoplanet HR8799b have been obtained. In addition, six new narrow-band photometric measurements have been taken across the H and K bands. These data are combined with previously published photometry for an analysis of the planet's atmospheric properties. Thick photospheric dust cloud opacity is invoked to explain the planet's red near-IR colors and relatively smooth near-IR spectrum. Strong water absorption is detected, indicating a Hydrogen-rich atmosphere. Only weak CH{sub 4} absorption is detected at K band, indicating efficient vertical mixing and a disequilibrium CO/CH{sub 4} ratio at photospheric depths. The H-band spectrum has a distinct triangular shape consistent with low surface gravity. New giant planet atmosphere models are compared to these data with best fitting bulk parameters, T{sub eff} = 1100K {+-} 100 and log(g) = 3.5 {+-} 0.5 (for solar composition). Given the observed luminosity (log L{sub obs}/L{sub {circle_dot}} {approx} -5.1), these values correspond to a radius of 0.75 R{sub Jup{sub 0.12}{sup +0.17}} and mass {approx} 0.72 M{sub Jup{sub -0.6}{sup +2.6}} - strikingly inconsistent with interior/evolution models. Enhanced metallicity (up to {approx} 10 x that of the Sun) along with thick clouds and non-equilibrium chemistry are likely required to reproduce the complete ensemble of spectroscopic and photometric data and the low effective temperatures (< 1000K) required by the evolution models.

  12. The nitrogen cycle: Atmosphere interactions

    Science.gov (United States)

    Levine, J. S.

    1984-01-01

    Atmospheric interactions involving the nitrogen species are varied and complex. These interactions include photochemical reactions, initiated by the absorption of solar photons and chemical kinetic reactions, which involve both homogeneous (gas-to-gas reactions) and heterogeneous (gas-to-particle) reactions. Another important atmospheric interaction is the production of nitrogen oxides by atmospheric lightning. The nitrogen cycle strongly couples the biosphere and atmosphere. Many nitrogen species are produced by biogenic processes. Once in the atmosphere nitrogen oxides are photochemically and chemically transformed to nitrates, which are returned to the biosphere via precipitation, dry deposition and aerosols to close the biosphere-atmosphere nitrogen cycle. The sources, sinks and photochemistry/chemistry of the nitrogen species; atmospheric nitrogen species; souces and sinks of nitrous oxide; sources; sinks and photochemistry/chemistry of ammonia; seasonal variation of the vertical distribution of ammonia in the troposphere; surface and atmospheric sources of the nitrogen species, and seasonal variation of ground level ammonia are summarized.

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

    Directory of Open Access Journals (Sweden)

    Z. Peng

    2016-04-01

    Full Text Available 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

  14. Modelling stratospheric chemistry in a global three-dimensional chemical transport model

    Energy Technology Data Exchange (ETDEWEB)

    Rummukainen, M [Finnish Meteorological Inst., Sodankylae (Finland). Sodankylae Observatory

    1996-12-31

    Numerical modelling of atmospheric chemistry aims to increase the understanding of the characteristics, the behavior and the evolution of atmospheric composition. These topics are of utmost importance in the study of climate change. The multitude of gases and particulates making up the atmosphere and the complicated interactions between them affect radiation transfer, atmospheric dynamics, and the impacts of anthropogenic and natural emissions. Chemical processes are fundamental factors in global warming, ozone depletion and atmospheric pollution problems in general. Much of the prevailing work on modelling stratospheric chemistry has so far been done with 1- and 2-dimensional models. Carrying an extensive chemistry parameterisation in a model with high spatial and temporal resolution is computationally heavy. Today, computers are becoming powerful enough to allow going over to 3-dimensional models. In order to concentrate on the chemistry, many Chemical Transport Models (CTM) are still run off-line, i.e. with precalculated and archived meteorology and radiation. In chemistry simulations, the archived values drive the model forward in time, without interacting with the chemical evolution. This is an approach that has been adopted in stratospheric chemistry modelling studies at the Finnish Meteorological Institute. In collaboration with the University of Oslo, a development project was initiated in 1993 to prepare a stratospheric chemistry parameterisation, fit for global 3-dimensional modelling. This article presents the parameterisation approach. Selected results are shown from basic photochemical simulations

  15. Modelling stratospheric chemistry in a global three-dimensional chemical transport model

    Energy Technology Data Exchange (ETDEWEB)

    Rummukainen, M. [Finnish Meteorological Inst., Sodankylae (Finland). Sodankylae Observatory

    1995-12-31

    Numerical modelling of atmospheric chemistry aims to increase the understanding of the characteristics, the behavior and the evolution of atmospheric composition. These topics are of utmost importance in the study of climate change. The multitude of gases and particulates making up the atmosphere and the complicated interactions between them affect radiation transfer, atmospheric dynamics, and the impacts of anthropogenic and natural emissions. Chemical processes are fundamental factors in global warming, ozone depletion and atmospheric pollution problems in general. Much of the prevailing work on modelling stratospheric chemistry has so far been done with 1- and 2-dimensional models. Carrying an extensive chemistry parameterisation in a model with high spatial and temporal resolution is computationally heavy. Today, computers are becoming powerful enough to allow going over to 3-dimensional models. In order to concentrate on the chemistry, many Chemical Transport Models (CTM) are still run off-line, i.e. with precalculated and archived meteorology and radiation. In chemistry simulations, the archived values drive the model forward in time, without interacting with the chemical evolution. This is an approach that has been adopted in stratospheric chemistry modelling studies at the Finnish Meteorological Institute. In collaboration with the University of Oslo, a development project was initiated in 1993 to prepare a stratospheric chemistry parameterisation, fit for global 3-dimensional modelling. This article presents the parameterisation approach. Selected results are shown from basic photochemical simulations

  16. Biomass burning in the tropics: Impact on atmospheric chemistry and biogeochemical cycles

    International Nuclear Information System (INIS)

    Crutzen, P.J.; Andreae, M.O.

    1990-01-01

    Biomass burning is widespread, especially in the tropics. It serves to clear land for shifting cultivation, to convert forests to agricultural and pastoral lands, and to remove dry vegetation in order to promote agricultural productivity and the growth of higher yield grasses. Furthermore, much agricultural waste and fuel wood is being combusted, particularly in developing countries. Biomass containing 2 to 5 petagrams of carbon is burned annually (1 petagram = 10 15 grams), producing large amounts of trace gases and aerosol particles that play important roles in atmospheric chemistry and climate. Emissions of carbon monoxide and methane by biomass burning affect the oxidation efficiency of the atmosphere by reacting with hydroxyl radicals, and emissions of nitric oxide and hydrocarbons lead to high ozone concentrations in the tropics during the dry season. Large quantities of smoke particles are produced as well, and these can serve as cloud condensation nuclei. These particles may thus substantially influence cloud microphysical and optical properties, an effect that could have repercussions for the radiation budget and the hydrological cycle in the tropics. Widespread burning may also disturb biogeochemical cycles, especially that of nitrogen. About 50% of the nitrogen in the biomass fuel can be released as molecular nitrogen. This pyrodenitrification process causes a sizable loss of fixed nitrogen in tropical ecosystems, in the range of 10 to 20 teragrams per year (1 teragram = 10 12 grams)

  17. Anthropogenous modifications of the atmosphere. The atmospheric ozone threat

    International Nuclear Information System (INIS)

    Aimedieu, P.

    1991-01-01

    Ozone role and atmospheric chemistry are first reviewed: chemical reactions and vertical distribution of ozone in the atmosphere. The origins of chlorofluorocarbon air pollution and the role of the various types of CFC on ozone depletion, greenhouse effect, cancer, etc. are then discussed. The political and environmental discussions concerning these phenomena are also reviewed

  18. Tropospheric Halogen Chemistry

    Science.gov (United States)

    von Glasow, R.; Crutzen, P. J.

    2003-12-01

    Halogens are very reactive chemicals that are known to play an important role in anthropogenic stratospheric ozone depletion chemistry, first recognized by Molina and Rowland (1974). However, they also affect the chemistry of the troposphere. They are of special interest because they are involved in many reaction cycles that can affect the oxidation power of the atmosphere indirectly by influencing the main oxidants O3 and its photolysis product OH and directly, e.g., by reactions of the Cl radical with hydrocarbons (e.g., CH4).Already by the middle of the nineteenth century, Marchand (1852) reported the presence of bromine and iodine in rain and other natural waters. He also mentions the benefits of iodine in drinking water through the prevention of goitres and cretinism. In a prophetic monograph "Air and Rain: The Beginnings of a Chemical Climatology," Smith (1872) describes measurements of chloride in rain water, which he states to originate partly from the oceans by a process that he compares with the bursting of "soap bubbles" which produces "small vehicles" that transfer small spray droplets of seawater to the air. From deviations of the sulfate-to-chloride ratio in coastal rain compared to seawater, Smith concluded that chemical processes occur once the particles are airborne.For almost a century thereafter, however, atmospheric halogens received little attention. One exception was the work by Cauer (1939), who reported that iodine pollution has been significant in Western and Central Europe due to the inefficient burning of seaweed, causing mean gas phase atmospheric concentrations as high as or greater than 0.5 μg m-3. In his classical textbook Air Chemistry and Radioactivity, Junge (1963) devoted less than three pages to halogen gas phase chemistry, discussing chlorine and iodine. As reviewed by Eriksson (1959a, b), the main atmospheric source of halogens is sea salt, derived from the bursting of bubbles of air which are produced by ocean waves and other

  19. Assessment of two physical parameterization schemes for desert dust emissions in an atmospheric chemistry general circulation model

    Science.gov (United States)

    Astitha, M.; Abdel Kader, M.; Pozzer, A.; Lelieveld, J.

    2012-04-01

    Atmospheric particulate matter and more specific desert dust has been the topic of numerous research studies in the past due to the wide range of impacts in the environment and climate and the uncertainty of characterizing and quantifying these impacts in a global scale. In this work we present two physical parameterizations of the desert dust production that have been incorporated in the atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy2.41 Atmospheric Chemistry). The scope of this work is to assess the impact of the two physical parameterizations in the global distribution of desert dust and highlight the advantages and disadvantages of using either technique. The dust concentration and deposition has been evaluated using the AEROCOM dust dataset for the year 2000 and data from the MODIS and MISR satellites as well as sun-photometer data from the AERONET network was used to compare the modelled aerosol optical depth with observations. The implementation of the two parameterizations and the simulations using relatively high spatial resolution (T106~1.1deg) has highlighted the large spatial heterogeneity of the dust emission sources as well as the importance of the input parameters (soil size and texture, vegetation, surface wind speed). Also, sensitivity simulations with the nudging option using reanalysis data from ECMWF and without nudging have showed remarkable differences for some areas. Both parameterizations have revealed the difficulty of simulating all arid regions with the same assumptions and mechanisms. Depending on the arid region, each emission scheme performs more or less satisfactorily which leads to the necessity of treating each desert differently. Even though this is a quite different task to accomplish in a global model, some recommendations are given and ideas for future improvements.

  20. Impact of two chemistry mechanisms fully coupled with mesoscale model on the atmospheric pollutants distribution

    Science.gov (United States)

    Arteta, J.; Cautenet, S.; Taghavi, M.; Audiffren, N.

    Air quality models (AQM) consist of many modules (meteorology, emission, chemistry, deposition), and in some conditions such as: vicinity of clouds or aerosols plumes, complex local circulations (mountains, sea breezes), fully coupled models (online method) are necessary. In order to study the impact of lumped chemical mechanisms in AQM simulations, we examine the ability of both different chemical mechanisms: (i) simplified: Condensed Version of the MOdèle de Chimie Atmosphérique 2.2 (CV-MOCA2.2), and (ii) reference: Regional Atmospheric Chemistry Model (RACM), which are coupled online with the Regional Atmospheric Modeling Systems (RAMS) model, on the distribution of pollutants. During the ESCOMPTE experiment (Expérience sur Site pour COntraindre les Modèles de Pollution et de Transport d'Emissions) conducted over Southern France (including urban and industrial zones), Intensive observation periods (IOP) characterized by various meteorological and mixed chemical conditions are simulated. For both configurations of modeling, numerical results are compared with surface measurements (75 stations) for primary (NO x) and secondary (O 3) species. We point out the impact of the two different chemical mechanisms on the production of species involved in the oxidizing capacity such as ozone and radicals within urban and industrial areas. We highlight that both chemical mechanisms produce very similar results for the main pollutants (NO x and O 3) in three-dimensional (3D) distribution, despite large discrepancies in 0D modeling. For ozone concentration, we found sometimes small differences (5-10 ppb) between the mechanisms under study according to the cases (polluted or not). The relative difference between the two mechanisms over the whole domain is only -7% for ozone from CV-MOCA 2.2 versus RACM. When the order of magnitude is needed rather than an accurate estimate, a reduced mechanism is satisfactory. It has the advantage of running faster (four times less than CPU

  1. Atmospheric and precipitation chemistry over the North Atlantic Ocean: Shipboard results, April-May 1984

    Science.gov (United States)

    Church, T. M.; Tramontano, J. M.; Whelpdale, D. M.; Andreae, M. O.; Galloway, J. N.; Keene, W. C.; Knap, A. H.; Tokos, J.

    1991-10-01

    During a North Atlantic cruise from Dakar, Senegal, to Woods Hole, Massachusetts (April 14-May 11, 1984), crossing the area of 14°-48°N; 17°-70°W, we collected atmospheric aerosols (C, N, S species), gases (SO4, HNO3, dimethyl sulfide (DMS), synthetic organic chemicals), and precipitation (major inorganic/organic ions, trace metals). Air masses that had not contacted land for over 5 days had a composition close to that from the remote marine atmosphere. Oxidation of biogenic DMS to SO4= aerosol accounted for most nss-SO4= in these air masses. Air masses that had transected densely populated North America (in the westerlies) or the Mediterranean/North Africa ( in the easterlies) within 2-5 days of being sampled over the North Atlantic were enriched in acid precursor compounds and synthetic hydrocarbons relative to air that had spent longer over the North Atlantic. Strong acids and trace metals were also elevated in precipitation. Air masses that had transected regions of strong emissions within the preceding 2 days had concentrations of atmospheric pollutants approaching those typically found in continental air masses. More frequent storm tracks between the Icelandic low and the Bermuda high favored transport of North American emissions northeasterly, toward Europe. Trajectory analyses suggested that air masses sampled off the northwest African coast had passed over the Mediterranean. Composition of the aerosol and precipitation of these air masses was also indicative of continental emissions, including biomass and petroleum burning. Transport and deposition of continental emissions to the North Atlantic were significantly influencing surface atmospheric and oceanic chemistry of this region.

  2. Elements of environmental chemistry

    National Research Council Canada - National Science Library

    Hites, R. A; Raff, Jonathan D

    2012-01-01

    ... more. Extensively revised, updated, and expanded, this second edition includes new chapters on atmospheric chemistry, climate change, and polychlorinated biphenyls and dioxins, and brominated flame retardants...

  3. Atmospheric sciences annual progress report, 1974

    International Nuclear Information System (INIS)

    Tucker, W.D.

    1975-11-01

    Activities in atmospheric sciences in the Department of Applied Science at Brookhaven National Laboratory carried out during 1974 are described. Included are contributions from the Meteorology, Atmospheric Diagnostics, Atmospheric Chemistry Research, and Atmospheric Instrumentation Groups. Programs in Meteorology reported on include diffusion from an off-shore source, plume dynamics studies, modeling of coastal effects on wind and temperature fields and pollutant distributions, effects of indoor shelter on inhalation of airborne radionuclides, chemical-dynamical interactions, techniques for determining acid-rain impact upon the ecology of the eastern U.S., and climatology. Work under Atmospheric Chemistry Research was concentrated on atmospheric aerosol studies, including formation by free radical and neutral association reactions, identification of reactive systems leading to aerosol formation, growth of sodium aerosols under atmospheric conditions and clustering reactions. Atmospheric Diagnostics presents work on field sampling and analytical technology for atmospheric pollutants, airborne sampling systems, atmospheric sulfate particulates methodology, and on a pyroturbidometric method for particulate sulfate discrimination and determination. Methodology for the use of sulfur hexafluoride in field tracer studies is discussed under Atmospheric Instrumentation. A list of publications is included

  4. Dimethylsulfide Chemistry: Annual, Seasonal, and Spatial Impacts on Sulfate

    Science.gov (United States)

    We incorporated oceanic emissions and atmospheric chemistry of dimethylsulfide (DMS) into the hemispheric Community Multiscale Air Quality model and performed annual model simulations without and with DMS chemistry. The model without DMS chemistry predicts higher concentrations o...

  5. Gas phase ion chemistry

    CERN Document Server

    Bowers, Michael T

    1979-01-01

    Gas Phase Ion Chemistry, Volume 1 covers papers on the advances of gas phase ion chemistry. The book discusses the advances in flow tubes and the measurement of ion-molecule rate coefficients and product distributions; the ion chemistry of the earth's atmosphere; and the classical ion-molecule collision theory. The text also describes statistical methods in reaction dynamics; the state selection by photoion-photoelectron coincidence; and the effects of temperature and pressure in the kinetics of ion-molecule reactions. The energy distribution in the unimolecular decomposition of ions, as well

  6. THE ROLE OF NITROGEN IN TITAN’S UPPER ATMOSPHERIC HYDROCARBON CHEMISTRY OVER THE SOLAR CYCLE

    Energy Technology Data Exchange (ETDEWEB)

    Luspay-Kuti, A.; Mandt, K. E.; Greathouse, T. K. [Department of Space Research, Southwest Research Institute, San Antonio, TX 78228 (United States); Westlake, J. H. [Johns Hopkins University Applied Physics Laboratory, Laurel, MD 20723 (United States); Plessis, S., E-mail: aluspaykuti@swri.edu [Fund Kis, F-92160 Antony (France)

    2016-06-01

    Titan’s thermospheric photochemistry is primarily driven by solar radiation. Similarly to other planetary atmospheres, such as Mars’, Titan’s atmospheric structure is also directly affected by variations in the solar extreme-UV/UV output in response to the 11-year-long solar cycle. Here, we investigate the influence of nitrogen on the vertical production, loss, and abundance profiles of hydrocarbons as a function of the solar cycle. Our results show that changes in the atmospheric nitrogen atomic density (primarily in its ground state N({sup 4}S)) as a result of photon flux variations have important implications for the production of several minor hydrocarbons. The solar minimum enhancement of CH{sub 3}, C{sub 2}H{sub 6}, and C{sub 3}H{sub 8}, despite the lower CH{sub 4} photodissociation rates compared with solar maximum conditions, is explained by the role of N({sup 4}S). N({sup 4}S) indirectly controls the altitude of termolecular versus bimolecular chemical regimes through its relationship with CH{sub 3}. When in higher abundance during solar maximum at lower altitudes, N({sup 4}S) increases the importance of bimolecular CH{sub 3} + N({sup 4}S) reactions producing HCN and H{sub 2}CN. The subsequent remarkable CH{sub 3} loss and decrease in the CH{sub 3} abundance at lower altitudes during solar maximum affects the overall hydrocarbon chemistry.

  7. Modeling the Explicit Chemistry of Anthropogenic and Biogenic Organic Aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Madronich, Sasha [Univ. Corporation for Atmospheric Research, Boulder, CO (United States)

    2015-12-09

    The atmospheric burden of Secondary Organic Aerosols (SOA) remains one of the most important yet uncertain aspects of the radiative forcing of climate. This grant focused on improving our quantitative understanding of SOA formation and evolution, by developing, applying, and improving a highly detailed model of atmospheric organic chemistry, the Generation of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) model. Eleven (11) publications have resulted from this grant.

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

    Science.gov (United States)

    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.

  9. Contrasting characteristics of sub-microsecond pulsed atmospheric air and atmospheric pressure helium-oxygen glow discharges

    International Nuclear Information System (INIS)

    Walsh, J L; Liu, D X; Iza, F; Kong, M G; Rong, M Z

    2010-01-01

    Glow discharges in air are often considered to be the ultimate low-temperature atmospheric pressure plasmas for numerous chamber-free applications. This is due to the ubiquitous presence of air and the perceived abundance of reactive oxygen and nitrogen species in air plasmas. In this paper, sub-microsecond pulsed atmospheric air plasmas are shown to produce a low concentration of excited oxygen atoms but an abundance of excited nitrogen species, UV photons and ozone molecules. This contrasts sharply with the efficient production of excited oxygen atoms in comparable helium-oxygen discharges. Relevant reaction chemistry analysed with a global model suggests that collisional excitation of O 2 by helium metastables is significantly more efficient than electron dissociative excitation of O 2 , electron excitation of O and ion-ion recombination. These results suggest different practical uses of the two oxygen-containing atmospheric discharges, with air plasmas being well suited for nitrogen and UV based chemistry and He-O 2 plasmas for excited atomic oxygen based chemistry. (fast track communication)

  10. Containment Sodium Chemistry Models in MELCOR.

    Energy Technology Data Exchange (ETDEWEB)

    Louie, David [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Humphries, Larry L. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Denman, Matthew R [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2017-04-01

    To meet regulatory needs for sodium fast reactors’ future development, including licensing requirements, Sandia National Laboratories is modernizing MELCOR, a severe accident analysis computer code developed for the U.S. Nuclear Regulatory Commission (NRC). Specifically, Sandia is modernizing MELCOR to include the capability to model sodium reactors. However, Sandia’s modernization effort primarily focuses on the containment response aspects of the sodium reactor accidents. Sandia began modernizing MELCOR in 2013 to allow a sodium coolant, rather than water, for conventional light water reactors. In the past three years, Sandia has been implementing the sodium chemistry containment models in CONTAIN-LMR, a legacy NRC code, into MELCOR. These chemistry models include spray fire, pool fire and atmosphere chemistry models. Only the first two chemistry models have been implemented though it is intended to implement all these models into MELCOR. A new package called “NAC” has been created to manage the sodium chemistry model more efficiently. In 2017 Sandia began validating the implemented models in MELCOR by simulating available experiments. The CONTAIN-LMR sodium models include sodium atmosphere chemistry and sodium-concrete interaction models. This paper presents sodium property models, the implemented models, implementation issues, and a path towards validation against existing experimental data.

  11. Design of and initial results from a Highly Instrumented Reactor for Atmospheric Chemistry (HIRAC

    Directory of Open Access Journals (Sweden)

    D. R. Glowacki

    2007-10-01

    Full Text Available The design of a Highly Instrumented Reactor for Atmospheric Chemistry (HIRAC is described and initial results obtained from HIRAC are presented. The ability of HIRAC to perform in-situ laser-induced fluorescence detection of OH and HO2 radicals with the Fluorescence Assay by Gas Expansion (FAGE technique establishes it as internationally unique for a chamber of its size and pressure/temperature variable capabilities. In addition to the FAGE technique, HIRAC features a suite of analytical instrumentation, including: a multipass FTIR system; a conventional gas chromatography (GC instrument and a GC instrument for formaldehyde detection; NO/NO2, CO, O3, and H2O vapour analysers. Ray tracing simulations and NO2 actinometry have been utilized to develop a detailed model of the radiation field within HIRAC. Comparisons between the analysers and the FTIR coupled to HIRAC have been performed, and HIRAC has also been used to investigate pressure dependent kinetics of the chlorine atom reaction with ethene and the reaction of O3 and t-2-butene. The results obtained are in good agreement with literature recommendations and Master Chemical Mechanism predictions. HIRAC thereby offers a highly instrumented platform with the potential for: (1 high precision kinetics investigations over a range of atmospheric conditions; (2 detailed mechanism development, significantly enhanced according to its capability for measuring radicals; and (3 field instrument intercomparison, calibration, development, and investigations of instrument response at a range of atmospheric conditions.

  12. Global volcanic emissions: budgets, plume chemistry and impacts

    Science.gov (United States)

    Mather, T. A.

    2012-12-01

    Over the past few decades our understanding of global volcanic degassing budgets, plume chemistry and the impacts of volcanic emissions on our atmosphere and environment has been revolutionized. Global volcanic emissions budgets are needed if we are to make effective use of regional and global atmospheric models in order to understand the consequences of volcanic degassing on global environmental evolution. Traditionally volcanic SO2 budgets have been the best constrained but recent efforts have seen improvements in the quantification of the budgets of other environmentally important chemical species such as CO2, the halogens (including Br and I) and trace metals (including measurements relevant to trace metal atmospheric lifetimes and bioavailability). Recent measurements of reactive trace gas species in volcanic plumes have offered intriguing hints at the chemistry occurring in the hot environment at volcanic vents and during electrical discharges in ash-rich volcanic plumes. These reactive trace species have important consequences for gas plume chemistry and impacts, for example, in terms of the global fixed nitrogen budget, volcanically induced ozone destruction and particle fluxes to the atmosphere. Volcanically initiated atmospheric chemistry was likely to have been particularly important before biological (and latterly anthropogenic) processes started to dominate many geochemical cycles, with important consequences in terms of the evolution of the nitrogen cycle and the role of particles in modulating the Earth's climate. There are still many challenges and open questions to be addressed in this fascinating area of science.

  13. The Influence of CO2 Admixtures on the Product Composition in a Nitrogen-Methane Atmospheric Glow Discharge Used as a Prebiotic Atmosphere Mimic.

    Science.gov (United States)

    Mazankova, V; Torokova, L; Krcma, F; Mason, N J; Matejcik, S

    2016-11-01

    This work extends our previous experimental studies of the chemistry of Titan's atmosphere by atmospheric glow discharge. The Titan's atmosphere seems to be similarly to early Earth atmospheric composition. The exploration of Titan atmosphere was initiated by the exciting results of the Cassini-Huygens mission and obtained results increased the interest about prebiotic atmospheres. Present work is devoted to the role of CO 2 in the prebiotic atmosphere chemistry. Most of the laboratory studies of such atmosphere were focused on the chemistry of N 2  + CH 4 mixtures. The present work is devoted to the study of the oxygenated volatile species in prebiotic atmosphere, specifically CO 2 reactivity. CO 2 was introduced to the standard N 2  + CH 4 mixture at different mixing ratio up to 5 % CH 4 and 3 % CO 2 . The reaction products were characterized by FTIR spectroscopy. This work shows that CO 2 modifies the composition of the gas phase with the detection of oxygenated compounds: CO and others oxides. There is a strong influence of CO 2 on increasing concentration other products as cyanide (HCN) and ammonia (NH 3 ).

  14. DISEQUILIBRIUM CARBON, OXYGEN, AND NITROGEN CHEMISTRY IN THE ATMOSPHERES OF HD 189733b AND HD 209458b

    International Nuclear Information System (INIS)

    Moses, Julianne I.; Visscher, C.; Fortney, J. J.; Showman, A. P.; Lewis, N. K.; Griffith, C. A.; Klippenstein, S. J.; Shabram, M.; Friedson, A. J.; Marley, M. S.; Freedman, R. S.

    2011-01-01

    We have developed a one-dimensional photochemical and thermochemical kinetics and diffusion model to study the effects of disequilibrium chemistry on the atmospheric composition of 'hot-Jupiter' exoplanets. Here we investigate the coupled chemistry of neutral carbon, hydrogen, oxygen, and nitrogen species on HD 189733b and HD 209458b and we compare the model results with existing transit and eclipse observations. We find that the vertical profiles of molecular constituents are significantly affected by transport-induced quenching and photochemistry, particularly on the cooler HD 189733b; however, the warmer stratospheric temperatures on HD 209458b help maintain thermochemical equilibrium and reduce the effects of disequilibrium chemistry. For both planets, the methane and ammonia mole fractions are found to be enhanced over their equilibrium values at pressures of a few bar to less than an mbar due to transport-induced quenching, but CH 4 and NH 3 are photochemically removed at higher altitudes. Disequilibrium chemistry also enhances atomic species, unsaturated hydrocarbons (particularly C 2 H 2 ), some nitriles (particularly HCN), and radicals like OH, CH 3 , and NH 2 . In contrast, CO, H 2 O, N 2 , and CO 2 more closely follow their equilibrium profiles, except at pressures ∼ 2 O, and N 2 are photochemically destroyed and CO 2 is produced before its eventual high-altitude destruction. The enhanced abundances of CH 4 , NH 3 , and HCN are expected to affect the spectral signatures and thermal profiles of HD 189733b and other relatively cool, transiting exoplanets. We examine the sensitivity of our results to the assumed temperature structure and eddy diffusion coefficients and discuss further observational consequences of these models.

  15. Chemistry in protoplanetary disks

    Science.gov (United States)

    Semenov, D. A.

    2012-01-01

    In this lecture I discuss recent progress in the understanding of the chemical evolution of protoplanetary disks that resemble our Solar system during the first ten million years. At the verge of planet formation, strong variations of temperature, density, and radiation intensities in these disks lead to a layered chemical structure. In hot, dilute and heavily irradiated atmosphere only simple radicals, atoms, and atomic ions can survive, formed and destroyed by gas-phase processes. Beneath the atmosphere a partly UV-shielded, warm molecular layer is located, where high-energy radiation drives rich chemistry, both in the gas phase and on dust surfaces. In a cold, dense, dark disk midplane many molecules are frozen out, forming thick icy mantles where surface chemistry is active and where complex (organic) species are synthesized.

  16. A three-dimensional model of the atmospheric chemistry of E and Z-CF3CH=CHCl (HCFO-1233(zd) (E/Z))

    Science.gov (United States)

    Sulbaek Andersen, Mads P.; Schmidt, Johan A.; Volkova, Aleksandra; Wuebbles, Donald J.

    2018-04-01

    Using a 3-dimensional global atmospheric chemistry and transport model we investigated the atmospheric degradation of HCFO-1233zd(E), E-CF3CH=CHCl, a commercially important, new hydrofluorocarbon replacement compound. Atmospheric degradation of E-CF3CH=CHCl is initiated by reaction with OH radicals, which leads to several chemical oxidation products. Dissemination of these oxidation products to the environment is of concern due to the possible formation of trifluoroacetic acid (TFA) as a degradation product. The model indicates that the average global yield of TFA from atmospheric processing of E-CF3CH=CHCl is approximately 2%. The annually averaged atmospheric lifetime of E-CF3CH=CHCl was found to be approximately 36 days (12 days for Z-CF3CH=CHCl). As E-CF3CH=CHCl is short lived, by far the majority of its Cl atoms will be released and deposited in the lower atmosphere, and the impact on stratospheric ozone is insignificant. An Ozone Depletion Potential of 0.00030 was determined. The Photochemical Ozone Creation Potential was evaluated and a value of 3.6 determined. Finally, we derive a Global Warming Potential for E-CF3CH=CHCl for a 100 year time horizon of model.

  17. Atmospheric Research 2016 Technical Highlights

    Science.gov (United States)

    Platnick, Steven

    2017-01-01

    Atmospheric research in the Earth Sciences Division (610) consists of research and technology development programs dedicated to advancing knowledge and understanding of the atmosphere and its interaction with the climate of Earth. The Divisions goals are to improve understanding of the dynamics and physical properties of precipitation, clouds, and aerosols; atmospheric chemistry, including the role of natural and anthropogenic trace species on the ozone balance in the stratosphere and the troposphere; and radiative properties of Earth's atmosphere and the influence of solar variability on the Earth's climate. Major research activities are carried out in the Mesoscale Atmospheric Processes Laboratory, the Climate and Radiation Laboratory, the Atmospheric Chemistry and Dynamics Laboratory, and the Wallops Field Support Office. The overall scope of the research covers an end-to-end process, starting with the identification of scientific problems, leading to observation requirements for remote-sensing platforms, technology and retrieval algorithm development; followed by flight projects and satellite missions; and eventually, resulting in data processing, analyses of measurements, and dissemination from flight projects and missions. Instrument scientists conceive, design, develop, and implement ultraviolet, infrared, optical, radar, laser, and lidar technology to remotely sense the atmosphere. Members of the various laboratories conduct field measurements for satellite sensor calibration and data validation, and carry out numerous modeling activities. These modeling activities include climate model simulations, modeling the chemistry and transport of trace species on regional-to-global scales, cloud resolving models, and developing the next-generation Earth system models. Satellite missions, field campaigns, peer-reviewed publications, and successful proposals are essential at every stage of the research process to meeting our goals and maintaining leadership of the

  18. Observations of biogenic isoprene emissions and atmospheric chemistry components at the Savé super site in Benin, West Africa, during the DACCIWA field campaign.

    Science.gov (United States)

    Jambert, Corinne; Pacifico, Federica; Delon, Claire; Lohou, Fabienne; Reinares Martinez, Irene; Brilouet, Pierre-Etienne; Derrien, Solene; Dione, Cheikh; Brosse, Fabien; Gabella, Omar; Pedruzzo Bagazgoitia, Xavier; Durand, Pierre

    2017-04-01

    Tropospheric oxidation of VOCs (Volatile Organic Compounds), including isoprene, in the presence of NOx and sunlight leads to the formation of O3 and Secondary Organic Aerosols (SOA). Changes in NO or VOCs sources will consequently modify their atmospheric concentrations and thus, the rate of O3 production and SOA formation. NOx have also an impact on the abundance of the hydroxyl radical (OH) which determines the lifetime of some pollutants and greenhouse gases. Anthropogenic emissions of pollutants from mega cities located on the Guinean coast in South West Africa are likely to increase in the next decades due to a strong anthropogenic pressure and to land use changes at the regional or continental scale. The consequences on regional air quality and on pollutant deposition onto surfaces may have some harmful effects on human and ecosystem health. Furthermore, the regional climate and water cycle are affected by changes in atmospheric chemistry. When transported northward on the African continent, polluted air masses meet biogenic emissions from rural areas which contributes to increase ozone and SOA production, in high temperature and solar radiation conditions, highly favourable to enhanced photochemistry. During the Dynamics-aerosol-chemistry-cloud interactions in West Africa (DACCIWA) field campaign, we measured the atmospheric chemical composition and the exchanges of trace components in a hinterland area of Benin, at the Savé super-site (8°02'03" N, 2°29'11″ E). The observations, monitored in June and July 2016, in a rural mixed agricultural area, include near surface concentrations of ozone (O3), carbon monoxide (CO), nitrogen oxides (NOx) and isoprene, isoprene fluxes and meteorological parameters. We observed hourly average concentrations of O3 up to 50 ppb, low NOx concentrations (ca. 1 ppb and CO concentrations between 75 and 300 ppb. An 8 m tower was equipped with a Fast Isoprene Sensor and sonic anemometer to measure isoprene concentrations and

  19. ECHMERIT: A new on-line global mercury-chemistry model

    Science.gov (United States)

    Jung, G.; Hedgecock, I. M.; Pirrone, N.

    2009-04-01

    Mercury is a volatile metal, that is of concern because when deposited and transformed to methylmercury accumulates within the food-web. Due to the long lifetime of elemental mercury, which is the dominant fraction of mercury species in the atmosphere, mercury is prone to long-range transport and therefore distributed over the globe, transported and hence deposited even in regions far from anthropogenic emission sources. Mercury is released to the atmosphere from a variety of natural and anthropogenic sources, in elementary and oxidised forms, and as particulate mercury. It is then transported, but also transformed chemically in the gaseous phase, as well as in aqueous phase within cloud and rain droplets. Mercury (particularly its oxidised forms) is removed from the atmosphere though wet and dry deposition processes, a large fraction of deposited mercury is, after chemical or biological reduction, re-emitted to the atmosphere as elementary mercury. To investigate mercury chemistry and transport processes on the global scale, the new, global model ECHMERIT has been developed. ECHMERIT simulates meteorology, transport, deposition, photolysis and chemistry on-line. The general circulation model on which ECHMERIT is based is ECHAM5. Sophisticated chemical modules have been implemented, including gas phase chemistry based on the CBM-Z chemistry mechanism, as well as aqueous phase chemistry, both of which have been adapted to include Hg chemistry and Hg species gas-droplet mass transfer. ECHMERIT uses the fast-J photolysis routine. State-of-the-art procedures simulating wet and dry deposition and emissions were adapted and included in the model as well. An overview of the model structure, development, validation and sensitivity studies is presented.

  20. Dimethylsulfide chemistry: annual, seasonal, and spatial impacts on SO_4^(2-)

    Science.gov (United States)

    We incorporated oceanic emissions and atmospheric chemistry of dimethylsulfide (DMS) into the hemispheric Community Multiscale Air Quality model and performed annual model simulations without and with DMS chemistry. The model without DMS chemistry predicts higher concentrations o...

  1. Partial Overhaul and Initial Parallel Optimization of KINETICS, a Coupled Dynamics and Chemistry Atmosphere Model

    Science.gov (United States)

    Nguyen, Howard; Willacy, Karen; Allen, Mark

    2012-01-01

    KINETICS is a coupled dynamics and chemistry atmosphere model that is data intensive and computationally demanding. The potential performance gain from using a supercomputer motivates the adaptation from a serial version to a parallelized one. Although the initial parallelization had been done, bottlenecks caused by an abundance of communication calls between processors led to an unfavorable drop in performance. Before starting on the parallel optimization process, a partial overhaul was required because a large emphasis was placed on streamlining the code for user convenience and revising the program to accommodate the new supercomputers at Caltech and JPL. After the first round of optimizations, the partial runtime was reduced by a factor of 23; however, performance gains are dependent on the size of the data, the number of processors requested, and the computer used.

  2. FAST TRACK COMMUNICATION: Contrasting characteristics of sub-microsecond pulsed atmospheric air and atmospheric pressure helium-oxygen glow discharges

    Science.gov (United States)

    Walsh, J. L.; Liu, D. X.; Iza, F.; Rong, M. Z.; Kong, M. G.

    2010-01-01

    Glow discharges in air are often considered to be the ultimate low-temperature atmospheric pressure plasmas for numerous chamber-free applications. This is due to the ubiquitous presence of air and the perceived abundance of reactive oxygen and nitrogen species in air plasmas. In this paper, sub-microsecond pulsed atmospheric air plasmas are shown to produce a low concentration of excited oxygen atoms but an abundance of excited nitrogen species, UV photons and ozone molecules. This contrasts sharply with the efficient production of excited oxygen atoms in comparable helium-oxygen discharges. Relevant reaction chemistry analysed with a global model suggests that collisional excitation of O2 by helium metastables is significantly more efficient than electron dissociative excitation of O2, electron excitation of O and ion-ion recombination. These results suggest different practical uses of the two oxygen-containing atmospheric discharges, with air plasmas being well suited for nitrogen and UV based chemistry and He-O2 plasmas for excited atomic oxygen based chemistry.

  3. Colour chemistry in water

    OpenAIRE

    Cardona, Maria

    2015-01-01

    Atmospheric carbon dioxide (CO2) levels have increased dramatically in the last few decades. Famous for causing global warming, CO2 is also resulting in the acidification of seas and oceans. http://www.um.edu.mt/think/colour-chemistry-in-water/

  4. Clouds and Hazes in Exoplanet Atmospheres

    OpenAIRE

    Marley, Mark S.; Ackerman, Andrew S.; Cuzzi, Jeffrey N.; Kitzmann, Daniel

    2013-01-01

    Clouds and hazes are commonplace in the atmospheres of solar system planets and are likely ubiquitous in the atmospheres of extrasolar planets as well. Clouds affect every aspect of a planetary atmosphere, from the transport of radiation, to atmospheric chemistry, to dynamics and they influence - if not control - aspects such as surface temperature and habitability. In this review we aim to provide an introduction to the role and properties of clouds in exoplanetary atmospheres. We consider t...

  5. Design of a new multi-phase experimental simulation chamber for atmospheric photosmog, aerosol and cloud chemistry research

    Directory of Open Access Journals (Sweden)

    J. Wang

    2011-11-01

    Full Text Available A new simulation chamber has been built at the Interuniversitary Laboratory of Atmospheric Systems (LISA. The CESAM chamber (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber is designed to allow research in multiphase atmospheric (photo- chemistry which involves both gas phase and condensed phase processes including aerosol and cloud chemistry. CESAM has the potential to carry out variable temperature and pressure experiments under a very realistic artificial solar irradiation. It consists of a 4.2 m3 stainless steel vessel equipped with three high pressure xenon arc lamps which provides a controlled and steady environment. Initial characterization results, all carried out at 290–297 K under dry conditions, concerning lighting homogeneity, mixing efficiency, ozone lifetime, radical sources, NOy wall reactivity, particle loss rates, background PM, aerosol formation and cloud generation are given. Photolysis frequencies of NO2 and O3 related to chamber radiation system were found equal to (4.2 × 10−3 s−1 for JNO2 and (1.4 × 10−5 s−1 for JO1D which is comparable to the solar radiation in the boundary layer. An auxiliary mechanism describing NOy wall reactions has been developed. Its inclusion in the Master Chemical Mechanism allowed us to adequately model the results of experiments on the photo-oxidation of propene-NOx-Air mixtures. Aerosol yields for the α-pinene + O3 system chosen as a reference were determined and found in good agreement with previous studies. Particle lifetime in the chamber ranges from 10 h to 4 days depending on particle size distribution which indicates that the chamber can provide high quality data on aerosol aging processes and their effects. Being evacuable, it is possible to generate in this new chamber

  6. HIGH-TEMPERATURE PHOTOCHEMISTRY IN THE ATMOSPHERE OF HD 189733b

    International Nuclear Information System (INIS)

    Line, M. R.; Yung, Y. L.; Liang, M. C.

    2010-01-01

    Recent infrared spectroscopy of hot exoplanets is beginning to reveal their atmospheric composition. Deep within the planetary atmosphere, the composition is controlled by thermochemical equilibrium. Photochemistry becomes important higher in the atmosphere, at levels above ∼1 bar. These two chemistries compete between ∼1 and 10 bars in hot-Jupiter-like atmospheres, depending on the strength of the eddy mixing and temperature. HD 189733b provides an excellent laboratory in which to study the consequences of chemistry of hot atmospheres. The recent spectra of HD 189733b contain signatures of CH 4 , CO 2 , CO, and H 2 O. Here we identify the primary chemical pathways that govern the abundances of CH 4 , CO 2 , CO, and H 2 O in the cases of thermochemical equilibrium chemistry, photochemistry, and their combination. Our results suggest that the disequilibrium mechanisms can significantly enhance the abundances of these species above their thermochemical equilibrium value, so some caution must be taken when assuming that an atmosphere is in strict thermochemical equilibrium.

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

    Science.gov (United States)

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

    2016-01-01

    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. PMID:28057962

  8. Atmospheric chemistry of peroxynitrates

    International Nuclear Information System (INIS)

    Hendry, D.G.; Kenley, R.A.

    1979-01-01

    The thermochemistry and kinetics of the various types of peroxy nitrates are discussed, and the influence of these compounds on smog formation is evaluated. The heats of formation and of two dissociation reactions for various peroxyalkyl nitrates are calculated and it is shown that dissociation into nitrogen dioxide is more favorable than into nitrogen trioxide for the peroxyalkyl and peroxyacetyl nitrates (PANs). The atmospheric lifetimes of peroxynitric acid, peroxyalkyl nitrates and peroxyacyl nitrates are estimated as a function of temperature and it is found that PANs can exhibit lifetimes greater than a day at low temperatures, resulting in significant concentrations. In the presence of NO, PANs are shown to be an important source of OH radicals in the early morning and at night. A computer simulation reveals the contribution of PANs to ozone formation by the oxidation of NO to NO2

  9. Atmospheric chemistry of polycyclic aromatic compounds with special emphasis on nitro derivatives

    Energy Technology Data Exchange (ETDEWEB)

    Feilberg, A.

    2000-04-01

    Field measurements of polycyclic aromatic compounds (PAC) have been carried out at a semi-rural site and at an urban site. Correlation analyses, PAC indicators, and PAC ratios have been used to evaluate the importance of various sources of nitro-PAHs. A major source of nitro-PAHs is atmospheric transformation of PAHs initiated by OH radicals. Especially during long-range transport (LRT) of air pollution from Central Europe, the nitro-PAH composition in Denmark is dominated by nitro-PAHs formed in the atmosphere. Locally emitted nitro-PAHs are primarily from diesel vehicles. Levels of unsubstituted PAHs can also be strongly elevated in connection with LRT episodes. The ratio of 2-nitrofluoranthene relative to 1-nitropyrene is proposed as a measure of the relative photochemical age of particulate matter. Using this ratio, the relative mutagenicity of particle extracts appears to increase with increasing photochemical age. In connection with the field measurements, a method for measuring nitro-PAHs in particle extracts based on MS-MS detection has been developed. The atmospheric chemistry of nitronaphthalenes has been investigated with a smog chamber system combined with simulation with photochemical kinetics software. A methodology to implement gas-particle partitioning in a model based on chemical kinetics is described. Equilibrium constants (KP) for gas-particle partitioning of 1- and 2-nitronaphthalene have been determined. Mass transfer between the two phases appears to occur on a very short timescale. The gas phase photolysis of the nitronaphthalenes depends upon the molecular conformation. Significantly faster photolysis of 1-nitronaphthalene than of 2-nitronaphthalene is observed. The photochemistry of nitro-PAHs, and to some extent other PAC, associated with organic aerosols, has been studied with model systems simulating organic aerosol material. A number of aerosol constituents, including substituted phenols, benzaldehydes, and oxy-PAHs, are demonstrated to

  10. Fine-Structure Measurements of Oxygen A Band Absorbance for Estimating the Thermodynamic Average Temperature of the Earth's Atmosphere: An Experiment in Physical and Environmental Chemistry

    Science.gov (United States)

    Myrick, M. L.; Greer, A. E.; Nieuwland, A.; Priore, R. J.; Scaffidi, J.; Andreatta, Daniele; Colavita, Paula

    2006-01-01

    The experiment describe the measures of the A band transitions of atmospheric oxygen, a rich series of rotation-electronic absorption lines falling in the deep red portion of the optical spectrum and clearly visible owing to attenuation of solar radiation. It combines pure physical chemistry with analytical and environmental science and provides a…

  11. Mass Spectrometry of Single Particles Levitated in an Electrodynamic Balance: Applications to Laboratory Atmospheric Chemistry Research

    Science.gov (United States)

    Birdsall, A.; Krieger, U. K.; Keutsch, F. N.

    2017-12-01

    Dynamic changes to atmospheric aerosol particle composition (e.g., originating from evaporation/condensation, oxidative aging, or aqueous-phase chemical reactions) impact particle properties with importance for understanding particle effects on climate and human health. These changes can take place over the entire lifetime of an atmospheric particle, which can extend over multiple days. Previous laboratory studies of such processes have included analyzing single particles suspended in a levitation device, such as an electrodynamic balance (EDB), an optical levitator, or an acoustic trap, using optical detection techniques. However, studying chemically complex systems can require an analytical method, such as mass spectrometry, that provides more molecular specificity. Existing work coupling particle levitation with mass spectrometry is more limited and largely has consisted of acoustic levitation of millimeter-sized droplets.In this work an EDB has been coupled with a custom-built ionization source and commercial time-of-flight mass spectrometer (MS) as a platform for laboratory atmospheric chemistry research. Single charged particles (radius 10 μm) have been injected into an EDB, levitated for an arbitrarily long period of time, and then transferred to a vaporization-corona discharge ionization region for MS analysis. By analyzing a series of particles of identical composition, residing in the controlled environment of the EDB for varying times, we can trace the chemical evolution of a particle over hours or days, appropriate timescales for understanding transformations of atmospheric particles.To prove the concept of our EDB-MS system, we have studied the evaporation of particles consisting of polyethylene glycol (PEG) molecules of mixed chain lengths, used as a benchmark system. Our system can quantify the composition of single particles (see Figure for sample spectrum of a single PEG-200 particle: PEG parent ions labeled with m/z, known PEG fragment ions

  12. Ground-based Observations and Atmospheric Modelling of Energetic Electron Precipitation Effects on Antarctic Mesospheric Chemistry

    Science.gov (United States)

    Newnham, D.; Clilverd, M. A.; Horne, R. B.; Rodger, C. J.; Seppälä, A.; Verronen, P. T.; Andersson, M. E.; Marsh, D. R.; Hendrickx, K.; Megner, L. S.; Kovacs, T.; Feng, W.; Plane, J. M. C.

    2016-12-01

    The effect of energetic electron precipitation (EEP) on the seasonal and diurnal abundances of nitric oxide (NO) and ozone in the Antarctic middle atmosphere during March 2013 to July 2014 is investigated. Geomagnetic storm activity during this period, close to solar maximum, was driven primarily by impulsive coronal mass ejections. Near-continuous ground-based atmospheric measurements have been made by a passive millimetre-wave radiometer deployed at Halley station (75°37'S, 26°14'W, L = 4.6), Antarctica. This location is directly under the region of radiation-belt EEP, at the extremity of magnetospheric substorm-driven EEP, and deep within the polar vortex during Austral winter. Superposed epoch analyses of the ground based data, together with NO observations made by the Solar Occultation For Ice Experiment (SOFIE) onboard the Aeronomy of Ice in the Mesosphere (AIM) satellite, show enhanced mesospheric NO following moderate geomagnetic storms (Dst ≤ -50 nT). Measurements by co-located 30 MHz riometers indicate simultaneous increases in ionisation at 75-90 km directly above Halley when Kp index ≥ 4. Direct NO production by EEP in the upper mesosphere, versus downward transport of NO from the lower thermosphere, is evaluated using a new version of the Whole Atmosphere Community Climate Model incorporating the full Sodankylä Ion Neutral Chemistry Model (WACCM SIC). Model ionization rates are derived from the Polar orbiting Operational Environmental Satellites (POES) second generation Space Environment Monitor (SEM 2) Medium Energy Proton and Electron Detector instrument (MEPED). The model data are compared with observations to quantify the impact of EEP on stratospheric and mesospheric odd nitrogen (NOx), odd hydrogen (HOx), and ozone.

  13. D-region ion-neutral coupled chemistry (Sodankylä Ion Chemistry, SIC) within the Whole Atmosphere Community Climate Model (WACCM 4) - WACCM-SIC and WACCM-rSIC

    Science.gov (United States)

    Kovács, Tamás; Plane, John M. C.; Feng, Wuhu; Nagy, Tibor; Chipperfield, Martyn P.; Verronen, Pekka T.; Andersson, Monika E.; Newnham, David A.; Clilverd, Mark A.; Marsh, Daniel R.

    2016-09-01

    This study presents a new ion-neutral chemical model coupled into the Whole Atmosphere Community Climate Model (WACCM). The ionospheric D-region (altitudes ˜ 50-90 km) chemistry is based on the Sodankylä Ion Chemistry (SIC) model, a one-dimensional model containing 307 ion-neutral and ion recombination, 16 photodissociation and 7 photoionization reactions of neutral species, positive and negative ions, and electrons. The SIC mechanism was reduced using the simulation error minimization connectivity method (SEM-CM) to produce a reaction scheme of 181 ion-molecule reactions of 181 ion-molecule reactions of 27 positive and 18 negative ions. This scheme describes the concentration profiles at altitudes between 20 km and 120 km of a set of major neutral species (HNO3, O3, H2O2, NO, NO2, HO2, OH, N2O5) and ions (O2+, O4+, NO+, NO+(H2O), O2+(H2O), H+(H2O), H+(H2O)2, H+(H2O)3, H+(H2O)4, O3-, NO2-, O-, O2, OH-, O2-(H2O), O2-(H2O)2, O4-, CO3-, CO3-(H2O), CO4-, HCO3-, NO2-, NO3-, NO3-(H2O), NO3-(H2O)2, NO3-(HNO3), NO3-(HNO3)2, Cl-, ClO-), which agree with the full SIC mechanism within a 5 % tolerance. Four 3-D model simulations were then performed, using the impact of the January 2005 solar proton event (SPE) on D-region HOx and NOx chemistry as a test case of four different model versions: the standard WACCM (no negative ions and a very limited set of positive ions); WACCM-SIC (standard WACCM with the full SIC chemistry of positive and negative ions); WACCM-D (standard WACCM with a heuristic reduction of the SIC chemistry, recently used to examine HNO3 formation following an SPE); and WACCM-rSIC (standard WACCM with a reduction of SIC chemistry using the SEM-CM method). The standard WACCM misses the HNO3 enhancement during the SPE, while the full and reduced model versions predict significant NOx, HOx and HNO3 enhancements in the mesosphere during solar proton events. The SEM-CM reduction also identifies the important ion-molecule reactions that affect the partitioning of

  14. A user-orientated approach to provenance capture and representation for in silico experiments, explored within the atmospheric chemistry community.

    Science.gov (United States)

    Martin, Chris J; Haji, Mohammed H; Jimack, Peter K; Pilling, Michael J; Dew, Peter M

    2009-07-13

    We present a novel user-orientated approach to provenance capture and representation for in silico experiments, contrasted against the more systems-orientated approaches that have been typical within the e-Science domain. In our approach, we seek to capture the scientist's reasoning in the form of annotations as an experiment evolves, while using the scientist's terminology in the representation of process provenance. Our user-orientated approach is applied in a case study within the atmospheric chemistry domain: we consider the design, development and evaluation of an electronic laboratory notebook, a provenance capture and storage tool, for iterative model development.

  15. Current Status of the Validation of the Atmospheric Chemistry Instruments on Envisat

    Science.gov (United States)

    Lecomte, P.; Koopman, R.; Zehner, C.; Laur, H.; Attema, E.; Wursteisen, P.; Snoeij, P.

    2003-04-01

    Envisat is ESA's advanced Earth observing satellite launched in March 2002 and is designed to provide measurements of the atmosphere, ocean, land and ice over a five-year period. After the launch and the switch-on period, a six-month commissioning phase has taken place for instrument calibration and geophysical validation, concluded with the Envisat Calibration Review held in September 2002. In addition to ESA and its industrial partners in the Envisat consortium, many other companies and research institutes have contributed to the calibration and validation programme under ESA contract as expert support laboratories (ESLs). A major contribution has also been made by the Principal Investigators of approved proposals submitted to ESA in response to a worldwide "Announcement of Opportunity for the Exploitation of the Envisat Data Products" in 1998. Working teams have been formed in which the different participants worked side by side to achieve the objectives of the calibration and validation programme. Validation is a comparison of Envisat level-2 data products and estimates of the different geophysical variables obtained by independent means, the validation instruments. Validation is closely linked to calibration because inconsistencies discovered in the comparison of Envisat Level 2 data products to well-known external instruments can have many different sources, including inaccuracies of the Envisat instrument calibration and the data calibration algorithms. Therefore, initial validation of the geophysical variables has provided feedback to calibration, de-bugging and algorithm improvement. The initial validation phase ended in December 2002 with the Envisat Validation Workshop at which, for a number of products, a final quality statement was given. Full validation of all data products available from the Atmospheric Chemistry Instruments on Envisat (MIPAS, GOMOS and SCIAMACHY) is quite a challenge and therefore it has been decided to adopt a step-wise approach

  16. Comparison of the HadGEM2 climate-chemistry model against in situ and SCIAMACHY atmospheric methane data

    Directory of Open Access Journals (Sweden)

    G. D. Hayman

    2014-12-01

    Full Text Available Wetlands are a major emission source of methane (CH4 globally. In this study, we evaluate wetland emission estimates derived using the UK community land surface model (JULES, the Joint UK Land Earth Simulator against atmospheric observations of methane, including, for the first time, total methane columns derived from the SCIAMACHY instrument on board the ENVISAT satellite. Two JULES wetland emission estimates are investigated: (a from an offline run driven with Climatic Research Unit–National Centers for Environmental Prediction (CRU-NCEP meteorological data and (b from the same offline run in which the modelled wetland fractions are replaced with those derived from the Global Inundation Extent from Multi-Satellites (GIEMS remote sensing product. The mean annual emission assumed for each inventory (181 Tg CH4 per annum over the period 1999–2007 is in line with other recently published estimates. There are regional differences as the unconstrained JULES inventory gives significantly higher emissions in the Amazon (by ~36 Tg CH4 yr−1 and lower emissions in other regions (by up to 10 Tg CH4 yr−1 compared to the JULES estimates constrained with the GIEMS product. Using the UK Hadley Centre's Earth System model with atmospheric chemistry (HadGEM2, we evaluate these JULES wetland emissions against atmospheric observations of methane. We obtain improved agreement with the surface concentration measurements, especially at high northern latitudes, compared to previous HadGEM2 runs using the wetland emission data set of Fung et al. (1991. Although the modelled monthly atmospheric methane columns reproduce the large-scale patterns in the SCIAMACHY observations, they are biased low by 50 part per billion by volume (ppb. Replacing the HadGEM2 modelled concentrations above 300 hPa with HALOE–ACE assimilated TOMCAT output results in a significantly better agreement with the SCIAMACHY observations. The use of the GIEMS product to constrain the JULES

  17. Organic chemistry on Titan

    Science.gov (United States)

    Chang, S.; Scattergood, T.; Aronowitz, S.; Flores, J.

    1979-01-01

    Features taken from various models of Titan's atmosphere are combined in a working composite model that provides environmental constraints within which different pathways for organic chemical synthesis are determined. Experimental results and theoretical modeling suggest that the organic chemistry of the satellite is dominated by two processes: photochemistry and energetic particle bombardment. Photochemical reactions of CH4 in the upper atmosphere can account for the presence of C2 hydrocarbons. Reactions initiated at various levels of the atmosphere by cosmic rays, Saturn 'wind', and solar wind particle bombardment of a CH4-N2 atmospheric mixture can account for the UV-visible absorbing stratospheric haze, the reddish appearance of the satellite, and some of the C2 hydrocarbons. In the lower atmosphere photochemical processes will be important if surface temperatures are sufficiently high for gaseous NH3 to exist. It is concluded that the surface of Titan may contain ancient or recent organic matter (or both) produced in the atmosphere.

  18. Analytical chemistry in space

    CERN Document Server

    Wainerdi, Richard E

    1970-01-01

    Analytical Chemistry in Space presents an analysis of the chemical constitution of space, particularly the particles in the solar wind, of the planetary atmospheres, and the surfaces of the moon and planets. Topics range from space engineering considerations to solar system atmospheres and recovered extraterrestrial materials. Mass spectroscopy in space exploration is also discussed, along with lunar and planetary surface analysis using neutron inelastic scattering. This book is comprised of seven chapters and opens with a discussion on the possibilities for exploration of the solar system by

  19. A steady-state continuous flow chamber for the study of daytime and nighttime chemistry under atmospherically relevant NO levels

    Science.gov (United States)

    Zhang, Xuan; Ortega, John; Huang, Yuanlong; Shertz, Stephen; Tyndall, Geoffrey S.; Orlando, John J.

    2018-05-01

    Experiments performed in laboratory chambers have contributed significantly to the understanding of the fundamental kinetics and mechanisms of the chemical reactions occurring in the atmosphere. Two chemical regimes, classified as high-NO vs. zero-NO conditions, have been extensively studied in previous chamber experiments. Results derived from these two chemical scenarios are widely parameterized in chemical transport models to represent key atmospheric processes in urban and pristine environments. As the anthropogenic NOx emissions in the United States have decreased remarkably in the past few decades, the classic high-NO and zero-NO conditions are no longer applicable to many regions that are constantly impacted by both polluted and background air masses. We present here the development and characterization of the NCAR Atmospheric Simulation Chamber, which is operated in steady-state continuous flow mode for the study of atmospheric chemistry under intermediate NO conditions. This particular chemical regime is characterized by constant sub-ppb levels of NO and can be created in the chamber by precise control of the inflow NO concentration and the ratio of chamber mixing to residence timescales. Over the range of conditions achievable in the chamber, the lifetime of peroxy radicals (RO2), a key intermediate from the atmospheric degradation of volatile organic compounds (VOCs), can be extended to several minutes, and a diverse array of reaction pathways, including unimolecular pathways and bimolecular reactions with NO and HO2, can thus be explored. Characterization experiments under photolytic and dark conditions were performed and, in conjunction with model predictions, provide a basis for interpretation of prevailing atmospheric processes in environments with intertwined biogenic and anthropogenic activities. We demonstrate the proof of concept of the steady-state continuous flow chamber operation through measurements of major first-generation products

  20. A steady-state continuous flow chamber for the study of daytime and nighttime chemistry under atmospherically relevant NO levels

    Directory of Open Access Journals (Sweden)

    X. Zhang

    2018-05-01

    Full Text Available Experiments performed in laboratory chambers have contributed significantly to the understanding of the fundamental kinetics and mechanisms of the chemical reactions occurring in the atmosphere. Two chemical regimes, classified as high-NO vs. zero-NO conditions, have been extensively studied in previous chamber experiments. Results derived from these two chemical scenarios are widely parameterized in chemical transport models to represent key atmospheric processes in urban and pristine environments. As the anthropogenic NOx emissions in the United States have decreased remarkably in the past few decades, the classic high-NO and zero-NO conditions are no longer applicable to many regions that are constantly impacted by both polluted and background air masses. We present here the development and characterization of the NCAR Atmospheric Simulation Chamber, which is operated in steady-state continuous flow mode for the study of atmospheric chemistry under intermediate NO conditions. This particular chemical regime is characterized by constant sub-ppb levels of NO and can be created in the chamber by precise control of the inflow NO concentration and the ratio of chamber mixing to residence timescales. Over the range of conditions achievable in the chamber, the lifetime of peroxy radicals (RO2, a key intermediate from the atmospheric degradation of volatile organic compounds (VOCs, can be extended to several minutes, and a diverse array of reaction pathways, including unimolecular pathways and bimolecular reactions with NO and HO2, can thus be explored. Characterization experiments under photolytic and dark conditions were performed and, in conjunction with model predictions, provide a basis for interpretation of prevailing atmospheric processes in environments with intertwined biogenic and anthropogenic activities. We demonstrate the proof of concept of the steady-state continuous flow chamber operation through measurements of major first

  1. Electron-induced chemistry in microhydrated sulfuric acid clusters

    Czech Academy of Sciences Publication Activity Database

    Lengyel, Jozef; Pysanenko, Andriy; Fárník, Michal

    2017-01-01

    Roč. 17, č. 22 (2017), s. 14171-14180 ISSN 1680-7324 R&D Projects: GA ČR(CZ) GA17-04068S Grant - others:Austrian Science Fund (FWF)(AT) M1983-N34 Institutional support: RVO:61388955 Keywords : induced aerosol formation * particle formation * atmospheric implication Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry

  2. Isotope and Nuclear Chemistry Division annual report, FY 1983

    International Nuclear Information System (INIS)

    Heiken, J.H.; Lindberg, H.A.

    1984-05-01

    This report describes progress in the major research and development programs carried out in FY 1983 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques; development and applications; atmospheric chemistry and transport; and earth and planetary processes

  3. Isotope and Nuclear Chemistry Division annual report, FY 1983

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, J.H.; Lindberg, H.A. (eds.)

    1984-05-01

    This report describes progress in the major research and development programs carried out in FY 1983 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques; development and applications; atmospheric chemistry and transport; and earth and planetary processes.

  4. Isotope and Nuclear Chemistry Division annual report, FY 1984

    International Nuclear Information System (INIS)

    Heiken, J.H.

    1985-04-01

    This report describes progress in the major research and development programs carried out in FY 1984 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques: development and applications; atmospheric chemistry and transport; and earth and planetary processes. 287 refs

  5. Influence of biomass burning emissions on precipitation chemistry in the equatorial forests of Africa

    International Nuclear Information System (INIS)

    Lacaux, J.P.; Lefeivre, B.; Delmas, R.A.; Cros, B.; Andreae, M.O.

    1991-01-01

    As part of the DESCAFE program (Dynamics and Chemistry of the Atmosphere in Equatorial Forest), measurements of precipitation chemistry were made at two sampling sites of the equatorial forest in the Republic of Congo. The measurements were made in order to identify and compare atmospheric sources of gases and particles (mainly biogenic sources and emissions from burning vegetation)

  6. The atmospheric chemistry general circulation model ECHAM5/MESSy1: consistent simulation of ozone from the surface to the mesosphere

    Directory of Open Access Journals (Sweden)

    P. Jöckel

    2006-01-01

    Full Text Available The new Modular Earth Submodel System (MESSy describes atmospheric chemistry and meteorological processes in a modular framework, following strict coding standards. It has been coupled to the ECHAM5 general circulation model, which has been slightly modified for this purpose. A 90-layer model setup up to 0.01 hPa was used at spectral T42 resolution to simulate the lower and middle atmosphere. With the high vertical resolution the model simulates the Quasi-Biennial Oscillation. The model meteorology has been tested to check the influence of the changes to ECHAM5 and the radiation interactions with the new representation of atmospheric composition. In the simulations presented here a Newtonian relaxation technique was applied in the tropospheric part of the domain to weakly nudge the model towards the analysed meteorology during the period 1998–2005. This allows an efficient and direct evaluation with satellite and in-situ data. It is shown that the tropospheric wave forcing of the stratosphere in the model suffices to reproduce major stratospheric warming events leading e.g. to the vortex split over Antarctica in 2002. Characteristic features such as dehydration and denitrification caused by the sedimentation of polar stratospheric cloud particles and ozone depletion during winter and spring are simulated well, although ozone loss in the lower polar stratosphere is slightly underestimated. The model realistically simulates stratosphere-troposphere exchange processes as indicated by comparisons with satellite and in situ measurements. The evaluation of tropospheric chemistry presented here focuses on the distributions of ozone, hydroxyl radicals, carbon monoxide and reactive nitrogen compounds. In spite of minor shortcomings, mostly related to the relatively coarse T42 resolution and the neglect of inter-annual changes in biomass burning emissions, the main characteristics of the trace gas distributions are generally reproduced well. The MESSy

  7. Volatile organic compounds and secondary organic aerosol in the Earth's atmosphere

    International Nuclear Information System (INIS)

    Galbally, Ian

    2007-01-01

    Full text: Recent research, when considered as a whole, suggests that a substantial fraction of both gas-phase and aerosol atmospheric organics have not been, or have very rarely been, directly measured. A review of the global budget for organic gases shows that we cannot account for the loss of approximately half the non-methane organic carbon entering the atmosphere. We suggest that this unaccounted-for loss most likely occurs through formation of secondary organic aerosols (SOAs), indicating that the source for these aerosols is an order of magnitude larger than current estimates. There is evidence that aged secondary organic aerosol can participate in both direct and indirect (cloud modifying) radiative forcing and that this influence may change with other global climate change. Even though our knowledge of the organic composition of the atmosphere is limited, these compounds clearly influence the reactive chemistry of the atmosphere and the formation, composition, and climate impact of aerosols A major challenge in the coming decade of atmospheric chemistry research will be to elucidate the sources, structure, chemistry, fate and influences of these clearly ubiquitous yet poorly constrained organic atmospheric constituents

  8. Observations of Inland Snowpack-driven Bromine Chemistry near the Brooks Range, Alaska

    Science.gov (United States)

    Peterson, P.; Pöhler, D.; Sihler, H.; Zielcke, J.; S., General; Friess, U.; Platt, U.; Simpson, W. R.; Nghiem, S. V.; Shepson, P. B.; Stirm, B. H.; Pratt, K.

    2017-12-01

    The snowpack produces high amounts of reactive bromine in the polar regions during spring. The resulting atmospheric bromine chemistry depletes boundary layer ozone to near-zero levels and alters oxidation of atmospheric pollutants, particularly elemental mercury. To improve our understanding of the spatial extent of this bromine chemistry in Arctic coastal regions, the Purdue Airborne Laboratory for Atmospheric Research (ALAR), equipped with the Heidelberg Imaging differential optical absorption spectroscopy (DOAS) instrument, measured the spatial distribution of BrO, an indicator of active bromine chemistry, over northern Alaska during the March 2012 BRomine Ozone Mercury Experiment (BROMEX). Here we show that this bromine chemistry, commonly associated with snow-covered sea ice regions in the Arctic Ocean, is active 200 km inland in the foothills of the Brooks Range. Profiles retrieved from limb-viewing measurements show this event was located near the snowpack surface, with measured BrO mole ratios of 20 pmol mol-1 in a 500 m thick layer. This observed bromine chemistry is likely enabled by deposition of transported sea salt aerosol or gas phase bromine species from prior activation events to the snowpack. These observations of halogen activation hundreds of km from the coast suggest the impacts of this springtime bromine chemistry are not restricted to sea ice regions and directly adjacent coastal regions.

  9. Correlation between the surface chemistry and the atmospheric corrosion of AZ31, AZ80 and AZ91D magnesium alloys

    International Nuclear Information System (INIS)

    Feliu, S.; Pardo, A.; Merino, M.C.; Coy, A.E.; Viejo, F.; Arrabal, R.

    2009-01-01

    X-ray photoelectron spectroscopy (XPS) was used in order to investigate the correlation between the surface chemistry and the atmospheric corrosion of AZ31, AZ80 and AZ91D magnesium alloys exposed to 98% relative humidity at 50 deg. C. Commercially pure magnesium, used as the reference material, revealed MgO, Mg(OH) 2 and tracers of magnesium carbonate in the air-formed film. For the AZ80 and AZ91D alloys, the amount of magnesium carbonate formed on the surface reached similar values to those of MgO and Mg(OH) 2 . A linear relation between the amount of magnesium carbonate formed on the surface and the subsequent corrosion behaviour in the humid environment was found. The AZ80 alloy revealed the highest amount of magnesium carbonate in the air-formed film and the highest atmospheric corrosion resistance, even higher than the AZ91D alloy, indicating that aluminium distribution in the alloy microstructure influenced the amount of magnesium carbonate formed.

  10. Planetary Sources for Reducing Sulfur Compounds for Cyanosulfidic Origins of Life Chemistry

    Science.gov (United States)

    Ranjan, S.; Todd, Z. R.; Sutherland, J.; Sasselov, D. D.

    2017-12-01

    A key challenge in origin-of-life studies is understanding the chemistry that lead to the origin of the key biomolecules of life, such as the components of nucleic acids, sugars, lipids, and proteins. Prebiotic reaction networks based upon reductive homologation of nitriles (e.g., Patel et al. 2015), are building a tantalizing picture of sustained abiotic synthesis of activated ribonucleotides, amino acids and lipid precursors under environmental conditions thought to have been available on early Earth. Sulfidic anions in aqueous solution (e.g., HS-, HSO3-) under near-UV irradiation play important roles in these chemical pathways. However, the sources and availability of these anions on early Earth have not yet been quantitatively constrained. Here, we evaluate the potential for the atmosphere to serve as a source of sulfidic anions, via dissolution of volcanically-outgassed SO2 and H2S into water reservoirs. We combine photochemical modeling from the literature (Hu et al. 2013) with equilibrium chemistry calculations to place constraints on the partial pressures of SO2 and H2S required to reach the elevated concentrations of sulfidic anions (≥1 μM) thought to be necessary for prebiotic chemistry. We find that micromolar levels of SO2-derived anions (HSO3-, SO3(2-)) are possible through simple exposure of aqueous reservoirs like shallow lakes to the atmosphere, assuming total sulfur emission flux comparable to today. Millimolar levels of these compounds are available during the epochs of elevated volcanism, due to elevated sulfur emission flux. Radiative transfer modeling suggests the atmospheric sulfur will not block the near-UV radiation also required for the cyanosulfidic chemistry. However, H2S-derived anions (e.g., HS-) reach only sub-micromolar levels from atmospheric sources, meaning that prebiotic chemistry invoking such molecules must invoke specialized, local sources. Prebiotic chemistry invoking SO2-derived anions may be considered more robust than

  11. A Model of Titan-like Chemistry to Connect Experiments and Cassini Observations

    Science.gov (United States)

    Raymond, Alexander W.; Sciamma-O’Brien, Ella; Salama, Farid; Mazur, Eric

    2018-02-01

    A numerical model is presented for interpreting the chemical pathways that lead to the experimental mass spectra acquired in the Titan Haze Simulation (THS) laboratory experiments and for comparing the electron density and temperature of the THS plasma to observations made at Titan by the Cassini spacecraft. The THS plasma is a pulsed glow-discharge experiment designed to simulate the reaction of N2/CH4-dominated gas in Titan's upper atmosphere. The transient, one-dimensional model of THS chemistry tracks the evolution of more than 120 species in the direction of the plasma flow. As the minor species C2H2 and C2H4 are added to the N2/CH4-based mixture, the model correctly predicts the emergence of reaction products with up to five carbon atoms in relative abundances that agree well with measured mass spectra. Chemical growth in Titan's upper atmosphere transpires through ion–neutral and neutral–neutral chemistry, and the main reactions involving a series of known atmospheric species are retrieved from the calculation. The model indicates that the electron density and chemistry are steady during more than 99% of the 300 μs long discharge pulse. The model also suggests that the THS ionization fraction and electron temperature are comparable to those measured in Titan's upper atmosphere. These findings reaffirm that the THS plasma is a controlled analog environment for studying the first and intermediate steps of chemistry in Titan's upper atmosphere.

  12. Reactions of substituted benzene anions with N and O atoms: Chemistry in Titan’s upper atmosphere and the interstellar medium

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Zhe-Chen; Bierbaum, Veronica M. [Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309 (United States)

    2016-06-07

    The likely existence of aromatic anions in many important extraterrestrial environments, from the atmosphere of Titan to the interstellar medium (ISM), is attracting increasing attention. Nitrogen and oxygen atoms are also widely observed in the ISM and in the ionospheres of planets and moons. In the current work, we extend previous studies to explore the reactivity of prototypical aromatic anions (deprotonated toluene, aniline, and phenol) with N and O atoms both experimentally and computationally. The benzyl and anilinide anions both exhibit slow associative electron detachment (AED) processes with N atom, and moderate reactivity with O atom in which AED dominates but ionic products are also formed. The reactivity of phenoxide is dramatically different; there is no measurable reaction with N atom, and the moderate reactivity with O atom produces almost exclusively ionic products. The reaction mechanisms are studied theoretically by employing density functional theory calculations, and spin conversion is found to be critical for understanding some product distributions. This work provides insight into the rich gas-phase chemistry of aromatic ion-atom reactions and their relevance to ionospheric and interstellar chemistry.

  13. Atmospheric chemistry of isoflurane, desflurane, and sevoflurane

    DEFF Research Database (Denmark)

    Andersen, Mads P. Sulbæk; Nielsen, Ole John; Karpichev, Boris

    2012-01-01

    (sevoflurane) are estimated at 3.2, 14, and 1.1 years, respectively. The 100 year time horizon global warming potentials of isoflurane, desflurane, and sevoflurane are 510, 2540, and 130, respectively. The atmospheric degradation products of these anesthetics are not of environmental concern....

  14. Observations of peroxyacetyl nitrate (PAN) in the upper troposphere by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS)

    Science.gov (United States)

    Tereszchuk, K. A.; Moore, D. P.; Harrison, J. J.; Boone, C. D.; Park, M.; Remedios, J. J.; Randel, W. J.; Bernath, P. F.

    2013-01-01

    Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short life-time and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) Version 3.0 data set. We report measurements of PAN in Boreal biomass burning plumes recorded during the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) campaign. The retrieval method employed and errors analysis are described in full detail. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) ENVIronmental SATellite (ENVISAT). Three ACE-FTS occultations containing measurements of Boreal biomass burning outflows, recorded during BORTAS, were identified as having coincident measurements with MIPAS. In each case, the MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN. The ACE-FTS PAN data set is used to obtain zonal mean distributions of seasonal averages from ~5 to 20 km. A strong seasonality is clearly observed for PAN concentrations in the global UTLS. Since the

  15. The global atmospheric environment for the next generation

    NARCIS (Netherlands)

    Dentener, F.; Stevenson, D.; Ellingsen, K.; Noije, van T.; Schultz, M.; Amann, M.; Atherton, C.; Bell, N.; Bergmann, D.; Bey, I.; Bouwman, L.; Butler, T.; Cofala, J.; Collins, B.; Drevet, J.; Doherty, R.; Eickhout, B.; Eskes, H.; Fiore, A.; Gauss, M.; Hauglustaine, D.; Horowitz, L.; Isaksen, I.S.A.; Josse, B.; Lawrence, M.; Krol, M.C.; Lamarque, J.F.; Montanaro, V.; Müller, J.F.; Peuch, V.H.; Pitari, G.; Pyle, J.; Rast, S.; Rodriguez, J.; Sanderson, M.; Savage, N.H.; Shindell, D.; Strahan, S.; Szopa, S.; Sudo, K.; Dingenen, van R.; Wild, O.; Zeng, G.

    2006-01-01

    Air quality, ecosystem exposure to nitrogen deposition, and climate change are intimately coupled problems: we assess changes in the global atmospheric environment between 2000 and 2030 using 26 state-of-the-art global atmospheric chemistry models and three different emissions scenarios. The first

  16. Response of lake chemistry to changes in atmospheric deposition and climate in three high-elevation wilderness areas of Colorado

    Science.gov (United States)

    Mast, M. Alisa; Turk, John T.; Clow, David W.; Campbell, Donald D.

    2011-01-01

    Trends in precipitation chemistry and hydrologic and climatic data were examined as drivers of long-term changes in the chemical composition of high-elevation lakes in three wilderness areas in Colorado during 1985-2008. Sulfate concentrations in precipitation decreased at a rate of -0.15 to -0.55 μeq/l/year at 10 high-elevation National Atmospheric Deposition Program stations in the state during 1987-2008 reflecting regional reductions in SO2 emissions. In lakes where sulfate is primarily derived from atmospheric inputs, sulfate concentrations also decreased although the rates generally were less, ranging from -0.12 to -0.27 μeq/l/year. The similarity in timing and sulfur isotopic data support the hypothesis that decreases in atmospheric deposition are driving the response of high-elevation lakes in some areas of the state. By contrast, in lakes where sulfate is derived primarily from watershed weathering sources, sulfate concentrations showed sharp increases during 1985-2008. Analysis of long-term climate records indicates that annual air temperatures have increased between 0.45 and 0.93°C per decade throughout most mountainous areas of Colorado, suggesting climate as a factor. Isotopic data reveal that sulfate in these lakes is largely derived from pyrite, which may indicate climate warming is preferentially affecting the rate of pyrite weathering.

  17. Nitrogen Compounds in Radiation Chemistry

    International Nuclear Information System (INIS)

    Sims, H.E.; Dey, G.R.; Vaudey, C.E.; Peaucelle, C.; Boucher, J.L.; Toulhoat, N.; Bererd, N.; Koppenol, W.H.; Janata, E.; Dauvois, V.; Durand, D.; Legand, S.; Roujou, J.L.; Doizi, D.; Dannoux, A.; Lamouroux, C.

    2009-01-01

    Water radiolysis in presence of N 2 is probably the topic the most controversy in the field of water radiolysis. It still exists a strong discrepancy between the different reports of ammonia formation by water radiolysis in presence of N 2 and moreover in absence of oxygen there is no agreement on the formation or not of nitrogen oxide like NO 2 - and NO 3 -. These discrepancies come from multiple sources: - the complexity of the reaction mechanisms where nitrogen is involved - the experimental difficulties - and, the irradiation conditions. The aim of the workshop is to capitalize the knowledge needed to go further in simulations and understanding the problems caused (or not) by the presence of nitrogen / water in the environment of radioactive materials. Implications are evident in terms of corrosion, understanding of biological systems and atmospheric chemistry under radiation. Topics covered include experimental and theoretical approaches, application and fundamental researches: - Nitrate and Ammonia in radiation chemistry in nuclear cycle; - NOx in biological systems and atmospheric chemistry; - Formation of Nitrogen compounds in Nuclear installations; - Nitrogen in future power plant projects (Gen4, ITER...) and large particle accelerators. This document gathers the transparencies available for 7 of the presentations given at this workshop. These are: - H.E SIMS: 'Radiation Chemistry of Nitrogen Compounds in Nuclear Power Plant'; - G.R. DEY: 'Nitrogen Compounds Formation in the Radiolysis of Aqueous Solutions'; - C.E. VAUDEY et al.: 'Radiolytic corrosion of nuclear graphite studied with the dedicated gas irradiation cell of IPNL'; - J.L. BOUCHER: 'Roles and biosynthesis of NO in eukaryotes and prokaryotes'; - W.H. KOPPENOL: 'Chemistry of NOx'; - E. JANATA: 'Yield of OH in N 2 O saturated aqueous solution'; - V. DAUVOIS: 'Analytical strategy for the study of radiolysis gases'

  18. Methane Feedback on Atmospheric Chemistry: Methods, Models, and Mechanisms

    Science.gov (United States)

    Holmes, Christopher D.

    2018-04-01

    The atmospheric methane (CH4) chemical feedback is a key process for understanding the behavior of atmospheric CH4 and its environmental impact. This work reviews how the feedback is defined and used, then examines the meteorological, chemical, and emission factors that control the feedback strength. Geographical and temporal variations in the feedback are described and explained by HOx (HOx = OH + HO2) production and partitioning. Different CH4 boundary conditions used by models, however, make no meaningful difference to the feedback calculation. The strength of the CH4 feedback depends on atmospheric composition, particularly the atmospheric CH4 burden, and is therefore not constant. Sensitivity tests show that the feedback depends very weakly on temperature, insolation, water vapor, and emissions of NO. While the feedback strength has likely remained within 10% of its present value over the industrial era and likely will over the twenty-first century, neglecting these changes biases our understanding of CH4 impacts. Most environmental consequences per kg of CH4 emissions, including its global warming potential (GWP), scale with the perturbation time, which may have grown as much as 40% over the industrial era and continues to rise.

  19. Presidential Green Chemistry Challenge: 2001 Academic Award

    Science.gov (United States)

    Presidential Green Chemistry Challenge 2001 award winner, Professor Chao-Jun Li, uses metal catalysts in water to carry out chemical reactions that used to need both an oxygen-free atmosphere and hazardous organic solvents.

  20. Experimental and Theoretical Studies of Atmosphereic Inorganic Chlorine Chemistry

    Science.gov (United States)

    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.

  1. Atmospheric Gas-Phase Reactions of Fluorinated Compounds and Alkenes

    DEFF Research Database (Denmark)

    Østerstrøm, Freja From

    Experimental studies have been performed using three different smog chamber setups to investigate the atmospheric chemistry of fluorinated compounds as well as alkenes. The three instruments were at Ford Motor Company, USA, National Center for Atmospheric Research, USA, and Copenhagen Center...

  2. Atmospheric Constituents in GEOS-5: Components for an Earth System Model

    Science.gov (United States)

    Pawson, Steven; Douglass, Anne; Duncan, Bryan; Nielsen, Eric; Ott, Leslie; Strode, Sarah

    2011-01-01

    The GEOS-S model is being developed for weather and climate processes, including the implementation of "Earth System" components. While the stratospheric chemistry capabilities are mature, we are presently extending this to include predictions of the tropospheric composition and chemistry - this includes CO2, CH4, CO, nitrogen species, etc. (Aerosols are also implemented, but are beyond the scope of this paper.) This work will give an overview of our chemistry modules, the approaches taken to represent surface emissions and uptake of chemical species, and some studies of the sensitivity of the atmospheric circulation to changes in atmospheric composition. Results are obtained through focused experiments and multi-decadal simulations.

  3. WATER FORMATION IN THE UPPER ATMOSPHERE OF THE EARLY EARTH

    Energy Technology Data Exchange (ETDEWEB)

    Fleury, Benjamin; Carrasco, Nathalie; Marcq, Emmanuel; Vettier, Ludovic; Määttänen, Anni, E-mail: benjamin.fleury@latmos.ipsl.fr [Université Versailles St-Quentin, Sorbonne Universités, UPMC Univ. Paris 06, CNRS/INSU, LATMOS-IPSL, 11 Boulevard d’Alembert, F-78280 Guyancourt (France)

    2015-07-10

    The water concentration and distribution in the early Earth's atmosphere are important parameters that contribute to the chemistry and the radiative budget of the atmosphere. If the atmosphere above the troposphere is generally considered as dry, photochemistry is known to be responsible for the production of numerous minor species. Here we used an experimental setup to study the production of water in conditions simulating the chemistry above the troposphere of the early Earth with an atmospheric composition based on three major molecules: N{sub 2}, CO{sub 2}, and H{sub 2}. The formation of gaseous products was monitored using infrared spectroscopy. Water was found as the major product, with approximately 10% of the gas products detected. This important water formation is discussed in the context of the early Earth.

  4. Modeling the Chemical Complexity in Titan's Atmosphere

    Science.gov (United States)

    Vuitton, Veronique; Yelle, Roger; Klippenstein, Stephen J.; Horst, Sarah; Lavvas, Panayotis

    2018-06-01

    Titan's atmospheric chemistry is extremely complicated because of the multiplicity of chemical as well as physical processes involved. Chemical processes begin with the dissociation and ionization of the most abundant species, N2 and CH4, by a variety of energy sources, i.e. solar UV and X-ray photons, suprathermal electrons (reactions involving radicals as well as positive and negative ions, all possibly in some excited electronic and vibrational state. Heterogeneous chemistry at the surface of the aerosols could also play a significant role. The efficiency and outcome of these reactions depends strongly on the physical characteristics of the atmosphere, namely pressure and temperature, ranging from 1.5×103 to 10-10 mbar and from 70 to 200 K, respectively. Moreover, the distribution of the species is affected by molecular diffusion and winds as well as escape from the top of the atmosphere and condensation in the lower stratosphere.Photochemical and microphysical models are the keystones of our understanding of Titan's atmospheric chemistry. Their main objective is to compute the distribution and nature of minor chemical species (typically containing up to 6 carbon atoms) and haze particles, respectively. Density profiles are compared to the available observations, allowing to identify important processes and to highlight those that remain to be constrained in the laboratory, experimentally and/or theoretically. We argue that positive ion chemistry is at the origin of complex organic molecules, such as benzene, ammonia and hydrogen isocyanide while neutral-neutral radiative association reactions are a significant source of alkanes. We find that negatively charged macromolecules (m/z ~100) attract the abundant positive ions, which ultimately leads to the formation of the aerosols. We also discuss the possibility that an incoming flux of oxygen from Enceladus, another Saturn's satellite, is responsible for the presence of oxygen-bearing species in Titan's reductive

  5. Atmospheric chemistry of 4:2 fluorotelomer alcohol (n-C4F9CH2CH2OH)

    DEFF Research Database (Denmark)

    Andersen, Mads Peter Sulbæk; Nielsen, Ole John; Hurley, M. D.

    2005-01-01

    Smog chamber/FTIR techniques were used to study the Cl atom initiated oxidation of 4:2 fluorotelomer alcohol (C4F9CH2CH2OH, 4:2 FTOH) in the presence of NOx in 700 Torr of N-2/O-2 diluent at 296 K. Chemical activation effects play an important role in the atmospheric chemistry of the peroxy...

  6. Validation of ozone measurements from the Atmospheric Chemistry Experiment (ACE

    Directory of Open Access Journals (Sweden)

    E. Dupuy

    2009-01-01

    Full Text Available This paper presents extensive {bias determination} analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO instrument. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from nearly 20 satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the average values of the mean relative differences are nearly all within +1 to +8%. At higher altitudes (45–60 km, the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments, with mean relative differences of up to +40% (about +20% on average. For the ACE-MAESTRO version 1.2 ozone data product, mean relative differences are within ±10% (average values within ±6% between 18 and 40 km for both the sunrise and sunset measurements. At higher altitudes (~35–55 km, systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (with mean relative differences down to −10%, the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS, indicating a large positive bias (mean relative differences within +10 to +30% in the 45–55 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

  7. Tropospheric ozone changes, radiative forcing and attribution to emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP

    Directory of Open Access Journals (Sweden)

    D. S. Stevenson

    2013-03-01

    Full Text Available 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%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% 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%, nitrogen oxides (31 ± 9%, carbon monoxide (15 ± 3% and non-methane volatile organic compounds (9 ± 2%; 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 coherent responses of ozone to climate change

  8. Description and Evaluation of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry Model (NMMB-MONARCH) Version 1.0: Gas-Phase Chemistry at Global Scale

    Science.gov (United States)

    Badia, Alba; Jorba, Oriol; Voulgarakis, Apostolos; Dabdub, Donald; Garcia-Pando, Carlos Perez; Hilboll, Andreas; Goncalves, Maria; Janjic, Zavisa

    2017-01-01

    This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMBMONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT).We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3-0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error - RMSE - below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability).

  9. Chemistry Simulations Using MERRA-2 Reanalysis with the GMI CTM and Replay in Support of the Atmospheric Composition Community

    Science.gov (United States)

    Oman, Luke D.; Strahan, Susan E.

    2016-01-01

    Simulations using reanalyzed meteorological conditions have been long used to understand causes of atmospheric composition change over the recent past. Using the new Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) meteorology, chemistry simulations are being conducted to create products covering 1980-2016 for the atmospheric composition community. These simulations use the Global Modeling Initiative (GMI) chemical mechanism in two different models: the GMI Chemical Transport Model (CTM) and the GEOS-5 model developed Replay mode. Replay mode means an integration of the GEOS-5 general circulation model that is incrementally adjusted each time step toward the MERRA-2 analysis. The GMI CTM is a 1 x 1.25 simulation and the MERRA-2 GMI Replay simulation uses the native MERRA-2 approximately horizontal resolution on the cubed sphere. The Replay simulations is driven by the online use of key MERRA-2 meteorological variables (i.e. U, V, T, and surface pressure) with all other variables calculated in response to those variables. A specialized set of transport diagnostics is included in both runs to better understand trace gas transport and changes over the recent past.

  10. Reactor coolant system and containment aqueous chemistry

    International Nuclear Information System (INIS)

    Torgerson, D.F.

    1986-01-01

    Fission products released from fuel during reactor accidents can be subject to a variety of environments that will affect their ultimate behavior. In the reactor coolant system (RCS), for example, neutral or reducing steam conditions, radiation, and surfaces could all have an effect on fission product retention and chemistry. Furthermore, if water is encountered in the RCS, the high temperature aqueous chemistry of fission products must be assessed to determine the quantity and chemical form of fission products released to the containment building. In the containment building, aqueous chemistry will determine the longer-term release of volatile fission products to the containment atmosphere. Over the past few years, the principles of physical chemistry have been rigorously applied to the various chemical conditions described above. This paper reviews the current state of knowledge and discusses the future directions of chemistry research relating to the behavior of fission products in the RCS and containment

  11. Atmospheric Research 2012 Technical Highlights

    Science.gov (United States)

    Lau, William K -M.

    2013-01-01

    This annual report, as before, is intended for a broad audience. Our readers include colleagues within NASA, scientists outside the Agency, science graduate students, and members of the general public. Inside are descriptions of atmospheric research science highlights and summaries of our education and outreach accomplishments for calendar year 2012.The report covers research activities from the Mesoscale Atmospheric Processes Laboratory, the Climate and Radiation Laboratory, the Atmospheric Chemistry and Dynamics Laboratory, and the Wallops Field Support Office under the Office of Deputy Director for Atmospheres, Earth Sciences Division in the Sciences and Exploration Directorate of NASAs Goddard Space Flight Center. The overall mission of the office is advancing knowledge and understanding of the Earths atmosphere. Satellite missions, field campaigns, peer-reviewed publications, and successful proposals are essential to our continuing research.

  12. Atmospheric chemistry of HFC-134a. Kinetic and mechanistic study of the CF3CFHO2 + NO2 reaction

    DEFF Research Database (Denmark)

    Møgelberg, T.E.; Nielsen, O.J.; Sehested, J.

    1994-01-01

    A pulse radiolysis system was used to study the kinetics of the reaction of CF3CFHO2 with NO2. By monitoring the rate of the decay of NO2 using its absorption at 400 nm the reaction rate constant was determined to be k = (5.0 +/- 0.5) x 10(-12) cm3 molecule-1 s-1. A long path length Fourier......-transform infrared technique was used to investigate the thermal decomposition of the product CF3CFHO2NO2. At 296 K in the presence of 700 Torr of air, decomposition of CF3CFHO2NO2 was rapid (greater than 90% decomposition within 3 min). The results are discussed in the context of atmospheric chemistry of CF3CFH2...

  13. Atmospheric chemistry of hydrofluorocarbons and hydrochlorofluorocarbons

    Energy Technology Data Exchange (ETDEWEB)

    Sehested, J

    1995-03-01

    Pulse radiolysis coupled with a time resolved UV absorption detection system and a FTIR spectrometer coupled to a 140 l reaction chamber was used to study the degradation of HCFCs and HFCs in the atmosphere. Reaction rates for a series of reactions of HFCs and HCFCs were investigated: F + RH, R + O{sub 2} + RO{sub 2} + NO, and RO{sub 2} + NO{sub 2} + M, together with UV absorption spectra of the halogenated alkyl (R) and halogenated alkyl peroxy radicals (RO{sub 2}). The products following the self reactions for RO{sub 2} radicals for RO{sub 2} = CF{sub 3}CF{sub 2}O{sub 2}, CF{sub 2}HCF{sub 2}O{sub 2}, CF{sub 3}CH{sub 2}O{sub 2}, CFH{sub 2}CFHO{sub 2}, CF{sub 3}O{sub 2}, and CF{sub 3}C(O)O{sub 2} were investigated by the FTIR setup. The results show that the self reaction of halogenated peroxy radicals give the alkoxy radical, RO, as product. The atmospheric fate of these radicals were C-C bond cleavage for CF{sub 3}CF{sub 2}O, CHF{sub 2}CF{sub 2}O, CFH{sub 2}CHFO, and CF{sub 3}C(O)O; while CF{sub 3}CH{sub 2}O radicals rect with O{sub 2} to give CF{sub 3}CHO and HO{sub 2}. the reaction between CFH{sub 2}O{sub 2} and HO{sub 2} was shown to give 29{+-}7 % CH{sub 2}FCOOH and 72{+-}11 % HCOF as the carbon containing products. (Abstract Truncated)

  14. Atmospheric plasma processes for environmental applications

    OpenAIRE

    Shapoval, Volodymyr

    2012-01-01

    Plasma chemistry is a rapidly growing field which covers applications ranging from technological processing of materials, including biological tissues, to environmental remediation and energy production. The so called atmospheric plasma, produced by electric corona or dielectric barrier discharges in a gas at atmospheric pressure, is particularly attractive for the low costs and ease of operation and maintenance involved. The high concentrations of energetic and chemically active species (e.g...

  15. Numerical modelling of the atmospheric transport, chemical tranformations and deposition of mercury

    Energy Technology Data Exchange (ETDEWEB)

    Petersen, G; Schneider, B; Eppel, D [GKSS-Forschungszentrum Geesthacht GmbH, Geesthacht-Tesperhude (Germany, F.R.). Inst. fuer Physik; Grassl, H [Hamburg Univ. (Germany, F.R.). Meteorologisches Inst. Max-Planck-Institut fuer Meteorologie, Hamburg (Germany, F.R.); Iverfeldt, A [Swedish Environmental Research Inst., Goeteborg (Sweden); Misra, P K; Bloxam, R; Wong, S [Ontario Ministry of the

    1990-01-01

    Based on recent progress in the understanding of mercury chemistry and biogeochemistry and on the availability of mercury emission data bases this study makes an attempt to model the atmospheric transport of mercury, its chemical transformations in the atmosphere, and the fluxes of mercury to and from the earth's surface by means of an EMEP-type Lagrangian trajectory model for Europe and an Eulerian grid model (ADOM) for North America. Preliminary results with a simplified mercury chemistry scheme in the comprehensive Eulerian model and with a linear chemistry in the Lagrangian model show reasonable agreement with observed mercury concentrations in air and precipitation. (orig.) With 3 figs., 4 tabs.

  16. Atmospheric environmental implications of propulsion systems

    Science.gov (United States)

    Mcdonald, Allan J.; Bennett, Robert R.

    1995-01-01

    Three independent studies have been conducted for assessing the impact of rocket launches on the earth's environment. These studies have addressed issues of acid rain in the troposphere, ozone depletion in the stratosphere, toxicity of chemical rocket exhaust products, and the potential impact on global warming from carbon dioxide emissions from rocket launches. Local, regional, and global impact assessments were examined and compared with both natural sources and anthropogenic sources of known atmospheric pollutants with the following conclusions: (1) Neither solid nor liquid rocket launches have a significant impact on the earth's global environment, and there is no real significant difference between the two. (2) Regional and local atmospheric impacts are more significant than global impacts, but quickly return to normal background conditions within a few hours after launch. And (3) vastly increased space launch activities equivalent to 50 U.S. Space Shuttles or 50 Russian Energia launches per year would not significantly impact these conclusions. However, these assessments, for the most part, are based upon homogeneous gas phase chemistry analysis; heterogeneous chemistry from exhaust particulates, such as aluminum oxide, ice contrails, soot, etc., and the influence of plume temperature and afterburning of fuel-rich exhaust products, need to be further addressed. It was the consensus of these studies that computer modeling of interactive plume chemistry with the atmosphere needs to be improved and computer models need to be verified with experimental data. Rocket exhaust plume chemistry can be modified with propellant reformulation and changes in operating conditions, but, based upon the current state of knowledge, it does not appear that significant environmental improvements from propellant formulation changes can be made or are warranted. Flight safety, reliability, and cost improvements are paramount for any new rocket system, and these important aspects

  17. Atmospheric Physics Background – Methods – Trends

    CERN Document Server

    2012-01-01

    On the occasion of the 50th anniversary of the Institute of Atmospheric Physics of the German Aerospace Center (DLR), this book presents more than 50 chapters highlighting results of the institute’s research. The book provides an up-to-date, in-depth survey across the entire field of atmospheric science, including atmospheric dynamics, radiation, cloud physics, chemistry, climate, numerical simulation, remote sensing, instruments and measurements, as well as atmospheric acoustics. The authors have provided a readily comprehensible and self-contained presentation of the complex field of atmospheric science. The topics are of direct relevance for aerospace science and technology. Future research challenges are identified.

  18. Chemical effects in 11-year solar cycle simulations with the Freie Universität Berlin Climate Middle Atmosphere Model with online chemistry (FUB-CMAM-CHEM)

    OpenAIRE

    U. Langematz; J. Grenfell; K. Matthes; P. Mieth; M. Kunze; B. Steil; C. Brühl;  

    2005-01-01

    The impact of 11-year solar cycle variations on stratospheric ozone (O3) is studied with the Freie Universität Berlin Climate Middle Atmosphere Model with interactive chemistry (FUB-CMAM-CHEM). To consider the effect of variations in charged particle precipitation we included an idealized NO x source in the upper mesosphere representing relativistic electron precipitation (REP). Our results suggest that the NO x source by particles and its transport from the mesosphere to the stratosphe...

  19. Assessing the impact of atmospheric chemistry on the fate, transport, and transformation of adulticides in an urban atmosphere

    Science.gov (United States)

    Guberman, S.; Yoon, S.; Guagenti, M. C.; Sheesley, R. J.; Usenko, S.

    2017-12-01

    Urban areas are literal hot spots of mosquito-borne disease transmission and air pollution during the summer months. Public health authorities release aerosolized adulticides to target adult mosquitoes directly in to the atmosphere to control mosquito populations and reduce the threat of diseases (e.g. Zika). Permethrin and malathion are the primary adulticides for controlling adult mosquito populations in Houston, TX and are typically sprayed at night. After being released into the atmosphere adulticides are subject to atmospheric oxidation initiated by atmospheric oxidants (e.g. O3 and NO3) which are driven by anthropogenic air pollutants (e.g. NOx; NO and NO2). Particulate matter (PM) samples were measured at both application and downwind locations. Sampling sites were determined using the combination of atmospheric plume transport models and adulticide application data provided by Harris County Public Health Mosquito Division. Atmospheric PM samples were taken using a Mobile Laboratory, equipped with total suspended PM and PM2.5 (PM with diameter Interestingly, during malathion-use periods, atmospheric malaoxon concentrations measured in the PM2.5 samples were similar to corresponding TSP samples. This suggests that the majority of the malathion (and malaoxon) was associated with fine PM. During permethrin-use periods, atmospheric permethrin concentrations measured in the PM2.5 samples were an order and half lower in magnitude. This suggests that permethrin may be undergoing less volatilization into the gas phase after application as compared to malathion (and or malaoxon). Unlike permethrin, malathion was not sprayed with a carrier or a synergistic compound. As a result, malathion may be more prone to volatilization. The atmospheric oxidation and migration to fine PM may result in decreased efficacy and increase atmospheric transport, both of which have environmental and human health consequences.

  20. Analyzing atmospheric kinetic pathways using PumpKin

    Science.gov (United States)

    Markosyan, A. H.; Luque, A.; Gordillo-Vázquez, F. J.; Ebert, U.

    2013-09-01

    In the present work we show the application of our software tool called PumpKin (pathway reduction method for plasma kinetic models) to find all principal pathways of atmospheric kinetic system, i.e. the dominant reaction sequences, in chemical reaction systems. The goal was to reduce a complex plasma chemistry model. Recent kinetic models of atmospheric chemistry, or any industrial application, contain thousands of chemical reactions and species. The main difficulty is that these reduced chemical pathways depend on timescales, electric field, temperature, pressure etc. PumpKin is a universal tool, which only requires from user the temporal profile of the densities of species and the reaction rates, as well the stoichiometric matrix of the system. Also, the user should specify the timescale of interest.

  1. Trends in lake chemistry in response to atmospheric deposition and climate in selected Class I wilderness areas in Colorado, Idaho, Utah, and Wyoming, 1993-2009

    Science.gov (United States)

    Mast, M. Alisa; Ingersoll, George P.

    2011-01-01

    In 2010, the U.S. Geological Survey, in cooperation with the U.S. Department of Agriculture Forest Service, Air Resource Management, began a study to evaluate long-term trends in lake-water chemistry for 64 high-elevation lakes in selected Class I wilderness areas in Colorado, Idaho, Utah, and Wyoming during 1993 to 2009. The purpose of this report is to describe trends in the chemical composition of these high-elevation lakes. Trends in emissions, atmospheric deposition, and climate variables (air temperature and precipitation amount) are evaluated over a similar period of record to determine likely drivers of changing lake chemistry. Sulfate concentrations in precipitation decreased over the past two decades at high-elevation monitoring stations in the Rocky Mountain region. The trend in deposition chemistry is consistent with regional declines in sulfur dioxide emissions resulting from installation of emission controls at large stationary sources. Trends in nitrogen deposition were not as widespread as those for sulfate. About one-half of monitoring stations showed increases in ammonium concentrations, but few showed significant changes in nitrate concentrations. Trends in nitrogen deposition appear to be inconsistent with available emission inventories, which indicate modest declines in nitrogen emissions in the Rocky Mountain region since the mid-1990s. This discrepancy may reflect uncertainties in emission inventories or changes in atmospheric transformations of nitrogen species that may be affecting deposition processes. Analysis of long-term climate records indicates that average annual mean air temperature minimums have increased from 0.57 to 0.75 °C per decade in mountain areas of the region with warming trends being more pronounced in Colorado. Trends in annual precipitation were not evident over the period 1990 to 2006, although wetter than average years during 1995 to 1997 and drier years during 2001 to 2004 caused a notable decline in precipitation

  2. Laboratory Investigations of Stratospheric Halogen Chemistry

    Science.gov (United States)

    Wine, Paul H.; Nicovich, J. Michael; Stickel, Robert E.; Hynes, Anthony J.

    1997-01-01

    A final report for the NASA-supported project on laboratory investigations of stratospheric halogen chemistry is presented. In recent years, this project has focused on three areas of research: (1) kinetic, mechanistic, and thermochemical studies of reactions which produce weakly bound chemical species of atmospheric interest; (2) development of flash photolysis schemes for studying radical-radical reactions of stratospheric interest; and (3) photochemistry studies of interest for understanding stratospheric chemistry. The first section of this paper contains a discussion of work which has not yet been published. All subsequent chapters contain reprints of published papers that acknowledge support from this grant.

  3. Atmospheric Research 2014 Technical Highlights

    Science.gov (United States)

    Platnick, Steven

    2015-01-01

    Atmospheric research in the Earth Sciences Division (610) consists of research and technology development programs dedicated to advancing knowledge and understanding of the atmosphere and its interaction with the climate of Earth. The Division's goals are to improve understanding of the dynamics and physical properties of precipitation, clouds, and aerosols; atmospheric chemistry, including the role of natural and anthropogenic trace species on the ozone balance in the stratosphere and the troposphere; and radiative properties of Earth's atmosphere and the influence of solar variability on the Earth's climate. Major research activities are carried out in the Mesoscale Atmospheric Processes Laboratory, the Climate and Radiation Laboratory, the Atmospheric Chemistry and Dynamics Laboratory, and the Wallops Field Support Office. The overall scope of the research covers an end-to-end process, starting with the identification of scientific problems, leading to observation requirements for remote-sensing platforms, technology and retrieval algorithm development; followed by flight projects and satellite missions; and eventually, resulting in data processing, analyses of measurements, and dissemination from flight projects and missions. Instrument scientists conceive, design, develop, and implement ultraviolet, infrared, optical, radar, laser, and lidar technology to remotely sense the atmosphere. Members of the various Laboratories conduct field measurements for satellite sensor calibration and data validation, and carry out numerous modeling activities. These modeling activities include climate model simulations, modeling the chemistry and transport of trace species on regional-to-global scales, cloud resolving models, and developing the next-generation Earth system models. Satellite missions, field campaigns, peer-reviewed publications, and successful proposals are essential at every stage of the research process to meeting our goals and maintaining leadership of the

  4. High Energy Radical Chemistry Formation of HCN- rich Atmospheres on early Earth

    Czech Academy of Sciences Publication Activity Database

    Ferus, Martin; Kubelík, Petr; Knížek, Antonín; Pastorek, Adam; Sutherland, J.D.; Civiš, Svatopluk

    2017-01-01

    Roč. 7, č. 1 (2017), č. článku 6275. ISSN 2045-2322 R&D Projects: GA ČR GA17-05076S; GA MŠk(CZ) LM2015083; GA MŠk LG15013 Grant - others:Akademie věd - GA AV ČR(CZ) R200401521 Institutional support: RVO:61388955 Keywords : high-power laser * transform emission-spectroscopy * induced dielectric-breakdown * prebiotic organic-synthesis * nucleobase formation Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 4.259, year: 2016

  5. Self-consistent atmosphere modeling with cloud formation for low-mass stars and exoplanets

    Science.gov (United States)

    Juncher, Diana; Jørgensen, Uffe G.; Helling, Christiane

    2017-12-01

    Context. Low-mass stars and extrasolar planets have ultra-cool atmospheres where a rich chemistry occurs and clouds form. The increasing amount of spectroscopic observations for extrasolar planets requires self-consistent model atmosphere simulations to consistently include the formation processes that determine cloud formation and their feedback onto the atmosphere. Aims: Our aim is to complement the MARCS model atmosphere suit with simulations applicable to low-mass stars and exoplanets in preparation of E-ELT, JWST, PLATO and other upcoming facilities. Methods: The MARCS code calculates stellar atmosphere models, providing self-consistent solutions of the radiative transfer and the atmospheric structure and chemistry. We combine MARCS with a kinetic model that describes cloud formation in ultra-cool atmospheres (seed formation, growth/evaporation, gravitational settling, convective mixing, element depletion). Results: We present a small grid of self-consistently calculated atmosphere models for Teff = 2000-3000 K with solar initial abundances and log (g) = 4.5. Cloud formation in stellar and sub-stellar atmospheres appears for Teff day-night energy transport and no temperature inversion.

  6. Radiation chemistry and the environment

    International Nuclear Information System (INIS)

    Getoff, F.

    1998-01-01

    The rather strong and many-sided pollution of the environment (atmosphere, water resources, soil) as a consequence of human activities is summarized. The solution of the arised problems by application of radiation chemistry methods and the utilization of modern environmentally ''clean'' and economical technologies, founded on electron beam processing, are mentioned. Some basic environmental problems and their solution are briefly discussed: i) Removal of CO 2 from flue gases and its radiation induced utilization. ii) Principals for degradation of aqueous pollutants by electron beam processing in the presence of ozone (synergistic effect). The radiation chemistry as a modern and manifold discipline with very broad applications can also essentially contribute in the conservation of the environment

  7. Radiation chemistry and the environment

    International Nuclear Information System (INIS)

    Getoff, Nikola

    1999-01-01

    The rather strong and many-sided pollution of the environment (atmosphere, water resources, soil) as a consequence of human activity is summarized. The solution of the arised problems by application of radiation chemistry methods and the utilization of modern environmentally 'clean' and economical technologies, founded on electron beam processing, are mentioned. Some basic environmental problems and their solution are briefly discussed. (i) Removal of CO 2 from flue gases and its radiation induced utilization. (ii) Principals for degradation of aqueous pollutants by electron beam processing in the presence of ozone (synergistic effect). The radiation chemistry as a modern and manifold discipline with very broad applications can also essentially contribute in the conservation of the environment

  8. Southeast Atmosphere Studies: learning from model-observation syntheses

    Directory of Open Access Journals (Sweden)

    J. Mao

    2018-02-01

    Full Text Available Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales.This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and

  9. Southeast Atmosphere Studies: learning from model-observation syntheses

    Science.gov (United States)

    Mao, Jingqiu; Carlton, Annmarie; Cohen, Ronald C.; Brune, William H.; Brown, Steven S.; Wolfe, Glenn M.; Jimenez, Jose L.; Pye, Havala O. T.; Ng, Nga Lee; Xu, Lu; McNeill, V. Faye; Tsigaridis, Kostas; McDonald, Brian C.; Warneke, Carsten; Guenther, Alex; Alvarado, Matthew J.; de Gouw, Joost; Mickley, Loretta J.; Leibensperger, Eric M.; Mathur, Rohit; Nolte, Christopher G.; Portmann, Robert W.; Unger, Nadine; Tosca, Mika; Horowitz, Larry W.

    2018-02-01

    Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes) elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS) conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales.This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA) and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and elsewhere. Here we

  10. Impact of RACM2, halogen chemistry, and updated ozone deposition velocity onhemispheric ozone predictions

    Science.gov (United States)

    We incorporate the Regional Atmospheric Chemistry Mechanism (RACM2) into the Community Multiscale Air Quality (CMAQ) hemispheric model and compare model predictions to those obtained using the existing Carbon Bond chemical mechanism with the updated toluene chemistry (CB05TU). Th...

  11. Water physics and chemistry data from bottle casts from the GERDA as part of the Rosenstiel School of Marine and Atmospheric Science (RSMAS) project from 20 July 1955 to 29 May 1957 (NODC Accession 7000057)

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — Water physics and chemistry data were collected from bottle casts from the GERDA from 20 July 1955 to 29 May 1957. Data were collected as part of the Rosenstiel...

  12. Towards a converged barrier height for the entrance channel transition state of the N( 2D) + CH 4 reaction and its implication for the chemistry in Titan's atmosphere

    Science.gov (United States)

    Ouk, Chanda-Malis; Zvereva-Loëte, Natalia; Bussery-Honvault, Béatrice

    2011-10-01

    The N( 2D) + CH 4 reaction appears to be a key reaction for the chemistry of Titan's atmosphere, opening the door to nitrile formation as recently observed by the Cassini-Huygens mission. Faced to the controversy concerning the existence or not of a potential barrier for this reaction, we have carried out accurate ab initio calculations by means of multi-state multi-reference configuration interaction (MS-MR-SDCI) method. These calculations have been partially corrected for the size-consistency errors (SCE) by Davidson, Pople or AQCC corrections. We suggest a barrier height of 3.86 ± 0.84 kJ/mol, including ZPE, for the entrance transition state, in good agreement with the experimental value. Its implication in Titan's atmopsheric chemistry is discussed.

  13. Improvements to the Characterization of Organic Nitrogen Chemistry

    Science.gov (United States)

    Excess atmospheric nitrogen deposition can cause significant harmful effects to ecosystems. Organic nitrogen deposition can be an important contributor to the total nitrogen budget, contributing 10-30%, however there are large uncertainties in the chemistry and deposition of thes...

  14. A synthesis of atmospheric mercury depletion event chemistry in the atmosphere and snow

    Directory of Open Access Journals (Sweden)

    A. J. Poulain

    2008-03-01

    Full Text Available It was discovered in 1995 that, during the spring time, unexpectedly low concentrations of gaseous elemental mercury (GEM occurred in the Arctic air. This was surprising for a pollutant known to have a long residence time in the atmosphere; however conditions appeared to exist in the Arctic that promoted this depletion of mercury (Hg. This phenomenon is termed atmospheric mercury depletion events (AMDEs and its discovery has revolutionized our understanding of the cycling of Hg in Polar Regions while stimulating a significant amount of research to understand its impact to this fragile ecosystem. Shortly after the discovery was made in Canada, AMDEs were confirmed to occur throughout the Arctic, sub-Artic and Antarctic coasts. It is now known that, through a series of photochemically initiated reactions involving halogens, GEM is converted to a more reactive species and is subsequently associated to particles in the air and/or deposited to the polar environment. AMDEs are a means by which Hg is transferred from the atmosphere to the environment that was previously unknown. In this article we review Hg research taken place in Polar Regions pertaining to AMDEs, the methods used to collect Hg in different environmental media, research results of the current understanding of AMDEs from field, laboratory and modeling work, how Hg cycles around the environment after AMDEs, gaps in our current knowledge and the future impacts that AMDEs may have on polar environments. The research presented has shown that while considerable improvements in methodology to measure Hg have been made but the main limitation remains knowing the speciation of Hg in the various media. The processes that drive AMDEs and how they occur are discussed. As well, the role that the snow pack and the sea ice play in the cycling of Hg is presented. It has been found that deposition of Hg from AMDEs occurs at marine coasts and not far inland and that a fraction of the deposited Hg does

  15. Atmospheric evolution on inhabited and lifeless worlds

    CERN Document Server

    Catling, David C

    2017-01-01

    As the search for Earth-like exoplanets gathers pace, in order to understand them, we need comprehensive theories for how planetary atmospheres form and evolve. Written by two well-known planetary scientists, this text explains the physical and chemical principles of atmospheric evolution and planetary atmospheres, in the context of how atmospheric composition and climate determine a planet's habitability. The authors survey our current understanding of the atmospheric evolution and climate on Earth, on other rocky planets within our Solar System, and on planets far beyond. Incorporating a rigorous mathematical treatment, they cover the concepts and equations governing a range of topics, including atmospheric chemistry, thermodynamics, radiative transfer, and atmospheric dynamics, and provide an integrated view of planetary atmospheres and their evolution. This interdisciplinary text is an invaluable one-stop resource for graduate-level students and researchers working across the fields of atmospheric science...

  16. Isotope and Nuclear Chemistry Division annual report FY 1986, October 1985-September 1986

    International Nuclear Information System (INIS)

    Heiken, J.H.

    1987-06-01

    This report describes progress in the major research and development programs carried out in FY 1986 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical diagnostics and weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry

  17. Isotope and Nuclear Chemistry Division annual report FY 1986, October 1985-September 1986

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, J.H. (ed.)

    1987-06-01

    This report describes progress in the major research and development programs carried out in FY 1986 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical diagnostics and weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry.

  18. Seasonal Variation of Atmospheric Composition of Water-Soluble ...

    African Journals Online (AJOL)

    `123456789jkl''''#

    Background Site in Tanzania, East Africa. 1Mkoma S.L. ... fine, coarse and PM10 mass were, 17±4, 52±27 and 69±29 µg/m3 during the 2005 dry season campaign and. 13±5, 34±23 ... particles in ambient air, atmospheric particulate ... especially the fine particle fraction with ..... Atmospheric Chemistry and Physics: From Air.

  19. Chemistry and Heritage

    Science.gov (United States)

    Vittoria Barbarulo, Maria

    2014-05-01

    Chemistry is the central science, as it touches every aspect of the society we live in and it is intertwined with many aspects of our culture; in particular, the strong link between Chemistry and Archaeology and Art History is being explored, offering a penetrating insight into an area of growing interest from an educational point of view. A series of vital and vibrant examples (i.e., ancient bronzes composition, colour changes due to natural pigment decomposition, marble degradation) has been proposed, on one hand, to improve student understanding of the relationship between cultural and scientific issues arising from the examination, the conservation, and the maintenance of cultural Heritage, on the other, to illustrate the role of the underlying Chemistry. In some case studies, a survey of the most relevant atmospheric factors, which are involved in the deterioration mechanisms, has also been presented to the students. First-hand laboratory experiences have been providing an invaluable means of discovering the full and varied world of Chemistry. Furthermore, the promotion of an interdisciplinary investigation of a famous painting or fresco, involving the study of its nature and significance, the definition of its historical context, any related literature, the chemical knowledge of the materials used, may be an excellent occasion to experiment the Content and Language Integrated Learning (CLIL). The aim of this approach is to convey the important message that everyone has the responsibility to care for and preserve Heritage for the benefit of present and future generations.

  20. Dynamics and Chemistry in Jovian Atmospheres: 2D Hydrodynamical Simulations

    Science.gov (United States)

    Bordwell, B. R.; Brown, B. P.; Oishi, J.

    2016-12-01

    A key component of our understanding of the formation and evolution of planetary systems is chemical composition. Problematically, however, in the atmospheres of cooler gas giants, dynamics on the same timescale as chemical reactions pull molecular abundances out of thermochemical equilibrium. These disequilibrium abundances are treated using what is known as the "quench" approximation, based upon the mixing length theory of convection. The validity of this approximation is questionable, though, as the atmospheres of gas giants encompass two distinct dynamic regimes: convective and radiative. To resolve this issue, we conduct 2D hydrodynamical simulations using the state-of-the-art pseudospectral simulation framework Dedalus. In these simulations, we solve the fully compressible equations of fluid motion in a local slab geometry that mimics the structure of a planetary atmosphere (convective zone underlying a radiative zone). Through the inclusion of passive tracers, we explore the transport properties of both regimes, and assess the validity of the classical eddy diffusion parameterization. With the addition of active tracers, we examine the interactions between dynamical and chemical processes, and generate prescriptions for the observational community. By providing insight into mixing and feedback mechanisms in Jovian atmospheres, this research lays a solid foundation for future global simulations and the construction of physically-sound models for current and future observations.

  1. Theory of planetary atmospheres an introduction to their physics and chemistry

    CERN Document Server

    Chamberlain, Joseph W; Marshall, Samantha

    1978-01-01

    For advanced undergraduate and beginning graduate students in atmospheric, oceanic, and climate science, Atmosphere, Ocean and Climate Dynamics is an introductory textbook on the circulations of the atmosphere and ocean and their interaction, with an emphasis on global scales. It will give students a good grasp of what the atmosphere and oceans look like on the large-scale and why they look that way. The role of the oceans in climate and paleoclimate is also discussed. The combination of observations, theory and accompanying illustrative laboratory experiments sets this text apart by making it accessible to students with no prior training in meteorology or oceanography. * Written at a mathematical level that is appealing for undergraduates and beginning graduate students * Provides a useful educational tool through a combination of observations and laboratory demonstrations which can be viewed over the web * Contains instructions on how to reproduce the simple but informative laboratory experiments * Includes...

  2. Presidential Green Chemistry Challenge: 2016 Greener Reaction Conditions Award

    Science.gov (United States)

    Presidential Green Chemistry Challenge 2016 award winner, Dow Agrosciences LLC, developed Instinct®, a technology that reduces fertilizer nitrate leaching to ground and surface waters and atmospheric nitrous oxide emissions. More corn and reduces CO2.

  3. The significance of species segregation for Amazonian chemistry

    NARCIS (Netherlands)

    Ouwersloot, H.G.; Vilà-Guerau de Arellano, J.; Ganzeveld, L.N.; Krol, M.C.; Lelieveld, J.

    2010-01-01

    Tropical rain forest chemistry is driven by the exchange of biogenic compounds, dynamic processes like turbulent mixing and the diurnal variability of the atmospheric boundary layer. The segregation of species due to inefficient turbulent mixing has recently been recognized as a possible relevant

  4. The Atmospheric Chemistry and Canopy Exchange Simulation System (ACCESS: model description and application to a temperate deciduous forest canopy

    Directory of Open Access Journals (Sweden)

    R. D. Saylor

    2013-01-01

    Full Text Available Forest canopies are primary emission sources of biogenic volatile organic compounds (BVOCs and have the potential to significantly influence the formation and distribution of secondary organic aerosol (SOA mass. Biogenically-derived SOA formed as a result of emissions from the widespread forests across the globe may affect air quality in populated areas, degrade atmospheric visibility, and affect climate through direct and indirect forcings. In an effort to better understand the formation of SOA mass from forest emissions, a 1-D column model of the multiphase physical and chemical processes occurring within and just above a vegetative canopy is being developed. An initial, gas-phase-only version of this model, the Atmospheric Chemistry and Canopy Exchange Simulation System (ACCESS, includes processes accounting for the emission of BVOCs from the canopy, turbulent vertical transport within and above the canopy and throughout the height of the planetary boundary layer (PBL, near-explicit representation of chemical transformations, mixing with the background atmosphere and bi-directional exchange between the atmosphere and canopy and the atmosphere and forest floor. The model formulation of ACCESS is described in detail and results are presented for an initial application of the modeling system to Walker Branch Watershed, an isoprene-emission-dominated forest canopy in the southeastern United States which has been the focal point for previous chemical and micrometeorological studies. Model results of isoprene profiles and fluxes are found to be consistent with previous measurements made at the simulated site and with other measurements made in and above mixed deciduous forests in the southeastern United States. Sensitivity experiments are presented which explore how canopy concentrations and fluxes of gas-phase precursors of SOA are affected by background anthropogenic nitrogen oxides (NOx. Results from these experiments suggest that the

  5. Role of Atmospheric Chemistry in the Climate Impacts of Stratospheric Volcanic Injections

    Science.gov (United States)

    Legrande, Allegra N.; Tsigaridis, Kostas; Bauer, Susanne E.

    2016-01-01

    The climate impact of a volcanic eruption is known to be dependent on the size, location and timing of the eruption. However, the chemistry and composition of the volcanic plume also control its impact on climate. It is not just sulfur dioxide gas, but also the coincident emissions of water, halogens and ash that influence the radiative and climate forcing of an eruption. Improvements in the capability of models to capture aerosol microphysics, and the inclusion of chemistry and aerosol microphysics modules in Earth system models, allow us to evaluate the interaction of composition and chemistry within volcanic plumes in a new way. These modeling efforts also illustrate the role of water vapor in controlling the chemical evolution, and hence climate impacts, of the plume. A growing realization of the importance of the chemical composition of volcanic plumes is leading to a more sophisticated and realistic representation of volcanic forcing in climate simulations, which in turn aids in reconciling simulations and proxy reconstructions of the climate impacts of past volcanic eruptions. More sophisticated simulations are expected to help, eventually, with predictions of the impact on the Earth system of any future large volcanic eruptions.

  6. Isotope and Nuclear Chemistry Division annual report FY 1985, October 1984-September 1985

    International Nuclear Information System (INIS)

    Heiken, J.H.

    1986-04-01

    This report describes progress in the major research and development programs carried out in FY 1985 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiations facilities; advanced analytical techniques; development and applications; atmospheric chemistry and transport; and earth and planetary processes

  7. “Impact of RACM2, halogen chemistry, and updated ozonedeposition velocity on hemispheric ozone predictions”

    Science.gov (United States)

    We incorporate the Regional Atmospheric Chemistry Mechanism (RACM2) into the Community Multiscale Air Quality (CMAQ) hemispheric model and compare model predictions to those obtained using the existing Carbon Bond chemical mechanism with updated toluene chemistry (CB05TU). The RA...

  8. Introduction to chemistry and applications in nature of mass independent isotope effects special feature.

    Science.gov (United States)

    Thiemens, Mark H

    2013-10-29

    Stable isotope ratio variations are regulated by physical and chemical laws. These rules depend on a relation with mass differences between isotopes. New classes of isotope variation effects that deviate from mass dependent laws, termed mass independent isotope effects, were discovered in 1983 and have a wide range of applications in basic chemistry and nature. In this special edition, new applications of these effects to physical chemistry, solar system origin models, terrestrial atmospheric and biogenic evolution, polar paleo climatology, snowball earth geology, and present day atmospheric sciences are presented.

  9. Enzymes - important players in green chemistry

    Directory of Open Access Journals (Sweden)

    Agata Tarczykowska

    2017-09-01

    Full Text Available Green chemistry has become a worldwide approach that leads to sustainable growth through application and development of its principles. A lot of work has to be put into designing new processes comprising of materials which do not emit pollutants to the atmosphere. Inventing new safer methods and finding less harmful products can be challenging. Enzymes are a great hope of scientists in the field of green chemistry. Enzymes as catalysts require mild conditions therefore it is a great way of saving resources such as energy or water. Processes with the use of enzymes have become more feasible by being more cost effective and eco friendly. Taking into account the benefits of green chemistry, enzyme biocatalysis has quickly replaced traditional chemical processes in several fields, and this substitution is going to reach even more areas because of new emerging technologies in enzyme engineering.

  10. Laboratory experiments in the study of the chemistry of the outer planets

    Science.gov (United States)

    Scattergood, Thomas W.

    1987-01-01

    It is shown that much information about planetary chemistry and physics can be gained through laboratory work. The types of experiments relevant to planetary research concern fundamental properties, spectral/optical properties, 'Miller-Urey' syntheses, and detailed syntheses. Specific examples of studies of the chemistry in the atmosphere of Titan are described with attention given to gas phase chemistry in the troposphere and the composition of model Titan aerosols. A list of work that still needs to be done is provided.

  11. Chemistry and Transport In a Multi-Dimensional Model

    Science.gov (United States)

    Yung, Yuk L.; Allen, M.; Zurek, R. W.; Salawitch, R. J.

    2002-01-01

    The focus of the work funded under this proposal is the exchange between the stratosphere and the troposphere, and between the troposphere and the blaspheme. These two interfaces represent the frontiers of atmospheric chemistry. It is the combination of exchange processes at both interfaces that ultimately controls how the blaspheme (including human activities) affects the ozone layer. The modeling work was motivated by and attempts to integrate information obtained by aircraft, spacecraft, shuttle and oceanic measurements. The model development and research activities accomplished in the past three years provide a technical and intellectual basis for the research in this group. The innovative part of our research program is related to the IAV of ozone and the hydrological cycle. Other related but independently supported work include the study of isotopic fractionation of atmospheric species, e.g., N2O and CO2. Our theory suggests that we now have the ability to probe the middle atmosphere at a level of sensitivity where subtle details such as the isotopic composition of simple molecules can yield measurable systematic effects. This creates the possibility for probing the chemistry and dynamics of the middle atmosphere using all of the N2O and CO2 isotopologues. In the following we will briefly describe the model development and review the highlights of recent accomplishments.

  12. Atmospheric Electricity

    Science.gov (United States)

    Aplin, Karen; Fischer, Georg

    2018-02-01

    Electricity occurs in atmospheres across the Solar System planets and beyond, spanning spectacular lightning displays in clouds of water or dust, to more subtle effects of charge and electric fields. On Earth, lightning is likely to have existed for a long time, based on evidence from fossilized lightning strikes in ancient rocks, but observations of planetary lightning are necessarily much more recent. The generation and observations of lightning and other atmospheric electrical processes, both from within-atmosphere measurements, and spacecraft remote sensing, can be readily studied using a comparative planetology approach, with Earth as a model. All atmospheres contain charged molecules, electrons, and/or molecular clusters created by ionization from cosmic rays and other processes, which may affect an atmosphere's energy balance both through aerosol and cloud formation, and direct absorption of radiation. Several planets are anticipated to host a "global electric circuit" by analogy with the circuit occurring on Earth, where thunderstorms drive current of ions or electrons through weakly conductive parts of the atmosphere. This current flow may further modulate an atmosphere's radiative properties through cloud and aerosol effects. Lightning could potentially have implications for life through its effects on atmospheric chemistry and particle transport. It has been observed on many of the Solar System planets (Earth, Jupiter, Saturn, Uranus, and Neptune) and it may also be present on Venus and Mars. On Earth, Jupiter, and Saturn, lightning is thought to be generated in deep water and ice clouds, but discharges can be generated in dust, as for terrestrial volcanic lightning, and on Mars. Other, less well-understood mechanisms causing discharges in non-water clouds also seem likely. The discovery of thousands of exoplanets has recently led to a range of further exotic possibilities for atmospheric electricity, though lightning detection beyond our Solar System

  13. Recent advances in study of uranium surface chemistry in China

    International Nuclear Information System (INIS)

    Luo, Lizhu; Lai, Xinchun; Wang, Xiaolin

    2014-01-01

    Uranium is very important in nuclear energy industry; however, uranium and its alloys corrode seriously in various atmospheres because of their chemical reactivities. In China, continuous investigations focused on surface chemistry have been carried out for a thorough understanding of uranium in order to provide technical support for its engineering applications. Oxidation kinetics of uranium and its alloys in oxidizing atmospheres are in good agreement with those in the literature. In addition to the traditional techniques, non-traditional methods have been applied for oxidation kinetics of uranium, and it has been verified that spectroscopic ellipsometry and X-ray diffraction are effective and nondestructive tools for in situ kinetic studies. The inhibition efficiency of oxidizing gas impurities on uranium hydrogenation is found to follow the order CO 2 > CO > O 2 , and the broadening of XPS shoulders with temperature in depth profile of hydrogenated uranium surface is discussed, which is not mentioned in the literature. Significant progress on surface chemistry of alloyed uranium (U-Nb and U-Ti) in hydrogen atmosphere is reported, and it is revealed that the hydrating nucleation and subsequent growth of alloyed uranium are closely connected with the surface states, underlying metal matrix, and it is microstructure-dependent. In this review, the recent advances in uranium surface chemistry in China, published so far mostly in Chinese language, are briefly summarized. Suggestions for further study are made. (orig.)

  14. Upper atmosphere research at INPE

    International Nuclear Information System (INIS)

    Clemesha, B.R.

    1984-01-01

    Upper atmosphere research at INPE is mainly concerned with the chemistry and dynamics of the stratosphere, upper mesosphere and lower thermosphere, and the middle thermosphere. Experimental work includes lidar observations of the stratospheric aerosol, measurements of stratospheric ozone by Dobson spectrophotometers and by balloon and rocket-borne sondes, lidar measurements of atmospheric sodium, and photometric observations of O, O 2 , OH and Na emissions, including interferrometric measurements of the OI6300 emission for the purpose of determing thermospheric winds and temperature. The airglow observations also include measurements of a number of emissions produced by the precipitation of energetic neutral particles generated by charge exchange in the ring current. Some recent results of INPE's upper atmosphere program are presented. (Author) [pt

  15. Atmospheric Oxidation Mechanism of Furfural Initiated by Hydroxyl Radicals.

    Science.gov (United States)

    Zhao, Xiaocan; Wang, Liming

    2017-05-04

    Furfural is emitted into the atmosphere because of its potential applications as an intermediate to alkane fuels from biomass, industrial usages, and biomass burning. The kinetic and mechanistic information on the furfural chemistry is necessary to assess the fate of furfural in the atmosphere and its impact on the air quality. Here we studied the atmospheric oxidation mechanisms of furfural initiated by the OH radicals using quantum chemistry and kinetic calculations. The reaction of OH and furfural was initiated mainly by OH additions to C 2 and C 5 positions, forming R2 and R5 adducts, which could undergo rapid ring-breakage to form R2B and R5B, respectively. Our calculations showed that these intermediate radicals reacted rather slowly with O 2 under the atmospheric conditions because the additions of O 2 to these radicals are only slightly exothermic and highly reversible. Alternatively, these radicals would react directly with O 3 , NO 2 , HO 2 /RO 2 , etc. Namely, the atmospheric oxidation of furfural would unlikely result in ozone formation. Under typical atmospheric conditions, the main products in OH-initiated furfural oxidation include 2-oxo-3-pentene-1,5-dialdehyde, 5-hydroxy-2(5H)-furanone, 4-oxo-2- butenoic acid, and 2,5-furandione. These compounds will likely stay in the gas phase and are subject to further photo-oxidation.

  16. Equilibrium and disequilibrium chemistry of adiabatic, solar-composition planetary atmospheres

    Science.gov (United States)

    Lewis, J. S.

    1976-01-01

    The impact of atmospheric and cloud-structure models on the nonequilibrium chemical behavior of the atmospheres of the Jovian planets is discussed. Quantitative constraints on photochemical, lightning, and charged-particle production of organic matter and chromophores are emphasized whenever available. These considerations imply that inorganic chromophore production is far more important than that of organic chromophores, and that lightning is probably a negligibly significant process relative to photochemistry on Jupiter. Production of complex molecules by gas-phase disequilibrium processes on Saturn, Uranus, and Neptune is severely limited by condensation of even simple intermediates.

  17. Mukilteo water sensor time series - Field work coupling measurements of carbon chemistry and distribution of free-living organisms

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — To estimate the carbon chemistry conditions experienced by free-living organisms, we will conduct coupled biological/carbon chemistry sampling for key zooplankton...

  18. Emerging pattern of global change in the upper atmosphere and ionosphere

    Czech Academy of Sciences Publication Activity Database

    Laštovička, Jan; Akmaev, R. A.; Beig, G.; Bremer, J.; Emmert, J. T.; Jacobi, C.; Jarvis, M.J.; Nedoluha, G.; Portnyagin, Yu. I.; Ulich, T.

    2008-01-01

    Roč. 26, č. 5 (2008), s. 1255-1268 ISSN 0992-7689 R&D Projects: GA MŠk OC 091 Institutional research plan: CEZ:AV0Z30420517 Keywords : Atmospheric composition and structure * Thermosphere – composition and chemistry * Evolution of the atmosphere * Ionosphere * Ionosphere-atmosphere interactions Subject RIV: DG - Athmosphere Sciences, Meteorology Impact factor: 1.660, year: 2008 http://www.ann-geophys.net/26/1255/2008/

  19. New Frontiers Science at Venus from Orbit plus Atmospheric Gas Sampling

    Science.gov (United States)

    Smrekar, Suzanne; Dyar, Melinda; Hensley, Scott; Helbert, Joern; VOX Science and Engineering Teams

    2017-10-01

    Venus remains the most Earth-like body in terms of size, composition, surface age, and insulation. Venus Origins Explorer (VOX) determines how Earth’s twin diverged, and enables breakthroughs in our understanding of rocky planet evolution and habitability. At the time of the Decadal Survey the ability to map mineralogy from orbit (Helbert et al.) and present-day radar techniques to detect active deformation were not fully appreciated. VOX leverages these methods and in-situ noble gases to answer New Frontiers science objectives:1. Atmospheric physics/chemistry: noble gases and isotopes to constrain atmospheric sources, escape processes, and integrated volcanic outgassing; global search for current volcanically outgassed water.2. Past hydrological cycles: global tessera composition to determine the role of volatiles in crustal formation.3. Crustal physics/chemistry: global crustal mineralogy/chemistry, tectonic processes, heat flow, resolve the catastrophic vs. equilibrium resurfacing debate, active geologic processes and possible crustal recycling.4. Crustal weathering: surface-atmosphere weathering reactions from redox state and the chemical equilibrium of the near-surface atmosphere.5. Atmospheric properties/winds: map cloud particle modes and their temporal variations, and track cloud-level winds in the polar vortices.6. Surface-atmosphere interactions: chemical reactions from mineralogy; weathering state between new, recent and older flows; possible volcanically outgassed water.VOX’s Atmosphere Sampling Vehicle (ASV) dips into and samples the well-mixed atmosphere, using Venus Original Constituents Experiment (VOCE) to measure noble gases. VOX’s orbiter carries the Venus Emissivity Mapper (VEM) and the Venus Interferometric Synthetic Aperture Radar (VISAR), and maps the gravity field using Ka-band tracking.VOX is the logical next mission to Venus because it delivers: 1) top priority atmosphere, surface, and interior science; 2) key global data for

  20. Describing the direct and indirect radiative effects of atmospheric aerosols over Europe by using coupled meteorology-chemistry simulations: a contribution from the AQMEII-Phase II exercise

    Science.gov (United States)

    Jimenez-Guerrero, Pedro; Balzarini, Alessandra; Baró, Rocío; Curci, Gabriele; Forkel, Renate; Hirtl, Marcus; Honzak, Luka; Langer, Matthias; Pérez, Juan L.; Pirovano, Guido; San José, Roberto; Tuccella, Paolo; Werhahn, Johannes; Zabkar, Rahela

    2014-05-01

    The study of the response of the aerosol levels in the atmosphere to a changing climate and how this affects the radiative budget of the Earth (direct, semi-direct and indirect effects) is an essential topic to build confidence on climate science, since these feedbacks involve the largest uncertainties nowadays. Air quality-climate interactions (AQCI) are, therefore, a key, but uncertain contributor to the anthropogenic forcing that remains poorly understood. To build confidence in the AQCI studies, regional-scale integrated meteorology-atmospheric chemistry models (i.e., models with on-line chemistry) that include detailed treatment of aerosol life cycle and aerosol impacts on radiation (direct effects) and clouds (indirect effects) are in demand. In this context, the main objective of this contribution is the study and definition of the uncertainties in the climate-chemistry-aerosol-cloud-radiation system associated to the direct radiative forcing and the indirect effect caused by aerosols over Europe, using an ensemble of fully-coupled meteorology-chemistry model simulations with the WRF-Chem model run under the umbrella of AQMEII-Phase 2 international initiative. Simulations were performed for Europe for the entire year 2010. According to the common simulation strategy, the year was simulated as a sequence of 2-day time slices. For better comparability, the seven groups applied the same grid spacing of 23 km and shared common processing of initial and boundary conditions as well as anthropogenic and fire emissions. With exception of a simulation with different cloud microphysics, identical physics options were chosen while the chemistry options were varied. Two model set-ups will be considered here: one sub-ensemble of simulations not taking into account any aerosol feedbacks (the baseline case) and another sub-ensemble of simulations which differs from the former by the inclusion of aerosol-radiation feedback. The existing differences for meteorological

  1. Impact of a future H2-based road transportation sector on the composition and chemistry of the atmosphere – Part 1: Tropospheric composition and air quality

    Directory of Open Access Journals (Sweden)

    D. Wang

    2013-07-01

    Full Text Available Vehicles burning fossil fuel emit a number of substances that change the composition and chemistry of the atmosphere, and contribute to global air and water pollution and climate change. For example, nitrogen oxides and volatile organic compounds (VOCs emitted as byproducts of fossil fuel combustion are key precursors to ground-level ozone and aerosol formation. In addition, on-road vehicles are major CO2 emitters. In order to tackle these problems, molecular hydrogen (H2 has been proposed as an energy carrier to substitute for fossil fuels in the future. However, before implementing any such strategy it is crucial to evaluate its potential impacts on air quality and climate. Here, we evaluate the impact of a future (2050 H2-based road transportation sector on tropospheric chemistry and air quality for several possible growth and technology adoption scenarios. The growth scenarios are based on the high and low emissions Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios, A1FI and B1, respectively. The technological adoption scenarios include H2 fuel cell and H2 internal combustion engine options. The impacts are evaluated with the Community Atmospheric Model Chemistry global chemistry transport model (CAM-Chem. Higher resolution simulations focusing on the contiguous United States are also carried out with the Community Multiscale Air Quality Modeling System (CMAQ regional chemistry transport model. For all scenarios future air quality improves with the adoption of a H2-based road transportation sector; however, the magnitude and type of improvement depend on the scenario. Model results show that the adoption of H2 fuel cells would decrease tropospheric burdens of ozone (7%, CO (14%, NOx (16%, soot (17%, sulfate aerosol (4%, and ammonium nitrate aerosol (12% in the A1FI scenario, and would decrease those of ozone (5%, CO (4%, NOx (11%, soot (7%, sulfate aerosol (4%, and ammonium nitrate aerosol (9% in the B1 scenario

  2. Isotope and nuclear chemistry division. Annual report, FY 1987. Progress report, October 1986-September 1987

    International Nuclear Information System (INIS)

    Barr, D.W.; Heiken, J.H.

    1988-05-01

    This report describes progress in the major research and development programs carried out in FY 1987 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical weapons diagnostics and research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry

  3. Nighttime NOx Chemistry in Coal-Fired Power Plant Plumes

    Science.gov (United States)

    Fibiger, D. L.; McDuffie, E. E.; Dube, W. P.; Veres, P. R.; Lopez-Hilfiker, F.; Lee, B. H.; Green, J. R.; Fiddler, M. N.; Ebben, C. J.; Sparks, T.; Weinheimer, A. J.; Montzka, D.; Campos, T. L.; Cohen, R. C.; Bililign, S.; Holloway, J. S.; Thornton, J. A.; Brown, S. S.

    2015-12-01

    Nitrogen oxides (NOx = NO + NO2) play a key role in atmospheric chemistry. During the day, they catalyze ozone (O3) production, while at night they can react to form nitric acid (HNO3) and nitryl chloride (ClNO2) and remove O3 from the atmosphere. These processes are well studied in the summer, but winter measurements are more limited. Coal-fired power plants are a major source of NOx to the atmosphere, making up approximately 30% of emissions in the US (epa.gov). NOx emissions can vary seasonally, as well as plant-to-plant, with important impacts on the details of the plume chemistry. In particular, due to inefficient plume dispersion, nighttime NOx emissions from power plants are held in concentrated plumes, where rates of mixing with ambient O3 have a strong influence on plume evolution. We will show results from the aircraft-based WINTER campaign over the northeastern United States, where several nighttime intercepts of power plant plumes were made. Several of these intercepts show complete O3 titration, which can have a large influence on NOx lifetime, and thus O3 production, in the plume. When power plant NO emissions exceed background O3 levels, O3 is completely consumed converting NO to NO2. In the presence of O3, NO2 will be oxidized to NO3, which will then react with NO2 to form N2O5, which can then form HNO3 and/or ClNO2 and, ultimately, remove NOx from the atmosphere or provide next-day oxidant sources. If there is no O3 present, however, no further chemistry can occur and NO and NO2 will be transported until mixing with sufficient O3 for higher oxidation products. Modeling results of plume development and mixing, which can tell us more about this transport, will also be presented.

  4. Formation of nucleobases in a Miller–Urey reducing atmosphere

    Czech Academy of Sciences Publication Activity Database

    Ferus, Martin; Pietrucci, F.; Saitta, A. M.; Knížek, Antonín; Kubelík, Petr; Ivanek, Ondřej; Shestivska, Violetta; Civiš, Svatopluk

    2017-01-01

    Roč. 114, č. 17 (2017), s. 4306-4311 ISSN 0027-8424 R&D Projects: GA MŠk LG15013; GA ČR(CZ) GA14-12010S; GA MŠk(CZ) LM2015083; GA MŠk(CZ) 7AMB16FR035 Institutional support: RVO:61388955 Keywords : origin of life * asteroid impact * reducing atmosphere Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 9.661, year: 2016

  5. Organics in environmental ices: sources, chemistry, and impacts

    Directory of Open Access Journals (Sweden)

    V. F. McNeill

    2012-10-01

    Full Text Available The physical, chemical, and biological processes involving organics in ice in the environment impact a number of atmospheric and biogeochemical cycles. Organic material in snow or ice may be biological in origin, deposited from aerosols or atmospheric gases, or formed chemically in situ. In this manuscript, we review the current state of knowledge regarding the sources, properties, and chemistry of organic materials in environmental ices. Several outstanding questions remain to be resolved and fundamental data gathered before an accurate model of transformations and transport of organic species in the cryosphere will be possible. For example, more information is needed regarding the quantitative impacts of chemical and biological processes, ice morphology, and snow formation on the fate of organic material in cold regions. Interdisciplinary work at the interfaces of chemistry, physics and biology is needed in order to fully characterize the nature and evolution of organics in the cryosphere and predict the effects of climate change on the Earth's carbon cycle.

  6. Numerical Modeling of Climate-Chemistry Connections: Recent Developments and Future Challenges

    Directory of Open Access Journals (Sweden)

    Patrick Jöckel

    2013-05-01

    Full Text Available This paper reviews the current state and development of different numerical model classes that are used to simulate the global atmospheric system, particularly Earth’s climate and climate-chemistry connections. The focus is on Chemistry-Climate Models. In general, these serve to examine dynamical and chemical processes in the Earth atmosphere, their feedback, and interaction with climate. Such models have been established as helpful tools in addition to analyses of observational data. Definitions of the global model classes are given and their capabilities as well as weaknesses are discussed. Examples of scientific studies indicate how numerical exercises contribute to an improved understanding of atmospheric behavior. There, the focus is on synergistic investigations combining observations and model results. The possible future developments and challenges are presented, not only from the scientific point of view but also regarding the computer technology and respective consequences for numerical modeling of atmospheric processes. In the future, a stronger cross-linkage of subject-specific scientists is necessary, to tackle the looming challenges. It should link the specialist discipline and applied computer science.

  7. Desorption atmospheric pressure photoionization high-resolution mass spectrometry: a complementary approach for the chemical analysis of atmospheric aerosols

    Czech Academy of Sciences Publication Activity Database

    Parshintsev, J.; Vaikkinen, A.; Lipponen, K.; Vrkoslav, Vladimír; Cvačka, Josef; Kostiainen, R.; Kotiaho, T.; Hartonen, K.; Riekkola, M. L.; Kauppila, T. J.

    2015-01-01

    Roč. 29, č. 13 (2015), s. 1233-1241 ISSN 0951-4198 Grant - others:GA AV ČR(CZ) M200551204 Institutional support: RVO:61388963 Keywords : atmospheric aerosols * mass spectrometry * ambient ionization Subject RIV: CB - Analytical Chemistry , Separation Impact factor: 2.226, year: 2015

  8. The OH-initiated oxidation of atmospheric peroxyacetic acid: Experimental and model studies

    Science.gov (United States)

    Wu, Huihui; Wang, Yin; Li, Huan; Huang, Liubin; Huang, Dao; Shen, Hengqing; Xing, Yanan; Chen, Zhongming

    2017-09-01

    Peroxyacetic acid (PAA, CH3C(O)OOH) plays an important role in atmospheric chemistry, serving as reactive oxidant and affecting radical recycling. However, previous studies revealed an obvious gap between modelled and observed concentrations of atmospheric PAA, which may be partly ascribed to the uncertainty in the kinetics and mechanism of OH-oxidation. In this study, we measured the rate constant of OH radical reaction with PAA (kPAA+OH) and investigated the products in order to develop a more robust atmospheric PAA chemistry. Using the relative rates technique and employing toluene and meta-xylene as reference compounds, the kPAA+OH was determined to be (9.4-11.9) × 10-12 cm3 molecule-1 s-1 at 298 K and 1 atm, which is about (2.5-3.2) times larger than that parameter used in Master Chemical Mechanism v3.3.1 (MCM v3.3.1) (3.70 × 10-12 cm3 molecule-1 s-1). Incorporation of a box model and MCM v3.3.1 with revised PAA chemistry represented a better simulation of atmospheric PAA observed during Wangdu Campaign 2014, a rural site in North China Plain. It is found that OH-oxidation is an important sink of atmospheric PAA in this rural area, accounting for ∼30% of the total loss. Moreover, the major terminal products of PAA-OH reaction were identified as formaldehyde (HCHO) and formic acid (HC(O)OH). The modelled results show that both primary and secondary chemistry play an important role in the large HCHO and HC(O)OH formation under experimental conditions. There should exist the channel of methyl H-abstraction for PAA-OH reaction, which may also provide routes to HCHO and HC(O)OH formation.

  9. Chemical Characterization and Source Apportionment of Size Fractionated Atmospheric Aerosols, and, Evaluating Student Attitudes and Learning in Large Lecture General Chemistry Classes

    Science.gov (United States)

    Allen, Gregory Harold

    Chemical speciation and source apportionment of size fractionated atmospheric aerosols were investigated using laser desorption time-of-flight mass spectrometry (LD TOF-MS) and source apportionment was carried out using carbon-14 accelerator mass spectrometry (14C AMS). Sample collection was carried out using the Davis Rotating-drum Unit for Monitoring impact analyzer in Davis, Colfax, and Yosemite, CA. Ambient atmospheric aerosols collected during the winter of 2010/11 and 2011/12 showed a significant difference in the types of compounds found in the small and large sized particles. The difference was due to the increase number of oxidized carbon species that were found in the small particles size ranges, but not in the large particles size ranges. Overall, the ambient atmospheric aerosols collected during the winter in Davis, CA had and average fraction modern of F14C = 0.753 +/- 0.006, indicating that the majority of the size fractionated particles originated from biogenic sources. Samples collected during the King Fire in Colfax, CA were used to determine the contribution of biomass burning (wildfire) aerosols. Factor analysis was used to reduce the ions found in the LD TOF-MS analysis of the King Fire samples. The final factor analysis generated a total of four factors that explained an overall 83% of the variance in the data set. Two of the factors correlated heavily with increased smoke events during the sample period. The increased smoke events produced a large number of highly oxidized organic aerosols (OOA2) and aromatic compounds that are indicative of biomass burning organic aerosols (WBOA). The signal intensities of the factors generated in the King Fire data were investigated in samples collected in Yosemite and Davis, CA to look at the impact of biomass burning on ambient atmospheric aerosols. In both comparison sample collections the OOA2 and WBOA factors both increased during biomass burning events located near the sampling sites. The correlation

  10. Laboratory Studies of Atmospheric Heterogeneous Chemistry

    Science.gov (United States)

    Keyser, L. F.; Leu, M-T.

    1993-01-01

    In the laboratory, ice films formed by freezing from the liquid or more frequently by deposition from the vapor phase have been used to simulate stratospheric cloud surfaces for measurements of reaction and uptake rates. To obtain intrinsic surface reaction probabilities that can be used in atmospheric models, the area of the film surface that actually takes part in the reaction must be known. It is important to know not only the total surface area but also the film morphology in order to determine where and how the surface is situated and, thus, what fraction of it is available for reaction. Information on the structure of these ice films has been obtained by using several experimental methods. In the sections that follow, these methods will be discussed, then the results will be used to construct a working model of the ice films, and finally the model will be applied to an experimental study of HC1 uptake by H_2O ice.

  11. NWFSC OA facility water chemistry - Ocean acidification species exposure experimental facility

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — We have developed a unique facility for conducting high-quality experiments on marine organisms in seawater with controlled carbon chemistry conditions. The...

  12. Multi-model study of mercury dispersion in the atmosphere: vertical and interhemispheric distribution of mercury species

    Directory of Open Access Journals (Sweden)

    J. Bieser

    2017-06-01

    Full Text Available Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model intercomparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground-based observations of mercury concentration and deposition, here we investigate the vertical and interhemispheric distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on intercontinental flights. The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including interhemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury patterns depending on altitude. High concentrations of oxidized mercury in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parameterizations in the chemistry transport models also proved to have a substantial impact on model results.

  13. A numerical study for global atmospheric transport-chemistry problems

    NARCIS (Netherlands)

    E.J. Spee (Edwin); J.G. Verwer (Jan); P.M. de Zeeuw (Paul); J.G. Blom (Joke); W. Hundsdorfer (Willem)

    1998-01-01

    htmlabstractAtmospheric air quality modeling relies in part on numerical simulation. Required numerical simulations are often hampered by lack of computer capacity and computational speed. This problem is most severe in the field of global modeling where transport and exchange of trace constituents

  14. A numerical study for global atmospheric transport-chemistry problems

    NARCIS (Netherlands)

    E.J. Spee (Edwin); J.G. Verwer (Jan); P.M. de Zeeuw (Paul); J.G. Blom (Joke); W. Hundsdorfer (Willem)

    1997-01-01

    textabstractAtmospheric air quality modeling relies in part on numerical simulation. Required numerical simulations are often hampered by lack of computer capacity and computational speed. This problem is most severe in the field of global modeling where transport and exchange of trace constituents

  15. The GEOS Chemistry Climate Model: Comparisons to Satellite Data

    Science.gov (United States)

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

    2008-05-01

    The Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) has been developed by combining the atmospheric chemistry and transport modules developed over the years at Goddard and the GEOS general circulation model, also developed at Goddard. We will compare model simulations of ozone, and the minor constituents that affect ozone, for the period around 1980 with newly released revised data from the Limb Infrared Monitor of the Stratosphere (LIMS) instrument on Nimbus 4. We will also compare model simulations for the period of the early 2000s with the data from the Microwave Limb Sounder (MLS) and the High Resolution Dynamic Limb Sounder (HRDLS) on the Aura satellite. We will use these comparisons to examine the performance of the model for the present atmosphere and for the change that has occurred during the last 2 decades of ozone loss due to chlorine and bromine compounds released from chlorofluorocarbons and halons.

  16. Tropospheric Ozone Assessment Report: Present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation

    Directory of Open Access Journals (Sweden)

    A. Gaudel

    2018-05-01

    Full Text Available 'The Tropospheric Ozone Assessment Report' (TOAR is an activity of the International Global Atmospheric Chemistry Project. This paper is a component of the report, focusing on the present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation. Utilizing the TOAR surface ozone database, several figures present the global distribution and trends of daytime average ozone at 2702 non-urban monitoring sites, highlighting the regions and seasons of the world with the greatest ozone levels. Similarly, ozonesonde and commercial aircraft observations reveal ozone’s distribution throughout the depth of the free troposphere. Long-term surface observations are limited in their global spatial coverage, but data from remote locations indicate that ozone in the 21st century is greater than during the 1970s and 1980s. While some remote sites and many sites in the heavily polluted regions of East Asia show ozone increases since 2000, many others show decreases and there is no clear global pattern for surface ozone changes since 2000. Two new satellite products provide detailed views of ozone in the lower troposphere across East Asia and Europe, revealing the full spatial extent of the spring and summer ozone enhancements across eastern China that cannot be assessed from limited surface observations. Sufficient data are now available (ozonesondes, satellite, aircraft across the tropics from South America eastwards to the western Pacific Ocean, to indicate a likely tropospheric column ozone increase since the 1990s. The 2014–2016 mean tropospheric ozone burden (TOB between 60°N–60°S from five satellite products is 300 Tg ± 4%. While this agreement is excellent, the products differ in their quantification of TOB trends and further work is required to reconcile the differences. Satellites can now estimate ozone’s global long-wave radiative effect, but evaluation is difficult due to limited

  17. Radiation chemistry in the Jovian stratosphere - Laboratory simulations

    Science.gov (United States)

    Mcdonald, Gene D.; Thompson, W. R.; Sagan, Carl

    1992-01-01

    The results of the present low-pressure/continuous-flow laboratory simulations of H2/He/CH4/NH3 atmospheres' plasma-induced chemistry indicate radiation yields of both hydrocarbon and N2-containing organic compounds which increase with decreasing pressure. On the basis of these findings, upper limits of 1 million-1 billion molecules/sq cm/sec are established for production rates of major auroral-chemistry species in the Jovian stratosphere. It is noted that auroral processes may account for 10-100 percent of the total abundances of most of the observed polar-region organic species.

  18. Recent advances in study of uranium surface chemistry in China

    Energy Technology Data Exchange (ETDEWEB)

    Luo, Lizhu; Lai, Xinchun [Science and Technology on Surface Physics and Chemistry Laboratory, Sichuan (China); Wang, Xiaolin [China Academy of Engineering Physics, Sichuan (China)

    2014-04-01

    Uranium is very important in nuclear energy industry; however, uranium and its alloys corrode seriously in various atmospheres because of their chemical reactivities. In China, continuous investigations focused on surface chemistry have been carried out for a thorough understanding of uranium in order to provide technical support for its engineering applications. Oxidation kinetics of uranium and its alloys in oxidizing atmospheres are in good agreement with those in the literature. In addition to the traditional techniques, non-traditional methods have been applied for oxidation kinetics of uranium, and it has been verified that spectroscopic ellipsometry and X-ray diffraction are effective and nondestructive tools for in situ kinetic studies. The inhibition efficiency of oxidizing gas impurities on uranium hydrogenation is found to follow the order CO{sub 2} > CO > O{sub 2}, and the broadening of XPS shoulders with temperature in depth profile of hydrogenated uranium surface is discussed, which is not mentioned in the literature. Significant progress on surface chemistry of alloyed uranium (U-Nb and U-Ti) in hydrogen atmosphere is reported, and it is revealed that the hydrating nucleation and subsequent growth of alloyed uranium are closely connected with the surface states, underlying metal matrix, and it is microstructure-dependent. In this review, the recent advances in uranium surface chemistry in China, published so far mostly in Chinese language, are briefly summarized. Suggestions for further study are made. (orig.)

  19. Isoprene emission response to drought and the impact on global atmospheric chemistry

    Science.gov (United States)

    Jiang, Xiaoyan; Guenther, Alex; Potosnak, Mark; Geron, Chris; Seco, Roger; Karl, Thomas; Kim, Saewung; Gu, Lianhong; Pallardy, Stephen

    2018-06-01

    Biogenic isoprene emissions play a very important role in atmospheric chemistry. These emissions are strongly dependent on various environmental conditions, such as temperature, solar radiation, plant water stress, ambient ozone and CO2 concentrations, and soil moisture. Current biogenic emission models (i.e., Model of Emissions of Gases and Aerosols from Nature, MEGAN) can simulate emission responses to some of the major driving variables, such as short-term variations in temperature and solar radiation, but the other factors are either missing or poorly represented. In this paper, we propose a new modelling approach that considers the physiological effects of drought stress on plant photosynthesis and isoprene emissions for use in the MEGAN3 biogenic emission model. We test the MEGAN3 approach by integrating the algorithm into the existing MEGAN2.1 biogenic emission model framework embedded into the global Community Land Model of the Community Earth System Model (CLM4.5/CESM1.2). Single-point simulations are compared against available field measurements at the Missouri Ozarks AmeriFlux (MOFLUX) field site. The modelling results show that the MEGAN3 approach of using of a photosynthesis parameter (Vcmax) and soil wetness factor (βt) to determine the drought activity factor leads to better simulated isoprene emissions in non-drought and drought periods. The global simulation with the MEGAN3 approach predicts a 17% reduction in global annual isoprene emissions, in comparison to the value predicted using the default CLM4.5/MEGAN2.1 without any drought effect. This reduction leads to changes in surface ozone and oxidants in the areas where the reduction of isoprene emissions is observed. Based on the results presented in this study, we conclude that it is important to simulate the drought-induced response of biogenic isoprene emission accurately in the coupled Earth System model.

  20. Validation of NO2 and NO from the Atmospheric Chemistry Experiment (ACE

    Directory of Open Access Journals (Sweden)

    M. Schneider

    2008-10-01

    Full Text Available Vertical profiles of NO2 and NO have been obtained from solar occultation measurements by the Atmospheric Chemistry Experiment (ACE, using an infrared Fourier Transform Spectrometer (ACE-FTS and (for NO2 an ultraviolet-visible-near-infrared spectrometer, MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation. In this paper, the quality of the ACE-FTS version 2.2 NO2 and NO and the MAESTRO version 1.2 NO2 data are assessed using other solar occultation measurements (HALOE, SAGE II, SAGE III, POAM III, SCIAMACHY, stellar occultation measurements (GOMOS, limb measurements (MIPAS, OSIRIS, nadir measurements (SCIAMACHY, balloon-borne measurements (SPIRALE, SAOZ and ground-based measurements (UV-VIS, FTIR. Time differences between the comparison measurements were reduced using either a tight coincidence criterion, or where possible, chemical box models. ACE-FTS NO2 and NO and the MAESTRO NO2 are generally consistent with the correlative data. The ACE-FTS and MAESTRO NO2 volume mixing ratio (VMR profiles agree with the profiles from other satellite data sets to within about 20% between 25 and 40 km, with the exception of MIPAS ESA (for ACE-FTS and SAGE II (for ACE-FTS (sunrise and MAESTRO and suggest a negative bias between 23 and 40 km of about 10%. MAESTRO reports larger VMR values than the ACE-FTS. In comparisons with HALOE, ACE-FTS NO VMRs typically (on average agree to ±8% from 22 to 64 km and to +10% from 93 to 105 km, with maxima of 21% and 36%, respectively. Partial column comparisons for NO2 show that there is quite good agreement between the ACE instruments and the FTIRs, with a mean difference of +7.3% for ACE-FTS and +12.8% for MAESTRO.

  1. Wildland fire emissions, carbon, and climate: Plume rise, atmospheric transport, and chemistry processes

    Science.gov (United States)

    Warren Heilman; Yongqiang Liu; Shawn Urbanski; Vladimir Kovalev; Robert Mickler

    2014-01-01

    This paper provides an overview and summary of the current state of knowledge regarding critical atmospheric processes that affect the distribution and concentrations of greenhouse gases and aerosols emitted from wildland fires or produced through subsequent chemical reactions in the atmosphere. These critical atmospheric processes include the dynamics of plume rise,...

  2. Scientific Value of a Saturn Atmospheric Probe Mission

    Science.gov (United States)

    Simon-Miller, A. A.; Lunine, J. I.; Atreya, S. K.; Spilker, T. R.; Coustenis, A.; Atkinson, D. H.

    2012-01-01

    Atmospheric entry probe mISSions to the giant planets can uniquely discriminate between competing theories of solar system formation and the origin and evolution of the giant planets and their atmospheres. This provides for important comparative studies of the gas and ice giants, and to provide a laboratory for studying the atmospheric chemistries, dynamics, and interiors of all the planets including Earth. The giant planets also represent a valuable link to extrasolar planetary systems. As outlined in the recent Planetary Decadal Survey, a Saturn Probe mission - with a shallow probe - ranks as a high priority for a New Frontiers class mission [1].

  3. OH, HO2, and HO2* Radical Chemistry During PROPHET-AMOS 2016: Measurements and Model Comparison

    Science.gov (United States)

    Bottorff, B.; Lew, M.; Rickly, P.; Stevens, P. S.

    2017-12-01

    The hydroxyl (OH) and peroxy radicals, both the hydroperoxy radical (HO2) and organic peroxy radicals (RO2), play an important role in atmospheric chemistry. In addition to controlling lifetimes of many trace gases important to issues of global climate change, reactions of these radicals can also lead to the production of ozone and secondary organic aerosols in the atmosphere. Previous measurements of these radicals in remote forest environments have shown serious discrepancies with modeled concentrations. These results bring into question our understanding of the atmospheric chemistry of isoprene and other biogenic VOCs under low NOX conditions. In the summer of 2016, OH, HO2 and HO2* (HO2 + αRO2) radicals were measured using the Indiana University Laser-Induced Fluorescence Fluorescence Assay by Gas Expansion (LIF-FAGE) technique as part of the Program for Research on Oxidants: PHtochemistry, Emissions, and Transport- Atmospheric Measurements of Oxidants in Summer (PROPHET-AMOS). This campaign took place in a forested area in northern Michigan characterized by high mixing ratios of isoprene and low mixing ratios of NOX. Ambient measurements from this campaign will be compared to previous measurements at this site and to modeled predictions using both the Regional Atmospheric Chemistry Mechanism (RACM2) and the Master Chemical Mechanism. Potential interferences associated with the OH measurements will also be examined.

  4. Opportunities for Laboratory Opacity Chemistry Studies to Facilitate Characterization of Young Giant Planets and Brown Dwarfs

    Science.gov (United States)

    Marley, Mark; Freedman, Richard S.

    2015-01-01

    The thermal emission spectra of young giant planets is shaped by the opacity of atoms and molecules residing in their atmospheres. While great strides have been made in improving the opacities of important molecules, particularly NH3 and CH4, at high temperatures, much more work is needed to understand the opacity and chemistry of atomic Na and K. The highly pressure broadened fundamental band of Na and K in the optical stretches into the near-infrared, strongly influencing the shape of the Y and K spectral bands. Since young giant planets are bright in these bands it is important to understand the influences on the spectral shape. Discerning gravity and atmospheric composition is difficult, if not impossible, without both good atomic opacities as well as an excellent understanding of the relevant atmospheric chemistry. Since Na and K condense at temperatures near 500 to 600 K, the chemistry of the condensation process must be well understood as well, particularly any disequilibrium chemical pathways. Comparisons of the current generation of sophisticated atmospheric models and available data, however, reveal important shortcomings in the models. We will review the current state of observations and theory of young giant planets and will discuss these and other specific examples where improved laboratory measurements for alkali compounds have the potential of substantially improving our understanding of these atmospheres.

  5. THE DISSOCIATIVE RECOMBINATION OF PROTONATED ACRYLONITRILE, CH2CHCNH+, WITH IMPLICATIONS FOR THE NITRILE CHEMISTRY IN DARK MOLECULAR CLOUDS AND THE UPPER ATMOSPHERE OF TITAN

    International Nuclear Information System (INIS)

    Vigren, E.; Hamberg, M.; Zhaunerchyk, V.; Kaminska, M.; Thomas, R. D.; Larsson, M.; Geppert, W. D.; Millar, T. J.; Walsh, C.

    2009-01-01

    Measurements on the dissociative recombination (DR) of protonated acrylonitrile, CH 2 CHCNH + , have been performed at the heavy ion storage ring CRYRING located in the Manne Siegbahn Laboratory in Stockholm, Sweden. It has been found that at ∼2 meV relative kinetic energy about 50% of the DR events involve only ruptures of X-H bonds (where X = C or N) while the rest leads to the production of a pair of fragments each containing two heavy atoms (alongside H and/or H 2 ). The absolute DR cross section has been investigated for relative kinetic energies ranging from ∼1 meV to 1 eV. The thermal rate coefficient has been determined to follow the expression k(T) = 1.78 x 10 -6 (T/300) - 0.80 cm 3 s -1 for electron temperatures ranging from ∼10 to 1000 K. Gas-phase models of the nitrile chemistry in the dark molecular cloud TMC-1 have been run and results are compared with observations. Also, implications of the present results for the nitrile chemistry of Titan's upper atmosphere are discussed.

  6. The GMES Sentinel-5 mission for operational atmospheric monitoring: status and developments

    Science.gov (United States)

    Sierk, Bernd; Bezy, Jean-Loup; Caron, Jerôme; Meynard, Roland; Veihelmann, Ben; Ingmann, Paul

    2017-11-01

    Sentinel-5 is an atmospheric monitoring mission planned in the frame of the joint EU/ESA initiative Global Monitoring for Environment and Security (GMES). The objective of the mission, planned to be launched in 2020, is the operational monitoring of trace gas concentrations for atmospheric chemistry and climate applications.

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

    Science.gov (United States)

    Leone, Stephen R.

    1995-01-01

    The objectives of the research are to measure low temperature laboratory rate coefficients for key reactions relevant to the atmospheres of Titan and Saturn. These reactions are, for example, C2H + H2, CH4, C2H2, and other hydrocarbons which need to be measured at low temperatures, down to approximately 150 K. The results of this work are provided to NASA specialists who study modeling of the hydrocarbon chemistry of the outer planets. The apparatus for this work consists of a pulsed laser photolysis system and a tunable F-center probe laser to monitor the disappearance of C2H. A low temperature cell with a cryogenic circulating fluid in the outer jacket provides the gas handling system for this work. These elements have been described in detail in previous reports. Several new results are completed and the publications are just being prepared. The reaction of C2H with C2H2 has been measured with an improved apparatus down to 154 K. An Arrhenius plot indicates a clear increase in the rate coefficient at the lowest temperatures, most likely because of the long-lived (C4H3) intermediate. The capability to achieve the lowest temperatures in this work was made possible by construction of a new cell and addition of a multipass arrangement for the probe laser, as well as improvements to the laser system.

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

    Science.gov (United States)

    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.

  9. Silicon Chemistry in the Mesosphere and Lower Thermosphere

    Science.gov (United States)

    Plane, John M. C.; Gomez-Martin, Juan Carlos; Feng, Wuhu; Janches, Diego

    2016-01-01

    Silicon is one of the most abundant elements in cosmic dust, and meteoric ablation injects a significant amount of Si into the atmosphere above 80 km. In this study, a new model for silicon chemistry in the mesosphere lower thermosphere is described, based on recent laboratory kinetic studies of Si, SiO,SiO2, and S(exp +). Electronic structure calculations and statistical rate theory are used to show that the likely fate of SiO2 is a two-step hydration to silicic acid (Si(OH)4), which then polymerizes with metal oxides and hydroxides to form meteoric smoke particles. This chemistry is then incorporated into a whole atmosphere chemistry-climate model. The vertical profiles of Si+ and the Si(exp +)Fe(exp +) ratio are shown to be in good agreement with rocket-borne mass spectrometric measurements between 90 and 110 km. Si(exp +) has consistently been observed to be the major meteoric ion around 110 km; this implies that the relative injection rate of Si from meteoric ablation, compared to metals such as Fe and Mg, is significantly larger than expected based on the irrelative chondritic abundances. Finally, the global abundances of SiO and Si(OH)4 show clear evidence of the seasonal meteoric input function, which is much less pronounced in the case of other meteoric species.

  10. Coupled Photochemical and Condensation Model for the Venus Atmosphere

    Science.gov (United States)

    Bierson, Carver; Zhang, Xi; Mendonca, Joao; Liang, Mao-Chang

    2017-10-01

    Ground based and Venus Express observations have provided a wealth of information on the vertical and latitudinal distribution of many chemical species in the Venus atmosphere [1,2]. Previous 1D models have focused on the chemistry of either the lower [3] or middle atmosphere [4,5]. Photochemical models focusing on the sulfur gas chemistry have also been independent from models of the sulfuric acid haze and cloud formation [6,7]. In recent years sulfur-bearing particles have become important candidates for the observed SO2 inversion above 80 km [5]. To test this hypothesis it is import to create a self-consistent model that includes photochemistry, transport, and cloud condensation.In this work we extend the domain of the 1D chemistry model of Zhang et al. (2012) [5] to encompass the region between the surface to 110 km. This model includes a simple sulfuric acid condensation scheme with gravitational settling. It simultaneously solves for the chemistry and condensation allowing for self-consistent cloud formation. We compare the resulting chemical distributions to observations at all altitudes. We have also validated our model cloud mass against pioneer Venus observations [8]. This updated full atmosphere chemistry model is also being applied in our 2D solver (altitude and altitude). With this 2D model we can model how the latitudinal distribution of chemical species depends on the meridional circulation. This allows us to use the existing chemical observations to place constraints on Venus GCMs [9-11].References: [1] Arney et al., JGR:Planets, 2014 [2] Vandaele et al., Icarus 2017 (pt. 1 & 2) [3] Krasnopolsky, Icarus, 2007 [4] Krasnopolsky, Icarus, 2012 [5] Zhang et al., Icarus 2012 [6] Gao et al., Icarus, 2014 [7] Krasnopolsky, Icarus, 2015 [8] Knollenberg and Hunten, JGR:Space Physics, 1980 [9] Lee et al., JGR:Planets, 2007 [10] Lebonnois et al., Towards Understanding the Climate of Venus, 2013 [11] Mendoncca and Read, Planetary and Space Science, 2016

  11. Emission Data For Climate-Chemistry Interactions

    Science.gov (United States)

    Smith, S. J.

    2012-12-01

    Data on anthropogenic and natural emissions of reactive species are a critical input for studies of atmospheric chemistry and climate. The availability and characteristics of anthropogenic emissions data that can be used for such studies are reviewed and pathways for future work discuss Global and regional datasets for historical and future emissions are available, but their characteristics and applicability for specific studies differ. For the first time, a coordinated set of historical emissions (Lamarque et al 2010) and the future projections (van Vuurren et al. 2011) have been developed for use in the CMIP5 and ACCMIP long-term simulation comparison projects. These data have decadal resolution and were designed for long-term, global simulations. These data, however, lack finer-scale spatial and temporal detail that might be needed for some studies. Robust and timely updates of emissions data is generally lacking, although recent updates will be presented. While historical emission data is often treated as known, emissions are uncertain, even though this uncertainty is rarely quantified. Uncertainty varies by species and location. Inverse modeling is starting to indicate where emission data may be uncertain, which opens the way to improving these data overall. Further interaction between the chemistry modeling and inventory development communities are needed. Future projections are intrinsically uncertain, and while institutions and processes are in place to develop and review long-term century-scale scenarios, a need has remained for a wider range in shorter-term (e.g., several decade) projections. Emissions and scenario development communities have been working to fill this need. Communication across disciplines of the assumptions embedded in emissions projections remains a challenge. Atmospheric chemistry models are a central tool needed for studying chemistry-climate interactions. Simpler models, however, are also needed in order to examine interactions

  12. Dust cloud evolution in sub-stellar atmospheres via plasma deposition and plasma sputtering

    Science.gov (United States)

    Stark, C. R.; Diver, D. A.

    2018-04-01

    Context. In contemporary sub-stellar model atmospheres, dust growth occurs through neutral gas-phase surface chemistry. Recently, there has been a growing body of theoretical and observational evidence suggesting that ionisation processes can also occur. As a result, atmospheres are populated by regions composed of plasma, gas and dust, and the consequent influence of plasma processes on dust evolution is enhanced. Aim. This paper aims to introduce a new model of dust growth and destruction in sub-stellar atmospheres via plasma deposition and plasma sputtering. Methods: Using example sub-stellar atmospheres from DRIFT-PHOENIX, we have compared plasma deposition and sputtering timescales to those from neutral gas-phase surface chemistry to ascertain their regimes of influence. We calculated the plasma sputtering yield and discuss the circumstances where plasma sputtering dominates over deposition. Results: Within the highest dust density cloud regions, plasma deposition and sputtering dominates over neutral gas-phase surface chemistry if the degree of ionisation is ≳10-4. Loosely bound grains with surface binding energies of the order of 0.1-1 eV are susceptible to destruction through plasma sputtering for feasible degrees of ionisation and electron temperatures; whereas, strong crystalline grains with binding energies of the order 10 eV are resistant to sputtering. Conclusions: The mathematical framework outlined sets the foundation for the inclusion of plasma deposition and plasma sputtering in global dust cloud formation models of sub-stellar atmospheres.

  13. ATMOSPHERIC CHEMISTRY FOR ASTROPHYSICISTS: A SELF-CONSISTENT FORMALISM AND ANALYTICAL SOLUTIONS FOR ARBITRARY C/O

    International Nuclear Information System (INIS)

    Heng, Kevin; Tsai, Shang-Min; Lyons, James R.

    2016-01-01

    We present a self-consistent formalism for computing and understanding the atmospheric chemistry of exoplanets from the viewpoint of an astrophysicist. Starting from the first law of thermodynamics, we demonstrate that the van’t Hoff equation (which describes the equilibrium constant), Arrhenius equation (which describes the rate coefficients), and procedures associated with the Gibbs free energy (minimization, rescaling) have a common physical and mathematical origin. We address an ambiguity associated with the equilibrium constant, which is used to relate the forward and reverse rate coefficients, and restate its two definitions. By necessity, one of the equilibrium constants must be dimensionless and equate to an exponential function involving the Gibbs free energy, while the other is a ratio of rate coefficients and must therefore possess physical units. We demonstrate that the Arrhenius equation takes on a functional form that is more general than previously stated without recourse to tagging on ad hoc functional forms. Finally, we derive analytical models of chemical systems, in equilibrium, with carbon, hydrogen, and oxygen. We include acetylene and are able to reproduce several key trends, versus temperature and carbon-to-oxygen ratio, published in the literature. The rich variety of behavior that mixing ratios exhibit as a function of the carbon-to-oxygen ratio is merely the outcome of stoichiometric book-keeping and not the direct consequence of temperature or pressure variations

  14. ATMOSPHERIC CHEMISTRY FOR ASTROPHYSICISTS: A SELF-CONSISTENT FORMALISM AND ANALYTICAL SOLUTIONS FOR ARBITRARY C/O

    Energy Technology Data Exchange (ETDEWEB)

    Heng, Kevin; Tsai, Shang-Min [University of Bern, Center for Space and Habitability, Sidlerstrasse 5, CH-3012, Bern (Switzerland); Lyons, James R., E-mail: kevin.heng@csh.unibe.ch [Arizona State University, School of Earth and Space Exploration, Bateman Physical Sciences, Tempe, AZ 85287-1404 (United States)

    2016-01-10

    We present a self-consistent formalism for computing and understanding the atmospheric chemistry of exoplanets from the viewpoint of an astrophysicist. Starting from the first law of thermodynamics, we demonstrate that the van’t Hoff equation (which describes the equilibrium constant), Arrhenius equation (which describes the rate coefficients), and procedures associated with the Gibbs free energy (minimization, rescaling) have a common physical and mathematical origin. We address an ambiguity associated with the equilibrium constant, which is used to relate the forward and reverse rate coefficients, and restate its two definitions. By necessity, one of the equilibrium constants must be dimensionless and equate to an exponential function involving the Gibbs free energy, while the other is a ratio of rate coefficients and must therefore possess physical units. We demonstrate that the Arrhenius equation takes on a functional form that is more general than previously stated without recourse to tagging on ad hoc functional forms. Finally, we derive analytical models of chemical systems, in equilibrium, with carbon, hydrogen, and oxygen. We include acetylene and are able to reproduce several key trends, versus temperature and carbon-to-oxygen ratio, published in the literature. The rich variety of behavior that mixing ratios exhibit as a function of the carbon-to-oxygen ratio is merely the outcome of stoichiometric book-keeping and not the direct consequence of temperature or pressure variations.

  15. A Global Atmospheric Model of Meteoric Iron

    Science.gov (United States)

    Feng, Wuhu; Marsh, Daniel R.; Chipperfield, Martyn P.; Janches, Diego; Hoffner, Josef; Yi, Fan; Plane, John M. C.

    2013-01-01

    The first global model of meteoric iron in the atmosphere (WACCM-Fe) has been developed by combining three components: the Whole Atmosphere Community Climate Model (WACCM), a description of the neutral and ion-molecule chemistry of iron in the mesosphere and lower thermosphere (MLT), and a treatment of the injection of meteoric constituents into the atmosphere. The iron chemistry treats seven neutral and four ionized iron containing species with 30 neutral and ion-molecule reactions. The meteoric input function (MIF), which describes the injection of Fe as a function of height, latitude, and day, is precalculated from an astronomical model coupled to a chemical meteoric ablation model (CABMOD). This newly developed WACCM-Fe model has been evaluated against a number of available ground-based lidar observations and performs well in simulating the mesospheric atomic Fe layer. The model reproduces the strong positive correlation of temperature and Fe density around the Fe layer peak and the large anticorrelation around 100 km. The diurnal tide has a significant effect in the middle of the layer, and the model also captures well the observed seasonal variations. However, the model overestimates the peak Fe+ concentration compared with the limited rocket-borne mass spectrometer data available, although good agreement on the ion layer underside can be obtained by adjusting the rate coefficients for dissociative recombination of Fe-molecular ions with electrons. Sensitivity experiments with the same chemistry in a 1-D model are used to highlight significant remaining uncertainties in reaction rate coefficients, and to explore the dependence of the total Fe abundance on the MIF and rate of vertical transport.

  16. Department of Nuclear Physical Chemistry

    International Nuclear Information System (INIS)

    Mikulski, J.

    1994-01-01

    The research program at the Department of Nuclear Physical Chemistry of the Niewodniczanski Institute of Nuclear Physics is described. The Department consist of three laboratories. First - Laboratory of Physical Chemistry of Separation Processes on which the activity is concentrated on production and separation of neutron deficient isotopes for medical diagnostic. Recently, the main interest was in 111 In which is a promising tracer for cancer diagnostic. To increase the effectiveness of production of indium 111 In the reaction with deuterons on the enriched cadmium target was carried out instead of the previously used one with alpha particles on natural silver. In the second one - Laboratory of Chemistry and Radiochemistry - the systematic studies of physicochemical properties of transition elements in solutions are carried out. The results of the performed experiments were used for the elaboration of new rapid and selective methods for various elements. Some of these results have been applied for separation of trans actinide elements at U-400 cyclotron of JINR Dubna. The third one laboratory -Environmental Radioactivity Laboratory - conducts continuous monitoring of radioactivity contamination of atmosphere. The investigation of different radionuclides concentration in natural environment, mainly in the forest had been carried out

  17. On the numerical treatment of problems in atmospheric chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Aro, Colin J. [Univ. of California, Davis, CA (United States)

    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.

  18. 1988 activity report of the Atmospheric and Aquatic Environment Department

    International Nuclear Information System (INIS)

    Mery, P.

    1988-01-01

    The 1988 activity report of the Atmospheric and Aquatic Environment Department of EDF (Electricity of France) is presented. The activities are focused on the following subjects: development studies in the fields of hydraulic, hydrobiology, meteorology and atmospheric polluants physico-chemistry; application studies involving data analysis from operating or under development power systems; actions concerning cooperation with the Minister of the Environment and the Minister of the Industry. The investigations related to water and atmosphere are reported, as well as congress communications and papers [fr

  19. A Decade of Field Changing Atmospheric Aerosol Research: Outcomes of EPA’s STAR Program

    Science.gov (United States)

    Conference: Gordon Research Conference in Atmospheric Chemistry, July 28 – August 2, 2013, VermontPresentation Type: PosterTitle: An Analysis of EPA’s STAR Program and a Decade of Field Changing Research in Atmospheric AerosolsAuthors: Kristina M. Wagstrom1,2, Sherri ...

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

    Science.gov (United States)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  2. An advanced modeling study on the impacts and atmospheric implications of multiphase dimethyl sulfide chemistry

    Science.gov (United States)

    Hoffmann, Erik Hans; Tilgner, Andreas; Schrödner, Roland; Bräuer, Peter; Wolke, Ralf; Herrmann, Hartmut

    2016-01-01

    Oceans dominate emissions of dimethyl sulfide (DMS), the major natural sulfur source. DMS is important for the formation of non-sea salt sulfate (nss-SO42−) aerosols and secondary particulate matter over oceans and thus, significantly influence global climate. The mechanism of DMS oxidation has accordingly been investigated in several different model studies in the past. However, these studies had restricted oxidation mechanisms that mostly underrepresented important aqueous-phase chemical processes. These neglected but highly effective processes strongly impact direct product yields of DMS oxidation, thereby affecting the climatic influence of aerosols. To address these shortfalls, an extensive multiphase DMS chemistry mechanism, the Chemical Aqueous Phase Radical Mechanism DMS Module 1.0, was developed and used in detailed model investigations of multiphase DMS chemistry in the marine boundary layer. The performed model studies confirmed the importance of aqueous-phase chemistry for the fate of DMS and its oxidation products. Aqueous-phase processes significantly reduce the yield of sulfur dioxide and increase that of methyl sulfonic acid (MSA), which is needed to close the gap between modeled and measured MSA concentrations. Finally, the simulations imply that multiphase DMS oxidation produces equal amounts of MSA and sulfate, a result that has significant implications for nss-SO42− aerosol formation, cloud condensation nuclei concentration, and cloud albedo over oceans. Our findings show the deficiencies of parameterizations currently used in higher-scale models, which only treat gas-phase chemistry. Overall, this study shows that treatment of DMS chemistry in both gas and aqueous phases is essential to improve the accuracy of model predictions. PMID:27688763

  3. Physical-chemical processes of astrophysical interest: nitrogen chemistry

    International Nuclear Information System (INIS)

    Loison, Jean-Christophe; Hickson, Kevin; Hily-Blant, Pierre; Faure, Alexandre; Vuitton, Veronique; Bacmann, A.; Maret, Sebastien; Legal, Romane; Rist, Claire; Roncero, Octavio; Larregaray, Pascal; Hochlaf, Majdi; Senent, M. L.; Capron, Michael; Biennier, Ludovic; Carles, Sophie; Bourgalais, Jeremy; Le Picard, Sebastien; Cordier, Daniel; Guillemin, Jean-Claude; Trolez, Yann; Bertin, M.; Poderoso, H.A.M.; Michaut, X.; Jeseck, P.; Philippe, L.; Fillion, J.H.; Fayolle, E.C.; Linnartz, H.; Romanzin, C.; Oeberg, K.I.; Roueff, Evelyne; Pagani, Laurent; Padovani, Marco; Wakelam, Veronique; Honvault, Beatrice; Zvereva-Loete, Natalia; Ouk, Chanda-Malis; Scribano, Yohann; Hartmann, J.M.; Pineau des Forets, Guillaume; Hernandez, Mario; Lique, Francois; Kalugina, Yulia N.; Stoecklin, T.; Hochlaf, M.; Crespos, C.; Larregaray, P.; Martin-Gondre, L.; Petuya, R.; Quintas Sanchez, E.L.; Zanchet, Alexandre; Rodriguez-Lazcano, Yamilet; Mate, Belen

    2013-06-01

    This document contains the programme and abstracts of contributions to a workshop on nitrogen chemistry within an astrophysical perspective. These contributions have been presented in sessions: Introduction (opening lecture, experimental approaches to molecular astrophysics, theoretical approaches to astrophysics, observations in molecular astrophysics), Physical-chemical theory of the gas phase (time-dependent approach in elementary activity, statistic approach in elementary activity in the case of the N+H_2 reaction, potential energy surfaces for inelastic and reactive collisions, collision rate for N_2H"+, ortho/para selection rules in the chemistry of nitrogen hydrides, cyanides/iso-cyanides excitation in the ISM, CN excitation, radiative association with N_2H as new interstellar anion, ro-vibratory excitation of HCN) Laboratory astrophysics (measurement of reaction products in the CRESUSOL project, reactivity of the CN- anion, N_2 photo-desorption in ices, CRESU study of nitrogen chemistry, chemistry of nitrogen complex molecules), Observations and chemistry of astrophysical media (the problem of interstellar nitrogen fractioning, abundance of N_2 in proto-stellar cores, HNC in Titan atmosphere and nitrogen-related mechanisms in hot Jupiters, HCN and HNC in dark clouds or how theoretical modelling helps in interpreting observations, nitrogen chemistry in cold clouds, deuteration of nitrogen hydrides, nitrogen in interstellar ices, biochemical molecules on Titan, coupling between excitation and chemistry, radiative transfer of nitrogen hydrides, ortho/para chemistry of nitrogen hydrides), Physical-chemical theory of gas-grain interactions (nitrogen reactivity on surfaces, IR spectra of ices of NH_3 and NH_3/N_2 mixtures)

  4. Atmospheric chemistry of ethane and ethylene

    International Nuclear Information System (INIS)

    Aikin, A.C.; Herman, J.R.; Maier, E.J.; McQuillian, C.J.

    1982-01-01

    A detailed study of ethane and ethylene photochemistry is presented for the troposphere and stratosphere. It is demonstrated that the loss of ethane is controlled by OH in the troposphere and Cl in the stratosphere. Observation of ethane show a stratospheric behavior indicative of a free chlorine concentration below 30 km that is only 10% of the predicted value given by both our photochemical model calculations and those done by others. The inferred lower amount of chlorine cannot be explained by heterogeneous processes for concentration of aerosols representing average background conditions, nor does current stratospheric photochemistry show agreement. Chemical destruction of ethane and ethylene within the atmosphere leads to the production of carbon monoxide, formaldehyde, and other products. Tropospheric concentrations of formaldehyde are enhanced by nearly a factor of 3 for an ethylene mixing ratio of 2 ppb. Simultaneous monitoring of formaldehyde and carbon monoxide, as well as other products, will greatly aid in determining the relative importance of different tropospheric CO sources. Peroxyacetyl nitrate (PAN) acts as a reservoir for odd-nitrogen at the expense of HNO 3 HO 2 NO 2 , NO, and NO 2

  5. Atmospheric anthropic impacts tracked by the French atmospheric mobile observatory

    Science.gov (United States)

    Cuesta, J.; Chazette, P.; Flamant, P. H.

    2009-04-01

    A new ATmospheric Mobile ObServatory, so called "ATMOS", has been developed by the LiMAG "Lidar, Meteorology and Geophysics" team of the Institut Pierre Simon Laplace (IPSL) in France, in order to contribute to international field campaigns for studying atmospheric physico-chemistry, air quality and climate (i.e. aerosols, clouds, trace gazes, atmospheric dynamics and energy budget) and the ground-based validation of satellite observations. ATMOS has been deployed in the framework of i) LISAIR, for monitoring air quality in Paris in 2005, ii) AMMA "African Monsoon Multidisciplinary Analysis", in Tamanrasset and in Niamey for observing the aerosols and the atmospheric boundary layer in the Sahara and in the Sahel in 2006, iii) COPS "Convectively and Orographycally driven Precipitation Study" in the Rhin Valley in 2007 and iv) the validation of the spatial mission CALIPSO, launched in April 2006. In the coming years, ATMOS will be deployed i) in the Paris Megacity, in the framework of MEGAPOLI (2009-2010), ii) in southern France (near Marseille) for the Chemistry-Aerosol Mediterranean Experiment CHARMEX (2011-2012) and iii) the validation of ADM-Aeolus in 2010-2011 and Earth-Care in 2012. ATMOS payload is modular, accounting for the different platforms, instruments and measuring techniques. The deployment of ATMOS is an essential contribution to field campaigns, complementing the fixed sites, and a potential alternative of airborne platforms, heavier and more expensive. ATMOS mobile payload comprises both the remote sensing platform MOBILIS ("Moyens mOBIles de téLédetection de l'IPSL") and the in-situ physico-chemical station SAMMO ("Station Aérosols et chiMie MObile"). MOBILIS is an autonomous and high-performance system constituted by a full set of active and passive remote sensing instrumentation (i.e. Lidars and radiometers), whose payload may be adapted for either i) long term fixed monitoring in a maritime container or a shelter, ii) ground-based transect

  6. The Atmospheres of Directly Imaged Planets: Where Has All the Methane Gone?

    Science.gov (United States)

    Marley, Mark S.; Zahnle, Kevin

    2014-01-01

    Methane and ammonia both first appear at lower effective temperatures in brown dwarf atmospheres than equilibrium chemistry models would suggest. This has traditionally been understood as a consequence of vertical mixing timescales being shorter than chemical equilibration timescales in brown dwarf photospheres. Indeed the eddy diffusivity, a variable accounting for the vigor of vertical mixing, has become a standard part of the description of brown dwarf atmosphere models, along with Teff and log g. While some models have suggested that methane is less favored at lower gravity, the almost complete absence of methane in the atmospheres of directly imaged planets, such as those orbiting HR 8799, even at effective temperatures where methane is readily apparent in brown dwarf spectra, has been puzzling. To better understand the paucity of methane in low gravity atmospheres we have revisited the problem of methane chemistry and mixing. We employed a 1-D atmospheric chemistry code augmented with an updated and complete network of the chemical reactions that link CO to CH4. We find the methane abundance at altitudes at or above the effective photosphere is a strong function of surface gravity because higher g shifts the p-T structure to higher pressures (i.e., a given optical depth is proportional to p/g, a relation mitigated somewhat by pressure broadening). Thus quenching in more massive brown dwarfs occurs at a lower temperature and higher pressure, both favoring CH4. We predict that in the lowest mass young giant planets, methane will appear very late, at effective temperatures as low as 600 K rather than the 1200 K seen among field brown dwarfs. This methane deficiency has important implications for the interpretation of spectra as well as methane-based planetary companion searches, such as the NICI survey. The GPI and SPHERE surveys will test these ideas and probe atmospheric chemistry and composition in an entire new range of parameter space. A caveat is that

  7. Improvements to the treatment of organic nitrogen chemistry & deposition in CMAQ

    Science.gov (United States)

    Excess atmospheric nitrogen deposition can cause significant harmful effects to ecosystems. Organic nitrogen deposition can be an important contributor to the total nitrogen budget, contributing 10-30%, however there are large uncertainties in the chemistry and deposition of thes...

  8. Atmospheric chemistry of hydrofluorocarbons and hydrochlorofluorocarbons

    International Nuclear Information System (INIS)

    Sehested, J.

    1995-03-01

    Pulse radiolysis coupled with a time resolved UV absorption detection system and a FTIR spectrometer coupled to a 140 l reaction chamber was used to study the degradation of HCFCs and HFCs in the atmosphere. Reaction rates for a series of reactions of HFCs and HCFCs were investigated: F + RH, R + O 2 + RO 2 + NO, and RO 2 + NO 2 + M, together with UV absorption spectra of the halogenated alkyl (R) and halogenated alkyl peroxy radicals (RO 2 ). The products following the self reactions for RO 2 radicals for RO 2 = CF 3 CF 2 O 2 , CF 2 HCF 2 O 2 , CF 3 CH 2 O 2 , CFH 2 CFHO 2 , CF 3 O 2 , and CF 3 C(O)O 2 were investigated by the FTIR setup. The results show that the self reaction of halogenated peroxy radicals give the alkoxy radical, RO, as product. The atmospheric fate of these radicals were C-C bond cleavage for CF 3 CF 2 O, CHF 2 CF 2 O, CFH 2 CHFO, and CF 3 C(O)O; while CF 3 CH 2 O radicals rect with O 2 to give CF 3 CHO and HO 2 . The reaction between CFH 2 O 2 and HO 2 was shown to give 29±7 % CH 2 FCOOH and 72±11 % HCOF as the carbon containing products. The following CF 3 O reactions were studied: CF 3 O+NO, (5.2±2.7)x10 -11 cm 3 molecule -1 s -1 ; CF 3 O+ 10 13 molecule -1 s -1 ; CF 3 O+H 2 O, 0.2-40x10 -17 cm 3 molecule. Reactions of FCO x , x=1,2,3 and FO x , x=0,1,2, were also studied: k(FC(O)+NO)=(1.0±0.2)x10 -11 cm 3 molecule -1 s -1 , k(FC(O)O 2 +NO)=(2.5±0.8)x10 -11 cm 3 molecule -1 s -1 , k(FC(O)O+NO=(1.3±0.7)x10 -10 cm 3 molecule -1 s -1 , k(FC(O)O+O 3 ) -14 cm 3 molecule - 1 s -1 , k(FO 2 +NO)=(1.45±0 cm 3 molecule -1 s -1 , k(FO 2 +NO 2 )=(1.05±0.15)x10 -13 cm 3 mole k(FO 2 +CO) -16 cm 3 molecule -1 s -1 , k(FO 2 +CH 4 ) - molecule -1 s -1 , k(FO 2 +O 3 )z3.4x10 -16 cm 3 molecule -1 s -1 k(FO+O 3 ) -12 cm 3 molecule -1 s -1 . The results from this together with data available in the literature indicate that HFCs do not destroy stratospheric ozone. (author). 11 tabs.; 23 ills.; 106 refs

  9. Description and Evaluation of IAP-AACM: A Global-regional Aerosol Chemistry Model for the Earth System Model CAS-ESM

    Science.gov (United States)

    Wei, Y.; Chen, X.

    2017-12-01

    We present a first description and evaluation of the IAP Atmospheric Aerosol Chemistry Model (IAP-AACM) which has been integrated into the earth system model CAS-ESM. In this way it is possible to research into interaction of clouds and aerosol by its two-way coupling with the IAP Atmospheric General Circulation Model (IAP-AGCM). The model has a nested global-regional grid based on the Global Environmental Atmospheric Transport Model (GEATM) and the Nested Air Quality Prediction Modeling System (NAQPMS). The AACM provides two optional gas chemistry schemes, the CBM-Z gas chemistry as well as a sulfur oxidize box designed specifically for the CAS-ESM. Now the model driven by AGCM has been applied to a 1-year simulation of tropospheric chemistry both on global and regional scales for 2014, and been evaluated against various observation datasets, including aerosol precursor gas concentration, aerosol mass and number concentrations. Furthermore, global budgets in AACM are compared with other global aerosol models. Generally, the AACM simulations are within the range of other global aerosol model predictions, and the model has a reasonable agreement with observations of gases and particles concentration both on global and regional scales.

  10. Reactions of CF3O radicals with selected alkenes and aromatics under atmospheric conditions

    DEFF Research Database (Denmark)

    Kelly, C.; Sidebottom, H.W.; Treacy, J.

    1994-01-01

    Rate data for the reactions of CF3O radicals with alkenes and aromatic compounds have been determined at 298 K using a relative rate method. The data are analyzed in terms of structure-reactivity relationships, and their importance to the atmospheric chemistry of CF3O discussed.......Rate data for the reactions of CF3O radicals with alkenes and aromatic compounds have been determined at 298 K using a relative rate method. The data are analyzed in terms of structure-reactivity relationships, and their importance to the atmospheric chemistry of CF3O discussed....

  11. Composition and Chemistry of the Neutral Atmosphere of Venus

    Science.gov (United States)

    Marcq, Emmanuel; Mills, Franklin P.; Parkinson, Christopher D.; Vandaele, Ann Carine

    2018-02-01

    This paper deals with the composition and chemical processes occurring in the neutral atmosphere of Venus. Since the last synthesis, observers as well as modellers have emphasised the spatial and temporal variability of minor species, going beyond a static and uniform picture that may have prevailed in the past. The outline of this paper acknowledges this situation and follows closely the different dimensions along which variability in composition can be observed: vertical, latitudinal, longitudinal, temporal. The strong differences between the atmosphere below and above the cloud layers also dictate the structure of this paper. Observational constraints, obtained from both Earth and Venus Express, as well as 1D, 2D and 3D models results obtained since 1997 are also extensively referred and commented by the authors. An non-exhaustive list of topics included follows: modelled and observed latitudinal and vertical profiles of CO and OCS below the clouds of Venus; vertical profiles of CO and SO2 above the clouds as observed by solar occultation and modelled; temporal and spatial variability of sulphur oxides above the clouds. As a conclusion, open questions and topics of interest for further studies are discussed.

  12. Radiation chemistry - extravaganza or an integral component of radiation processing of food

    International Nuclear Information System (INIS)

    Simic, M.G.; DeGraff, E.

    1983-01-01

    The role of radiation chemistry in radiation processing of foods is discussed in detail. A few examples demonstrating the relevance of the radiation chemistry of model systems to food-irradiation technology are given. The importance of irradiation parameters such as dose, dose rate, temperature, atmosphere, physical state and additives in achieving acceptable and high quality of irradiated foods are emphasized. A few examples of radiation-induced free radical reactions in model compounds relevant to foods are also discussed. (author)

  13. The extrapolar SWIFT-model: Fast stratospheric ozone chemistry for global climate models

    OpenAIRE

    Kreyling, Daniel

    2016-01-01

    The goal of this PhD-thesis was the development of a fast yet accurate chemistry scheme for an interactive calculation of the extrapolar stratospheric ozone layer. The SWIFT-model is mainly intended for use in Global Climate Models (GCMs). For computing-time reasons GCMs often do not employ full stratospheric chemistry modules, but use prescribed ozone instead. This method does not consider the interaction between atmospheric dynamics and the ozone layer and can neither resolve the inter-annu...

  14. Sulphur isotope variations in the atmosphere

    International Nuclear Information System (INIS)

    Newman, L.; Krouse, H.R.; Grinenko, V.A.

    1991-01-01

    The measurement of the isotope ratios of sulphur and oxygen can in principal be used to assess sulphur inputs into, transformation within, and removal from the atmosphere. Major inputs arise from both anthropogenic and biogenic activities. Transformations arise from oxidation, neutralization, and other chemical reactions. Advection causes dilution and the main removal processes are dry deposition (governed by gravitation and diffusion) and rain. The admixture of sources can be discerned from their isotopic signatures whereas transformations and removal can be followed from the isotopic fractionation that might occur. In this chapter, the atmospheric sulphur cycle and the associated chemistry are summarized. Also presented is information on natural isotopic variations and fundamental concepts relating to the use of isotopic data to delineate anthropogenic S in the atmosphere. Examples of successful applications of these concepts are given. Finally, consideration is given to the potential of using isotopically enriched sulphur to study transport and transformation of atmospheric S compounds. Refs, figs and tabs

  15. Implementation of an Online Chemistry Model to a Large Eddy Simulation Model (PALM-4U0

    Science.gov (United States)

    Mauder, M.; Khan, B.; Forkel, R.; Banzhaf, S.; Russo, E. E.; Sühring, M.; Kanani-Sühring, F.; Raasch, S.; Ketelsen, K.

    2017-12-01

    Large Eddy Simulation (LES) models permit to resolve relevant scales of turbulent motion, so that these models can capture the inherent unsteadiness of atmospheric turbulence. However, LES models are so far hardly applied for urban air quality studies, in particular chemical transformation of pollutants. In this context, BMBF (Bundesministerium für Bildung und Forschung) funded a joint project, MOSAIK (Modellbasierte Stadtplanung und Anwendung im Klimawandel / Model-based city planning and application in climate change) with the main goal to develop a new highly efficient urban climate model (UCM) that also includes atmospheric chemical processes. The state-of-the-art LES model PALM; Maronga et al, 2015, Geosci. Model Dev., 8, doi:10.5194/gmd-8-2515-2015), has been used as a core model for the new UCM named as PALM-4U. For the gas phase chemistry, a fully coupled 'online' chemistry model has been implemented into PALM. The latest version of the Kinetic PreProcessor (KPP) Version 2.3, has been utilized for the numerical integration of chemical species. Due to the high computational demands of the LES model, compromises in the description of chemical processes are required. Therefore, a reduced chemistry mechanism, which includes only major pollutants namely O3, NO, NO2, CO, a highly simplified VOC chemistry and a small number of products have been implemented. This work shows preliminary results of the advection, and chemical transformation of atmospheric pollutants. Non-cyclic boundaries have been used for inflow and outflow in east-west directions while periodic boundary conditions have been implemented to the south-north lateral boundaries. For practical applications, our approach is to go beyond the simulation of single street canyons to chemical transformation, advection and deposition of air pollutants in the larger urban canopy. Tests of chemistry schemes and initial studies of chemistry-turbulence, transport and transformations are presented.

  16. Solid State Laser Technology Development for Atmospheric Sensing Applications

    Science.gov (United States)

    Barnes, James C.

    1998-01-01

    NASA atmospheric scientists are currently planning active remote sensing missions that will enable global monitoring of atmospheric ozone, water vapor, aerosols and clouds as well as global wind velocity. The measurements of these elements and parameters are important because of the effects they have on climate change, atmospheric chemistry and dynamics, atmospheric transport and, in general, the health of the planet. NASA will make use of Differential Absorption Lidar (DIAL) and backscatter lidar techniques for active remote sensing of molecular constituents and atmospheric phenomena from advanced high-altitude aircraft and space platforms. This paper provides an overview of NASA Langley Research Center's (LaRC's) development of advanced solid state lasers, harmonic generators, and wave mixing techniques aimed at providing the broad range of wavelengths necessary to meet measurement goals of NASA's Earth Science Enterprise.

  17. Chemistry between the stars

    International Nuclear Information System (INIS)

    Kroto, H.W.

    1986-01-01

    During the past 15 years the techniques used by chemists to determine accurate molecular structures have combined with those of radio astronomers to probe the space between the stars. Together they paint a new picture of interstellar space, a picture which shows that vast clouds of gas and dust are continually collapsing to form stars and planets and that the main constituents of these clouds are molecules, some of which are quite complex organic species. It is now known that many of the organic building blocks, useful in the evolution of biologically significant macromolecules, existed long before the Earth was formed. These findings present a challenge to previous widely-accepted theories that such molecules were first generated in the Earth's primaeval atmosphere. In this paper certain aspects of these discoveries are considered with particular emphasis on the contributions made by techniques of use in general chemistry. After a brief astronomical introduction to the Interstellar Medium (ISM) the interaction between chemistry and radioastronomy is discussed. This is followed by details of some exciting, new and quite unexpected advances in our understanding of carbon chemistry, discovered during experiments aimed at understanding some of the more perplexing radioastronomy results. Finally an overview is given of the present knowledge of the molecular composition of the ISM and the resulting implications in so far as the origins of life are concerned. (author)

  18. Chemistry between the stars

    Energy Technology Data Exchange (ETDEWEB)

    Kroto, H W

    1986-01-01

    During the past 15 years the techniques used by chemists to determine accurate molecular structures have combined with those of radio astronomers to probe the space between the stars. Together they paint a new picture of interstellar space, a picture which shows that vast clouds of gas and dust are continually collapsing to form stars and planets and that the main constituents of these clouds are molecules, some of which are quite complex organic species. It is now known that many of the organic building blocks, useful in the evolution of biologically significant macromolecules, existed long before the Earth was formed. These findings present a challenge to previous widely-accepted theories that such molecules were first generated in the Earth's primaeval atmosphere. In this paper certain aspects of these discoveries are considered with particular emphasis on the contributions made by techniques of use in general chemistry. After a brief astronomical introduction to the Interstellar Medium (ISM) the interaction between chemistry and radioastronomy is discussed. This is followed by details of some exciting, new and quite unexpected advances in our understanding of carbon chemistry, discovered during experiments aimed at understanding some of the more perplexing radioastronomy results. Finally an overview is given of the present knowledge of the molecular composition of the ISM and the resulting implications in so far as the origins of life are concerned.

  19. Effects of hydraulic shellfish harvesting on benthic communities and sediment chemistry 2009-2013

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — The effects of hydraulic shellfish harvesting on the ecology of biological communities and chemistry of benthic sediments were investigated through a series of...

  20. Dragonfly: In Situ Exploration of Titan's Organic Chemistry and Habitability

    Science.gov (United States)

    Turtle, E. P.; Barnes, J. W.; Trainer, M. G.; Lorenz, R. D.

    2017-12-01

    Titan's abundant complex carbon-rich chemistry, interior ocean, and past presence of liquid water on the surface make it an ideal destination to study prebiotic chemical processes and document the habitability of an extraterrestrial environment. Titan exploration is a high science priority due to the level of organic synthesis that it supports. Moreover, opportunities for organics to have interacted with liquid water at the surface (e.g., in impact melt sheets) increase the potential for chemical processes to progress further, providing an unparalleled opportunity to investigate prebiotic chemistry, as well as to search for signatures of potential water-based or even hydrocarbon-based life. The diversity of Titan's surface materials and environments drives the scientific need to be able to sample a variety of locations, thus mobility is key for in situ measurements. Titan's atmosphere is 4 times denser than Earth's reducing the wing/rotor area required to generate a given amount of lift, and the low gravity reduces the required magnitude of lift, making heavier-than-air mobility highly efficient. Dragonfly is a rotorcraft lander mission proposed to NASA's New Frontiers Program to take advantage of Titan's unique natural laboratory to understand how far chemistry can progress in environments that provide key ingredients for life. Measuring the compositions of materials in different environments will reveal how far organic chemistry has progressed. Surface material can be sampled into a mass spectrometer to identify the chemical components available and processes at work to produce biologically relevant compounds. Bulk elemental surface composition can be determined by a neutron-activated gamma-ray spectrometer. Meteorology measurements can characterize Titan's atmosphere and diurnal and spatial variations therein. Geologic features can be characterized via remote-sensing observations, which also provide context for samples. Seismic sensing can probe subsurface

  1. High Resolution Spectra of Carbon Monoxide, Propane and Ammonia for Atmospheric Remote Sensing

    Science.gov (United States)

    Beale, Christopher Andrew

    Spectroscopy is a critical tool for analyzing atmospheric data. Identification of atmospheric parameters such as temperature, pressure and the existence and concentrations of constituent gases via remote sensing techniques are only possible with spectroscopic data. These form the basis of model atmospheres which may be compared to observations to determine such parameters. To this end, this dissertation explores the spectroscopy of three molecules: ammonia, propane and carbon monoxide. Infrared spectra have been recorded for ammonia in the region 2400-9000 cm-1. These spectra were recorded at elevated temperatures (from 293-973 K) using a Fourier Transform Spectrometer (FTS). Comparison between the spectra recorded at different temperatures yielded experimental lower state energies. These spectra resulted in the measurement of roughly 30000 lines and about 3000 quantum assignments. In addition spectra of propane were recorded at elevated temperatures (296-700 K) using an FTS. Atmospheres with high temperatures require molecular data at appropriate conditions. This dissertation describes collection of such data and the potential application to atmospheres in our solar system, such as auroral regions in Jupiter, to those of planets orbiting around other stars and cool sub-stellar objects known as brown dwarfs. The spectra of propane and ammonia provide the highest resolution and most complete experimental study of these gases in their respective spectral regions at elevated temperatures. Detection of ammonia in an exoplanet or detection of propane in the atmosphere of Jupiter will most likely rely on the work presented here. The best laboratory that we have to study atmospheres is our own planet. The same techniques that are applied to these alien atmospheres originated on Earth. As such it is appropriate to discuss remote sensing of our own atmosphere. This idea is explored through analysis of spectroscopic data recorded by an FTS on the Atmospheric Chemistry

  2. Chapter 4 Gaseous Elemental Mercury in the Ambient Atmosphere

    DEFF Research Database (Denmark)

    Ariya, Parisa A.; Skov, Henrik; Grage, Mette M L

    2008-01-01

    Understanding the kinetics and mechanisms associated with the atmospheric chemistry of mercury is of great importance to protecting the environment. This review will focus on theoretical calculations to advance understanding of gas phase oxidation of gaseous elemental mercury (GEM) by halogen spe...

  3. Global atmospheric particle formation from CERN CLOUD measurements

    CERN Document Server

    Dunne, E M; Kurten, A; Almeida, J; Duplissy, J; Williamson, C; Ortega, I K; Pringle, K J; Adamov, A; Baltensperger, U; Barmet, P; Benduhn, F; Bianchi, F; Breitenlechner, M; Clarke, A; Curtius, J; Dommen, J; Donahue, N M; Ehrhart, S; Flagan, R C; Franchin, A; Guida, R; Hakala, J; Hansel, A; Heinritzi, M; Jokinen, T; Kangasluoma, J; Kirkby, J; Kulmala, M; Kupc, A; Lawler, M J; Lehtipalo, K; Makhmutov, V; Mann, G; Mathot, S; Merikanto, J; Miettinen, P; Nenes, A; Onnela, A; Rap, A; Reddington, C L S; Riccobono, F; Richards, N A D; Rissanen, M P; Rondo, L; Sarnela, N; Schobesberger, S; Sengupta, K; Simon, M; Sipila, M; Smith, J N; Stozkhov, Y; Tome, A; Trostl, J; Wagner, P E; Wimmer, D; Winkler, P M; Worsnop, D R; Carslaw, K S

    2016-01-01

    Fundamental questions remain about the origin of newly formed atmospheric aerosol particles because data from laboratory measurements have been insufficient to build global models. In contrast, gas-phase chemistry models have been based on laboratory kinetics measurements for decades. Here we build a global model of aerosol formation using extensive laboratory-measured nucleation rates involving sulfuric acid, ammonia, ions and organic compounds. The simulations and a comparison with atmospheric observations show that nearly all nucleation throughout the present-day atmosphere involves ammonia or biogenic organic compounds in addition to sulfuric acid. A significant fraction of nucleation involves ions, but the relatively weak dependence on ion concentrations indicates that for the processes studied variations in cosmic ray intensity do not significantly affect climate via nucleation in the present-day atmosphere.

  4. Alaska Steller sea lion pup serum chemistry and hematology values, 1998-2011

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — These data were used for an analysis of Steller sea lion pup health and condition by Lander et al. (2013). Serum chemistry and hematological values were measured by...

  5. How does Interactive Chemistry Influence the Representation of Stratosphere-Troposphere Coupling in a Climate Model?

    Science.gov (United States)

    Haase, S.; Matthes, K. B.

    2017-12-01

    Changes in stratospheric ozone can trigger tropospheric circulation changes. In the Southern hemisphere (SH), the observed shift of the Southern Annular Mode was attributed to the observed trend in lower stratospheric ozone. In the Northern Hemisphere (NH), a recent study showed that extremely low stratospheric ozone conditions during spring produce robust anomalies in the troposphere (zonal wind, temperature and precipitation). This could only be reproduced in a coupled chemistry climate model indicating that chemical-dynamical feedbacks are also important on the NH. To further investigate the importance of interactive chemistry for surface climate, we conducted a set of experiments using NCAR's Community Earth System Model (CESM1) with the Whole Atmosphere Community Climate Model (WACCM) as the atmosphere component. WACCM contains a fully interactive stratospheric chemistry module in its standard configuration. It also allows for an alternative configuration, referred to as SC-WACCM, in which the chemistry (O3, NO, O, O2, CO2 and chemical and shortwave heating rates) is specified as a 2D field in the radiation code. A comparison of the interactive vs. the specified chemistry version enables us to evaluate the relative importance of interactive chemistry by systematically inhibiting the feedbacks between chemistry and dynamics. To diminish the effect of temporal interpolation when prescribing ozone, we use daily resolved zonal mean ozone fields for the specified chemistry run. Here, we investigate the differences in stratosphere-troposphere coupling between the interactive and specified chemistry simulations for the mainly chemically driven SH as well as for the mainly dynamically driven NH. We will especially consider years that are characterized by extremely low stratospheric ozone on the one hand and by large dynamical disturbances, i.e. Sudden Stratospheric Warmings, on the other hand.

  6. Manual for the GAW Precipitation Chemistry Programme: Guidelines, Data Quality Objectives and Standard Operating Procedures

    Science.gov (United States)

    2004-11-01

    Prof. Dr. Hans-Walter Georgii, February 1982. 9. An Assessment of BAPMoN Data Currently Available on the Concentration of CO2 in the Atmosphere by...134). 35. Provisional Daily Atmospheric CO2 Concentrations as Measured at BAPMoN Sites for the Year 1983. December 1985 (WMO TD No. 77). 36...and Atmospheric Chemistry, Santiago , Chile , 9-15 January 1991 (WMO TD No. 633). 71. Report of the Consultation of Experts to Consider Desirable

  7. Laser experiments for chemistry and physics

    CERN Document Server

    Compton, Robert N

    2016-01-01

    Lasers are employed throughout science and technology, in fundamental research, the remote sensing of atmospheric gases or pollutants, communications, medical diagnostics and therapies, and the manufacturing of microelectronic devices. Understanding the principles of their operation, which underlie all of these areas, is essential for a modern scientific education. This text introduces the characteristics and operation of lasers through laboratory experiments designed for the undergraduate curricula in chemistry and physics. Introductory chapters describe the properties of light, the history of laser invention, the atomic, molecular, and optical principles behind how lasers work, and the kinds of lasers available today. Other chapters include the basic theory of spectroscopy and computational chemistry used to interpret laser experiments. Experiments range from simple in-class demonstrations to more elaborate configurations for advanced students. Each chapter has historical and theoretical background, as well...

  8. PREP-CHEM-SRC – 1.0: a preprocessor of trace gas and aerosol emission fields for regional and global atmospheric chemistry models

    Directory of Open Access Journals (Sweden)

    S. R. Freitas

    2011-05-01

    Full Text Available The preprocessor PREP-CHEM-SRC presented in the paper is a comprehensive tool aiming at preparing emission fields of trace gases and aerosols for use in atmospheric-chemistry transport models. The considered emissions are from the most recent databases of urban/industrial, biogenic, biomass burning, volcanic, biofuel use and burning from agricultural waste sources. For biomass burning, emissions can be also estimated directly from satellite fire detections using a fire emission model included in the tool. The preprocessor provides emission fields interpolated onto the transport model grid. Several map projections can be chosen. The inclusion of these emissions in transport models is also presented. The preprocessor is coded using Fortran90 and C and is driven by a namelist allowing the user to choose the type of emissions and the databases.

  9. Chemistry in Titan

    Science.gov (United States)

    Plessis, S.; Carrasco, N.; Pernot, P.

    2009-04-01

    , D.A. Gell, H.B. Niemann, I.C.F. Müller-Wodarg, N. Borggren, G.G. Fletcher, E.L. Patrick, E. Raaen, and B.A. Magee. Analysis of Titan's neutral upper atmosphere from Cassini ion neutral mass spectrometer measurements. Icarus, In Press, Accepted Manuscript:-, 2008. [2] V. Vuitton, R. V. Yelle, and M.J. McEwan. Ion chemistry and N-containing molecules in Titan's upper atmosphere. Icarus, 191:722-742, 2007. [3] V. De La Haye, J.H. Waite Jr., T.E. Cravens, I.P. Robertson, and S. Lebonnois. Coupled ion and neutral rotating model of Titan's upper atmosphere. Icarus, 197(1):110 - 136, 2008. [4] J. B. A. Mitchell, C. Rebrion-Rowe, J. L. Le Garrec, G. Angelova, H. Bluhme, K. Seiersen, and L. H. Andersen. Branching ratios for the dissociative recombination of hydrocarbon ions. I: The cases of C4H9+ and C4H5+. International Journal of Mass Spectrometry, 227(2):273-279, June 2003. [5] N. Carrasco and P. Pernot. Modeling of branching ratio uncertainty in chemical networks by Dirichlet distributions. Journal of Physical Chemistry A, 11(18):3507-3512, 2007.

  10. Observable Signatures of Wind-driven Chemistry with a Fully Consistent Three-dimensional Radiative Hydrodynamics Model of HD 209458b

    Science.gov (United States)

    Drummond, B.; Mayne, N. J.; Manners, J.; Carter, A. L.; Boutle, I. A.; Baraffe, I.; Hébrard, É.; Tremblin, P.; Sing, D. K.; Amundsen, D. S.; Acreman, D.

    2018-03-01

    We present a study of the effect of wind-driven advection on the chemical composition of hot-Jupiter atmospheres using a fully consistent 3D hydrodynamics, chemistry, and radiative transfer code, the Met Office Unified Model (UM). Chemical modeling of exoplanet atmospheres has primarily been restricted to 1D models that cannot account for 3D dynamical processes. In this work, we couple a chemical relaxation scheme to the UM to account for the chemical interconversion of methane and carbon monoxide. This is done consistently with the radiative transfer meaning that departures from chemical equilibrium are included in the heating rates (and emission) and hence complete the feedback between the dynamics, thermal structure, and chemical composition. In this Letter, we simulate the well studied atmosphere of HD 209458b. We find that the combined effect of horizontal and vertical advection leads to an increase in the methane abundance by several orders of magnitude, which is directly opposite to the trend found in previous works. Our results demonstrate the need to include 3D effects when considering the chemistry of hot-Jupiter atmospheres. We calculate transmission and emission spectra, as well as the emission phase curve, from our simulations. We conclude that gas-phase nonequilibrium chemistry is unlikely to explain the model–observation discrepancy in the 4.5 μm Spitzer/IRAC channel. However, we highlight other spectral regions, observable with the James Webb Space Telescope, where signatures of wind-driven chemistry are more prominant.

  11. A STUDY ON LEGIONELLA PNEUMOPHILA, WATER CHEMISTRY, AND ATMOSPHERIC CONDITIONS IN COOLING TOWERS AT THE SAVANNAH RIVER SITE

    Energy Technology Data Exchange (ETDEWEB)

    Smith, C.; Brigmon, R.

    2009-10-20

    elevated Legionella concentrations when the dew point temperature was high--a summertime occurrence. However, analysis of the three years of Legionella monitoring data of the 14 different SRS Cooling Towers demonstrated that elevated concentrations are observed at all temperatures and seasons. The objective of this study is to evaluate the ecology of L. pneumophila including serogroups and population densities, chemical, and atmospheric data, on cooling towers at SRS to determine whether relationships exist among water chemistry, and atmospheric conditions. The goal is to more fully understand the conditions which inhibit or encourage L. pneumophila growth and supply this data and associated recommendations to SRS Cooling Tower personnel for improved management of operation. Hopefully this information could then be used to help control L. pneumophila growth more effectively in SRS cooling tower water.

  12. Atmospheric Ozone and Methane in a Changing Climate

    Directory of Open Access Journals (Sweden)

    Ivar S. A. Isaksen

    2014-07-01

    Full Text Available Ozone and methane are chemically active climate-forcing agents affected by climate–chemistry interactions in the atmosphere. Key chemical reactions and processes affecting ozone and methane are presented. It is shown that climate-chemistry interactions have a significant impact on the two compounds. Ozone, which is a secondary compound in the atmosphere, produced and broken down mainly in the troposphere and stratosphre through chemical reactions involving atomic oxygen (O, NOx compounds (NO, NO2, CO, hydrogen radicals (OH, HO2, volatile organic compounds (VOC and chlorine (Cl, ClO and bromine (Br, BrO. Ozone is broken down through changes in the atmospheric distribution of the afore mentioned compounds. Methane is a primary compound emitted from different sources (wetlands, rice production, livestock, mining, oil and gas production and landfills.Methane is broken down by the hydroxyl radical (OH. OH is significantly affected by methane emissions, defined by the feedback factor, currently estimated to be in the range 1.3 to 1.5, and increasing with increasing methane emission. Ozone and methane changes are affected by NOx emissions. While ozone in general increase with increases in NOx emission, methane is reduced, due to increases in OH. Several processes where current and future changes have implications for climate-chemistry interactions are identified. It is also shown that climatic changes through dynamic processes could have significant impact on the atmospheric chemical distribution of ozone and methane, as we can see through the impact of Quasi Biennial Oscillation (QBO. Modeling studies indicate that increases in ozone could be more pronounced toward the end of this century. Thawing permafrost could lead to important positive feedbacks in the climate system. Large amounts of organic material are stored in the upper layers of the permafrost in the yedoma deposits in Siberia, where 2 to 5% of the deposits could be organic material

  13. The potential impact of hydrogen energy use on the atmosphere

    Science.gov (United States)

    van Ruijven, B. J.; Lamarque, J. F.; van Vuuren, D. P.; Kram, T.; Eerens, H.

    2009-04-01

    Energy models show very different trajectories for future energy systems (partly as function of future climate policy). One possible option is a transition towards a hydrogen-based energy system. The potential impact of such hydrogen economy on atmospheric emissions is highly uncertain. On the one hand, application of hydrogen in clean fuel cells reduces emissions of local air pollutants, like SOx and NOx. On the other hand, emissions of hydrogen from system leakages are expected to change the atmospheric concentrations and behaviour (see also Price et al., 2007; Sanderson et al., 2003; Schultz et al., 2003; Tromp et al., 2003). The uncertainty arises from several sources: the expected use of hydrogen, the intensity of leakages and emissions, and the atmospheric chemical behaviour of hydrogen. Existing studies to the potential impacts of a hydrogen economy on the atmosphere mostly use hydrogen emission scenarios that are based on simple assumptions. This research combines two different modelling efforts to explore the range of impacts of hydrogen on atmospheric chemistry. First, the potential role of hydrogen in the global energy system and the related emissions of hydrogen and other air pollutants are derived from the global energy system simulation model TIMER (van Vuuren, 2007). A set of dedicated scenarios on hydrogen technology development explores the most pessimistic and optimistic cases for hydrogen deployment (van Ruijven et al., 2008; van Ruijven et al., 2007). These scenarios are combined with different assumptions on hydrogen emission factors. Second, the emissions from the TIMER model are linked to the NCAR atmospheric model (Lamarque et al., 2005; Lamarque et al., 2008), in order to determine the impacts on atmospheric chemistry. By combining an energy system model and an atmospheric model, we are able to consistently explore the boundaries of both hydrogen use, emissions and impacts on atmospheric chemistry. References: Lamarque, J.-F., Kiehl, J. T

  14. Development of a MELCOR Sodium Chemistry (NAC) Package - FY17 Progress.

    Energy Technology Data Exchange (ETDEWEB)

    Louie, David [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Humphries, Larry L. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2018-02-01

    This report describes the status of the development of MELCOR Sodium Chemistry (NAC) package. This development is based on the CONTAIN-LMR sodium physics and chemistry models to be implemented in MELCOR. In the past three years, the sodium equation of state as a working fluid from the nuclear fusion safety research and from the SIMMER code has been implemented into MELCOR. The chemistry models from the CONTAIN-LMR code, such as the spray and pool fire mode ls, have also been implemented into MELCOR. This report describes the implemented models and the issues encountered. Model descriptions and input descriptions are provided. Development testing of the spray and pool fire models is described, including the code-to-code comparison with CONTAIN-LMR. The report ends with an expected timeline for the remaining models to be implemented, such as the atmosphere chemistry, sodium-concrete interactions, and experimental validation tests .

  15. Improvements to the characterization of organic nitrogen chemistry and deposition in CMAQ

    Science.gov (United States)

    Excess atmospheric nitrogen deposition can cause significant harmful effects to ecosystems. Organic nitrogen deposition can be an important contributor to the total nitrogen budget, contributing 10-30%, however there are large uncertainties in the chemistry and deposition of thes...

  16. Meso-scale modeling of air pollution transport/chemistry/deposition and its application

    International Nuclear Information System (INIS)

    Kitada, Toshihiro

    2007-01-01

    Transport/chemistry/deposition model for atmospheric trace chemical species is now regarded as an important tool for an understanding of the effects of various human activities, such as fuel combustion and deforestation, on human health, eco-system, and climate and for planning of appropriate control of emission sources. Several 'comprehensive' models have been proposed such as RADM (Chang, et al., 1987), STEM-II (Carmichael, et al., 1986), and CMAQ (Community Multi-scale Air Quality model, e.g., EPA website, 2003); the 'comprehensive' models include not only gas/aerosol phase chemistry but also aqueous phase chemistry in cloud/rain water in addition to the processes of advection, diffusion, wet deposition (mass transfer between aqueous and gas/aerosol phases), and dry deposition. The target of the development of the 'comprehensive' model will be that the model can correctly reproduce mass balance of various chemical species in the atmosphere with keeping adequate accuracy for calculated concentration distributions of chemical species. For the purpose, one of the important problems is a reliable wet deposition modeling, and here, we introduce two types of methods of 'cloud-resolving' and 'non-cloud-resolving' modeling for the wet deposition of pollutants. (author)

  17. Simulation of the vibrational chemistry and the infrared signature induced by a Sprite streamer in the mesosphere

    Science.gov (United States)

    Romand, F.; Payan, S.; Croize, L.

    2017-12-01

    Since their first observation in 1989, effect of TLEs on the atmospheric composition has become an open and important question. The lack of suitable experimental data is a shortcoming that hampers our understanding of the physics and chemistry induced by these effects. HALESIS (High-Altitude Luminous Events Studied by Infrared Spectro-imagery) is a future experiment dedicated to the measurement of the atmospheric perturbation induced by a TLE in the minutes following its occurrence, from a stratospheric balloon flying at an altitude of 25 km to 40 km. This work aims to quantify the local chemical impact of sprites in the stratosphere and mesosphere. In this paper, we will present the development of a tool which simulates (i) the impact of a sprite on the vibrational chemistry, (ii) the resulting infrared signature and (iii) the propagation of this signature through the atmosphere to an observer. First the Non Local Thermodynamic Equilibrium populations of a background atmosphere were computed using SAMM2 code. The initial thermodynamic and chemical description of atmosphere comes from the Whole Atmosphere community Climate Model (WACCM). Then a perturbation was applied to simulate a sprite. Chemistry due to TLEs was computed using Gordillo-Vazquez kinetic model. Rate coefficients that depend on the electron energy distribution function were calculated from collision cross-section data by solving the electron Boltzmann equation (BE). Time evolutions of the species densities and of vibrational populations in the non-thermal plasma consecutive to sprite discharge were simulated using the computer code ZDPlasKin (S. Pancheshn et al.). Finally, the resulting infrared signatures were propagated from the disturbed area through the atmosphere to an instrument placed in a limb line of sight using a line by line radiative transfer model. We will conclude that sprite could produce a significant infrared signature that last a few tens of seconds after the visible flash.

  18. Applications of high power microwaves to atmospheric modification and measurement

    International Nuclear Information System (INIS)

    Benford, J.

    1993-01-01

    The current state of proposals to use high power microwaves in the atmosphere is reviewed. HPM has been proposed to aid in the conservation of stratospheric ozone by partial breakdown, facilitating chemistry to eliminate chlorine. Another proposal is over-the-horizon radar using a partial breakdown area in the ionosphere. A key to any such effort is rapid diagnosis of the state of the atmosphere before, during and after intervention. Technology requirements of these modification and measurement proposals are reviewed. The elements of an atmospheric modification program are identified and political, economic and ideological factors are discussed

  19. On the comparison of numerical methods for the integration of kinetic equations in atmospheric chemistry and transport models

    Science.gov (United States)

    Saylor, Rick D.; Ford, Gregory D.

    The integration of systems of ordinary differential equations (ODEs) that arise in atmospheric photochemistry is of significant concern to tropospheric and stratospheric chemistry modelers. As a consequence of the stiff nature of these ODE systems, their solution requires a large fraction of the total computational effort in three-dimensional chemical model simulations. Several integration techniques have been proposed and utilized over the years in an attempt to provide computationally efficient, yet accurate, solutions to chemical kinetics ODES. In this work, we present a comparison of some of these techniques and argue that valid comparisons of ODE solvers must take into account the trade-off between solution accuracy and computational efficiency. Misleading comparison results can be obtained by neglecting the fact that any ODE solution method can be made faster or slower by manipulation of the appropriate error tolerances or time steps. Comparisons among ODE solution techniques should therefore attempt to identify which technique can provide the most accurate solution with the least computational effort over the entire range of behavior of each technique. We present here a procedure by which ODE solver comparisons can achieve this goal. Using this methodology, we compare a variety of integration techniques, including methods proposed by Hesstvedt et al. (1978, Int. J. Chem. Kinet.10, 971-994), Gong and Cho (1993, Atmospheric Environment27A, 2147-2160), Young and Boris (1977, J. phys. Chem.81, 2424-2427) and Hindmarsh (1983, In Scientific Computing (edited by Stepleman R. S. et al.), pp. 55-64. North-Holland, Amsterdam). We find that Gear-type solvers such as the Livermore Solver for ordinary differential equations (LSODE) and the sparse-matrix version of LSODE (LSODES) provide the most accurate solution of our test problems with the least computational effort.

  20. Global simulation of aromatic volatile organic compounds in the atmosphere

    Science.gov (United States)

    Cabrera Perez, David; Taraborrelli, Domenico; Pozzer, Andrea

    2015-04-01

    Among the large number of chemical compounds in the atmosphere, the organic group plays a key role in the tropospheric chemistry. Specifically the subgroup called aromatics is of great interest. Aromatics are the predominant trace gases in urban areas due to high emissions, primarily by vehicle exhausts and fuel evaporation. They are also present in areas where biofuel is used (i.e residential wood burning). Emissions of aromatic compounds are a substantial fraction of the total emissions of the volatile organic compounds (VOC). Impact of aromatics on human health is very important, as they do not only contribute to the ozone formation in the urban environment, but they are also highly toxic themselves, especially in the case of benzene which is able to trigger a range of illness under long exposure, and of nitro-phenols which cause detrimental for humans and vegetation even at very low concentrations. The aim of this work is to assess the atmospheric impacts of aromatic compounds on the global scale. The main goals are: lifetime and budget estimation, mixing ratios distribution, net effect on ozone production and OH loss for the most emitted aromatic compounds (benzene, toluene, xylenes, ethylbenzene, styrene and trimethylbenzenes). For this purpose, we use the numerical chemistry and climate simulation ECHAM/MESSy Atmospheric Chemistry (EMAC) model to build the global atmospheric budget for the most emitted and predominant aromatic compounds in the atmosphere. A set of emissions was prepared in order to include biomass burning, vegetation and anthropogenic sources of aromatics into the model. A chemical mechanism based on the Master Chemical Mechanism (MCM) was developed to describe the chemical oxidation in the gas phase of these aromatic compounds. MCM have been reduced in terms of number of chemical equation and species in order to make it affordable in a 3D model. Additionally other features have been added, for instance the production of HONO via ortho

  1. Venusian atmospheric equilibrium chemistry at the Pioneer Venus anomalous event altitude

    Science.gov (United States)

    Craig, Roger A.

    1994-01-01

    No convincing explanation for the anomalous behavior of the Atmospheric Structure Experiment temperature sensors at approximately 13 km altitude has been found. It occurred on all of the widely-spaced probes, in a similar fashion. A preliminary effort has been made to determine atmospheric chemical species which might be present at 13 km. The purpose of this effort is to initiate suggestions of possible chemical interactions and to explore the effects of the presence of possible metal reactants including condensation. Equilibrium fractions of chemical species were calculated at a variety of conditions. Baseline calculations were made for the altitudes near 13 km. For comparison calculations were also made at 13 km but with the introduction of plausible metal atoms.

  2. Changes in domestic heating fuel use in Greece: effects on atmospheric chemistry and radiation

    Science.gov (United States)

    Athanasopoulou, Eleni; Speyer, Orestis; Brunner, Dominik; Vogel, Heike; Vogel, Bernhard; Mihalopoulos, Nikolaos; Gerasopoulos, Evangelos

    2017-09-01

    For the past 8 years, Greece has been experiencing a major financial crisis which, among other side effects, has led to a shift in the fuel used for residential heating from fossil fuel towards biofuels, primarily wood. This study simulates the fate of the residential wood burning aerosol plume (RWB smog) and the implications on atmospheric chemistry and radiation, with the support of detailed aerosol characterization from measurements during the winter of 2013-2014 in Athens. The applied model system (TNO-MACC_II emissions and COSMO-ART model) and configuration used reproduces the measured frequent nighttime aerosol spikes (hourly PM10 > 75 µg m-3) and their chemical profile (carbonaceous components and ratios). Updated temporal and chemical RWB emission profiles, derived from measurements, were used, while the level of the model performance was tested for different heating demand (HD) conditions, resulting in better agreement with measurements for Tmin < 9 °C. Half of the aerosol mass over the Athens basin is organic in the submicron range, of which 80 % corresponds to RWB (average values during the smog period). Although organic particles are important light scatterers, the direct radiative cooling of the aerosol plume during wintertime is found low (monthly average forcing of -0.4 W m-2 at the surface), followed by a minor feedback to the concentration levels of aerosol species. The low radiative cooling of a period with such intense air pollution conditions is attributed to the timing of the smog plume appearance, both directly (longwave radiation increases during nighttime) and indirectly (the mild effect of the residual plume on solar radiation during the next day, due to removal and dispersion processes).

  3. Southwest Pacific deep water carbonate chemistry linked to high southern latitude climate and atmospheric CO2 during the Last Glacial Termination

    Science.gov (United States)

    Allen, Katherine A.; Sikes, Elisabeth L.; Hönisch, Bärbel; Elmore, Aurora C.; Guilderson, Thomas P.; Rosenthal, Yair; Anderson, Robert F.

    2015-08-01

    A greater amount of CO2 was stored in the deep sea during glacial periods, likely via greater efficiency of the biologic pump and increased uptake by a more alkaline ocean. Reconstructing past variations in seawater carbonate ion concentration (a major component of alkalinity) enables quantification of the relative roles of different oceanic CO2 storage mechanisms and also places constraints on the timing, magnitude, and location of subsequent deep ocean ventilation. Here, we present a record of deep-water inorganic carbon chemistry since the Last Glacial Maximum (LGM; ∼19-23 ka BP), derived from sediment core RR0503-83 raised from 1627 m in New Zealand's Bay of Plenty. The core site lies within the upper limit of southern-sourced Circumpolar Deep Water (CDW), just below the lower boundary of Antarctic Intermediate Water (AAIW). We reconstruct past changes in bottom water inorganic carbon chemistry from the trace element and stable isotopic composition of calcite shells of the epibenthic foraminifer Cibicidoides wuellerstorfi. A record of ΔCO32-(ΔCO32- = [COCO32-] in situ - [CO32-] saturation) derived from the foraminiferal boron to calcium ratio (B/Ca) provides evidence for greater ice-age storage of respired CO2 and reveals abrupt deglacial shifts in [CO32-] in situ of up to 30 μmol/kg (5 times larger than the difference between average LGM and Holocene values). The rapidity of these changes suggests the influence of changing water mass structure and atmospheric circulation in addition to a decrease in CO2 content of interior waters.

  4. Geochemistry of the Nsuta Mn deposit in Ghana: Implications for the Paleoproterozoic atmosphere and ocean chemistry

    Science.gov (United States)

    Goto, K. T.; Ito, T.; Suzuki, K.; Kashiwabara, T.; Takaya, Y.; Shimoda, G.; Nozaki, T.; Kiyokawa, S.; Tetteh, G. M.; Nyame, F. K.

    2013-12-01

    Oxygenation of the atmosphere and oceans has influenced the evolution of ocean chemistry and diversification of early life. A number of large manganese (Mn) deposits are distributed in the Paleoproterozoic sedimentary successions that were formed during the great oxidation event (GOE) around 2.4-2.2 Ga (Meynard, 2010). Due to the high redox potential of Mn, occurrences of Mn deposits have been regarded as important evidence for a highly oxidized environment during the Paleoproterozoic (Kirschvink et al., 2000). Furthermore, because Mn oxides strongly adsorb various elements, including bioessential elements such as Mo, formation of large Mn deposits may have affected the seawater chemical composition and ecology during the Paleoproterozoic. However, the genesis of each Mn deposit is poorly constrained, and the relationships among the formation of Mn deposits, the evolution of atmospheric and ocean chemistry, and the diversification of early life are still ambiguous. In this study, we report the Re-Os isotope compositions, rare earth element (REE) compositions, and abundance of manganophile elements in the Mn carbonate ore and host sedimentary rock samples collected from the Nsuta Mn deposit of the Birimian Supergroup, Ghana. The Nsuta deposit is one of the largest Paleoproterozoic Mn deposits, although its genesis remains controversial (Melcher et al., 1995; Mucke et al., 1999). The composite Re-Os isochron age (2149 × 130 Ma) of the Mn carbonate and sedimentary rock samples was consistent with the depositional age of the sedimentary rocks (~2.2 Ga) presumed from the U-Pb zircon age of volcanic rocks (Hirdes and Davis, 1998), suggesting that the timing of Mn ore deposition was almost equivalent to the host rock sedimentation. The PAAS-normalized REE pattern showed a positive Eu anomaly in all samples and a positive Ce anomaly only in the Mn carbonate ore. These REE patterns indicate the possible contribution of Eu-enriched fluids derived from hydrothermal activity

  5. The chemistry of the global atmosphere; International Symposium of the Commission for Atmospheric Chemistry and Global Pollution of IAMAP, 7th, Chamrousse, France, Sept. 5-11, 1990, Selected Papers

    Science.gov (United States)

    Buat-Menard, P. (Editor); Delmas, R. J. (Editor)

    1992-01-01

    Topics presented include the adsorption and reaction of trichlorofluoromethane on various particles, equilibria of the marine multiphase ammonia system, a novel ozone sensor for direct eddy flux measurements, and characterization of the carbonate content of atmospheric aerosols. Also presented are variations in heavy metals concentrations in Antarctic snows, sources of continental dust over Antarctica during the last glacial cycle, an inventory of anthropogenic emissions and air pollution in the USSR, and atmospheric nuclei in the remote free-troposphere.

  6. Atmospheric science and power production

    Energy Technology Data Exchange (ETDEWEB)

    Randerson, D. (ed.)

    1984-07-01

    This is the third in a series of scientific publications sponsored by the US Atomic Energy Commission and the two later organizations, the US Energy Research and Development Adminstration, and the US Department of Energy. The first book, Meteorology and Atomic Energy, was published in 1955; the second, in 1968. The present volume is designed to update and to expand upon many of the important concepts presented previously. However, the present edition draws heavily on recent contributions made by atmospheric science to the analysis of air quality and on results originating from research conducted and completed in the 1970s. Special emphasis is placed on how atmospheric science can contribute to solving problems relating to the fate of combustion products released into the atmosphere. The framework of this book is built around the concept of air-quality modeling. Fundamentals are addressed first to equip the reader with basic background information and to focus on available meteorological instrumentation and to emphasize the importance of data management procedures. Atmospheric physics and field experiments are described in detail to provide an overview of atmospheric boundary layer processes, of how air flows around obstacles, and of the mechanism of plume rise. Atmospheric chemistry and removal processes are also detailed to provide fundamental knowledge on how gases and particulate matter can be transformed while in the atmosphere and how they can be removed from the atmosphere. The book closes with a review of how air-quality models are being applied to solve a wide variety of problems. Separate analytics have been prepared for each chapter.

  7. Manual for the GAW Precipitation Chemistry Programme: Guidelines, Data Quality Objectives and Standard Operating Procedures

    National Research Council Canada - National Science Library

    Allan, Mary A

    2004-01-01

    This is a manual for the Global Atmosphere Watch Precipitation Chemistry (GAW-PC) Programme. Where possible, it describes standard operating procedures and otherwise provides guidance on methods and procedures...

  8. Revised mineral dust emissions in the atmospheric chemistry-climate model EMAC (MESSy 2.52 DU_Astitha1 KKDU2017 patch)

    Science.gov (United States)

    Klingmüller, Klaus; Metzger, Swen; Abdelkader, Mohamed; Karydis, Vlassis A.; Stenchikov, Georgiy L.; Pozzer, Andrea; Lelieveld, Jos

    2018-03-01

    To improve the aeolian dust budget calculations with the global ECHAM/MESSy atmospheric chemistry-climate model (EMAC), which combines the Modular Earth Submodel System (MESSy) with the ECMWF/Hamburg (ECHAM) climate model developed at the Max Planck Institute for Meteorology in Hamburg based on a weather prediction model of the European Centre for Medium-Range Weather Forecasts (ECMWF), we have implemented new input data and updates of the emission scheme.The data set comprises land cover classification, vegetation, clay fraction and topography. It is based on up-to-date observations, which are crucial to account for the rapid changes of deserts and semi-arid regions in recent decades. The new Moderate Resolution Imaging Spectroradiometer (MODIS)-based land cover and vegetation data are time dependent, and the effect of long-term trends and variability of the relevant parameters is therefore considered by the emission scheme. All input data have a spatial resolution of at least 0.1° compared to 1° in the previous version, equipping the model for high-resolution simulations.We validate the updates by comparing the aerosol optical depth (AOD) at 550 nm wavelength from a 1-year simulation at T106 (about 1.1°) resolution with Aerosol Robotic Network (AERONET) and MODIS observations, the 10 µm dust AOD (DAOD) with Infrared Atmospheric Sounding Interferometer (IASI) retrievals, and dust concentration and deposition results with observations from the Aerosol Comparisons between Observations and Models (AeroCom) dust benchmark data set. The update significantly improves agreement with the observations and is therefore recommended to be used in future simulations.

  9. Quantification of air plasma chemistry for surface disinfection

    International Nuclear Information System (INIS)

    Pavlovich, Matthew J; Clark, Douglas S; Graves, David B

    2014-01-01

    Atmospheric-pressure air plasmas, created by a variety of discharges, are promising sources of reactive species for the emerging field of plasma biotechnology because of their convenience and ability to operate at ambient conditions. One biological application of ambient-air plasma is microbial disinfection, and the ability of air plasmas to decontaminate both solid surfaces and liquid volumes has been thoroughly established in the literature. However, the mechanism of disinfection and which reactive species most strongly correlate with antimicrobial effects are still not well understood. We describe quantitative gas-phase measurements of plasma chemistry via infrared spectroscopy in confined volumes, focusing on air plasma generated via surface micro-discharge (SMD). Previously, it has been shown that gaseous chemistry is highly sensitive to operating conditions, and the measurements we describe here extend those findings. We quantify the gaseous concentrations of ozone (O 3 ) and nitrogen oxides (NO and NO 2 , or NO x ) throughout the established ‘regimes’ for SMD air plasma chemistry: the low-power, ozone-dominated mode; the high-power, nitrogen oxides-dominated mode; and the intermediate, unstable transition region. The results presented here are in good agreement with previously published experimental studies of aqueous chemistry and parameterized models of gaseous chemistry. The principal finding of the present study is the correlation of bacterial inactivation on dry surfaces with gaseous chemistry across these time and power regimes. Bacterial decontamination is most effective in ‘NO x mode’ and less effective in ‘ozone mode’, with the weakest antibacterial effects in the transition region. Our results underscore the dynamic nature of air plasma chemistry and the importance of careful chemical characterization of plasma devices intended for biological applications. (paper)

  10. Quantification of air plasma chemistry for surface disinfection

    Science.gov (United States)

    Pavlovich, Matthew J.; Clark, Douglas S.; Graves, David B.

    2014-12-01

    Atmospheric-pressure air plasmas, created by a variety of discharges, are promising sources of reactive species for the emerging field of plasma biotechnology because of their convenience and ability to operate at ambient conditions. One biological application of ambient-air plasma is microbial disinfection, and the ability of air plasmas to decontaminate both solid surfaces and liquid volumes has been thoroughly established in the literature. However, the mechanism of disinfection and which reactive species most strongly correlate with antimicrobial effects are still not well understood. We describe quantitative gas-phase measurements of plasma chemistry via infrared spectroscopy in confined volumes, focusing on air plasma generated via surface micro-discharge (SMD). Previously, it has been shown that gaseous chemistry is highly sensitive to operating conditions, and the measurements we describe here extend those findings. We quantify the gaseous concentrations of ozone (O3) and nitrogen oxides (NO and NO2, or NOx) throughout the established ‘regimes’ for SMD air plasma chemistry: the low-power, ozone-dominated mode; the high-power, nitrogen oxides-dominated mode; and the intermediate, unstable transition region. The results presented here are in good agreement with previously published experimental studies of aqueous chemistry and parameterized models of gaseous chemistry. The principal finding of the present study is the correlation of bacterial inactivation on dry surfaces with gaseous chemistry across these time and power regimes. Bacterial decontamination is most effective in ‘NOx mode’ and less effective in ‘ozone mode’, with the weakest antibacterial effects in the transition region. Our results underscore the dynamic nature of air plasma chemistry and the importance of careful chemical characterization of plasma devices intended for biological applications.

  11. Integrating chemistry into 3D climate models: Detailed kinetics in the troposphere and stratosphere of a global climate model

    Energy Technology Data Exchange (ETDEWEB)

    Kao, C.Y.J.; Elliott, S. [Los Alamos National Lab., NM (United States). Earth and Environmental Sciences Div.; Turco, R.P.; Zhao, X. [Univ. of California, Los Angeles, CA (United States)

    1997-11-01

    This is the final report of a three-year, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). The motivation for the project is to create the first complete, three-dimensional climate model that enfolds atmospheric photochemistry. The LANL chemical global climate model (GCM) not only distributes the trace greenhouse gases and modifies their concentrations within the detailed photochemical web, but also permits them to influence the radiation field and so force their own transport. Both atmospheric chemistry and fluid dynamics are nonlinear and zonally asymmetric phenomena. They can only be adequately modeled in three dimensions on the global grid. The kinetics-augmented GCM is the only program within the atmospheric community capable of investigating interaction involving chemistry and transport. The authors have conducted case studies of timely three-dimensional chemistry issues. Examples include ozone production from biomass burning plumes, kinetic feedbacks in zonally asymmetric transport phenomena with month- to year-long time scales, and volcano sulfate aerosols with respect to their potential effects on tropospheric ozone depletion.

  12. Online coupled regional meteorology chemistry models in Europe : Current status and prospects

    NARCIS (Netherlands)

    Baklanov, A.; Schlünzen, K.; Suppan, P.; Baldasano, J.; Brunner, D.; Aksoyoglu, S.; Carmichael, G.; Douros, J.; Flemming, J.; Forkel, R.; Galmarini, S.; Gauss, M.; Grell, G.; Hirtl, M.; Joffre, S.; Jorba, O.; Kaas, E.; Kaasik, M.; Kallos, G.; Kong, X.; Korsholm, U.; Kurganskiy, A.; Kushta, J.; Lohmann, U.; Mahura, A.; Manders-Groot, A.; Maurizi, A.; Moussiopoulos, N.; Rao, S.T.; Savage, N.; Seigneur, C.; Sokhi, R.S.; Solazzo, E.; Solomos, S.; Sørensen, B.; Tsegas, G.; Vignati, E.; Vogel, B.; Zhang, Y.

    2014-01-01

    Online coupled mesoscale meteorology atmospheric chemistry models have undergone a rapid evolution in recent years. Although mainly developed by the air quality modelling community, these models are also of interest for numerical weather prediction and regional climate modelling as they can consider

  13. Comparing the Atmospheric Losses at Io and Europa

    Science.gov (United States)

    Dols, V. J.; Bagenal, F.; Crary, F. J.; Cassidy, T.

    2017-12-01

    At Io and Europa, the interaction of the Jovian plasma with the moon atmosphere leads to a significant loss of atomic/molecular neutrals and ions to space. The processes that lead to atmospheric escape are diverse: atmospheric sputtering, molecular dissociation, molecular ion recombination, Jeans escape etc. Each process leads to neutrals escaping at different velocities (i.e. electron impact dissociation leads to very slow atomic neutrals, sputtering might eject faster molecular neutrals). Some neutrals will be ejected out of the Jovian system; others will form extended neutral clouds along the orbit of the moons. These atomic/molecular extended neutral clouds are probably the main source of plasma for the Jovian magnetosphere. They are difficult to observe directly thus their composition and density are still poorly constrained. A future modeling of the formation of these extended clouds requires an estimate of their atmospheric sources. We estimate the atmospheric losses at Io and Europa for each loss process with a multi-species chemistry model, using a prescribed atmospheric distribution consistent with the observations. We compare the neutral losses at Io and Europa.

  14. Using WRF-Chem to investigate the impact of night time nitrate radical chemistry and N2O5 heterogeneous chemistry on the chemical composition of the UK troposphere.

    Science.gov (United States)

    Archer-Nicholls, S.; Lowe, D.; Utembe, S.; McFiggans, G.

    2012-04-01

    It is believed that NO3 is the primary oxidant at night time, significantly impacting ozone formation, rain acidification and the formation and transformation of aerosols, particularly through the formation of the ammonium nitrate particulate (Allan et. al., 2000). However, many of the basic chemical processes controlling the formation and removal of NO3, in particular, the N2O5 heterogeneous reactions, are often not represented in models, although general parameterisations have been developed (c.f. Bertram & Thornton, 2009). The ROle of Night time chemistry in controlling the Oxidising Capacity of the atmOsphere (RONOCO) campaign is a project being funded by NERC and being carried out by a collaboration of UK Universities. It aims to better understand the role of the NO3 radical on the chemistry of the night time atmosphere, its oxidation capacity and thus its overall effects on the composition of the troposphere. The Weather Research and Forecasting model with Chemistry (WRF-Chem) is a state of the art regional climate model with fully coupled online air quality and meteorological components allowing for better resolution of aerosol and gas-phase chemistry (Grell et. al., 2005). It has been extended to include the Common Representative Intermediates scheme (CRIv2-R5) (Watson et. al., 2008), a reduced chemical scheme designed to simulate the atmospheric degradation of 220 species of hydrocarbons and VOCs. The MOSAIC aerosol scheme (Zaveri et. al., 2008), has been extended to include a reduced complexity condensed organic phase consisting of 13 semi-volatile and 2 involatile species (Topping et. al., 2012), as well as the N2O5 heterogeneous reaction scheme of Bertram & Thornton (2009). We aim to use WRF-Chem to compare the oxidation capacity of nighttime NO3 chemistry with that of daytime OH chemistry. The model was run using two nested grids: a 15km resolution domain over western Europe, containing a 5km resolution domain over the UK. The RONOCO campaign consisted

  15. Soil-atmosphere trace gas exchange in semiarid and arid zones.

    Science.gov (United States)

    Galbally, Ian E; Kirstine, Wayne V; Meyer, C P Mick; Wang, Ying Ping

    2008-01-01

    A review is presented on trace gas exchange of CH4, CO, N2O, and NOx arising from agriculture and natural sources in the world's semiarid and arid zones due to soil processes. These gases are important contributors to the radiative forcing and the chemistry of the atmosphere. Quantitative information is summarized from the available studies. Between 5 and 40% of the global soil-atmosphere exchange for these gases (CH4, CO, N2O, and NOx) may occur in semiarid and arid zones, but for each of these gases there are fewer than a dozen studies to support the individual estimates, and these are from a limited number of locations. Significant differences in the biophysical and chemical processes controlling these trace gas exchanges are identified through the comparison of semiarid and arid zones with the moist temperate or wet/dry savanna land regions. Therefore, there is a poorly quantified understanding of the contribution of these regions to the global trace gas cycles and atmospheric chemistry. More importantly, there is a poor understanding of the feedback between these exchanges, global change, and regional land use and air pollution issues. A set of research issues is presented.

  16. Atmospheric chemistry of CH3CHF2 (HFC-152a)

    DEFF Research Database (Denmark)

    Taketani, Fumikazu; Nakayama, Tomoki; Takahashi, Kenshi

    2005-01-01

    Smog chamber/Fourier transform infrared (FTIR) and laser-induced fluorescence (LIF) spectroscopic techniques were used to study the atmospheric degradation of CH3CHF2. The kinetics and products of the Cl(2P(3/2)) (denoted Cl) atom- and the OH radical-initiated oxidation of CH3CHF2 in 700 Torr of ...

  17. Microbiology and atmospheric processes: research challenges concerning the impact of airborne micro-organisms on the atmosphere and climate

    Directory of Open Access Journals (Sweden)

    C. E. Morris

    2011-01-01

    Full Text Available For the past 200 years, the field of aerobiology has explored the abundance, diversity, survival and transport of micro-organisms in the atmosphere. Micro-organisms have been explored as passive and severely stressed riders of atmospheric transport systems. Recently, an interest in the active roles of these micro-organisms has emerged along with proposals that the atmosphere is a global biome for microbial metabolic activity and perhaps even multiplication. As part of a series of papers on the sources, distribution and roles in atmospheric processes of biological particles in the atmosphere, here we describe the pertinence of questions relating to the potential roles that air-borne micro-organisms might play in meteorological phenomena. For the upcoming era of research on the role of air-borne micro-organisms in meteorological phenomena, one important challenge is to go beyond descriptions of abundance of micro-organisms in the atmosphere toward an understanding of their dynamics in terms of both biological and physico-chemical properties and of the relevant transport processes at different scales. Another challenge is to develop this understanding under contexts pertinent to their potential role in processes related to atmospheric chemistry, the formation of clouds, precipitation and radiative forcing. This will require truly interdisciplinary approaches involving collaborators from the biological and physical sciences, from disciplines as disparate as agronomy, microbial genetics and atmosphere physics, for example.

  18. Microbiology and atmospheric processes: research challenges concerning the impact of airborne micro-organisms on the atmosphere and climate

    Science.gov (United States)

    Morris, C. E.; Sands, D. C.; Bardin, M.; Jaenicke, R.; Vogel, B.; Leyronas, C.; Ariya, P. A.; Psenner, R.

    2011-01-01

    For the past 200 years, the field of aerobiology has explored the abundance, diversity, survival and transport of micro-organisms in the atmosphere. Micro-organisms have been explored as passive and severely stressed riders of atmospheric transport systems. Recently, an interest in the active roles of these micro-organisms has emerged along with proposals that the atmosphere is a global biome for microbial metabolic activity and perhaps even multiplication. As part of a series of papers on the sources, distribution and roles in atmospheric processes of biological particles in the atmosphere, here we describe the pertinence of questions relating to the potential roles that air-borne micro-organisms might play in meteorological phenomena. For the upcoming era of research on the role of air-borne micro-organisms in meteorological phenomena, one important challenge is to go beyond descriptions of abundance of micro-organisms in the atmosphere toward an understanding of their dynamics in terms of both biological and physico-chemical properties and of the relevant transport processes at different scales. Another challenge is to develop this understanding under contexts pertinent to their potential role in processes related to atmospheric chemistry, the formation of clouds, precipitation and radiative forcing. This will require truly interdisciplinary approaches involving collaborators from the biological and physical sciences, from disciplines as disparate as agronomy, microbial genetics and atmosphere physics, for example.

  19. Proceedings of impact of aircraft emissions upon the atmosphere. V. 1

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1998-12-31

    The study of the effect of aircraft on atmosphere is a new challenge that the scientific community has to face. This conference`s topics are various aspects of this challenge. The seven sessions of Volume 1 are: Present status and perspectives; Emission and traffic; Physics and chemistry of the aircraft wake; Natural and anthropogenic emissions - specific instrumentation; Global scale - chemistry; Global scale - climate. The 51 papers of Vol. 1. were indexed and abstracted individually for the Energy Database. (R.P.)

  20. Proceedings of impact of aircraft emissions upon the atmosphere. V. 1

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-12-31

    The study of the effect of aircraft on atmosphere is a new challenge that the scientific community has to face. This conference`s topics are various aspects of this challenge. The seven sessions of Volume 1 are: Present status and perspectives; Emission and traffic; Physics and chemistry of the aircraft wake; Natural and anthropogenic emissions - specific instrumentation; Global scale - chemistry; Global scale - climate. The 51 papers of Vol. 1. were indexed and abstracted individually for the Energy Database. (R.P.)

  1. Atmospheric plasma generates oxygen atoms as oxidizing species in aqueous solutions

    Czech Academy of Sciences Publication Activity Database

    Hefny, M.M.; Pattyn, C.; Lukeš, Petr; Benedikt, J.

    2016-01-01

    Roč. 49, č. 40 (2016), s. 404002 ISSN 0022-3727 R&D Projects: GA MŠk(CZ) LD14080 Grant - others:European Cooperation in Science and Technology(XE) COST TD1208 Institutional support: RVO:61389021 Keywords : atmospheric pressure plasma * transport of reactive species * reactive oxygen species * aqueous phase chemistry * plasma and liquids * phenol aqueous chemistry Subject RIV: BL - Plasma and Gas Discharge Physics Impact factor: 2.588, year: 2016 http://iopscience.iop.org/article/10.1088/0022-3727/49/40/404002

  2. Proceedings of impact of aircraft emissions upon the atmosphere. V. 2

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-12-31

    The study of the effect of aircraft on atmosphere is a new challenge that the scientific community has to face. This conference`s topics are various aspects of this challenge. The poster sessions of Volume 2 accompanying sessions 1 through 7 contain various aspects of aerosols, contrails, instruments, measurements, modelling, climatic impacts, projects, transport, atmospheric chemistry etc. The 49 papers of Vol.2. were indexed and abstracted individually for the Energy Database. (R.P.)

  3. Third Chemistry Conference on Recent Trends in Chemistry

    International Nuclear Information System (INIS)

    Saeed, M.M.; Wheed, S.

    2011-01-01

    The third chemistry conference 2011 on recent trends in chemistry was held from October 17-19, 2001 at Islamabad, Pakistan. More than 65 papers and oral presentation. The scope of the conference was wide open and provides and opportunity for participation of broad spectrum of chemists. This forum provided a platform for the dissemination of the latest research followed by discussion pertaining to new trends in chemistry. This con fence covered different aspects of subjects including analytical chemistry, environmental chemistry, polymer chemistry, industrial chemistry, biochemistry and nano chemistry etc. (A.B.)

  4. Compendium of NASA data base for the global tropospheric experiment's Transport and Atmospheric Chemistry Near the Equator-Atlantic (TRACE-A)

    Science.gov (United States)

    Gregory, Gerald L.; Scott, A. Donald, Jr.

    1995-01-01

    This compendium describes aircraft data that are available from NASA's Transport and Atmospheric Chemistry near the Equator - Atlantic (TRACE-A) conducted in September/October 1992. The broad objectives of TRACE-A were to study chemical processes and long-range transport associated with South American and African continental outflow during periods of widespread vegetation burning, and to understand the ozone enhancements observed from satellite data measured over the southern tropical Atlantic Ocean during the September/October time period. Flight experiments were conducted from Brazil, South Africa, Namibia, and the Ascension Island. This document provides a representation of aircraft data that are available from NASA Langley's Distributed Active Archive Center (DAAC). The data format of time series and altitude profile plots is not intended to support original analyses, but to assist the reader in identifying data that are of interest. This compendium is for only the NASA aircraft data. The DAAC data base includes numerous supporting data-meteorological products, results from surface studies, satellite observations, and data from sonde releases.

  5. Impacts of Cosmic Dust on Planetary Atmospheres and Surfaces

    Science.gov (United States)

    Plane, John M. C.; Flynn, George J.; Määttänen, Anni; Moores, John E.; Poppe, Andrew R.; Carrillo-Sanchez, Juan Diego; Listowski, Constantino

    2018-02-01

    Recent advances in interplanetary dust modelling provide much improved estimates of the fluxes of cosmic dust particles into planetary (and lunar) atmospheres throughout the solar system. Combining the dust particle size and velocity distributions with new chemical ablation models enables the injection rates of individual elements to be predicted as a function of location and time. This information is essential for understanding a variety of atmospheric impacts, including: the formation of layers of metal atoms and ions; meteoric smoke particles and ice cloud nucleation; perturbations to atmospheric gas-phase chemistry; and the effects of the surface deposition of micrometeorites and cosmic spherules. There is discussion of impacts on all the planets, as well as on Pluto, Triton and Titan.

  6. Constitutional dynamic chemistry: bridge from supramolecular chemistry to adaptive chemistry.

    Science.gov (United States)

    Lehn, Jean-Marie

    2012-01-01

    Supramolecular chemistry aims at implementing highly complex chemical systems from molecular components held together by non-covalent intermolecular forces and effecting molecular recognition, catalysis and transport processes. A further step consists in the investigation of chemical systems undergoing self-organization, i.e. systems capable of spontaneously generating well-defined functional supramolecular architectures by self-assembly from their components, thus behaving as programmed chemical systems. Supramolecular chemistry is intrinsically a dynamic chemistry in view of the lability of the interactions connecting the molecular components of a supramolecular entity and the resulting ability of supramolecular species to exchange their constituents. The same holds for molecular chemistry when the molecular entity contains covalent bonds that may form and break reversibility, so as to allow a continuous change in constitution by reorganization and exchange of building blocks. These features define a Constitutional Dynamic Chemistry (CDC) on both the molecular and supramolecular levels.CDC introduces a paradigm shift with respect to constitutionally static chemistry. The latter relies on design for the generation of a target entity, whereas CDC takes advantage of dynamic diversity to allow variation and selection. The implementation of selection in chemistry introduces a fundamental change in outlook. Whereas self-organization by design strives to achieve full control over the output molecular or supramolecular entity by explicit programming, self-organization with selection operates on dynamic constitutional diversity in response to either internal or external factors to achieve adaptation.The merging of the features: -information and programmability, -dynamics and reversibility, -constitution and structural diversity, points to the emergence of adaptive and evolutive chemistry, towards a chemistry of complex matter.

  7. The Atmospheric Chemistry Suite (ACS) of Three Spectrometers for the ExoMars 2016 Trace Gas Orbiter

    Science.gov (United States)

    Korablev, O.; Montmessin, F.; Trokhimovskiy, A.; Fedorova, A. A.; Shakun, A. V.; Grigoriev, A. V.; Moshkin, B. E.; Ignatiev, N. I.; Forget, F.; Lefèvre, F.; Anufreychik, K.; Dzuban, I.; Ivanov, Y. S.; Kalinnikov, Y. K.; Kozlova, T. O.; Kungurov, A.; Makarov, V.; Martynovich, F.; Maslov, I.; Merzlyakov, D.; Moiseev, P. P.; Nikolskiy, Y.; Patrakeev, A.; Patsaev, D.; Santos-Skripko, A.; Sazonov, O.; Semena, N.; Semenov, A.; Shashkin, V.; Sidorov, A.; Stepanov, A. V.; Stupin, I.; Timonin, D.; Titov, A. Y.; Viktorov, A.; Zharkov, A.; Altieri, F.; Arnold, G.; Belyaev, D. A.; Bertaux, J. L.; Betsis, D. S.; Duxbury, N.; Encrenaz, T.; Fouchet, T.; Gérard, J.-C.; Grassi, D.; Guerlet, S.; Hartogh, P.; Kasaba, Y.; Khatuntsev, I.; Krasnopolsky, V. A.; Kuzmin, R. O.; Lellouch, E.; Lopez-Valverde, M. A.; Luginin, M.; Määttänen, A.; Marcq, E.; Martin Torres, J.; Medvedev, A. S.; Millour, E.; Olsen, K. S.; Patel, M. R.; Quantin-Nataf, C.; Rodin, A. V.; Shematovich, V. I.; Thomas, I.; Thomas, N.; Vazquez, L.; Vincendon, M.; Wilquet, V.; Wilson, C. F.; Zasova, L. V.; Zelenyi, L. M.; Zorzano, M. P.

    2018-02-01

    The Atmospheric Chemistry Suite (ACS) package is an element of the Russian contribution to the ESA-Roscosmos ExoMars 2016 Trace Gas Orbiter (TGO) mission. ACS consists of three separate infrared spectrometers, sharing common mechanical, electrical, and thermal interfaces. This ensemble of spectrometers has been designed and developed in response to the Trace Gas Orbiter mission objectives that specifically address the requirement of high sensitivity instruments to enable the unambiguous detection of trace gases of potential geophysical or biological interest. For this reason, ACS embarks a set of instruments achieving simultaneously very high accuracy (ppt level), very high resolving power (>10,000) and large spectral coverage (0.7 to 17 μm—the visible to thermal infrared range). The near-infrared (NIR) channel is a versatile spectrometer covering the 0.7-1.6 μm spectral range with a resolving power of ˜20,000. NIR employs the combination of an echelle grating with an AOTF (Acousto-Optical Tunable Filter) as diffraction order selector. This channel will be mainly operated in solar occultation and nadir, and can also perform limb observations. The scientific goals of NIR are the measurements of water vapor, aerosols, and dayside or night side airglows. The mid-infrared (MIR) channel is a cross-dispersion echelle instrument dedicated to solar occultation measurements in the 2.2-4.4 μm range. MIR achieves a resolving power of >50,000. It has been designed to accomplish the most sensitive measurements ever of the trace gases present in the Martian atmosphere. The thermal-infrared channel (TIRVIM) is a 2-inch double pendulum Fourier-transform spectrometer encompassing the spectral range of 1.7-17 μm with apodized resolution varying from 0.2 to 1.3 cm-1. TIRVIM is primarily dedicated to profiling temperature from the surface up to ˜60 km and to monitor aerosol abundance in nadir. TIRVIM also has a limb and solar occultation capability. The technical concept of

  8. Atmospheric Nitrogen Deposition in the Western United States: Sources, Sinks and Changes over Time

    Science.gov (United States)

    Anderson, Sarah Marie

    Anthropogenic activities have greatly modified the way nitrogen moves through the atmosphere and terrestrial and aquatic environments. Excess reactive nitrogen generated through fossil fuel combustion, industrial fixation, and intensification of agriculture is not confined to anthropogenic systems but leaks into natural ecosystems with consequences including acidification, eutrophication, and biodiversity loss. A better understanding of where excess nitrogen originates and how that changes over time is crucial to identifying when, where, and to what degree environmental impacts occur. A major route into ecosystems for excess nitrogen is through atmospheric deposition. Excess nitrogen is emitted to the atmosphere where it can be transported great distances before being deposited back to the Earth's surface. Analyzing the composition of atmospheric nitrogen deposition and biological indicators that reflect deposition can provide insight into the emission sources as well as processes and atmospheric chemistry that occur during transport and what drives variation in these sources and processes. Chapter 1 provides a review and proof of concept of lichens to act as biological indicators and how their elemental and stable isotope composition can elucidate variation in amounts and emission sources of nitrogen over space and time. Information on amounts and emission sources of nitrogen deposition helps inform natural resources and land management decisions by helping to identify potentially impacted areas and causes of those impacts. Chapter 2 demonstrates that herbaria lichen specimens and field lichen samples reflect historical changes in atmospheric nitrogen deposition from urban and agricultural sources across the western United States. Nitrogen deposition increases throughout most of the 20 th century because of multiple types of emission sources until the implementation of the Clean Air Act Amendments of 1990 eventually decrease nitrogen deposition around the turn of

  9. Global atmospheric particle formation from CERN CLOUD measurements.

    Science.gov (United States)

    Dunne, Eimear M; Gordon, Hamish; Kürten, Andreas; Almeida, João; Duplissy, Jonathan; Williamson, Christina; Ortega, Ismael K; Pringle, Kirsty J; Adamov, Alexey; Baltensperger, Urs; Barmet, Peter; Benduhn, Francois; Bianchi, Federico; Breitenlechner, Martin; Clarke, Antony; Curtius, Joachim; Dommen, Josef; Donahue, Neil M; Ehrhart, Sebastian; Flagan, Richard C; Franchin, Alessandro; Guida, Roberto; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Jokinen, Tuija; Kangasluoma, Juha; Kirkby, Jasper; Kulmala, Markku; Kupc, Agnieszka; Lawler, Michael J; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mann, Graham; Mathot, Serge; Merikanto, Joonas; Miettinen, Pasi; Nenes, Athanasios; Onnela, Antti; Rap, Alexandru; Reddington, Carly L S; Riccobono, Francesco; Richards, Nigel A D; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Sengupta, Kamalika; Simon, Mario; Sipilä, Mikko; Smith, James N; Stozkhov, Yuri; Tomé, Antonio; Tröstl, Jasmin; Wagner, Paul E; Wimmer, Daniela; Winkler, Paul M; Worsnop, Douglas R; Carslaw, Kenneth S

    2016-12-02

    Fundamental questions remain about the origin of newly formed atmospheric aerosol particles because data from laboratory measurements have been insufficient to build global models. In contrast, gas-phase chemistry models have been based on laboratory kinetics measurements for decades. We built a global model of aerosol formation by using extensive laboratory measurements of rates of nucleation involving sulfuric acid, ammonia, ions, and organic compounds conducted in the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber. The simulations and a comparison with atmospheric observations show that nearly all nucleation throughout the present-day atmosphere involves ammonia or biogenic organic compounds, in addition to sulfuric acid. A considerable fraction of nucleation involves ions, but the relatively weak dependence on ion concentrations indicates that for the processes studied, variations in cosmic ray intensity do not appreciably affect climate through nucleation in the present-day atmosphere. Copyright © 2016, American Association for the Advancement of Science.

  10. The ozone hole and the 1995 Nobel prize in chemistry; Trou d`ozone et Prix Nobel 1995 de chimie

    Energy Technology Data Exchange (ETDEWEB)

    Berger, A. [Universite Catholique de Louvain (UCL), Louvain-la-Neuve (Belgium). Inst. d`Astronomie et de Geophysique G. Lemaitre

    1996-03-01

    To mark to award of the 1995 Nobel Prize in chemistry to three world renowned atmospheric chemists, this paper recalls the history of scientific progress in stratospheric ozone chemistry. Then it summarizes current knowledge of ozone-layer depletion and its impact on climate, vegetation and human health. (author). 21 refs., 12 figs.

  11. The Nitrous Oxide (N2O) Budget: Constraints from Atmospheric Observations and Models

    Science.gov (United States)

    Tian, H.; Thompson, R.; Canadell, J.; Winiwarter, W.; Tian, H.; Thompson, R.; Prather, M. J.

    2017-12-01

    The increasing global abundance of N2O poses a threat to human health and society over this coming century through both climate change and ozone depletion. In the sense of greenhouse gases, N2O ranks third behind CO2 and CH4. In the sense of ozone depletion, N2O stands alone. In order to identify the cause of these increases and hopefully reverse them, we need to have a thorough understanding of the sources and sinks (a.k.a. the budget) of N2O and how they can be altered. A bottom-up approach to the budget evaluates individual biogeochemical sources of N2O from the land and ocean; whereas, a top-down approach uses atmospheric observations of the variability, combined with modeling of the atmospheric chemistry and transport, to infer the magnitude of sources and sinks throughout the Earth system. This paper reviews top-down approaches using atmospheric data; a similar top-down approach can be taken with oceanic measurements of N2O, but is not covered here. Stratospheric chemistry is the predominant loss of N2O, and here we review how a merging of new measurements with stratospheric chemistry models is able to provide a constrained budget for the global N2O sink. N2O surface sources are transported and mixed throughout the atmosphere, providing positive anomalies in the N2O abundance (mole fraction of N2O with respect to dry air); while N2O-depleted air from the stratosphere provides negative anomalies. With accurate atmospheric transport models, including for stratosphere-troposphere exchange, the observed tropospheric variability in N2O is effectively a fingerprint of the location and magnitude of sources. This inverse modeling of sources is part of the top-down constraints and is reviewed here.

  12. Atmospheric chemistry and physics in the atmosphere of a developed megacity (London: an overview of the REPARTEE experiment and its conclusions

    Directory of Open Access Journals (Sweden)

    R. M. Harrison

    2012-03-01

    Full Text Available The REgents PARk and Tower Environmental Experiment (REPARTEE comprised two campaigns in London in October 2006 and October/November 2007. The experiment design involved measurements at a heavily trafficked roadside site, two urban background sites and an elevated site at 160–190 m above ground on the BT Tower, supplemented in the second campaign by Doppler lidar measurements of atmospheric vertical structure. A wide range of measurements of airborne particle physical metrics and chemical composition were made as well as measurements of a considerable range of gas phase species and the fluxes of both particulate and gas phase substances. Significant findings include (a demonstration of the evaporation of traffic-generated nanoparticles during both horizontal and vertical atmospheric transport; (b generation of a large base of information on the fluxes of nanoparticles, accumulation mode particles and specific chemical components of the aerosol and a range of gas phase species, as well as the elucidation of key processes and comparison with emissions inventories; (c quantification of vertical gradients in selected aerosol and trace gas species which has demonstrated the important role of regional transport in influencing concentrations of sulphate, nitrate and secondary organic compounds within the atmosphere of London; (d generation of new data on the atmospheric structure and turbulence above London, including the estimation of mixed layer depths; (e provision of new data on trace gas dispersion in the urban atmosphere through the release of purposeful tracers; (f the determination of spatial differences in aerosol particle size distributions and their interpretation in terms of sources and physico-chemical transformations; (g studies of the nocturnal oxidation of nitrogen oxides and of the diurnal behaviour of nitrate aerosol in the urban atmosphere, and (h new information on the chemical composition and source apportionment of particulate

  13. Radiation chemistry

    International Nuclear Information System (INIS)

    Rodgers, F.; Rodgers, M.A.

    1987-01-01

    The contents of this book include: Interaction of ionizing radiation with matter; Primary products in radiation chemistry; Theoretical aspects of radiation chemistry; Theories of the solvated electron; The radiation chemistry of gases; Radiation chemistry of colloidal aggregates; Radiation chemistry of the alkali halides; Radiation chemistry of polymers; Radiation chemistry of biopolymers; Radiation processing and sterilization; and Compound index

  14. Modeling of the chemistry in oxidation flow reactors with high initial NO

    Science.gov (United States)

    Peng, Zhe; Jimenez, Jose L.

    2017-10-01

    Oxidation flow reactors (OFRs) are increasingly employed in atmospheric chemistry research because of their high efficiency of OH radical production from low-pressure Hg lamp emissions at both 185 and 254 nm (OFR185) or 254 nm only (OFR254). OFRs have been thought to be limited to studying low-NO chemistry (in which peroxy radicals (RO2) react preferentially with HO2) because NO is very rapidly oxidized by the high concentrations of O3, HO2, and OH in OFRs. However, many groups are performing experiments by aging combustion exhaust with high NO levels or adding NO in the hopes of simulating high-NO chemistry (in which RO2 + NO dominates). This work systematically explores the chemistry in OFRs with high initial NO. Using box modeling, we investigate the interconversion of N-containing species and the uncertainties due to kinetic parameters. Simple initial injection of NO in OFR185 can result in more RO2 reacted with NO than with HO2 and minor non-tropospheric photolysis, but only under a very narrow set of conditions (high water mixing ratio, low UV intensity, low external OH reactivity (OHRext), and initial NO concentration (NOin) of tens to hundreds of ppb) that account for a very small fraction of the input parameter space. These conditions are generally far away from experimental conditions of published OFR studies with high initial NO. In particular, studies of aerosol formation from vehicle emissions in OFRs often used OHRext and NOin several orders of magnitude higher. Due to extremely high OHRext and NOin, some studies may have resulted in substantial non-tropospheric photolysis, strong delay to RO2 chemistry due to peroxynitrate formation, VOC reactions with NO3 dominating over those with OH, and faster reactions of OH-aromatic adducts with NO2 than those with O2, all of which are irrelevant to ambient VOC photooxidation chemistry. Some of the negative effects are the worst for alkene and aromatic precursors. To avoid undesired chemistry, vehicle emissions

  15. Effects of vegetation burning on the atmospheric chemistry of the Venezuelan savanna

    International Nuclear Information System (INIS)

    Sanhueza, E.

    1991-01-01

    Biomass burning in tropical savanna and rainforest regions is an important factor in the chemical composition of the atmosphere. On the global scale, burning of savanna grass procedures three to four times greater emission of trace gases than deforestation processes of tropical rainforest. As part of a comprehensive study of the Venezuelan savanna atmosphere, measurements of gases and particles, chemical composition of rain, and biogenic soil emission were made during burning and nonburning periods at several rural savanna sites. A review of the most significant findings is presented in this chapter, and their regional and global implications are discussed

  16. Magnetic susceptibility measurement of single iron/cobalt carbonyl microcrystal by atmospheric magnetophoresis

    Czech Academy of Sciences Publication Activity Database

    Suwa, M.; Oshino, Y.; Watarai, H.; Kasai, A.; Šubrt, Jan

    2008-01-01

    Roč. 9, č. 2 (2008), , 024215-1-024215-6 ISSN 1468-6996 Institutional research plan: CEZ:AV0Z40320502 Keywords : magnetophoresis under atmosphere Subject RIV: CA - Inorganic Chemistry Impact factor: 1.267, year: 2008

  17. Validation of the Atmospheric Chemistry Experiment (ACE version 2.2 temperature using ground-based and space-borne measurements

    Directory of Open Access Journals (Sweden)

    R. J. Sica

    2008-01-01

    Full Text Available An ensemble of space-borne and ground-based instruments has been used to evaluate the quality of the version 2.2 temperature retrievals from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS. The agreement of ACE-FTS temperatures with other sensors is typically better than 2 K in the stratosphere and upper troposphere and 5 K in the lower mesosphere. There is evidence of a systematic high bias (roughly 3–6 K in the ACE-FTS temperatures in the mesosphere, and a possible systematic low bias (roughly 2 K in ACE-FTS temperatures near 23 km. Some ACE-FTS temperature profiles exhibit unphysical oscillations, a problem fixed in preliminary comparisons with temperatures derived using the next version of the ACE-FTS retrieval software. Though these relatively large oscillations in temperature can be on the order of 10 K in the mesosphere, retrieved volume mixing ratio profiles typically vary by less than a percent or so. Statistical comparisons suggest these oscillations occur in about 10% of the retrieved profiles. Analysis from a set of coincident lidar measurements suggests that the random error in ACE-FTS version 2.2 temperatures has a lower limit of about ±2 K.

  18. Present State of Knowledge of the Upper Atmosphere 1996: An Assessment Report to Congress and the Environmental Protection Agency

    Science.gov (United States)

    Kurylo, M. J.; Kaye, J. A.; Decola, P. L.; Friedl, R. R.; Peterson, D. B.

    1997-01-01

    This document is issued in response to the Clean Air Act Amendment of 1990, Public Law 101-549, which mandates that the National Aeronautics and Space Administration (NASA) and other key agencies submit triennial report to congress and the Environmental Protection Agency. NASA is charged with the responsibility to report on the state of our knowledge of the Earth's upper atmosphere, particularly the Stratosphere. Part 1 of this report summarizes the objectives, status, and accomplishments of the research tasks supported under NASA's Upper Atmosphere Research Program and Atmospheric Chemistry Modeling and Analysis Program for the period of 1994-1996. Part 2 (this document) presents summaries of several scientific assessments, reviews, and summaries. These include the executive summaries of two scientific assessments: (Section B) 'Scientific Assessment of Ozone Depletion: 1994'; (Section C) 'l995 Scientific Assessment of the Atmospheric Effects of Stratospheric Aircraft); end of mission/series statements for three stratospherically-focused measurement campaigns: (Section D) 'ATLAS End-of-Series Statement'; (Section E) 'ASHOE/MAESA End-of-Mission Statement'; (Section F) 'TOTE/VOTE End-of-Mission Statement'; a summary of NASA's latest biennial review of fundamental photochemical processes important to atmospheric chemistry 'Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling'; and (Section H) the section 'Atmospheric Ozone Research" from the Mission to Planet Earth Science Research Plan, which describes NASA's current and future research activities related to both tropospheric and stratospheric chemistry.

  19. Occultations for probing atmosphere and climate

    CERN Document Server

    Foelsche, Ulrich; Steiner, Andrea

    2004-01-01

    Use of occultation methodology for observing the Earth's atmosphere and climate has become so broad as to comprise solar, lunar, stellar, navigation and satellite­ crosslink occultation methods. The atmospheric parameters obtained extend from the fundamental variables temperature, density, pressure, water vapor, and ozone via a multitude of trace gas species to particulate species such as aerosols and cloud liquid water. Ionospheric electron density is sensed as well. The methods all share the key properties of self-calibration, high accuracy and vertical resolution, global coverage, and (if using radio signals) all-weather capability. Occultation data are thus of high value in a wide range of fields including climate monitoring and research, atmospheric physics and chemistry, operational meteorology, and other fields such as space weather and planetary science. This wide area of variants and uses of the occultation method has led to a diversi­ fication of the occultation-related scientific community into a...

  20. Response of ocean acidification to a gradual increase and decrease of atmospheric CO2

    International Nuclear Information System (INIS)

    Cao, Long; Zhang, Han; Zheng, Meidi; Wang, Shuangjing

    2014-01-01

    We perform coupled climate–carbon cycle model simulations to examine changes in ocean acidity in response to idealized change of atmospheric CO 2 . Atmospheric CO 2 increases at a rate of 1% per year to four times its pre-industrial level of 280 ppm and then decreases at the same rate to the pre-industrial level. Our simulations show that changes in surface ocean chemistry largely follow changes in atmospheric CO 2 . However, changes in deep ocean chemistry in general lag behind the change in atmospheric CO 2 because of the long time scale associated with the penetration of excess CO 2 into the deep ocean. In our simulations with the effect of climate change, when atmospheric CO 2 reaches four times its pre-industrial level, global mean aragonite saturation horizon (ASH) shoals from the pre-industrial value of 1288 to 143 m. When atmospheric CO 2 returns from the peak value of 1120 ppm to pre-industrial level, ASH is 630 m, which is approximately the value of ASH when atmospheric CO 2 first increases to 719 ppm. At pre-industrial CO 2 9% deep-sea cold-water corals are surrounded by seawater that is undersaturated with aragonite. When atmospheric CO 2 reaches 1120 ppm, 73% cold-water coral locations are surrounded by seawater with aragonite undersaturation, and when atmospheric CO 2 returns to the pre-industrial level, 18% cold-water coral locations are surrounded by seawater with aragonite undersaturation. Our analysis indicates the difficulty for some marine ecosystems to recover to their natural chemical habitats even if atmospheric CO 2 content can be lowered in the future. (paper)

  1. Theoretical chemistry periodicities in chemistry and biology

    CERN Document Server

    Eyring, Henry

    1978-01-01

    Theoretical Chemistry: Periodicities in Chemistry and Biology, Volume 4 covers the aspects of theoretical chemistry. The book discusses the stably rotating patterns of reaction and diffusion; the chemistry of inorganic systems exhibiting nonmonotonic behavior; and population cycles. The text also describes the mathematical modeling of excitable media in neurobiology and chemistry; oscillating enzyme reactions; and oscillatory properties and excitability of the heart cell membrane. Selected topics from the theory of physico-chemical instabilities are also encompassed. Chemists, mechanical engin

  2. Phosphorus Chemistry in the Atmosphere of Jupiter: A Reassessment

    Science.gov (United States)

    Borunov, Sergei; Dorofeeva, Vera; Khodakovsky, Igor; Drossart, Pierre; Lellouch, Emmanuel; Encrenaz, Thérèse

    1995-02-01

    A new distribution of phosphorus compounds in the atmosphere of Jupiter is given, using revised values for the chemical constants. In contrast with previous works, it is shown that phosphine PH 3 remains the most abundant equilibrium gaseous compound even at the upper levels of Jupiter's troposphere. The observed PH 3 abundance is equal to the equilibrium value, at all temperatures above 535 K for solar P and O elemental abundances, and above 600 K for a reasonable range of P and O abundances. P 4O 6 does not take part in the phosphorus cycle on Jupiter.

  3. Temporal characteristics of atmospheric ammonia and nitrogen dioxide over China based on emission data, satellite observations and atmospheric transport modeling since 1980

    Science.gov (United States)

    Liu, Lei; Zhang, Xiuying; Xu, Wen; Liu, Xuejun; Li, Yi; Lu, Xuehe; Zhang, Yuehan; Zhang, Wuting

    2017-08-01

    China is experiencing intense air pollution caused in large part by anthropogenic emissions of reactive nitrogen (Nr). Atmospheric ammonia (NH3) and nitrogen dioxide (NO2) are the most important precursors for Nr compounds (including N2O5, HNO3, HONO and particulate NO3- and NH4+) in the atmosphere. Understanding the changes in NH3 and NO2 has important implications for the regulation of anthropogenic Nr emissions and is a requirement for assessing the consequence of environmental impacts. We conducted the temporal trend analysis of atmospheric NH3 and NO2 on a national scale since 1980 based on emission data (during 1980-2010), satellite observation (for NH3 since 2008 and for NO2 since 2005) and atmospheric chemistry transport modeling (during 2008-2015).Based on the emission data, during 1980-2010, significant continuous increasing trends in both NH3 and NOx were observed in REAS (Regional Emission inventory in Asia, for NH3 0.17 and for NOx 0.16 kg N ha-1 yr-2) and EDGAR (Emissions Database for Global Atmospheric Research, for NH3 0.24 and for NOx 0.17 kg N ha-1 yr-2) over China. Based on the satellite data and atmospheric chemistry transport model (CTM) MOZART-4 (Model for Ozone and Related chemical Tracers, version 4), the NO2 columns over China increased significantly from 2005 to 2011 and then decreased significantly from 2011 to 2015; the satellite-retrieved NH3 columns from 2008 to 2014 increased at a rate of 2.37 % yr-1. The decrease in NO2 columns since 2011 may result from more stringent strategies taken to control NOx emissions during the 12th Five Year Plan, while no control policy has focused on NH3 emissions. Our findings provided an overall insight into the temporal trends of both NO2 and NH3 since 1980 based on emission data, satellite observations and atmospheric transport modeling. These findings can provide a scientific background for policy makers that are attempting to control atmospheric pollution in China. Moreover, the multiple datasets

  4. Quantification of Atmospheric Formaldehyde by Near-Infrared Cavity Ring-Down Spectroscopy

    Science.gov (United States)

    Rella, C.; Hoffnagle, J.; Fleck, D.; Kim-Hak, D.

    2017-12-01

    Formaldehyde is an important species in atmospheric chemistry, especially in urban environments, where it is a decay product of methane and volatile hydrocarbons. It is also a toxic, carcinogenic compound that can contaminate ambient air from incomplete combustion, or outgassing of commercial products such as adhesives used to fabricate plywood or to affix indoor carpeting. Formaldehyde has a clearly resolved ro-vibrational absorption spectrum that is well-suited to optical analysis of formaldehyde concentration. We describe an instrument based on cavity ring-down spectroscopy for the quantitative analysis of formaldehyde concentration in ambient air. The instrument has a precision (1-sigma) of about 1 ppb at a measurement rate of 1 second, and provides measurements of less than 100 ppt with averaging. The instrument provides stable measurements (drift < 1 ppb) over long periods of time (days). The instrument has been ruggedized for mobile applications, and with a fast response time of a couple of seconds, it is suitable for ground-based vehicle deployments for fenceline monitoring of formaldehyde emissions. In addition, we report on ambient atmospheric measurements at a 10m urban tower, which demonstrate the suitability of the instrument for applications in atmospheric chemistry.

  5. Plasma chemistry in an atmospheric pressure Ar/NH3 dielectric barrier discharge

    DEFF Research Database (Denmark)

    Fateev, A.; Leipold, F.; Kusano, Y.

    2005-01-01

    An atmospheric pressure dielectric barrier discharge (DBD) in Ar/NH3 (0.1 - 10%) mixtures with a parallel plate electrode geometry was studied. The plasma was investigated by emission and absorption spectroscopy in the UV spectral range. Discharge current and voltage were measured as well. UV...... of an atmospheric pressure Ar/NH3 DBD are H-2, N-2 and N2H4. The hydrazine (N2H4) concentration in the plasma and in the exhaust gases at various ammonia concentrations and different discharge powers was measured. Thermal N2H4 decomposition into NH2 radicals may be used for NOx reduction processes....

  6. Improvements to the characterization of organic nitrogen chemistry and deposition in CMAQ (CMAS Presentation)

    Science.gov (United States)

    Excess atmospheric nitrogen deposition can cause significant harmful effects to ecosystems. Organic nitrogen deposition can be an important contributor to the total nitrogen budget, contributing 10-30%, however there are large uncertainties in the chemistry and deposition of thes...

  7. TRANSMISSION SPECTRA OF THREE-DIMENSIONAL HOT JUPITER MODEL ATMOSPHERES

    International Nuclear Information System (INIS)

    Fortney, J. J.; Shabram, M.; Showman, A. P.; Lian, Y.; Lewis, N. K.; Freedman, R. S.; Marley, M. S.

    2010-01-01

    We compute models of the transmission spectra of planets HD 209458b, HD 189733b, and generic hot Jupiters. We examine the effects of temperature, surface gravity, and metallicity for the generic planets as a guide to understanding transmission spectra in general. We find that carbon dioxide absorption at 4.4 and 15 μm is prominent at high metallicity, and is a clear metallicity indicator. For HD 209458b and HD 189733b, we compute spectra for both one-dimensional and three-dimensional model atmospheres and examine the differences between them. The differences are usually small, but can be large if atmospheric temperatures are near important chemical abundance boundaries. The calculations for the three-dimensional atmospheres, and their comparison with data, serve as constraints on these dynamical models that complement the secondary eclipse and light curve data sets. For HD 209458b, even if TiO and VO gases are abundant on the dayside, their abundances can be considerably reduced on the cooler planetary limb. However, given the predicted limb temperatures and TiO abundances, the model's optical opacity is too high. For HD 189733b we find a good match with some infrared data sets and constrain the altitude of a postulated haze layer. For this planet, substantial differences can exist between the transmission spectra of the leading and trailing hemispheres, which are an excellent probe of carbon chemistry. In thermochemical equilibrium, the cooler leading hemisphere is methane-dominated, and the hotter trailing hemisphere is CO-dominated, but these differences may be eliminated by non-equilibrium chemistry due to vertical mixing. It may be possible to constrain the carbon chemistry of this planet, and its spatial variation, with James Webb Space Telescope.

  8. Aerosolization and Atmospheric Transformation of Engineered Nanoparticles

    Science.gov (United States)

    Tiwari, Andrea J.

    While research on the environmental impacts of engineered nanoparticles (ENPs) is growing, the potential for them to be chemically transformed in the atmosphere has been largely ignored. The overall objective of this work was to assess the atmospheric transformation of carbonaceous nanoparticles (CNPs). The research focuses on C60 fullerene because it is an important member of the carbonaceous nanoparticle (CNP) family and is used in a wide variety of applications. The first specific objective was to review the potential of atmospheric transformations to alter the environmental impacts of CNPs. We described atmospheric processes that were likely to physically or chemically alter aerosolized CNPs and demonstrated their relevance to CNP behavior and toxicity in the aqueous and terrestrial environment. In order to investigate the transformations of CNP aerosols under controlled conditions, we developed an aerosolization technique that produces nano-scale aerosols without using solvents, which can alter the surface chemistry of the aerosols. We demonstrated the technique with carbonaceous (C60) and metal oxide (TiO2, CeO2) nanoparticle powders. All resulting aerosols exhibited unimodal size distributions and mode particle diameters below 100 nm. We used the new aerosolization technique to investigate the reaction between aerosolized C60 and atmospherically realistic levels of ozone (O3) in terms of reaction products, reaction rate, and oxidative stress potential. We identified C60O, C60O2, and C60O3 as products of the C60-O3 reaction. We demonstrated that the oxidative stress potential of C 60 may be enhanced by exposure to O3. We found the pseudo-first order reaction rate to be 9 x 10-6 to 2 x 10 -5 s-1, which is several orders of magnitude lower than the rate for several PAH species under comparable conditions. This research has demonstrated that a thorough understanding of atmospheric chemistry of ENPs is critical for accurate prediction of their environmental

  9. Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry.

    Science.gov (United States)

    Farmer, D K; Matsunaga, A; Docherty, K S; Surratt, J D; Seinfeld, J H; Ziemann, P J; Jimenez, J L

    2010-04-13

    Organonitrates (ON) are important products of gas-phase oxidation of volatile organic compounds in the troposphere; some models predict, and laboratory studies show, the formation of large, multifunctional ON with vapor pressures low enough to partition to the particle phase. Organosulfates (OS) have also been recently detected in secondary organic aerosol. Despite their potential importance, ON and OS remain a nearly unexplored aspect of atmospheric chemistry because few studies have quantified particulate ON or OS in ambient air. We report the response of a high-resolution time-of-flight aerosol mass spectrometer (AMS) to aerosol ON and OS standards and mixtures. We quantify the potentially substantial underestimation of organic aerosol O/C, commonly used as a metric for aging, and N/C. Most of the ON-nitrogen appears as NO(x)+ ions in the AMS, which are typically dominated by inorganic nitrate. Minor organonitrogen ions are observed although their identity and intensity vary between standards. We evaluate the potential for using NO(x)+ fragment ratios, organonitrogen ions, HNO(3)+ ions, the ammonium balance of the nominally inorganic ions, and comparison to ion-chromatography instruments to constrain the concentrations of ON for ambient datasets, and apply these techniques to a field study in Riverside, CA. OS manifests as separate organic and sulfate components in the AMS with minimal organosulfur fragments and little difference in fragmentation from inorganic sulfate. The low thermal stability of ON and OS likely causes similar detection difficulties for other aerosol mass spectrometers using vaporization and/or ionization techniques with similar or larger energy, which has likely led to an underappreciation of these species.

  10. Bacteria in atmospheric waters: Detection, characteristics and implications

    Science.gov (United States)

    Hu, Wei; Niu, Hongya; Murata, Kotaro; Wu, Zhijun; Hu, Min; Kojima, Tomoko; Zhang, Daizhou

    2018-04-01

    In this review paper, we synthesize the current knowledges about bacteria in atmospheric waters, e.g., cloud, fog, rain, and snow, most of which were obtained very recently. First, we briefly describe the importance of bacteria in atmospheric waters, i.e., the essentiality of studying bacteria in atmospheric waters in understanding aerosol-cloud-precipitation-climate interactions in the Earth system. Next, approaches to collect atmospheric water samples for the detection of bacteria and methods to identify the bacteria are summarized and compared. Then the available data on the abundance, viability and community composition of bacteria in atmospheric waters are summarized. The average bacterial concentration in cloud water was usually on the order 104-105 cells mL-1, while that in precipitation on the order 103-104 cells mL-1. Most of the bacteria were viable or metabolically active. Their community composition was highly diverse and differed at various sites. Factors potentially influencing the bacteria, e.g., air pollution levels and sources, meteorological conditions, seasonal effect, and physicochemical properties of atmospheric waters, are described. After that, the implications of bacteria present in atmospheric waters, including their effect on nucleation in clouds, atmospheric chemistry, ecosystems and public health, are briefly discussed. Finally, based on the current knowledges on bacteria in atmospheric waters, which in fact remains largely unknown, we give perspectives that should be paid attention to in future studies.

  11. Complex chemistry

    International Nuclear Information System (INIS)

    Kim, Bong Gon; Kim, Jae Sang; Kim, Jin Eun; Lee, Boo Yeon

    2006-06-01

    This book introduces complex chemistry with ten chapters, which include development of complex chemistry on history coordination theory and Warner's coordination theory and new development of complex chemistry, nomenclature on complex with conception and define, chemical formula on coordination compound, symbol of stereochemistry, stereo structure and isomerism, electron structure and bond theory on complex, structure of complex like NMR and XAFS, balance and reaction on solution, an organo-metallic chemistry, biology inorganic chemistry, material chemistry of complex, design of complex and calculation chemistry.

  12. The 13th Winter Conference on Medicinal and Bioorganic Chemistry.

    Science.gov (United States)

    Williams, Scott D

    2017-04-06

    The Medicinal and Bioorganic Chemistry Foundation (MBCF) hosted its 13 th biannual Winter Conference on Medicinal and Bioorganic Chemistry (WCMBC) this past January 22 nd -26 th in Steamboat Springs, Colorado (USA). The gathering this year kept true to the tradition of this conference series, with an impressive lineup of presenters from both academia and industry. With about 125 delegates, the conference took all the advantages of a mid-sized gathering: a sufficiently wide spectrum of scientists in attendance, yet an intimate atmosphere conducive to solid networking and frank, open discussions. This conference report summarizes the presentations that were given this year. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  13. Identification of atmospheric mercury sources and transport pathways on local and regional sales

    Science.gov (United States)

    Gratz, Lynne E.

    Mercury (Hg) is a hazardous air pollutant and bioaccumulative neurotoxin whose intricate atmospheric chemistry complicates our ability to define Hg source-receptor relationships on all scales. Our detailed measurements of Hg in its different forms together with atmospheric tracers have improved our understanding of Hg chemistry and transport. Daily-event precipitation samples collected from 1995 to 2006 in Underhill, VT were examined to identify Hg wet deposition trends and source influences. Analysis revealed that annual Hg deposition at this fairly remote location did not vary significantly over the 12-year period. While a decreasing trend in volume-weighted mean Hg concentration was observed, Hg wet deposition did not decline as transport of emissions from the Midwest and along the Atlantic Coast consistently contributed to the largest observed Hg wet deposition events. Receptor modeling of Hg and trace elements in precipitation indicated that ---60% of Hg wet deposition at Underhill could be attributed to emissions from coal-fired utility boilers (CFUBs), and their contribution to Hg wet deposition did not change significantly over time. Hybrid-receptor modeling further defined these CFUBs to be located predominantly in the Midwestern U.S. Atmospheric Hg chemistry and transport from the Chicago urban/industrial area was the focus of speciated Hg measurements performed in the southern Lake Michigan basin during summer 2007. Transport from Chicago, IL to Holland, MI occurred during 27% of the study period, resulting in a five-fold increase in divalent reactive gaseous Hg (RGM) at the downwind Holland site. Dispersion modeling of case study periods demonstrated that under southwesterly flow approximately half of the RGM in Holland could be attributed to primary RGM emissions from Chicago after transport and dispersion, with the remainder due to Hg0 oxidation in the atmosphere en route. Precipitation and ambient vapor phase samples were also collected in Chicago

  14. Soil HONO Emissions and Its Potential Impact on the Atmospheric Chemistry and Nitrogen Cycle

    Science.gov (United States)

    Su, H.; Chen, C.; Zhang, Q.; Poeschl, U.; Cheng, Y.

    2014-12-01

    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. The HONO emissions rates are estimated to be comparable to that of nitric oxide (NO) and could be an important source of atmospheric reactive nitrogen. Fertilized soils appear to be particularly strong sources of HONO. Thus, agricultural activities and land-use changes may strongly influence the oxidizing capacity of the atmosphere. A new HONO-DNDC model was developed to simulate the evolution of HONO emissions in agriculture ecosystems. 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. Reference: Su, H. et al., Soil Nitrite as a Source of Atmospheric HONO and OH Radicals, Science, 333, 1616-1618, 10.1126/science.1207687, 2011.

  15. The Effects of Interactive Stratospheric Chemistry on Antarctic and Southern Ocean Climate Change in an AOGCM

    Science.gov (United States)

    Li, Feng; Newman, Paul; Pawson, Steven; Waugh, Darryn

    2014-01-01

    Stratospheric ozone depletion has played a dominant role in driving Antarctic climate change in the last decades. In order to capture the stratospheric ozone forcing, many coupled atmosphere-ocean general circulation models (AOGCMs) prescribe the Antarctic ozone hole using monthly and zonally averaged ozone field. However, the prescribed ozone hole has a high ozone bias and lacks zonal asymmetry. The impacts of these biases on model simulations, particularly on Southern Ocean and the Antarctic sea ice, are not well understood. The purpose of this study is to determine the effects of using interactive stratospheric chemistry instead of prescribed ozone on Antarctic and Southern Ocean climate change in an AOGCM. We compare two sets of ensemble simulations for the 1960-2010 period using different versions of the Goddard Earth Observing System 5 - AOGCM: one with interactive stratospheric chemistry, and the other with prescribed monthly and zonally averaged ozone and 6 other stratospheric radiative species calculated from the interactive chemistry simulations. Consistent with previous studies using prescribed sea surface temperatures and sea ice concentrations, the interactive chemistry runs simulate a deeper Antarctic ozone hole and consistently larger changes in surface pressure and winds than the prescribed ozone runs. The use of a coupled atmosphere-ocean model in this study enables us to determine the impact of these surface changes on Southern Ocean circulation and Antarctic sea ice. The larger surface wind trends in the interactive chemistry case lead to larger Southern Ocean circulation trends with stronger changes in northerly and westerly surface flow near the Antarctica continent and stronger upwelling near 60S. Using interactive chemistry also simulates a larger decrease of sea ice concentrations. Our results highlight the importance of using interactive chemistry in order to correctly capture the influences of stratospheric ozone depletion on climate

  16. Atmospheric chemistry of CF3C(O)O2 radicals. Kinetics of their reaction with NO2 and kinetics of the thermal decomposition of the product CF3C(O)O2NO2

    DEFF Research Database (Denmark)

    Wallington, T.J.; Sehested, J.; Nielsen, O.J.

    1994-01-01

    A pulse radiolysis technique has been used to measure a rate constant of (6.6 +/- 1.3) x 10(-12) cm3 molecule-1 s-1 for the association reaction between CF3C(O)O2 radicals and NO2 at 295 K and one atmosphere total pressure of SF6 diluent. A FTIR/smog chamber system was used to study the thermal...... decomposition CF3C(O)O2NO2. The rate of decomposition of CF3C(O)O2NO2 was independent of the total pressure of N2 diluent over the range 100-700 Torr and was fit by the expression k-1 = (1.9(-1.5)+7.6) x 10(16) exp[(-14000 +/- 480)/T] s-1. Implications for the atmospheric chemistry of CFC replacements...

  17. Radiation chemistry and origins of life on earth

    International Nuclear Information System (INIS)

    Zagorski, Z.P.

    2002-01-01

    Complete text of publication follows. Radiation chemistry is involved in mechanisms of origins of life on Earth in three aspects: 1. The formation of prebiotic 'soup' of organic compounds related to future life, 2. Possible role in formation of pure enantiomers of chiral compounds, 3. Role in rejection of hypothesis of Life transported from the outside worlds (Panspermia). As concerns 1, radiation chemistry explains better the formation of proper prebiotic 'soup' than Miller hypothesis of electric discharges in gaseous atmosphere. Radiation-induced reactions proceeded in liquid phase, also in the presence of solid state and as specific surface reactions, all at the ambient temperature. As concerns 2, radiation chemistry offers limited possibilities, but papers still are published to that effect and efforts are needed to tell facts from artifacts. As concerns 3, radiation chemistry and its cousin - radiobiology speak out definitively, that any transportation of life, even of low organisation, from the outer space is impossible. The main reason is irreversible dehydrogenation even at very low temperatures, during the travel lasting for years and light-years. The same applies in higher degree to the well organised life, making an appearance of 'ET' on Earth not likely. Even the manned travels to Mars and living in houses at the surface, can end with radiation sickness and premature death

  18. Resolving the Strange Behavior of Extraterrestrial Potassium in the Upper Atmosphere

    Science.gov (United States)

    Plane, J. M. C.; Feng, W.; Dawkins, E.; Chipperfield, M. P.; Hoeffner, J.; Janches, D.; Marsh, D. R.

    2014-01-01

    It has been known since the 1960s that the layers of Na and K atoms, which occur between 80 and 105km in the Earth's atmosphere as a result of meteoric ablation, exhibit completely different seasonal behavior. In the extratropics Na varies annually, with a pronounced wintertime maximum and summertime minimum. However, K varies semiannually with a small summertime maximum and minima at the equinoxes. This contrasting behavior has never been satisfactorily explained. Here we use a combination of electronic structure and chemical kinetic rate theory to determine two key differences in the chemistries of K and Na. First, the neutralization of K+ ions is only favored at low temperatures during summer. Second, cycling between K and its major neutral reservoir KHCO3 is essentially temperature independent. A whole atmosphere model incorporating this new chemistry, together with a meteor input function, now correctly predicts the seasonal behavior of the K layer.

  19. Composition of Estonian atmosphere

    International Nuclear Information System (INIS)

    Punning, J. M.; Karindi, A.

    1996-01-01

    Atmospheric study, particularly that of its chemical composition, has a long tradition in Estonia. Since middle of this century, in addition to meteorological observations, some chemical compounds in precipitations have been regularly measured in many meteorological stations. The main aim was to acquire information about the state and dynamics of the atmosphere. Therefore, main attention was paid to monitoring chemical compounds which have a direct impact on the human environment. As energy production developed intensively and SO 2 and NO x increased drastically in the atmosphere in acidic rock areas, like Scandinavia, the problem of acid rain became the most important environmental problem in Europe and North-America. As a consequence, monitoring the compounds of sulphur in precipitation was organized in Estonia. In the 1970 s, as related to large operating oil shale-based power plants, Estonia became a country , where emissions of sulphur compounds per capita were extremely high. In 1979, Estonia became a participant in the European Monitoring and Evaluation Programme - the network created to study transboundary air pollution. The aims of the precipitation chemistry study and the related problems of the formation and transformation of the atmospheric composition have varied over the years. But monitoring of pollutant (in particular, sulphur compound) loads has been a central issue. Over recent years, an attempt was made to estimate the spatial regularities of atmospheric impurities and their impact on the pH of mean monthly precipitations. Furthermore, calculations were provided to find out the origin of atmospheric impurities washed out in Estonia. Until the 1990 s, CO 2 , and some other greenhouse gas (GHG) emissions were not studied in Estonia. The first inventory of GHG for Estonia was provided in 1995 using the Intergovernmental Panel on Climate Change (IPCC) methodology

  20. Radiological and Environmental Research Division annual report, January-December 1980. Atmospheric physics

    International Nuclear Information System (INIS)

    1981-08-01

    Contained are twenty-six abstracts of on-going research programs at Argonne National Laboratory concerning the modeling of environmental air pollutants concentration and transport for January-December 1980. Studies on pollutant transport modeling, fluid flow models, and atmospheric precipitations chemistry are included

  1. SMOG-CHAMBER TOXICOLOGY BETTER ESTIMATES THE TRUE TOXIC POTENTIAL OF ATMOSPHERIC MIXTURES

    Science.gov (United States)

    The chemistry of hazardous air pollutants (HAPs) have been studied for many years, yet little is known about how these chemicals, once interacted with urban atmospheres, affect healthy and susceptible individuals. The toxic potential of these very reactive compounds once they int...

  2. Titan 2D: Understanding Titan’s Seasonal Atmospheric Cycles

    Science.gov (United States)

    Wong, Michael; Zhang, X.; Li, C.; Hu, R.; Shia, R.; Newman, C.; Müller-Wodarg, I.; Yung, Y.

    2013-10-01

    In this study, we present results from a novel two-dimensional (2D) model that simulates the physics and chemistry of Titan’s atmosphere. Despite being an icy moon of Saturn, Titan is the only Solar System object aside from Earth that is sheathed by a thick nitrogen-dominated atmosphere. This vulnerable gaseous envelope—an embodiment of a delicate coupling between photochemistry, radiation, and dynamics—is Nature’s laboratory for the synthesis of complex organic molecules. Titan’s large obliquity generates pronounced seasonal cycles in its atmosphere, and the Cassini spacecraft has been observing these variations since 2004. In particular, Cassini measurements show that the latitudinal distribution of Titan’s rich mélange of hydrocarbon species follows seasonal patterns. The mixing ratios of hydrocarbons increase with latitude towards the winter pole, suggesting a pole-to-pole circulation that reverses after equinox. Using a one-dimensional photochemical model of Titan’s atmosphere, we show that photochemistry alone cannot produce the observed meridional hydrocarbon distribution. This necessitates the employment of a 2D chemistry-transport model that includes meridional circulation as well as diffusive processes and photochemistry. Of additional concern, no previous 2D model of Titan extends beyond 500 km altitude—a critical limitation since the peak of methane photolysis is at 800 km. Our 2D model is the first to include Titan’s stratosphere, mesosphere, and thermosphere. The meridional circulation in our 2D model is derived from the outputs of two general circulation models (GCMs): the TitanWRF GCM (Newman et al. 2011) covering the troposphere, stratosphere, and lower mesosphere, and a thermosphere general circulation model (TGCM) covering the remainder of the atmosphere through the thermosphere (Müller-Wodarg et al. 2003; 2008). This presentation will focus on the utilization of these advances applied to the 2D Caltech/JPL KINETICS model to

  3. Combustion Chemistry of Fuels: Quantitative Speciation Data Obtained from an Atmospheric High-temperature Flow Reactor with Coupled Molecular-beam Mass Spectrometer.

    Science.gov (United States)

    Köhler, Markus; Oßwald, Patrick; Krueger, Dominik; Whitside, Ryan

    2018-02-19

    This manuscript describes a high-temperature flow reactor experiment coupled to the powerful molecular beam mass spectrometry (MBMS) technique. This flexible tool offers a detailed observation of chemical gas-phase kinetics in reacting flows under well-controlled conditions. The vast range of operating conditions available in a laminar flow reactor enables access to extraordinary combustion applications that are typically not achievable by flame experiments. These include rich conditions at high temperatures relevant for gasification processes, the peroxy chemistry governing the low temperature oxidation regime or investigations of complex technical fuels. The presented setup allows measurements of quantitative speciation data for reaction model validation of combustion, gasification and pyrolysis processes, while enabling a systematic general understanding of the reaction chemistry. Validation of kinetic reaction models is generally performed by investigating combustion processes of pure compounds. The flow reactor has been enhanced to be suitable for technical fuels (e.g. multi-component mixtures like Jet A-1) to allow for phenomenological analysis of occurring combustion intermediates like soot precursors or pollutants. The controlled and comparable boundary conditions provided by the experimental design allow for predictions of pollutant formation tendencies. Cold reactants are fed premixed into the reactor that are highly diluted (in around 99 vol% in Ar) in order to suppress self-sustaining combustion reactions. The laminar flowing reactant mixture passes through a known temperature field, while the gas composition is determined at the reactors exhaust as a function of the oven temperature. The flow reactor is operated at atmospheric pressures with temperatures up to 1,800 K. The measurements themselves are performed by decreasing the temperature monotonically at a rate of -200 K/h. With the sensitive MBMS technique, detailed speciation data is acquired and

  4. Ocean acidification 2.0: Managing our Changing Coastal Ocean Chemistry

    OpenAIRE

    Strong, AL; Kroeker, KJ; Teneva, LT; Mease, LA; Kelly, RP

    2014-01-01

    Ocean acidification (OA) is rapidly emerging as a significant problem for organisms, ecosystems, and human societies. Globally, addressing OA and its impacts requires international agreements to reduce rising atmospheric carbon dioxide concentrations. However, the complex suite of drivers of changing carbonate chemistry in coastal environments also requires regional policy analysis, mitigation, and adaptation responses. In order to fundamentally address the threat of OA, environmental manager...

  5. Climate effects of anthropogenic sulfate: Simulations from a coupled chemistry/climate model

    International Nuclear Information System (INIS)

    Chuang, C.C.; Penner, J.E.; Taylor, K.E.; Walton, J.J.

    1993-09-01

    In this paper, we use a more comprehensive approach by coupling a climate model with a 3-D global chemistry model to investigate the forcing by anthropogenic aerosol sulfate. The chemistry model treats the global-scale transport, transformation, and removal of SO 2 , DMS and H 2 SO 4 species in the atmosphere. The mass concentration of anthropogenic sulfate from fossil fuel combustion and biomass burning is calculated in the chemistry model and provided to the climate model where it affects the shortwave radiation. We also investigate the effect, with cloud nucleation parameterized in terms of local aerosol number, sulfate mass concentration and updraft velocity. Our simulations indicate that anthropogenic sulfate may result in important increases in reflected solar radiation, which would mask locally the radiative forcing from increased greenhouse gases. Uncertainties in these results will be discussed

  6. On the relationship between the greenhouse effect, atmospheric photochemistry, and species distribution

    Science.gov (United States)

    Callis, L. B.; Boughner, R. E.; Natarajan, M.

    1983-01-01

    The coupling that exists between infrared opacity changes and tropospheric (and to a lesser extent stratospheric) chemistry is explored in considerable detail, and the effects arising from various perturbations are examined. The studies are carried out with a fully coupled one-dimensional radiative-convective-photochemical model (RCP) that extends from the surface to 53.5 km and has the capability of calculating surface temperature changes due to both chemical and radiative perturbations. The model encompasses contemporary atmospheric chemistry and photochemistry involving the O(x), HO(x), NO(x), and Cl(x) species.

  7. National Status and Trends, Benthic Surveillance Project Chemistry Data, 1984-1992, National Centers for Coastal Ocean Science

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — The National Status and Trends (NS&T) Benthic Surveillance Project Chemistry data file reports the trace concentrations of a suite of chemical contaminants in...

  8. National Status and Trends, Benthic Surveillance Project Chemistry Data, 1984-1992, National Centers for Coastal Ocean Science

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — The National Status and Trends (NSandT) Benthic Surveillance Project Chemistry data file reports the trace concentrations of a suite of chemical contaminants in...

  9. Sentinel-5: the new generation European operational atmospheric chemistry mission in polar orbit

    Science.gov (United States)

    Pérez Albiñana, Abelardo; Erdmann, Matthias; Wright, Norrie; Martin, Didier; Melf, Markus; Bartsch, Peter; Seefelder, Wolfgang

    2017-08-01

    Sentinel-5 is an Earth Observation instrument to be flown on the Metop Second Generation (Metop-SG) satellites with the fundamental objective of monitoring atmospheric composition from polar orbit. The Sentinel-5 instrument consists of five spectrometers to measure the solar spectral radiance backscattered by the earth atmosphere in five bands within the UV (270nm) to SWIR (2385nm) spectral range. Data provided by Sentinel-5 will allow obtaining the distribution of important atmospheric constituents such as ozone, on a global daily basis and at a finer spatial resolution than its precursor instruments on the first generation of Metop satellites. The launch of the first Metop-SG satellite is foreseen for 2021. The Sentinel-5 instrument is being developed by Airbus DS under contract to the European Space Agency. The Sentinel-5 mission is part of the Space Component of the Copernicus programme, a joint initiative by ESA, EUMETSAT and the European Commission. The Preliminary Design Review (PDR) for the Sentinel-5 development was successfully completed in 2015. This paper provides a description of the Sentinel-5 instrument design and data calibration.

  10. Molecular line parameters for the atmospheric trace molecule spectroscopy experiment

    Science.gov (United States)

    Brown, L. R.; Farmer, C. B.; Toth, R. A.; Rinsland, Curtis P.

    1987-01-01

    During its first mission in 1985 onboard Spacelab 3, the ATMOS (atmospheric trace molecule spectroscopy) instrument, a high speed Fourier transform spectrometer, produced a large number of high resolution infrared solar absorption spectra recorded in the occultation mode. The analysis and interpretation of these data in terms of composition, chemistry, and dynamics of the earth's upper atmosphere required good knowledge of the molecular line parameters for those species giving rise to the absorptions in the atmospheric spectra. This paper describes the spectroscopic line parameter database compiled for the ATMOS experiment and referenced in other papers describing ATMOS results. With over 400,000 entries, the linelist catalogs parameters of 46 minor and trace species in the 1-10,000/cm region.

  11. An advanced technique for speciation of organic nitrogen in atmospheric aerosols

    Science.gov (United States)

    Samy, S.; Robinson, J.; Hays, M. D.

    2011-12-01

    The chemical composition of organic nitrogen (ON) in the environment is a research topic of broad significance. The topic intersects the branches of atmospheric, aquatic, and ecological science; thus, a variety of instrumentation, analytical methods, and data interpretation tools have evolved for determination of ON. Recent studies that focus on atmospheric particulate nitrogen (N) suggest a significant fraction (20-80%) of total N is bound in organic compounds. The sources, bioavailability and transport mechanisms of these N-containing compounds can differ, producing a variety of environmental consequences. Amino acids (AA) are a key class of atmospheric ON compounds that can contribute to secondary organic aerosol (SOA) formation and potentially influence water cycles, air pollutant scavenging, and the radiation balance. AA are water-soluble organic compounds (WSOC) that can significantly alter the acid-base chemistry of aerosols, and may explain the buffering capacity that impacts heterogeneous atmospheric chemistry. The chemical transformations that N-containing organic compounds (including AA) undergo can increase the light-absorbing capacity of atmospheric carbon via formation of 'brown carbon'. Suggested sources of atmospheric AA include: marine surface layer transport from bursting sea bubbles, the suspension of bacteria, fungi, algae, pollen, spores, or biomass burning. Methodology for detection of native (underivatized) amino acids (AA) in atmospheric aerosols has been developed and validated (Samy et al., 2011). This presentation describes the use of LC-MS (Q-TOF) and microwave-assisted gas phase hydrolysis for detection of free and combined amino acids in aerosols collected in a Southeastern U.S. forest environment. Accurate mass detection and the addition of isotopically labeled surrogates prior to sample preparation allows for sensitive quantitation of target AA in a complex aerosol matrix. A total of 16 native AA were detected above the reporting

  12. Raman spectroscopy in high temperature chemistry

    International Nuclear Information System (INIS)

    Drake, M.C.; Rosenblatt, G.M.

    1979-01-01

    Raman spectroscopy (largely because of advances in laser and detector technology) is assuming a rapidly expanding role in many areas of research. This paper reviews the contribution of Raman spectroscopy in high temperature chemistry including molecular spectroscopy on static systems and gas diagnostic measurements on reactive systems. An important aspect of high temperature chemistry has been the identification and study of the new, and often unusual, gaseous molecules which form at high temperatures. Particularly important is the investigation of vibrational-rotational energy levels and electronic states which determine thermodynamic properties and describe chemical bonding. Some advantages and disadvantages of high temperature Raman spectrosocpy for molecular studies on static systems are compared: (1) Raman vs infrared; (2) gas-phase vs condensed in matries; and (3) atmospheric pressure Raman vs low pressure techniques, including mass spectroscopy, matrix isolation, and molecular beams. Raman studies on molecular properties of gases, melts, and surfaces are presented with emphasis on work not covered in previous reviews of high temperature and matrix isolation Raman spectroscopy

  13. Raman spectroscopy in high temperature chemistry

    International Nuclear Information System (INIS)

    Drake, M.C.; Rosenblatt, G.M.

    1979-01-01

    Raman spectroscopy (largely because of advances in laser and detector technology) is assuming a rapidly expanding role in many areas of research. This paper reviews the contribution of Raman spectroscopy in high temperature chemistry including molecular spectroscopy on static systems and gas diagnostic measurements on reactive systems. An important aspect of high temperature chemistry has been the identification and study of the new, and often unusual, gaseous molecules which form at high temperatures. Particularly important is the investigation of vibrational-rotational energy levels and electronic states which determine thermodynamic properties and describe chemical bonding. Some advantages and disadvantages of high temperature Raman spectrosocpy for molecular studies on static systems are compared: (1) Raman vs infrared; (2) gas-phase vs condensed in matrices; and (3) atmospheric pressure Raman vs low pressure techniques, including mass spectroscopy, matrix isolation, and molecular beams. Raman studies on molecular properties of gases, melts, and surfaces are presented with emphasis on work not covered in previous reviews of high temperature and matrix isolation Raman spectroscopy

  14. Chemical kinetic studies of atmospheric reactions using tunable diode laser spectroscopy

    Science.gov (United States)

    Worsnop, Douglas R.; Nelson, David D.; Zahniser, Mark S.

    1993-01-01

    IR absorption using tunable diode laser spectroscopy provides a sensitive and quantitative detection method for laboratory kinetic studies of atmospheric trace gases. Improvements in multipass cell design, real time signal processing, and computer controlled data acquisition and analysis have extended the applicability of the technique. We have developed several optical systems using off-axis resonator mirror designs which maximize path length while minimizing both the sample volume and the interference fringes inherent in conventional 'White' cells. Computerized signal processing using rapid scan (300 kHz), sweep integration with 100 percent duty cycle allows substantial noise reduction while retaining the advantages of using direct absorption for absolute absorbance measurements and simultaneous detection of multiple species. Peak heights and areas are determined by curve fitting using nonlinear least square methods. We have applied these techniques to measurements of: (1) heterogeneous uptake chemistry of atmospheric trace gases (HCl, H2O2, and N2O5) on aqueous and sulfuric acid droplets; (2) vapor pressure measurements of nitric acid and water over prototypical stratospheric aerosol (nitric acid trihydrate) surfaces; and (3) discharge flow tube kinetic studies of the HO2 radical using isotopic labeling for product channel and mechanistic analysis. Results from each of these areas demonstrate the versatility of TDL absorption spectroscopy for atmospheric chemistry applications.

  15. MAP3S precipitation chemistry network: fourth periodic summary report (1980)

    Energy Technology Data Exchange (ETDEWEB)

    1981-12-01

    This, the fourth in a series of summary reports, contains complete field and chemical data from the MAP3S/RAINE (Multistate Atmospheric Power Production Pollution Studies) Precipitation Chemistry Network for the year 1980. The 1980 data were added to the previous data base, and an update of the previous statistical summary completed. Included are basic statistics, time trend analyses, and monthly averages.

  16. Chemistry and physics

    International Nuclear Information System (INIS)

    Broerse, J.J.; Barendsen, G.W.; Kal, H.B.; Kogel, A.J. van der

    1983-01-01

    This book contains the extended abstracts of the contributions of the poster workshop sessions on chemistry and physics of the 7th international congress of radiation research. They cover the following main topics: primary processes in radiation physics and chemistry, general chemistry in radiation chemistry, DNA and model systems in radiation chemistry, molecules of biological interest in radiation chemistry, techniques in radiation chemistry, hot atom chemistry. refs.; figs.; tabs

  17. The Atmosphere and Climate of Venus

    Science.gov (United States)

    Bullock, M. A.; Grinspoon, D. H.

    Venus lies just sunward of the inner edge of the Sun's habitable zone. Liquid water is not stable. Like Earth and Mars, Venus probably accreted at least an ocean's worth of water, although there are alternative scenarios. The loss of this water led to the massive, dry CO2 atmosphere, extensive H2SO4 clouds (at least some of the time), and an intense CO2 greenhouse effect. This chapter describes the current understanding of Venus' atmosphere, established from the data of dozens of spacecraft and atmospheric probe missions since 1962, and by telescopic observations since the nineteenth century. Theoretical work to model the temperature, chemistry, and circulation of Venus' atmosphere is largely based on analogous models developed in the Earth sciences. We discuss the data and modeling used to understand the temperature structure of the atmosphere, as well as its composition, cloud structure, and general circulation. We address what is known and theorized about the origin and early evolution of Venus' atmosphere. It is widely understood that Venus' dense CO2 atmosphere is the ultimate result of the loss of an ocean to space, but the timing of major transitions in Venus' climate is very poorly constrained by the available data. At present, the bright clouds allow only 20% of the sunlight to drive the energy balance and therefore determine conditions at Venus' surface. Like Earth and Mars, differential heating between the equator and poles drives the atmospheric circulation. Condensable species in the atmosphere create clouds and hazes that drive feedbacks that alter radiative forcing. Also in common with Earth and Mars, the loss of light, volatile elements to space produces long-term changes in composition and chemistry. As on Earth, geologic processes are most likely modifying the atmosphere and clouds by injecting gases from volcanos as well as directly through chemical reactions with the surface. The sensitivity of Venus' atmospheric energy balance is quantified in

  18. High fidelity chemistry and radiation modeling for oxy -- combustion scenarios

    Science.gov (United States)

    Abdul Sater, Hassan A.

    To account for the thermal and chemical effects associated with the high CO2 concentrations in an oxy-combustion atmosphere, several refined gas-phase chemistry and radiative property models have been formulated for laminar to highly turbulent systems. This thesis examines the accuracies of several chemistry and radiative property models employed in computational fluid dynamic (CFD) simulations of laminar to transitional oxy-methane diffusion flames by comparing their predictions against experimental data. Literature review about chemistry and radiation modeling in oxy-combustion atmospheres considered turbulent systems where the predictions are impacted by the interplay and accuracies of the turbulence, radiation and chemistry models. Thus, by considering a laminar system we minimize the impact of turbulence and the uncertainties associated with turbulence models. In the first section of this thesis, an assessment and validation of gray and non-gray formulations of a recently proposed weighted-sum-of-gray gas model in oxy-combustion scenarios was undertaken. Predictions of gas, wall temperatures and flame lengths were in good agreement with experimental measurements. The temperature and flame length predictions were not sensitive to the radiative property model employed. However, there were significant variations between the gray and non-gray model radiant fraction predictions with the variations in general increasing with decrease in Reynolds numbers possibly attributed to shorter flames and steeper temperature gradients. The results of this section confirm that non-gray model predictions of radiative heat fluxes are more accurate than gray model predictions especially at steeper temperature gradients. In the second section, the accuracies of three gas-phase chemistry models were assessed by comparing their predictions against experimental measurements of temperature, species concentrations and flame lengths. The chemistry was modeled employing the Eddy

  19. Temporal characteristics of atmospheric ammonia and nitrogen dioxide over China based on emission data, satellite observations and atmospheric transport modeling since 1980

    Directory of Open Access Journals (Sweden)

    L. Liu

    2017-08-01

    Full Text Available China is experiencing intense air pollution caused in large part by anthropogenic emissions of reactive nitrogen (Nr. Atmospheric ammonia (NH3 and nitrogen dioxide (NO2 are the most important precursors for Nr compounds (including N2O5, HNO3, HONO and particulate NO3− and NH4+ in the atmosphere. Understanding the changes in NH3 and NO2 has important implications for the regulation of anthropogenic Nr emissions and is a requirement for assessing the consequence of environmental impacts. We conducted the temporal trend analysis of atmospheric NH3 and NO2 on a national scale since 1980 based on emission data (during 1980–2010, satellite observation (for NH3 since 2008 and for NO2 since 2005 and atmospheric chemistry transport modeling (during 2008–2015.Based on the emission data, during 1980–2010, significant continuous increasing trends in both NH3 and NOx were observed in REAS (Regional Emission inventory in Asia, for NH3 0.17 and for NOx 0.16 kg N ha−1 yr−2 and EDGAR (Emissions Database for Global Atmospheric Research, for NH3 0.24 and for NOx 0.17 kg N ha−1 yr−2 over China. Based on the satellite data and atmospheric chemistry transport model (CTM MOZART-4 (Model for Ozone and Related chemical Tracers, version 4, the NO2 columns over China increased significantly from 2005 to 2011 and then decreased significantly from 2011 to 2015; the satellite-retrieved NH3 columns from 2008 to 2014 increased at a rate of 2.37 % yr−1. The decrease in NO2 columns since 2011 may result from more stringent strategies taken to control NOx emissions during the 12th Five Year Plan, while no control policy has focused on NH3 emissions. Our findings provided an overall insight into the temporal trends of both NO2 and NH3 since 1980 based on emission data, satellite observations and atmospheric transport modeling. These findings can provide a scientific background for policy makers that are attempting to control atmospheric

  20. Surface organization of aqueous MgCl2 and application to atmospheric marine aerosol chemistry

    Czech Academy of Sciences Publication Activity Database

    Casillas-Ituarte, N. N.; Callahan, K. M.; Tang, CH. Y.; Chen, X.; Roeselová, Martina; Tobias, D. J.; Allen, H. C.

    2010-01-01

    Roč. 107, č. 15 (2010), s. 6616-6621 ISSN 0027-8424 R&D Projects: GA MŠk LC512; GA MŠk ME09064 Institutional research plan: CEZ:AV0Z40550506 Keywords : magnesium chloride * fatty acid * air/aqueous interface Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 9.771, year: 2010

  1. Atmospheric chemistry of Z- and E-CF3CH=CHCF3

    DEFF Research Database (Denmark)

    Østerstrøm, Freja From; Andersen, Simone Thirstrup; Sølling, Theis Ivan

    2017-01-01

    radicals. The atmospheric lifetimes of Z- and E-CF3CH[double bond, length as m-dash]CHCF3 are estimated as 27 and 67 days, respectively. IR absorption cross sections are reported and the global warming potentials (GWPs) of Z- and E-CF3CH[double bond, length as m-dash]CHCF3 for the 100 year time horizon...

  2. Reaction Mechanisms on Multiwell Potential Energy Surfaces in Combustion (and Atmospheric) Chemistry

    International Nuclear Information System (INIS)

    Osborn, David L.

    2017-01-01

    Chemical reactions occurring on a potential energy surface with multiple wells are ubiquitous in low temperature combustion and the oxidation of volatile organic compounds in earth’s atmosphere. The rich variety of structural isomerizations that compete with collisional stabilization make characterizing such complex-forming reactions challenging. This review describes recent experimental and theoretical advances that deliver increasingly complete views of their reaction mechanisms. New methods for creating reactive intermediates coupled with multiplexed measurements provide many experimental observables simultaneously. Automated methods to explore potential energy surfaces can uncover hidden reactive pathways, while master equation methods enable a holistic treatment of both sequential and well-skipping pathways. Our ability to probe and understand nonequilibrium effects and reaction sequences is increasing. These advances provide the fundamental science base for predictive models of combustion and the atmosphere that are crucial to address global challenges.

  3. Reaction Mechanisms on Multiwell Potential Energy Surfaces in Combustion (and Atmospheric) Chemistry

    Science.gov (United States)

    Osborn, David L.

    2017-05-01

    Chemical reactions occurring on a potential energy surface with multiple wells are ubiquitous in low-temperature combustion and in the oxidation of volatile organic compounds in Earth's atmosphere. The rich variety of structural isomerizations that compete with collisional stabilization makes characterizing such complex-forming reactions challenging. This review describes recent experimental and theoretical advances that deliver increasingly complete views of their reaction mechanisms. New methods for creating reactive intermediates coupled with multiplexed measurements provide many experimental observables simultaneously. Automated methods to explore potential energy surfaces can uncover hidden reactive pathways, and master equation methods enable a holistic treatment of both sequential and well-skipping pathways. Our ability to probe and understand nonequilibrium effects and reaction sequences is increasing. These advances provide the fundamental science base for predictive models of combustion and the atmosphere that are crucial to address global challenges.

  4. Thin-Layer Chromatography/Desorption Atmospheric Pressure Photoionization Orbitrap Mass Spectrometry of Lipids

    Czech Academy of Sciences Publication Activity Database

    Rejšek, Jan; Vrkoslav, Vladimír; Vaikkinen, A.; Haapala, M.; Kauppila, T. J.; Kostiainen, R.; Cvačka, Josef

    2016-01-01

    Roč. 88, č. 24 (2016), s. 12279-12286 ISSN 0003-2700 R&D Projects: GA ČR GAP206/12/0750 Institutional support: RVO:61388963 Keywords : desorption atmospheric pressure photoionization * thin-layer chromatography * lipids Subject RIV: CB - Analytical Chemistry, Separation Impact factor: 6.320, year: 2016

  5. From hot atom chemistry to epithermal chemistry

    International Nuclear Information System (INIS)

    Roessler, K.

    2004-01-01

    The rise and fall of hot atom chemistry (HAC) over the years from 1934 to 2004 is reviewed. Several applications are discussed, in particular to astrophysics and the interaction of energetic ions and atoms in space. Epithermal chemistry (ETC) is proposed to substitute the old name, since it better fits the energy range as well as the non-thermal and non-equilibrium character of the reactions. ETC also avoids the strong connexion of HAC to nuclear chemistry and stands for the opening of the field to physical chemistry and astrophysics. (orig.)

  6. Mathematical Chemistry

    OpenAIRE

    Trinajstić, Nenad; Gutman, Ivan

    2002-01-01

    A brief description is given of the historical development of mathematics and chemistry. A path leading to the meeting of these two sciences is described. An attempt is made to define mathematical chemistry, and journals containing the term mathematical chemistry in their titles are noted. In conclusion, the statement is made that although chemistry is an experimental science aimed at preparing new compounds and materials, mathematics is very useful in chemistry, among other things, to produc...

  7. HMSRP Hawaiian Monk Seal Blood Values (Establishing hematology and serum chemistry reference ranges for wild Hawaiian Monk Seals)

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — Hematology and serum chemistry evaluations are essential to a patients comprehensive health exam by providing measures of organ function, blood cell volume and...

  8. Methods of gas purification and effect on the ion composition in an RF atmospheric pressure plasma jet investigated by mass spectrometry

    International Nuclear Information System (INIS)

    Grosse-Kreul, Simon; Huebner, Simon; Schneider, Simon; Keudell, Achim von; Benedikt, Jan

    2016-01-01

    The analysis of the ion chemistry of atmospheric pressure plasmas is essential to evaluate ionic reaction pathways during plasma-surface or plasma-analyte interactions. In this contribution, the ion chemistry of a radio-frequency atmospheric pressure plasma jet (μ-APPJ) operated in helium is investigated by mass spectrometry (MS). It is found, that the ion composition is extremely sensitive to impurities such as N 2 , O 2 and H 2 O. Without gas purification, protonated water cluster ions of the form H + (H 2 O) n are dominating downstream the positive ion mass spectrum. However, even after careful feed gas purification to the sub-ppm level using a molecular sieve trap and a liquid nitrogen trap as well as operation of the plasma in a controlled atmosphere, the positive ion mass spectrum is strongly influenced by residual trace gases. The observations support the idea that species with a low ionization energy serve as a major source of electrons in atmospheric pressure helium plasmas. Similarly, the neutral density of atomic nitrogen measured by MS in a He/N 2 mixture is varying up to a factor 3, demonstrating the significant influence of impurities on the neutral species chemistry as well. (orig.)

  9. Methods of gas purification and effect on the ion composition in an RF atmospheric pressure plasma jet investigated by mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Grosse-Kreul, Simon; Huebner, Simon; Schneider, Simon; Keudell, Achim von; Benedikt, Jan [Ruhr-Universitaet Bochum, Institute for Experimental Physics II, Bochum (Germany)

    2016-12-15

    The analysis of the ion chemistry of atmospheric pressure plasmas is essential to evaluate ionic reaction pathways during plasma-surface or plasma-analyte interactions. In this contribution, the ion chemistry of a radio-frequency atmospheric pressure plasma jet (μ-APPJ) operated in helium is investigated by mass spectrometry (MS). It is found, that the ion composition is extremely sensitive to impurities such as N{sub 2}, O{sub 2} and H{sub 2}O. Without gas purification, protonated water cluster ions of the form H{sup +}(H{sub 2}O){sub n} are dominating downstream the positive ion mass spectrum. However, even after careful feed gas purification to the sub-ppm level using a molecular sieve trap and a liquid nitrogen trap as well as operation of the plasma in a controlled atmosphere, the positive ion mass spectrum is strongly influenced by residual trace gases. The observations support the idea that species with a low ionization energy serve as a major source of electrons in atmospheric pressure helium plasmas. Similarly, the neutral density of atomic nitrogen measured by MS in a He/N{sub 2} mixture is varying up to a factor 3, demonstrating the significant influence of impurities on the neutral species chemistry as well. (orig.)

  10. Towards a Comprehensive Dynamic-chemistry Assimilation for Eos-Chem: Plans and Status in NASA's Data Assimilation Office

    Science.gov (United States)

    Pawson, Steven; Lin, Shian-Jiann; Rood, Richard B.; Stajner, Ivanka; Nebuda, Sharon; Nielsen, J. Eric; Douglass, Anne R.

    2000-01-01

    In order to support the EOS-Chem project, a comprehensive assimilation package for the coupled chemical-dynamical system is being developed by the Data Assimilation Office at NASA GSFC. This involves development of a coupled chemistry/meteorology model and of data assimilation techniques for trace species and meteorology. The model is being developed using the flux-form semi-Lagrangian dynamical core of Lin and Rood, the physical parameterizations from the NCAR Community Climate Model, and atmospheric chemistry modules from the Atmospheric Chemistry and Dynamics branch at NASA GSFC. To date the following results have been obtained: (i) multi-annual simulations with the dynamics-radiation model show the credibility of the package for atmospheric simulations; (ii) initial simulations including a limited number of middle atmospheric trace gases reveal the realistic nature of transport mechanisms, although there is still a need for some improvements. Samples of these results will be shown. A meteorological assimilation system is currently being constructed using the model; this will form the basis for the proposed meteorological/chemical assimilation package. The latter part of the presentation will focus on areas targeted for development in the near and far terms, with the objective of Providing a comprehensive assimilation package for the EOS-Chem science experiment. The first stage will target ozone assimilation. The plans also encompass a reanalysis (ReSTS) for the 1991-1995 period, which includes the Mt. Pinatubo eruption and the time when a large number of UARS observations were available. One of the most challenging aspects of future developments will be to couple theoretical advances in tracer assimilation with the practical considerations of a real environment and eventually a near-real-time assimilation system.

  11. Hydroxyl and Hydroperoxy Radical Chemistry during the MCMA-2006 Field Campaign: Measurement and Model Comparison

    Science.gov (United States)

    Dusanter, S.; Vimal, D.; Stevens, P. S.; Volkamer, R.; Molina, L. T.

    2007-12-01

    The Mexico City Metropolitan Area (MCMA) field campaign, held in March 2006, was a unique opportunity to collect data in one of the most polluted megacities in the world. Such environments exhibit a complex oxidation chemistry involving a strong coupling between odd hydrogen radicals (HOX=OH+HO2) and nitrogen oxides species (NOX=NO+NO2). High levels of volatile organic compounds (VOCs) and NOX control the HOX budget and lead to elevated tropospheric ozone formation. The HOX-NOX coupling can be investigated by comparing measured and model-predicted HOx concentrations. Atmospheric HOX concentrations were measured by the Indiana University laser-induced fluorescence instrument and data were collected at the Instituto Mexicano del Petroleo between 14 and 31 March. Measured hydroxyl radical (OH) concentrations are comparable to that measured in less polluted urban environments and suggest that the OH concentrations are highly buffered under high NOX conditions. In contrast, hydroperoxy radical (HO2) concentrations are more sensitive to the NOX levels and are highly variable between different urban sites. Enhanced levels of OH and HO2 radicals were observed on several days between 9h30-11h00 AM and suggest an additional HOX source for the morning hours and/or a fast HOX cycling under the high NOX conditions of the MCMA. A preliminary investigation of the HOX chemistry occurring in the MCMA urban atmosphere was performed using a photochemical box model based on the Regional Atmospheric Chemistry Mechanism (RACM). Model comparisons will be presented and the agreement between measured and predicted HOX concentrations will be discussed.

  12. Measurements of Positively Charged Ions in Premixed Methane-Oxygen Atmospheric Flames

    KAUST Repository

    Alquaity, Awad

    2016-08-22

    Cations and anions are formed as a result of chemi-ionization processes in combustion systems. Electric fields can be applied to reduce emissions and improve combustion efficiency by active control of the combustion process. Detailed flame ion chemistry models are needed to understand and predict the effect of external electric fields on combustion plasmas. In this work, a molecular beam mass spectrometer (MBMS) is utilized to measure ion concentration profiles in premixed methane–oxygen argon burner-stabilized atmospheric flames. Lean and stoichiometric flames are considered to assess the dependence of ion chemistry on flame stoichiometry. Relative ion concentration profiles are compared with numerical simulations using various temperature profiles, and good qualitative agreement was observed for the stoichiometric flame. However, for the lean flame, numerical simulations misrepresent the spatial distribution of selected ions greatly. Three modifications are suggested to enhance the ion mechanism and improve the agreement between experiments and simulations. The first two modifications comprise the addition of anion detachment reactions to increase anion recombination at low temperatures. The third modification involves restoring a detachment reaction to its original irreversible form. To our knowledge, this work presents the first detailed measurements of cations and flame temperature in canonical methane–oxygen-argon atmospheric flat flames. The positive ion profiles reported here may be useful to validate and improve ion chemistry models for methane-oxygen flames.

  13. Influence of timing and spatial extent of savanna fires in southern Africa on atmospheric emissions

    CSIR Research Space (South Africa)

    Korontzi, S

    2003-06-01

    Full Text Available Biomass burning is an important ecosystem process in southern Africa, with significant implications for regional and. global atmospheric chemistry and biogeochemical cycles. In this paper, representative Land sat path-row scene locations...

  14. Regional emission and loss budgets of atmospheric methane (2002-2012)

    Science.gov (United States)

    Saeki, T.; Patra, P. K.; Dlugokencky, E. J.; Ishijima, K.; Umezawa, T.; Ito, A.; Aoki, S.; Morimoto, S.; Kort, E. A.; Crotwell, A. M.; Ravi Kumar, K.; Nakazawa, T.

    2015-12-01

    Methane (CH4) plays important roles in atmospheric chemistry and short-term forcing of climate. Clear understanding of atmospheric CH4's budget of emissions and losses is required to aid sustainable development of Earth's future environment. We used an atmospheric chemistry-transport model (JAMSTEC's ACTM) for simulating atmospheric CH4. An inverse modeling system has been developed for estimating CH4 emissions (7 ensemble cases) from 53 land regions for 2002-2012 using measurements at 39 sites. Global net CH4 emissions varied between 505-509 and 524-545 Tg/yr during 2002-2004 and 2010-2012, respectively (ranges based on 6 inversion cases), with a step like increase in 2007 in agreement with atmospheric measurement. The inversion system did not account for interannual variations in radicals reacting with CH4 in atmosphere. Our results suggest that the recent update of EDGAR inventory (version 4.2FT2010) overestimated global total emissions by at least 25 Tg/yr in 2010. Increase in CH4 emission since 2004 originated in the tropical and southern hemisphere regions, with timing consistent with an increase of non-dairy cattle stocks by ~10% in 2012 from 1056 million heads in 2002, leading to ~10 Tg/yr increase in emissions from enteric fermentation. All 7 inversions robustly estimated the interannual variations in emissions, but poorly constrained the seasonal cycle amplitude or phase consistently for all regions due to sparse observational network. Forward simulation results using both the a priori and a posteriori emissions are compared with independent aircraft measurements for validation. By doing that we are able to reject the upper limit (545 Tg/yr) of global total emissions as 14 Tg/yr too high during 2008-2012, which allows us to further conclude that CH4 emission increase rate over the East Asia (China mainly) region was 7-8 Tg/yr between the 2002-2006 and 2008-2012 periods, contrary to 1-17 Tg/yr in the a priori emissions.

  15. Concentrations and fate of decamethylcyclopentasiloxane (D(5)) in the atmosphere.

    Science.gov (United States)

    McLachlan, Michael S; Kierkegaard, Amelie; Hansen, Kaj M; van Egmond, Roger; Christensen, Jesper H; Skjøth, Carsten A

    2010-07-15

    Decamethylcyclopentasiloxane (D(5)) is a volatile compound used in personal care products that is released to the atmosphere in large quantities. Although D(5) is currently under consideration for regulation, there have been no field investigations of its atmospheric fate. We employed a recently developed, quality assured method to measure D(5) concentration in ambient air at a rural site in Sweden. The samples were collected with daily resolution between January and June 2009. The D(5) concentration ranged from 0.3 to 9 ng m(-3), which is 1-3 orders of magnitude lower than previous reports. The measured data were compared with D(5) concentrations predicted using an atmospheric circulation model that included both OH radical and D(5) chemistry. The model was parametrized using emissions estimates and physical chemical properties determined in laboratory experiments. There was good agreement between the measured and modeled D(5) concentrations. The results show that D(5) is clearly subject to long-range atmospheric transport, but that it is also effectively removed from the atmosphere via phototransformation. Atmospheric deposition has little influence on the atmospheric fate. The good agreement between the model predictions and the field observations indicates that there is a good understanding of the major factors governing D(5) concentrations in the atmosphere.

  16. Effects of elevated CO2 on litter chemistry and subsequent invertebrate detritivore feeding responses.

    Directory of Open Access Journals (Sweden)

    Matthew W Dray

    Full Text Available Elevated atmospheric CO2 can change foliar tissue chemistry. This alters leaf litter palatability to macroinvertebrate detritivores with consequences for decomposition, nutrient turnover, and food-web structure. Currently there is no consensus on the link between CO2 enrichment, litter chemistry, and macroinvertebrate-mediated leaf decomposition. To identify any unifying mechanisms, we presented eight invertebrate species from aquatic and terrestrial ecosystems with litter from Alnus glutinosa (common alder or Betula pendula (silver birch trees propagated under ambient (380 ppm or elevated (ambient +200 ppm CO2 concentrations. Alder litter was largely unaffected by CO2 enrichment, but birch litter from leaves grown under elevated CO2 had reduced nitrogen concentrations and greater C/N ratios. Invertebrates were provided individually with either (i two litter discs, one of each CO2 treatment ('choice', or (ii one litter disc of each CO2 treatment alone ('no-choice'. Consumption was recorded. Only Odontocerum albicorne showed a feeding preference in the choice test, consuming more ambient- than elevated-CO2 birch litter. Species' responses to alder were highly idiosyncratic in the no-choice test: Gammarus pulex and O. albicorne consumed more elevated-CO2 than ambient-CO2 litter, indicating compensatory feeding, while Oniscus asellus consumed more of the ambient-CO2 litter. No species responded to CO2 treatment when fed birch litter. Overall, these results show how elevated atmospheric CO2 can alter litter chemistry, affecting invertebrate feeding behaviour in species-specific ways. The data highlight the need for greater species-level information when predicting changes to detrital processing-a key ecosystem function-under atmospheric change.

  17. Characterizing the Atmosphere of a Young Planet

    Science.gov (United States)

    Marley, Mark

    2016-01-01

    Since the discovery of the young, directly imaged planet 51 Eri b, its emergent spectrum has proved challenging to interpret. The initial discovery paper (Macintosh et al. 2015) interpreted the spectrum as indicative of a low mass (few Jupiter masses), effective temperature near 700 degrees Kelvin, and partial cloudiness. Subsequent observations in the K band, however, seem to invalidate the early models. In addition, newly improved photochemical data point to the likely presence of exotic haze species in the atmosphere. In my presentation I will explore the photochemistry of the atmosphere and discuss whether disequilibrium chemistry, hazes, clouds, or non-solar abundances of heavy elements may be responsible for the unusual spectrum of this planet. The implications for the interpretation of other young Jupiters in this mass and effective temperature range will also be considered.

  18. A new 2D climate model with chemistry and self consistent eddy-parameterization. The impact of airplane NO{sub x} on the chemistry of the atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Gepraegs, R.; Schmitz, G.; Peters, D. [Institut fuer Atmosphaerenphysik, Kuehlungsborn (Germany)

    1997-12-31

    A 2D version of the ECHAM T21 climate model has been developed. The new model includes an efficient spectral transport scheme with implicit diffusion. Furthermore, photodissociation and chemistry of the NCAR 2D model have been incorporated. A self consistent parametrization scheme is used for eddy heat- and momentum flux in the troposphere. It is based on the heat flux parametrization of Branscome and mixing-length formulation for quasi-geostrophic vorticity. Above 150 hPa the mixing-coefficient K{sub yy} is prescribed. Some of the model results are discussed, concerning especially the impact of aircraft NO{sub x} emission on the model chemistry. (author) 6 refs.

  19. A new 2D climate model with chemistry and self consistent eddy-parameterization. The impact of airplane NO{sub x} on the chemistry of the atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Gepraegs, R; Schmitz, G; Peters, D [Institut fuer Atmosphaerenphysik, Kuehlungsborn (Germany)

    1998-12-31

    A 2D version of the ECHAM T21 climate model has been developed. The new model includes an efficient spectral transport scheme with implicit diffusion. Furthermore, photodissociation and chemistry of the NCAR 2D model have been incorporated. A self consistent parametrization scheme is used for eddy heat- and momentum flux in the troposphere. It is based on the heat flux parametrization of Branscome and mixing-length formulation for quasi-geostrophic vorticity. Above 150 hPa the mixing-coefficient K{sub yy} is prescribed. Some of the model results are discussed, concerning especially the impact of aircraft NO{sub x} emission on the model chemistry. (author) 6 refs.

  20. Impact of acid atmosphere deposition on soils : field monitoring and aluminum chemistry

    NARCIS (Netherlands)

    Mulder, J.

    1988-01-01

    The effect of acid atmospheric deposition on concentrations and transfer of major solutes in acid, sandy soils was studied. Emphasis was given to mobilization and transport of potentially toxic aluminum. Data on solute concentrations and fluxes in meteoric water as well as soil solutions

  1. Industrial chemistry engineering

    International Nuclear Information System (INIS)

    1993-01-01

    This book on industrial chemistry engineering is divided in two parts. The first part deals with industrial chemistry, inorganic industrial chemistry, organic industrial chemistry, analytical chemistry and practical questions. The last parts explain the chemical industry, a unit parts and thermodynamics in chemical industry and reference. It reveals the test subjects for the industrial chemistry engineering with a written examination and practical skill.

  2. Advanced chemistry management system to optimize BWR chemistry control

    International Nuclear Information System (INIS)

    Maeda, K.; Nagasawa, K.

    2002-01-01

    BWR plant chemistry control has close relationships among nuclear safety, component reliability, radiation field management and fuel integrity. Advanced technology is required to improve chemistry control [1,3,6,7,10,11]. Toshiba has developed TACMAN (Toshiba Advanced Chemistry Management system) to support BWR chemistry control. The TACMAN has been developed as response to utilities' years of requirements to keep plant operation safety, reliability and cost benefit. The advanced technology built into the TACMAN allows utilities to make efficient chemistry control and to keep cost benefit. TACMAN is currently being used in response to the needs for tools those plant chemists and engineers could use to optimize and identify plant chemistry conditions continuously. If an incipient condition or anomaly is detected at early stage, root causes evaluation and immediate countermeasures can be provided. Especially, the expert system brings numerous and competitive advantages not only to improve plant chemistry reliability but also to standardize and systematize know-how, empirical knowledge and technologies in BWR chemistry This paper shows detail functions of TACMAN and practical results to evaluate actual plant. (authors)

  3. Evidence for a link between atmospheric thermonuclear detonations and nitric acid.

    Science.gov (United States)

    Holdsworth, G

    1986-12-11

    Suitably located glacier cores, obtained from high-altitude, low-temperature sites, can reveal detailed information about atmospheric air chemistry at sub-annual resolution 1 . Such data may provide input to climate-change models, the study of acid precipitation patterns and many other phenomena. Here I present data from an ice core which show that during the era of intense atmospheric thermonuclear weapons testing (ATWT) a significant part of the nitrate content in the snow was modulated by the intensity of the nuclear detonations. The fixation of nitrogen by nuclear fireballs leads to NO x gases in the atmosphere 2 and ultimately to nitric acid in precipitation. At certain concentrations, these gases and the associated aerosols may perturb the climate 3,4 .

  4. ACS experiment for atmospheric studies on "ExoMars-2016" Orbiter

    Science.gov (United States)

    Korablev, O. I.; Montmessin, F.; Fedorova, A. A.; Ignatiev, N. I.; Shakun, A. V.; Trokhimovskiy, A. V.; Grigoriev, A. V.; Anufreichik, K. A.; Kozlova, T. O.

    2015-12-01

    ACS is a set of spectrometers for atmospheric studies (Atmospheric Chemistry Suite). It is one of the Russian instruments for the Trace Gas Orbiter (TGO) of the Russian-European "ExoMars" program. The purpose of the experiment is to study the Martian atmosphere by means of two observations regimes: sensitive trace gases measurements in solar occultations and by monitoring the atmospheric state during nadir observations. The experiment will allow us to approach global problems of Mars research such as current volcanism, and the modern climate status and its evolution. Also, the experiment is intended to solve the mystery of methane presence in the Martian atmosphere. Spectrometers of the ACS set cover the spectral range from the near IR-range (0.7 μm) to the thermal IR-range (17 μm) with spectral resolution λ/Δλ reaching 50000. The ACS instrument consists of three independent IR spectrometers and an electronics module, all integrated in a single unit with common mechanical, electrical and thermal interfaces. The article gives an overview of scientific tasks and presents the concept of the experiment.

  5. Microbiology and atmospheric processes: chemical interactions of primary biological aerosols

    Directory of Open Access Journals (Sweden)

    L. Deguillaume

    2008-07-01

    Full Text Available This paper discusses the influence of primary biological aerosols (PBA on atmospheric chemistry and vice versa through microbiological and chemical properties and processes. Several studies have shown that PBA represent a significant fraction of air particulate matter and hence affect the microstructure and water uptake of aerosol particles. Moreover, airborne micro-organisms, namely fungal spores and bacteria, can transform chemical constituents of the atmosphere by metabolic activity. Recent studies have emphasized the viability of bacteria and metabolic degradation of organic substances in cloud water. On the other hand, the viability and metabolic activity of airborne micro-organisms depend strongly on physical and chemical atmospheric parameters such as temperature, pressure, radiation, pH value and nutrient concentrations. In spite of recent advances, however, our knowledge of the microbiological and chemical interactions of PBA in the atmosphere is rather limited. Further targeted investigations combining laboratory experiments, field measurements, and modelling studies will be required to characterize the chemical feedbacks, microbiological activities at the air/snow/water interface supplied to the atmosphere.

  6. Atmospheric Pressure Plasma Induced Sterilization and Chemical Neutralization

    Science.gov (United States)

    Garate, Eusebio; Evans, Kirk; Gornostaeva, Olga; Alexeff, Igor; Lock Kang, Weng; Wood, Thomas K.

    1998-11-01

    We are studying chemical neutralization and surface decontamination using atmospheric pressure plasma discharges. The plasma is produced by corona discharge from an array of pins and a ground plane. The array is constructed so that various gases, like argon or helium, can be flowed past the pins where the discharge is initiated. The pin array can be biased using either DC, AC or pulsed discharges. Results indicate that the atmospheric plasma is effective in sterilizing surfaces with biological contaminants like E-coli and bacillus subtilus cells. Exposure times of less than four minutes in an air plasma result in a decrease in live colony counts by six orders of magnitude. Greater exposure times result in a decrease of live colony counts of up to ten orders of magnitude. The atmospheric pressure discharge is also effective in decomposing organic phosphate compounds that are simulants for chemical warfare agents. Details of the decomposition chemistry, by-product formation, and electrical energy consumption of the system will be discussed.

  7. Photoionization of atmospheric gases studied by time-resolved terahertz spectroscopy

    Czech Academy of Sciences Publication Activity Database

    Mics, Zoltan; Kužel, Petr; Jungwirth, Pavel; Bradforth, S. E.

    2008-01-01

    Roč. 465, 1-3 (2008), s. 20-24 ISSN 0009-2614 R&D Projects: GA MŠk LC512; GA ČR(CZ) GA202/06/0286 Institutional research plan: CEZ:AV0Z10100520; CEZ:AV0Z40550506 Keywords : terahertz * pump -probe * atmospheric gases * photoionization * plasma Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.169, year: 2008

  8. Current organic chemistry

    National Research Council Canada - National Science Library

    1997-01-01

    Provides in depth reviews on current progress in the fields of asymmetric synthesis, organometallic chemistry, bioorganic chemistry, heterocyclic chemistry, natural product chemistry, and analytical...

  9. Aquatic Chemistry

    International Nuclear Information System (INIS)

    Kim, Dong Yeun; Kim, Oh Sik; Kim, Chang Guk; Park, Cheong Gil; Lee, Gwi Hyeon; Lee, Cheol Hui

    1987-07-01

    This book deals aquatic chemistry, which treats water and environment, chemical kinetics, chemical balance like dynamical characteristic, and thermodynamics, acid-base chemistry such as summary, definition, kinetics, and PH design for mixture of acid-base chemistry, complex chemistry with definition, and kinetics, precipitation and dissolution on summary, kinetics of precipitation and dissolution, and balance design oxidation and resolution with summary, balance of oxidation and resolution.

  10. Combinatorial chemistry

    DEFF Research Database (Denmark)

    Nielsen, John

    1994-01-01

    An overview of combinatorial chemistry is presented. Combinatorial chemistry, sometimes referred to as `irrational drug design,' involves the generation of molecular diversity. The resulting chemical library is then screened for biologically active compounds.......An overview of combinatorial chemistry is presented. Combinatorial chemistry, sometimes referred to as `irrational drug design,' involves the generation of molecular diversity. The resulting chemical library is then screened for biologically active compounds....

  11. Atmospheric chemistry

    Science.gov (United States)

    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...

  12. Forensic Chemistry

    Science.gov (United States)

    Bell, Suzanne

    2009-07-01

    Forensic chemistry is unique among chemical sciences in that its research, practice, and presentation must meet the needs of both the scientific and the legal communities. As such, forensic chemistry research is applied and derivative by nature and design, and it emphasizes metrology (the science of measurement) and validation. Forensic chemistry has moved away from its analytical roots and is incorporating a broader spectrum of chemical sciences. Existing forensic practices are being revisited as the purview of forensic chemistry extends outward from drug analysis and toxicology into such diverse areas as combustion chemistry, materials science, and pattern evidence.

  13. Environmental consequences of nuclear war (SCOPE 28), Vol. 1: Physical and atmospheric effects

    International Nuclear Information System (INIS)

    Pittock, A.B.; Ackerman, T.P.; Crutzen, P.J.; MacCracken, M.C.; Shapiro, C.S.; Turco, R.P.

    1986-01-01

    This book presents an interdisciplinary look at current scientific knowledge of the possible environmental consequences of a nuclear war. The authors assess the likely magnitude of changes in sunlight, temperature, precipitation, atmospheric chemistry, and more. Volume One reviews existing nuclear arsenals, war scenarios, immediate and subsequent effects

  14. The Brazilian medicinal chemistry from 1998 to 2008 in the Journal of Medicinal Chemistry, Bioorganic and Medicinal Chemistry, Bioorganic and Medicinal Chemistry Letters and European Journal of Medicinal Chemistry [A química medicinal brasileira de 1998 a 2008 nos periódicos Journal of Medicinal Chemistry, Bioorganic and Medicinal Chemistry, Bioorganic and Medicinal Chemistry Letters e European Journal of Medicinal Chemistry

    OpenAIRE

    Bárbara Vasconcellos da Silva; Renato Saldanha Bastos; Angelo da Cunha Pinto

    2009-01-01

    In this article we present the Brazilian publications, the research groups involved, the contributions per states and the main diseases studied from 1998 to 2008 in the following periodicals: Journal of Medicinal Chemistry, Bioorganic and Medicinal Chemistry, Bioorganic and Medicinal Chemistry Letters and European Journal of Medicinal Chemistry.

  15. Modeling UTLS water vapor: Transport/Chemistry interactions

    International Nuclear Information System (INIS)

    Gulstad, Line

    2005-01-01

    This thesis was initially meant to be a study on the impact on chemistry and climate from UTLS water vapor. However, the complexity of the UTLS water vapor and its recent changes turned out to be a challenge by it self. In the light of this, the overall motivation for the thesis became to study the processes controlling UTLS water vapor and its changes. Water vapor is the most important greenhouse gas, involved in important climate feedback loops. Thus, a good understanding of the chemical and dynamical behavior of water vapor in the atmosphere is crucial for understanding the climate changes in the last century. Additionally, parts of the work was motivated by the development of a coupled climate chemistry model based on the CAM3 model coupled with the Chemical Transport Model Oslo CTM2. The future work will be concentrated on the UTLS water vapor impact on chemistry and climate. We are currently studying long term trends in UTLS water vapor, focusing on identification of the different processes involved in the determination of such trends. The study is based on natural as well as anthropogenic climate forcings. The ongoing work on the development of a coupled climate chemistry model will continue within our group, in collaboration with Prof. Wei-Chyung Wang at the State University of New York, Albany. Valuable contacts with observational groups are established during the work on this thesis. These collaborations will be continued focusing on continuous model validation, as well as identification of trends and new features in UTLS water vapor, and other tracers in this region. (Author)

  16. Russian contribution to ExoMars Trace Gas Orbiter: Atmospheric Chemistry Suite (ACS)

    Science.gov (United States)

    Shakun, Alexey; Korablev, Oleg; Trokhimovskiy, Alexander; Grigoriev, Alexey; Anufreychik, Konstantin; Fedorova, Anna; Ignatiev, Nikolay; Ivanov, Yuriy; Moshkin, Boris; Kalinnikov, Yuriy; Montmessin, Franck

    2016-04-01

    Atmospheric Chemistry Suite (ACS) is a part of science payload of Trace Gas Orbiter (TGO), ExoMars mission. This project developed by European Space Agency (ESA) in collaboration with Russian Space Agency (Roscosmos). Russian contribution to ExoMars TGO is the Proton rocket and two science instruments ACS (three infrared spectrometers) and FREND (neutron detector). ACS consists of three infrared spectrometers (ACS/NIR, ACS/MIR and ACS/TIRVIM) capable to take spectral measurements from near to thermal infrared range simultaneously or separately. Spectrometric channels of ACS share common mechanical, electrical, and thermal interfaces. Electronic box (ACS/BE) provides to spectrometric channels power and data transfer interfaces. SpaceWire link is used for science data transfer and MIL-1553 link - for commanding and housekeeping data transfer. The NIR channel is an echelle spectrometer with acousto-optic tunable filter (AOTF) for the selection of diffraction orders. ACS NIR is capable to perform nadir and occultation observations. NIR covers the spectral range of 0.7-1.7 μm with resolving power of ~25000. NIR will perform unique for TGO instruments nightglow science (searching for O2, OH, NO nightglow emissions on Mars). From the 1.38 μm band NIR will do water vapour mapping in nadir and H2O vertical profiling in solar occultations. High resolution NIR measurements of 1.27 μm O2(a1Δg) dayglow will supply indirect ozone observations on the dayside on nadir. In solar occultation mode, the O2 vertical profiles will be measured from the surface (in case of low dust activity) to the 40 km altitude based on 0.76 μm absorption band. Together with MIR channel in solar occultation NIR will support the measurements of CO2 density profiles (based on 1.43 μm band) and aerosols characterization from 0.7 to 4 μm. The wide spectral range will allow not just determine aerosol particle sizes and density at different altitudes, but also distinguish between dust and ice particles

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  18. Study of the atmospheric chemistry of radon progeny in laboratory and real indoor atmospheres

    Energy Technology Data Exchange (ETDEWEB)

    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.

  19. Cloud processing of gases and aerosols in the Community Multiscale Air Quality (CMAQ) model: Impacts of extended chemistry

    Science.gov (United States)

    Clouds and fogs can significantly impact the concentration and distribution of atmospheric gases and aerosols through chemistry, scavenging, and transport. This presentation summarizes the representation of cloud processes in the Community Multiscale Air Quality (CMAQ) modeling ...

  20. Application of a coupled ecosystem-chemical equilibrium model, DayCent-Chem, to stream and soil chemistry in a Rocky Mountain watershed

    Science.gov (United States)

    Hartman, M.D.; Baron, Jill S.; Ojima, D.S.

    2007-01-01

    Atmospheric deposition of sulfur and nitrogen species have the potential to acidify terrestrial and aquatic ecosystems, but nitrate and ammonium are also critical nutrients for plant and microbial productivity. Both the ecological response and the hydrochemical response to atmospheric deposition are of interest to regulatory and land management agencies. We developed a non-spatial biogeochemical model to simulate soil and surface water chemistry by linking the daily version of the CENTURY ecosystem model (DayCent) with a low temperature aqueous geochemical model, PHREEQC. The coupled model, DayCent-Chem, simulates the daily dynamics of plant production, soil organic matter, cation exchange, mineral weathering, elution, stream discharge, and solute concentrations in soil water and stream flow. By aerially weighting the contributions of separate bedrock/talus and tundra simulations, the model was able to replicate the measured seasonal and annual stream chemistry for most solutes for Andrews Creek in Loch Vale watershed, Rocky Mountain National Park. Simulated soil chemistry, net primary production, live biomass, and soil organic matter for forest and tundra matched well with measurements. This model is appropriate for accurately describing ecosystem and surface water chemical response to atmospheric deposition and climate change. ?? 2006 Elsevier B.V. All rights reserved.

  1. Direct observations of reactive atmospheric gases at ZOTTO station in the middle of Siberia as a base for large-scale modeling of atmospheric chemistry over Northern Eurasia

    Science.gov (United States)

    Skorokhod, Andrey; Belikov, Igor; Shtabkin, Yury; Moiseenko, Konstantin; Pankratova, Natalia; Vasileva, Anastasia; Rakitin, Vadim; Heimann, Martin

    2015-04-01

    Direct observations of atmospheric air composition are very important for a comprehensive understanding of atmospheric chemistry over Northern Eurasia and its variability and trends driven by abrupt climatic and ecosystem changes and anthropogenic pressure. Atmospheric air composition (including greenhouse gases and aerosols), its trends and variability is still insufficiently known for most of the nearly uninhabited areas of Northern Eurasia. This limits the accuracy of both global and regional models, which simulate climatological and ecosystem changes in this highly important region. From that point of view, the Zotino Tall Tower Observatory (ZOTTO) in the middle of Siberia (near 60N, 90E), launched in 2006 and governed by a scientific international consortium plays an important role providing unique information about concentrations of greenhouse and reactive trace gases, as well as aerosols. Simulations of surface concentrations of O3, NOx and CO performed by global chemical-transport model GEOS-Chem using up-to-date anthropogenic and biogenic emissions databases show very good agreement with values observed at ZOTTO in 2007-2012. Observed concentration of ozone has a pronounced seasonal variation with a clear peak in spring (40-45 ppbv in average and up to 80 ppbv in extreme cases) and minimum in winter. Average ozone level is about 20 ppbv that corresponds to the background conditions. Enhanced concentration in March-July is due to increased stratospheric-tropospheric exchange. In autumn and winter distribution of ozone is close to uniform. NOx concentration does not exceed 1 ppb that is typical for background areas but may vary by order and some more in few hours. Higher surface NOx(=NO+NO2) concentrations during day time generally correspond to higher ozone when NO/NO2 ratio indicates on clean or slightly polluted conditions. CO surface concentration has a vivid seasonal course and varies from about 100 ppb in summer till 150 ppb in winter. But during

  2. BARTTest: Community-Standard Atmospheric Radiative-Transfer and Retrieval Tests

    Science.gov (United States)

    Harrington, Joseph; Himes, Michael D.; Cubillos, Patricio E.; Blecic, Jasmina; Challener, Ryan C.

    2018-01-01

    Atmospheric radiative transfer (RT) codes are used both to predict planetary and brown-dwarf spectra and in retrieval algorithms to infer atmospheric chemistry, clouds, and thermal structure from observations. Observational plans, theoretical models, and scientific results depend on the correctness of these calculations. Yet, the calculations are complex and the codes implementing them are often written without modern software-verification techniques. The community needs a suite of test calculations with analytically, numerically, or at least community-verified results. We therefore present the Bayesian Atmospheric Radiative Transfer Test Suite, or BARTTest. BARTTest has four categories of tests: analytically verified RT tests of simple atmospheres (single line in single layer, line blends, saturation, isothermal, multiple line-list combination, etc.), community-verified RT tests of complex atmospheres, synthetic retrieval tests on simulated data with known answers, and community-verified real-data retrieval tests.BARTTest is open-source software intended for community use and further development. It is available at https://github.com/ExOSPORTS/BARTTest. We propose this test suite as a standard for verifying atmospheric RT and retrieval codes, analogous to the Held-Suarez test for general circulation models. This work was supported by NASA Planetary Atmospheres grant NX12AI69G, NASA Astrophysics Data Analysis Program grant NNX13AF38G, and NASA Exoplanets Research Program grant NNX17AB62G.

  3. Bad chemistry

    OpenAIRE

    Petsko, Gregory A

    2004-01-01

    General chemistry courses haven't changed significantly in forty years. Because most basic chemistry students are premedical students, medical schools have enormous influence and could help us start all over again to create undergraduate chemistry education that works.

  4. Model analyses of atmospheric mercury: present air quality and effects of transpacific transport on the United States

    Science.gov (United States)

    Lei, H.; Liang, X.-Z.; Wuebbles, D. J.; Tao, Z.

    2013-11-01

    Atmospheric mercury is a toxic air and water pollutant that is of significant concern because of its effects on human health and ecosystems. A mechanistic representation of the atmospheric mercury cycle is developed for the state-of-the-art global climate-chemistry model, CAM-Chem (Community Atmospheric Model with Chemistry). The model simulates the emission, transport, transformation and deposition of atmospheric mercury (Hg) in three forms: elemental mercury (Hg(0)), reactive mercury (Hg(II)), and particulate mercury (PHg). Emissions of mercury include those from human, land, ocean, biomass burning and volcano related sources. Land emissions are calculated based on surface solar radiation flux and skin temperature. A simplified air-sea mercury exchange scheme is used to calculate emissions from the oceans. The chemistry mechanism includes the oxidation of Hg(0) in gaseous phase by ozone with temperature dependence, OH, H2O2 and chlorine. Aqueous chemistry includes both oxidation and reduction of Hg(0). Transport and deposition of mercury species are calculated through adapting the original formulations in CAM-Chem. The CAM-Chem model with mercury is driven by present meteorology to simulate the present mercury air quality during the 1999-2001 period. The resulting surface concentrations of total gaseous mercury (TGM) are then compared with the observations from worldwide sites. Simulated wet depositions of mercury over the continental United States are compared to the observations from 26 Mercury Deposition Network stations to test the wet deposition simulations. The evaluations of gaseous concentrations and wet deposition confirm a strong capability for the CAM-Chem mercury mechanism to simulate the atmospheric mercury cycle. The general reproduction of global TGM concentrations and the overestimation on South Africa indicate that model simulations of TGM are seriously affected by emissions. The comparison to wet deposition indicates that wet deposition patterns

  5. Chemistry and sustainable environment (abstract)

    International Nuclear Information System (INIS)

    Hussain, M.

    2011-01-01

    Chemistry is one of the oldest branches of science; the human beings had ever come across. It has consistently contributed towards meeting the human needs from the dawn of civilization. However, its role has multiplied since the inception of industrial revolution. Although anthropogenic activities have made the human life comfortable and even luxurious yet their impacts on the physical, biological and socio-economic environments had been destructive. Numerous kinds of chemicals have engulfed us and our environment. Modern chemistry has leading role in sculpting the present as well as future of human lifestyle. It is serving the man and other biodiversity by providing countless products in every sphere of life. At the same time it is playing villain role in the destruction of environment at an alarming rate. Today the world is confronted with heinous environmental issues hitherto unknown to the living beings mostly triggered by chemicals. Thousands of chemicals are used in industrial products, agricultural chemicals, persistent organic pollutants, freezers, pharmaceuticals, chemical and radiological warfare, construction industry, synthetic materials, electrical goods, medical gadgets etc. Some natural sources of chemicals are acid rains, volcanic eruptions, eutrophication and photochemical smog. The fact of matter is that chemicals are being consistently added into atmosphere, biosphere and lithosphere. For the sustainable environment it is imperative that the chemicals must not be added into human environment beyond its carrying capacity. It is responsibility of chemists to introduce environmentally benign and biodegradable chemicals. All types of chemistry need to be green and environment friendly. The scientists and engineers should develop chemicals and technologies which do not harm the living creatures during any stage of their life-cycle. (author)

  6. Modeling the global atmospheric transport and deposition of mercury to the Great Lakes

    Directory of Open Access Journals (Sweden)

    Mark D. Cohen

    2016-07-01

    Full Text Available Abstract Mercury contamination in the Great Lakes continues to have important public health and wildlife ecotoxicology impacts, and atmospheric deposition is a significant ongoing loading pathway. The objective of this study was to estimate the amount and source-attribution for atmospheric mercury deposition to each lake, information needed to prioritize amelioration efforts. A new global, Eulerian version of the HYSPLIT-Hg model was used to simulate the 2005 global atmospheric transport and deposition of mercury to the Great Lakes. In addition to the base case, 10 alternative model configurations were used to examine sensitivity to uncertainties in atmospheric mercury chemistry and surface exchange. A novel atmospheric lifetime analysis was used to characterize fate and transport processes within the model. Model-estimated wet deposition and atmospheric concentrations of gaseous elemental mercury (Hg(0 were generally within ∼10% of measurements in the Great Lakes region. The model overestimated non-Hg(0 concentrations by a factor of 2–3, similar to other modeling studies. Potential reasons for this disagreement include model inaccuracies, differences in atmospheric Hg fractions being compared, and the measurements being biased low. Lake Erie, downwind of significant local/regional emissions sources, was estimated by the model to be the most impacted by direct anthropogenic emissions (58% of the base case total deposition, while Lake Superior, with the fewest upwind local/regional sources, was the least impacted (27%. The U.S. was the largest national contributor, followed by China, contributing 25% and 6%, respectively, on average, for the Great Lakes. The contribution of U.S. direct anthropogenic emissions to total mercury deposition varied between 46% for the base case (with a range of 24–51% over all model configurations for Lake Erie and 11% (range 6–13% for Lake Superior. These results illustrate the importance of atmospheric

  7. Learning Chemistry by ICT (Virtual Animation at Maumere High School, East Nusa Tenggara

    Directory of Open Access Journals (Sweden)

    Yusnidar Yusuf

    2017-03-01

    Full Text Available This research was aimed to create attractive learning atmosphere which can make students excited inside theclass.Education was a right for every nation. It had to be given to improving a nation. Chemistry subject, especially in hydrocarbon chapter, was less-favorable by most students due to its difficulty level. Learning outcomes score were low. Many research showed that various method, strategy or another approach in teaching chemistry subject had significantlyimproved towards learning theoutcome of students.  One of the approaches was by virtual animation as part of ICT. Based on data result analysis from this research, there was 0,000 < α = 0.05 significance. As result, H0 was rejected. Itmeans that there was significant improve learning outcome using multimedia animation. The role of ICT as learning model should be utilised for granted by teachers to enriched chemistry science in school’s scope.

  8. Positronium chemistry

    CERN Document Server

    Green, James

    1964-01-01

    Positronium Chemistry focuses on the methodologies, reactions, processes, and transformations involved in positronium chemistry. The publication first offers information on positrons and positronium and experimental methods, including mesonic atoms, angular correlation measurements, annihilation spectra, and statistical errors in delayed coincidence measurements. The text then ponders on positrons in gases and solids. The manuscript takes a look at the theoretical chemistry of positronium and positronium chemistry in gases. Topics include quenching, annihilation spectrum, delayed coincidence

  9. Adsorption of polycyclic aromatic hydrocarbons at the air-water interface: Molecular dynamics simulations and experimental atmospheric observations

    Czech Academy of Sciences Publication Activity Database

    Vácha, Robert; Jungwirth, Pavel; Chen, J.; Valsaraj, K.

    2006-01-01

    Roč. 8, č. 38 (2006), s. 4461-4467 ISSN 1463-9076 R&D Projects: GA MŠk(CZ) LC512; GA MŠk(CZ) ME 644 Grant - others:NSF(US) CHE0431312; NSF(US) CHE0209719; NSF(US) ATM-0355291 Institutional research plan: CEZ:AV0Z40550506 Keywords : polycyclic aromatic hydrocarbons * water surface * molecular dynamics simulations * heterogeneous atmospheric chemistry Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.892, year: 2006

  10. Non-thermally activated chemistry

    International Nuclear Information System (INIS)

    Stiller, W.

    1987-01-01

    The subject is covered under the following headings: state-of-the art of non-thermally activated chemical processes; basic phenomena in non-thermal chemistry including mechanochemistry, photochemistry, laser chemistry, electrochemistry, photo-electro chemistry, high-field chemistry, magneto chemistry, plasma chemistry, radiation chemistry, hot-atom chemistry, and positronium and muonium chemistry; elementary processes in non-thermal chemistry including nuclear chemistry, interactions of electromagnetic radiations, electrons and heavy particles with matter, ionic elementary processes, elementary processes with excited species, radicalic elementary processes, and energy-induced elementary processes on surfaces and interfaces; and comparative considerations. An appendix with historical data and a subject index is given. 44 figs., 41 tabs., and 544 refs

  11. Evidence of water vapor in excess of saturation in the atmosphere of Mars.

    Science.gov (United States)

    Maltagliati, L; Montmessin, F; Fedorova, A; Korablev, O; Forget, F; Bertaux, J-L

    2011-09-30

    The vertical distribution of water vapor is key to the study of Mars' hydrological cycle. To date, it has been explored mainly through global climate models because of a lack of direct measurements. However, these models assume the absence of supersaturation in the atmosphere of Mars. Here, we report observations made using the SPICAM (Spectroscopy for the Investigation of the Characteristics of the Atmosphere of Mars) instrument onboard Mars Express that provide evidence of the frequent presence of water vapor in excess of saturation, by an amount far surpassing that encountered in Earth's atmosphere. This result contradicts the widespread assumption that atmospheric water on Mars cannot exist in a supersaturated state, directly affecting our long-term representation of water transport, accumulation, escape, and chemistry on a global scale.

  12. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    Science.gov (United States)

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-06

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

  13. Impact of isoprene and nitrogen oxides on O3 chemistry at the local and the regional scale : the ESCOMPTE experiment

    Science.gov (United States)

    Cortinovis, J.; Solmon, F.; Personne, E.; Serça, D.; Rosset, R.

    2003-04-01

    Concentrations of nitrogen oxides (NOx = NO+NO2) and volatile organic compounds (VOCs) play a crucial role in the atmospheric chemistry through the production-destruction of tropospheric O3. In rural areas, NOx concentrations are much lower than in urban areas, whereas VOCs emissions can be relatively high. This is due to a relative longer residence time of VOCs, and to the substantial contribution of Biogenic VOCs (BVOCs) representing more than 85% of all the VOCs emitted at the Earth surface (half of it being isoprene). For these reasons, O3 production in rural areas is most of the time NOx-limited. Taking into account biogenic emissions of isoprene in global scale atmospheric chemistry modeling adds from 10 to 40% to the ozone produced when compared to the same simulation without isoprene. This suggests that BVOCs and NOx emissions must be accounted for in models of atmospheric pollution forecasting at local and regional scales. In this study, we present a sensitivity analysis on the impact of the isoprene and nitrogen oxides emissions at the local and the regional scale. This study is done from data collected during the ESCOMPTE campaign which took place in June and July 2001 in the Marseille region (Southwest France) characterized by both strong natural and anthropogenic sources of trace gases. Isoprene emission experimental data from a Quercus Pubescens Mediterranean forest are used to constrain the 1Dz Soil-Vegetation-Atmospheric-Transfer ISBA model. This SVAT is used in the 3D MESO-NH-Chemistry model to simulate scenarios of pollution at the regional scale including the measured biogenic source for isoprene, and GENEMIS anthropogenic sources for other trace gases. To focus on the chemistry aspect of these simulations, the atmospheric dynamics are set to an "ideal" configuration. We have investigated the impact of the relative position and distance between the biogenic and anthropogenic sources on the O3 budget. According to this, and to the intensity of the

  14. Forcing of stratospheric chemistry and dynamics during the Dalton Minimum

    Science.gov (United States)

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

    2013-11-01

    The response of atmospheric chemistry and dynamics to volcanic eruptions and to a decrease in solar activity during the Dalton Minimum is investigated with the fully coupled atmosphere-ocean chemistry general circulation model SOCOL-MPIOM (modeling tools for studies of SOlar Climate Ozone Links-Max Planck Institute Ocean Model) covering the time period 1780 to 1840 AD. We carried out several sensitivity ensemble experiments to separate the effects of (i) reduced solar ultra-violet (UV) irradiance, (ii) reduced solar visible and near infrared irradiance, (iii) enhanced galactic cosmic ray intensity as well as less intensive solar energetic proton events and auroral electron precipitation, and (iv) volcanic aerosols. The introduced changes of UV irradiance and volcanic aerosols significantly influence stratospheric dynamics in the early 19th century, whereas changes in the visible part of the spectrum and energetic particles have smaller effects. A reduction of UV irradiance by 15%, which represents the presently discussed highest estimate of UV irradiance change caused by solar activity changes, causes global ozone decrease below the stratopause reaching as much as 8% in the midlatitudes at 5 hPa and a significant stratospheric cooling of up to 2 °C in the mid-stratosphere and to 6 °C in the lower mesosphere. Changes in energetic particle precipitation lead only to minor changes in the yearly averaged temperature fields in the stratosphere. Volcanic aerosols heat the tropical lower stratosphere, allowing more water vapour to enter the tropical stratosphere, which, via HOx reactions, decreases upper stratospheric and mesospheric ozone by roughly 4%. Conversely, heterogeneous chemistry on aerosols reduces stratospheric NOx, leading to a 12% ozone increase in the tropics, whereas a decrease in ozone of up to 5% is found over Antarctica in boreal winter. The linear superposition of the different contributions is not equivalent to the response obtained in a simulation

  15. Modelling Chemical Patterns of Atmospheric Polycyclic Aromatic Hydrocarbons (PAHs) in the Iberian Peninsula

    Science.gov (United States)

    Ratola, Nuno; Jiménez-Guerrero, Pedro

    2013-04-01

    Semi-volatile organic compounds (SVOCs) such as PBDEs, PCBs, organochlorine pesticides (OCPs) or PAHs, are widespread and generated in a multitude of anthropogenic (and natural for PAHs) processes and although they are found in the environment at low concentrations, possess an extraordinary carcinogenic capacity (Baussant et al., 2001) and high ecotoxicity due to their persistence in different matrices (air, soil, water, living organisms). In particular, PAHs are originated by combustion processes or release from fossil fuels and can be transported in the atmosphere over long distances in gaseous or particulate matter (Baek et al., 1991). The establishment of strategies for sampling and chemical transport modelling of SVOCs in the atmosphere aiming the definition and validation of the spatial, temporal and chemical transport patterns of contaminants can be achieved by an integrated system of third-generation models that represent the current state of knowledge in air quality modelling and experimental data collected in field campaigns. This has implications in the fields of meteorology, atmospheric chemistry and even climate change. In this case, an extensive database already obtained on levels of atmospheric PAHs from biomonitoring schemes in the Iberian Peninsula fuelled the establishment of the first models of behaviour for PAHs. The modelling system WRF+CHIMERE was implemented with high spatial and temporal resolution to the Iberian Peninsula in this first task (9 km for the Iberian Peninsula, 3 km to Portugal, 1 hour), using PAHs atmospheric levels collected over a year-long sampling scheme comprising 4 campaigns (one per season) in over 30 sites. Daily information on meteorological parameters such as air temperature, humidity, rainfall or wind speed and direction was collected from the weather stations closest to the sampling sites. Diagnosis and forecasts of these meteorological variables using MM5 or WRF were used to feed a chemistry transport model

  16. Laser-pulsed Plasma Chemistry: Laser-initiated Plasma Oxidation Of Niobium

    OpenAIRE

    Marks R.F.; Pollak R.A.; Avouris Ph.; Lin C.T.; Thefaine Y.J.

    1983-01-01

    We report the first observation of the chemical modification of a solid surface exposed to an ambient gas plasma initiated by the interaction of laser radiation with the same surface. A new technique, which we designate laser-pulsed plasma chemistry (LPPC), is proposed for activating heterogeneous chemical reactions at solid surfaces in a gaseous ambient by means of a plasma initiated by laser radiation. Results for niobium metal in one atmosphere oxygen demonstrate single-pulse, self-limitin...

  17. Online-coupled meteorology and chemistry models: history, current status, and outlook

    Directory of Open Access Journals (Sweden)

    Y. Zhang

    2008-06-01

    Full Text Available The climate-chemistry-aerosol-cloud-radiation feedbacks are important processes occurring in the atmosphere. Accurately simulating those feedbacks requires fully-coupled meteorology, climate, and chemistry models and presents significant challenges in terms of both scientific understanding and computational demand. This paper reviews the history and current status of the development and application of online-coupled meteorology and chemistry models, with a focus on five representative models developed in the US including GATOR-GCMOM, WRF/Chem, CAM3, MIRAGE, and Caltech unified GCM. These models represent the current status and/or the state-of-the science treatments of online-coupled models worldwide. Their major model features, typical applications, and physical/chemical treatments are compared with a focus on model treatments of aerosol and cloud microphysics and aerosol-cloud interactions. Aerosol feedbacks to planetary boundary layer meteorology and aerosol indirect effects are illustrated with case studies for some of these models. Future research needs for model development, improvement, application, as well as major challenges for online-coupled models are discussed.

  18. The role of post accident chemistry data in nuclear safety

    International Nuclear Information System (INIS)

    Bradshaw, R.W.; Caruthers, G.F.

    1982-01-01

    The NRC instituted the NUREG-0737 requirements as implementation of the Post-TMI Action Plan in October, 1980. Among these requirements was the capability to obtain chemistry samples of the reactor coolant and containment building atmosphere under post accident conditions. The quantitative criteria were, in general, beyond the capabilities of existing plant systems. As a consequence the nuclear industry expended substantial efforts to design and install the post-accident sampling systems necessary to comply with these criteria. With such efforts essentially complete, the task remains to establish the role that data provided by these systems would play in mitigating the consequences of a nuclear plant accident. This role definition must include a characterization of the timing and priority for the post accident chemistry data. This paper defines that role using the Safety Level and Safety Function concepts as a matrix

  19. Turbidity, SOLAR RADIATION - ATMOSPHERIC and other data from unknown platforms in the TOGA Area - Pacific from 1992-11-10 to 1993-02-20 (NODC Accession 9600030)

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — The accession contains Ocean Station Chemistry data collected in TOGA Area - Pacific (30 N to 30 S) as part of Tropical Ocean Global Atmosphere (TOGA) and Coupled...

  20. Green chemistry: A tool in Pharmaceutical Chemistry

    OpenAIRE

    Smita Talaviya; Falguni Majumdar

    2012-01-01

    Green chemistry expresses an area of research developing from scientific discoveries about pollution awareness and it utilizes a set of principles that reduces or eliminates the use or generation of hazardous substances in all steps of particular synthesis or process. Chemists and medicinal scientists can greatly reduce the risk to human health and the environment by following all the valuable principles of green chemistry. The most simple and direct way to apply green chemistry in pharmaceut...