WorldWideScience

Sample records for impact atmospheric chemistry

  1. 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

  2. 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.

  3. 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.

  4. 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

  5. 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.

  6. 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

  7. 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...

  8. 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.

  9. 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

  10. 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

  11. Atmospheric Chemistry Over Southern Africa

    Science.gov (United States)

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

    2011-01-01

    campaigns such as Transport and Atmospheric Chemistry Near the Equator-Atlantic (TRACE-A), Southern African Fire-Atmosphere Research Initiative (SAFARI-92), and Southern African Regional Science Initiative (SAFARI 2000). Since those large international efforts, satellites have matured enough to enable quantifiable measurements of regional land surface, atmosphere, and ocean. In addition, global and chemical transport models have also been advanced to incorporate various data. Thus, the timing of the workshop was right for a full-fledged re-assessment of the chemistry, physics, and socio-economical impacts caused by pollution in the region, including a characterization of sources, deposition, and feedbacks with climate change.

  12. 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

  13. 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

    of marine aerosol production on the microphysical properties of aerosol populations and clouds over the ocean and the corresponding direct and indirect effects on radiative transfer; (2) atmospheric burdens of reactive halogen species and their impacts on O3, NOx, OH, DMS, and particulate non-sea-salt SO42-; and (3) the global production and influences of marine-derived particulate organic carbon. The model reproduced major characteristics of the marine aerosol system and demonstrated the potential sensitivity of global, decadal-scale climate metrics to multiphase marine-derived components of Earth's troposphere. Due to the combined computational burden of the coupled system, the currently available computational resources were the limiting factor preventing the adequate statistical analysis of the overall impact that multiphase chemistry might have on climate-scale radiative transfer and climate.

  14. 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.)

  15. 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.

  16. 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.

  17. 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

  18. 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

  19. 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

  20. 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.

  1. 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.

  2. (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.

  3. 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...

  4. 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.

  5. 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

  6. 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...

  7. 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...

  8. 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...

  9. 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.

  10. 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.

  11. 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.

  12. 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

  13. 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.

  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. 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.

  17. 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.

  18. 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

  19. 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.

  20. 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

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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

  7. 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.

  8. 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)

  9. 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.

  10. 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

  11. 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

  12. 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

  13. 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.

  14. 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.

  15. 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...

  16. 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

  17. 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

  18. 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.)

  19. 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.

  20. Atmosphere Impact Losses

    Science.gov (United States)

    Schlichting, Hilke E.; Mukhopadhyay, Sujoy

    2018-02-01

    Determining the origin of volatiles on terrestrial planets and quantifying atmospheric loss during planet formation is crucial for understanding the history and evolution of planetary atmospheres. Using geochemical observations of noble gases and major volatiles we determine what the present day inventory of volatiles tells us about the sources, the accretion process and the early differentiation of the Earth. We further quantify the key volatile loss mechanisms and the atmospheric loss history during Earth's formation. Volatiles were accreted throughout the Earth's formation, but Earth's early accretion history was volatile poor. Although nebular Ne and possible H in the deep mantle might be a fingerprint of this early accretion, most of the mantle does not remember this signature implying that volatile loss occurred during accretion. Present day geochemistry of volatiles shows no evidence of hydrodynamic escape as the isotopic compositions of most volatiles are chondritic. This suggests that atmospheric loss generated by impacts played a major role during Earth's formation. While many of the volatiles have chondritic isotopic ratios, their relative abundances are certainly not chondritic again suggesting volatile loss tied to impacts. Geochemical evidence of atmospheric loss comes from the {}3He/{}^{22}Ne, halogen ratios (e.g., F/Cl) and low H/N ratios. In addition, the geochemical ratios indicate that most of the water could have been delivered prior to the Moon forming impact and that the Moon forming impact did not drive off the ocean. Given the importance of impacts in determining the volatile budget of the Earth we examine the contributions to atmospheric loss from both small and large impacts. We find that atmospheric mass loss due to impacts can be characterized into three different regimes: 1) Giant Impacts, that create a strong shock transversing the whole planet and that can lead to atmospheric loss globally. 2) Large enough impactors (m_{cap} ≳ √{2

  1. 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.

  2. 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.

  3. 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.

  4. 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...

  5. 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.

  6. 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

  7. 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.

  8. 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.

  9. 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...

  10. 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

  11. 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.

  12. 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

  13. 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)

  14. Impacts of Atmosphere-Ocean Coupling on Southern Hemisphere Climate Change

    Science.gov (United States)

    Li, Feng; Newman, Paul; Pawson, Steven

    2013-01-01

    Climate in the Southern Hemisphere (SH) has undergone significant changes in recent decades. These changes are closely linked to the shift of the Southern Annular Mode (SAM) towards its positive polarity, which is driven primarily by Antarctic ozone depletion. There is growing evidence that Antarctic ozone depletion has significant impacts on Southern Ocean circulation change. However, it is poorly understood whether and how ocean feedback might impact the SAM and climate change in the SH atmosphere. This outstanding science question is investigated using the Goddard Earth Observing System Coupled Atmosphere-Ocean-Chemistry Climate Model(GEOS-AOCCM).We perform ensemble simulations of the recent past (1960-2010) with and without the interactive ocean. For simulations without the interactive ocean, we use sea surface temperatures and sea ice concentrations produced by the interactive ocean simulations. The differences between these two ensemble simulations quantify the effects of atmosphere-ocean coupling. We will investigate the impacts of atmosphere-ocean coupling on stratospheric processes such as Antarctic ozone depletion and Antarctic polar vortex breakup. We will address whether ocean feedback affects Rossby wave generation in the troposphere and wave propagation into the stratosphere. Another focuson this study is to assess how ocean feedback might affect the tropospheric SAM response to Antarctic ozone depletion

  15. 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.

  16. 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.

  17. 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

  18. 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.

  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. 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)

  1. 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...

  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. 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

  4. 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.

  5. Future changes of the atmospheric composition and the impact of climate change

    Energy Technology Data Exchange (ETDEWEB)

    Grewe, V.; Dameris, M.; Hein, R.; Sausen, R. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Steil, B. [Max-Planck-Institut fuer Chemie (Otto-Hahn-Institut), Mainz (Germany). Abt. Chemie der Atmosphaere

    1999-05-01

    The development of the future atmospheric chemical composition, with respect of NO{sub y} and O{sub 3} is investigated by means of the off-line coupled dynamic-chemical general circulation model ECHAM3/CHEM. Two time slice experiments have been performed for the years 1992 and 2015, which include changes in sea surface temperatures, greenhouse gas concentrations, emissions of CFCs, NO{sub x} and other species, i.e., the 2015 simulation accounts for changes in chemically relevant emissions and for a climate change and its impact on air chemistry. The 2015 simulation clearly shows a global increase in ozone except for large areas of the lower stratosphere, where no significant changes or even decreases in the ozone concentration are found. For a better understanding of the importance of (A) emissions like NO{sub x} and CFCs, (B) future changes of air temperature and water vapour concentration, and (C) other dynamic parameters, like precipitation and changes in the circulation, i.e. wind speed, diabatic circulation, stratosphere-troposphere-exchange, the simulation of the future atmosphere has been performed stepwise. This method requires a climate-chemistry model without interactive coupling of chemical species. Model results show that the direct effect of emissions (A) plays a major role for the composition of the future atmosphere, but they also clearly show that climate change has a significant impact and strongly reduces the NO{sub y} and ozone concentration in the lower stratosphere. (orig.)

  6. Impacts of bromine and iodine chemistry on tropospheric OH and HO2: comparing observations with box and global model perspectives

    Science.gov (United States)

    Stone, Daniel; Sherwen, Tomás; Evans, Mathew J.; Vaughan, Stewart; Ingham, Trevor; Whalley, Lisa K.; Edwards, Peter M.; Read, Katie A.; Lee, James D.; Moller, Sarah J.; Carpenter, Lucy J.; Lewis, Alastair C.; Heard, Dwayne E.

    2018-03-01

    The chemistry of the halogen species bromine and iodine has a range of impacts on tropospheric composition, and can affect oxidising capacity in a number of ways. However, recent studies disagree on the overall sign of the impacts of halogens on the oxidising capacity of the troposphere. We present simulations of OH and HO2 radicals for comparison with observations made in the remote tropical ocean boundary layer during the Seasonal Oxidant Study at the Cape Verde Atmospheric Observatory in 2009. We use both a constrained box model, using detailed chemistry derived from the Master Chemical Mechanism (v3.2), and the three-dimensional global chemistry transport model GEOS-Chem. Both model approaches reproduce the diurnal trends in OH and HO2. Absolute observed concentrations are well reproduced by the box model but are overpredicted by the global model, potentially owing to incomplete consideration of oceanic sourced radical sinks. The two models, however, differ in the impacts of halogen chemistry. In the box model, halogen chemistry acts to increase OH concentrations (by 9.8 % at midday at the Cape Verde Atmospheric Observatory), while the global model exhibits a small increase in OH at the Cape Verde Atmospheric Observatory (by 0.6 % at midday) but overall shows a decrease in the global annual mass-weighted mean OH of 4.5 %. These differences reflect the variety of timescales through which the halogens impact the chemical system. On short timescales, photolysis of HOBr and HOI, produced by reactions of HO2 with BrO and IO, respectively, increases the OH concentration. On longer timescales, halogen-catalysed ozone destruction cycles lead to lower primary production of OH radicals through ozone photolysis, and thus to lower OH concentrations. The global model includes more of the longer timescale responses than the constrained box model, and overall the global impact of the longer timescale response (reduced primary production due to lower O3 concentrations

  7. 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.

  8. 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.

  9. 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

  10. Process analysis of the modelled 3-D mesoscale impact of aircraft emissions on the atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Hendricks, J; Ebel, A; Lippert, E; Petry, H [Koeln Univ. (Germany). Inst. fuer Geophysik und Meterorologie

    1998-12-31

    A mesoscale chemistry transport model is applied to study the impact of aircraft emissions on the atmospheric trace gas composition. A special analysis of the simulations is conducted to separate the effects of chemistry, transport, diffusion and cloud processes on the transformation of the exhausts of a subsonic fleet cruising over the North Atlantic. The aircraft induced ozone production strongly depends on the tropopause height and the cruise altitude. Aircraft emissions may undergo an effective downward transport under the influence of stratosphere-troposphere exchange activity. (author) 12 refs.

  11. Process analysis of the modelled 3-D mesoscale impact of aircraft emissions on the atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Hendricks, J.; Ebel, A.; Lippert, E.; Petry, H. [Koeln Univ. (Germany). Inst. fuer Geophysik und Meterorologie

    1997-12-31

    A mesoscale chemistry transport model is applied to study the impact of aircraft emissions on the atmospheric trace gas composition. A special analysis of the simulations is conducted to separate the effects of chemistry, transport, diffusion and cloud processes on the transformation of the exhausts of a subsonic fleet cruising over the North Atlantic. The aircraft induced ozone production strongly depends on the tropopause height and the cruise altitude. Aircraft emissions may undergo an effective downward transport under the influence of stratosphere-troposphere exchange activity. (author) 12 refs.

  12. 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...

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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

  19. 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.

  20. 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

  1. 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

  2. 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...

  3. "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…

  4. 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

  5. Titan’s Oxygen Chemistry and its Impact on Haze Formation

    Science.gov (United States)

    Vuitton, Veronique; He, Chao; Moran, Sarah; Wolters, Cedric; Flandinet, Laurene; Orthous-Daunay, Francois-Regis; Thissen, Roland; Horst, Sarah

    2018-06-01

    Though Titan's atmosphere is reducing with its 98% N2, 2% CH4 and 0.1% H2, CO is the fourth most abundant molecule with a uniform mixing ratio of ~50 ppm. Two other oxygen bearing molecules have also been observed in Titan's atmosphere: CO2 and H2O, with a mixing ratio of ~15 and ~1 ppb, respectively. The physical and chemical processes that determine the abundances of these species on Titan have been at the centre of a long-standing debate as they place constraints on the origin and evolution of its atmosphere. Moreover, laboratory experiments have shown that oxygen can be incorporated into complex molecules, some of which are building blocks of life. Finally, the presence of CO modifies the production rate and size of tholins, which transposed to Titan's haze may have some strong repercussions on the temperature structure and dynamics of the atmosphere.We present here our current understanding of Titan's oxygen chemistry and of its impact on the chemical composition of the haze. We base our discussion on state-of-the-art laboratory experiments for the synthesis and chemical analysis of aerosol analogues. We used a very-high resolution mass spectrometer (LTQ-Orbitrap XL instrument) to characterize the soluble part of tholin samples generated from N2/CH4/CO mixtures at different mixing ratios. These composition measurements provide some understanding of the chemical mechanisms by which CO affects particle formation and growth. Our final objective is to obtain a global picture of the fate and impact of oxygen on Titan, from its origin to prebiotic molecules to haze particles to material deposited on the surface.

  6. 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

  7. 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

  8. 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

  9. 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.

  10. 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

  11. 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.

  12. 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

  13. 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.

  14. 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.

  15. 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

  16. 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.

  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. 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. Causes and impacts of changes in the stratospheric meridional circulation in a chemistry-climate model

    Energy Technology Data Exchange (ETDEWEB)

    Garny, Hella

    2011-05-13

    The stratospheric meridional circulation is projected to be subject to changes due to enhanced greenhouse-gas concentrations in the atmosphere. This study aims to diagnose and explain long-term changes in the stratospheric meridional circulation using the chemistry-climate model E39CA. The diagnosed strengthening of the circulation is found to be driven by increases in tropical sea surface temperatures which lead to a strengthening and upward shift of the subtropical jets. This enables enhanced vertical propagation of large scale waves into the lower stratosphere, and therefore stronger local wave forcing of the meridional circulation in the tropical lower stratosphere. The impact of changes in transport on the ozone layer is analysed using a newly developed method that allows the separation of the effects of transport and chemistry changes on ozone. It is found that future changes of mean stratospheric ozone concentrations are largely determined by changes in chemistry, while changes in transport of ozone play a minor role. (orig.)

  1. 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.

  2. Assessment of the atmospheric impact of volcanic eruptions

    Science.gov (United States)

    Sigurdsson, H.

    1988-01-01

    The dominant global impact of volcanic activity is likely to be related to the effects of volcanic gases on the Earth's atmosphere. Volcanic gas emissions from individual volcanic arc eruptions are likely to cause increases in the stratospheric optical depth that result in surface landmass temperature decline of 2 to 3 K for less than a decade. Trachytic and intermediate magmas are much more effective in this regard than high-silica magmas, and may also lead to extensive ozone depletion due to effect of halogens and magmatic water. Given the assumed relationship between arc volcanism and subduction rate, and the relatively small variation in global spreading rates in the geologic record, it is unlikely that the rates of arc volcanism have varied greatly during the Cenozoic. Hotspot related basaltic fissure eruptions in the subaerial environment have a higher mass yield of sulfur, but lofting of the valcanic aerosol to levels above the tropopause is required for a climate impact. High-latitude events, such as the Laki 1783 eruption can easily penetrate the tropopause and enter the stratosphere, but formation of a stratospheric volcanic aerosol form low-latitude effusive basaltic eruptions is problematical, due to the elevated low-latitude tropopause. Due to the high sulfur content of hotspot-derived basaltic magmas, their very high mass eruption rates and the episodic behavior, hotspots must be regarded as potentially major modifiers of Earth's climate through the action of their volcanic volatiles on the chemistry and physics of the atmosphere.

  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. 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

  5. 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

  6. 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

  7. 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

  8. 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.

  9. 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.

  10. Biogenic and pyrogenic emissions from Africa and their impact on the global atmosphere

    International Nuclear Information System (INIS)

    Scholes, Mary; Andreae, M.O.

    2000-01-01

    Tropical regions, with their high biological activity, have the potential to emit large amounts of trace gases and aerosols to the atmosphere. This can take the form of trace gas fluxes from soils and vegetation, where gaseous species are produced and consumed by living organisms, or of smoke emissions from vegetation fires. In the last decade, considerable scientific effort has gone into quantifying these fluxes from the African continent. We find that both biogenic and pyrogenic emissions have a powerful impact on regional and global atmospheric chemistry, particularly on photooxidation processes and tropospheric ozone. The emissions of radiatively active gases and aerosols from the African continent are likely to have a significant climatic effect, but presently available data are not sufficient for reliable quantitative estimates of this effect

  11. 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.

  12. 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

  13. 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...

  14. 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

  15. 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

  16. 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.

  17. 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.

  18. 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.

  19. 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

  20. Simulation of the impact of thunderstorm activity on atmospheric gas composition

    Science.gov (United States)

    Smyshlyaev, S. P.; Mareev, E. A.; Galin, V. Ya.

    2010-08-01

    A chemistry-climate model of the lower and middle atmosphere has been used to estimate the sensitivity of the atmospheric gas composition to the rate of thunderstorm production of nitrogen oxides at upper tropospheric and lower stratospheric altitudes. The impact that nitrogen oxides produced by lightning have on the atmospheric gas composition is treated as a subgrid-scale process and included in the model parametrically. The natural uncertainty in the global production rate of nitrogen oxides in lightning flashes was specified within limits from 2 to 20 Tg N/year. Results of the model experiments have shown that, due to the variability of thunderstorm-produced nitrogen oxides, their concentration in the upper troposphere and lower stratosphere can vary by a factor of 2 or 3, which, given the influence of nitrogen oxides on ozone and other gases, creates the potential for a strong perturbation of the atmospheric gas composition and thermal regime. Model calculations have shown the strong sensitivity of ozone and the OH hydroxyl to the amount of lightning nitrogen oxides at different atmospheric altitudes. These calculations demonstrate the importance of nitrogen oxides of thunderstorm origin for the balance of atmospheric odd ozone and gases linked to it, such as ozone and hydroxyl radicals. Our results demonstrate that one important task is to raise the accuracy of estimates of the rate of nitrogen oxide production by lightning discharges and to use physical parametrizations that take into account the local lightning effects and feedbacks arising in this case rather than climatological data in models of the gas composition and general circulation of the atmosphere.

  1. 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

  2. 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.

  3. 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.

  4. 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)

  5. 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.

  6. 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.

  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. 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.

  9. 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.

  10. 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.

  11. 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

  12. Impact of aircraft exhaust on the atmosphere. Box model studies and 3-D mesoscale numerical case studies of seasonal differences

    Energy Technology Data Exchange (ETDEWEB)

    Petry, H; Ebel, A; Franzkowiak, V; Hendricks, J; Lippert, E; Moellhoff, M [Koeln Univ. (Germany). Inst. fuer Geophysik und Meteorologie

    1998-12-31

    The impact of aircraft emissions released in the tropopause region on atmospheric trace gases as O{sub 3} or HNO{sub 3} is investigated by means of model studies. Special emphasis is drawn on seasonal effects. A box model is applied as well as a 3-D mesoscale chemistry transport model. These model studies show that the impact of aircraft emissions on ozone in the tropopause region is much stronger in summer than in late autumn with a difference of one order of magnitude. (author) 14 refs.

  13. Impact of aircraft exhaust on the atmosphere. Box model studies and 3-D mesoscale numerical case studies of seasonal differences

    Energy Technology Data Exchange (ETDEWEB)

    Petry, H.; Ebel, A.; Franzkowiak, V.; Hendricks, J.; Lippert, E.; Moellhoff, M. [Koeln Univ. (Germany). Inst. fuer Geophysik und Meteorologie

    1997-12-31

    The impact of aircraft emissions released in the tropopause region on atmospheric trace gases as O{sub 3} or HNO{sub 3} is investigated by means of model studies. Special emphasis is drawn on seasonal effects. A box model is applied as well as a 3-D mesoscale chemistry transport model. These model studies show that the impact of aircraft emissions on ozone in the tropopause region is much stronger in summer than in late autumn with a difference of one order of magnitude. (author) 14 refs.

  14. Impact of preindustrial to present-day changes in short-lived pollutant emissions on atmospheric composition and climate forcing

    Science.gov (United States)

    Naik, Vaishali; Horowitz, Larry W.; Fiore, Arlene M.; Ginoux, Paul; Mao, Jingqiu; Aghedo, Adetutu M.; Levy, Hiram

    2013-07-01

    We describe and evaluate atmospheric chemistry in the newly developed Geophysical Fluid Dynamics Laboratory chemistry-climate model (GFDL AM3) and apply it to investigate the net impact of preindustrial (PI) to present (PD) changes in short-lived pollutant emissions (ozone precursors, sulfur dioxide, and carbonaceous aerosols) and methane concentration on atmospheric composition and climate forcing. The inclusion of online troposphere-stratosphere interactions, gas-aerosol chemistry, and aerosol-cloud interactions (including direct and indirect aerosol radiative effects) in AM3 enables a more complete representation of interactions among short-lived species, and thus their net climate impact, than was considered in previous climate assessments. The base AM3 simulation, driven with observed sea surface temperature (SST) and sea ice cover (SIC) over the period 1981-2007, generally reproduces the observed mean magnitude, spatial distribution, and seasonal cycle of tropospheric ozone and carbon monoxide. The global mean aerosol optical depth in our base simulation is within 5% of satellite measurements over the 1982-2006 time period. We conduct a pair of simulations in which only the short-lived pollutant emissions and methane concentrations are changed from PI (1860) to PD (2000) levels (i.e., SST, SIC, greenhouse gases, and ozone-depleting substances are held at PD levels). From the PI to PD, we find that changes in short-lived pollutant emissions and methane have caused the tropospheric ozone burden to increase by 39% and the global burdens of sulfate, black carbon, and organic carbon to increase by factors of 3, 2.4, and 1.4, respectively. Tropospheric hydroxyl concentration decreases by 7%, showing that increases in OH sinks (methane, carbon monoxide, nonmethane volatile organic compounds, and sulfur dioxide) dominate over sources (ozone and nitrogen oxides) in the model. Combined changes in tropospheric ozone and aerosols cause a net negative top-of-the-atmosphere

  15. 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...

  16. 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.

  17. 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

  18. 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.

  19. 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

  20. 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

  1. 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

  2. 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.

  3. 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

  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. 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.)

  9. 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.)

  10. 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

  11. 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.

  12. 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.

  13. 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....

  14. 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/

  15. Impact of General Chemistry on Student Achievement and Progression to Subsequent Chemistry Courses: A Regression Discontinuity Analysis

    Science.gov (United States)

    Shultz, Ginger V.; Gottfried, Amy C.; Winschel, Grace A.

    2015-01-01

    General chemistry is a gateway course that impacts the STEM trajectory of tens of thousands of students each year, and its role in the introductory curriculum as well as its pedagogical design are the center of an ongoing debate. To investigate the role of general chemistry in the curriculum, we report the results of a posthoc analysis of 10 years…

  16. 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.)

  17. 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.

  18. 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

  19. 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.

  20. Effects of meteorite impacts on the atmospheric evolution of Mars.

    Science.gov (United States)

    Pham, Lê Binh San; Karatekin, Ozgür; Dehant, Véronique

    2009-01-01

    Early in its history, Mars probably had a denser atmosphere with sufficient greenhouse gases to sustain the presence of stable liquid water at the surface. Impacts by asteroids and comets would have played a significant role in the evolution of the martian atmosphere, not only by causing atmospheric erosion but also by delivering material and volatiles to the planet. We investigate the atmospheric loss and the delivery of volatiles with an analytical model that takes into account the impact simulation results and the flux of impactors given in the literature. The atmospheric loss and the delivery of volatiles are calculated to obtain the atmospheric pressure evolution. Our results suggest that the impacts alone cannot satisfactorily explain the loss of significant atmospheric mass since the Late Noachian (approximately 3.7-4 Ga). A period with intense bombardment of meteorites could have increased the atmospheric loss; but to explain the loss of a speculative massive atmosphere in the Late Noachian, other factors of atmospheric erosion and replenishment also need to be taken into account.

  1. Impacts of the January 2005 solar particle events on middle atmospheric chlorine species

    Science.gov (United States)

    Winkler, Holger; Sinnhuber, Miriam; Notholt, Justus; Maik Wissing, Jan; Kallenrode, May-Britt; Santee, Michelle

    It is well established that solar particle events (SPEs) are sources of significant chemical dis-turbances in the Earth's polar atmosphere. The observed SPE effects on nitrogen, hydrogen and oxygen compounds have been investigated in some detail in recent years, and they can be reproduced by atmospheric models using basic parametrizations for NOx and HOx produc-tion as a funtion of the particle impact ionisation. However, there are considerable differences between model predictions and measurements concerning several other trace gases including chlorine species. Two major SPEs occurred on January 17, and January 20, 2005. The latter had an exceptionally hard energy spectrum which caused maximum particle impact ionization at stratospheric altitudes. The Microwave Limb Sounder (MLS) instrument on-board the Aura satellite has measured a short-term decrease of HCl in the northern polar region corresponding to January 2005 SPEs. The peak HCl depletion is ˜300 ppt at 35-40 km. This is comparable to the depletion of messopheric HCl observed by the HALOE instrument during the July 2000 SPE. We will present simulation results of the University of Bremen Ion Chemistry (UBIC) model for the SPEs in January 2005 focusing on chlorine species. The simulations indicate that the observed short-term decrease of middle atmospheric HCl is due to a conversion into active chlorine species such as Cl, ClO and HOCl. The magnitude of the observed HCl loss can only be reproduced if reactions of negative chlorine species and the production of O(1 D) from the reaction N(2 D) + O2 are taken into account. The model results will be compared to MLS/Aura data of HCl, HOCl and ClO. Additionally, the impacts of the observed chlorine activation, e.g. on ozone, will be assessed.

  2. 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.

  3. Biomass burning: Its history, use, and distribution and its impact on environmental quality and global climate

    International Nuclear Information System (INIS)

    Andreae, M.O.

    1991-01-01

    In this chapter, the following topics are discussed: global estimates of amounts of biomass burning; kinds and amounts of emissions to the atmosphere; environmental transport and atmospheric chemistry of these emissions; and environmental impacts. These impacts include acid deposition, climate changes, disruption of nutrient cycles, soil degradation, perturbation of stratospheric chemistry and the ozone layer

  4. 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.

  5. 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

  6. 10-year record of atmospheric composition in the high Himalayas: source, transport and impact

    Science.gov (United States)

    Bonasoni, Paolo; Laj, Paolo; Marinoni, Angela; Cristofanelli, Paolo; Maione, Michela; Putero, Davide; Calzolari, Francescopiero; Decesari, Stefano; Facchini, Maria Cristina; Fuzzi, Sandro; Gobbi, Gianpaolo; Sellegri, Karine; Verza, Gianpietro; Vuillermoz, Elisa; Arduini, Jgor

    2016-04-01

    South Asia represents a global "hot-spot" for air-quality and climate impacts. Since the end of the 20th Century, field experiments and satellite observations identified a thick layer of atmospheric pollutants extending from the Indian Ocean up to the atmosphere of the Himalayas. Since large amount of short-lived climate pollutants (SLCPs) - like atmospheric aerosol (in particular, the light-absorbing aerosol) and ozone - characterize this region, severe implications were recognized for population health, ecosystem integrity as well as regional climate impacts, especially for what concerns hydrological cycle, monsoon regimes and cryosphere. Since 2006, the Nepal Climate Observatory - Pyramid (NCO-P, 27.95N, 86.82 E, 5079 m a.s.l.), a global station of the WMO/GAW programme has been active in the eastern Nepal Himalaya, not far from the Mt. Everest. NCO-P is located away from large direct anthropogenic pollution sources. The closest major urban area is Kathmandu (200 km south-west from the measurement site). As being located along the Khumbu valley, the observations are representative of synoptic-scale and mountain thermal circulation, providing direct information about the vertical transport of pollutants/climate-altering compounds to the Himalayas and to the free troposphere. In the framework of international programmes (GAW/WMO, UNEP-ABC, AERONET) the following continuous measurement programmes have been carried out at NCO-P: surface ozone, aerosol size distribution (from 10 nm to 25 micron), total particle number, aerosol scattering and absorption coefficients, equivalent BC, PM1-PM10, AOD by sun-photometry, global solar radiation (SW and LW), meteorology. Long-term sampling programmes for the off-line determination of halogenated gases and aerosol chemistry have been also activated. The atmospheric observation records at NCO-P, now representing the longest time series available for the high Himalayas, provided the first direct evidences about the systematic

  7. 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.

  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. 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.

  10. 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.

  11. 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

  12. 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.

  13. 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

  14. 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

  15. 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

  16. 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

  17. 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.

  18. 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.

  19. 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

  20. 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.)

  1. 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

  2. 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

  3. Impacts of aerosol direct effects on tropospheric ozone through changes in atmospheric dynamics and photolysis rates

    Science.gov (United States)

    Xing, Jia; Wang, Jiandong; Mathur, Rohit; Wang, Shuxiao; Sarwar, Golam; Pleim, Jonathan; Hogrefe, Christian; Zhang, Yuqiang; Jiang, Jingkun; Wong, David C.; Hao, Jiming

    2017-08-01

    Aerosol direct effects (ADEs), i.e., scattering and absorption of incoming solar radiation, reduce radiation reaching the ground and the resultant photolysis attenuation can decrease ozone (O3) formation in polluted areas. One the other hand, evidence also suggests that ADE-associated cooling suppresses atmospheric ventilation, thereby enhancing surface-level O3. Assessment of ADE impacts is thus important for understanding emission reduction strategies that seek co-benefits associated with reductions in both particulate matter and O3 levels. This study quantifies the impacts of ADEs on tropospheric ozone by using a two-way online coupled meteorology and atmospheric chemistry model, WRF-CMAQ, using a process analysis methodology. Two manifestations of ADE impacts on O3 including changes in atmospheric dynamics (ΔDynamics) and changes in photolysis rates (ΔPhotolysis) were assessed separately through multiple scenario simulations for January and July of 2013 over China. Results suggest that ADEs reduced surface daily maxima 1 h O3 (DM1O3) in China by up to 39 µg m-3 through the combination of ΔDynamics and ΔPhotolysis in January but enhanced surface DM1O3 by up to 4 µg m-3 in July. Increased O3 in July is largely attributed to ΔDynamics, which causes a weaker O3 sink of dry deposition and a stronger O3 source of photochemistry due to the stabilization of the atmosphere. Meanwhile, surface OH is also enhanced at noon in July, though its daytime average values are reduced in January. An increased OH chain length and a shift towards more volatile organic compound (VOC)-limited conditions are found due to ADEs in both January and July. This study suggests that reducing ADEs may have the potential risk of increasing O3 in winter, but it will benefit the reduction in maxima O3 in summer.

  4. Impact of Chemistry Teachers' Knowledge and Practices on Student Achievement

    Science.gov (United States)

    Scantlebury, Kathryn

    2008-10-01

    Professional development programs promoting inquiry-based teaching are challenged with providing teachers content knowledge and using pedagogical approaches that model standards based instruction. Inquiry practices are also important for undergraduate students. This paper focuses on the evaluation of an extensive professional development program for chemistry teachers that included chemistry content tests for students and the teachers and the impact of undergraduate research experiences on college students' attitudes towards chemistry. Baseline results for the students showed that there were no gender differences on the achievement test but white students scored significantly higher than non-white students. However, parent/adult involvement with chemistry homework and projects, was a significant negative predictor of 11th grade students' test chemistry achievement score. This paper will focus on students' achievement and attitude results for teachers who are mid-way through the program providing evidence that on-going, sustained professional development in content and pedagogy is critical for improving students' science achievement.

  5. 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.

  6. 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

  7. 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

  8. 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.

  9. 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....

  10. 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

  11. 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.

  12. Comets, impacts, and atmospheres

    Science.gov (United States)

    Owen, Tobias; Bar-Nun, Akiva

    Studies of element abundances and values of D/H in the atmospheres of the giant planets and Titan have emphasized the important role of icy planetesimals in the formation of these bodies. In these atmospheres, C/H and D/H increase as the relative masses of the 'cores' of the planets increase. N/H appears to deviate from this trend in an interesting way. In the inner solar system, the traditional approach of using carbonaceous chondrites as the source of planetary volatiles is in serious trouble because of the depletion of xenon and the unusual pattern of xenon isotopes found in the atmospheres of Earth and Mars, and because of the solar-type abundance ratios of argon, krypton and xenon and the large amounts of neon and argon on Venus. Recent studies of elemental abundances in comets, especially P/Halley, coupled with laboratory studies of the trapping of gas in ice formed at low temperatures by A. Bar-Nun et al. provide a consistent interpretation of all of these results. This interpretation emphasizes the fundamental importance of icy planetesimals (comets) and the randomness of early impacts in the formation of planetary systems. Cometary delivery by itself will not explain the noble gas abundances on the inner planets. There is good evidence for at least one additional source, which presumably consists of the rocky material making up the bulk of the planets. The existence of this rocky reservoir is manifested in the nucleogenic isotopes and in the neon which is found in all these atmospheres and is also present in the Earth's mantle. This neon may well be a relic of the planets' earliest, accretional atmospheres.

  13. 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

  14. 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.

  15. 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

  16. 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

  17. 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

  18. Fire Influences on Atmospheric Composition, Air Quality, and Climate

    Science.gov (United States)

    Voulgarakis, Apostolos; Field, Robert D.

    2015-01-01

    Fires impact atmospheric composition through their emissions, which range from long-lived gases to short-lived gases and aerosols. Effects are typically larger in the tropics and boreal regions but can also be substantial in highly populated areas in the northern mid-latitudes. In all regions, fire can impact air quality and health. Similarly, its effect on large-scale atmospheric processes, including regional and global atmospheric chemistry and climate forcing, can be substantial, but this remains largely unexplored. The impacts are primarily realised in the boundary layer and lower free troposphere but can also be noticeable in upper troposphere/lower stratosphere (UT/LS) region, for the most intense fires. In this review, we summarise the recent literature on findings related to fire impact on atmospheric composition, air quality and climate. We explore both observational and modelling approaches and present information on key regions and on the globe as a whole. We also discuss the current and future directions in this area of research, focusing on the major advances in emission estimates, the emerging efforts to include fire as a component in Earth system modelling and the use of modelling to assess health impacts of fire emissions.

  19. 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.

  20. 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.

  1. Impact of seawater carbonate chemistry on the calcification of marine bivalves

    Science.gov (United States)

    Thomsen, J.; Haynert, K.; Wegner, K. M.; Melzner, F.

    2015-07-01

    Bivalve calcification, particularly of the early larval stages, is highly sensitive to the change in ocean carbonate chemistry resulting from atmospheric CO2 uptake. Earlier studies suggested that declining seawater [CO32-] and thereby lowered carbonate saturation affect shell production. However, disturbances of physiological processes such as acid-base regulation by adverse seawater pCO2 and pH can affect calcification in a secondary fashion. In order to determine the exact carbonate system component by which growth and calcification are affected it is necessary to utilize more complex carbonate chemistry manipulations. As single factors, pCO2 had no effects and [HCO3-] and pH had only limited effects on shell growth, while lowered [CO32-] strongly impacted calcification. Dissolved inorganic carbon (CT) limiting conditions led to strong reductions in calcification, despite high [CO32-], indicating that [HCO3-] rather than [CO32-] is the inorganic carbon source utilized for calcification by mytilid mussels. However, as the ratio [HCO3-] / [H+] is linearly correlated with [CO32-] it is not possible to differentiate between these under natural seawater conditions. An equivalent of about 80 μmol kg-1 [CO32-] is required to saturate inorganic carbon supply for calcification in bivalves. Below this threshold biomineralization rates rapidly decline. A comparison of literature data available for larvae and juvenile mussels and oysters originating from habitats differing substantially with respect to prevailing carbonate chemistry conditions revealed similar response curves. This suggests that the mechanisms which determine sensitivity of calcification in this group are highly conserved. The higher sensitivity of larval calcification seems to primarily result from the much higher relative calcification rates in early life stages. In order to reveal and understand the mechanisms that limit or facilitate adaptation to future ocean acidification, it is necessary to better

  2. 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.

  3. The global impact of the transport sectors on atmospheric aerosol in 2030 – Part 1: Land transport and shipping

    Directory of Open Access Journals (Sweden)

    M. Righi

    2015-01-01

    Full Text Available Using the EMAC (ECHAM/MESSy Atmospheric Chemistry global climate-chemistry model coupled to the aerosol module MADE (Modal Aerosol Dynamics model for Europe, adapted for global applications, we simulate the impact of land transport and shipping emissions on global atmospheric aerosol and climate in 2030. Future emissions of short-lived gas and aerosol species follow the four Representative Concentration Pathways (RCPs designed in support of the Fifth Assessment Report of the Intergovernmental Panel on Climate Change. We compare the resulting 2030 land-transport- and shipping-induced aerosol concentrations to the ones obtained for the year 2000 in a previous study with the same model configuration. The simulations suggest that black carbon and aerosol nitrate are the most relevant pollutants from land transport in 2000 and 2030 and their impacts are characterized by very strong regional variations during this time period. Europe and North America experience a decrease in the land-transport-induced particle pollution, although in these regions this sector remains a major source of surface-level pollution in 2030 under all RCPs. In Southeast Asia, however, a significant increase is simulated, but in this region the surface-level pollution is still controlled by other sources than land transport. Shipping-induced air pollution is mostly due to aerosol sulfate and nitrate, which show opposite trends towards 2030. Sulfate is strongly reduced as a consequence of sulfur reduction policies in ship fuels in force since 2010, while nitrate tends to increase due to the excess of ammonia following the reduction in ammonium sulfate. The aerosol-induced climate impact of both sectors is dominated by aerosol-cloud effects and is projected to decrease between 2000 and 2030, nevertheless still contributing a significant radiative forcing to Earth's radiation budget.

  4. Late Impacts and the Origins of the Atmospheres on the Terrestrial Planets

    Science.gov (United States)

    Mukhopadhyay, S.; Stewart, S. T.; Lock, S. J.; Parai, R.; Tucker, J. M.

    2014-12-01

    Models for the origin of terrestrial atmospheres typically require an intricate sequence of events, including hydrodynamic escape, outgassing of mantle volatiles and late delivery. Here we discuss the origin of the atmospheres on the terrestrial planets in light of new ideas about the formation of the Moon, giant impact induced atmospheric loss and recent noble gas measurements. Our new measurements indicate that noble gases in the Earth's atmosphere cannot be derived from any combination of fractionation of a nebular-derived atmosphere followed by outgassing of deep or shallow mantle volatiles. While Ne in the mantle retains a nebular component, the present-day atmosphere has no memory of nebular gases. Rather, atmospheric noble gases have a close affinity to chondrites. On the other hand, Venus's atmosphere has 20 and 70 times higher abundance of 20Ne and 36Ar, respectively, and a 20Ne/22Ne ratio closer to the solar value than Earth's atmosphere. While the present atmosphere of Mars is significantly fractionated in the lighter noble gases due to long term atmospheric escape, the Kr isotopic ratios in Martian atmosphere are identical to solar. Thus, while Earth's atmosphere has no memory of accretion of nebular gases, atmospheres on both Venus and Mars preserve at least a component of nebular gases. To explain the above observations, we propose that a common set of processes operated on the terrestrial planets, and that their subsequent evolutionary divergence is simply explained by planetary size and the stochastic nature of giant impacts. We present geochemical observations and simulations of giant impacts to show that most of Earth's mantle was degassed and the outgassed volatiles were largely lost during the final sequence of giant impacts onto Earth. Earth's noble gases were therefore dominantly derived from late-accreting planetesimals. In contrast, Venus did not suffer substantial atmospheric loss by a late giant impact and retains a higher abundance of

  5. 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.

  6. 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

  7. Impact of seawater carbonate chemistry on the calcification of marine bivalves

    OpenAIRE

    Thomsen Jörn; Haynert Kristin; Wegner K Mathias; Melzner Frank

    2015-01-01

    Bivalve calcification, particular of the early larval stages is highly sensitive to the change of ocean carbonate chemistry resulting from atmospheric CO2 uptake. Earlier studies suggested that declining seawater [CO32−] and thereby lowered carbonate saturation affect shell production. However, disturbances of physiological processes such as acid-base regulation by adverse seawater pCO2 and pH can affect calcification in a secondary fashion. In order to determine the e...

  8. 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

  9. Tropospheric Halogen Chemistry

    Science.gov (United States)

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

    2003-12-01

    processes. Early work by Cauer (1951) had shown that Cl/Na and Cl/Mg ratios were lower in air than in seawater, indicating loss of chlorine by "acid displacement" from sea salt by the strong acids, H2SO4 (Eriksson (1959a, b) and HNO3 (Robbins et al., 1959). Already the first measurements of bromine in aerosols by Duce et al. (1963) showed that bromine, like chlorine, was lost from the sea salt particles, whereas iodine was strongly enriched ( Duce et al., 1965). Research since the early 1980s has shown that photochemical processes are actively involved.Interest in the chemistry of atmospheric halogens took a steep upward surge after it was postulated that the release of industrially produced halocarbons, in particular the chlorofluorocarbons (CFCs), CFCl3, and CF2Cl2, could cause severe depletions in stratospheric ozone (Molina and Rowland, 1974) by the reactions involving the CFC photolytic product radicals, Cl and ClO, as catalysts. The first stratospheric measurements of ClO did indeed show its presence in significant quantities in the stratosphere so that by the end of the 1970s USA, Canada, and the Scandinavian countries issued laws against the use of CFC gases as propellants in spray cans. In the mid-1980s the springtime stratospheric ozone hole over Antarctica was discovered by Farman et al. (1985), involving heterogeneous reactions on polar stratospheric clouds that lead to chlorine activation ( Solomon et al., 1986). Ten years later, in 1996, a complete phaseout ofthe production of the CFCs and a number of other chlorine- or bromine-containing chemicals came into effect for all nations in the developed world. In this contribution we will, however, concentrate on the impact of reactive chlorine, bromine, and iodine on tropospheric ozone chemistry.Halogens have the potential to be important in many facets of tropospheric chemistry. A multitude of gas phase reactions and gas-particle interactions occur that include coupling with the sulfur cycle and reactions with

  10. 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.

  11. Impact of fuel chemistry on fission product behaviour

    International Nuclear Information System (INIS)

    Poortmans, C.; Van Uffelen, P.; Van den Berghe, S.

    1999-01-01

    The report contains a series of papers presented at SCK-CEN's workshop on the impact of fuel chemistry on fission product behaviour. Contributing authors discuss different processes affecting the behaviour of fission products in different types of spent nuclear fuel. In addition, a number of papers discusses the behaviour of actinides and fission products released from spent fuel and vitrified high-level waste in geological disposal conditions

  12. Modeling the present and future impact of aviation on climate: an AOGCM approach with online coupled chemistry

    Directory of Open Access Journals (Sweden)

    P. Huszar

    2013-10-01

    Full Text Available Our work is among the first that use an atmosphere-ocean general circulation model (AOGCM with online chemistry to evaluate the impact of future aviation emissions on temperature. Other particularities of our study include non-scaling to the aviation emissions, and the analysis of models' transient response using ensemble simulations. The model we use is the Météo-France CNRM-CM5.1 earth system model extended with the REPROBUS chemistry scheme. The time horizon of our interest is 1940–2100, assuming the A1B SRES scenario. We investigate the present and future impact of aviation emissions of CO2, NOx and H2O on climate, taking into account changes in greenhouse gases, contrails and contrail-induced cirrus (CIC. As in many transport-related impact studies, we distinguish between the climate impacts of CO2 emissions and those of non-CO2 emissions. Aviation-produced aerosol is not considered in the study. Our modeling system simulated a notable sea-ice bias in the Arctic, and therefore results concerning the surface should be viewed with caution. The global averaged near-surface CO2 impact reaches around 0.1 K by the end of the 21st century, while the non-CO2 impact reaches 0.2 K in the second half of the century. The NOx emissions impact is almost negligible in our simulations, as our aviation-induced ozone production is small. As a consequence, the non-CO2 signal is very similar to the CIC signal. The seasonal analysis shows that the strongest warming due to aviation is modeled for the late summer and early autumn. In the stratosphere, a significant cooling is attributed to aviation CO2 emissions (−0.25 K by 2100. A −0.3 K temperature decrease is modeled when considering all the aviation emissions, but no significant signal appears from the CIC or NOx forcings in the stratosphere.

  13. Ocean-Atmosphere Interactions Modulate Irrigation's Climate Impacts

    Science.gov (United States)

    Krakauer, Nir Y.; Puma, Michael J.; Cook, Benjamin I.; Gentine, Pierre; Nazarenko, Larissa

    2016-01-01

    Numerous studies have focused on the local and regional climate effects of irrigated agriculture and other land cover and land use change (LCLUC) phenomena, but there are few studies on the role of ocean- atmosphere interaction in modulating irrigation climate impacts. Here, we compare simulations with and without interactive sea surface temperatures of the equilibrium effect on climate of contemporary (year 2000) irrigation geographic extent and intensity. We find that ocean-atmosphere interaction does impact the magnitude of global-mean and spatially varying climate impacts, greatly increasing their global reach. Local climate effects in the irrigated regions remain broadly similar, while non-local effects, particularly over the oceans, tend to be larger. The interaction amplifies irrigation-driven standing wave patterns in the tropics and mid-latitudes in our simulations, approximately doubling the global-mean amplitude of surface temperature changes due to irrigation. The fractions of global area experiencing significant annual-mean surface air temperature and precipitation change also approximately double with ocean-atmosphere interaction. Subject to confirmation with other models, these findings imply that LCLUC is an important contributor to climate change even in remote areas such as the Southern Ocean, and that attribution studies should include interactive oceans and need to consider LCLUC, including irrigation, as a truly global forcing that affects climate and the water cycle over ocean as well as land areas.

  14. Desorption of 1,3,5-Trichlorobenzene from Multi-Walled Carbon Nanotubes: Impact of Solution Chemistry and Surface Chemistry

    Directory of Open Access Journals (Sweden)

    Sheikh Uddin

    2013-05-01

    Full Text Available The strong affinity of carbon nanotubes (CNTs to environmental contaminants has raised serious concern that CNTs may function as a carrier of environmental pollutants and lead to contamination in places where the environmental pollutants are not expected. However, this concern will not be realized until the contaminants are desorbed from CNTs. It is well recognized that the desorption of environmental pollutants from pre-laden CNTs varies with the environmental conditions, such as the solution pH and ionic strength. However, comprehensive investigation on the influence of solution chemistry on the desorption process has not been carried out, even though numerous investigations have been conducted to investigate the impact of solution chemistry on the adsorption of environmental pollutants on CNTs. The main objective of this study was to determine the influence of solution chemistry (e.g., pH, ionic strength and surface functionalization on the desorption of preloaded 1,3,5-trichlorobenzene (1,3,5-TCB from multi-walled carbon nanotubes (MWNTs. The results suggested that higher pH, ionic strength and natural organic matter in solution generally led to higher desorption of 1,3,5-TCB from MWNTs. However, the extent of change varied at different values of the tested parameters (e.g., pH 7. In addition, the impact of these parameters varied with MWNTs possessing different surface functional groups, suggesting that surface functionalization could considerably alter the environmental behaviors and impact of MWNTs.

  15. 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

  16. 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

  17. 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

  18. Designing global climate and atmospheric chemistry simulations for 1 and 10 km diameter asteroid impacts using the properties of ejecta from the K-Pg impact

    Directory of Open Access Journals (Sweden)

    O. B. Toon

    2016-10-01

    Full Text Available About 66 million years ago, an asteroid about 10 km in diameter struck the Yucatan Peninsula creating the Chicxulub crater. The crater has been dated and found to be coincident with the Cretaceous–Paleogene (K-Pg mass extinction event, one of six great mass extinctions in the last 600 million years. This event precipitated one of the largest episodes of rapid climate change in Earth's history, yet no modern three-dimensional climate calculations have simulated the event. Similarly, while there is an ongoing effort to detect asteroids that might hit Earth and to develop methods to stop them, there have been no modern calculations of the sizes of asteroids whose impacts on land would cause devastating effects on Earth. Here, we provide the information needed to initialize such calculations for the K-Pg impactor and for a 1 km diameter impactor. There is considerable controversy about the details of the events that followed the Chicxulub impact. We proceed through the data record in the order of confidence that a climatically important material was present in the atmosphere. The climatic importance is roughly proportional to the optical depth of the material. Spherules with diameters of several hundred microns are found globally in an abundance that would have produced an atmospheric layer with an optical depth around 20, yet their large sizes would only allow them to stay airborne for a few days. They were likely important for triggering global wildfires. Soot, probably from global or near-global wildfires, is found globally in an abundance that would have produced an optical depth near 100, which would effectively prevent sunlight from reaching the surface. Nanometer-sized iron particles are also present globally. Theory suggests these particles might be remnants of the vaporized asteroid and target that initially remained as vapor rather than condensing on the hundred-micron spherules when they entered the atmosphere. If present in the

  19. 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

  20. 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.

  1. 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

  2. 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

  3. 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.

  4. 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.

  5. 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

  6. 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

  7. 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.

  8. 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

  9. 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...

  10. 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

  11. 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.

  12. Impact of Metacognitive Awareness on Performance of Students in Chemistry

    Science.gov (United States)

    Rahman, Fazal ur; Jumani, Nabi Bux; Chaudry, Muhammad Ajmal; Chisti, Saeed ul Hasan; Abbasi, Fahim

    2010-01-01

    The impact of metacognitive awareness on students' performance has been examined in the present study. 900 students of grade X participated in the study. Metacognitive awareness was measured using inventory, while performance of students was measured with the help of researcher made test in the subject of chemistry. Results indicated that…

  13. 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

  14. 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

  15. The acid-catalyzed hydrolysis of an α-pinene-derived organic nitrate: kinetics, products, reaction mechanisms, and atmospheric impact

    Science.gov (United States)

    Rindelaub, Joel D.; Borca, Carlos H.; Hostetler, Matthew A.; Slade, Jonathan H.; Lipton, Mark A.; Slipchenko, Lyudmila V.; Shepson, Paul B.

    2016-12-01

    The production of atmospheric organic nitrates (RONO2) has a large impact on air quality and climate due to their contribution to secondary organic aerosol and influence on tropospheric ozone concentrations. Since organic nitrates control the fate of gas phase NOx (NO + NO2), a byproduct of anthropogenic combustion processes, their atmospheric production and reactivity is of great interest. While the atmospheric reactivity of many relevant organic nitrates is still uncertain, one significant reactive pathway, condensed phase hydrolysis, has recently been identified as a potential sink for organic nitrate species. The partitioning of gas phase organic nitrates to aerosol particles and subsequent hydrolysis likely removes the oxidized nitrogen from further atmospheric processing, due to large organic nitrate uptake to aerosols and proposed hydrolysis lifetimes, which may impact long-range transport of NOx, a tropospheric ozone precursor. Despite the atmospheric importance, the hydrolysis rates and reaction mechanisms for atmospherically derived organic nitrates are almost completely unknown, including those derived from α-pinene, a biogenic volatile organic compound (BVOC) that is one of the most significant precursors to biogenic secondary organic aerosol (BSOA). To better understand the chemistry that governs the fate of particle phase organic nitrates, the hydrolysis mechanism and rate constants were elucidated for several organic nitrates, including an α-pinene-derived organic nitrate (APN). A positive trend in hydrolysis rate constants was observed with increasing solution acidity for all organic nitrates studied, with the tertiary APN lifetime ranging from 8.3 min at acidic pH (0.25) to 8.8 h at neutral pH (6.9). Since ambient fine aerosol pH values are observed to be acidic, the reported lifetimes, which are much shorter than that of atmospheric fine aerosol, provide important insight into the fate of particle phase organic nitrates. Along with rate constant

  16. Impact on the earth, ocean and atmosphere

    Science.gov (United States)

    Ahrens, Thomas J.; O'Keefe, John D.

    1987-01-01

    On the basis of finite-difference techniques, cratering flow calculations are used to obtain the spatial attenuation of shock pressure with radius along the impact axis for the impact of silicate rock and iron impactors on a silicate half-space at speeds of 5 to 45 km/sec. Upon impact of a 10 to 30 km diameter silicate or water object onto a 5 km deep ocean overlying a silicate half-space planet at 30 km/sec, it is found that from 12 to 15 percent of the incident energy is coupled into the water. The mass of atmosphere lost due to impacts of 1 to 5 km radius projectiles is calculated.

  17. 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.

  18. 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...

  19. 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.

  20. Impact of harvesting and atmospheric pollution on nutrient depletion of eastern US hardwood forests

    Science.gov (United States)

    M.B. Adams; J.A. Burger; A.B. Jenkins; L. Zelazny

    2000-01-01

    The eastern hardwood forests of the US may be threatened by the changing atmospheric chemistry and by changes in harvesting levels. Many studies have documented accelerated base cation losses with intensive forest harvesting. Acidic deposition can also alter nutrient cycling in these forests. The combination of increased harvesting, shorter rotations, and more...

  1. Fire emission heights in the climate system – Part 2: Impact on transport, black carbon concentrations and radiation

    NARCIS (Netherlands)

    Veira, A.; Kloster, Silvia; Schutgens, N. A. J.; Kaiser, Johannes W.

    2015-01-01

    Wildfires represent a major source for aerosols impacting atmospheric radiation, atmospheric chemistry and cloud micro-physical properties. Previous case studies indicated that the height of the aerosol–radiation interaction may crucially affect atmospheric radiation, but the sensitivity to emission

  2. 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

  3. Three-dimensional modeling of HCFC-123 in the atmosphere: assessing its potential environmental impacts and rationale for continued use.

    Science.gov (United States)

    Wuebbles, Donald J; Patten, Kenneth O

    2009-05-01

    HCFC-123 (C2HCl2F3) is used in large refrigeration systems and as a fire suppression agent blend. Like other hydrochlorofluorocarbons, production and consumption of HCFC-123 is limited under the Montreal Protocol on Substances that Deplete the Ozone Layer. The purpose of this study is to update the understanding of the current and projected impacts of HCFC-123 on stratospheric ozone and on climate and to discuss the potential environmental effects from continued use of this chemical for specific applications. For the first time, the Ozone Depletion Potential (ODP) of a HCFC is determined using a three-dimensional model (MOZART-3) of atmospheric physics and chemistry. All previous studies have relied on results from two-dimensional models. The derived HCFC-123 ODP of 0.0098 is smaller than previous values. Analysis of the projected uses and emissions of HCFC-123, assuming reasonable levels of projected growth and use in centrifugal chiller and fire suppressant applications, suggests an extremely small impact on the environment due to its short atmospheric lifetime, low ODP, low Global Warming Potential (GWP), and the small production and emission of its limited applications. The current contribution of HCFC-123 to stratospheric reactive chlorine is too small to be measurable.

  4. 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

  5. Vulnerability assessment of atmospheric environment driven by human impacts.

    Science.gov (United States)

    Zhang, Yang; Shen, Jing; Ding, Feng; Li, Yu; He, Li

    2016-11-15

    Atmospheric environment quality worsening is a substantial threat to public health worldwide, and in many places, air pollution due to the intensification of the human activity is increasing dramatically. However, no studies have been investigated the integration of vulnerability assessment and atmospheric environment driven by human impacts. The objective of this study was to identify and prioritize the undesirable environmental changes as an early warning system for environment managers and decision makers in term of human, atmospheric environment, and social economic elements. We conduct a vulnerability assessment method of atmospheric environment associated with human impact, this method integrates spatial context of Geographic Information System (GIS) tool, multi-criteria decision analysis (MCDA) method, ordered weighted averaging (OWA) operators under the Exposure-Sensitivity- Adaptive Capacity (ESA) framework. Decision makers can find out relevant vulnerability assessment results with different vulnerable attitudes. In the Beijing-Tianjin-Hebei (BTH) region, China, we further applied this developed method and proved it to be reliable and consistent with the China Environmental Status Bulletin. Results indicate that the vulnerability of atmospheric environment in the BTH region is not optimistic, and environment managers should do more about air pollution. Thus, the most appropriate strategic decision and development program of city or state can be picked out assisting by the vulnerable results. Copyright © 2016 Elsevier B.V. All rights reserved.

  6. 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.

  7. 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.

  8. 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

  9. 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

  10. 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

  11. 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...

  12. Global impacts of surface ozone changes on crop yields and land use

    NARCIS (Netherlands)

    Chuwah, C.D.; Noije, van Twan; Vuuren, van Detlef P.; Stehfest, Elke; Hazeleger, Wilco

    2015-01-01

    Exposure to surface ozone has detrimental impacts on vegetation and crop yields. In this study, we estimate ozone impacts on crop production and subsequent impacts on land use in the 2005-2050 period using results of the TM5 atmospheric chemistry and IMAGE integrated assessment model. For the

  13. Global impacts of surface ozone changes on crop yields and land use

    NARCIS (Netherlands)

    Chuwah, Clifford; van Noije, Twan; van Vuuren, Detlef P.; Stehfest, Elke; Hazeleger, Wilco

    2015-01-01

    Exposure to surface ozone has detrimental impacts on vegetation and crop yields. In this study, we estimate ozone impacts on crop production and subsequent impacts on land use in the 2005-2050 period using results of the TM5 atmospheric chemistry and IMAGE integrated assessment model. For the crops

  14. Impact of biomass burning on the atmosphere

    International Nuclear Information System (INIS)

    Dignon, J.

    1993-03-01

    Fire has played an important part in biogeochemical cycling throughout most of the history of our planet. Ice core studies have been very beneficial in paleoclimate studies and constraining the budgets of biogeochemical cycles through the past 160,000 years of the Vostok ice core. Although to date there has been no way of determining cause and effect, concentration of greenhouse gases directly correlates with temperature in ice core analyses. Recent ice core studies on Greenland have shown that significant climate change can be very rapid on the order of a decade. This chapter addresses the coupled evolution of our planet's atmospheric composition and biomass burning. Special attention is paid to the chemical and climatic impacts of biomass burning on the atmosphere throughout the last century, specifically looking at the cycles of carbon, nitrogen, and sulfur. Information from ice core measurements may be useful in understanding the history of fire and its historic affect on the composition of the atmosphere and climate

  15. Formation of C7F15COOH (PFOA) and other perfluorocarboxylic acids during the atmospheric oxidation of 8:2 fluorotelomer alcohol

    DEFF Research Database (Denmark)

    Wallington, T. J.; Hurley, M. D.; Xia, J.

    2006-01-01

    Calculations using a three-dimensional global atmospheric chemistry model (IMPACT) indicate that n-C8F17CH2CH2-OH (widely used in industrial and consumer products) degrades in the atmosphere to give perfluorooctanoic acid (PFOA) and other perfluorocarboxylic acids (PFCAs). PFOA is persistent, bio...

  16. 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

  17. 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

  18. 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.

  19. Atmospheric impacts of evaporative cooling systems

    International Nuclear Information System (INIS)

    Carson, J.E.

    1976-10-01

    The report summarizes available information on the effects of various power plant cooling systems on the atmosphere. While evaporative cooling systems sharply reduce the biological impacts of thermal discharges in water bodies, they create (at least, for heat-release rates comparable to those of two-unit nuclear generating stations) atmospheric changes. For an isolated site such as required for a nuclear power plant, these changes are rather small and local, and usually environmentally acceptable. However, one cannot say with certainty that these effects will remain small as the number of reactors on a given site increases. There must exist a critical heat load for a specific site which, if exceeded, can create its own weather patterns, and thus create inadvertent weather changes such as rain and snow, severe thunderstorms, and tornadoes. Because proven mathematical models are not available, it is not now possible to forecast precisely the extent and frequency of the atmospheric effects of a particular heat-dissipation system at a particular site. Field research on many aspects of cooling system operation is needed in order to document and quantify the actual atmospheric changes caused by a given cooling system and to provide the data needed to develop and verify mathematical and physical models. The more important topics requiring field study are plume rise, fogging and icing (from certain systems), drift emission and deposition rates, chemical interactions, cloud and precipitation formation and critical heat-release rates

  20. 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.

  1. 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

  2. Green Chemistry Metrics with Special Reference to Green Analytical Chemistry

    Directory of Open Access Journals (Sweden)

    Marek Tobiszewski

    2015-06-01

    Full Text Available The concept of green chemistry is widely recognized in chemical laboratories. To properly measure an environmental impact of chemical processes, dedicated assessment tools are required. This paper summarizes the current state of knowledge in the field of development of green chemistry and green analytical chemistry metrics. The diverse methods used for evaluation of the greenness of organic synthesis, such as eco-footprint, E-Factor, EATOS, and Eco-Scale are described. Both the well-established and recently developed green analytical chemistry metrics, including NEMI labeling and analytical Eco-scale, are presented. Additionally, this paper focuses on the possibility of the use of multivariate statistics in evaluation of environmental impact of analytical procedures. All the above metrics are compared and discussed in terms of their advantages and disadvantages. The current needs and future perspectives in green chemistry metrics are also discussed.

  3. Green Chemistry Metrics with Special Reference to Green Analytical Chemistry.

    Science.gov (United States)

    Tobiszewski, Marek; Marć, Mariusz; Gałuszka, Agnieszka; Namieśnik, Jacek

    2015-06-12

    The concept of green chemistry is widely recognized in chemical laboratories. To properly measure an environmental impact of chemical processes, dedicated assessment tools are required. This paper summarizes the current state of knowledge in the field of development of green chemistry and green analytical chemistry metrics. The diverse methods used for evaluation of the greenness of organic synthesis, such as eco-footprint, E-Factor, EATOS, and Eco-Scale are described. Both the well-established and recently developed green analytical chemistry metrics, including NEMI labeling and analytical Eco-scale, are presented. Additionally, this paper focuses on the possibility of the use of multivariate statistics in evaluation of environmental impact of analytical procedures. All the above metrics are compared and discussed in terms of their advantages and disadvantages. The current needs and future perspectives in green chemistry metrics are also discussed.

  4. Size Resolved Mass Concentration and Elemental Composition of Atmospheric Aerosols over the Eastern Mediterranean Area

    Czech Academy of Sciences Publication Activity Database

    Smolík, Jiří; Ždímal, Vladimír; Schwarz, Jaroslav; Lazaridis, M.; Havránek, Vladimír; Eleftheriadis, K.; Mihalopoulos, N.; Bryant, C.; Colbeck, I.

    2003-01-01

    Roč. 3, - (2003), s. 2207-2216 ISSN 1680-7324 Grant - others:ENVK2(XE) 1999/00052 Institutional research plan: CEZ:AV0Z1048901; CEZ:AV0Z4072921 Keywords : atmospheric particles * elemental composition * PM1 Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.317, year: 2003

  5. Atmospheric sulfur and climate changes: a modelling study at mid and high-southern latitudes

    International Nuclear Information System (INIS)

    Castebrunet, H.

    2007-09-01

    The mid and high-southern latitudes are still marginally affected by anthropogenic sulfur emissions. They are the only regions in the world where the natural cycle of the atmospheric sulfur may still be observed. Sulfur aerosols are well-known for their radiative impact, and thus interact with climate. Climate can in turn affect atmospheric sulfur sources, distribution and chemistry. Antarctic ice cores provide information on the evolution of climate and sulfur deposition at the surface of the ice sheet at glacial-interglacial time scales. The aim of this thesis is to develop and use modeling towards a better understanding of the atmospheric sulfur cycle in antarctic and sub-antarctic regions. Ice core data are used to validate model results under glacial climate conditions. An Atmospheric General Circulation Model (AGCM) coupled to a sulfur chemistry module is used: the LMD-ZTSulfur model, version 4. An update of both the physical and chemical parts of the model. The model was first performed. The impact of there changes on modelled sulfur cycle are evaluated for modern climate. Further, boundary conditions are adapted to simulate the atmospheric circulation and sulfur cycle at the Last Glacial Maximum, approximately 20,000 years ago. In the model, sulfur is found to be highly sensitive to antarctic sea-ice coverage, which is still poorly known during the ice age. An original dataset of ice-age sea-ice coverage was developed. Its impact on the oceanic emissions of dimethyl sulfide, main precursor of sulfur aerosols at high-southern latitudes, is discussed. Using the same oceanic sulfur reservoirs as for present day climate, the model broadly reproduces the glacial deposits of sulfur aerosols on the Antarctic plateau, suggesting little impact of climate on oceanic sulfur production in the Antarctic region. Sensitivity tests were carried out to draw an up-to-date status of major uncertainties and difficulties facing future progress in understanding atmospheric

  6. Examining the Impact of Chemistry Education Research Articles from 2007 through 2013 by Citation Counts

    Science.gov (United States)

    Ye, Li; Lewis, Scott E.; Raker, Jeffrey R.; Oueini, Razanne

    2015-01-01

    Evaluating the impact of Chemistry Education Research articles has historically centered on the impact factor of the publishing journal. With the advent of electronic journal indices, it is possible to determine the impact of individual research articles by the number of citations it has received. However, in a relatively new discipline, such as…

  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. Analysis of insect triacylglycerols using liquid chromatography-atmospheric pressure chemical ionization-mass spectrometry

    Czech Academy of Sciences Publication Activity Database

    Kofroňová, Edita; Cvačka, Josef; Jiroš, Pavel; Sýkora, D.; Valterová, Irena

    2009-01-01

    Roč. 111, č. 5 (2009), s. 519-525 ISSN 1438-7697 R&D Projects: GA AV ČR IAA4055403; GA MŠk 2B06007 Institutional research plan: CEZ:AV0Z40550506 Keywords : atmospheric pressure chemical ionization * bumblebees * fat body * NARP-HPLC Subject RIV: CC - Organic Chemistry Impact factor: 1.831, year: 2009

  11. CFD modelling for atmospheric pollutants/aerosols studies within the complex terrains of urban areas and industrial sites

    Czech Academy of Sciences Publication Activity Database

    Střižík, Michal; Zelinger, Zdeněk; Nevrlý, V.; Kubát, Pavel; Berger, P.; Černý, A.; Engst, P.; Bitala, P.; Janečková, Radmila; Grigorová, Eva; Bestová, I.; Čadil, J.; Danihelka, P.; Kadeřábek, P.; Kozubková, M.; Drábková, S.; Hartman, D.; Bojko, M.; Zavila, O.

    2014-01-01

    Roč. 54, č. 1 (2014), s. 73-90 ISSN 0957-4352 R&D Projects: GA MŠk LD12020 Institutional support: RVO:61388955 Keywords : Air pollution * Atmospheric movements * Computational fluid dynamics Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 0.433, year: 2014

  12. Minimal Impact of Organic Chemistry Prerequisite on Student Performance in Introductory Biochemistry

    Science.gov (United States)

    Wright, Robin; Cotner, Sehoya; Winkel, Amy

    2009-01-01

    Curriculum design assumes that successful completion of prerequisite courses will have a positive impact on student performance in courses that require the prerequisite. We recently had the opportunity to test this assumption concerning the relationship between completion of the organic chemistry prerequisite and performance in introductory…

  13. 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.

  14. Using advanced surface complexation models for modelling soil chemistry under forests: Solling forest, Germany

    Energy Technology Data Exchange (ETDEWEB)

    Bonten, Luc T.C., E-mail: luc.bonten@wur.nl [Alterra-Wageningen UR, Soil Science Centre, P.O. Box 47, 6700 AA Wageningen (Netherlands); Groenenberg, Jan E. [Alterra-Wageningen UR, Soil Science Centre, P.O. Box 47, 6700 AA Wageningen (Netherlands); Meesenburg, Henning [Northwest German Forest Research Station, Abt. Umweltkontrolle, Sachgebiet Intensives Umweltmonitoring, Goettingen (Germany); Vries, Wim de [Alterra-Wageningen UR, Soil Science Centre, P.O. Box 47, 6700 AA Wageningen (Netherlands)

    2011-10-15

    Various dynamic soil chemistry models have been developed to gain insight into impacts of atmospheric deposition of sulphur, nitrogen and other elements on soil and soil solution chemistry. Sorption parameters for anions and cations are generally calibrated for each site, which hampers extrapolation in space and time. On the other hand, recently developed surface complexation models (SCMs) have been successful in predicting ion sorption for static systems using generic parameter sets. This study reports the inclusion of an assemblage of these SCMs in the dynamic soil chemistry model SMARTml and applies this model to a spruce forest site in Solling Germany. Parameters for SCMs were taken from generic datasets and not calibrated. Nevertheless, modelling results for major elements matched observations well. Further, trace metals were included in the model, also using the existing framework of SCMs. The model predicted sorption for most trace elements well. - Highlights: > Surface complexation models can be well applied in field studies. > Soil chemistry under a forest site is adequately modelled using generic parameters. > The model is easily extended with extra elements within the existing framework. > Surface complexation models can show the linkages between major soil chemistry and trace element behaviour. - Surface complexation models with generic parameters make calibration of sorption superfluous in dynamic modelling of deposition impacts on soil chemistry under nature areas.

  15. Using advanced surface complexation models for modelling soil chemistry under forests: Solling forest, Germany

    International Nuclear Information System (INIS)

    Bonten, Luc T.C.; Groenenberg, Jan E.; Meesenburg, Henning; Vries, Wim de

    2011-01-01

    Various dynamic soil chemistry models have been developed to gain insight into impacts of atmospheric deposition of sulphur, nitrogen and other elements on soil and soil solution chemistry. Sorption parameters for anions and cations are generally calibrated for each site, which hampers extrapolation in space and time. On the other hand, recently developed surface complexation models (SCMs) have been successful in predicting ion sorption for static systems using generic parameter sets. This study reports the inclusion of an assemblage of these SCMs in the dynamic soil chemistry model SMARTml and applies this model to a spruce forest site in Solling Germany. Parameters for SCMs were taken from generic datasets and not calibrated. Nevertheless, modelling results for major elements matched observations well. Further, trace metals were included in the model, also using the existing framework of SCMs. The model predicted sorption for most trace elements well. - Highlights: → Surface complexation models can be well applied in field studies. → Soil chemistry under a forest site is adequately modelled using generic parameters. → The model is easily extended with extra elements within the existing framework. → Surface complexation models can show the linkages between major soil chemistry and trace element behaviour. - Surface complexation models with generic parameters make calibration of sorption superfluous in dynamic modelling of deposition impacts on soil chemistry under nature areas.

  16. 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.

  17. Micro-physics of aircraft-generated aerosols and their potential impact on heterogeneous plume chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Kaercher, B; Luo, B P [Muenchen Univ., Freising (Germany). Lehrstuhl fuer Bioklimatologie und Immissionsforschung

    1998-12-31

    Answers are attempted to give to open questions concerning physico-chemical processes in near-field aircraft plumes, with emphasis on their potential impact on subsequent heterogeneous chemistry. Research issues concerning the nucleation of aerosols and their interactions among themselves and with exhaust gases are summarized. Microphysical properties of contrail ice particles, formation of liquid ternary mixtures, and nucleation of nitric acid trihydrate particles in contrails are examined and possible implications for heterogeneous plume chemistry are discussed. (author) 19 refs.

  18. Micro-physics of aircraft-generated aerosols and their potential impact on heterogeneous plume chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Kaercher, B.; Luo, B.P. [Muenchen Univ., Freising (Germany). Lehrstuhl fuer Bioklimatologie und Immissionsforschung

    1997-12-31

    Answers are attempted to give to open questions concerning physico-chemical processes in near-field aircraft plumes, with emphasis on their potential impact on subsequent heterogeneous chemistry. Research issues concerning the nucleation of aerosols and their interactions among themselves and with exhaust gases are summarized. Microphysical properties of contrail ice particles, formation of liquid ternary mixtures, and nucleation of nitric acid trihydrate particles in contrails are examined and possible implications for heterogeneous plume chemistry are discussed. (author) 19 refs.

  19. The Impact of Nursing Students' Prior Chemistry Experience on Academic Performance and Perception of Relevance in a Health Science Course

    Science.gov (United States)

    Boddey, Kerrie; de Berg, Kevin

    2015-01-01

    Nursing students have typically found the study of chemistry to be one of their major challenges in a nursing course. This mixed method study was designed to explore how prior experiences in chemistry might impact chemistry achievement during a health science unit. Nursing students (N = 101) studying chemistry as part of a health science unit were…

  20. 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 ).

  1. 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)

  2. [Special impact of supramolecular chemistry on Chinese medicine theories].

    Science.gov (United States)

    He, Fu-Yuan; Zhou, Yi-Qun; Deng, Kai-Wen; Deng, Jun-Lin; Shi, Ji-Lian; Liu, Wen-Long; Yang, Yan-Tao; Tang, Yu; Liu, Zhi-Gang

    2014-04-01

    The paper aimed to elucidate the specific impact of supramolecular chemistry on the Chinese medicine theories (CMT) in their modernization, after had summarized up the research status of supramolecular chemistry and analyzed the possible supramolecular forms of Chinese medicine (CM), as well as considered the problems in modernization of CM theories. On comparison of the classical chemistry that delt with chemical bonds among atoms, the supramolecular chemistry was rather concerned with varietes of weak noncovalent bonds intermolecules, and reflected the macro-apparent chemical properties of each molecules, and was the most appropriate chemical theories to explain the CMT and microcosmic materials. The molecules in the human body and Chinese material medica (CMM) formed supramolecules by way of self-assembly, self-organization, self-recognition and self-replication, with themselves or with complexation, composition, chelation, inclusion, neutralization etc. Meridian and Zang-fu viscera in CMT might be a space channel structure continuously consisted of unique molecules cavity that was imprinted with the supramolecularly template inside and outside of cells, through which the molecules in CMM interacted with the meridian and Zang-fu viscera. When small molecules in human body imprinted with macromolecules in meridian and Zang-fu viscera, in other words, they migrated along within imprinting channels of meridian and Zang-fu viscera on behavior of "Qi chromatography" impulsed by the heart beat, finally showed up on macroscopic the anisotropy of tissue and organ, as described namely as visceral manifestation in Chinese medical science. When small molecules in CMM interacted with imprinting channel on meridian and Zang-fu viscera, the natural properties and efficacy regularities of CMM was reflected on macroscopic. Therefore, the special representation forms of basic CMT is based on the macroscopic expression of "Qi chromatography" abided by imprinting effect

  3. 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.

  4. GESAMP Working Group 38, The Atmospheric Input of Chemicals to the Ocean

    Science.gov (United States)

    Duce, Robert; Liss, Peter

    2014-05-01

    There is growing recognition of the impact of the atmospheric input of both natural and anthropogenic substances on ocean chemistry, biology, and biogeochemistry as well as climate. These inputs are closely related to a number of important global change issues. For example, the increasing input of anthropogenic nitrogen species from the atmosphere to much of the ocean may cause a low level fertilization that could result in an increase in marine 'new' productivity of up to ~3% and thus impact carbon drawdown from the atmosphere. Similarly, much of the oceanic iron, which is a limiting nutrient in significant areas of the ocean, originates from the atmospheric input of minerals as a result of the long-range transport of mineral dust from continental regions. The increased supply of soluble phosphorus from atmospheric anthropogenic sources (through large-scale use of fertilizers) may also have a significant impact on surface-ocean biogeochemistry, but estimates of any effects are highly uncertain. There have been few assessments of the atmospheric inputs of sulfur and nitrogen oxides to the ocean and their impact on the rates of ocean acidification. These inputs may be particularly critical in heavily trafficked shipping lanes and in ocean regions proximate to highly industrialized land areas. Other atmospheric substances may also have an impact on the ocean, in particular lead, cadmium, and POPs. To address these and related issues the United Nations Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP) initiated Working Group 38, The Atmospheric Input of Chemicals to the Ocean, in 2008. This Working Group has had four meetings. To date four peer reviewed papers have been produced from this effort, with a least eight others in the process of being written or published. This paper will discuss some of the results of the Working Group's deliberations and its plans for possible future work.

  5. Biological aerosol particles in the atmosphere and their impact on clouds (BIOCLOUDS)

    Science.gov (United States)

    Amato, Pierre; Attard, Eleonore; Deguillaume, Laurent; Delort, Anne-Marie; Flossmann, Andrea; Good, Nicholas; Joly, Muriel; Koop, Thomas; Möhler, Ottmar; Monier, Marie; Morris, Cindy; Oehm, Caroline; Pöschl, Ulrich; Sancelme, Martine

    2015-04-01

    , IN activity of bacteria was followed with time, our results suggest that bacteria are precipitated in the cloud chamber as a result of their IN activity. Also the coating of bacteria with sulfates decreased their IN activity, pointing out the negative potential anthropogenic influence on IN bacteria activity. 3. Modeling study to see if any impact of bacteria on cloud development and/or precipitation is realistic. Modeling studies were performed with DESCAM (Detailed SCAvenging Model) using as an input the new data from the different campaigns in AIDA. M. VAÏTILINGOM et al. Atmospheric Environment, 2012, 56, 88-100. E. ATTARD et al. Atmospheric Chemistry and Physics, 2012, 12, 10667-10677. M. JOLY et al. Atmospheric Environment, 2013, 70, 392-400.

  6. 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.

  7. Investigating the Longitudinal Impact of a Successful Reform in General Chemistry on Student Enrollment and Academic Performance

    Science.gov (United States)

    Lewis, Scott E.

    2014-01-01

    Considerable effort in chemistry education research has been dedicated to developing and evaluating reform pedagogies designed to improve student success in general chemistry. Policy recommendations propose adoption of these techniques as a means to increase the number of science graduates, however there is the potential that the impact of these…

  8. Estimation of NH3 emissions from a naturally ventilated livestock farm using local-scale atmospheric dispersion modelling

    Czech Academy of Sciences Publication Activity Database

    Hensen, A.; Loubet, B.; Mosquera, J.; van den Bulk, W. C. M.; Erisman, J. W.; Daemmgen, U.; Milford, C.; Loepmeier, F. J.; Cellier, P.; Mikuška, Pavel; Sutton, M. A.

    2009-01-01

    Roč. 6, č. 12 (2009), s. 2847-2860 ISSN 1726-4170 Institutional research plan: CEZ:AV0Z40310501 Keywords : NH3 livestock farm emissions * concentration measurement * atmospheric dispersion Subject RIV: CB - Analytical Chemistry, Separation Impact factor: 3.246, year: 2009 http://www.biogeosciences.net/6/2847/2009/

  9. Molecular Structure of Salt Solutions: A New View of the Interface with Implications for Heterogeneous Atmospheric Chemistry

    Czech Academy of Sciences Publication Activity Database

    Jungwirth, Pavel; Tobias, D. J.

    2001-01-01

    Roč. 105, č. 43 (2001), s. 10468-10472 ISSN 1089-5647 R&D Projects: GA MŠk LN00A032 Institutional research plan: CEZ:AV0Z4040901 Keywords : air-solution interface * salt solutions * molecular dynamics Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.379, year: 2001

  10. Combustion's impact on the global atmosphere

    International Nuclear Information System (INIS)

    Prather, M.J.; Logan, J.A.

    1994-01-01

    The combustion of a hydrocarbon fuel removes molecular oxygen (O 2 ) from the atmosphere and releases equivalent amounts of water (H 2 ) and carbon dioxide (CO 2 ), almost always with trace amounts of numerous other compounds including hydrocarbon (CH 4 , C 2 H 2 , C 2 H 4 , C 2 H 6 , C 3 H 8 , C 6 H 6 , CH 3 CHO, etc.), carbon monoxide (CO), nitrogen oxides (NO, N 2 O) and reduced nitrogen (NH 3 and HCN), sulfur gases (SO 2 , OCS, CS 2 ), halocarbons (CH 3 Al and CH 3 Br), and particles. A review of the atmospheric budgets of these gases shows that burning of fossil fuels and recent biomass has led to global alterations in the composition of the atmosphere. Combustion is clearly responsible for most of the enhanced greenhouse forcing to date (through CO 2 , tropospheric O 3 , soot) and also some counteracting effects (through SO 2 ). It has had minimal impact on stratospheric O 3 (through CH 3 Cl, CH 3 Br, CH 4 ), but has likely changed the tropospheric oxidant levels (through CO, NO x , NMHC), at least over the northern hemisphere. Most of the important greenhouse gases and tropospheric oxidant gases have significant natural sources, which are not well defined today and may be changing; and thus, quantifying the role of combustion is difficult. 113 refs

  11. Impacts of heterogeneous reactions to atmospheric peroxides: Observations and budget analysis study

    Science.gov (United States)

    Qin, Mengru; Chen, Zhongming; Shen, Hengqing; Li, Huan; Wu, Huihui; Wang, Yin

    2018-06-01

    Atmospheric peroxides play important roles in atmospheric chemistry, acting as reactive oxidants and reservoirs of HOX and ROX radicals. Field measurements of atmospheric peroxides were conducted over urban Beijing from 2015 to 2016, including dust storm days, haze days and different seasons. We employed a box model based on RACM2 mechanism to conduct concentration simulation and budget analysis of hydrogen peroxide (H2O2) and peroxyacetic acid (PAA). In this study, heterogeneous reaction is found to be a significant sink for atmospheric H2O2 and PAA in urban Beijing. Here, we recommend a suitable uptake coefficient formula considering the water effect for model research of peroxides. It is found that H2O2 and PAA unexpectedly maintained considerable concentrations on haze days, even higher than that on non-haze days. This phenomenon is mainly ascribed to relatively high levels of volatile organic compounds and ozone on haze days. In addition, high levels of water vapor in pollution episode can promote not only the heterogeneous uptake to aerosol phase but also the production of H2O2. Atmospheric PAA formation is suggested to be sensitive to alkenes and NOX in urban Beijing. In particular, with the help of peroxides, sulfate formation rate from heterogeneous uptake could increase by ∼4 times on haze days, indicating the potential effect of peroxides on enhancement of aerosol oxidative property and secondary sulfate formation.

  12. 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

  13. The Impact of Iodide-Mediated Ozone Deposition and Halogen Chemistry on Surface Ozone Concentrations Across the Continental United States

    Science.gov (United States)

    The air quality of many large coastal areas in the United States is affected by the confluence of polluted urban and relatively clean marine airmasses, each with distinct atmospheric chemistry. In this context, the role of iodide-mediated ozone (O3) deposition over seawater and m...

  14. Amine chemistry. Update on impact on resin

    International Nuclear Information System (INIS)

    Bachman, Gregory; Kellogg, Douglas; Wilkes, Marty

    2012-01-01

    Impurity removal in the steam cycle and the associated prevention of corrosion and/or fouling of system components are the goals of ion exchange resins. However, in many instances (such as a switch to amine chemistry or a change in product specifications), resins do not remove, and, in fact, contribute impurities to the steam cycle. This paper reviews recent data compiled to determine the direct and indirect effects of amines on ion exchange resins used in the power industry. Water chemistries have improved in recent years, in large part due to changes in chemistry and resins, but it is necessary to continue to develop products, processes and techniques to reduce impurities and improve overall water chemistry in power plant systems. (orig.)

  15. Amine chemistry. Update on impact on resin

    Energy Technology Data Exchange (ETDEWEB)

    Bachman, Gregory; Kellogg, Douglas [Siemens Industry, Inc., Rockford, IL (United States). Technology and Lab Services; Wilkes, Marty [Siemens Industry, Inc., Rockford, IL (United States). Water Technologies Div.

    2012-03-15

    Impurity removal in the steam cycle and the associated prevention of corrosion and/or fouling of system components are the goals of ion exchange resins. However, in many instances (such as a switch to amine chemistry or a change in product specifications), resins do not remove, and, in fact, contribute impurities to the steam cycle. This paper reviews recent data compiled to determine the direct and indirect effects of amines on ion exchange resins used in the power industry. Water chemistries have improved in recent years, in large part due to changes in chemistry and resins, but it is necessary to continue to develop products, processes and techniques to reduce impurities and improve overall water chemistry in power plant systems. (orig.)

  16. 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.

  17. Impact of Instructional Decisions on the Effectiveness of Cooperative Learning in Chemistry through Meta-Analysis

    Science.gov (United States)

    Apugliese, Andrew; Lewis, Scott E.

    2017-01-01

    Meta-analysis can provide a robust description of the impact of educational reforms and also offer an opportunity to explore the conditions where such reforms are more or less effective. This article describes a meta-analysis on the impact of cooperative learning on students' chemistry understanding. Modifiers in the meta-analysis are purposefully…

  18. 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

  19. 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

  20. Impact of finite rate chemistry on the hydrodynamic stability of shear flows in turbulent lean premixed combustion

    Science.gov (United States)

    Dagan, Yuval; Ghoniem, Ahmed

    2017-11-01

    Recent experimental observations show that the dynamic response of a reactive flow is strongly impacted by the fuel chemistry. In order to gain insight into some of the underlying mechanisms we formulate a new linear stability model that incorporates the impact of finite rate chemistry on the hydrodynamic stability of shear flows. Contrary to previous studies which typically assume that the velocity field is independent of the kinetic rates, the velocity field in our study is coupled with the temperature field. Using this formulation, we reproduce previous results, e.g., most unstable global modes, obtained for non-reacting shear flow. Moreover, we show that these modes are significantly altered in frequency and gain by the presence of a reaction region within the shear layer. This qualitatively agrees with results of our recent experimental and numerical studies, which show that the flame surface location relative to the shear layer influences the stability characteristics in combustion tunnels. This study suggests a physical explanation for the observed impact of finite rate chemistry on shear flow stability.

  1. Impact of chemistry on Standard High Solids Vessel Design mixing

    Energy Technology Data Exchange (ETDEWEB)

    Poirier, M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-03-02

    The plan for resolving technical issues regarding mixing performance within vessels of the Hanford Waste Treatment Plant Pretreatment Facility directs a chemical impact study to be performed. The vessels involved are those that will process higher (e.g., 5 wt % or more) concentrations of solids. The mixing equipment design for these vessels includes both pulse jet mixers (PJM) and air spargers. This study assesses the impact of feed chemistry on the effectiveness of PJM mixing in the Standard High Solids Vessel Design (SHSVD). The overall purpose of this study is to complement the Properties that Matter document in helping to establish an acceptable physical simulant for full-scale testing. The specific objectives for this study are (1) to identify the relevant properties and behavior of the in-process tank waste that control the performance of the system being tested, (2) to assess the solubility limits of key components that are likely to precipitate or crystallize due to PJM and sparger interaction with the waste feeds, (3) to evaluate the impact of waste chemistry on rheology and agglomeration, (4) to assess the impact of temperature on rheology and agglomeration, (5) to assess the impact of organic compounds on PJM mixing, and (6) to provide the technical basis for using a physical-rheological simulant rather than a physical-rheological-chemical simulant for full-scale vessel testing. Among the conclusions reached are the following: The primary impact of precipitation or crystallization of salts due to interactions between PJMs or spargers and waste feeds is to increase the insoluble solids concentration in the slurries, which will increase the slurry yield stress. Slurry yield stress is a function of pH, ionic strength, insoluble solids concentration, and particle size. Ionic strength and chemical composition can affect particle size. Changes in temperature can affect SHSVD mixing through its effect on properties such as viscosity, yield stress, solubility

  2. Understanding the Impact of a General Chemistry Course on Students' Transition to Organic Chemistry

    Science.gov (United States)

    Collins-Webb, Alexandra; Jeffery, Kathleen A.; Sweeder, Ryan D.

    2016-01-01

    The move from general chemistry to organic chemistry can be a challenge for students as it often involves a transition from quantitatively-oriented to mechanistically-oriented thinking. This study found that the design of the general chemistry course can change the student experience of this transition as assessed by a reflective survey. The…

  3. 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.

  4. Atmospheric Aerosol Properties and Climate Impacts

    Science.gov (United States)

    Chin, Mian; Kahn, Ralph A.; Remer, Lorraine A.; Yu, Hongbin; Rind, David; Feingold, Graham; Quinn, Patricia K.; Schwartz, Stephen E.; Streets, David G.; DeCola, Phillip; hide

    2009-01-01

    This report critically reviews current knowledge about global distributions and properties of atmospheric aerosols, as they relate to aerosol impacts on climate. It assesses possible next steps aimed at substantially reducing uncertainties in aerosol radiative forcing estimates. Current measurement techniques and modeling approaches are summarized, providing context. As a part of the Synthesis and Assessment Product in the Climate Change Science Program, this assessment builds upon recent related assessments, including the Fourth Assessment Report of the Intergovernmental Panel on Climate Change (IPCC AR4, 2007) and other Climate Change Science Program reports. The objectives of this report are (1) to promote a consensus about the knowledge base for climate change decision support, and (2) to provide a synthesis and integration of the current knowledge of the climate-relevant impacts of anthropogenic aerosols for policy makers, policy analysts, and general public, both within and outside the U.S government and worldwide.

  5. 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.

  6. Impact of Atmospheric Albedo on Amazon Evapotranspiration

    Science.gov (United States)

    Lopes, A. V.; Thompson, S. E.; Dracup, J. A.

    2013-12-01

    The vulnerability of the Amazon region to climate and anthropogenic driven disturbances has been the subject of extensive research efforts, given its importance in the global and regional climate and ecologic systems. The evaluation of such vulnerabilities requires the proper understanding of physical mechanisms controlling water and energy balances and how the disturbances change them. Among those mechanisms, the effects of atmospheric albedo on evapotranspiration have not been fully explored yet and are explored in this study. Evapotranspiration in the Amazon is sustained at high levels across all seasons and represents a large fraction of water and energy surface budgets. In this study, statistical analysis of data from four flux towers installed at Amazon primary forest sites was employed to quantify the impact of atmospheric albedo, mostly resulted from cloudiness, on evapotranspiration and to compare it to the effect of water limitation. Firstly, the difference in eddy-flux derived evapotranspiration at the flux towers under rainy and non-rainy antecedent conditions was tested for significance. Secondly, the same statistical comparison was performed under cloudy and clear sky conditions at hourly and daily time scales, using the reduction in incoming solar radiation as an indicator of cloudiness. Finally, the sensitivity of seasonal evapotranspiration totals to atmospheric albedo resulted from rainfall patterns is evaluated. That was done by sampling daily evapotranspiration estimates from empirical probability distribution functions conditioned to rainfall occurrence and then varying the number of dry days in each season. It was found that light limitation is much more important than water limitation in the Amazon, resulting in up to 43% reduction in daily evapotranspiration. Also, this effect varies by location and by season, the largest impact being in wet season, from December do January. Moreover, seasonal evapotranspiration totals were found to be

  7. A High Five for ChemistryOpen.

    Science.gov (United States)

    Peralta, David; Ortúzar, Natalia

    2016-02-01

    Fabulous at five! When ChemistryOpen was launched in 2011, it was the first society-owned general chemistry journal to publish open-access articles exclusively. Five years down the line, it has featured excellent work in all fields of chemistry, leading to an impressive first full impact factor of 3.25. In this Editorial, read about how ChemistryOpen has grown over the past five years and made its mark as a high-quality open-access journal with impact.

  8. Impact of marine mercury cycling on coastal atmospheric mercury concentrations in the North- and Baltic Sea region

    Directory of Open Access Journals (Sweden)

    Johannes Bieser

    2016-06-01

    Full Text Available Abstract The cycling of mercury between ocean and atmosphere is an important part of the global Hg cycle. Here we study the regional contribution of the air-sea exchange in the North- and Baltic Sea region. We use a newly developed coupled regional chemistry transport modeling (CTM system to determine the flux between atmosphere and ocean based on the meteorological model COSMO-CLM, the ocean-ecosystem model ECOSMO, the atmospheric CTM CMAQ and a newly developed module for mercury partitioning and speciation in the ocean (MECOSMO. The model was evaluated using atmospheric observations of gaseous elemental mercury (GEM, surface concentrations of dissolved gaseous mercury (DGM, and air-sea flux (ASF calculations based on observations made on seven cruises in the western and central Baltic Sea and three cruises in the North Sea performed between 1991 and 2006. It was shown that the model is in good agreement with observations: DGM (Normalized Mean Bias NMB=-0.27 N=413, ASF (NMB=-0.32, N=413, GEM (NMB=0.07, N=2359. Generally, the model was able to reproduce the seasonal DGM cycle with the best agreement during winter and autumn (NMBWinter=-0.26, NMBSpring=-0.41, NMBSummer=-0.29, NMBAutumn=-0.03. The modelled mercury evasion from the Baltic Sea ranged from 3400 to 4000 kg/a for the simulation period 1994–2007 which is on the lower end of previous estimates. Modelled atmospheric deposition, river inflow and air-sea exchange lead to an annual net Hg accumulation in the Baltic Sea of 500 to 1000 kg/a. For the North Sea the model calculates an annual mercury flux into the atmosphere between 5700 and 6000 kg/a. The mercury flux from the ocean influenced coastal atmospheric mercury concentrations. Running CMAQ coupled with the ocean model lead to better agreement with GEM observations. Directly at the coast GEM concentrations could be increased by up to 10% on annual average and observed peaks could be reproduced much better. At stations 100km downwind

  9. 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/

  10. 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...

  11. 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

  12. 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.

  13. Green Chemistry Metrics with Special Reference to Green Analytical Chemistry

    OpenAIRE

    Marek Tobiszewski; Mariusz Marć; Agnieszka Gałuszka; Jacek Namieśnik

    2015-01-01

    The concept of green chemistry is widely recognized in chemical laboratories. To properly measure an environmental impact of chemical processes, dedicated assessment tools are required. This paper summarizes the current state of knowledge in the field of development of green chemistry and green analytical chemistry metrics. The diverse methods used for evaluation of the greenness of organic synthesis, such as eco-footprint, E-Factor, EATOS, and Eco-Scale are described. Both the well-establis...

  14. 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

  15. 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

  16. 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

  17. Publicising chemistry in a multicultural society through chemistry outreach

    Directory of Open Access Journals (Sweden)

    Joyce D. Sewry

    2011-11-01

    Full Text Available Given the emphasis in Higher Education on community engagement in South Africa and the importance of international collaboration, we discuss a joint approach to chemistry outreach in two countries on two continents with widely differing target school audiences. We describe the history of the partnership between the chemistry departments at Rhodes University and the University of Bristol and provide an outline of the chemistry content of their outreach initiatives, the modes of delivery, the advantages to both departments and their students for involvement in various levels of outreach, the challenges they still face and additional opportunities that such work facilitated. The lecture demonstration ‘A Pollutant’s Tale’ was presented to thousands of learners all over the world, including learners at resource-deprived schools in South Africa. Challenges to extend outreach activities in South Africa include long travelling distances, as well as a lack of facilities (such as school halls and electricity at schools. Outreach activities not only impacted on the target audience of young learners, they also impacted upon the postgraduate and other chemistry students taking part in these initiatives. This collaboration strengthened both institutions and their outreach work and may also lead to chemistry research collaborations between the academics involved.

  18. African land degradation in a world of global atmospheric change: fertilization conceals degradation?

    Science.gov (United States)

    Le, Lulseged Tamene, Paul L. G. Vlek, Quang Bao

    2009-04-01

    Land degradation is one of the most widespread environmental problems worldwide. The sub-Saharan Africa (SSA) is one of the most seriously affected regions with huge implications on food security and economic development. To plan plausible management measures, understanding the magnitude of the problem and identification of hotspot areas are necessary. Analysis of remote sensing and climate data observed from space for the period 1982 - 2003 showed significant improvement in vegetation productivity across 30% of SSA with decline on 5% of the subcontinent. Global change in atmospheric chemistry is likely responsible for the observed increasing trend in vegetation productivity. Such widespread greening observed from space could mask anthropogenic land degradation processes such as land conversion, selective logging, and soil nutrient mining. To assess this possible masking effect, a re-analysis of the vegetation productivity dynamics, taking into account atmospheric fertilization, was conducted. This was performed by analyzing the long-term trend in vegetation productivity of pristine lands (areas with minimum human- and climate- related impacts) identified across different biomes in SSA. The baseline slope values of biomass accrual calculated for those pristine lands were estimated and used to re-calculate the long-term trend of green biomass with and without the impact of atmospheric fertilization. This ultimately enabled to delineate the areas that would have experienced significant loss in vegetation productivity had the atmospheric chemistry not changed. The result suggests that seven times more than the area of actual productivity decline in SSA is affected by land degradation processes that are concealed by atmospheric fertilization. With this rate of surreptitious loss of vital land attributes and with the current rate of population growth (3%), the SSA subcontinent may soon lack the land resources necessary to foster economic development. Spatially

  19. 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…

  20. The fate of Mercury in Arctic regions: New understanding of atmospheric chemical processes and mercury stability in snow.

    Science.gov (United States)

    Steffen, A.; Ferrari, C.; Dommergue, A.; Scherz, T.; Lawson, G.; Leiatch, R.

    2006-12-01

    Mercury is a known toxic pollutant in the Arctic environment. Atmospheric mercury depletion events (AMDEs) have been studied in the Arctic since 1995. While advances in understanding this newly discovered cycling of mercury in the atmosphere have been made, much of the chemistry and the impact of this annually reoccurring event to the Arctic ecosystem are not well understood. Four years of continuous measurements at Alert, Canada of so-called reactive gaseous mercury (RGM) and mercury associated to particles (PHg) coupled with ongoing snow sampling have produced new information on the atmospheric chemistry and deposition of these mercury species to the Arctic. A distinct pattern during the springtime period in the distribution of these atmospheric mercury species has emerged. This pattern is characterized by the predominance of PHg concentration at the onset of the AMDEs. During the latter part of the AMDE season, there is an obvious swicth in the speciation of mercury to RGM as the main component during AMDEs. This swicth from PHg to RGM is clearly linked to a significant increase of mercury in the snow. In addition, concentrations of PHg are clearly linked with particles in the air that are primarily associated with Arctic haze. Recently, similar results have also been observed in Ny-Alesund (Svalbard). Further observations indicate that once deposited, the deposited mercury appears to evolve chemically in the snow. This change in mercury may impact the transfer of mercury to the environment during snow melt. These first time observed links between atmospheric conditions and subsequent deposition of mercury may help to ascertain the conditions throughout the Arctic as to when significant deposition of mercury will occur. It is proposed that should the concentration of atmospheric particles increase in the Arctic due to long range transport from emission sources, an increase in the deposition of mercury to this environment will increase during the springtime

  1. Molecular dynamics simulations of small halogenated organics at the air-water interface: implications in water treatment and atmospheric chemistry

    Czech Academy of Sciences Publication Activity Database

    Habartová, Alena; Valsaraj, K. T.; Roeselová, Martina

    2013-01-01

    Roč. 117, č. 38 (2013), s. 9205-9215 ISSN 1089-5639 R&D Projects: GA ČR GA13-06181S Institutional support: RVO:61388963 Keywords : aerosol * air bubbles * interfacial concentration Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.775, year: 2013

  2. Zhamanshin astrobleme provides evidence for carbonaceous chondrite and post-impact exchange between ejecta and Earth's atmosphere

    Czech Academy of Sciences Publication Activity Database

    Magna, T.; Žák, Karel; Pack, A.; Moynier, F.; Mougel, B.; Peters, S.; Skála, Roman; Jonášová, Šárka; Mizera, Jiří; Řanda, Zdeněk

    2017-01-01

    Roč. 8, AUG 9 2017 (2017), č. článku 227. ISSN 2041-1723 R&D Projects: GA ČR GA13-22351S Institutional support: RVO:67985831 ; RVO:61389005 Keywords : chondrite * moldavites * Zhamanshin astrobleme, Kazakhstan Subject RIV: DB - Geology ; Mineralogy; CB - Analytical Chemistry, Separation (UJF-V) OBOR OECD: Geology; Analytical chemistry (UJF-V) Impact factor: 12.124, year: 2016

  3. The use of high impact practices (HIPs) on chemistry lesson design and implementation by pre-service teachers

    Science.gov (United States)

    Chamrat, Suthida; Apichatyotin, Nattaya; Puakanokhirun, Kittaporn

    2018-01-01

    The quality of lesson design is essential to learning effectiveness. Research shows some characteristics of lessons have strong effect on learning which were grouped into "High Impact Practices or HIPs. This research aims to examine the use of HIPs on chemistry lesson design as a part of Teaching Science Strand in Chemistry Concepts course. At the first round of lesson design and implementing in classroom, 14 chemistry pre-services teachers freely selected topics, designed and implemented on their own ideas. The lessons have been reflected by instructors and their peers. High Impact Practices were overtly used as the conceptual framework along with the After-Action Review and Reflection (AARR). The selected High Impact practice in this study consisted of 6 elements: well-designed lesson, vary cognitive demand/academic challenge, students center approach, opportunity of students to reflect by discussion or writing, the assignment of project based learning or task, and the lesson reflects pre-service teachers' Technological Pedagogical Content Knowledge (TPACK). The second round, pre-service teachers were encouraged to explicitly used 6 High Impact Practices in cooperated with literature review specified on focused concepts for bettering designed and implemented lessons. The data were collected from 28 lesson plans and 28 classroom observations to compare and discuss between the first and second lesson and implementation. The results indicated that High Impact Practices effect on the quality of delivered lesson. However, there are some elements that vary on changes which were detailed and discussed in this research article.

  4. The impact of relative humidity and atmospheric pressure on mortality in Guangzhou, China.

    Science.gov (United States)

    Ou, Chun Quan; Yang, Jun; Ou, Qiao Qun; Liu, Hua Zhang; Lin, Guo Zhen; Chen, Ping Yan; Qian, Jun; Guo, Yu Ming

    2014-12-01

    Although many studies have examined the effects of ambient temperatures on mortality, little evidence is on health impacts of atmospheric pressure and relative humidity. This study aimed to assess the impacts of atmospheric pressure and relative humidity on mortality in Guangzhou, China. This study included 213,737 registered deaths during 2003-2011 in Guangzhou, China. A quasi-Poisson regression with a distributed lag non-linear model was used to assess the effects of atmospheric pressure/relative humidity. We found significant effect of low atmospheric pressure/relative humidity on mortality. There was a 1.79% (95% confidence interval: 0.38%-3.22%) increase in non-accidental mortality and a 2.27% (0.07%-4.51%) increase in cardiovascular mortality comparing the 5th and 25th percentile of atmospheric pressure. A 3.97% (0.67%-7.39%) increase in cardiovascular mortality was also observed comparing the 5th and 25th percentile of relative humidity. Women were more vulnerable to decrease in atmospheric pressure and relative humidity than men. Age and education attainment were also potential effect modifiers. Furthermore, low atmospheric pressure and relative humidity increased temperature-related mortality. Both low atmospheric pressure and relative humidity are important risk factors of mortality. Our findings would be helpful to develop health risk assessment and climate policy interventions that would better protect vulnerable subgroups of the population. Copyright © 2014 The Editorial Board of Biomedical and Environmental Sciences. Published by China CDC. All rights reserved.

  5. Impact of sea ice cover changes on the Northern Hemisphere atmospheric winter circulation

    Directory of Open Access Journals (Sweden)

    D. Handorf

    2012-01-01

    Full Text Available The response of the Arctic atmosphere to low and high sea ice concentration phases based on European Center for Medium-Range Weather Forecast (ECMWF Re-Analysis Interim (ERA-Interim atmospheric data and Hadley Centre's sea ice dataset (HadISST1 from 1989 until 2010 has been studied. Time slices of winter atmospheric circulation with high (1990–2000 and low (2001–2010 sea ice concentration in the preceding August/September have been analysed with respect to tropospheric interactions between planetary and baroclinic waves. It is shown that a changed sea ice concentration over the Arctic Ocean impacts differently the development of synoptic and planetary atmospheric circulation systems. During the low ice phase, stronger heat release to the atmosphere over the Arctic Ocean reduces the atmospheric vertical static stability. This leads to an earlier onset of baroclinic instability that further modulates the non-linear interactions between baroclinic wave energy fluxes on time scales of 2.5–6 d and planetary scales of 10–90 d. Our analysis suggests that Arctic sea ice concentration changes exert a remote impact on the large-scale atmospheric circulation during winter, exhibiting a barotropic structure with similar patterns of pressure anomalies at the surface and in the mid-troposphere. These are connected to pronounced planetary wave train changes notably over the North Pacific.

  6. Impact of a future H2-based road transportation sector on the composition and chemistry of the atmosphere - Part 2: Stratospheric ozone

    Science.gov (United States)

    Wang, D.; Jia, W.; Olsen, S. C.; Wuebbles, D. J.; Dubey, M. K.; Rockett, A. A.

    2013-07-01

    The prospective future adoption of molecular hydrogen (H2) to power the road transportation sector could greatly improve tropospheric air quality but also raises the question of whether the adoption would have adverse effects on the stratospheric ozone. The possibility of undesirable impacts must be fully evaluated to guide future policy decisions. Here we evaluate the possible impact of a future (2050) H2-based road transportation sector on stratospheric composition and chemistry, especially on the stratospheric ozone, with the MOZART (Model for OZone And Related chemical Tracers) model. Since future growth is highly uncertain, we evaluate the impact of two world evolution scenarios, one based on an IPCC (Intergovernmental Panel on Climate Change) high-emitting scenario (A1FI) and the other on an IPCC low-emitting scenario (B1), as well as two technological options: H2 fuel cells and H2 internal combustion engines. We assume a H2 leakage rate of 2.5% and a complete market penetration of H2 vehicles in 2050. The model simulations show that a H2-based road transportation sector would reduce stratospheric ozone concentrations as a result of perturbed catalytic ozone destruction cycles. The magnitude of the impact depends on which growth scenario evolves and which H2 technology option is applied. For the evolution growth scenario, stratospheric ozone decreases more in the H2 fuel cell scenarios than in the H2 internal combustion engine scenarios because of the NOx emissions in the latter case. If the same technological option is applied, the impact is larger in the A1FI emission scenario. The largest impact, a 0.54% decrease in annual average global mean stratospheric column ozone, is found with a H2 fuel cell type road transportation sector in the A1FI scenario; whereas the smallest impact, a 0.04% increase in stratospheric ozone, is found with applications of H2 internal combustion engine vehicles in the B1 scenario. The impacts of the other two scenarios fall

  7. Sulfur mass loading of the atmosphere from volcanic eruptions: Calibration of the ice core record on basis of sulfate aerosol deposition in polar regions from the 1982 El Chichon eruption

    Science.gov (United States)

    Sigurdsson, Haraldur; Laj, Paolo

    1990-01-01

    Major volcanic eruptions disperse large quantities of sulfur compound throughout the Earth's atmosphere. The sulfuric acid aerosols resulting from such eruptions are scavenged by snow within the polar regions and appear in polar ice cores as elevated acidity layers. Glacio-chemical studies of ice cores can, thus, provide a record of past volcanism, as well as the means for understanding the fate of volcanic sulfur in the atmosphere. The primary objectives of this project are to study the chemistry and physical properties of volcanic fallout in a Greenland Ice Core in order to evaluate the impact of the volcanic gases on the atmospheric chemistry and the total atmospheric mass of volcanic aerosols emitted by major volcanic eruptions. We propose to compare the ice core record to other atmospheric records performed during the last 10 years to investigate transport and deposition of volcanic materials.

  8. The impact of a future H2-based road transportation sector on the composition and chemistry of the atmosphere - Part 2: Stratospheric ozone

    Science.gov (United States)

    Wang, D.; Jia, W.; Olsen, S. C.; Wuebbles, D. J.; Dubey, M. K.; Rockett, A. A.

    2012-08-01

    The prospective future adoption of hydrogen to power the road transportation sector could greatly improve tropospheric air quality but also raises the question whether the adoption would have adverse effects on stratospheric ozone. The possibility of these undesirable impacts must be fully evaluated to guide future policy decisions. Here we evaluate the possible impact of a future (2050) H2-based road transportation sector on stratospheric composition and chemistry, especially on stratospheric ozone, with the MOZART chemical transport model. Since future growth is highly uncertain we evaluate the impact for two world evolution scenarios, one based on a high emitting scenario (IPCC A1FI) and the other on a low emitting scenario (IPCC B1), as well as two technological options: H2 fuel cells and H2 internal combustion engines. We assume a H2 leakage rate of 2.5% and a complete market penetration of H2 vehicles in 2050. The model simulations show that a H2-based road transportation sector would reduce stratospheric ozone concentrations as a result of perturbed catalytic ozone destruction cycles. The magnitude of the impact depends on which growth scenario the world evolves and which H2 technology option is applied. For the same world evolution scenario, stratospheric ozone decreases more in the H2 fuel cell scenarios than in the H2 internal combustion engine scenarios because of the NOx emissions in the latter case. If the same technological option is applied, the impact is larger in the A1FI emission scenario. The largest impact, a 0.54% decrease in annual average global mean stratospheric column ozone, is found with a H2 fuel cell type road transportation sector in the A1FI scenario; whereas the smallest impact, a 0.04% increase in stratospheric ozone, is found with applications of H2 internal combustion engine vehicles in the B1 scenario. The impacts of the other two scenarios fall between the above two bounding scenarios. However, the magnitude of these changes is

  9. Titanocene sulfide chemistry

    Czech Academy of Sciences Publication Activity Database

    Horáček, Michal

    2016-01-01

    Roč. 314, MAY 2016 (2016), s. 83-102 ISSN 0010-8545 R&D Projects: GA ČR(CZ) GAP207/12/2368 Institutional support: RVO:61388955 Keywords : titanocene sulfide chemistry * photolysis * titanocene hydrosulfides Ti-(SH)n Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 13.324, year: 2016

  10. 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.

  11. 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

  12. 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

  13. 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

  14. 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.

  15. 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

  16. Effective Chemistry Communication in Informal Environments

    Science.gov (United States)

    National Academies Press, 2016

    2016-01-01

    Chemistry plays a critical role in daily life, impacting areas such as medicine and health, consumer products, energy production, the ecosystem, and many other areas. Communicating about chemistry in informal environments has the potential to raise public interest and understanding of chemistry around the world. However, the chemistry community…

  17. Atmospheric photochemistry at a fatty acid coated air/water interface

    Science.gov (United States)

    George, Christian; Rossignol, Stéphanie; Passananti, Monica; Tinel, Liselotte; Perrier, Sebastien; Kong, Lingdong; Brigante, Marcello; Bianco, Angelica; Chen, Jianmin; Donaldson, James

    2017-04-01

    Over the past 20 years, interfacial processes have become increasingly of interest in the field of atmospheric chemistry, with many studies showing that environmental surfaces display specific chemistry and photochemistry, enhancing certain reactions and acting as reactive sinks or sources for various atmospherically relevant species. Many molecules display a free energy minimum at the air-water interface, making it a favored venue for compound accumulation and reaction. Indeed, surface active molecules have been shown to undergo specific photochemistry at the air-water interface. This presentation will address some recent surprises. Indeed, while fatty acids are believed to be photochemically inert in the actinic region, complex volatile organic compounds (VOCs) are produced during illumination of an air-water interface coated solely with a monolayer of carboxylic acid. When aqueous solutions containing nonanoic acid (NA) at bulk concentrations that give rise to just over monolayer NA coverage are illuminated with actinic radiation, saturated and unsaturated aldehydes are seen in the gas phase and more highly oxygenated products appear in the aqueous phase. This chemistry is probably initiated by triplet state NA molecules excited by direct absorption of actinic light at the water surface. As fatty acids covered interfaces are ubiquitous in the environment, such photochemical processing will have a significant impact on local ozone and particle formation. In addition, it was shown recently that a heterogeneous reaction between SO2 and oleic acid (OA; an unsaturated fatty acid) takes place and leads efficiently to the formation of organosulfur products. Here, we demonstrate that this reaction proceeds photochemically on various unsaturated fatty acids compounds, and may therefore have a general environmental impact. This is probably due to the chromophoric nature of the SO2 adduct with C=C bonds, and means that the contribution of this direct addition of SO2 could

  18. The impact of dynamic processes on chemistry in atmospheric boundary layers over tropical and boreal forest

    NARCIS (Netherlands)

    Ouwersloot, H.G.

    2013-01-01

    Improving our knowledge of the atmospheric processes that drive climate and air quality is very relevant for society. The application of this knowledge enables us to predict and mitigate the effects of human induced perturbations to our environment. Key factors in the current and future climate

  19. Characterization of regional atmospheric aerosols over Hungary by PIXE elemental analysis

    International Nuclear Information System (INIS)

    Koltay, E.; Szabo, G.; Borbely Kiss, I.; Somorjai, E.; Kiss, A.Z.

    1994-01-01

    Studying the characteristic features of atmospheric aerosols emitted by natural and anthropogenic sources is of basic importance for a detailed understanding of the physics and chemistry of the atmosphere. Environmental pollution by atmospheric aerosols and their impact can be tested in the same way, too. The separation of natural and anthropogenic components of the aerosol can be done through enrichment factors and size distribution curves deduced from analytical information. The Particle Induced X-ray Emission (PIXE) technique has been applied in aerosol studies by the authors. Results obtained on atmospheric aerosols collected over Hungary and presented in terms of concentrations, enrichment factors, regional signatures, deposition velocities, transport properties and apportionment of sources illustrate the scope and proportions of the potential contribution of PIXE to the methodology of atmospheric aerosol studies. Continued activity planned in the framework of the present CRP may widen the scope of the investigations mainly in the field of size-fractioned sampling and - possibly - in the direction of individual characterization of aerosol particles. (author). 14 refs

  20. Experimental research of the impact of the dosing of chemical reagents on the dynamic behavior of regulation system of cycle chemistry

    Science.gov (United States)

    Yegoshina, O. V.; Bolshakova, N. A.

    2017-11-01

    Organization of reliable chemical control for maintaining cycle chemistry is one of the most important problems to be solved at the present time the design and operation of thermal power plants. To maintain optimal parameters of cycle chemistry are used automated chemical control system and regulation system of dosing chemical reagents. Reliability and stability analyzer readings largely determine the reliability of the water cycle chemistry. Now the most common reagents are ammonia, alkali and film-forming amines. In this paper are presented the results of studies of the impact of concentration and composition of chemical reagents for readings stability of automatic analyzers and transients time of control systems for cycles chemistry. Research of the impact of chemical reagents on the dynamic behavior of regulation system for cycle chemistry was conducted at the experimental facility of the Department of thermal power stations of the Moscow Engineering Institute. This experimental facility is model of the work of regulation system for cycle chemistry close to the actual conditions on the energy facilities CHP. Analysis of results of the impact of chemical reagent on the dynamic behavior of ammonia and film forming amines dosing systems showed that the film-forming amines dosing system is more inertia. This emphasizes the transition process of the system, in which a half times longer dosing of ammonia. Results of the study can be used to improve the monitoring systems of water chemical treatment.

  1. Modeling of urban atmospheric pollution and impact on health

    International Nuclear Information System (INIS)

    Myrto, Valari

    2009-10-01

    The goal of this dissertation, is to develop a methodology that provides an improved knowledge of the associations between atmospheric contaminant concentrations and health impact. The propagation of uncertainties from input data to the output concentrations through a Chemistry Transport Model was first studied. The influence of the resolutions of meteorological parameters and emissions data were studied separately, and their relative role was compared. It was found that model results do not improve linearly with the resolution of emission input. A critical resolution was found, beyond which model error becomes higher and the model breaks down. Based on this first investigation concerning the direct down scaling, further research focused on sub grid scale modeling. Thus, a statistical down scaling approach was adopted for the modeling of sub grid-scale concentration variability due to heterogeneous surface emissions. Emission fractions released from different types of sources (industry, roads, residential, natural etc.) were calculated from a high-resolution emission inventory. Then emission fluxes were mapped on surfaces emitting source-specific species. Simulations were run independently over the defined micro-environments allowing the modeling of sub grid-scale concentration variability. Sub grid scale concentrations were therefore combined with demographic and human activity data to provide exposure estimates. The spatial distribution of human exposure was parameterized through a Monte-Carlo model. The new information concerning exposure variability was added to an existing epidemiological model to study relative health risks. A log-linear Poisson regression model was used for this purpose. The principal outcome of the investigation was that a new functionality was added to the regression model which allows the dissociation of the health risk associated with each pollutant (e.g. NO 2 and PM 2.5 ). (author)

  2. Impact of the Fused Deposition (FDM Printing Process on Polylactic Acid (PLA Chemistry and Structure

    Directory of Open Access Journals (Sweden)

    Michael Arthur Cuiffo

    2017-06-01

    Full Text Available Polylactic acid (PLA is an organic polymer commonly used in fused deposition (FDM printing and biomedical scaffolding that is biocompatible and immunologically inert. However, variations in source material quality and chemistry make it necessary to characterize the filament and determine potential changes in chemistry occurring as a result of the FDM process. We used several spectroscopic techniques, including laser confocal microscopy, Fourier transform infrared (FTIR spectroscopy and photoacousitc FTIR spectroscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS in order to characterize both the bulk and surface chemistry of the source material and printed samples. Scanning electron microscopy (SEM and differential scanning calorimetry (DSC were used to characterize morphology, cold crystallinity, and the glass transition and melting temperatures following printing. Analysis revealed calcium carbonate-based additives which were reacted with organic ligands and potentially trace metal impurities, both before and following printing. These additives became concentrated in voids in the printed structure. This finding is important for biomedical applications as carbonate will impact subsequent cell growth on printed tissue scaffolds. Results of chemical analysis also provided evidence of the hygroscopic nature of the source material and oxidation of the printed surface, and SEM imaging revealed micro- and submicron-scale roughness that will also impact potential applications.

  3. Metformin: A Review of Characteristics, Properties, Analytical Methods and Impact in the Green Chemistry.

    Science.gov (United States)

    da Trindade, Mariana Teixeira; Kogawa, Ana Carolina; Salgado, Hérida Regina Nunes

    2018-01-02

    Diabetes mellitus (DM) is considered a public health problem. The initial treatment consists of improving the lifestyle and making changes in the diet. When these changes are not enough, the use of medication becomes necessary. The metformin aims to reduce the hepatic production of glucose and is the preferred treatment for type 2. The objective is to survey the characteristics and properties of metformin, as well as hold a discussion on the existing analytical methods to green chemistry and their impacts for both the operator and the environment. For the survey, data searches were conducted by scientific papers in the literature as well as in official compendium. The characteristics and properties are shown, also, methods using liquid chromatography techniques, titration, absorption spectrophotometry in the ultraviolet and the infrared region. Most of the methods presented are not green chemistry oriented. It is necessary the awareness of everyone involved in the optimization of the methods applied through the implementation of green chemistry to determine the metformin.

  4. Impacts of Stratospheric Sulfate Geoengineering on PM2.5

    Science.gov (United States)

    Robock, A.; Xia, L.; Tilmes, S.; Mills, M. J.; Richter, J.; Kravitz, B.; MacMartin, D.

    2017-12-01

    Particulate matter (PM) includes sulfate, nitrate, organic carbon, elemental carbon, soil dust, and sea salt. The first four components are mostly present near the ground as fine particulate matter with a diameter less than 2.5 µm (PM2.5), and these are of the most concern for human health. PM is efficiently scavenged by precipitation, which is its main atmospheric sink. Here we examine the impact of stratospheric climate engineering on this important pollutant and health risk, taking advantage of two sets of climate model simulations conducted at the National Center for Atmospheric Research. We use the full tropospheric and stratospheric chemistry version of the Community Earth System Model - Community Atmospheric Model 4 (CESM CAM4-chem) with a horizontal resolution of 0.9° x 1.25° lat-lon to simulate a stratospheric sulfate injection climate intervention of 8 Tg SO2 yr-1 combined with an RCP6.0 global warming forcing, the G4 Specified Stratospheric Aerosol (G4SSA) scenario. We also analyze the output from a 20-member ensemble of Community Earth System Model, version 1 with the Whole Atmosphere Community Climate Model as its atmospheric component (CESM1(WACCM)) simulations, also at 0.9° x 1.25° lat-lon resolution, with sulfur dioxide injection at 15°N, 15°S, 30°N, and 30°S varying in time to balance RCP8.5 forcing. While the CESM CAM4-chem model has full tropospheric and stratospheric chemistry, CESM1(WACCM) has an internally generated quasi-biennial oscillation and a comprehensive tropospheric and stratospheric sulfate aerosol treatment, but only stratospheric chemistry. For G4SSA, there are a global temperature reduction of 0.8 K and global averaged precipitation decrease of 3% relative to RCP6.0. The global averaged surface PM2.5 reduces about 1% compared with RCP6.0, mainly over Eurasian and East Asian regions in Northern Hemisphere winter. The PM2.5 concentration change is a combination of effects from tropospheric chemistry and precipitation

  5. Removal of Atmospheric Ethanol by Wet Deposition: A Global Flux Estimate

    Science.gov (United States)

    Felix, J. D. D.; Willey, J. D.; Avery, B.; Thomas, R.; Mullaugh, K.; Kieber, R. J.; Mead, R. N.; Helms, J. R.; Campos, L.; Shimizu, M. S.; Guibbina, F.

    2017-12-01

    Global ethanol fuel consumption has increased exponentially over the last two decades and the US plans to double annual renewable fuel production in the next five years as required by the renewable fuel standard. Regardless of the technology or feedstock used to produce the renewable fuel, the primary end product will be ethanol. Increasing ethanol fuel consumption will have an impact on the oxidizing capacity of the atmosphere and increase atmospheric concentrations of the secondary pollutant peroxyacetyl nitrate as well a variety of VOCs with relatively high ozone reactivities (e.g. ethanol, formaldehyde, acetaldehyde). Despite these documented effects of ethanol emissions on atmospheric chemistry, current global atmospheric ethanol budget models have large uncertainties in the magnitude of ethanol sources and sinks. The presented work investigates the global wet deposition sink by providing the first estimate of the global wet deposition flux of ethanol (2.4 ± 1.6 Tg/yr) based on empirical wet deposition data (219 samples collected at 12 locations). This suggests the wet deposition sink removes between 6 and 17% of atmospheric ethanol annually. Concentrations of ethanol in marine wet deposition (25 ± 6 nM) were an order of magnitude less than in the majority of terrestrial deposition (345 ± 280 nM). Terrestrial deposition collected in locations impacted by high local sources of biofuel usage and locations downwind from ethanol distilleries were an order of magnitude higher in ethanol concentration (3090 ± 448 nM) compared to deposition collected in terrestrial locations not impacted by these sources. These results indicate that wet deposition of ethanol is heavily influenced by local sources and ethanol emission impacts on air quality may be more significant in highly populated areas. As established and developing countries continue to rapidly increase ethanol fuel consumption and subsequent emissions, understanding the magnitude of all ethanol sources and

  6. Effects of changes in carbonate chemistry speciation on Coccolithus braarudii: a discussion of coccolithophorid sensitivities

    Directory of Open Access Journals (Sweden)

    U. Riebesell

    2011-03-01

    Full Text Available Ocean acidification and associated shifts in carbonate chemistry speciation induced by increasing levels of atmospheric carbon dioxide (CO2 have the potential to impact marine biota in various ways. The process of biogenic calcification, for instance, is usually shown to be negatively affected. In coccolithophores, an important group of pelagic calcifiers, changes in cellular calcification rates in response to changing ocean carbonate chemistry appear to differ among species. By applying a wider CO2 range we show that a species previously reported insensitive to seawater acidification, Coccolithus braarudii, responds both in terms of calcification and photosynthesis, although at higher levels of CO2. Thus, observed differences between species seem to be related to individual sensitivities while the underlying mechanisms could be the same. On this basis we develop a conceptual model of coccolithophorid calcification and photosynthesis in response to CO2-induced changes in seawater carbonate chemistry speciation.

  7. 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

  8. Assessing the impact of aerosol-atmosphere interactions in convection-permitting regional climate simulations: the Rolf medicane in 2011

    Science.gov (United States)

    José Gómez-Navarro, Juan; María López-Romero, José; Palacios-Peña, Laura; Montávez, Juan Pedro; Jiménez-Guerrero, Pedro

    2017-04-01

    A critical challenge for assessing regional climate change projections relies on improving the estimate of atmospheric aerosol impact on clouds and reducing the uncertainty associated with the use of parameterizations. In this sense, the horizontal grid spacing implemented in state-of-the-art regional climate simulations is typically 10-25 kilometers, meaning that very important processes such as convective precipitation are smaller than a grid box, and therefore need to be parameterized. This causes large uncertainties, as closure assumptions and a number of parameters have to be established by model tuning. Convection is a physical process that may be strongly conditioned by atmospheric aerosols, although the solution of aerosol-cloud interactions in warm convective clouds remains nowadays a very important scientific challenge, rendering parametrization of these complex processes an important bottleneck that is responsible from a great part of the uncertainty in current climate change projections. Therefore, the explicit simulation of convective processes might improve the quality and reliability of the simulations of the aerosol-cloud interactions in a wide range of atmospheric phenomena. Particularly over the Mediterranean, the role of aerosol particles is very important, being this a crossroad that fuels the mixing of particles from different sources (sea-salt, biomass burning, anthropogenic, Saharan dust, etc). Still, the role of aerosols in extreme events in this area such as medicanes has been barely addressed. This work aims at assessing the role of aerosol-atmosphere interaction in medicanes with the help of the regional chemistry/climate on-line coupled model WRF-CHEM run at a convection-permitting resolution. The analysis is exemplary based on the "Rolf" medicane (6-8 November 2011). Using this case study as reference, four sets of simulations are run with two spatial resolutions: one at a convection-permitting configuration of 4 km, and other at the

  9. Fogwater Chemistry and Air Quality in the Texas-Louisiana Gulf Coast Corridor

    Science.gov (United States)

    Kommalapati, R. R.; Raja, S.; Ravikrishna, R.; Murugesan, K.; Collett, J. L.; Valsaraj, K.

    2007-05-01

    The presence of fog water in polluted atmosphere can influence atmospheric chemistry and air quality. The study of interactions between fog water and atmospheric gases and aerosols are very important in understanding the atmospheric fate of the pollutants. In this Study several air samples and fogwater samples were collected in the heavily industrialized area of Gulf Coast corridor( Houston, TX and Baton Rouge, LA). A total of 32 fogwater samples were collected, comprising of nine fog events in Baton Rouge (Nov 2004 to Feb 2005) and two fog events in Houston (Feb, 2006), during the fog sampling campaigns. These samples were analyzed for pH, total and dissolved carbon, major inorganic ions, organic acids, and aromatics, aldehydes, VOCs, and linear alkanes organic compounds. Fogwater samples collected in Houston show clear influence of marine and anthropogenic environment, while Baton Rouge samples reveal a relatively less polluted environment. Also, a time series observation of air samples indicated that fog event at the monitoring site impacted the air concentrations of the pollutants. This is attributed to presence of surface active organic matter in fog water.

  10. The chemistry-climate model ECHAM6.3-HAM2.3-MOZ1.0

    Science.gov (United States)

    Schultz, Martin G.; Stadtler, Scarlet; Schröder, Sabine; Taraborrelli, Domenico; Franco, Bruno; Krefting, Jonathan; Henrot, Alexandra; Ferrachat, Sylvaine; Lohmann, Ulrike; Neubauer, David; Siegenthaler-Le Drian, Colombe; Wahl, Sebastian; Kokkola, Harri; Kühn, Thomas; Rast, Sebastian; Schmidt, Hauke; Stier, Philip; Kinnison, Doug; Tyndall, Geoffrey S.; Orlando, John J.; Wespes, Catherine

    2018-05-01

    The chemistry-climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols using either a modal scheme (M7) or a bin scheme (SALSA). This article describes and evaluates the model version ECHAM6.3-HAM2.3-MOZ1.0 with a focus on the tropospheric gas-phase chemistry. A 10-year model simulation was performed to test the stability of the model and provide data for its evaluation. The comparison to observations concentrates on the year 2008 and includes total column observations of ozone and CO from IASI and OMI, Aura MLS observations of temperature, HNO3, ClO, and O3 for the evaluation of polar stratospheric processes, an ozonesonde climatology, surface ozone observations from the TOAR database, and surface CO data from the Global Atmosphere Watch network. Global budgets of ozone, OH, NOx, aerosols, clouds, and radiation are analyzed and compared to the literature. ECHAM-HAMMOZ performs well in many aspects. However, in the base simulation, lightning NOx emissions are very low, and the impact of the heterogeneous reaction of HNO3 on dust and sea salt aerosol is too strong. Sensitivity simulations with increased lightning NOx or modified heterogeneous chemistry deteriorate the comparison with observations and yield excessively large ozone budget terms and too much OH. We hypothesize that this is an impact of potential issues with tropical convection in the ECHAM model.

  11. Pathways, Impacts, and Policies on Severe Aerosol Injections into the Atmosphere: 2011 Severe Atmospheric Aerosols Events Conference

    KAUST Repository

    Weil, Martin

    2012-09-01

    The 2011 severe atmospheric events conference, held on August 11-12, 2011, Hamburg, Germany, discussed climatic and environmental changes as a result of various kinds of huge injections of aerosols into the atmosphere and the possible consequences for the world population. Various sessions of the conference dealt with different aspects of large aerosol injections and severe atmospheric aerosol events along the geologic time scale. A presentation about radiative heating of aerosols as a self-lifting mechanism in the Australian forest fires discussed the question of how the impact of tropical volcanic eruptions depends on the eruption season. H.-F. Graf showed that cloud-resolving plume models are more suitable to predict the volcanic plume height and dispersion than one-dimensional models. G. Stenchikov pointed out that the absorbing smoke plumes in the upper troposphere can be partially mixed into the lower stratosphere because of the solar heating and lofting effect.

  12. Pathways, Impacts, and Policies on Severe Aerosol Injections into the Atmosphere: 2011 Severe Atmospheric Aerosols Events Conference

    KAUST Repository

    Weil, Martin; Grassl, Hartmut; Hoshyaripour, Gholamali; Kloster, Silvia; Kominek, Jasmin; Misios, Stergios; Scheffran, Juergen; Starr, Steven; Stenchikov, Georgiy L.; Sudarchikova, Natalia; Timmreck, Claudia; Zhang, Dan; Kalinowski, Martin

    2012-01-01

    The 2011 severe atmospheric events conference, held on August 11-12, 2011, Hamburg, Germany, discussed climatic and environmental changes as a result of various kinds of huge injections of aerosols into the atmosphere and the possible consequences for the world population. Various sessions of the conference dealt with different aspects of large aerosol injections and severe atmospheric aerosol events along the geologic time scale. A presentation about radiative heating of aerosols as a self-lifting mechanism in the Australian forest fires discussed the question of how the impact of tropical volcanic eruptions depends on the eruption season. H.-F. Graf showed that cloud-resolving plume models are more suitable to predict the volcanic plume height and dispersion than one-dimensional models. G. Stenchikov pointed out that the absorbing smoke plumes in the upper troposphere can be partially mixed into the lower stratosphere because of the solar heating and lofting effect.

  13. 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

  14. 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.

  15. 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

  16. 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)

  17. 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

  18. Impact of a future H2-based road transportation sector on the composition and chemistry of the atmosphere – Part 2: Stratospheric ozone

    Directory of Open Access Journals (Sweden)

    D. Wang

    2013-07-01

    Full Text Available The prospective future adoption of molecular hydrogen (H2 to power the road transportation sector could greatly improve tropospheric air quality but also raises the question of whether the adoption would have adverse effects on the stratospheric ozone. The possibility of undesirable impacts must be fully evaluated to guide future policy decisions. Here we evaluate the possible impact of a future (2050 H2-based road transportation sector on stratospheric composition and chemistry, especially on the stratospheric ozone, with the MOZART (Model for OZone And Related chemical Tracers model. Since future growth is highly uncertain, we evaluate the impact of two world evolution scenarios, one based on an IPCC (Intergovernmental Panel on Climate Change high-emitting scenario (A1FI and the other on an IPCC low-emitting scenario (B1, as well as two technological options: H2 fuel cells and H2 internal combustion engines. We assume a H2 leakage rate of 2.5% and a complete market penetration of H2 vehicles in 2050. The model simulations show that a H2-based road transportation sector would reduce stratospheric ozone concentrations as a result of perturbed catalytic ozone destruction cycles. The magnitude of the impact depends on which growth scenario evolves and which H2 technology option is applied. For the evolution growth scenario, stratospheric ozone decreases more in the H2 fuel cell scenarios than in the H2 internal combustion engine scenarios because of the NOx emissions in the latter case. If the same technological option is applied, the impact is larger in the A1FI emission scenario. The largest impact, a 0.54% decrease in annual average global mean stratospheric column ozone, is found with a H2 fuel cell type road transportation sector in the A1FI scenario; whereas the smallest impact, a 0.04% increase in stratospheric ozone, is found with applications of H2 internal combustion engine vehicles in the B1 scenario. The impacts of the other two

  19. 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.

  20. Roles of transport and chemistry processes in global ozone change on interannual and multidecadal time scales

    Science.gov (United States)

    Sekiya, T.; Sudo, K.

    2014-04-01

    This study investigates ozone changes and the individual impacts of transport and chemistry on those changes. We specifically examine (1) variation related to El Niño Southern Oscillation, which is a dominant mode of interannual variation of tropospheric ozone, and (2) long-term change between the 2000s and 2100s. During El Niño, the simulated ozone shows an increase (1 ppbv/K) over Indonesia, a decrease (2-10 ppbv/K) over the eastern Pacific in the tropical troposphere, and an increase (50 ppbv/K) over the eastern Pacific in the midlatitude lower stratosphere. These variations fundamentally agree with those observed by Microwave Limb Sounder/Tropospheric Emission Spectrometer instruments. The model demonstrates that tropospheric chemistry has a strong impact on the variation over the eastern Pacific in the tropical lower troposphere and that transport dominates the variation in the midlatitude lower stratosphere. Between the 2000s and 2100s, the model predicts an increase in the global burden of stratospheric ozone (0.24%/decade) and a decrease in the global burden of tropospheric ozone (0.82%/decade). The increase in the stratospheric burden is controlled by stratospheric chemistry. Tropospheric chemistry reduces the tropospheric burden by 1.07%/decade. However, transport (i.e., stratosphere-troposphere exchange and tropospheric circulation) causes an increase in the burden (0.25%/decade). Additionally, we test the sensitivity of ozone changes to increased horizontal resolution of the representation of atmospheric circulation and advection apart from any aspects of the nonlinearity of chemistry sensitivity to horizontal resolution. No marked difference is found in medium-resolution or high-resolution simulations, suggesting that the increased horizontal resolution of transport has a minor impact.

  1. 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

  2. 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.

  3. 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.

  4. 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....

  5. Investigation of Laser Plasma Chemistry in CO2-N-2-H2O Using O-18 Labeled Water

    Czech Academy of Sciences Publication Activity Database

    Ferus, Martin; Kubelík, Petr; Juha, Libor; Civiš, Svatopluk

    2009-01-01

    Roč. 39, 3-4 (2009), s. 245-245 ISSN 0169-6149 R&D Projects: GA MŠk LC510; GA MŠk(CZ) LC528; GA ČR GA203/06/1278; GA MŠk LA08024 Institutional research plan: CEZ:AV0Z40400503; CEZ:AV0Z10100523 Keywords : LIDB plasma * atmosphere * isotopes Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.053, year: 2009

  6. Electron-impact vibrational excitation of the hydroxyl radical in the nighttime upper atmosphere

    Science.gov (United States)

    Campbell, Laurence; Brunger, Michael J.

    2018-02-01

    Chemical processes produce vibrationally excited hydroxyl (OH) in a layer centred at an altitude of about 87 km in the Earth's atmosphere. Observations of this layer are used to deduce temperatures in the mesosphere and to observe the passage of atmospheric gravity waves. Due to the low densities and energies at night of electrons at the relevant altitude, it is not expected that electron-impact excitation of OH would be significant. However, there are unexplained characteristics of OH densities and radiative emissions that might be explained by electron impact. These are measurements of higher than expected densities of OH above 90 km and of emissions at higher energies that cannot be explained by the chemical production processes. This study simulates the role of electron impact in these processes, using theoretical cross sections for electron-impact excitation of OH. The simulations show that electron impact, even in a substantial aurora, cannot fully explain these phenomena. However, in the process of this investigation, apparent inconsistencies in the theoretical cross sections and reaction rates were found, indicating that measurements of electron-impact excitation of OH are needed to resolve these problems and scale the theoretical predictions to allow more accurate simulations.

  7. 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

  8. Modeling impacts of NH3 on uptake of H2SO4 by charged nucleating nanoparticles in the Earth's atmosphere

    International Nuclear Information System (INIS)

    Nadykto, A. B.; Nazarenko, K. M.; Markov, P. N.; Yu, F.

    2016-01-01

    The understanding of the role of ammonia, a well-known stabilizer of binary sulfuric acid-water clusters, in the gas-to-nanoparticle conversion in the Earth atmosphere is critically important for the assessment of aerosol radiative forcing associated with the climate changes. The sulfuric acid H 2 SO 4 is present in the atmosphere in the form of the gas-phase hydrates (H 2 SO 4 )(H 2 O) n , whose interaction with NH 3 leads to the formation of more stable bisulfate clusters (NH 3 )(H 2 SO 4 )(H 2 O) n . Although the impact of NH 3 on the thermochemical stability of binary clusters nucleating homogeneously has been studied in some detail in the past, the effect of ammonia on other microphysical properties relevant to nucleation remains insufficiently well understood. In the present study, the effect of ammonia on the electrical dipole moment controlling the nucleation of airborne ions via the dipole-charge interaction has been investigated using the Density Functional Theory (DFT), ab initio MP2 and model chemistry G3 methods. The presence of ammonia in (H 2 SO 4 )(H 2 O) n is found to lead to very large enhancement in the dipole moment, which exceeds 2.0-2.5 Debyes (∼60-80%), 3.7-5.0 Debyes (∼90-180%), 1.4-4.5 Debyes (∼50-150%) and 2.1-5.5 Debyes (∼60-700%) for n = 0, n = 1, n = 2 and n = 3, respectively. The implications of this include the significantly increased uptake of the sulfuric acid, the key atmospheric nucleation precursor, by airborne ions and neutrals (due to dipole-dipole interaction), enhanced nucleation rates and the elevated production of ultrafine particles, which cause adverse health impacts.

  9. Analysis Of The 2009 July Impact Debris In Jupiter'S Atmosphere

    Science.gov (United States)

    Sanchez-Lavega, Agustin; Hueso, R.; Legarreta, J.; Pérez-Hoyos, S.; García-Melendo, E.; Gómez, J. M.; Rojas, J. F.; Orton, G. S.; Wesley, A.; IOPW International Outer Planet Watch Team

    2009-09-01

    We report the analysis of images obtained by the contributors to the International Outer Planet Watch (IOPW) of the debris left in the atmosphere of Jupiter by the object that impacted the planet between 18 and 19 July 2009. The discovery images by Anthony Wesley in July 19.625 and the first two days of its tracking, shows a dark debris spot (continuum wavelength) located at planetocentric latitude -55.1 deg and 304.5 deg System III longitude. The imaging survey indicates that the spot was not present in July 18.375, so the impact occurred during a window between both dates. The main spot had a size of about 4,500 km and to its Northwest a thin debris halo of similar size was initially observed. Methane band images at a wavelength of 890 nm shows the spot to be bright indicating that the debris aerosols are highly placed in the atmosphere relative to surrounding clouds. At the central latitude of the impact, the Jovian flow has nearly zero speed but anticyclonic vorticity bounded by jets at -51.5 deg (directed westward with velocity -10 m/s) and at -57.5 deg (directed eastward with velocity 25 m/s). The morphology in the continuum and the spot brightness in the methane band strongly suggest that the feature was caused by a cometary or asteroidal impact, similar in behaviour to the SL9 impacts of 1994. This work has been funded by Spanish MEC AYA2006-07735 with FEDER support and Grupos Gobierno Vasco IT-464-07. RH acknowledges a "Ramón y Cajal” contract from MEC.

  10. An Analytical Framework for the Steady State Impact of Carbonate Compensation on Atmospheric CO2

    Science.gov (United States)

    Omta, Anne Willem; Ferrari, Raffaele; McGee, David

    2018-04-01

    The deep-ocean carbonate ion concentration impacts the fraction of the marine calcium carbonate production that is buried in sediments. This gives rise to the carbonate compensation feedback, which is thought to restore the deep-ocean carbonate ion concentration on multimillennial timescales. We formulate an analytical framework to investigate the impact of carbonate compensation under various changes in the carbon cycle relevant for anthropogenic change and glacial cycles. Using this framework, we show that carbonate compensation amplifies by 15-20% changes in atmospheric CO2 resulting from a redistribution of carbon between the atmosphere and ocean (e.g., due to changes in temperature, salinity, or nutrient utilization). A counterintuitive result emerges when the impact of organic matter burial in the ocean is examined. The organic matter burial first leads to a slight decrease in atmospheric CO2 and an increase in the deep-ocean carbonate ion concentration. Subsequently, enhanced calcium carbonate burial leads to outgassing of carbon from the ocean to the atmosphere, which is quantified by our framework. Results from simulations with a multibox model including the minor acids and bases important for the ocean-atmosphere exchange of carbon are consistent with our analytical predictions. We discuss the potential role of carbonate compensation in glacial-interglacial cycles as an example of how our theoretical framework may be applied.

  11. 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.

  12. 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'

  13. Study of the impact of atmospheric emissions (41AR) during operation of a nuclear reactor research

    International Nuclear Information System (INIS)

    Alves, Simone F.; Barreto, Alberto A.; Jacomino, Vanusa Maria F.; Rodrigues, Paulo Cesar H.

    2013-01-01

    The knowledge of the atmosphere dispersion of radionuclides, resulting from a nuclear reactor emissions during normal operation, is an important step in the process of nuclear licensing and environmental. This step requires a study to evaluate the radiological environmental impact. The results of this study are used by radiation protection agents to control the exposure of public to radiation during the operation of nuclear facilities. The elaboration of environmental impact assessment due to atmospheric emissions is based on a study of atmospheric dispersion. The aim of this study is estimate the concentrations of radionuclides in different compartments of the ecosystem and calculate the dose received by man as a result of radiation exposure in different scenarios of interest. This paper deals with the case study of the impact of atmospheric emissions of 41 Ar during operation of a nuclear research reactor. This study was accomplished with the application of the dispersion model ARTM (Radionuclide Transport Atmospheric Model), along with the geoprocessing resources. Among the results are: the spatial distribution of population by age; topography of the region, local wind rose, atmospheric stability and the estimate of the concentration of radionuclide 41 Ar and of dose. The results indicate that the dose, by external irradiation due to immersion in the cloud, was below the limits established by regulatory agencies. (author)

  14. Impact of reactor water chemistry on cladding performance

    Energy Technology Data Exchange (ETDEWEB)

    Cox, B. [University of Toronto, Centre for Nuclear Engineering, Toronto, Ontario (Canada)

    1997-07-01

    Water chemistry may have a major impact on fuel cladding performance in PWRs. If the saturation temperature on the surface of fuel cladding is exceeded, either because of the thermal hydraulics of the system, or because of crud deposition, then LiOH concentration can occur within thick porous oxide films on the cladding. This can degrade the protective film and accelerate the corrosion rate of the cladding. If sufficient boric acid is also present in the coolant then these effects may be mitigated. This is normally the case through most of any reactor fuel cycle. Extensive surface boiling may disrupt this equilibrium because of the volatility of boric acid in steam. Under such conditions severe cladding corrosion can ensue. The potential for such effects on high burnup cladding in CANDU reactors, where bone acid is not present in the primary coolant, is discussed. (author)

  15. Impact of reactor water chemistry on cladding performance

    International Nuclear Information System (INIS)

    Cox, B.

    1997-01-01

    Water chemistry may have a major impact on fuel cladding performance in PWRs. If the saturation temperature on the surface of fuel cladding is exceeded, either because of the thermal hydraulics of the system, or because of crud deposition, then LiOH concentration can occur within thick porous oxide films on the cladding. This can degrade the protective film and accelerate the corrosion rate of the cladding. If sufficient boric acid is also present in the coolant then these effects may be mitigated. This is normally the case through most of any reactor fuel cycle. Extensive surface boiling may disrupt this equilibrium because of the volatility of boric acid in steam. Under such conditions severe cladding corrosion can ensue. The potential for such effects on high burnup cladding in CANDU reactors, where bone acid is not present in the primary coolant, is discussed. (author)

  16. Survey of PWR water chemistry

    International Nuclear Information System (INIS)

    Gorman, J.

    1989-02-01

    This report surveys available information regarding primary and secondary water chemistries of pressurized water reactors (PWRs) and the impact of these water chemistries on reactor operation. The emphasis of the document is on aspects of water chemistry that affect the integrity of the primary pressure boundary and the radiation dose associated with maintenance and operation. The report provides an historical overview of the development of primary and secondary water chemistries, and describes practices currently being followed. Current problems and areas of research associated with water chemistry are described. Recommendations for further research are included. 183 refs., 9 figs., 19 tabs

  17. Quantification of trace elements and speciation of iron in atmospheric particulate matter

    Science.gov (United States)

    Upadhyay, Nabin

    Trace metal species play important roles in atmospheric redox processes and in the generation of oxidants in cloud systems. The chemical impact of these elements on atmospheric and cloud chemistry is dependent on their occurrence, solubility and speciation. First, analytical protocols have been developed to determine trace elements in particulate matter samples collected for carbonaceous analysis. The validated novel protocols were applied to the determination of trace elements in particulate samples collected in the remote marine atmosphere and urban areas in Arizona to study air pollution issues. The second part of this work investigates on solubility and speciation in environmental samples. A detailed study on the impact of the nature and strength of buffer solutions on solubility and speciation of iron lead to a robust protocol, allowing for comparative measurements in matrices representative of cloud water conditions. Application of this protocol to samples from different environments showed low iron solubility (less than 1%) in dust-impacted events and higher solubility (5%) in anthropogenically impacted urban samples. In most cases, Fe(II) was the dominant oxidation state in the soluble fraction of iron. The analytical protocol was then applied to investigate iron processing by fogs. Field observations showed that only a small fraction (1%) of iron was scavenged by fog droplets for which each of the soluble and insoluble fraction were similar. A coarse time resolution limited detailed insights into redox cycling within fog system. Overall results suggested that the major iron species in the droplets was Fe(1I) (80% of soluble iron). Finally, the occurrence and sources of emerging organic pollutants in the urban atmosphere were investigated. Synthetic musk species are ubiquitous in the urban environment (less than 5 ng m-3) and investigations at wastewater treatment plants showed that wastewater aeration basins emit a substantial amount of these species to

  18. 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.

  19. 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.

  20. 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)

  1. Maintenance, outages and chemistry really can be compatible

    International Nuclear Information System (INIS)

    Roberts, J.G.; Deaconescu, R.

    2006-01-01

    'Full text:' In their address to the Canadian Nuclear Society, Bruce Power's Chemistry Design staff will describe how maintenance and outages can impact negatively on chemistry control and asset protection. Considerations of material impacts and material condition have significant influences on the approach to, and control of, chemistry. This applies equally to operation as it does during unit and/or system outages. Ideas will be presented as to how to facilitate making maintenance, outages and chemistry compatible. It will be shown how the lack of such an approach can lead to disastrous results. (author)

  2. 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...

  3. Predicting the Response of Molluscs to the Impact of Ocean Acidification

    Directory of Open Access Journals (Sweden)

    John M. Wright

    2013-04-01

    Full Text Available Elevations in atmospheric carbon dioxide (CO2 are anticipated to acidify oceans because of fundamental changes in ocean chemistry created by CO2 absorption from the atmosphere. Over the next century, these elevated concentrations of atmospheric CO2 are expected to result in a reduction of the surface ocean waters from 8.1 to 7.7 units as well as a reduction in carbonate ion (CO32− concentration. The potential impact that this change in ocean chemistry will have on marine and estuarine organisms and ecosystems is a growing concern for scientists worldwide. While species-specific responses to ocean acidification are widespread across a number of marine taxa, molluscs are one animal phylum with many species which are particularly vulnerable across a number of life-history stages. Molluscs make up the second largest animal phylum on earth with 30,000 species and are a major producer of CaCO3. Molluscs also provide essential ecosystem services including habitat structure and food for benthic organisms (i.e., mussel and oyster beds, purification of water through filtration and are economically valuable. Even sub lethal impacts on molluscs due to climate changed oceans will have serious consequences for global protein sources and marine ecosystems.

  4. Predicting the Response of Molluscs to the Impact of Ocean Acidification

    Science.gov (United States)

    Parker, Laura M.; Ross, Pauline M.; O’Connor, Wayne A.; Pörtner, Hans O.; Scanes, Elliot; Wright, John M.

    2013-01-01

    Elevations in atmospheric carbon dioxide (CO2) are anticipated to acidify oceans because of fundamental changes in ocean chemistry created by CO2 absorption from the atmosphere. Over the next century, these elevated concentrations of atmospheric CO2 are expected to result in a reduction of the surface ocean waters from 8.1 to 7.7 units as well as a reduction in carbonate ion (CO32−) concentration. The potential impact that this change in ocean chemistry will have on marine and estuarine organisms and ecosystems is a growing concern for scientists worldwide. While species-specific responses to ocean acidification are widespread across a number of marine taxa, molluscs are one animal phylum with many species which are particularly vulnerable across a number of life-history stages. Molluscs make up the second largest animal phylum on earth with 30,000 species and are a major producer of CaCO3. Molluscs also provide essential ecosystem services including habitat structure and food for benthic organisms (i.e., mussel and oyster beds), purification of water through filtration and are economically valuable. Even sub lethal impacts on molluscs due to climate changed oceans will have serious consequences for global protein sources and marine ecosystems. PMID:24832802

  5. Plants, Pollution and Public Engagement with Atmospheric Chemistry: Sharing the TEMPO Story Through Ozone Garden Activities

    Science.gov (United States)

    Reilly, L. G.; Pippin, M. R.; Malick, E.; Summers, D.; Dussault, M. E.; Wright, E. A.; Skelly, J.

    2016-12-01

    What do a snap-bean plant and a future NASA satellite instrument named TEMPO have in common? They are both indicators of the quality of the air we breathe. Scientists, educators, and museum and student collaborators of the Tropospheric Emissions: Monitoring Pollution (TEMPO) instrument team are developing a program model to engage learners of all ages via public ozone garden exhibits and associated activities. TEMPO, an ultraviolet and visible spectroscopy instrument due for launch on a geostationary host satellite between 2019 and 2021, will scan North America hourly to measure the major elements in the tropospheric ozone chemistry cycle, providing near real-time data with high temporal and spatial resolution. The TEMPO mission provides a unique opportunity to share the story of the effects of air quality on living organisms. A public ozone garden exhibit affords an accessible way to understand atmospheric science through a connection with nature, while providing a visual representation of the impact of ozone pollution on living organisms. A prototype ozone garden exhibit was established at the Virginia Living Museum in partnership with NASA Langley, and has served as a site to formatively evaluate garden planting and exhibit display protocols, hands-on interpretive activities, and citizen science data collection protocols for learners as young as 3 to 10 as well as older adults. The fun and engaging activities, optimized for adult-child interaction in informal or free-choice learning environments, are aimed at developing foundational science skills such as observing, comparing, classifying, and collecting and making sense of data in the context of thinking about air quality - all NGSS-emphasized scientific practices, as well as key capabilities for future contributing members of the citizen science community. As the launch of TEMPO approaches, a major public engagement effort will include disseminating this ozone garden exhibit and program model to a network of

  6. 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.

  7. 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.

  8. Technical Note: The CCCma third generation AGCM and its extension into the middle atmosphere

    Directory of Open Access Journals (Sweden)

    J. F. Scinocca

    2008-12-01

    Full Text Available The Canadian Centre for Climate Modelling and Analysis third generation atmospheric general circulation model (AGCM3 is described. The discussion summarizes the details of the complete physics package emphasizing the changes made relative to the second generation version of the model. AGCM3 is the underlying model for applications which include the IPCC fourth assessment, coupled atmosphere-ocean seasonal forecasting, the first generation of the CCCma earth system model (CanESM1, and middle-atmosphere chemistry-climate modelling (CCM. Here we shall focus on issues related to an upwardly extended version of AGCM3, the Canadian Middle-Atmosphere Model (CMAM. The CCM version of CMAM participated in the 2006 WMO/UNEP Scientific Assessment of Ozone Depletion and issues concerning its climate such as the impact of gravity-wave drag, the modelling of a spontaneous QBO, and the seasonality of the breakdown of the Southern Hemisphere polar vortex are discussed here.

  9. The detection and mapping of the spatial distribution of insect defense compounds by desorption atmospheric pressure photoionization Orbitrap mass spectrometry

    Czech Academy of Sciences Publication Activity Database

    Rejšek, Jan; Vrkoslav, Vladimír; Hanus, Robert; Vaikkinen, A.; Haapala, M.; Kauppila, T. J.; Kostiainen, R.; Cvačka, Josef

    2015-01-01

    Roč. 886, Jul 30 (2015), s. 91-97 ISSN 0003-2670 R&D Projects: GA ČR GP13-25137P Grant - others:GA AV ČR(CZ) M200551204 Institutional support: RVO:61388963 Keywords : desorption atmospheric pressure photoionization * ambient mass spectrometry * insect chemical defense * exocrine glands * termite * stink bug Subject RIV: CB - Analytical Chemistry, Separation Impact factor: 4.712, year: 2015

  10. Optimum coolant chemistry in BWRs

    International Nuclear Information System (INIS)

    Lin, C.C.; Cowan, R.L.; Kiss, E.

    2004-01-01

    LWR water chemistry parameters are directly or indirectly related to the plant's operational performance and for a significant amount of Operation and Maintenance (O and M) costs. Obvious impacts are the operational costs associated with water treatment, monitoring and associated radwaste generation. Less obvious is the important role water chemistry plays in the magnitude of drywell shutdown dose rates, fuel corrosion performance and, (probably most importantly) materials degradation such as from stress corrosion cracking of piping and Reactor Pressure Vessel (RPV) internal components. To improve the operational excellence of the BWR and to minimize the impact of water chemistry on O and M costs. General Electric has developed the concept of Optimum Water Chemistry (OWC). The 'best practices' and latest technology findings from the U.S., Asia and Europe are integrated into the suggested OWC Specification. This concept, together with cost effective ways to meet the requirement, are discussed. (author)

  11. 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

  12. 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...

  13. 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.

  14. 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).

  15. Impact of Climate Change on Soil and Groundwater Chemistry Subject to Process Waste Land Application

    Science.gov (United States)

    McNab, W. W.

    2013-12-01

    Nonhazardous aqueous process waste streams from food and beverage industry operations are often discharged via managed land application in a manner designed to minimize impacts to underlying groundwater. Process waste streams are typically characterized by elevated concentrations of solutes such as ammonium, organic nitrogen, potassium, sodium, and organic acids. Land application involves the mixing of process waste streams with irrigation water which is subsequently applied to crops. The combination of evapotranspiration and crop salt uptake reduces the downward mass fluxes of percolation water and salts. By carefully managing application schedules in the context of annual climatological cycles, growing seasons, and process requirements, potential adverse environmental impacts to groundwater can be mitigated. However, climate change poses challenges to future process waste land application efforts because the key factors that determine loading rates - temperature, evapotranspiration, seasonal changes in the quality and quantity of applied water, and various crop factors - are all likely to deviate from current averages. To assess the potential impact of future climate change on the practice of land application, coupled process modeling entailing transient unsaturated fluid flow, evapotranspiration, crop salt uptake, and multispecies reactive chemical transport was used to predict changes in salt loading if current practices are maintained in a warmer, drier setting. As a first step, a coupled process model (Hydrus-1D, combined with PHREEQC) was calibrated to existing data sets which summarize land application loading rates, soil water chemistry, and crop salt uptake for land disposal of process wastes from a food industry facility in the northern San Joaquin Valley of California. Model results quantify, for example, the impacts of evapotranspiration on both fluid flow and soil water chemistry at shallow depths, with secondary effects including carbonate mineral

  16. Bioorthogonal Chemistry-Introduction and Overview

    Czech Academy of Sciences Publication Activity Database

    Carell, T.; Vrábel, Milan

    2016-01-01

    Roč. 374, č. 1 (2016), č. článku 9. ISSN 2365-0869 Institutional support: RVO:61388963 Keywords : bioorthogonal reactions * click chemistry * biomolecule labeling * 1,3-dipolar cycloaddition * Diels-Alder reaction Subject RIV: CC - Organic Chemistry Impact factor: 4.033, year: 2016

  17. Modelling of atmospheric transport of heavy metals emitted from Polish power sector

    International Nuclear Information System (INIS)

    Zysk, Janusz

    2016-01-01

    Modelling of atmospheric transport of heavy metals emitted from Polish power sector. Many studies have been conducted to investigate the atmospheric heavy metals contamination and its deposition to ecosystems. The increasing attention to mercury pollution has been mainly driven by the growing evidence of its negative impacts on wildlife, ecosystems and particularly human health. Lead and cadmium are also toxics which are being emitted into the atmosphere by anthropogenic as well as natural sources. The harmful influence of these three heavy metals was underlined in the Aarhus Protocol on Heavy Metals of 1998. The Parties of this protocol (including Poland) are obligated to reduce emissions, observe the transport and the amounts of lead, mercury and cadmium in the environment. Poland is one of the biggest emitter of mercury, lead and cadmium in Europe mainly due to emission from coal combustion processes. Therefore in Poland, research efforts to study the heavy metals emission, atmospheric transport, concentration and deposition are extremely important. The objectives of this work were twofold: - The practical objective was to develop and run a model to represent the atmospheric dispersion of mercury and to implement it in the air quality modelling platform Polyphemus.- The scientific objective was to perform heavy metals dispersion studies over Europe and detailed studies of the impact of the polish power sector on the air quality regarding mercury, cadmium and lead. To meet the declared aim, a new mercury chemical model was implemented into the Polyphemus air quality system. The scientific literature was reviewed regarding mercury chemistry and mercury chemical models. It can be concluded that the chemistry of mercury is still not well known. The models also differ in the way of calculating the dry and wet deposition of mercury. The elemental gaseous mercury ambient concentrations are evenly distributed, on the contrary, high variations in the spatial gradients of

  18. Coupled atmosphere-soil-vegetation modelling for the assessment of the impact of atmospheric releases of heavy metals and of persistent organic pollutants at the European scale

    International Nuclear Information System (INIS)

    Queguiner, Solen

    2008-01-01

    The objective of this research thesis is to couple a model of atmospheric dispersion with a multi-environment model in order to perform impact studies related to atmospheric pollution by heavy metals and POPs (persistent organic pollutants). The author first presents the studied pollutants, their physical and chemical properties, and their effects on health. Then, he addresses the atmospheric modelling with a presentation of the used atmospheric dispersion model (POLAIR3D), and an application to heavy metals. Simulations are performed on a 4-year period in order to try to represent the inter-annual variability of atmospheric lead and cadmium concentrations. The next part reports the modelling of POPs which required the introduction of a soil model to address re-emissions. Results are compared with provided measurements. The fourth part reports the modelling of agricultural environments in the impact model, and more particularly physical processes and parameters proper to heavy metals and POPs. The author finally reports two case studies, one related to heavy metals, and the other to POPs [fr

  19. Comprehensive two-dimensional liquid chromatography–time-of-flight mass spectrometry in the analysis of acidic compounds in atmospheric aerosols

    Czech Academy of Sciences Publication Activity Database

    Pól, Jaroslav; Hohnová, B.; Jussila, M.; Hyötyläinen, T.

    2006-01-01

    Roč. 1130, č. 1 (2006), s. 64-71 ISSN 0021-9673. [International Symposium on Hyphenated Techniques in Chromatography and Hyphenated Chromatographic Analyzers /9./. York, 08.02.2006-10.02.2006] Institutional research plan: CEZ:AV0Z40310501 Keywords : comprehensive two-dimensional liquid chromatography * time-of-flight mass spectrometry * atmospheric aerosol analysis Subject RIV: CB - Analytical Chemistry, Separation Impact factor: 3.554, year: 2006

  20. A New Top-Down Decadal Constraint on Black Carbon Emissions over Asia - Capturing The Influence of Widespread and Regularly Occurring Fires and Urbanization: Greater Atmospheric Loading and Variability, Larger Impacts on Radiative Forcing at the Surface and in the Atmosphere, and Possible Feedback Mechanisms

    Science.gov (United States)

    Cohen, J. B.

    2014-12-01

    A global top-down study of Black Carbon (BC) Emissions has found that sources are considerably higher than present day emissions datasets, with most of this underestimation stemming from the rapidly developing areas of East and Southeast Asia. An additional source in these regions is the frequent and sometimes annual influence of extreme biomass burning events, which emit additional BC and other aerosols into the atmosphere. An additional top-down study has shown that the emissions of BC from these biomass burning events in Southeast Asia contribute an additional 30% increase in the annual average BC emissions, and an additional 110% increase during the highest fire year. One important reason for this underestimation is that many of these source regions do not appear as fires, due to missing MODIS overpasses, intense cloud cover, and low fire temperatures at the wet surface. These new temporally and spatially varying emissions of BC are run in a state-of-the art combined model of aerosol physics, chemistry, and general circulation, including urban scale chemical processing and core/shell aerosol mixture impacts on radiation. The results reveal that this new dataset matches in space, time, and magnitude, an array of observations (remotely sensed, ground, and column) far better than other emission datasets: IPCC SRES, AEROCOM, BOND, and GFED. The modeled mean atmospheric extinction and loading are both much higher and more variable than previous modelling efforts, leading to a larger negative surface radiative forcing. At the same time, atmospheric absorption is enhanced and more variable, leading to intense atmospheric heating, with the average impact from 1.0-1.5 W/m2. This has impacts on the vertical stability in the source areas, and leads to changes in the dynamics such as a shifting of the ITCZ, reducing light precipitation and increasing strong convection. To support this, a bit of measurement-based evidence presented for each of these phenomena.

  1. 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.

  2. Study of Chinese pollution with the 3D regional chemistry transport CHIMERE model and remote sensing observations, with a focus on mineral dust impacts

    Science.gov (United States)

    Lachatre, Mathieu; Foret, Gilles; Beekmann, Matthias; Cheiney, Audrey; Dufour, Gaëlle; Laurent, Benoit; Cuesta, Juan

    2017-04-01

    Since the end of the 20th century, China has observed important growth in numerous sectors. China's Gross Domestic Product (GDP) has been multiply by 4 during the 2000-2010 decade (National Bureau of Statistics of China), mostly because of the industry's growth. These evolutions have been accompanied by important increases of atmospheric pollutants emissions (Yinmin et al, Atmo Env, 2016). As a consequence and for about 10 years now, Chinese authorities have been working to reduce pollutant levels, because atmospheric pollution is a major health issue for Chinese population especially within cities, for which World Health Organisation's standards for major pollutants (Ozone, PM2.5, PM10) are often exceeded. Particles have multiple issues, as they impact on health and global warming. Their impacts will depend on their sources (primary or secondary pollutants) and natures (Particle size distribution, chemical composition…). Controlling particles loading is a complex task as their sources are various and dispersed on the Chinese territories: mineral dust can be emitted from Chinese deserts in large amount (Laurent et al., GPC, 2006), ammonia can be emitted from agriculture and livestock (Kang et al., ACP, 2016) and lots of urban primary pollutants can be emitted from urbanized areas. It is then necessary to work from a continental to local scales to understand more precisely pollution of urbanized areas. It is then mandatory to discriminate and quantify pollution sources and to estimate the impact of natural pollution and the major contributing sources. We propose here an approach based on a model and satellite observation synergy to estimate what controls Chinese pollution. We use the regional chemistry transport model CHIMERE (Menut et al., GMD, 2013) to simulate atmospheric pollutants concentrations. A large domain (72°E-145°E; 17.5°N-55°N), with a ¼°x¼° resolution is used to make multi-annual simulations. CHIMERE model include most of the pollutants

  3. Indoor Chemistry

    DEFF Research Database (Denmark)

    Weschler, Charles J.; Carslaw, Nicola

    2018-01-01

    This review aims to encapsulate the importance, ubiquity, and complexity of indoor chemistry. We discuss the many sources of indoor air pollutants and summarize their chemical reactions in the air and on surfaces. We also summarize some of the known impacts of human occupants, who act as sources...... and sinks of indoor chemicals, and whose activities (e.g., cooking, cleaning, smoking) can lead to extremely high pollutant concentrations. As we begin to use increasingly sensitive and selective instrumentation indoors, we are learning more about chemistry in this relatively understudied environment....

  4. Maintenance, outages and chemistry really can be compatible

    Energy Technology Data Exchange (ETDEWEB)

    Roberts, J.G.; Deaconescu, R. [Bruce Power, Tiverton, Ontario (Canada)

    2006-07-01

    'Full text:' In their address to the Canadian Nuclear Society, Bruce Power's Chemistry Design staff will describe how maintenance and outages can impact negatively on chemistry control and asset protection. Considerations of material impacts and material condition have significant influences on the approach to, and control of, chemistry. This applies equally to operation as it does during unit and/or system outages. Ideas will be presented as to how to facilitate making maintenance, outages and chemistry compatible. It will be shown how the lack of such an approach can lead to disastrous results. (author)

  5. 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

  6. 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.

  7. 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...

  8. HCN Production via Impact Ejecta Reentry During the Late Heavy Bombardment

    Science.gov (United States)

    Parkos, Devon; Pikus, Aaron; Alexeenko, Alina; Melosh, H. Jay

    2018-04-01

    Major impact events have shaped the Earth as we know it. The Late Heavy Bombardment is of particular interest because it immediately precedes the first evidence of life. The reentry of impact ejecta creates numerous chemical by-products, including biotic precursors such as HCN. This work examines the production of HCN during the Late Heavy Bombardment in more detail. We stochastically simulate the range of impacts on the early Earth and use models developed from existing studies to predict the corresponding ejecta properties. Using multiphase flow methods and finite-rate equilibrium chemistry, we then find the HCN production due to the resulting atmospheric heating. We use Direct Simulation Monte Carlo to develop a correction factor to account for increased yields due to thermochemical nonequilibrium. We then model 1-D atmospheric turbulent diffusion to find the time accurate transport of HCN to lower altitudes and ultimately surface water. Existing works estimate the necessary HCN molarity threshold to promote polymerization that is 0.01 M. For a mixing depth of 100 m, we find that the Late Heavy Bombardment will produce at least one impact event above this threshold with probability 24.1% for an oxidized atmosphere and 56.3% for a partially reduced atmosphere. For a mixing depth of 10 m, the probability is 79.5% for an oxidized atmosphere and 96.9% for a partially reduced atmosphere. Therefore, Late Heavy Bombardment impact ejecta is likely an HCN source sufficient for polymerization in shallow bodies of water, particularly if the atmosphere were in a partially reduced state.

  9. Analytical Chemistry and Measurement Science: (What Has DOE Done for Analytical Chemistry?)

    Science.gov (United States)

    Shults, W. D.

    1989-04-01

    Over the past forty years, analytical scientists within the DOE complex have had a tremendous impact on the field of analytical chemistry. This paper suggests six "high impact" research/development areas that either originated within or were brought to maturity within the DOE laboratories. "High impact" means they lead to new subdisciplines or to new ways of doing business.

  10. Tracking an atmospheric river in a warmer climate: from water vapor to economic impacts

    Science.gov (United States)

    Dominguez, Francina; Dall'erba, Sandy; Huang, Shuyi; Avelino, Andre; Mehran, Ali; Hu, Huancui; Schmidt, Arthur; Schick, Lawrence; Lettenmaier, Dennis

    2018-03-01

    Atmospheric rivers (ARs) account for more than 75 % of heavy precipitation events and nearly all of the extreme flooding events along the Olympic Mountains and western Cascade Mountains of western Washington state. In a warmer climate, ARs in this region are projected to become more frequent and intense, primarily due to increases in atmospheric water vapor. However, it is unclear how the changes in water vapor transport will affect regional flooding and associated economic impacts. In this work we present an integrated modeling system to quantify the atmospheric-hydrologic-hydraulic and economic impacts of the December 2007 AR event that impacted the Chehalis River basin in western Washington. We use the modeling system to project impacts under a hypothetical scenario in which the same December 2007 event occurs in a warmer climate. This method allows us to incorporate different types of uncertainty, including (a) alternative future radiative forcings, (b) different responses of the climate system to future radiative forcings and (c) different responses of the surface hydrologic system. In the warming scenario, AR integrated vapor transport increases; however, these changes do not translate into generalized increases in precipitation throughout the basin. The changes in precipitation translate into spatially heterogeneous changes in sub-basin runoff and increased streamflow along the entire Chehalis main stem. Economic losses due to stock damages increase moderately, but losses in terms of business interruption are significant. Our integrated modeling tool provides communities in the Chehalis region with a range of possible future physical and economic impacts associated with AR flooding.

  11. 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)

  12. 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...

  13. 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.

  14. Chemical Impact of Solar Energetic Particle Event From The Young Sun: Implications for the Origin of Prebiotic Chemistry and the Fain Young Sun Paradox

    Science.gov (United States)

    Airapetian, V.; Gronoff, G.; Hébrard, E.; Danchi, W.

    2015-12-01

    Understanding how the simple molecules present on the early Earth and possibly Mars may have set a path for complex biological molecules, the building blocks of life, represents one of greatest unsolved questions. Here we present a new model of the rise of the abiotic nitrogen fixation and associated pre-biotic chemistry in the early Earth and Mars atmosphere mediated by solar eruptive events. Our physical models of interaction of magnetic clouds ejected from the young Sun with magnetospheres of the early Earth show significant perturbations of geomagnetic fields that produce extended polar caps. These polar caps provide pathways for energetic particles associated with magnetic clouds to penetrate into the nitrogen-rich weakly reducing atmosphere and initiate the reactive chemistry by breaking molecular nitrogen, carbon dioxide, methane and producing hydrogen cyanide, the essential compound for life. The model also shows that contrary to the current models of warming of early Earth and Mars, major atmospheric constituents, CO2 and CH4 will be destroyed due to collisional dissociation with energetic particles. Instead, efficient formation of the potent greenhouse gas, nitrous oxide, as a by-product of these processes is expected. This mechanism can consistently explain the Faint Young Sun's paradox for the early atmospheres of Earth and Mars. Our new model provides insight into how life may have initiated on Earth and Mars and how to search for the spectral signatures on planets "pregnant" with the potential for life.

  15. 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.

  16. Impacts of elevated atmospheric CO2 on forest trees and forest ecosystems: knowledge gaps

    International Nuclear Information System (INIS)

    Karnosky, D.F.

    2003-06-01

    Atmospheric CO 2 is rising rapidly, and options for slowing the CO 2 rise are politically charged as they largely require reductions in industrial CO 2 emissions for most developed countries. As forests cover some 43% of the Earth's surface, account for some 70% of terrestrial net primary production (NPP), and are being bartered for carbon mitigation, it is critically important that we continue to reduce the uncertainties about the impacts of elevated atmospheric CO 2 on forest tree growth, productivity, and forest ecosystem function. In this paper, 1 review knowledge gaps and research needs on the effects of elevated atmospheric CO 2 on forest above- and below-ground growth and productivity, carbon sequestration, nutrient cycling, water relations, wood quality, phonology, community dynamics and biodiversity, antioxidants and stress tolerance, interactions with air pollutants, heterotrophic interactions, and ecosystem functioning. Finally, 1 discuss research needs regarding modelling of the impacts of elevated atmospheric CO 2 on forests. Even though there has been a tremendous amount of research done with elevated CO 2 and forest trees, it remains difficult to predict future forest growth and productivity under elevated atmospheric CO 2 . Likewise, it is not easy to predict how forest ecosystem processes will respond to enriched CO 2 . The more we study the impacts of increasing CO 2 , the more we realize that tree and forest responses are yet largely uncertain due to differences in responsiveness by species, genotype, and functional group, and the complex interactions of elevated atmospheric CO 2 with soil fertility, drought, pests, and co-occurring atmospheric pollutants such as nitrogen deposition and O 3 . Furthermore, it is impossible to predict ecosystem-level responses based on short-term studies of young trees grown without interacting stresses and in small spaces without the element of competition. Long-term studies using free-air CO 2 enrichment (FACE

  17. Impact of pH on Urine Chemistry Assayed on Roche Analyzers.

    Science.gov (United States)

    Cohen, R; Alkouri, R; Tostivint, I; Djiavoudine, S; Mestari, F; Dever, S; Atlan, G; Devilliers, C; Imbert-Bismut, F; Bonnefont-Rousselot, D; Monneret, D

    2017-10-01

    The pH may impact the concentration of certain urinary parameters, making urine pre-treatment questionable. 1) Determining the impact of pH in vitro on the urinary concentration of chemistry parameters assayed on Roche Modular analyzers. 2) Evaluating whether concentrations depended on pH in non-pretreated urines from patients. 1) The optimal urinary pH values for each measurement were: 6.3 ± 0.8 (amylase), 6.5 (uric acid). Urinary creatinine, sodium and urea concentrations were not pH-dependent. 2) In urines from patients, the pH was negatively associated with the concentration of some urinary parameters. However, concentrations of all the parameters were strongly and positively correlated with urinary creatinine, and relationships with pH were no longer evidenced after creatinine-normalization. The need for urine pH adjustment does not seem necessary when considering renal function. However, from an analytical and accreditation standpoint, the relationship between urine pH and several parameters justifies its measurement.

  18. The Potential Impact of Mars' Atmospheric Dust on Future Human Exploration of the Red Planet

    Science.gov (United States)

    Winterhalter, D.; Levine, J. S.; Kerschmann, R.; Beaty, D. W.; Carrier, B. L.; Ashley, J. W.

    2017-12-01

    With the increasing focus by NASA and other space agencies on a crewed mission to Mars in the 2039 time-frame, many Mars-specific environmental factors are now starting to be considered by NASA and other engineering teams. Learning from NASA's Apollo Missions to the Moon, where lunar dust turned out to be a significant challenge to mission and crew safety, attention is now turning to the dust in Mars' atmosphere and regolith. To start the process of identifying possible dust-caused challenges to the human presence on Mars, and thus aid early engineering and mission design efforts, the NASA Engineering and Safety Center (NESC) Robotic Spacecraft Technical Discipline Team organized and conducted a Workshop on the "Dust in Mars' Atmosphere and Its Impact on the Human Exploration of Mars", held at the Lunar and Planetary Institute (LPI), Houston, TX, June 13-15, 2017. The workshop addressed the following general areas: 1. What is known about Mars' dust in terms of its physical and chemical properties, its local and global abundance and composition, and its variability.2. What is the impact of Mars atmospheric dust on human health.3. What is the impact of Mars atmospheric dust on surface mechanical systems (e.g., spacesuits, habitats, mobility systems, etc.). We present the top priority issues identified in the workshop.

  19. Heterogeneous Uptake of HO2 Radicals onto Atmospheric Aerosols

    Science.gov (United States)

    George, I. J.; Matthews, P. S.; Brooks, B.; Goddard, A.; Whalley, L. K.; Baeza-Romero, M. T.; Heard, D. E.

    2011-12-01

    The hydroxyl (OH) and hydroperoxyl (HO2) radicals, together known as HOx, play a vital role in atmospheric chemistry by controlling the oxidative capacity of the troposphere. The atmospheric lifetime and concentrations of many trace reactive species, such as volatile organic compounds (VOCs), are determined by HOx radical levels. Therefore, the ability to accurately predict atmospheric HOx concentrations from a detailed knowledge of their sources and sinks is a very useful diagnostic tool to assess our current understanding of atmospheric chemistry. Several recent field studies have observed significantly lower concentrations of HO2 radicals than predicted using box models, where HO2 loss onto aerosols was suggested as a possible missing sink [1, 2]. However, the mechanism on HO2 uptake onto aerosols and its impact on ambient HOx levels are currently not well understood. To improve our understanding of this process, we have conducted laboratory experiments to measure HO2 uptake coefficients onto submicron aerosol particles. The FAGE (Fluorescence Assay by Gas Expansion) technique, a highly sensitive laser induced fluorescence based detection method, was used to monitor HO2 uptake kinetics onto aerosol particles in an aerosol flow tube. The application of the FAGE technique allowed for kinetic experiments to be performed under low HO2 concentrations, i.e. [HO2] atomizing dilute salt solutions or by homogeneous nucleation. HO2 uptake coefficients (γ) have been measured for single-component solid and aqueous inorganic salt and organic aerosol particles with a wide range of hygroscopicities. HO2 uptake coefficients on solid particles were below the detection limit (γ < 0.001), whereas on aqueous aerosols uptake coefficients were somewhat larger (γ = 0.001 - 0.008). HO2 uptake coefficients were highest on aerosols containing metal ions, such as Cu and Fe. Humidity and aerosol pH did not significantly impact the reactive HO2 uptake. Preliminary experiments have also

  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. Ozone in the atmosphere. Basic principles, natural and human impacts

    Energy Technology Data Exchange (ETDEWEB)

    Fabian, Peter [Technical Univ. Munich (Germany). Immission Research; Dameris, Martin [German Aerospace Center (DLR), Oberpfaffenhofen-Wessling (Germany). Inst. of Atmospheric Physics

    2014-09-01

    Comprehensive coverage of ozone both in the upper and the lower atmosphere. Essential overview of atmospheric ozone research written by two experienced and acknowledged experts. Numerous qualified references to the scientific literature. Peter Fabian and Martin Dameris provide a concise yet comprehensive overview of established scientific knowledge about ozone in the atmosphere. They present both ozone changes and trends in the stratosphere, as well as the effects of overabundance in the troposphere including the phenomenon of photosmog. Aspects such as photochemistry, atmospheric dynamics and global ozone distribution as well as various techniques for ozone measurement are treated. The authors outline the various causes for ozone depletion, the effects of ozone pollution and the relation to climate change. The book provides a handy reference guide for researchers active in atmospheric ozone research and a useful introduction for advanced students specializing in this field. Non-specialists interested in this field will also profit from reading the book. Peter Fabian can look back on a life-long active career in ozone research, having first gained international recognition for his measurements of the global distribution of halogenated hydrocarbons. He also pioneered photosmog investigations in the metropolitan areas of Munich, Berlin, Athens and Santiago de Chile, and his KROFEX facility provided controlled ozone fumigation of adult tree canopies for biologists to investigate the effects of ozone increases on forests. Besides having published a broad range of scientific articles, he has also been the author or editor of numerous books. From 2002 to 2005 he served the European Geosciences Union (EGU) as their first and Founding President. Martin Dameris is a prominent atmospheric modeler whose interests include the impacts of all kinds of natural and man-made disturbances on the atmospheric system. His scientific work focuses on the connections between ozone and

  2. Ozone in the atmosphere. Basic principles, natural and human impacts

    International Nuclear Information System (INIS)

    Fabian, Peter; Dameris, Martin

    2014-01-01

    Comprehensive coverage of ozone both in the upper and the lower atmosphere. Essential overview of atmospheric ozone research written by two experienced and acknowledged experts. Numerous qualified references to the scientific literature. Peter Fabian and Martin Dameris provide a concise yet comprehensive overview of established scientific knowledge about ozone in the atmosphere. They present both ozone changes and trends in the stratosphere, as well as the effects of overabundance in the troposphere including the phenomenon of photosmog. Aspects such as photochemistry, atmospheric dynamics and global ozone distribution as well as various techniques for ozone measurement are treated. The authors outline the various causes for ozone depletion, the effects of ozone pollution and the relation to climate change. The book provides a handy reference guide for researchers active in atmospheric ozone research and a useful introduction for advanced students specializing in this field. Non-specialists interested in this field will also profit from reading the book. Peter Fabian can look back on a life-long active career in ozone research, having first gained international recognition for his measurements of the global distribution of halogenated hydrocarbons. He also pioneered photosmog investigations in the metropolitan areas of Munich, Berlin, Athens and Santiago de Chile, and his KROFEX facility provided controlled ozone fumigation of adult tree canopies for biologists to investigate the effects of ozone increases on forests. Besides having published a broad range of scientific articles, he has also been the author or editor of numerous books. From 2002 to 2005 he served the European Geosciences Union (EGU) as their first and Founding President. Martin Dameris is a prominent atmospheric modeler whose interests include the impacts of all kinds of natural and man-made disturbances on the atmospheric system. His scientific work focuses on the connections between ozone and

  3. The global impact of the transport sectors on atmospheric aerosol: simulations for year 2000 emissions

    Directory of Open Access Journals (Sweden)

    M. Righi

    2013-10-01

    Full Text Available We use the EMAC (ECHAM/MESSy Atmospheric Chemistry global model with the aerosol module MADE (Modal Aerosol Dynamics model for Europe, adapted for global applications to quantify the impact of transport emissions (land transport, shipping and aviation on the global aerosol. We consider a present-day (2000 scenario according to the CMIP5 (Climate Model Intercomparison Project Phase 5 emission data set developed in support of the IPCC (Intergovernmental Panel on Climate Change Fifth Assessment Report. The model takes into account particle mass and number emissions: The latter are derived from mass emissions under different assumptions on the size distribution of particles emitted by the three transport sectors. Additional sensitivity experiments are performed to quantify the effects of the uncertainties behind such assumptions. The model simulations show that the impact of the transport sectors closely matches the emission patterns. Land transport is the most important source of black carbon (BC pollution in the USA, Europe and the Arabian Peninsula, contributing up to 60–70% of the total surface-level BC concentration in these regions. Shipping contributes about 40–60% of the total aerosol sulfate surface-level concentration along the most-traveled routes of the northern Atlantic and northern Pacific oceans, with a significant impact (~ 10–20% along the coastlines. Aviation mostly affects aerosol number, contributing about 30–40% of the particle number concentration in the northern midlatitudes' upper troposphere (7–12 km, although significant effects are also simulated at the ground, due to the emissions from landing and take-off cycles. The transport-induced perturbations to the particle number concentrations are very sensitive to the assumptions on the size distribution of emitted particles, with the largest uncertainties (about one order of magnitude obtained for the land transport sector. The simulated climate impacts, due to

  4. 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

  5. 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.

  6. Analysis of water-soluble fraction of metals in atmospheric aerosols using aerosol counterflow two-jets unit and chemiluminescent detection

    Czech Academy of Sciences Publication Activity Database

    Vojtěšek, Martin; Mikuška, Pavel; Večeřa, Zbyněk; Křůmal, Kamil

    2012-01-01

    Roč. 92, č. 4 (2012), s. 432-449 ISSN 0306-7319 R&D Projects: GA MŽP SP/1A3/148/08; GA MŽP SP/1B7/189/07; GA MŽP SP/1A3/55/08 Institutional research plan: CEZ:AV0Z40310501 Keywords : atmospheric aerosols * metals * continuous aerosol collector Subject RIV: CB - Analytical Chemistry, Separation Impact factor: 1.240, year: 2012

  7. 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

  8. Aerosol chemistry in Titan's ionosphere: simultaneous growth and etching processes

    Science.gov (United States)

    Carrasco, Nathalie; Cernogora, Guy; Jomard, François; Etcheberry, Arnaud; Vigneron, Jackie

    2016-10-01

    Since the Cassini-CAPS measurements, organic aerosols are known to be present and formed at high altitudes in the diluted and partially ionized medium that is Titan's ionosphere [1]. This unexpected chemistry can be further investigated in the laboratory with plasma experiments simulating the complex ion-neutral chemistry starting from N2-CH4 [2]. Two sorts of solid organic samples can be produced in laboratory experiments simulating Titan's atmospheric reactivity: grains in the volume and thin films on the reactor walls. We expect that grains are more representative of Titan's atmospheric aerosols, but films are used to provide optical indices for radiative models of Titan's atmosphere.The aim of the present study is to address if these two sorts of analogues are chemically equivalent or not, when produced in the same N2-CH4 plasma discharge. The chemical compositions of both these materials are measured by using elemental analysis, XPS analysis and Secondary Ion Mass Spectrometry. We find that films are homogeneous but significantly less rich in nitrogen and hydrogen than grains produced in the same experimental conditions. This surprising difference in their chemical compositions is explained by the efficient etching occurring on the films, which stay in the discharge during the whole plasma duration, whereas the grains are ejected after a few minutes [3]. The impact for our understanding of Titan's aerosols chemical composition is important. Our study shows that chemical growth and etching process are simultaneously at stake in Titan's ionosphere. The more the aerosols stay in the ionosphere, the more graphitized they get through etching process. In order to infer Titan's aerosols composition, our work highlights a need for constraints on the residence time of aerosols in Titan's ionosphere. [1] Waite et al. (2009) Science , 316, p. 870[2] Szopa et al. (2006) PSS, 54, p. 394[3] Carrasco et al. (2016) PSS, 128, p. 52

  9. Fog and precipitation chemistry at a mid-land forest in central Taiwan.

    Science.gov (United States)

    Liang, Yang-Ling; Lin, Teng-Chiu; Hwong, Jeen-Liang; Lin, Neng-Huei; Wang, Chiao-Ping

    2009-01-01

    We analyzed fog and bulk precipitation chemistry at a cloud forest in central Taiwan where mountain agriculture activities are highest. There were 320 foggy days (visibility agriculture has a major impact on atmospheric deposition at the surrounding forest ecosystems. The input of inorganic N reached 125 kg N ha(-1) yr(-1) and likely exceeded the biological demand of the forest ecosystem. Sulfate is the most abundant anion in fog at Chi-tou and in precipitation at various forests throughout Taiwan, suggesting that the emission and transport of large quantities of SO(2,) the precursor of SO(4)(2-), is an island-wide environmental issue.

  10. 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

  11. Coupled Regional Ocean-Atmosphere Modeling of the Mount Pinatubo Impact on the Red Sea

    Science.gov (United States)

    Stenchikov, G. L.; Osipov, S.

    2017-12-01

    The 1991 eruption of Mount Pinatubo had dramatic effects on the regional climate in the Middle East. Though acknowledged, these effects have not been thoroughly studied. To fill this gap and to advance understanding of the mechanisms that control variability in the Middle East's regional climate, we simulated the impact of the 1991 Pinatubo eruption using a regional coupled ocean-atmosphere modeling system set for the Middle East and North Africa (MENA) domain. We used the Coupled Ocean-Atmosphere-Wave-Sediment Transport (COAWST) framework, which couples the Weather Research and Forecasting Model (WRF) model with the Regional Oceanic Modeling System (ROMS). We modified the WRF model to account for the radiative effect of volcanic aerosols. Our coupled ocean-atmosphere simulations verified by available observations revealed strong perturbations in the energy balance of the Red Sea, which drove thermal and circulation responses. Our modeling approach allowed us to separate changes in the atmospheric circulation caused by the impact of the volcano from direct regional radiative cooling from volcanic aerosols. The atmospheric circulation effect was significantly stronger than the direct volcanic aerosols effect. We found that the Red Sea response to the Pinatubo eruption was stronger and qualitatively different from that of the global ocean system. Our results suggest that major volcanic eruptions significantly affect the climate in the Middle East and the Red Sea and should be carefully taken into account in assessments of long-term climate variability and warming trends in MENA and the Red Sea.

  12. The atmospheric impacts of monoterpene ozonolysis on global stabilised Criegee intermediate budgets and SO2 oxidation: experiment, theory and modelling

    Directory of Open Access Journals (Sweden)

    M. J. Newland

    2018-05-01

    Full Text Available The gas-phase reaction of alkenes with ozone is known to produce stabilised Criegee intermediates (SCIs. These biradical/zwitterionic species have the potential to act as atmospheric oxidants for trace pollutants such as SO2, enhancing the formation of sulfate aerosol with impacts on air quality and health, radiative transfer and climate. However, the importance of this chemistry is uncertain as a consequence of limited understanding of the abundance and atmospheric fate of SCIs. In this work we apply experimental, theoretical and numerical modelling methods to quantify the atmospheric impacts, abundance and fate of the structurally diverse SCIs derived from the ozonolysis of monoterpenes, the second most abundant group of unsaturated hydrocarbons in the atmosphere. We have investigated the removal of SO2 by SCIs formed from the ozonolysis of three atmospherically important monoterpenes (α-pinene, β-pinene and limonene in the presence of varying amounts of water vapour in large-scale simulation chamber experiments that are representative of boundary layer conditions. The SO2 removal displays a clear dependence on water vapour concentration, but this dependence is not linear across the range of [H2O] explored. At low [H2O] a strong dependence of SO2 removal on [H2O] is observed, while at higher [H2O] this dependence becomes much weaker. This is interpreted as being caused by the production of a variety of structurally (and hence chemically different SCIs in each of the systems studied, which displayed different rates of reaction with water and of unimolecular rearrangement or decomposition. The determined rate constants, k(SCI+H2O, for those SCIs that react primarily with H2O range from 4 to 310  ×  10−15 cm3 s−1. For those SCIs that predominantly react unimolecularly, determined rates range from 130 to 240 s−1. These values are in line with previous results for the (analogous stereo-specific SCI system of syn-/anti-CH3

  13. The atmospheric impacts of monoterpene ozonolysis on global stabilised Criegee intermediate budgets and SO2 oxidation: experiment, theory and modelling

    Science.gov (United States)

    Newland, Mike J.; Rickard, Andrew R.; Sherwen, Tomás; Evans, Mathew J.; Vereecken, Luc; Muñoz, Amalia; Ródenas, Milagros; Bloss, William J.

    2018-05-01

    The gas-phase reaction of alkenes with ozone is known to produce stabilised Criegee intermediates (SCIs). These biradical/zwitterionic species have the potential to act as atmospheric oxidants for trace pollutants such as SO2, enhancing the formation of sulfate aerosol with impacts on air quality and health, radiative transfer and climate. However, the importance of this chemistry is uncertain as a consequence of limited understanding of the abundance and atmospheric fate of SCIs. In this work we apply experimental, theoretical and numerical modelling methods to quantify the atmospheric impacts, abundance and fate of the structurally diverse SCIs derived from the ozonolysis of monoterpenes, the second most abundant group of unsaturated hydrocarbons in the atmosphere. We have investigated the removal of SO2 by SCIs formed from the ozonolysis of three atmospherically important monoterpenes (α-pinene, β-pinene and limonene) in the presence of varying amounts of water vapour in large-scale simulation chamber experiments that are representative of boundary layer conditions. The SO2 removal displays a clear dependence on water vapour concentration, but this dependence is not linear across the range of [H2O] explored. At low [H2O] a strong dependence of SO2 removal on [H2O] is observed, while at higher [H2O] this dependence becomes much weaker. This is interpreted as being caused by the production of a variety of structurally (and hence chemically) different SCIs in each of the systems studied, which displayed different rates of reaction with water and of unimolecular rearrangement or decomposition. The determined rate constants, k(SCI+H2O), for those SCIs that react primarily with H2O range from 4 to 310 × 10-15 cm3 s-1. For those SCIs that predominantly react unimolecularly, determined rates range from 130 to 240 s-1. These values are in line with previous results for the (analogous) stereo-specific SCI system of syn-/anti-CH3CHOO. The experimental results are

  14. Atmospheres of partially differentiated super-Earth exoplanets

    Science.gov (United States)

    Schaefer, Laura; Sasselov, Dimitar

    2015-11-01

    Terrestrial exoplanets have been discovered in a range of sizes, densities and orbital locations that defy our expectations based upon the Solar System. Planets discovered to date with radii less than ~1.5-1.6 Earth radii all seem to fall on an iso-density curve with the Earth [1]. However, mass and radius determinations, which depend on the known properties of the host star, are not accurate enough to distinguish between a fully differentiated three-layer planet (core, mantle, ocean/atmosphere) and an incompletely differentiated planet [2]. Full differentiation of a planet will depend upon the conditions at the time of accretion, including the abundance of short-lived radioisotopes, which will vary from system to system, as well as the number of giant impacts the planet experiences. Furthermore, separation of metal and silicates at the much larger pressures found inside super-Earths will depend on how the chemistry of these materials change at high pressures. There are therefore hints emerging that not all super-Earths will be fully differentiated. Incomplete differentiation will result in a more reduced mantle oxidation state and may have implications for the composition of an outgassed atmosphere. Here we will present the first results from a chemical equilibrium model of the composition of such an outgassed atmosphere and discuss the possibility of distinguishing between fully and incompletely differentiated planets through atmospheric observations.[1] Rogers, L. 2015. ApJ, 801, 41. [2] Zeng, L. & Sasselov, D. 2013. PASP, 125, 227.

  15. IMPACT OF ATMOSPHERIC CHROMATIC EFFECTS ON WEAK LENSING MEASUREMENTS

    International Nuclear Information System (INIS)

    Meyers, Joshua E.; Burchat, Patricia R.

    2015-01-01

    Current and future imaging surveys will measure cosmic shear with statistical precision that demands a deeper understanding of potential systematic biases in galaxy shape measurements than has been achieved to date. We use analytic and computational techniques to study the impact on shape measurements of two atmospheric chromatic effects for ground-based surveys such as the Dark Energy Survey and the Large Synoptic Survey Telescope (LSST): (1) atmospheric differential chromatic refraction and (2) wavelength dependence of seeing. We investigate the effects of using the point-spread function (PSF) measured with stars to determine the shapes of galaxies that have different spectral energy distributions than the stars. We find that both chromatic effects lead to significant biases in galaxy shape measurements for current and future surveys, if not corrected. Using simulated galaxy images, we find a form of chromatic “model bias” that arises when fitting a galaxy image with a model that has been convolved with a stellar, instead of galactic, PSF. We show that both forms of atmospheric chromatic biases can be predicted (and corrected) with minimal model bias by applying an ordered set of perturbative PSF-level corrections based on machine-learning techniques applied to six-band photometry. Catalog-level corrections do not address the model bias. We conclude that achieving the ultimate precision for weak lensing from current and future ground-based imaging surveys requires a detailed understanding of the wavelength dependence of the PSF from the atmosphere, and from other sources such as optics and sensors. The source code for this analysis is available at https://github.com/DarkEnergyScienceCollaboration/chroma

  16. IMPACT OF ATMOSPHERIC CHROMATIC EFFECTS ON WEAK LENSING MEASUREMENTS

    Energy Technology Data Exchange (ETDEWEB)

    Meyers, Joshua E.; Burchat, Patricia R., E-mail: jmeyers314@gmail.com [Kavli Institute for Particle Astrophysics and Cosmology, Department of Physics, Stanford University, Stanford, CA 94305 (United States)

    2015-07-10

    Current and future imaging surveys will measure cosmic shear with statistical precision that demands a deeper understanding of potential systematic biases in galaxy shape measurements than has been achieved to date. We use analytic and computational techniques to study the impact on shape measurements of two atmospheric chromatic effects for ground-based surveys such as the Dark Energy Survey and the Large Synoptic Survey Telescope (LSST): (1) atmospheric differential chromatic refraction and (2) wavelength dependence of seeing. We investigate the effects of using the point-spread function (PSF) measured with stars to determine the shapes of galaxies that have different spectral energy distributions than the stars. We find that both chromatic effects lead to significant biases in galaxy shape measurements for current and future surveys, if not corrected. Using simulated galaxy images, we find a form of chromatic “model bias” that arises when fitting a galaxy image with a model that has been convolved with a stellar, instead of galactic, PSF. We show that both forms of atmospheric chromatic biases can be predicted (and corrected) with minimal model bias by applying an ordered set of perturbative PSF-level corrections based on machine-learning techniques applied to six-band photometry. Catalog-level corrections do not address the model bias. We conclude that achieving the ultimate precision for weak lensing from current and future ground-based imaging surveys requires a detailed understanding of the wavelength dependence of the PSF from the atmosphere, and from other sources such as optics and sensors. The source code for this analysis is available at https://github.com/DarkEnergyScienceCollaboration/chroma.

  17. Uncertainty in biogenic isoprene emissions and its impacts on tropospheric chemistry in East Asia

    International Nuclear Information System (INIS)

    Han, K.M.; Park, R.S.; Kim, H.K.; Woo, J.H.; Kim, J.; Song, C.H.

    2013-01-01

    In this study, the accuracy of biogenic isoprene emission fluxes over East Asia during two summer months (July and August) was examined by comparing two tropospheric HCHO columns (Ω HCHO ) obtained from the SCIAMACHY sensor and the Community Multi-scale Air Quality (CMAQ v4.7.1) model simulations, using three available biogenic isoprene emission inventories over East Asia: i) GEIA, ii) MEGAN and iii) MOHYCAN. From this comparative analysis, the tropospheric HCHO columns from the CMAQ model simulations, using the MEGAN and MOHYCAN emission inventories (Ω CMAQ, MEGAN and Ω CMAQ, MOHYCAN ), were found to agree well with the tropospheric HCHO columns from the SCIAMACHY observations (Ω SCIA ). Secondly, the propagation of such uncertainties in the biogenic isoprene emission fluxes to the levels of atmospheric oxidants (e.g., OH and HO 2 ) and other atmospheric gaseous/particulate species over East Asia during the two summer months was also investigated. As the biogenic isoprene emission fluxes decreased from the GEIA to the MEGAN emission inventories, the levels of OH radicals increased by factors of 1.39 and 1.75 over Central East China (CEC) and South China, respectively. Such increases in the OH radical mixing ratios subsequently influence the partitioning of HO y species. For example, the HO 2 /OH ratios from the CMAQ model simulations with GEIA isoprene emissions were 2.7 times larger than those from the CMAQ model simulations based on MEGAN isoprene emissions. The large HO 2 /OH ratios from the CMAQ model simulations with the GEIA biogenic emission were possibly due to the overestimation of GEIA biogenic isoprene emissions over East Asia. It was also shown that such large changes in HO x radicals created large differences on other tropospheric compounds (e.g., NO y chemistry) over East Asia during the summer months. - Highlights: • GEIA isoprene emissions were possibly overestimated over East Asia. • Using MEGAN or MOHYCAN emissions in CMAQ well captured

  18. Transport impacts on atmosphere and climate: Shipping

    Science.gov (United States)

    Eyring, Veronika; Isaksen, Ivar S. A.; Berntsen, Terje; Collins, William J.; Corbett, James J.; Endresen, Oyvind; Grainger, Roy G.; Moldanova, Jana; Schlager, Hans; Stevenson, David S.

    2010-12-01

    Emissions of exhaust gases and particles from oceangoing ships are a significant and growing contributor to the total emissions from the transportation sector. We present an assessment of the contribution of gaseous and particulate emissions from oceangoing shipping to anthropogenic emissions and air quality. We also assess the degradation in human health and climate change created by these emissions. Regulating ship emissions requires comprehensive knowledge of current fuel consumption and emissions, understanding of their impact on atmospheric composition and climate, and projections of potential future evolutions and mitigation options. Nearly 70% of ship emissions occur within 400 km of coastlines, causing air quality problems through the formation of ground-level ozone, sulphur emissions and particulate matter in coastal areas and harbours with heavy traffic. Furthermore, ozone and aerosol precursor emissions as well as their derivative species from ships may be transported in the atmosphere over several hundreds of kilometres, and thus contribute to air quality problems further inland, even though they are emitted at sea. In addition, ship emissions impact climate. Recent studies indicate that the cooling due to altered clouds far outweighs the warming effects from greenhouse gases such as carbon dioxide (CO 2) or ozone from shipping, overall causing a negative present-day radiative forcing (RF). Current efforts to reduce sulphur and other pollutants from shipping may modify this. However, given the short residence time of sulphate compared to CO 2, the climate response from sulphate is of the order decades while that of CO 2 is centuries. The climatic trade-off between positive and negative radiative forcing is still a topic of scientific research, but from what is currently known, a simple cancellation of global mean forcing components is potentially inappropriate and a more comprehensive assessment metric is required. The CO 2 equivalent emissions using

  19. Spectroscopic Investigations of High-Power Laser Sparks in Gas Mixtures Containing Methane: A Laboratory Model of Energetic Events in Strongly Reduced Planetary Atmospheres

    Czech Academy of Sciences Publication Activity Database

    Civiš, Svatopluk; Civiš, Martin; Rašín, R.; Kamas, Michal; Dryahina, Kseniya; Španěl, Patrik; Juha, Libor; Ferus, Martin

    2009-01-01

    Roč. 39, 3-4 (2009), s. 217-217 ISSN 0169-6149 R&D Projects: GA MŠk LC510; GA MŠk(CZ) LC528; GA ČR GA203/06/1278 Institutional research plan: CEZ:AV0Z40400503; CEZ:AV0Z10100523 Keywords : planetary atmosphere * lasers * spectroscopy Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.053, year: 2009

  20. 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.

  1. Modeling impacts of NH{sub 3} on uptake of H{sub 2}SO{sub 4} by charged nucleating nanoparticles in the Earth's atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Nadykto, A. B., E-mail: anadykto@gmail.com [Atmospheric Science Research Center, State University of New York at Albany, 251 Fuller Road, Albany, NY 12203 (United States); Department of Applied Mathematics, Moscow State University of Technology “STANKIN”, Vadkovsky per. 1, Moscow 127055 (Russian Federation); Nazarenko, K. M.; Markov, P. N. [Department of Applied Mathematics, Moscow State University of Technology “STANKIN”, Vadkovsky per. 1, Moscow 127055 (Russian Federation); Yu, F. [Atmospheric Science Research Center, State University of New York at Albany, 251 Fuller Road, Albany, NY 12203 (United States)

    2016-06-08

    The understanding of the role of ammonia, a well-known stabilizer of binary sulfuric acid-water clusters, in the gas-to-nanoparticle conversion in the Earth atmosphere is critically important for the assessment of aerosol radiative forcing associated with the climate changes. The sulfuric acid H{sub 2}SO{sub 4} is present in the atmosphere in the form of the gas-phase hydrates (H{sub 2}SO{sub 4})(H{sub 2}O){sub n}, whose interaction with NH{sub 3} leads to the formation of more stable bisulfate clusters (NH{sub 3})(H{sub 2}SO{sub 4})(H{sub 2}O){sub n}. Although the impact of NH{sub 3} on the thermochemical stability of binary clusters nucleating homogeneously has been studied in some detail in the past, the effect of ammonia on other microphysical properties relevant to nucleation remains insufficiently well understood. In the present study, the effect of ammonia on the electrical dipole moment controlling the nucleation of airborne ions via the dipole-charge interaction has been investigated using the Density Functional Theory (DFT), ab initio MP2 and model chemistry G3 methods. The presence of ammonia in (H{sub 2}SO{sub 4})(H{sub 2}O){sub n} is found to lead to very large enhancement in the dipole moment, which exceeds 2.0-2.5 Debyes (∼60-80%), 3.7-5.0 Debyes (∼90-180%), 1.4-4.5 Debyes (∼50-150%) and 2.1-5.5 Debyes (∼60-700%) for n = 0, n = 1, n = 2 and n = 3, respectively. The implications of this include the significantly increased uptake of the sulfuric acid, the key atmospheric nucleation precursor, by airborne ions and neutrals (due to dipole-dipole interaction), enhanced nucleation rates and the elevated production of ultrafine particles, which cause adverse health impacts.

  2. 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

  3. 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

  4. The EtnaPlumeLab (EPL research cluster: advance the understanding of Mt. Etna plume, from source characterisation to downwind impact

    Directory of Open Access Journals (Sweden)

    Pasquale Sellitto

    2017-01-01

    Full Text Available In 2013, a multidisciplinary research cluster named EtnaPlumeLab (EPL was established, gathering experts from volcanology and atmospheric science communities. Target of EPL is to advance the understanding of Mt. Etna's gas and aerosol emissions and the related processes, from source to its regional climatic impact in the Mediterranean area. Here, we present the cluster and its three interacting modules: EPL-RADIO (Radioactive Aerosols and other source parameters for better atmospheric Dispersion and Impact estimatiOns, SMED (Sulfur MEditerranean Dispersion and Med-SuV (MEDiterranean SUpersite Volcanoes Work Package 5. Preliminary results have for the first time highlighted the relevance of Mt. Etna's plume impact at the Mediterranean regional scale. These results underline that further efforts need to be made to get insight into a synoptic volcanogenic-atmospheric chemistry/climatic understanding of volcanic plumes impact.

  5. 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...

  6. 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.

  7. 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...

  8. Climate/chemistry feedbacks and biogenic emissions.

    Science.gov (United States)

    Pyle, John A; Warwick, Nicola; Yang, Xin; Young, Paul J; Zeng, Guang

    2007-07-15

    The oxidizing capacity of the atmosphere is affected by anthropogenic emissions and is projected to change in the future. Model calculations indicate that the change in surface ozone at some locations could be large and have significant implications for human health. The calculations depend on the precise scenarios used for the anthropogenic emissions and on the details of the feedback processes included in the model. One important factor is how natural biogenic emissions will change in the future. We carry out a sensitivity calculation to address the possible increase in isoprene emissions consequent on increased surface temperature in a future climate. The changes in ozone are significant but depend crucially on the background chemical regime. In these calculations, we find that increased isoprene will increase ozone in the Northern Hemisphere but decrease ozone in the tropics. We also consider the role of bromine compounds in tropospheric chemistry and consider cases where, in a future climate, the impact of bromine could change.

  9. 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...

  10. Impact of urban atmospheric environment on hospital admissions in the elderly

    Directory of Open Access Journals (Sweden)

    Edelci Nunes da Silva

    2012-08-01

    Full Text Available OBJECTIVE: To analyze the impact of intra-urban atmospheric conditions on circulatory and respiratory diseases in elder adults. METHODS: Cross-sectional study based on data from 33,212 hospital admissions in adults over 60 years in the city of São Paulo, southeastern Brazil, from 2003 to 2007. The association between atmospheric variables from Congonhas airport and bioclimatic index, Physiological Equivalent Temperature, was analyzed according to the district's socioenvironmental profile. Descriptive statistical analysis and regression models were used. RESULTS: There was an increase in hospital admissions due to circulatory diseases as average and lowest temperatures decreased. The likelihood of being admitted to the hospital increased by 12% with 1ºC decrease in the bioclimatic index and with 1ºC increase in the highest temperatures in the group with lower socioenvironmental conditions. The risk of admission due to respiratory diseases increased with inadequate air quality in districts with higher socioenvironmental conditions. CONCLUSIONS: The associations between morbidity and climate variables and the comfort index varied in different groups and diseases. Lower and higher temperatures increased the risk of hospital admission in the elderly. Districts with lower socioenvironmental conditions showed greater adverse health impacts.

  11. Evaluation of Biogenic and Fire Emissions in a Global Chemistry Model with NOMADSS, DC3 and SEAC4RS observations

    Science.gov (United States)

    Emmons, L. K.; Wiedinmyer, C.; Park, M.; Kaser, L.; Apel, E. C.; Guenther, A. B.

    2014-12-01

    Numerous measurements of compounds produced by biogenic and fire emissions were made during several recent field campaigns in the southeast United States, providing a unique data set for emissions and chemical model evaluation. The NCAR Community Atmosphere Model with Chemistry (CAM-chem) is coupled to the Community Land Model (CLM), which includes the biogenic emissions model MEGAN-v2.1, allowing for online calculation of emissions from vegetation for 150 compounds. Simulations of CAM-chem for summers 2012 and 2013 are evaluated with the aircraft and ground-based observations from DC3, NOMADSS and SEAC4RS. Comparison of directly emitted biogenic species, such as isoprene, terpenes, methanol and acetone, are used to evaluate the MEGAN emissions. Evaluation of oxidation products, including methyl vinyl ketone (MVK), methacrolein, formaldehyde, and other oxygenated VOCs are used to test the model chemistry mechanism. In addition, several biomass burning inventories are used in the model, including FINN, QFED, and FLAMBE, and are compared for their impact on atmospheric composition and ozone production, and evaluated with the aircraft observations.

  12. 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

  13. 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.

  14. Review: Impacts of permafrost degradation on inorganic chemistry of surface fresh water

    Science.gov (United States)

    Colombo, Nicola; Salerno, Franco; Gruber, Stephan; Freppaz, Michele; Williams, Mark; Fratianni, Simona; Giardino, Marco

    2018-03-01

    Recent studies have shown that climate change is impacting the inorganic chemical characteristics of surface fresh water in permafrost areas and affecting aquatic ecosystems. Concentrations of major ions (e.g., Ca2 +, Mg2 +, SO42 -, NO3-) can increase following permafrost degradation with associated deepening of flow pathways and increased contributions of deep groundwater. In addition, thickening of the active layer and melting of near-surface ground ice can influence inorganic chemical fluxes from permafrost into surface water. Permafrost degradation has also the capability to modify trace element (e.g., Ni, Mn, Al, Hg, Pb) contents in surface water. Although several local and regional modifications of inorganic chemistry of surface fresh water have been attributed to permafrost degradation, a comprehensive review of the observed changes is lacking. The goal of this paper is to distil insight gained across differing permafrost settings through the identification of common patterns in previous studies, at global scale. In this review we focus on three typical permafrost configurations (pervasive permafrost degradation, thermokarst, and thawing rock glaciers) as examples and distinguish impacts on (i) major ions and (ii) trace elements. Consequences of warming climate have caused spatially-distributed progressive increases of major ion and trace element delivery to surface fresh water in both polar and mountain areas following pervasive permafrost degradation. Moreover, localised releases of major ions and trace elements to surface water due to the liberation of soluble materials sequestered in permafrost and ground ice have been found in ice-rich terrains both at high latitude (thermokarst features) and high elevation (rock glaciers). Further release of solutes and related transport to surface fresh water can be expected under warming climatic conditions. However, complex interactions among several factors able to influence the timing and magnitude of the impacts

  15. 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.

  16. 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.

  17. 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.

  18. Photochemical Haze Formation in the Atmospheres of Super-Earths and Mini-Neptunes

    Science.gov (United States)

    He, Chao; Hoerst, Sarah M.; Lewis, Nikole K.; Yu, Xinting; Moses, Julianne I.; Kempton, Eliza M.- R.; Marley, Mark S.; McGuiggan, Patricia; Morley, Caroline V.; Valenti, Jeff A.; hide

    2018-01-01

    UV (ultraviolet) radiation can induce photochemical processes in the atmospheres of exoplanet and produce haze particles. Recent transmission spectra of super-Earths and mini-Neptunes have demonstrated the possibility that exoplanets have haze/cloud layers at high altitudes in their atmospheres. Haze particles play an important role in planetary atmospheres because they affect the chemistry, dynamics, and radiation flux in planetary atmospheres, and may provide a source of organic material to the surface which may impact the origin or evolution of life. However, very little information is known about photochemical processes in cool, high-metallicity exoplanetary atmospheres. We present here photochemical haze formation in laboratory simulation experiments with UV radiation; we explored temperatures ranging from 300 to 600 degrees Kelvin and a range of atmospheric metallicities (100 times, 1000 times, and 10000 times solar metallicity). We find that photochemical hazes are generated in all simulated atmospheres, but the haze production rates appear to be temperature dependent: the particles produced in each metallicity group decrease as the temperature increases. The images taken with an atomic force microscope (AFM) show that the particle size (15 nanometers to 190 nanometers) varies with temperature and metallicity. Our results provide useful laboratory data on the photochemical haze formation and particle properties, which can serve as critical inputs for exoplanet atmosphere modeling, and guide future observations of exoplanets with the Transiting Exoplanet Survey Satellite (TESS), the James Webb Space Telescope (JWST), and the Wide-Field Infrared Survey Telescope (WFIRST).

  19. European Commission research on aircraft impacts in the atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Amanatidis, G T; Angeletti, G [European Commission (CEC), Brussels (Belgium)

    1998-12-31

    Aircraft engines release in the troposphere and lower stratosphere a number of chemical compounds (NO{sub x}, CO{sub 2}, CO, H{sub 2}O, hydrocarbons, sulphur, soot, etc.) which could potentially affect the ozone layer and the climate through chemical, dynamical and radiative changes. The global amount of gases and particles emitted by current subsonic and projected supersonic aircraft fleets can be estimated, but significant uncertainties remain about the fate of these emissions in the atmosphere. The European efforts concerning these potential atmospheric impacts of aircraft emissions are conducted by the Environment and Climate Research Programme of the European Commission (EC) as well as by national programmes of the Member States of the European Union (EU). The European research activities in this field, are described, divided for practical reasons in two periods. The first includes activities supported under the 3. Framework Programme for R and D activities which covered the period from 1992 up to 1996, while the second period has started in early 1996 and is supported under the 4. Framework Programme. (R.P.) 6 refs.

  20. European Commission research on aircraft impacts in the atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Amanatidis, G.T.; Angeletti, G. [European Commission (CEC), Brussels (Belgium)

    1997-12-31

    Aircraft engines release in the troposphere and lower stratosphere a number of chemical compounds (NO{sub x}, CO{sub 2}, CO, H{sub 2}O, hydrocarbons, sulphur, soot, etc.) which could potentially affect the ozone layer and the climate through chemical, dynamical and radiative changes. The global amount of gases and particles emitted by current subsonic and projected supersonic aircraft fleets can be estimated, but significant uncertainties remain about the fate of these emissions in the atmosphere. The European efforts concerning these potential atmospheric impacts of aircraft emissions are conducted by the Environment and Climate Research Programme of the European Commission (EC) as well as by national programmes of the Member States of the European Union (EU). The European research activities in this field, are described, divided for practical reasons in two periods. The first includes activities supported under the 3. Framework Programme for R and D activities which covered the period from 1992 up to 1996, while the second period has started in early 1996 and is supported under the 4. Framework Programme. (R.P.) 6 refs.

  1. Are clusters important in understanding the mechanisms in atmospheric pressure ionization? Part 1: Reagent ion generation and chemical control of ion populations.

    Science.gov (United States)

    Klee, Sonja; Derpmann, Valerie; Wißdorf, Walter; Klopotowski, Sebastian; Kersten, Hendrik; Brockmann, Klaus J; Benter, Thorsten; Albrecht, Sascha; Bruins, Andries P; Dousty, Faezeh; Kauppila, Tiina J; Kostiainen, Risto; O'Brien, Rob; Robb, Damon B; Syage, Jack A

    2014-08-01

    It is well documented since the early days of the development of atmospheric pressure ionization methods, which operate in the gas phase, that cluster ions are ubiquitous. This holds true for atmospheric pressure chemical ionization, as well as for more recent techniques, such as atmospheric pressure photoionization, direct analysis in real time, and many more. In fact, it is well established that cluster ions are the primary carriers of the net charge generated. Nevertheless, cluster ion chemistry has only been sporadically included in the numerous proposed ionization mechanisms leading to charged target analytes, which are often protonated molecules. This paper series, consisting of two parts, attempts to highlight the role of cluster ion chemistry with regard to the generation of analyte ions. In addition, the impact of the changing reaction matrix and the non-thermal collisions of ions en route from the atmospheric pressure ion source to the high vacuum analyzer region are discussed. This work addresses such issues as extent of protonation versus deuteration, the extent of analyte fragmentation, as well as highly variable ionization efficiencies, among others. In Part 1, the nature of the reagent ion generation is examined, as well as the extent of thermodynamic versus kinetic control of the resulting ion population entering the analyzer region.

  2. Catalysis and sustainable (green) chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Centi, Gabriele; Perathoner, Siglinda [Dipartimento di Chimica Industriale ed Ingegneria dei Materiali, University of Messina, Salita Sperone 31, 98166 Messina (Italy)

    2003-01-15

    Catalysis is a key technology to achieve the objectives of sustainable (green) chemistry. After introducing the concepts of sustainable (green) chemistry and a brief assessment of new sustainable chemical technologies, the relationship between catalysis and sustainable (green) chemistry is discussed and illustrated via an analysis of some selected and relevant examples. Emphasis is also given to the concept of catalytic technologies for scaling-down chemical processes, in order to develop sustainable production processes which reduce the impact on the environment to an acceptable level that allows self-depuration processes of the living environment.

  3. 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...

  4. From helical to planar chirality by on-surface chemistry

    Czech Academy of Sciences Publication Activity Database

    Stetsovych, Oleksandr; Švec, Martin; Vacek, Jaroslav; Vacek Chocholoušová, Jana; Jančařík, Andrej; Rybáček, Jiří; Kośmider, K.; Stará, Irena G.; Jelínek, Pavel; Starý, Ivo

    2017-01-01

    Roč. 9, č. 3 (2017), s. 213-218 ISSN 1755-4330 R&D Projects: GA ČR(CZ) GC14-16963J; GA ČR(CZ) GA14-29667S Institutional support: RVO:68378271 ; RVO:61388963 Keywords : chirality * AFM * STM * helicene * on surface chemistry * DFT Subject RIV: CF - Physical ; Theoretical Chemistry; CC - Organic Chemistry (UOCHB-X) OBOR OECD: Physical chemistry; Organic chemistry (UOCHB-X) Impact factor: 25.870, year: 2016

  5. 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.

  6. 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

  7. Study on the atmospheric component with the scope of analyses on the environmental impact

    International Nuclear Information System (INIS)

    Ferrara, V.; La Camera, F.

    1989-03-01

    This work has been carried out following a specific request from Italian National Department for Environment and shows technical approaches and methodologies of analyses and forecasts set up for environmental impact studies referred to 'atmospheric environment'. This work is presented according to the general items and objectives fixed by the same Department in the wider operative system for the application in Italy of environmental impact procedures. (author)

  8. 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

  9. 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

  10. Ultra-High Resolution Spectroscopic Remote Sensing: A Microscope on Planetary Atmospheres

    Science.gov (United States)

    Kostiuk, Theodor

    2010-01-01

    Remote sensing of planetary atmospheres is not complete without studies of all levels of the atmosphere, including the dense cloudy- and haze filled troposphere, relatively clear and important stratosphere and the upper atmosphere, which are the first levels to experience the effects of solar radiation. High-resolution spectroscopy can provide valuable information on these regions of the atmosphere. Ultra-high spectral resolution studies can directly measure atmospheric winds, composition, temperature and non-thermal phenomena, which describe the physics and chemistry of the atmosphere. Spectroscopy in the middle to long infrared wavelengths can also probe levels where dust of haze limit measurements at shorter wavelength or can provide ambiguous results on atmospheric species abundances or winds. A spectroscopic technique in the middle infrared wavelengths analogous to a radio receiver. infrared heterodyne spectroscopy [1], will be describe and used to illustrate the detailed study of atmospheric phenomena not readily possible with other methods. The heterodyne spectral resolution with resolving power greater than 1,000.000 measures the true line shapes of emission and absorption lines in planetary atmospheres. The information on the region of line formation is contained in the line shapes. The absolute frequency of the lines can be measured to I part in 100 ,000,000 and can be used to accurately measure the Doppler frequency shift of the lines, directly measuring the line-of-sight velocity of the gas to --Im/s precision (winds). The technical and analytical methods developed and used to measure and analyze infrared heterodyne measurements will be described. Examples of studies on Titan, Venus, Mars, Earth, and Jupiter will be presented. 'These include atmospheric dynamics on slowly rotating bodies (Titan [2] and Venus [3] and temperature, composition and chemistry on Mars 141, Venus and Earth. The discovery and studies of unique atmospheric phenomena will also be

  11. 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.

  12. On the Impact of Wind Farms on a Convective Atmospheric Boundary Layer

    Science.gov (United States)

    Lu, Hao; Porté-Agel, Fernando

    2015-10-01

    With the rapid growth in the number of wind turbines installed worldwide, a demand exists for a clear understanding of how wind farms modify land-atmosphere exchanges. Here, we conduct three-dimensional large-eddy simulations to investigate the impact of wind farms on a convective atmospheric boundary layer. Surface temperature and heat flux are determined using a surface thermal energy balance approach, coupled with the solution of a three-dimensional heat equation in the soil. We study several cases of aligned and staggered wind farms with different streamwise and spanwise spacings. The farms consist of Siemens SWT-2.3-93 wind turbines. Results reveal that, in the presence of wind turbines, the stability of the atmospheric boundary layer is modified, the boundary-layer height is increased, and the magnitude of the surface heat flux is slightly reduced. Results also show an increase in land-surface temperature, a slight reduction in the vertically-integrated temperature, and a heterogeneous spatial distribution of the surface heat flux.

  13. Atmospheric sulfur and climate changes: a modelling study at mid and high-southern latitudes; Soufre atmospherique et changements climatiques: une etude de modelisation pour les moyennes et hautes latitudes Sud

    Energy Technology Data Exchange (ETDEWEB)

    Castebrunet, H

    2007-09-15

    The mid and high-southern latitudes are still marginally affected by anthropogenic sulfur emissions. They are the only regions in the world where the natural cycle of the atmospheric sulfur may still be observed. Sulfur aerosols are well-known for their radiative impact, and thus interact with climate. Climate can in turn affect atmospheric sulfur sources, distribution and chemistry. Antarctic ice cores provide information on the evolution of climate and sulfur deposition at the surface of the ice sheet at glacial-interglacial time scales. The aim of this thesis is to develop and use modeling towards a better understanding of the atmospheric sulfur cycle in antarctic and sub-antarctic regions. Ice core data are used to validate model results under glacial climate conditions. An Atmospheric General Circulation Model (AGCM) coupled to a sulfur chemistry module is used: the LMD-ZTSulfur model, version 4. An update of both the physical and chemical parts of the model. The model was first performed. The impact of there changes on modelled sulfur cycle are evaluated for modern climate. Further, boundary conditions are adapted to simulate the atmospheric circulation and sulfur cycle at the Last Glacial Maximum, approximately 20,000 years ago. In the model, sulfur is found to be highly sensitive to antarctic sea-ice coverage, which is still poorly known during the ice age. An original dataset of ice-age sea-ice coverage was developed. Its impact on the oceanic emissions of dimethyl sulfide, main precursor of sulfur aerosols at high-southern latitudes, is discussed. Using the same oceanic sulfur reservoirs as for present day climate, the model broadly reproduces the glacial deposits of sulfur aerosols on the Antarctic plateau, suggesting little impact of climate on oceanic sulfur production in the Antarctic region. Sensitivity tests were carried out to draw an up-to-date status of major uncertainties and difficulties facing future progress in understanding atmospheric

  14. 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.

  15. 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.

  16. 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.

  17. 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

  18. 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.)

  19. Evaporating brine from frost flowers with electron microscopy and implications for atmospheric chemistry and sea-salt aerosol formation

    Czech Academy of Sciences Publication Activity Database

    Yang, X.; Neděla, Vilém; Runštuk, Jiří; Ondrušková, G.; Krausko, J.; Vetráková, L'.; Heger, D.

    2017-01-01

    Roč. 17, č. 10 (2017), s. 6291-6303 ISSN 1680-7316 R&D Projects: GA ČR(CZ) GA14-22777S Institutional support: RVO:68081731 Keywords : experimental-computational approach * aqueous-solutions * boundary-layer * blowing snow * spectroscopic properties * low-temperatures Subject RIV: JA - Electronics ; Optoelectronics, Electrical Engineering OBOR OECD: Meteorology and atmospheric sciences Impact factor: 5.318, year: 2016

  20. Changing Groundwater-Surface Water Interactions Impact Stream Chemistry and Ecology at the Arctic-Boreal Transition in Western Alaska

    Science.gov (United States)

    Koch, J. C.; Carey, M.; O'Donnell, J.; Sjoberg, Y.; Zimmerman, C. E.

    2016-12-01

    The arctic-boreal transition zone of Alaska is experiencing rapid change related to unprecedented warming and subsequent loss of permafrost. These changes in turn may affect groundwater-surface water (GW-SW) interactions, biogeochemical cycling, and ecosystem processes. While recent field and modeling studies have improved our understanding of hydrology in watersheds underlain by thawing permafrost, little is known about how these hydrologic shifts will impact bottom-up controls on stream food webs. To address this uncertainty, we are using an integrative experimental design to link GW-SW interactions to stream biogeochemistry and biota in 10 first-order streams in northwest Alaska. These study streams drain watersheds that span several gradients, including elevation, aspect, and vegetation (tundra vs. forest). We have developed a robust, multi-disciplinary data set to characterize GW-SW interactions and to mechanistically link GW-SW dynamics to water quality and the stream ecosystem. Data includes soil hydrology and chemistry; stream discharge, temperature, and inflow rates; water chemistry (including water isotopes, major ions, carbon concentration and isotopes, nutrients and chlorophyll-a), and invertebrate and fish communities. Stream recession curves indicate a decreasing rate later in the summer in some streams, consistent with seasonal thaw in lower elevation and south-facing catchments. Base cation and water isotope chemistry display similar impacts of seasonal thaw and also suggest the dominance of groundwater in many streams. Coupled with estimates of GW-SW exchange at point, reach, and catchment scales, these results will be used to predict how hydrology and water quality are likely to impact fish habitat and growth given continued warming at the arctic-boreal transition.