source atmospheric chemistry: Topics by WorldWideScience.org

Sample records for source atmospheric chemistry

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.
Atmospheric Chemistry Over Southern Africa

Science.gov (United States)

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

2011-01-01

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

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.
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.
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
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.
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.
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
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
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...
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.
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
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.
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
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.
Reference Sources in Chemistry

OpenAIRE

Sthapit, Dilip Man

1995-01-01

Information plays an important role in the development of every field. Therefore a brief knowledge regarding information sources is necessary to function in any field. There are many information sources about scientific and technical subjects. In this context there are many reference sources in Chemistry too. Chemistry is one important part of the science which deals with the study of the composition of substances and the chemical changes that they undergo. The purpose of this report is...
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.
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.
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.
Identification of atmospheric mercury sources and transport pathways on local and regional sales

Science.gov (United States)

Gratz, Lynne E.

Mercury (Hg) is a hazardous air pollutant and bioaccumulative neurotoxin whose intricate atmospheric chemistry complicates our ability to define Hg source-receptor relationships on all scales. Our detailed measurements of Hg in its different forms together with atmospheric tracers have improved our understanding of Hg chemistry and transport. Daily-event precipitation samples collected from 1995 to 2006 in Underhill, VT were examined to identify Hg wet deposition trends and source influences. Analysis revealed that annual Hg deposition at this fairly remote location did not vary significantly over the 12-year period. While a decreasing trend in volume-weighted mean Hg concentration was observed, Hg wet deposition did not decline as transport of emissions from the Midwest and along the Atlantic Coast consistently contributed to the largest observed Hg wet deposition events. Receptor modeling of Hg and trace elements in precipitation indicated that ---60% of Hg wet deposition at Underhill could be attributed to emissions from coal-fired utility boilers (CFUBs), and their contribution to Hg wet deposition did not change significantly over time. Hybrid-receptor modeling further defined these CFUBs to be located predominantly in the Midwestern U.S. Atmospheric Hg chemistry and transport from the Chicago urban/industrial area was the focus of speciated Hg measurements performed in the southern Lake Michigan basin during summer 2007. Transport from Chicago, IL to Holland, MI occurred during 27% of the study period, resulting in a five-fold increase in divalent reactive gaseous Hg (RGM) at the downwind Holland site. Dispersion modeling of case study periods demonstrated that under southwesterly flow approximately half of the RGM in Holland could be attributed to primary RGM emissions from Chicago after transport and dispersion, with the remainder due to Hg0 oxidation in the atmosphere en route. Precipitation and ambient vapor phase samples were also collected in Chicago
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)
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.

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

Energy Technology Data Exchange (ETDEWEB)

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

2013-05-20

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

assimilation of real tropospheric ozone concentrations mitigates these results and shows how hard atmospheric chemistry data assimilation is. A strong model error is indeed attached to these models, stemming from multiple uncertainty sources. Two steps must be taken to tackle this issue. First of all, the data assimilation method used must be able to efficiently take into account the model error. However, most methods are developed under the assumption of a perfect model. To avoid this hypothesis, a new method has then been developed. Called IEnKF-Q, it expands the IEnKS to the model error framework. It has been validated on a low-order model, proving its superiority over data assimilation methods naively adapted to take into account model error. Nevertheless, such methods need to know the exact nature and amplitude of the model error which needs to be accounted for. Therefore, the second step is to use statistical tools to quantify this model error. The expectation-maximization algorithm, the naive and unbiased randomize-then-optimize algorithms, an importance sampling based on a Laplace proposal, and a Markov chain Monte Carlo simulation, potentially trans-dimensional, have been assessed, expanded, and compared to estimate the uncertainty on the retrieval of the source term of the Chernobyl and Fukushima-Daiichi nuclear power plant accidents. This thesis therefore improves the domain of 4D EnVar data assimilation by its methodological input and by paving the way to applying these methods on atmospheric chemistry models. (author) [fr
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.;

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

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
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
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
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.
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
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
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...
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.
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.
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
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...

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
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.
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.
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.
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
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.
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.
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
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
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
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 O_x, HO_x, NO_x, 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.
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...
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.
Use of the HadGEM2 climate-chemistry model to investigate interannual variability in methane sources

Science.gov (United States)

Hayman, Garry; O'Connor, Fiona; Clark, Douglas; Huntingford, Chris; Gedney, Nicola

2013-04-01

The global mean atmospheric concentration of methane (CH4) has more than doubled during the industrial era [1] and now constitutes ? 20% of the anthropogenic climate forcing by greenhouse gases [2]. The globally-averaged CH4 growth rate, derived from surface measurements, has fallen significantly from a high of 16 ppb yr-1 in the late 1970s/early 1980s and was close to zero between 1999 and 2006 [1]. This overall period of declining or low growth was however interspersed with years of positive growth-rate anomalies (e.g., in 1991-1992, 1998-1999 and 2002-2003). Since 2007, renewed growth has been evident [1, 3], with the largest increases observed over polar northern latitudes and the Southern Hemisphere in 2007 and in the tropics in 2008. The observed inter-annual variability in atmospheric methane concentrations and the associated changes in growth rates have variously been attributed to changes in different methane sources and sinks [1, 4]. In this paper, we report results from runs of the HadGEM2 climate-chemistry model [5] using year- and month-specific emission datasets. The HadGEM2 model includes the comprehensive atmospheric chemistry and aerosol package, the UK Chemistry Aerosol community model (UKCA, http://www.ukca.ac.uk/wiki/index.php). The Standard Tropospheric Chemistry scheme was selected for this work. This chemistry scheme simulates the Ox, HOx and NOx chemical cycles and the oxidation of CO, methane, ethane and propane. Year- and month-specific emission datasets were generated for the period from 1997 to 2009 for the emitted species in the chemistry scheme (CH4, CO, NOx, HCHO, C2H6, C3H8, CH3CHO, CH3CHOCH3). The approach adopted varied depending on the source sector: Anthropogenic: The emissions from anthropogenic sources were based on decadal-averaged emission inventories compiled by [6] for the Coupled Carbon Cycle Climate Model Intercomparison Project (C4MIP). These were then used to derive year-specific emission datasets by scaling the
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 (NO_y species can comprise up to 28% of the N deposition budget under cooler conditions. Upward NO₂ fluxes cause the net above-canopy NO_y 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
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.
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)
Chemical composition and sources of atmospheric aerosols at Djougou (Benin)

Science.gov (United States)

Ouafo-Leumbe, Marie-Roumy; Galy-Lacaux, Corinne; Liousse, Catherine; Pont, Veronique; Akpo, Aristide; Doumbia, Thierno; Gardrat, Eric; Zouiten, Cyril; Sigha-Nkamdjou, Luc; Ekodeck, Georges Emmanuel

2017-06-01

In the framework of the INDAAF (International Network to study Deposition and Atmospheric chemistry in AFrica) program, atmospheric aerosols were collected in PM2.5 and PM10 size fractions at Djougou, Benin, in the West Africa, from November, 2005 to October, 2009. Particulate carbon, ionic species, and trace metals were analyzed. Weekly PM2.5 and PM10 total mass concentrations varied between 0.7 and 47.3 µg m-3 and 1.4-148.3 µg m-3, respectively. We grouped the aerosol chemical compounds into four classes: dust, particulate organic matter (POM), elemental carbon (EC), and ions. We studied the annual variation of each class to determine their contribution in the total aerosol mass concentration and finally to investigate their potential emission sources. On an annual basis, the species presented a well-marked seasonality, with the peak of mass concentration for both sizes registered in dry season, 67 ± 2 to 86 ± 9 versus 14 ± 9 to 34 ± 5% in wet season. These values emphasized the seasonality of the emissions and the relative weak interannual standard deviation indicates the low variability of the seasonality. At the seasonal scale, major contributions to the aerosol chemistry in the dry season are: dust (26-59%), POM (30-59%), EC (5-9%), and ions (3-5%), suggesting a predominance of Sahelian and Saharan dust emissions and biomass burning source in this season. In the wet season, POM is predominant, followed by dust, EC, and ions. These results point out the contribution of surrounded biofuel combustion used for cooking and biogenic emissions during the wet season.
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
[Regional atmospheric environment risk source identification and assessment].

Science.gov (United States)

Zhang, Xiao-Chun; Chen, Wei-Ping; Ma, Chun; Zhan, Shui-Fen; Jiao, Wen-Tao

2012-12-01

Identification and assessment for atmospheric environment risk source plays an important role in regional atmospheric risk assessment and regional atmospheric pollution prevention and control. The likelihood exposure and consequence assessment method (LEC method) and the Delphi method were employed to build a fast and effective method for identification and assessment of regional atmospheric environment risk sources. This method was applied to the case study of a large coal transportation port in North China. The assessment results showed that the risk characteristics and the harm degree of regional atmospheric environment risk source were in line with the actual situation. Fast and effective identification and assessment of risk source has laid an important foundation for the regional atmospheric environmental risk assessment and regional atmospheric pollution prevention and control.

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.
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.
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
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.
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)
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...
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.
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.
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 NO_x 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.
Atmospheric mercury in northern Wisconsin: sources and species

International Nuclear Information System (INIS)

Lamborg, C.H.; Fitzgerald, W.F.; Vandal, G.M.; Rolfhus, K.R.

1995-01-01

The atmospheric chemistry, deposition and transport of mercury (Hg) in the Upper Great Lakes region is being investigated at a near-remote sampling location in northern Wisconsin. Intensive sampling over two years has been completed. A multi-phase collection strategy was used to gain insight into the processes controlling concentrations and chemical/physical speciation of atmospheric Hg. Additional chemical and physical atmospheric determinations were also made during these periods to aid in the interpretation of the Hg determinations. For example, correlations of Hg with ozone, sulfur dioxide and synopticscale meteorological features suggest a regionally discernible signal in Hg. Comparison to isosigma backward air parcel trajectories confirms this regionality and implicates the areas south, southeast and northwest of the size to be source for Hg. Particle-phase Hg (Hg p ) was found to be approximately 40% in an oxidized form, or operationally defined as reactive but was variable. Hg p and other particle constituents show significant correlation and similarity in behavior. These observations support the hypothesis that precipitation-phase Hg arises from the scavenging of atmospheric particulates bearing Hg. Observed concentrations of rain and particle-Hg fit the theoretical expectations for nucleation and below-cloud scavenging. Increases in the Hg/aerosol mass ratio appear to take place during transport. Enrichment of aerosols is taken as evidence of gas/particle conversion which could represent the step linking gas-phase Hg with rain. The refined budget indicates ca. 24% of total deposition is from summer particle dry deposition, and that this deposition also contributes ca. 24% of all reactive Hg deposition. Most deposition occurs during the summer months. 40 refs., 4 figs., 7 tabs
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.
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.
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.
VULCAN: An Open-source, Validated Chemical Kinetics Python Code for Exoplanetary Atmospheres

Energy Technology Data Exchange (ETDEWEB)

Tsai, Shang-Min; Grosheintz, Luc; Kitzmann, Daniel; Heng, Kevin [University of Bern, Center for Space and Habitability, Sidlerstrasse 5, CH-3012, Bern (Switzerland); Lyons, James R. [Arizona State University, School of Earth and Space Exploration, Bateman Physical Sciences, Tempe, AZ 85287-1404 (United States); Rimmer, Paul B., E-mail: shang-min.tsai@space.unibe.ch, E-mail: kevin.heng@csh.unibe.ch, E-mail: jimlyons@asu.edu [University of St. Andrews, School of Physics and Astronomy, St. Andrews, KY16 9SS (United Kingdom)

2017-02-01

We present an open-source and validated chemical kinetics code for studying hot exoplanetary atmospheres, which we name VULCAN. It is constructed for gaseous chemistry from 500 to 2500 K, using a reduced C–H–O chemical network with about 300 reactions. It uses eddy diffusion to mimic atmospheric dynamics and excludes photochemistry. We have provided a full description of the rate coefficients and thermodynamic data used. We validate VULCAN by reproducing chemical equilibrium and by comparing its output versus the disequilibrium-chemistry calculations of Moses et al. and Rimmer and Helling. It reproduces the models of HD 189733b and HD 209458b by Moses et al., which employ a network with nearly 1600 reactions. We also use VULCAN to examine the theoretical trends produced when the temperature–pressure profile and carbon-to-oxygen ratio are varied. Assisted by a sensitivity test designed to identify the key reactions responsible for producing a specific molecule, we revisit the quenching approximation and find that it is accurate for methane but breaks down for acetylene, because the disequilibrium abundance of acetylene is not directly determined by transport-induced quenching, but is rather indirectly controlled by the disequilibrium abundance of methane. Therefore we suggest that the quenching approximation should be used with caution and must always be checked against a chemical kinetics calculation. A one-dimensional model atmosphere with 100 layers, computed using VULCAN, typically takes several minutes to complete. VULCAN is part of the Exoclimes Simulation Platform (ESP; exoclime.net) and publicly available at https://github.com/exoclime/VULCAN.
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
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
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...
"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…
Discovery and measurement of an isotopically distinct source of sulfate in Earth's atmosphere.

Science.gov (United States)

Dominguez, Gerardo; Jackson, Terri; Brothers, Lauren; Barnett, Burton; Nguyen, Bryan; Thiemens, Mark H

2008-09-02

Sulfate (SO(4)) and its precursors are significant components of the atmosphere, with both natural and anthropogenic sources. Recently, our triple-isotope ((16)O, (17)O, (18)O) measurements of atmospheric sulfate have provided specific insights into the oxidation pathways leading to sulfate, with important implications for models of the sulfur cycle and global climate change. Using similar isotopic measurements of aerosol sulfate in a polluted marine boundary layer (MBL) and primary sulfate (p-SO(4)) sampled directly from a ship stack, we quantify the amount of p-SO(4) found in the atmosphere from ships. We find that ships contribute between 10% and 44% of the non-sea-salt sulfate found in fine [diameter (D) sea salt particles may lead to the rapid removal of SO(2) in the MBL. When combined with the longer residence time of p-SO(4) emissions in the MBL, these findings suggest that the importance of p-SO(4) emissions in marine environments may be underappreciated in global chemical models. Given the expected increase of international shipping in the years to come, these findings have clear implications for public health, air quality, international maritime law, and atmospheric chemistry.
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

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
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.
Acetone in the atmosphere: Distribution, sources, and sinks

Science.gov (United States)

Singh, H. B.; O'Hara, D.; Herlth, D.; Sachse, W.; Blake, D. R.; Bradshaw, J. D.; Kanakidou, M.; Crutzen, P. J.

1994-01-01

Acetone (CH3COCH3) was found to be the dominant nonmethane organic species present in the atmosphere sampled primarily over eastern Canada (0-6 km, 35 deg-65 deg N) during ABLE3B (July to August 1990). A concentration range of 357 to 2310 ppt (= 10(exp -12) v/v) with a mean value of 1140 +/- 413 ppt was measured. Under extremely clean conditions, generally involving Arctic flows, lowest (background) mixing ratios of 550 +/- 100 ppt were present in much of the troposphere studied. Correlations between atmospheric mixing ratios of acetone and select species such as C2H2, CO, C3H8, C2Cl4 and isoprene provided important clues to its possible sources and to the causes of its atmospheric variability. Biomass burning as a source of acetone has been identified for the first time. By using atmospheric data and three-dimensional photochemical models, a global acetone source of 40-60 Tg (= 10(exp 12) g)/yr is estimated to be present. Secondary formation from the atmospheric oxidation of precursor hydrocarbons (principally propane, isobutane, and isobutene) provides the single largest source (51%). The remainder is attributable to biomass burning (26%), direct biogenic emissions (21%), and primary anthropogenic emissions (3%). Atmospheric removal of acetone is estimated to be due to photolysis (64%), reaction with OH radicals (24%), and deposition (12%). Model calculations also suggest that acetone photolysis contributed significantly to PAN formation (100-200 ppt) in the middle and upper troposphere of the sampled region and may be important globally. While the source-sink equation appears to be roughly balanced, much more atmospheric and source data, especially from the southern hemisphere, are needed to reliably quantify the atmospheric budget of acetone.
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.
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
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...
The difference between the metal ion extracted from the R.F. ion source by applying plasma chemistry reaction and by non-plasma range chemistry reaction

International Nuclear Information System (INIS)

Bai Gui Bin

1987-01-01

The paper introduced the difference between using plasma chemistry reaction draw metal ion and non-plasma range chemistry reaction in the R.F. ion source. By using of the plasma chemistry reaction draw metal ion higher percentage than non-plasma range chemistry reaction in the R.F. ion source. The authors plasma chemistry reaction to R.F. ion source and implanter successfully. The effect is very well, it has its own characteristic
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.
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
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
The sources of atmospheric gravity waves

International Nuclear Information System (INIS)

Nagpal, O.P.

1979-01-01

The gravity wave theory has been very successful in the interpretation of various upper atmospheric phenomena. This article offers a review of the present state of knowledge about the various sources of atmospheric gravity waves, particularly those which give rise to different types of travelling ionospheric disturbance. Some specific case studies are discussed. (author)
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
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
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
Geographical Distribution and Sources of Nutrients in Atmospheric Aerosol Over the Pacific Ocean

Science.gov (United States)

Uematsu, M.

2016-12-01

The Pacific Ocean, the world's largest (occupying about 30% of the Earth's total surface area) has several distinguishing biogeochemical features. In the western Pacific, dust particles originating from arid and semi-arid regions in Asia and Australia are transported to the north and south, respectively. Biomass burning emissions from Southeast Asia are exported to the tropical Pacific, and anthropogenic substances flowing out of Asia and Eurasia spread both regionally and globally. Over high primary productive areas such as the subarctic North Pacific, the equatorial Pacific and the Southern Ocean, biogenic gasses are released to the atmosphere and transported to other areas. These processes may affect cloud and rainfall patterns, air quality, and the radiative balance of downwind regions. The deposition of atmospheric aerosols containing iron and other essential nutrients is important for biogeochemical cycles in the oceans because this source of nutrients helps sustain primary production and affects food-web structure; these effects in turn influence the chemical properties of marine atmosphere. From an atmospheric chemistry standpoint, sea-salt aerosols produced by strong winds and marine biogenic gases emitted from highly productive waters affect the physicochemical characteristics of marine aerosols. As phytoplankton populations are patchy and atmospheric processes sporadic, the interactions between atmospheric chemical constituents and marine biota vary for different regions as well as seasonally and over longer timescales. To address these and other emerging issues, and more generally to better understand the important biogeochemical processes and interactions occurring over the open oceans, more long-term recurrent research cruises with standardized atmospheric shipboard measurements will be needed in the future.
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
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.
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.
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.
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.

Sources of atmospheric acidity

International Nuclear Information System (INIS)

Clarke, A.G.

1992-01-01

The emissions of acid gases from anthropogenic sources and their impact on the environment are the main concern of this book. However, that impact can only be assessed if all the naturally occurring sources of these gases are also known and can be quantified. Given the widely dispersed nature of the natural sources and the problems of measurement of trace species at low concentrations, often in remote regions, the quantification is a very difficult task. Nevertheless, considerable progress has been made over the last decade. In this chapter both man-made and natural sources of atmospheric acidity will be reviewed, but the emphasis will be placed not so much on the global balances as on the scale of the natural sources in relation to the man-made sources. This requires that the very uneven geographical distribution of emissions and the lifetime of individual chemical species be taken into account. The emissions considered are sulphur compounds, nitrogen compounds, chlorine compounds and organic acids. The anthropogenic sources discussed are the combustion of fossil fuels and certain industrial processes. Emissions data for anthropogenic sources are given for the United Kingdom, Europe, USA and globally. A list of 95 references is given. (Author)
Organofluorine chemistry : applications, sources and sustainability.

OpenAIRE

Harsanyi, A.; Sandford, G.

2015-01-01

Fluorine is an essential element for life in the developed world that impacts hugely on the general public because many pharmaceuticals, agrochemicals, anaesthetics, materials and air conditioning materials owe their important properties to the presence of fluorine atoms within their structures. All fluorine atoms used in organic chemistry are ultimately sourced from a mined raw material, fluorspar (CaF2), but, given current usage and global reserve estimates, there is only sufficient fluorsp...
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
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.
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.
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.
Open Data, Open Source and Open Standards in chemistry: The Blue Obelisk five years on

Science.gov (United States)

2011-01-01

Background The Blue Obelisk movement was established in 2005 as a response to the lack of Open Data, Open Standards and Open Source (ODOSOS) in chemistry. It aims to make it easier to carry out chemistry research by promoting interoperability between chemistry software, encouraging cooperation between Open Source developers, and developing community resources and Open Standards. Results This contribution looks back on the work carried out by the Blue Obelisk in the past 5 years and surveys progress and remaining challenges in the areas of Open Data, Open Standards, and Open Source in chemistry. Conclusions We show that the Blue Obelisk has been very successful in bringing together researchers and developers with common interests in ODOSOS, leading to development of many useful resources freely available to the chemistry community. PMID:21999342
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.
New constraints on terrestrial and oceanic sources of atmospheric methanol

Directory of Open Access Journals (Sweden)

D. B. Millet

2008-12-01

Full Text Available We use a global 3-D chemical transport model (GEOS-Chem to interpret new aircraft, surface, and oceanic observations of methanol in terms of the constraints that they place on the atmospheric methanol budget. Recent measurements of methanol concentrations in the ocean mixed layer (OML imply that in situ biological production must be the main methanol source in the OML, dominating over uptake from the atmosphere. It follows that oceanic emission and uptake must be viewed as independent terms in the atmospheric methanol budget. We deduce that the marine biosphere is a large primary source (85 Tg a⁻¹ of methanol to the atmosphere and is also a large sink (101 Tg a⁻¹, comparable in magnitude to atmospheric oxidation by OH (88 Tg a⁻¹. The resulting atmospheric lifetime of methanol in the model is 4.7 days. Aircraft measurements in the North American boundary layer imply that terrestrial plants are a much weaker source than presently thought, likely reflecting an overestimate of broadleaf tree emissions, and this is also generally consistent with surface measurements. We deduce a terrestrial plant source of 80 Tg a⁻¹, comparable in magnitude to the ocean source. The aircraft measurements show a strong correlation with CO (R²=0.51−0.61 over North America during summer. We reproduce this correlation and slope in the model with the reduced plant source, which also confirms that the anthropogenic source of methanol must be small. Our reduced plant source also provides a better simulation of methanol observations over tropical South America.
Magic gamma rays, extra-atmospheric source

International Nuclear Information System (INIS)

Bolufer, P.

2010-01-01

Without the atmospheric layer, the cosmos radiation would kill every living, our planet would be like the moon. The cosmic gamma ray to collide with gases in land cover, as it is disintegrated. They are harmless, they form a cone of light that points to the cosmic source comes from. On April 25, 2009 was born on the island of Palma Magic II and Magic I the best observer of atmospheric gamma rays of low intensity. (Author)
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 O_x and O₃ compared to other reactions involving, e.g., atomic oxygen. Thus the impact of vibrationally excited OH on the ozone or O_x 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
Tropospheric Halogen Chemistry

Science.gov (United States)

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

2003-12-01

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

OpenAIRE

Zaheri Sarabi, Shadi

2017-01-01

The current thesis deals with the development of a computational framework for performing plasma chemistry simulations and their uncertainty quantification analysis by suitably combining and extending existing open source computational tools. A plasma chemistry solver is implemented in the OpenFOAM C++ solver suite. The OpenFOAM plasma chemistry application solves the species conservation equations and the electron energy equation by accounting suitably for various production and loss terms b...
Atmospheric deposition of mercury in central Poland: Sources and seasonal trends

Science.gov (United States)

Siudek, Patrycja; Kurzyca, Iwona; Siepak, Jerzy

2016-03-01

Atmospheric deposition of total mercury was studied at two sites in central Poland, between April 2013 and October 2014. Hg in rainwater (bulk deposition) was analyzed in relation to meteorological parameters and major ions (H+, NO3-, Cl-, SO42 -) in order to investigate seasonal variation, identify sources and determine factors affecting atmospheric Hg chemistry and deposition. Total mercury concentrations varied between 1.24 and 22.1 ng L- 1 at the urban sampling site (Poznań) and between 0.57 and 18.3 ng L- 1 in the woodland protected area (Jeziory), with quite similar mean values of 6.96 and 6.37 ng L- 1, respectively. Mercury in precipitation exhibited lower spatial variability within the study domain (urban/forest transect) than the concentrations determined during other similar observations, reflecting the predominant influence of the same local sources. In our study, a significant seasonal pattern of Hg deposition was observed at both sampling sites, with higher and more variable concentrations of Hg reported for the urban area. In particular, deposition values of Hg were higher in the samples attributed to relatively large precipitation amounts in the summer and in those collected during the winter season (the result of higher contributions from combustion sources, i.e. intensive combustion of fossil fuels in residential and commercial boilers, individual power/heat-generating plants). In addition, a significant relationship between Hg concentration and precipitation amount was found while considering different types of wintertime samples (i.e. rain, snow and mixed precipitation). The analysis of backward trajectories showed that air masses arriving from polluted regions of western Europe and southern Poland largely affected the amount of Hg in rainwater. A seasonal variation in Hg deposition fluxes was also observed, with the maximum value of Hg in spring and minimum in winter. Our results indicated that rainwater Hg and, consequently, the wet deposition
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.;

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.

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)
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.
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
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.
Characteristics and sources of nitrous acid in an urban atmosphere of northern China: Results from 1-yr continuous observations

Science.gov (United States)

Li, Dandan; Xue, Likun; Wen, Liang; Wang, Xinfeng; Chen, Tianshu; Mellouki, Abdelwahid; Chen, Jianmin; Wang, Wenxing

2018-06-01

Nitrous acid (HONO) is a key reservoir of the hydroxyl radical (OH) and plays a central role in the atmospheric chemistry. To understand the sources and impact of HONO in the polluted atmosphere of northern China, continuous measurements of HONO and related parameters were conducted from September 2015 to August 2016 at an urban site in Ji'nan, the capital city of Shandong province. HONO showed well-defined seasonal and diurnal variation patterns with clear wintertime and nighttime concentration peaks. Elevated HONO concentrations (e.g., over 5 ppbv) were frequently observed with a maximum value of 8.36 ppbv. The HONO/NOX ratios of direct vehicle emissions varied in the range of 0.29%-0.87%, with a mean value of 0.53%. An average NO2-to-HONO nighttime conversion frequency (khet) was derived to be 0.0068 ± 0.0045 h-1 from 107 HONO formation cases. A detailed HONO budget analysis suggests an unexplained daytime missing source of 2.95 ppb h-1 in summer, which is about seven times larger than the homogeneous reaction of NO with OH. The effect of HONO on OH production was also quantified. HONO photolysis was the uppermost source of local OH radical throughout the daytime. This study provides the year-round continuous record of ambient HONO in the North China Plain, and offers some insights into the characteristics, sources and impacts of HONO in the polluted atmospheres of China.

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

Science.gov (United States)

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

2017-12-01

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

OpenAIRE

Cheng, I.; Xu, X.; Zhang, L.

2015-01-01

Receptor-based source apportionment studies of speciated atmospheric mercury are not only concerned with source contributions but also with the influence of transport, transformation, and deposition processes on speciated atmospheric mercury concentrations at receptor locations. Previous studies applied multivariate receptor models including principal components analysis and positive matrix factorization, and back trajectory receptor models including potential source contri...
GEOSPATIAL ANALYSIS OF ATMOSPHERIC HAZE EFFECT BY SOURCE AND SINK LANDSCAPE

Directory of Open Access Journals (Sweden)

T. Yu

2017-09-01

Full Text Available Based on geospatial analysis model, this paper analyzes the relationship between the landscape patterns of source and sink in urban areas and atmospheric haze pollution. Firstly, the classification result and aerosol optical thickness (AOD of Wuhan are divided into a number of square grids with the side length of 6 km, and the category level landscape indices (PLAND, PD, COHESION, LPI, FRAC_MN and AOD of each grid are calculated. Then the source and sink landscapes of atmospheric haze pollution are selected based on the analysis of the correlation between landscape indices and AOD. Next, to make the following analysis more efficient, the indices selected before should be determined through the correlation coefficient between them. Finally, due to the spatial dependency and spatial heterogeneity of the data used in this paper, spatial autoregressive model and geo-weighted regression model are used to analyze atmospheric haze effect by source and sink landscape from the global and local level. The results show that the source landscape of atmospheric haze pollution is the building, and the sink landscapes are shrub and woodland. PLAND, PD and COHESION are suitable for describing the atmospheric haze effect by source and sink landscape. Comparing these models, the fitting effect of SLM, SEM and GWR is significantly better than that of OLS model. The SLM model is superior to the SEM model in this paper. Although the fitting effect of GWR model is more unsuited than that of SLM, the influence degree of influencing factors on atmospheric haze of different geography can be expressed clearer. Through the analysis results of these models, following conclusions can be summarized: Reducing the proportion of source landscape area and increasing the degree of fragmentation could cut down aerosol optical thickness; And distributing the source and sink landscape evenly and interspersedly could effectively reduce aerosol optical thickness which represents
Geospatial Analysis of Atmospheric Haze Effect by Source and Sink Landscape

Science.gov (United States)

Yu, T.; Xu, K.; Yuan, Z.

2017-09-01

Based on geospatial analysis model, this paper analyzes the relationship between the landscape patterns of source and sink in urban areas and atmospheric haze pollution. Firstly, the classification result and aerosol optical thickness (AOD) of Wuhan are divided into a number of square grids with the side length of 6 km, and the category level landscape indices (PLAND, PD, COHESION, LPI, FRAC_MN) and AOD of each grid are calculated. Then the source and sink landscapes of atmospheric haze pollution are selected based on the analysis of the correlation between landscape indices and AOD. Next, to make the following analysis more efficient, the indices selected before should be determined through the correlation coefficient between them. Finally, due to the spatial dependency and spatial heterogeneity of the data used in this paper, spatial autoregressive model and geo-weighted regression model are used to analyze atmospheric haze effect by source and sink landscape from the global and local level. The results show that the source landscape of atmospheric haze pollution is the building, and the sink landscapes are shrub and woodland. PLAND, PD and COHESION are suitable for describing the atmospheric haze effect by source and sink landscape. Comparing these models, the fitting effect of SLM, SEM and GWR is significantly better than that of OLS model. The SLM model is superior to the SEM model in this paper. Although the fitting effect of GWR model is more unsuited than that of SLM, the influence degree of influencing factors on atmospheric haze of different geography can be expressed clearer. Through the analysis results of these models, following conclusions can be summarized: Reducing the proportion of source landscape area and increasing the degree of fragmentation could cut down aerosol optical thickness; And distributing the source and sink landscape evenly and interspersedly could effectively reduce aerosol optical thickness which represents atmospheric haze
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.
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
Atmospheric deposition as a source of carbon and nutrients to an alpine catchment of the Colorado Rocky Mountains

Science.gov (United States)

Mladenov, N.; Williams, M. W.; Schmidt, S. K.; Cawley, K.

2012-08-01

Many alpine areas are experiencing deglaciation, biogeochemical changes driven by temperature rise, and changes in atmospheric deposition. There is mounting evidence that the water quality of alpine streams may be related to these changes, including rising atmospheric deposition of carbon (C) and nutrients. Given that barren alpine soils can be severely C limited, atmospheric deposition sources may be an important source of C and nutrients for these environments. We evaluated the magnitude of atmospheric deposition of C and nutrients to an alpine site, the Green Lake 4 catchment in the Colorado Rocky Mountains. Using a long-term dataset (2002-2010) of weekly atmospheric wet deposition and snowpack chemistry, we found that volume weighted mean dissolved organic carbon (DOC) concentrations were 1.12 ± 0.19 mg l-1, and weekly concentrations reached peaks as high at 6-10 mg l-1 every summer. Total dissolved nitrogen concentration also peaked in the summer, whereas total dissolved phosphorus and calcium concentrations were highest in the spring. To investigate potential sources of C in atmospheric deposition, we evaluated the chemical quality of dissolved organic matter (DOM) and relationships between DOM and other solutes in wet deposition. Relationships between DOC concentration, fluorescence, and nitrate and sulfate concentrations suggest that pollutants from nearby urban and agricultural sources and organic aerosols derived from sub-alpine vegetation may influence high summer DOC wet deposition concentrations. Interestingly, high DOC concentrations were also recorded during "dust-in-snow" events in the spring, which may reflect an association of DOM with dust. Detailed chemical and spectroscopic analyses conducted for samples collected in 2010 revealed that the DOM in many late spring and summer samples was less aromatic and polydisperse and of lower molecular weight than that of winter and fall samples. Our C budget estimates for the Green Lake 4 catchment
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
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.
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
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
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.
A simplistic view of the iodine chemistry influence on source term assessment

International Nuclear Information System (INIS)

Herranz, L.E.; Rodriguez, J.J.

1994-01-01

The intrinsic characteristics of iodine make it a relevant concern as to its potential radiobiological impact in case of a hypothetical severe accident in nuclear power plants. This paper summarizes the major results drawn from a very simple but illustrative calculation exercise aimed at weighing how significant could be taking iodine chemistry in containment into account for source term assessments in case of a postulated severe reactor accident. The scenario chosen as representative of expected conditions in containment was LA-4 test of LACE programme. Several approximations and hypothesis concerning the scenario were necessary. Iodine chemistry analyses were performed with IODE code, as long as thermalhydraulic and aerosol behaviour analyses, providing initial and boundary conditions for iodine calculations, were carried out with CONTEMPT4/MOD5 and NAUA/MOD5 codes, respectively. In general, the results obtained agreed qualitatively with the current knowledge on the area; from a quantitative point of view, one of the major results was that iodine chemistry on acidic conditions could provide a substantial increase in the leaked mass from containment under the postulated circumstances. Hence, this study underlines the need of including iodine chemistry in source tenn assessments. (author)
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.
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.
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....

Influence of climate on alpine stream chemistry and water sources

Science.gov (United States)

Foks, Sydney; Stets, Edward; Singha, Kamini; Clow, David W.

2018-01-01

The resilience of alpine/subalpine watersheds may be viewed as the resistance of streamflow or stream chemistry to change under varying climatic conditions, which is governed by the relative size (volume) and transit time of surface and subsurface water sources. Here, we use end‐member mixing analysis in Andrews Creek, an alpine stream in Rocky Mountain National Park, Colorado, from water year 1994 to 2015, to explore how the partitioning of water sources and associated hydrologic resilience change in response to climate. Our results indicate that four water sources are significant contributors to Andrews Creek, including snow, rain, soil water, and talus groundwater. Seasonal patterns in source‐water contributions reflected the seasonal hydrologic cycle, which is driven by the accumulation and melting of seasonal snowpack. Flushing of soil water had a large effect on stream chemistry during spring snowmelt, despite making only a small contribution to streamflow volume. Snow had a large influence on stream chemistry as well, contributing large amounts of water with low concentrations of weathering products. Interannual patterns in end‐member contributions reflected responses to drought and wet periods. Moderate and significant correlations exist between annual end‐member contributions and regional‐scale climate indices (the Palmer Drought Severity Index, the Palmer Hydrologic Drought Index, and the Modified Palmer Drought Severity Index). From water year 1994 to 2015, the percent contribution from the talus‐groundwater end member to Andrews Creek increased an average of 0.5% per year (p < 0.0001), whereas the percent contributions from snow plus rain decreased by a similar amount (p = 0.001). Our results show how water and solute sources in alpine environments shift in response to climate variability and highlight the role of talus groundwater and soil water in providing hydrologic resilience to the system.
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
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.)
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.
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.
Global Particulate Matter Source Apportionment

Science.gov (United States)

Lamancusa, C.; Wagstrom, K.

2017-12-01

As our global society develops and grows it is necessary to better understand the impacts and nuances of atmospheric chemistry, in particular those associated with atmospheric particulate matter. We have developed a source apportionment scheme for the GEOS-Chem global atmospheric chemical transport model. While these approaches have existed for several years in regional chemical transport models, the Global Particulate Matter Source Apportionment Technology (GPSAT) represents the first incorporation into a global chemical transport model. GPSAT runs in parallel to a standard GEOS-Chem run. GPSAT uses the fact that all molecules of a given species have the same probability of undergoing any given process as a core principle. This allows GPSAT to track many different species using only the flux information provided by GEOS-Chem's many processes. GPSAT accounts for the change in source specific concentrations as a result of aqueous and gas-phase chemistry, horizontal and vertical transport, condensation and evaporation on particulate matter, emissions, and wet and dry deposition. By using fluxes, GPSAT minimizes computational cost by circumventing the computationally costly chemistry and transport solvers. GPSAT will allow researchers to address many pertinent research questions about global particulate matter including the global impact of emissions from different source regions and the climate impacts from different source types and regions. For this first application of GPSAT, we investigate the contribution of the twenty largest urban areas worldwide to global particulate matter concentrations. The species investigated include: ammonium, nitrates, sulfates, and the secondary organic aerosols formed by the oxidation of benzene, isoprene, and terpenes. While GPSAT is not yet publically available, we will incorporate it into a future standard release of GEOS-Chem so that all GEOS-Chem users will have access to this new tool.
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.
Tracking Reactive Nitrogen Sources, Chemistry and Deposition in Urban Environments Using Stable Isotopes

Science.gov (United States)

Hastings, M. G.; Clark, S. C.; Chai, J.; Joyce, E.; Miller, D. J.; Schiebel, H.; Walters, W.

2017-12-01

Reactive nitrogen (Nr) includes compounds such as nitrogen oxides (NOx, HONO), ammonia (NH3), nitrate (NO3-), ammonium (NH4+), and organic nitrates. These compounds serve major roles in controlling the composition of our atmosphere, and have a direct impact on ecosystem health and water quality. Our research is focused on using stable isotopes of Nr to investigate variations in sources, chemistry, atmospheric transport, and deposition. Our aim is to fingerprint distinct emission sources - such as vehicles, power plants, aircraft, agriculature, wildfires, and lightning - and track their influence in the environment. We have recently characterized vehicle emission plumes, emissions from agricultural soils under different management practices, and (in the near future) wildfire plumes in the western U.S. Our approach targets characterizing the isotopic composition of NOx, HONO, and NH3 at both the emissions source and the plume scale. In contrast to large ranges found for individual tailpipe emissions of NOx, on-road plumes in the U.S. have a mean δ15N of -4.7 ± 1.7‰. The plume scale approach integrates across the typical U.S. fleet giving a representative value that can be used for tracking the impact of this emission source in the environment. NH3 also tends towards a narrow isotopic range when considered at the roadside scale compared to individual vehicles. In agricultural settings, the isotopes of NOx and HONO released from soils under different fertilizer practices is typically very negative in δ15N (-40 to -10‰) and appears to vary most with soil N properties rather than meteorology. Our work is now extending to discern sources influencing Nr deposition in an urban area at the head of New England's largest estuary. National monitoring of N deposition shows decreases in NO3- (but not NH4+) deposition over the last two decades, following better controls on NOx emissions. Wet deposition collected in an urban area exhibits N concentrations that are often 3
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
Investigating diesel engines as an atmospheric source of isocyanic acid in urban areas

Directory of Open Access Journals (Sweden)

S. H. Jathar

2017-07-01

Full Text Available Isocyanic acid (HNCO, an acidic gas found in tobacco smoke, urban environments, and biomass-burning-affected regions, has been linked to adverse health outcomes. Gasoline- and diesel-powered engines and biomass burning are known to emit HNCO and hypothesized to emit precursors such as amides that can photochemically react to produce HNCO in the atmosphere. Increasingly, diesel engines in developed countries like the United States are required to use selective catalytic reduction (SCR systems to reduce tailpipe emissions of oxides of nitrogen. SCR chemistry is known to produce HNCO as an intermediate product, and SCR systems have been implicated as an atmospheric source of HNCO. In this work, we measure HNCO emissions from an SCR system-equipped diesel engine and, in combination with earlier data, use a three-dimensional chemical transport model (CTM to simulate the ambient concentrations and source/pathway contributions to HNCO in an urban environment. Engine tests were conducted at three different engine loads, using two different fuels and at multiple operating points. HNCO was measured using an acetate chemical ionization mass spectrometer. The diesel engine was found to emit primary HNCO (3–90 mg kg fuel−1 but we did not find any evidence that the SCR system or other aftertreatment devices (i.e., oxidation catalyst and particle filter produced or enhanced HNCO emissions. The CTM predictions compared well with the only available observational datasets for HNCO in urban areas but underpredicted the contribution from secondary processes. The comparison implied that diesel-powered engines were the largest source of HNCO in urban areas. The CTM also predicted that daily-averaged concentrations of HNCO reached a maximum of ∼ 110 pptv but were an order of magnitude lower than the 1 ppbv level that could be associated with physiological effects in humans. Precursor contributions from other combustion sources (gasoline and biomass
Investigating Diesel Engines as an Atmospheric Source of Isocyanic Acid in Urban Areas

Science.gov (United States)

Farmer, D.; Jathar, S.; Heppding, C.; Link, M.; Akherati, A.; Kleeman, M.; De Gouw, J. A.; Veres, P. R.; Roberts, J. M.

2017-12-01

Isocyanic acid (HNCO), an acidic gas found in tobacco smoke, urban environments and biomass burning-affected regions, has been linked to adverse health outcomes. Gasoline- and diesel-powered engines and biomass burning are known to emit HNCO and hypothesized to emit precursors such as amides that can photochemically react to produce HNCO in the atmosphere. Increasingly, diesel engines in developed countries like the United States are required to use Selective Catalytic Reduction (SCR) systems to reduce tailpipe emissions of oxides of nitrogen. SCR chemistry is known to produce HNCO as an intermediate product, and SCR systems have been implicated as an atmospheric source of HNCO. In this work, we measure HNCO emissions from an SCR system-equipped diesel engine and, in combination with earlier data, use a three-dimensional chemical transport model (CTM) to simulate the ambient concentrations and source/pathway contributions to HNCO in an urban environment. Engine tests were conducted at three different engine loads, using two different fuels and at multiple operating points. HNCO was measured using an acetate chemical ionization mass spectrometer. The diesel engine was found to emit primary HNCO (3-90 mg kg-fuel-1) but we did not find any evidence that the SCR system or other aftertreatment devices (i.e., oxidation catalyst and particle filter) produced or enhanced HNCO emissions. The CTM predictions compared well with the only available observational data sets for HNCO in urban areas but under-predicted the contribution from secondary processes. The comparison implied that diesel-powered engines were the largest source of HNCO in urban areas. The CTM also predicted that daily-averaged concentrations of HNCO reached a maximum of 110 pptv but were an order of magnitude lower than the 1 ppbv level that could be associated with physiological effects in humans. Precursor contributions from other combustion sources (gasoline and biomass burning) and wintertime conditions
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.
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
Sources of atmospheric emissions in the Athabasca oil sands region

International Nuclear Information System (INIS)

1996-01-01

An inventory of emissions for the Athabasca oil sands airshed that can be used as a basis for air quality assessments was presented. This report was prepared for the Suncor Steepbank Mine Environmental Impact Assessment (EIA) and for the Syncrude Aurora Mine EIA. Both Syncrude and Suncor have plans to develop new oil sands leases and to increase their crude oil and bitumen production. Suncor has proposed modifications to reduce SO 2 emissions to the atmosphere and Syncrude will develop additional ambient air quality, sulphur deposition and biomonitoring programs to ensure that environmental quality is not compromised because of atmospheric emissions associated with their operations. Major emission sources are controlled and monitored by regulatory statutes, regulations and guidelines. In this report, the following four types of emission sources were identified and quantified: (1) major industrial sources associated with Suncor's and Syncrude's current oil sands operations, (2) fugitive and area emission sources such as volatilization of hydrocarbons from tanks and tailings ponds, (3) other industrial emission sources in the area, including oil sands and non-oil sands related facilities, and (4) highway and residential emission sources. Emissions associated with mining operations include: SO 2 , NO x , CO, and CO 2 . The overall conclusion was that although there are other smaller sources of emissions that can influence air quality, there is no reason to doubt that Suncor and Syncrude oil sands operations are the major sources of emissions to the atmosphere. 13 refs., 12 tabs., 8 figs
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.
Atmospheric deposition as a source of carbon and nutrients to barren, alpine soils of the Colorado Rocky Mountains

Science.gov (United States)

Mladenov, N.; Williams, M. W.; Schmidt, S. K.; Cawley, K.

2012-03-01

Many alpine areas are experiencing intense deglaciation, biogeochemical changes driven by temperature rise, and changes in atmospheric deposition. There is mounting evidence that the water quality of alpine streams may be related to these changes, including rising atmospheric deposition of carbon (C) and nutrients. Given that barren alpine soils can be severely C limited, we evaluated the magnitude and chemical quality of atmospheric deposition of C and nutrients to an alpine site, the Green Lake 4 catchment in the Colorado Rocky Mountains. Using a long term dataset (2002-2010) of weekly atmospheric wet deposition and snowpack chemistry, we found that volume weighted mean dissolved organic carbon (DOC) concentrations were approximately 1.0 mg L-1and weekly concentrations reached peaks as high at 6-10 mg L-1 every summer. Total dissolved nitrogen concentration also peaked in the summer, whereas total dissolved phosphorus and calcium concentrations were highest in the spring. Relationships among DOC concentration, dissolved organic matter (DOM) fluorescence properties, and nitrate and sulfate concentrations suggest that pollutants from nearby urban and agricultural sources and organic aerosols derived from sub-alpine vegetation may influence high summer DOC wet deposition concentrations. Interestingly, high DOC concentrations were also recorded during "dust-in-snow" events in the spring. Detailed chemical and spectroscopic analyses conducted for samples collected in 2010 revealed that the DOM in many late spring and summer samples was less aromatic and polydisperse and of lower molecular weight than that of winter and fall samples and, therefore, likely to be more bioavailable to microbes in barren alpine soils. Bioavailability experiments with different types of atmospheric C sources are needed to better evaluate the substrate quality of atmospheric C inputs. Our C budget estimates for the Green Lake 4 catchment suggest that atmospheric deposition represents an
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, NO_y 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 J_NO₂ and (1.4 × 10⁻⁵ s⁻¹ for J_O¹D which is comparable to the solar radiation in the boundary layer. An auxiliary mechanism describing NO_y 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-NO_x-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
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.
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.
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.

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.
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.
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
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.
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.
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.)
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.
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
Sources and photochemistry of volatile organic compounds in the remote atmosphere of western China: results from the Mt. Waliguan Observatory

Directory of Open Access Journals (Sweden)

L. K. Xue

2013-09-01

Full Text Available The chemistry of the natural atmosphere and the influence by long-range transport of air pollution are key issues in the atmospheric sciences. Here we present two intensive field measurements of volatile organic compounds (VOCs in late spring and summer of 2003 at Mt. Waliguan (WLG, 36.28° N, 100.90° E, 3816 m a.s.l., a baseline station in the northeast part of the Qinghai-Tibetan Plateau. Most VOC species exhibited higher concentrations in late spring than in summer. A typical diurnal variation was observed with higher nighttime levels, in contrast to results from other mountainous sites. Five different air masses were identified from backward trajectory analysis showing distinct VOC speciation. Air masses originating from the central Eurasian continent contained the lowest VOC levels compared to the others that were impacted by anthropogenic emissions from China and the Indian subcontinent. A photochemical box model based on the Master Chemical Mechanism (version 3.2 and constrained by a full suite of measurements was developed to probe the photochemistry of atmosphere at WLG. Our results show net ozone production from in situ photochemistry during both late spring and summer. Oxidation of nitric oxide (NO by the hydroperoxyl radical (HO2 dominates the ozone production relative to the oxidation by the organic peroxy radicals (RO2, and the ozone is primarily destroyed by photolysis and reactions with the HOx (HOx = OH + HO2 radicals. Ozone photolysis is the predominant primary source of radicals (ROx = OH + HO2 + RO2, followed by the photolysis of secondary oxygenated VOCs and hydrogen peroxides. The radical losses are governed by the self and cross reactions among the radicals. Overall, the findings of the present study provide insights into the background chemistry and the impacts of pollution transport on the pristine atmosphere over the Eurasian continent.
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
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.
Identifying the Source of Large-Scale Atmospheric Variability in Jupiter

Science.gov (United States)

Orton, Glenn

2011-01-01

We propose to use the unique mid-infrared filtered imaging and spectroscopic capabilities of the Subaru COMICS instrument to determine the mechanisms associated with recent unusual rapid albedo and color transformations of several of Jupiter's bands, particularly its South Equatorial Belt (SEB), as a means to understand the coupling between its dynamics and chemistry. These observations will characterize the temperature, degree of cloud cover, and distribution of minor gases that serve as indirect tracers of vertical motions in regions that will be undergoing unusual large-scale changes in dynamics and chemistry: the SEB, as well as regions near the equator and Jupiter's North Temperate Belt. COMICS is ideal for this investigation because of its efficiency in doing both imaging and spectroscopy, its 24.5-mum filter that is unique to 8-meter-class telescopes, its wide field of view that allows imaging of nearly all of Jupiter's disk, coupled with a high diffraction-limited angular resolution and optimal mid-infrared atmospheric transparency.
Atmospheric mercury dispersion modelling from two nearest hypothetical point sources

Energy Technology Data Exchange (ETDEWEB)

Al Razi, Khandakar Md Habib; Hiroshi, Moritomi; Shinji, Kambara [Environmental and Renewable Energy System (ERES), Graduate School of Engineering, Gifu University, Yanagido, Gifu City, 501-1193 (Japan)

2012-07-01

The Japan coastal areas are still environmentally friendly, though there are multiple air emission sources originating as a consequence of several developmental activities such as automobile industries, operation of thermal power plants, and mobile-source pollution. Mercury is known to be a potential air pollutant in the region apart from SOX, NOX, CO and Ozone. Mercury contamination in water bodies and other ecosystems due to deposition of atmospheric mercury is considered a serious environmental concern. Identification of sources contributing to the high atmospheric mercury levels will be useful for formulating pollution control and mitigation strategies in the region. In Japan, mercury and its compounds were categorized as hazardous air pollutants in 1996 and are on the list of 'Substances Requiring Priority Action' published by the Central Environmental Council of Japan. The Air Quality Management Division of the Environmental Bureau, Ministry of the Environment, Japan, selected the current annual mean environmental air quality standard for mercury and its compounds of 0.04 ?g/m3. Long-term exposure to mercury and its compounds can have a carcinogenic effect, inducing eg, Minamata disease. This study evaluates the impact of mercury emissions on air quality in the coastal area of Japan. Average yearly emission of mercury from an elevated point source in this area with background concentration and one-year meteorological data were used to predict the ground level concentration of mercury. To estimate the concentration of mercury and its compounds in air of the local area, two different simulation models have been used. The first is the National Institute of Advanced Science and Technology Atmospheric Dispersion Model for Exposure and Risk Assessment (AIST-ADMER) that estimates regional atmospheric concentration and distribution. The second is the Hybrid Single Particle Lagrangian Integrated trajectory Model (HYSPLIT) that estimates the atmospheric
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....
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.
Utilizations of intense pulsed neutron source in radiochemistry and radiation chemistry

International Nuclear Information System (INIS)

Shiokawa, Takanobu; Yoshihara, Kenji; Kaji, Harumi; Kusaka, Yuzuru; Tabata, Yoneho.

1975-01-01

Intense pulsed neutron sources is expected to supply more useful and fundamental informations in radiochemistry and radiation chemistry. Short-lived intermediate species may be detected and the mechanisms of radiation induced reactions will be elucidated more precisely. Analytical application of pulsed neutrons is also very useful. (auth.)
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'
A review of atmospheric polycyclic aromatic hydrocarbons: sources, fate and behavior

International Nuclear Information System (INIS)

Baek, S.O.; Field, R.A.; Goldstone, M.E.; Kirk, P.W.; Lester, J.N.; Perry, R.

1991-01-01

A review has been written to assess the sources, fate and behavior of polycyclic aromatic hydrocarbons (PAH) in the atmosphere. PAH are formed mainly by anthropogenic processes, especially the combustion of organic fuels. PAH concentration in air will reflect the location of source emitters, with high concentrations corresponding with urban and industrial areas. PAH are however ubiquitous contaminants of the environment having been detected in remote areas of the world. This is thought to be due to long term transport in the atmosphere. PAH can also be subjected to chemical and/or photochemical change whilst resident in the atmosphere prior to their removal by either wet or dry deposition. 146 refs., 5 tabs
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
An investigation of the atmospheric sources and sinks of methyl bromide

International Nuclear Information System (INIS)

Singh, H.B.; Kanakidou, M.

1993-01-01

Methyl Bromide (CH 3 Br) is a ubiquitous component of the atmosphere and has been implicated as an important player in the depletion of stratospheric ozone. Atmospheric CH 3 Br abundances, interhemispheric gradients, oceanic concentrations, man-made emissions, and removal processes have been analyzed and interpreted with the help of a simple box model and a 2-D global photochemical model. Its calculated atmospheric lifetime (T) of 1.7-1.9 years, based on reaction with OH radicals, is consistent with a global source of 90-110 Gg (10 9 g)/year. Consequences of a much shorter lifetime of 1.2 years, due to possible deposition/hydrolysis losses, are also considered. Available data are used to estimate a CH 3 Br source that is 35% (20-50%) man-made and 65% (80-50%) natural. Oceans are substantially supersaturated and provide the most important natural source of ∼60 (40-80) Gg/year. Within the oceans 200-300 Gg/year of CH 3 Br may be produced. Indirect emissions from automobile exhaust and biomass burning can not be well quantified (1-10 Gg/year). A global trend of 0.1-0.2 ppt/year is predicted. Model results show significant vertical and seasonal variations in the atmospheric abundances and interhemispheric gradients of CH 3 Br. Substantial uncertainties in calibrations, source estimates, and deposition processes are present. 12 refs., 3 figs., 2 tabs

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.
White Dwarf Model Atmospheres: Synthetic Spectra for Supersoft Sources

Science.gov (United States)

Rauch, Thomas

2013-01-01

The Tübingen NLTE Model-Atmosphere Package (TMAP) calculates fully metal-line blanketed white dwarf model atmospheres and spectral energy distributions (SEDs) at a high level of sophistication. Such SEDs are easily accessible via the German Astrophysical Virtual Observatory (GAVO) service TheoSSA. We discuss applications of TMAP models to (pre) white dwarfs during the hottest stages of their stellar evolution, e.g. in the parameter range of novae and supersoft sources.
MEDINA: MECCA Development in Accelerators – KPP Fortran to CUDA source-to-source Pre-processor

Directory of Open Access Journals (Sweden)

Michail Alvanos

2017-04-01

Full Text Available The global climate model ECHAM/MESSy Atmospheric Chemistry (EMAC is a modular global model that simulates climate change and air quality scenarios. The application includes different sub-models for the calculation of chemical species concentrations, their interaction with land and sea, and the human interaction. The paper presents a source-to-source parser that enables support for Graphics Processing Units (GPU by the Kinetic Pre-Processor (KPP general purpose open-source software tool. The requirements of the host system are also described. The source code of the source-to-source parser is available under the MIT License.
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
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
NLTE Model Atmospheres for Super-Soft X-ray Sources

Science.gov (United States)

Rauch, Thomas; Werner, Klaus

2009-09-01

Spectral analysis by means of fully line-blanketed Non-LTE model atmospheres has arrived at a high level of sophistication. The Tübingen NLTE Model Atmosphere Package (TMAP) is used to calculate plane-parallel NLTE model atmospheres which are in radiative and hydrostatic equilibrium. Although TMAP is not especially designed for the calculation of burst spectra of novae, spectral energy distributions (SEDs) calculated from TMAP models are well suited e.g. for abundance determinations of Super Soft X-ray Sources like nova V4743 Sgr or line identifications in observations of neutron stars with low magnetic fields in low-mass X-ray binaries (LMXBs) like EXO 0748-676.
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
Response in atmospheric circulation and sources of Greenland precipitation to glacial boundary conditions

DEFF Research Database (Denmark)

Langen, Peter Lang; Vinther, Bo Møllesøe

2009-01-01

The response in northern hemisphere atmospheric circulation and the resulting changes in moisture sources for Greenland precipitation to glacial boundary conditions are studied in NCAR's CCM3 atmospheric general circulation model fitted with a moisture tracking functionality. We employ both...... seasonality, condensation temperatures and source temperatures are assessed. Udgivelsesdato: June 2009...
The chemistry of the global atmosphere; International Symposium of the Commission for Atmospheric Chemistry and Global Pollution of IAMAP, 7th, Chamrousse, France, Sept. 5-11, 1990, Selected Papers

Science.gov (United States)

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

1992-01-01

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

Science.gov (United States)

Blake, D. R.; Rowland, F. S.

1986-01-01

A study of the variation in ethane (C2H6) concentration between northern and southern latitudes over three years is presented together with a new estimate of its source strength. Ethane concentrations vary from 0.07 to 2 p.p.b.v. (parts per billion by volume) in air samples collected in remote surface locations in the Pacific (latitude 71 N-47 S) in all four seasons between September 1984 and June 1985. The variations are consistent with southerly transport from sources located chiefly in the Northern Hemisphere, further modified by seasonal variations in the strength of the reaction of C2H6 with OH radicals. These global data can be combined with concurrent data for CH4 and the laboratory reaction rates of each with OH to provide an estimate of three months as the average atmospheric lifetime for C2H6 and 13 + or - 3 Mtons for its annual atmospheric release.
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).
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.
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
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
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
The sources and fate of radionuclides emitted to the atmosphere

International Nuclear Information System (INIS)

Sandalls, J.

2001-01-01

The thesis represents an account of the sources and fate of radionuclides entering the atmosphere, and indicates where the candidate, through his own work, has contributed to the overall picture. The sources of the natural and man-made radionuclides found in the atmosphere are identified. New data on emissions from UK coal-fired power stations and UK steel works are reported. Radionuclides produced in nuclear fission and released to the atmosphere in the detonation of nuclear weapons, in nuclear accidents, and through routine discharges from nuclear sites have added to the atmospheric burden of radioactive materials; both acute and chronic low-level emissions are discussed. The various natural processes which remove radionuclides from the atmosphere are described. Soon after release, many radioactive materials become attached to the atmospheric aerosol, but others undergo gas-phase reactions. Some gases are sufficiently long-lived in the troposphere as to find their way into the stratosphere where their fate may be determined by the short-wave radiation from the sun. The nature of the particles of fuel emitted to the atmosphere in the explosion and fire at the Chernobyl nuclear power plant in 1986 are discussed, together with the associated environmental problems. The ground is the major sink for radionuclides leaving the atmosphere, and the behaviour of the more radiologically important radionuclides following deposition is described with special reference to: (i) fallout in both the urban and living environments; (ii) the pathways which may lead to contamination of the food chain; (iii) how the fuel particle fallout from Chernobyl was unique in nuclear accidents; (iv) soil-to-plant transfer of radioelements and (v) how radiation exposure of man can be mitigated in both the contaminated urban and rural environments. (author)
Atmospheric polychlorinated biphenyls in Indian cities: Levels, emission sources and toxicity equivalents

International Nuclear Information System (INIS)

Chakraborty, Paromita; Zhang, Gan; Eckhardt, Sabine; Li, Jun; Breivik, Knut; Lam, Paul K.S.; Tanabe, Shinsuke; Jones, Kevin C.

2013-01-01

Atmospheric concentration of Polychlorinated biphenyls (PCBs) were measured on diurnal basis by active air sampling during Dec 2006 to Feb 2007 in seven major cities from the northern (New Delhi and Agra), eastern (Kolkata), western (Mumbai and Goa) and southern (Chennai and Bangalore) parts of India. Average concentration of Σ 25 PCBs in the Indian atmosphere was 4460 (±2200) pg/m −3 with a dominance of congeners with 4–7 chlorine atoms. Model results (HYSPLIT, FLEXPART) indicate that the source areas are likely confined to local or regional proximity. Results from the FLEXPART model show that existing emission inventories cannot explain the high concentrations observed for PCB-28. Electronic waste, ship breaking activities and dumped solid waste are attributed as the possible sources of PCBs in India. Σ 25 PCB concentrations for each city showed significant linear correlation with Toxicity equivalence (TEQ) and Neurotoxic equivalence (NEQ) values. Highlights: •Unlike decreasing trend of PCBs in United States and European countries, high levels of PCBs remain in the Indian atmosphere. •Existing emission inventories cannot explain the high PCB concentrations in Indian atmosphere. •Electronic waste recycling, ship dismantling and open burning of municipal solid waste are implicated as potential sources. -- Measurement of atmospheric Polychlorinated biphenyls in seven major Indian cities
Chernobyl source term, atmospheric dispersion, and dose estimation

International Nuclear Information System (INIS)

Gudiksen, P.H.; Harvey, T.F.; Lange, R.

1988-02-01

The Chernobyl source term available for long-range transport was estimated by integration of radiological measurements with atmospheric dispersion modeling, and by reactor core radionuclide inventory estimation in conjunction with WASH-1400 release fractions associated with specific chemical groups. These analyses indicated that essentially all of the noble gases, 80% of the radioiodines, 40% of the radiocesium, 10% of the tellurium, and about 1% or less of the more refractory elements were released. Atmospheric dispersion modeling of the radioactive cloud over the Northern Hemisphere revealed that the cloud became segmented during the first day, with the lower section heading toward Scandinavia and the uppper part heading in a southeasterly direction with subsequent transport across Asia to Japan, the North Pacific, and the west coast of North America. The inhalation doses due to direct cloud exposure were estimated to exceed 10 mGy near the Chernobyl area, to range between 0.1 and 0.001 mGy within most of Europe, and to be generally less than 0.00001 mGy within the US. The Chernobyl source term was several orders of magnitude greater than those associated with the Windscale and TMI reactor accidents, while the 137 Cs from the Chernobyl event is about 6% of that released by the US and USSR atmospheric nuclear weapon tests. 9 refs., 3 figs., 6 tabs
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.
HELIOS: An Open-source, GPU-accelerated Radiative Transfer Code for Self-consistent Exoplanetary Atmospheres

Science.gov (United States)

Malik, Matej; Grosheintz, Luc; Mendonça, João M.; Grimm, Simon L.; Lavie, Baptiste; Kitzmann, Daniel; Tsai, Shang-Min; Burrows, Adam; Kreidberg, Laura; Bedell, Megan; Bean, Jacob L.; Stevenson, Kevin B.; Heng, Kevin

2017-02-01

We present the open-source radiative transfer code named HELIOS, which is constructed for studying exoplanetary atmospheres. In its initial version, the model atmospheres of HELIOS are one-dimensional and plane-parallel, and the equation of radiative transfer is solved in the two-stream approximation with nonisotropic scattering. A small set of the main infrared absorbers is employed, computed with the opacity calculator HELIOS-K and combined using a correlated-k approximation. The molecular abundances originate from validated analytical formulae for equilibrium chemistry. We compare HELIOS with the work of Miller-Ricci & Fortney using a model of GJ 1214b, and perform several tests, where we find: model atmospheres with single-temperature layers struggle to converge to radiative equilibrium; k-distribution tables constructed with ≳ 0.01 cm-1 resolution in the opacity function (≲ {10}3 points per wavenumber bin) may result in errors ≳ 1%-10% in the synthetic spectra; and a diffusivity factor of 2 approximates well the exact radiative transfer solution in the limit of pure absorption. We construct “null-hypothesis” models (chemical equilibrium, radiative equilibrium, and solar elemental abundances) for six hot Jupiters. We find that the dayside emission spectra of HD 189733b and WASP-43b are consistent with the null hypothesis, while the latter consistently underpredicts the observed fluxes of WASP-8b, WASP-12b, WASP-14b, and WASP-33b. We demonstrate that our results are somewhat insensitive to the choice of stellar models (blackbody, Kurucz, or PHOENIX) and metallicity, but are strongly affected by higher carbon-to-oxygen ratios. The code is publicly available as part of the Exoclimes Simulation Platform (exoclime.net).

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.
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
Thinking about online sources: Exploring students' epistemic cognition in internet-based chemistry learning

Science.gov (United States)

Dai, Ting

This dissertation investigated the relation between epistemic cognition---epistemic aims and source beliefs---and learning outcome in an Internet--based research context. Based on a framework of epistemic cognition (Chinn, Buckland, & Samarapungavan, 2011), a context--specific epistemic aims and source beliefs questionnaire (CEASBQ) was developed and administered to 354 students from college--level introductory chemistry courses. A series of multitrait--multimethod model comparisons provided evidence for construct convergent and discriminant validity for three epistemic aims--- true beliefs, justified beliefs, explanatory connection, which were all distinguished from, yet correlated with, mastery goals. Students' epistemic aims were specific to the chemistry topics in research. Multidimensional scaling results indicated that students' source evaluation was based on two dimensions--- professional expertise and first--hand knowledge, suggesting a multidimensional structure of source beliefs. Most importantly, online learning outcome was found to be significantly associated with two epistemic aims---justified beliefs and explanatory connection: The more students sought justifications in the online research, the lower they tended to score on the learning outcome measure, whereas the more students sought explanatory connections between information, the higher they scored on the outcome measure. There was a significant but small positive association between source beliefs and learning outcome. The influences of epistemic aims and source beliefs on learning outcome were found to be above and beyond the effects of a number of covariates, including prior knowledge and perceived ability with online sources.
The chemistry of molecular anions in circumstellar sources

Energy Technology Data Exchange (ETDEWEB)

Agúndez, Marcelino [LUTH, Observatoire de Paris-Meudon, 5 Place Jules Janssen, 92190 Meudon (France); Cernicharo, José [Departamento de Astrofísica, CAB, CSIC-INTA, Ctra. de Torrejón a Ajalvir km 4, 28850 Madrid (Spain); Guélin, Michel [Institut de Radioastronomie Millimétrique, 300 rue de la Piscine, 38406 Saint Martin d' Héres (France)

2015-01-22

The detection of negatively charged molecules in the interstellar and circumstellar medium in the past four years has been one of the most impacting surprises in the area of molecular astrophysics. It has motivated the interest of astronomers, physicists, and chemists on the study of the spectroscopy, chemical kinetics, and prevalence of molecular anions in the different astronomical regions. Up to six different molecular anions have been discovered in space to date, the last one being the small ion CN{sup −}, which has been observed in the envelope of the carbon star IRC +10216 and which contrary to the other larger anions is not formed by electron attachment to CN, but through reactions of large carbon anions with nitrogen atoms. Here we briefly review the current status of our knowledge of the chemistry of molecular anions in space, with particular emphasis on the circumstellar source IRC +10216, which to date is the astronomical source harboring the largest variety of anions.
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
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...
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
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
Parameterized isoprene and monoterpene emissions from the boreal forest floor: Implementation into a 1D chemistry-transport model and investigation of the influence on atmospheric chemistry

Science.gov (United States)

Mogensen, Ditte; Aaltonen, Hermanni; Aalto, Juho; Bäck, Jaana; Kieloaho, Antti-Jussi; Gierens, Rosa; Smolander, Sampo; Kulmala, Markku; Boy, Michael

2015-04-01

Volatile organic compounds (VOCs) are emitted from the biosphere and can work as precursor gases for aerosol particles that can affect the climate (e.g. Makkonen et al., ACP, 2012). VOC emissions from needles and leaves have gained the most attention, however other parts of the ecosystem also have the ability to emit a vast amount of VOCs. This, often neglected, source can be important e.g. at periods where leaves are absent. Both sources and drivers related to forest floor emission of VOCs are currently limited. It is thought that the sources are mainly due to degradation of organic matter (Isidorov and Jdanova, Chemosphere, 2002), living roots (Asensio et al., Soil Biol. Biochem., 2008) and ground vegetation. The drivers are biotic (e.g. microbes) and abiotic (e.g. temperature and moisture). However, the relative importance of the sources and the drivers individually are currently poorly understood. Further, the relative importance of these factors is highly dependent on the tree species occupying the area of interest. The emission of isoprene and monoterpenes where measured from the boreal forest floor at the SMEAR II station in Southern Finland (Hari and Kulmala, Boreal Env. Res., 2005) during the snow-free period in 2010-2012. We used a dynamic method with 3 automated chambers analyzed by Proton Transfer Reaction - Mass Spectrometer (Aaltonen et al., Plant Soil, 2013). Using this data, we have developed empirical parameterizations for the emission of isoprene and monoterpenes from the forest floor. These parameterizations depends on abiotic factors, however, since the parameterizations are based on field measurements, biotic features are captured. Further, we have used the 1D chemistry-transport model SOSAA (Boy et al., ACP, 2011) to test the seasonal relative importance of inclusion of these parameterizations of the forest floor compared to the canopy crown emissions, on the atmospheric reactivity throughout the canopy.
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

principal source of PAN in the UTLS is due to lofted biomass burning emissions from the pyroconvective updrafts created by large fires, the observed seasonality in enhanced PAN coincides with fire activity in different geographical regions throughout the year. This work is part of an in-depth investigation that is being conducted in an effort to study the aging and chemical evolution of biomass burning emissions in the UTLS by remote, space-borne measurements made by ACE-FTS to further our understanding of the impact of pyrogenic emissions on atmospheric chemistry. Included in this study will be the addition of new, pyrogenic, volatile organic hydrocarbons (VOCs) and oxygenated volatile organic compounds (OVOCs) to expand upon the already extensive suite of molecules retrieved by ACE-FTS to aid in elucidating biomass burning plume chemistry in the free troposphere.
Atmospheric heavy metals and Arsenic in China: Situation, sources and control policies

Science.gov (United States)

Duan, Jingchun; Tan, Jihua

2013-08-01

In recent years, heavy metal pollution accidents were reported frequently in China. The atmospheric heavy metal pollution is drawing all aspects of attention. This paper summarizes the recent research results from our studies and previous studies in recent years in China. The level, temporal variation, seasonal variation and size distribution of the heavy metals of atmospheric Lead(Pb), Vanadium(V), Manganese(Mn), Nickel(Ni), Chromium(Cr), Cadmium(Cd), Copper(Cu), Zinc(Zn) and Arsenic(As) were characterized in China. The emission characteristics and sources of atmospheric heavy metals and As in China were reviewed. Coal burning, iron and steel industry and vehicle emission are important sources in China. Control policies and effects in China were reviewed including emission standards, ambient air quality standards, phase out of leaded gasoline and so on, and further works for atmospheric heavy metals control were suggested. The comprehensive heavy metals pollution control measures and suggestions were put forward based on the summarization of the development and experience of the atmospheric heavy metal pollution control abroad.
Inversion of Atmospheric Tracer Measurements, Localization of Sources

Science.gov (United States)

Issartel, J.-P.; Cabrit, B.; Hourdin, F.; Idelkadi, A.

When abnormal concentrations of a pollutant are observed in the atmosphere, the question of its origin arises immediately. The radioactivity from Tchernobyl was de- tected in Sweden before the accident was announced. This situation emphasizes the psychological, political and medical stakes of a rapid identification of sources. In tech- nical terms, most industrial sources can be modeled as a fixed point at ground level with undetermined duration. The classical method of identification involves the cal- culation of a backtrajectory departing from the detector with an upstream integration of the wind field. We were first involved in such questions as we evaluated the ef- ficiency of the international monitoring network planned in the frame of the Com- prehensive Test Ban Treaty. We propose a new approach of backtracking based upon the use of retroplumes associated to available measurements. Firstly the retroplume is related to inverse transport processes, describing quantitatively how the air in a sam- ple originates from regions that are all the more extended and diffuse as we go back far in the past. Secondly it clarifies the sensibility of the measurement with respect to all potential sources. It is therefore calculated by adjoint equations including of course diffusive processes. Thirdly, the statistical interpretation, valid as far as sin- gle particles are concerned, should not be used to investigate the position and date of a macroscopic source. In that case, the retroplume rather induces a straightforward constraint between the intensity of the source and its position. When more than one measurements are available, including zero valued measurements, the source satisfies the same number of linear relations tightly related to the retroplumes. This system of linear relations can be handled through the simplex algorithm in order to make the above intensity-position correlation more restrictive. This method enables to manage in a quantitative manner the
White Dwarf Model Atmospheres: Synthetic Spectra for Super Soft Sources

OpenAIRE

Rauch, Thomas

2011-01-01

The T\\"ubingen NLTE Model-Atmosphere Package (TMAP) calculates fully metal-line blanketed white dwarf model atmospheres and spectral energy distributions (SEDs) at a high level of sophistication. Such SEDs are easily accessible via the German Astrophysical Virtual Observatory (GAVO) service TheoSSA. We discuss applications of TMAP models to (pre) white dwarfs during the hottest stages of their stellar evolution, e.g. in the parameter range of novae and super soft sources.
OrChem - An open source chemistry search engine for Oracle®

Science.gov (United States)

2009-01-01

Background Registration, indexing and searching of chemical structures in relational databases is one of the core areas of cheminformatics. However, little detail has been published on the inner workings of search engines and their development has been mostly closed-source. We decided to develop an open source chemistry extension for Oracle, the de facto database platform in the commercial world. Results Here we present OrChem, an extension for the Oracle 11G database that adds registration and indexing of chemical structures to support fast substructure and similarity searching. The cheminformatics functionality is provided by the Chemistry Development Kit. OrChem provides similarity searching with response times in the order of seconds for databases with millions of compounds, depending on a given similarity cut-off. For substructure searching, it can make use of multiple processor cores on today's powerful database servers to provide fast response times in equally large data sets. Availability OrChem is free software and can be redistributed and/or modified under the terms of the GNU Lesser General Public License as published by the Free Software Foundation. All software is available via http://orchem.sourceforge.net. PMID:20298521
OrChem - An open source chemistry search engine for Oracle(R).

Science.gov (United States)

Rijnbeek, Mark; Steinbeck, Christoph

2009-10-22

Registration, indexing and searching of chemical structures in relational databases is one of the core areas of cheminformatics. However, little detail has been published on the inner workings of search engines and their development has been mostly closed-source. We decided to develop an open source chemistry extension for Oracle, the de facto database platform in the commercial world. Here we present OrChem, an extension for the Oracle 11G database that adds registration and indexing of chemical structures to support fast substructure and similarity searching. The cheminformatics functionality is provided by the Chemistry Development Kit. OrChem provides similarity searching with response times in the order of seconds for databases with millions of compounds, depending on a given similarity cut-off. For substructure searching, it can make use of multiple processor cores on today's powerful database servers to provide fast response times in equally large data sets. OrChem is free software and can be redistributed and/or modified under the terms of the GNU Lesser General Public License as published by the Free Software Foundation. All software is available via http://orchem.sourceforge.net.
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 (F_10.7 in the tropics. The peak zonal mean tropical temperature response using the SORCE SSI is nearly 2 K per 100 units F_10.7 – 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
Sensitivity of Ambient Atmospheric Formaldehyde and Ozone to Precursor Species and Source Types Across the United States

Science.gov (United States)

Formaldehyde (HCHO) is an important air pollutant from both an atmospheric chemistry and human health standpoint. This study uses an instrumented photochemical Air Quality Model, CMAQ-DDM, to identify the sensitivity of HCHO concentrations across the United States (U.S.) to major...
Coal fly ash as a source of iron in atmospheric dust.

Science.gov (United States)

Chen, Haihan; Laskin, Alexander; Baltrusaitis, Jonas; Gorski, Christopher A; Scherer, Michelle M; Grassian, Vicki H

2012-02-21

Anthropogenic coal fly ash (FA) aerosol may represent a significant source of bioavailable iron in the open ocean. Few measurements have been made that compare the solubility of atmospheric iron from anthropogenic aerosols and other sources. We report here an investigation of iron dissolution for three FA samples in acidic aqueous solutions and compare the solubilities with that of Arizona test dust (AZTD), a reference material for mineral dust. The effects of pH, simulated cloud processing, and solar radiation on iron solubility have been explored. Similar to previously reported results on mineral dust, iron in aluminosilicate phases provides the predominant component of dissolved iron. Iron solubility of FA is substantially higher than of the crystalline minerals comprising AZTD. Simulated atmospheric processing elevates iron solubility due to significant changes in the morphology of aluminosilicate glass, a dominant material in FA particles. Iron is continuously released into the aqueous solution as FA particles break up into smaller fragments. These results suggest that the assessment of dissolved atmospheric iron deposition fluxes and their effect on the biogeochemistry at the ocean surface should be constrained by the source, environmental pH, iron speciation, and solar radiation.
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.
PREP-CHEM-SRC – 1.0: a preprocessor of trace gas and aerosol emission fields for regional and global atmospheric chemistry models

Directory of Open Access Journals (Sweden)

S. R. Freitas

2011-05-01

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

Sulphur isotope variations in the atmosphere

International Nuclear Information System (INIS)

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

1991-01-01

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

International Nuclear Information System (INIS)

Herranz Puebla, L.E.; Lopez Diez, I.; Rodriguez Maroto, J.J.; Martinez Lopez-Alcorocho, A.

1991-01-01

The major goal of a phenomenology analysis of containment during a severe accident situation can be splitedd into the following ones: to know the containment response to the different loads and to predict accurately the fission product and aerosol behavior. In this report, the main results coming from the study of a hypothetical accident scenario, based on LA-4 experiment of LACE project, are presented. In order to do it, several codes have been coupled: CONTEMPT4/MOD5 (thermalhydraulics), NAUA/MOD5 (aerosol physics) and IODE (iodine chemistry). 12 refs. It has been demonstrated the impossibility of assessing with confidence the Source Term if the chemical conduct of some radionuclides is not taken into account. In particular, the influence on the iodine retention efficiency of the sump of variables such as pH has been proven. (Author). 12 refs
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.
Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

Science.gov (United States)

Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray
Atmospheric chemistry of ethane and ethylene

International Nuclear Information System (INIS)

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

1982-01-01

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

Energy Technology Data Exchange (ETDEWEB)

Aghoyeh, Reza Gholizadeh [School of Research and Development of Nuclear Reactors and Accelerators, Nuclear Science and Technology Research Institute (NSTRI), Atomic Energy Organization of Iran (AEOI), P.O. Box: 14155-1339, Tehran (Iran, Islamic Republic of); Khalafi, Hossein, E-mail: hkhalafi@aeoi.org.i [School of Research and Development of Nuclear Reactors and Accelerators, Nuclear Science and Technology Research Institute (NSTRI), Atomic Energy Organization of Iran (AEOI), P.O. Box: 14155-1339, Tehran (Iran, Islamic Republic of)

2011-03-15

Research highlights: Effect of Pu-Be neutron source meltdown in core on reactor water chemistry. Water chemistry of primary cooling before, during and after of above incident was compared. Training importance. Management of nuclear incident and accident. - Abstract: Effect of Pu-Be neutron source meltdown in core on reactor water chemistry was main aim of this study. Leaving the neutron source in the core after reactor power exceeds a few hundred Watts was the main reason for its partial meltdown. Water chemistry of primary cooling before, during and after of above incident was compared. Activity of some radio-nuclides such as Ba-140, La-140, I-131, I-132, Te-132 and Xe-135 increased. Other radio-nuclides such as Nd-147, Xe-133, Sr-91, I-133 and I-135 are also detected which were not existed before this incident.
Based on a True Story: Using Movies as Source Material for General Chemistry Reports

Science.gov (United States)

Griep, Mark A.; Mikasen, Marjorie L.

2005-10-01

Research for chemical reports and case study analysis of chemical topics are two commonly used learning activities to engage and enrich student understanding of the content in introductory chemistry courses. Even though movies are excellent vehicles for exploring the human dimension of events, they have been used only sparingly as source material in introductory science courses. One reason for this sparing use has been the lack of a list of suitable movies. To fill this void, a list of one dozen highly rated movies is presented. The focus of these movies is either a scientist's chemical research or the societal impact of some chemical compound. The method by which two of these movies were used as source material for a written report in a general chemistry course is described. The student response to the exercise was enthusiastic.
Source, concentration, and distribution of elemental mercury in the atmosphere in Toronto, Canada

International Nuclear Information System (INIS)

Cairns, Elaine; Tharumakulasingam, Kavitharan; Athar, Makshoof; Yousaf, Muhammad; Cheng, Irene; Huang, Y.; Lu, Julia; Yap, Dave

2011-01-01

Atmospheric gaseous elemental mercury [GEM] at 1.8, 4, and 59 m above ground, in parking lots, and in indoor and outdoor air was measured in Toronto City, Canada from May 2008-July 2009. The average GEM value at 1.8 m was 1.89 ± 0.62 ng m -3 . The GEM values increased with elevation. The average GEM in underground parking lots ranged from 1.37 to 7.86 ng m -3 and was higher than those observed from the surface parking lots. The GEM in the indoor air ranged from 1.21 to 28.50 ng m -3 , was higher in the laboratories than in the offices, and was much higher than that in the outdoor air. All these indicate that buildings serve as sources of mercury to the urban atmosphere. More studies are needed to estimate the contribution of urban areas to the atmospheric mercury budget and the impact of indoor air on outdoor air quality and human health. - Highlights: → Buildings served as mercury sources to urban atmosphere. → Atmospheric mercury level increased with increasing height in the street canyon. → Emission from vehicles and ground surfaces was not the major sources of Hg to urban air. → Mercury levels were higher in indoor than outdoor air and in laboratories than in offices. → Mercury levels were higher in the outdoor air near building walls. - Buildings serve as sources of gaseous elemental mercury and research is needed to quantify the emission and to assess the impact of indoor air on outdoor air quality and human health.
Tracing the Atmospheric Source of Desert Nitrates Using Δ 17O

Science.gov (United States)

Michalski, G. M.; Holve, M.; Feldmeier, J.; Bao, H.; Reheis, M.; Bockheim, J. G.; Thiemens, M. H.

2001-05-01

Mineral, caliche, and soil nitrates are found throughout the worlds deserts, including the cold dry Wright Valley of Antarctica, the Atacama desert in Chile and the Mojave desert in the southwest United States. Several authors have suggested biologic sources of these nitrates while others have postulated atmospheric deposition. A recent study utilizing 18O indicated that 30%, and perhaps 100%, of nitrates found in the Atacama and Mojave were of atmospheric origin [1]. A more quantitative assessment of the source strength of atmospheric nitrates was impossible because of the high variability of δ 18 18O of atmospheric nitrates and uncertainties in conditions of biologic production. Mass independently fractionated (MIF) processes are defined and quantified by the equation Δ 17O = δ 17O - .52x δ 18O. MIF processes are associated with the photochemistry of trace gases in the atmosphere and have been found in O3, N2O, CO, and sulfate aerosols . A large MIF (Δ 17O ~ 28 ‰ ) in nitrate aerosols collected in polluted regions was recently reported [2]. Here we extend measurements of MIF in nitrate to the dry deposition of nitrate in less polluted areas (Mojave desert). In addition we trace the MIF signal as it accumulates in the regolith as nitrate salts and minerals and is mixed with biologically produced nitrate (nitrification). Also examined were the isotopic composition of soil nitrates from Antarctic dry valleys. Dust samples were collected as part of the NADP program and soils were collected throughout the Mojave and Death Valley regions of California. Isotope analysis was done in addition to soluble ion content (Cl, NO3, SO4). Dust samples collected by dry deposition samplers showed a large MIF > 20‰ approaching values measured in urban nitrate aerosol. Soils collected throughout the region showed large variations in Δ 17O from ~ 0 to 18 ‰ . The low Δ 17O values are nitrates dominated by biologic nitrification and higher values are nitrates derived by
Speciated atmospheric mercury and its potential source in Guiyang, China

Science.gov (United States)

Fu, Xuewu; Feng, Xinbin; Qiu, Guangle; Shang, Lihai; Zhang, Hui

2011-08-01

Speciated atmospheric mercury (Hg) including gaseous elemental mercury (GEM), particulate Hg (PHg), and reactive gaseous Hg (RGM) were continuously measured at an urban site in Guiyang city, southwest China from August to December 2009. The averaged concentrations for GEM, PHg, and RGM were 9.72 ± 10.2 ng m -3, 368 ± 676 pg m -3, and 35.7 ± 43.9 pg m -3, respectively, which were all highly elevated compared to observations at urban sites in Europe and North America. GEM and PHg were characterized by similar monthly and diurnal patterns, with elevated levels in cold months and nighttime, respectively. In contrast, RGM did not exhibit clear monthly and diurnal variations. The variations of GEM, PHg, and RGM indicate the sampling site was significantly impacted by sources in the city municipal area. Sources identification implied that both residential coal burning and large point sources were responsible to the elevated GEM and PHg concentrations; whereas point sources were the major contributors to elevated RGM concentrations. Point sources played a different role in regulating GEM, PHg, and RGM concentrations. Aside from residential emissions, PHg levels was mostly affected by small-scale coal combustion boilers situated to the east of the sampling site, which were scarcely equipped or lacking particulate control devices; whereas point sources situated to the east, southeast, and southwest of the sampling played an important role on the distribution of atmospheric GEM and RGM.
Atmospheric processing of combustion aerosols as a source of soluble iron to the open ocean

OpenAIRE

伊藤, 彰記; ITO, Akinori

2015-01-01

The majority of bioavailable iron (Fe) from the atmosphere is delivered from arid and semiarid regions to the oceans because the global deposition of iron from combustion sources is small compared with that from mineral dust. Atmospheric processing of mineral aerosols by inorganic and organic acids from anthropogenic and natural sources has been shown to increase the iron solubility of soils (initially < 0.5%) up to about 10%. On the other hand, atmospheric observations have shown that iron i...
Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer

Science.gov (United States)

Mungall, Emma L.; Abbatt, Jonathan P. D.; Wentzell, Jeremy J. B.; Lee, Alex K. Y.; Thomas, Jennie L.; Blais, Marjolaine; Gosselin, Michel; Miller, Lisa A.; Papakyriakou, Tim; Willis, Megan D.; Liggio, John

2017-06-01

Summertime Arctic shipboard observations of oxygenated volatile organic compounds (OVOCs) such as organic acids, key precursors of climatically active secondary organic aerosol (SOA), are consistent with a novel source of OVOCs to the marine boundary layer via chemistry at the sea surface microlayer. Although this source has been studied in a laboratory setting, organic acid emissions from the sea surface microlayer have not previously been observed in ambient marine environments. Correlations between measurements of OVOCs, including high levels of formic acid, in the atmosphere (measured by an online high-resolution time-of-flight mass spectrometer) and dissolved organic matter in the ocean point to a marine source for the measured OVOCs. That this source is photomediated is indicated by correlations between the diurnal cycles of the OVOC measurements and solar radiation. In contrast, the OVOCs do not correlate with levels of isoprene, monoterpenes, or dimethyl sulfide. Results from box model calculations are consistent with heterogeneous chemistry as the source of the measured OVOCs. As sea ice retreats and dissolved organic carbon inputs to the Arctic increase, the impact of this source on the summer Arctic atmosphere is likely to increase. Globally, this source should be assessed in other marine environments to quantify its impact on OVOC and SOA burdens in the atmosphere, and ultimately on climate.
Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer.

Science.gov (United States)

Mungall, Emma L; Abbatt, Jonathan P D; Wentzell, Jeremy J B; Lee, Alex K Y; Thomas, Jennie L; Blais, Marjolaine; Gosselin, Michel; Miller, Lisa A; Papakyriakou, Tim; Willis, Megan D; Liggio, John

2017-06-13

Summertime Arctic shipboard observations of oxygenated volatile organic compounds (OVOCs) such as organic acids, key precursors of climatically active secondary organic aerosol (SOA), are consistent with a novel source of OVOCs to the marine boundary layer via chemistry at the sea surface microlayer. Although this source has been studied in a laboratory setting, organic acid emissions from the sea surface microlayer have not previously been observed in ambient marine environments. Correlations between measurements of OVOCs, including high levels of formic acid, in the atmosphere (measured by an online high-resolution time-of-flight mass spectrometer) and dissolved organic matter in the ocean point to a marine source for the measured OVOCs. That this source is photomediated is indicated by correlations between the diurnal cycles of the OVOC measurements and solar radiation. In contrast, the OVOCs do not correlate with levels of isoprene, monoterpenes, or dimethyl sulfide. Results from box model calculations are consistent with heterogeneous chemistry as the source of the measured OVOCs. As sea ice retreats and dissolved organic carbon inputs to the Arctic increase, the impact of this source on the summer Arctic atmosphere is likely to increase. Globally, this source should be assessed in other marine environments to quantify its impact on OVOC and SOA burdens in the atmosphere, and ultimately on climate.
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.
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.
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
Atmospheric chemistry and physics in the atmosphere of a developed megacity (London: an overview of the REPARTEE experiment and its conclusions

Directory of Open Access Journals (Sweden)

R. M. Harrison

2012-03-01

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

Science.gov (United States)

Chemical risk assessment is both time-consuming and difficult because it requires the assembly of data for chemicals generally distributed across multiple sources. The US EPA CompTox Chemistry Dashboard is a publicly accessible web-based application providing access to various da...
Open-source Software for Exoplanet Atmospheric Modeling

Science.gov (United States)

Cubillos, Patricio; Blecic, Jasmina; Harrington, Joseph

2018-01-01

I will present a suite of self-standing open-source tools to model and retrieve exoplanet spectra implemented for Python. These include: (1) a Bayesian-statistical package to run Levenberg-Marquardt optimization and Markov-chain Monte Carlo posterior sampling, (2) a package to compress line-transition data from HITRAN or Exomol without loss of information, (3) a package to compute partition functions for HITRAN molecules, (4) a package to compute collision-induced absorption, and (5) a package to produce radiative-transfer spectra of transit and eclipse exoplanet observations and atmospheric retrievals.

Atmospheric hydroxyl radical production from electronically excited NO2 and H2O.

Science.gov (United States)

Li, Shuping; Matthews, Jamie; Sinha, Amitabha

2008-03-21

Hydroxyl radicals are often called the "detergent" of the atmosphere because they control the atmosphere's capacity to cleanse itself of pollutants. Here, we show that the reaction of electronically excited nitrogen dioxide with water can be an important source of tropospheric hydroxyl radicals. Using measured rate data, along with available solar flux and atmospheric mixing ratios, we demonstrate that the tropospheric hydroxyl contribution from this source can be a substantial fraction (50%) of that from the traditional O(1D) + H2O reaction in the boundary-layer region for high solar zenith angles. Inclusion of this chemistry is expected to affect modeling of urban air quality, where the interactions of sunlight with emitted NOx species, volatile organic compounds, and hydroxyl radicals are central in determining the rate of ozone formation.
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
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
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)
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
Modified ensemble Kalman filter for nuclear accident atmospheric dispersion: prediction improved and source estimated.

Science.gov (United States)

Zhang, X L; Su, G F; Yuan, H Y; Chen, J G; Huang, Q Y

2014-09-15

Atmospheric dispersion models play an important role in nuclear power plant accident management. A reliable estimation of radioactive material distribution in short range (about 50 km) is in urgent need for population sheltering and evacuation planning. However, the meteorological data and the source term which greatly influence the accuracy of the atmospheric dispersion models are usually poorly known at the early phase of the emergency. In this study, a modified ensemble Kalman filter data assimilation method in conjunction with a Lagrangian puff-model is proposed to simultaneously improve the model prediction and reconstruct the source terms for short range atmospheric dispersion using the off-site environmental monitoring data. Four main uncertainty parameters are considered: source release rate, plume rise height, wind speed and wind direction. Twin experiments show that the method effectively improves the predicted concentration distribution, and the temporal profiles of source release rate and plume rise height are also successfully reconstructed. Moreover, the time lag in the response of ensemble Kalman filter is shortened. The method proposed here can be a useful tool not only in the nuclear power plant accident emergency management but also in other similar situation where hazardous material is released into the atmosphere. Copyright © 2014 Elsevier B.V. All rights reserved.
A Comparison between Predicted and Observed Atmospheric States and their Effects on Infrasonic Source Time Function Inversion at Source Physics Experiment 6

Science.gov (United States)

Aur, K. A.; Poppeliers, C.; Preston, L. A.

2017-12-01

The Source Physics Experiment (SPE) consists of a series of underground chemical explosions at the Nevada National Security Site (NNSS) designed to gain an improved understanding of the generation and propagation of physical signals in the near and far field. Characterizing the acoustic and infrasound source mechanism from underground explosions is of great importance to underground explosion monitoring. To this end we perform full waveform source inversion of infrasound data collected from the SPE-6 experiment at distances from 300 m to 6 km and frequencies up to 20 Hz. Our method requires estimating the state of the atmosphere at the time of each experiment, computing Green's functions through these atmospheric models, and subsequently inverting the observed data in the frequency domain to obtain a source time function. To estimate the state of the atmosphere at the time of the experiment, we utilize the Weather Research and Forecasting - Data Assimilation (WRF-DA) modeling system to derive a unified atmospheric state model by combining Global Energy and Water Cycle Experiment (GEWEX) Continental-scale International Project (GCIP) data and locally obtained sonde and surface weather observations collected at the time of the experiment. We synthesize Green's functions through these atmospheric models using Sandia's moving media acoustic propagation simulation suite (TDAAPS). These models include 3-D variations in topography, temperature, pressure, and wind. We compare inversion results using the atmospheric models derived from the unified weather models versus previous modeling results and discuss how these differences affect computed source waveforms with respect to observed waveforms at various distances. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia LLC, a wholly owned subsidiary of Honeywell International Inc. for the U.S. Department of Energy's National Nuclear
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 (NO_x. Results from these experiments suggest that the
Model analyses of atmospheric mercury: present air quality and effects of transpacific transport on the United States

Science.gov (United States)

Lei, H.; Liang, X.-Z.; Wuebbles, D. J.; Tao, Z.

2013-11-01

Atmospheric mercury is a toxic air and water pollutant that is of significant concern because of its effects on human health and ecosystems. A mechanistic representation of the atmospheric mercury cycle is developed for the state-of-the-art global climate-chemistry model, CAM-Chem (Community Atmospheric Model with Chemistry). The model simulates the emission, transport, transformation and deposition of atmospheric mercury (Hg) in three forms: elemental mercury (Hg(0)), reactive mercury (Hg(II)), and particulate mercury (PHg). Emissions of mercury include those from human, land, ocean, biomass burning and volcano related sources. Land emissions are calculated based on surface solar radiation flux and skin temperature. A simplified air-sea mercury exchange scheme is used to calculate emissions from the oceans. The chemistry mechanism includes the oxidation of Hg(0) in gaseous phase by ozone with temperature dependence, OH, H2O2 and chlorine. Aqueous chemistry includes both oxidation and reduction of Hg(0). Transport and deposition of mercury species are calculated through adapting the original formulations in CAM-Chem. The CAM-Chem model with mercury is driven by present meteorology to simulate the present mercury air quality during the 1999-2001 period. The resulting surface concentrations of total gaseous mercury (TGM) are then compared with the observations from worldwide sites. Simulated wet depositions of mercury over the continental United States are compared to the observations from 26 Mercury Deposition Network stations to test the wet deposition simulations. The evaluations of gaseous concentrations and wet deposition confirm a strong capability for the CAM-Chem mercury mechanism to simulate the atmospheric mercury cycle. The general reproduction of global TGM concentrations and the overestimation on South Africa indicate that model simulations of TGM are seriously affected by emissions. The comparison to wet deposition indicates that wet deposition patterns
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
Meso-scale modeling of air pollution transport/chemistry/deposition and its application

International Nuclear Information System (INIS)

Kitada, Toshihiro

2007-01-01

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

Science.gov (United States)

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

2017-10-01

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

International Nuclear Information System (INIS)

Donovan, Geoffrey H.; Jovan, Sarah E.; Gatziolis, Demetrios; Burstyn, Igor; Michael, Yvonne L.; Amacher, Michael C.; Monleon, Vicente J.

2016-01-01

Urban networks of air-quality monitors are often too widely spaced to identify sources of air pollutants, especially if they do not disperse far from emission sources. The objectives of this study were to test the use of moss bio-indicators to develop a fine-scale map of atmospherically-derived cadmium and to identify the sources of cadmium in a complex urban setting. We collected 346 samples of the moss Orthotrichum lyellii from deciduous trees in December, 2013 using a modified randomized grid-based sampling strategy across Portland, Oregon. We estimated a spatial linear model of moss cadmium levels and predicted cadmium on a 50 m grid across the city. Cadmium levels in moss were positively correlated with proximity to two stained-glass manufacturers, proximity to the Oregon–Washington border, and percent industrial land in a 500 m buffer, and negatively correlated with percent residential land in a 500 m buffer. The maps showed very high concentrations of cadmium around the two stained-glass manufacturers, neither of which were known to environmental regulators as cadmium emitters. In addition, in response to our findings, the Oregon Department of Environmental Quality placed an instrumental monitor 120 m from the larger stained-glass manufacturer in October, 2015. The monthly average atmospheric cadmium concentration was 29.4 ng/m"3, which is 49 times higher than Oregon's benchmark of 0.6 ng/m"3, and high enough to pose a health risk from even short-term exposure. Both stained-glass manufacturers voluntarily stopped using cadmium after the monitoring results were made public, and the monthly average cadmium levels precipitously dropped to 1.1 ng/m"3 for stained-glass manufacturer #1 and 0.67 ng/m"3 for stained-glass manufacturer #2. - Highlights: • Bio-indicators are a valid method for measuring atmospheric pollutants • We used moss to map atmospheric cadmium in Portland, Oregon • Using a spatial linear model, we identified two stained
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.
When API Mass Spectrometry Meets Super Atmospheric Pressure Ion Sources

Science.gov (United States)

Chen, Lee Chuin

2015-01-01

In a tutorial paper on the application of free-jet technique for API-MS, John Fenn mentioned that “…for a number of years and a number of reasons, it has been found advantageous in many situations to carry out the ionization process in gas at pressures up to 1000 Torr or more” (Int. J. Mass Spectrom. 200: 459–478, 2000). In fact, the first ESI mass spectrometer constructed by Yamashita and Fenn had a counter-flow curtain gas source at 1050 Torr (ca. 1.4 atm) to sweep away the neutral (J. Phys. Chem. 88: 4451–4459, 1984). For gaseous ionization using electrospray plume, theoretical analysis also shows that “super-atmospheric operation would be more preferable in space-charge-limited situations.”(Int. J. Mass Spectrom. 300: 182–193, 2011). However, electrospray and the corona-based chemical ion source (APCI) in most commercial instrument are basically operated under an atmospheric pressure ambient, perhaps out of the concern of safety, convenience and simplicity in maintenance. Running the ion source at pressure much higher than 1 atm is not so common, but had been done by a number of groups as well as in our laboratory. A brief review on these ion sources will be given in this paper. PMID:26819912
Source contributions to atmospheric fine carbon particle concentrations

Science.gov (United States)

Andrew Gray, H.; Cass, Glen R.

A Lagrangian particle-in-cell air quality model has been developed that facilitates the study of source contributions to atmospheric fine elemental carbon and fine primary total carbon particle concentrations. Model performance was tested using spatially and temporally resolved emissions and air quality data gathered for this purpose in the Los Angeles area for the year 1982. It was shown that black elemental carbon (EC) particle concentrations in that city were dominated by emissions from diesel engines including both on-highway and off-highway applications. Fine primary total carbon particle concentrations (TC=EC+organic carbon) resulted from the accumulation of small increments from a great variety of emission source types including both gasoline and diesel powered highway vehicles, stationary source fuel oil and gas combustion, industrial processes, paved road dust, fireplaces, cigarettes and food cooking (e.g. charbroilers). Strategies for black elemental carbon particle concentration control will of necessity need to focus on diesel engines, while controls directed at total carbon particle concentrations will have to be diversified over a great many source types.
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
Atmospheric deposition having been one of the major source of Pb in Jiaozhou Bay

Science.gov (United States)

Yang, Dongfang; Miao, Zhenqing; Zhang, Xiaolong; Wang, Qi; Li, Haixia

2018-03-01

Many marine bays have been polluted by Pb due to the rapid development of industry, and identifying the major source of Pb is essential to pollution control. This paper analyzed the distribution and pollution source of Pb in Jiaozhou Bay in 1988. Results showed that Pb contents in surface waters in Jiaozhou Bay in April, July and October 1988 were 5.52-24.61 μg L‑1, 7.66-38.62 μg L‑1 and 6.89-19.30 μg L‑1, respectively. The major Pb sources in this bay were atmospheric deposition, and marine current, whose source strengths were 19.30-24.61μg L‑1 and 38.62 μg L‑1, respectively. Atmospheric deposition had been one of the major Pb sources in Jiaozhou Bay, and the source strengths were stable and strong. The pollution level of Pb in this bay in 1988 was moderate to heavy, and the source control measurements were necessary.
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...
Direct observations of reactive atmospheric gases at ZOTTO station in the middle of Siberia as a base for large-scale modeling of atmospheric chemistry over Northern Eurasia

Science.gov (United States)

Skorokhod, Andrey; Belikov, Igor; Shtabkin, Yury; Moiseenko, Konstantin; Pankratova, Natalia; Vasileva, Anastasia; Rakitin, Vadim; Heimann, Martin

2015-04-01

Direct observations of atmospheric air composition are very important for a comprehensive understanding of atmospheric chemistry over Northern Eurasia and its variability and trends driven by abrupt climatic and ecosystem changes and anthropogenic pressure. Atmospheric air composition (including greenhouse gases and aerosols), its trends and variability is still insufficiently known for most of the nearly uninhabited areas of Northern Eurasia. This limits the accuracy of both global and regional models, which simulate climatological and ecosystem changes in this highly important region. From that point of view, the Zotino Tall Tower Observatory (ZOTTO) in the middle of Siberia (near 60N, 90E), launched in 2006 and governed by a scientific international consortium plays an important role providing unique information about concentrations of greenhouse and reactive trace gases, as well as aerosols. Simulations of surface concentrations of O3, NOx and CO performed by global chemical-transport model GEOS-Chem using up-to-date anthropogenic and biogenic emissions databases show very good agreement with values observed at ZOTTO in 2007-2012. Observed concentration of ozone has a pronounced seasonal variation with a clear peak in spring (40-45 ppbv in average and up to 80 ppbv in extreme cases) and minimum in winter. Average ozone level is about 20 ppbv that corresponds to the background conditions. Enhanced concentration in March-July is due to increased stratospheric-tropospheric exchange. In autumn and winter distribution of ozone is close to uniform. NOx concentration does not exceed 1 ppb that is typical for background areas but may vary by order and some more in few hours. Higher surface NOx(=NO+NO2) concentrations during day time generally correspond to higher ozone when NO/NO2 ratio indicates on clean or slightly polluted conditions. CO surface concentration has a vivid seasonal course and varies from about 100 ppb in summer till 150 ppb in winter. But during

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

Science.gov (United States)

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

2008-01-01

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

Science.gov (United States)

Tan, Ji-Hua; Duan, Jing-Chun; Ma, Yong-Liang; Yang, Fu-Mo; Cheng, Yuan; He, Ke-Bin; Yu, Yong-Chang; Wang, Jie-Wen

2014-09-15

Foshan is a ceramics manufacturing center in the world and the most polluted city in the Pearl River Delta (PRD) in southern China measured by the levels of atmospheric heavy metals. PM2.5 samples were collected in Foshan in winter 2008. Among the 22 elements and ions analyzed, 7 heavy metals (Zn, V, Mn, Cu, As, Cd and Pb) were studied in depth for their levels, spatiotemporal variations and sources. The ambient concentrations of the heavy metals were much higher than the reported average concentrations in China. The levels of Pb (675.7 ± 378.5 ng/m(3)), As (76.6 ± 49.1 ng/m(3)) and Cd (42.6 ± 45.2 ng/m(3)) exceeded the reference values of NAAQS (GB3095-2012) and the health guidelines of the World Health Organization. Generally, the levels of atmospheric heavy metals showed spatial distribution as: downtown site (CC, Chancheng District)>urban sites (NH and SD, Nanhai and Shunde Districts)>rural site (SS, Shanshui District). Two sources of heavy metals, the ceramic and aluminum industries, were identified during the sampling period. The large number of ceramic manufactures was responsible for the high levels of atmospheric Zn, Pb and As in Chancheng District. Transport from an aluminum industry park under light north-west winds contributed high levels of Cd to the SS site (Shanshui District). The average concentration of Cd under north-west wind was 220 ng/m(3), 20.5 times higher than those under other wind directions. The high daily maximum enrichment factors (EFs) of Cd, Pb, Zn, As and Cu at all four sites indicated extremely high contamination by local emissions. Back trajectory analysis showed that the heavy metals were also closely associated with the pathway of air mass. A positive matrix factorization (PMF) method was applied to determine the source apportionment of these heavy metals. Five factors (industry including the ceramic industry and coal combustion, vehicle emissions, dust, transportation and sea salt) were identified and industry was the most
Influence of iodine chemistry on source term assessment

International Nuclear Information System (INIS)

Herranz Puebla, L. E.; Lopez Diez, I.; Rodriguez Maroto, J. J.; Martinez Lopez-Alcorocho, A.

1991-01-01

The major goal of a phenomenology analysis of containment during a severe accident situation can be spitted into the following ones: to know the containment response to the different loads and to predict accurately the fission product and aerosol behavior. In this report, the main results coming from the study of a hypothetical accident scenario, based on LA-4 experiment of LACE project, are presented. In order to do it, several codes have been coupled: CONTEMPT4/MOD5 (thermohydraulics), NAUA/MOD5 (aerosol physics) and IODE (iodine chemistry). It has been demonstrated the impossibility of assessing with confidence the Source Term if the chemical conduct of some radionuclides is not taken into account. In particular, the influence on the iodine retention efficiency of the sump of variables such as pH has been proven. (Author)12 refs
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.
Trimethylsilyl derivatives of organic compounds in source samples and in atmospheric fine particulate matter.

Science.gov (United States)

Nolte, Christopher G; Schauer, James J; Cass, Glen R; Simoneit, Bernd R T

2002-10-15

Source sample extracts of vegetative detritus, motor vehicle exhaust, tire dust paved road dust, and cigarette smoke have been silylated and analyzed by GC-MS to identify polar organic compounds that may serve as tracers for those specific emission sources of atmospheric fine particulate matter. Candidate molecular tracers were also identified in atmospheric fine particle samples collected in the San Joaquin Valley of California. A series of normal primary alkanols, dominated by even carbon-numbered homologues from C26 to C32, the secondary alcohol 10-nonacosanol, and some phytosterols are prominent polar compounds in the vegetative detritus source sample. No new polar organic compounds are found in the motor vehicle exhaust samples. Several hydrogenated resin acids are present in the tire dust sample, which might serve as useful tracers for those sources in areas that are heavily impacted by motor vehicle traffic. Finally, the alcohol and sterol emission profiles developed for all the source samples examined in this project are scaled according to the ambient fine particle mass concentrations attributed to those sources by a chemical mass balance receptor model that was previously applied to the San Joaquin Valley to compute the predicted atmospheric concentrations of individual alcohols and sterols. The resulting underprediction of alkanol concentrations at the urban sites suggests that alkanols may be more sensitive tracers for natural background from vegetative emissions (i.e., waxes) than the high molecular weight alkanes, which have been the best previously available tracers for that source.
On the calculation of atmospheric thermal pollution resulted from a flat area source

International Nuclear Information System (INIS)

Perkauskas, D.Ch.; Senuta, K.A.

1984-01-01

A spatial distribution of thermal atmospheric pollution from a flat area source - a great city or a lake-cooler of NPP was investigated. The numerical solution obtained lets to evaluate the horizontal and vertical spreading of the thermal atmospheric pollution by the different wind velocities in dependence of the inhomogeneities in humidity of the earth's surface
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

not remain in the same form in the snow. Kinetic studies undertaken have demonstrated that bromine is the major oxidant depleting Hg in the atmosphere. Modeling results demonstrate that there is a significant deposition of Hg to Polar Regions as a result of AMDEs. Models have also shown that Hg is readily transported to the Arctic from source regions, at times during springtime when this environment is actively transforming Hg from the atmosphere to the snow and ice surfaces. The presence of significant amounts of methyl Hg in snow in the Arctic surrounding AMDEs is important because this species is the link between the environment and impacts to wildlife and humans. Further, much work on methylation and demethylation processes has occurred but these processes are not yet fully understood. Recent changes in the climate and sea ice cover in Polar Regions are likely to have strong effects on the cycling of Hg in this environment; however more research is needed to understand Hg processes in order to formulate meaningful predictions of these changes.
Synthetic fibers in atmospheric fallout: A source of microplastics in the environment?

Science.gov (United States)

Dris, Rachid; Gasperi, Johnny; Saad, Mohamed; Mirande, Cécile; Tassin, Bruno

2016-03-15

Sources, pathways and reservoirs of microplastics, plastic particles smaller than 5mm, remain poorly documented in an urban context. While some studies pointed out wastewater treatment plants as a potential pathway of microplastics, none have focused on the atmospheric compartment. In this work, the atmospheric fallout of microplastics was investigated in two different urban and sub-urban sites. Microplastics were collected continuously with a stainless steel funnel. Samples were then filtered and observed with a stereomicroscope. Fibers accounted for almost all the microplastics collected. An atmospheric fallout between 2 and 355 particles/m(2)/day was highlighted. Registered fluxes were systematically higher at the urban than at the sub-urban site. Chemical characterization allowed to estimate at 29% the proportion of these fibers being all synthetic (made with petrochemicals), or a mixture of natural and synthetic material. Extrapolation using weight and volume estimates of the collected fibers, allowed a rough estimation showing that between 3 and 10 tons of fibers are deposited by atmospheric fallout at the scale of the Parisian agglomeration every year (2500 km(2)). These results could serve the scientific community working on the different sources of microplastic in both continental and marine environments. Copyright © 2016 Elsevier Ltd. All rights reserved.
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.
Using an epiphytic moss to identify previously unknown sources of atmospheric cadmium pollution

Science.gov (United States)

Geoffrey H. Donovan; Sarah E. Jovan; Demetrios Gatziolis; Igor Burstyn; Yvonne L. Michael; Michael C. Amacher; Vicente J. Monleon

2016-01-01

Urban networks of air-quality monitors are often too widely spaced to identify sources of air pollutants, especially if they do not disperse far from emission sources. The objectives of this study were to test the use of moss bio-indicators to develop a fine-scale map of atmospherically-derived cadmium and to identify the sources of cadmium in a complex urban setting....
Pulsed, atmospheric pressure plasma source for emission spectrometry

Science.gov (United States)

Duan, Yixiang; Jin, Zhe; Su, Yongxuan

2004-05-11

A low-power, plasma source-based, portable molecular light emission generator/detector employing an atmospheric pressure pulsed-plasma for molecular fragmentation and excitation is described. The average power required for the operation of the plasma is between 0.02 W and 5 W. The features of the optical emission spectra obtained with the pulsed plasma source are significantly different from those obtained with direct current (dc) discharge higher power; for example, strong CH emission at 431.2 nm which is only weakly observed with dc plasma sources was observed, and the intense CN emission observed at 383-388 nm using dc plasma sources was weak in most cases. Strong CN emission was only observed using the present apparatus when compounds containing nitrogen, such as aniline were employed as samples. The present apparatus detects dimethylsulfoxide at 200 ppb using helium as the plasma gas by observing the emission band of the CH radical. When coupled with a gas chromatograph for separating components present in a sample to be analyzed, the present invention provides an apparatus for detecting the arrival of a particular component in the sample at the end of the chromatographic column and the identity thereof.
Using an epiphytic moss to identify previously unknown sources of atmospheric cadmium pollution

Energy Technology Data Exchange (ETDEWEB)

Donovan, Geoffrey H., E-mail: gdonovan@fs.fed.us [USDA Forest Service, PNW Research Station, 620 SW Main, Suite 400, Portland, OR 97205 (United States); Jovan, Sarah E., E-mail: sjovan@fs.fed.us [USDA Forest Service, PNW Research Station, 620 SW Main, Suite 400, Portland, OR 97205 (United States); Gatziolis, Demetrios, E-mail: dgatziolis@fs.fed.us [USDA Forest Service, PNW Research Station, 620 SW Main, Suite 400, Portland, OR 97205 (United States); Burstyn, Igor, E-mail: igor.burstyn@drexel.edu [Dornsife School of Public Health, Drexel University, Nesbitt Hall, 3215 Market St, Philadelphia, PA 19104 (United States); Michael, Yvonne L., E-mail: ylm23@drexel.edu [Dornsife School of Public Health, Drexel University, Nesbitt Hall, 3215 Market St, Philadelphia, PA 19104 (United States); Amacher, Michael C., E-mail: mcamacher1@outlook.com [USDA Forest Service, Logan Forest Sciences Laboratory, 860 North 1200 East, Logan, UT 84321 (United States); Monleon, Vicente J., E-mail: vjmonleon@fs.fed.us [USDA Forest Service, PNW Research Station, 3200 SW Jefferson Way, Corvallis, OR 97331 (United States)

2016-07-15

Urban networks of air-quality monitors are often too widely spaced to identify sources of air pollutants, especially if they do not disperse far from emission sources. The objectives of this study were to test the use of moss bio-indicators to develop a fine-scale map of atmospherically-derived cadmium and to identify the sources of cadmium in a complex urban setting. We collected 346 samples of the moss Orthotrichum lyellii from deciduous trees in December, 2013 using a modified randomized grid-based sampling strategy across Portland, Oregon. We estimated a spatial linear model of moss cadmium levels and predicted cadmium on a 50 m grid across the city. Cadmium levels in moss were positively correlated with proximity to two stained-glass manufacturers, proximity to the Oregon–Washington border, and percent industrial land in a 500 m buffer, and negatively correlated with percent residential land in a 500 m buffer. The maps showed very high concentrations of cadmium around the two stained-glass manufacturers, neither of which were known to environmental regulators as cadmium emitters. In addition, in response to our findings, the Oregon Department of Environmental Quality placed an instrumental monitor 120 m from the larger stained-glass manufacturer in October, 2015. The monthly average atmospheric cadmium concentration was 29.4 ng/m{sup 3}, which is 49 times higher than Oregon's benchmark of 0.6 ng/m{sup 3}, and high enough to pose a health risk from even short-term exposure. Both stained-glass manufacturers voluntarily stopped using cadmium after the monitoring results were made public, and the monthly average cadmium levels precipitously dropped to 1.1 ng/m{sup 3} for stained-glass manufacturer #1 and 0.67 ng/m{sup 3} for stained-glass manufacturer #2. - Highlights: • Bio-indicators are a valid method for measuring atmospheric pollutants • We used moss to map atmospheric cadmium in Portland, Oregon • Using a spatial linear model, we identified two
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.
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)
Ultrashort particle sources: innovating advances for chemistry and trans-disciplinary domains

International Nuclear Information System (INIS)

Malka, V.; Faure, J.; Glinec, Y.; Gauduel, Y.A.

2005-01-01

High-energy laser interaction with matter (gaseous and solid targets) provides electric fields going beyond the limit of one tera-volt per meter (1 TV = 10 12 V) and permit efficient acceleration of particles in the relativistic regime, typically with MeV energy. Exceptional properties of these new particle sources (shortness, charge, emittance) may conjecture trans-disciplinary researches such as physics' accelerators, pre-thermal reactivity in soft matter, radiobiology and radiotherapy, imaging. The challenge of high-energy femto-chemistry is broached in the framework of water, 'the life's solvent'. (authors)
2007 California Aerosol Study: Evaluation of δ15N as a Tracer Of NOx Sources and Chemsitry

Science.gov (United States)

Katzman, T. L.

2017-12-01

Although stable isotopes of N are commonly used as a source tracer, how this tracer is applied is a point of contention. The "source" hypothesis argues that the δ15N value of NO3- reflects the δ15N value of NOx source inputs into the environment, and any observed variation is solely the result of differences in source contributions. Conversely, the "chemistry" hypothesis argues that N isotopes are influenced by chemical reactions, atmospheric or biologic processing, and post-depositional effects. Previous studies often apply the source hypothesis, writing off the chemistry hypothesis as "minor," but others have noted the impact chemistry should has on δ15N values. Given the known complications, this work seeks to assess the use of stable isotopes as tracers, specifically, the assumption that the δ15N value is a tracer of source alone without significant influence from chemical reactions. If the "source" hypothesis is correct, source emission data, known source δ15N values, and isotope mass balance should be able to approximate measured δ15NNO3 values and determine the δ15N value associated with wildfire derived NOx, which is currently unknown. Significant deviations from observed values would support the significance of equilibrium and kinetic isotope effects associated with chemical reactions and processing in the atmosphere. Aerosols collected in during 2007, emission data, and isotopic analysis were utilized to determine the utility of δ15N as tracer of NOx sources. San Diego, California is a coastal urban area influenced by sea salt aerosols, anthropogenic combustion emissions, and seasonal wildfires. Wildfires also have a significant influence on local atmospheric chemistry and 2007 was notable for being one of the worst fire seasons in the San Diego region on record. Isotopic analysis of collected NO3- has suggested that source δ15N values are likely not conserved as NOx is oxidized into NO3-. Given known source contributions and known δ15N values
Emission, transmission, deposition and environmental effects of ammonia from agricultural sources

Energy Technology Data Exchange (ETDEWEB)

Erisman, J.W. [ECN Clean Fossil Fuels, Petten (Netherlands); Dammgen, U. [Federal Agricultural Research Centre, Institute of Agroecology, Braunschweig (Germany)

2005-05-01

Air pollution in Europe has been regarded as a severe problem for several decades, the adverse effects being: the influence on the physical properties of the atmosphere itself, in particular its energy balance (global warming), and visibility; the influence on atmospheric chemistry (formation and destruction of both ground level and stratospheric ozone); the input of chemicals into terrestrial and aquatic ecosystems causing acidification and eutrophication leading to forest decline as well as changes in ecosystem structure and function; the effects on human health and welfare (the respiratory system). Since the sulfur dioxide problem seems to have been solved to a large extent in most countries in Western Europe, atmospheric nitrogen compounds are considered a major source of acidification. As most natural and near-natural ecosystems have developed with nitrogen as a limiting factor, increased inputs of reactive atmospheric nitrogen cause changes in their structure, function and nutrient dynamics. These effects are attributed to surplus nutrition (eutrophication) of the respective systems as the result of increased nitrogen inputs. At first it seemed logical to connect them with sources similar to those for sulfur (power plants, combustion engines, domestic heating); however, it soon became clear that reduced nitrogen (ammonia and ammonium in particulates) also plays a major role. This review is to collate the present state of knowledge with regard to ammonia emissions, its atmospheric transport and chemistry as well as its deposition and the resulting effects. It restricts itself to a description of the situation in Europe.
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.

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.
Natural and anthropogenic sources and processes affecting water chemistry in two South Korean streams

Energy Technology Data Exchange (ETDEWEB)

Shin, Woo-Jin [Division of Earth and Environmental Sciences, Korea Basic Science Institute, Cheongwon-gun, Chungbuk 363-883 (Korea, Republic of); Department of Geoscience, University of Calgary, Calgary, Alberta T2N 1N4 (Canada); Ryu, Jong-Sik [Division of Earth and Environmental Sciences, Korea Basic Science Institute, Cheongwon-gun, Chungbuk 363-883 (Korea, Republic of); Mayer, Bernhard [Department of Geoscience, University of Calgary, Calgary, Alberta T2N 1N4 (Canada); Lee, Kwang-Sik, E-mail: kslee@kbsi.re.kr [Division of Earth and Environmental Sciences, Korea Basic Science Institute, Cheongwon-gun, Chungbuk 363-883 (Korea, Republic of); Lee, Sin-Woo [Division of Earth and Environmental Sciences, Korea Basic Science Institute, Cheongwon-gun, Chungbuk 363-883 (Korea, Republic of); Department of Geology, Chungnam National University, Yuseong-gu, Daejeon 305-764 (Korea, Republic of)

2014-07-01

Acid mine drainage (AMD) in a watershed provides potential sources of pollutants for surface and subsurface waters that can deteriorate water quality. Between March and early August 2011, water samples were collected from two streams in South Korea, one dominantly draining a watershed with carbonate bedrock affected by coal mines and another draining a watershed with silicate bedrock and a relatively undisturbed catchment area. The objective of the study was to identify the sources and processes controlling water chemistry, which was dependent on bedrock and land use. In the Odae stream (OS), the stream in the silicate-dominated catchment, Ca, Na, and HCO{sub 3} were the dominant ions and total dissolved solids (TDS) was low (26.1–165 mg/L). In the Jijang stream (JS), in the carbonate-dominated watershed, TDS (224–434 mg/L) and ion concentrations were typically higher, and Ca and SO{sub 4} were the dominant ions due to carbonate weathering and oxidation of pyrite exposed at coal mines. Dual isotopic compositions of sulfate (δ{sup 34}S{sub SO4} and δ{sup 18}O{sub SO4}) verified that the SO{sub 4} in JS is derived mainly from sulfide mineral oxidation in coal mines. Cl in JS was highest upstream and decreased progressively downstream, which implies that pollutants from recreational facilities in the uppermost part of the catchment are the major source governing Cl concentrations within the discharge basin. Dual isotopic compositions of nitrate (δ{sup 15}N{sub NO3} and δ{sup 18}O{sub NO3}) indicated that NO{sub 3} in JS is attributable to nitrification of soil organic matter but that NO{sub 3} in OS is derived mostly from manure. Additionally, the contributions of potential anthropogenic sources to the two streams were estimated in more detail by using a plot of δ{sup 34}S{sub SO4} and δ{sup 15}N{sub NO3}. This study suggests that the dual isotope approach for sulfate and nitrate is an excellent additional tool for elucidating the sources and processes
Natural and anthropogenic sources and processes affecting water chemistry in two South Korean streams

International Nuclear Information System (INIS)

Shin, Woo-Jin; Ryu, Jong-Sik; Mayer, Bernhard; Lee, Kwang-Sik; Lee, Sin-Woo

2014-01-01

Acid mine drainage (AMD) in a watershed provides potential sources of pollutants for surface and subsurface waters that can deteriorate water quality. Between March and early August 2011, water samples were collected from two streams in South Korea, one dominantly draining a watershed with carbonate bedrock affected by coal mines and another draining a watershed with silicate bedrock and a relatively undisturbed catchment area. The objective of the study was to identify the sources and processes controlling water chemistry, which was dependent on bedrock and land use. In the Odae stream (OS), the stream in the silicate-dominated catchment, Ca, Na, and HCO 3 were the dominant ions and total dissolved solids (TDS) was low (26.1–165 mg/L). In the Jijang stream (JS), in the carbonate-dominated watershed, TDS (224–434 mg/L) and ion concentrations were typically higher, and Ca and SO 4 were the dominant ions due to carbonate weathering and oxidation of pyrite exposed at coal mines. Dual isotopic compositions of sulfate (δ 34 S SO4 and δ 18 O SO4 ) verified that the SO 4 in JS is derived mainly from sulfide mineral oxidation in coal mines. Cl in JS was highest upstream and decreased progressively downstream, which implies that pollutants from recreational facilities in the uppermost part of the catchment are the major source governing Cl concentrations within the discharge basin. Dual isotopic compositions of nitrate (δ 15 N NO3 and δ 18 O NO3 ) indicated that NO 3 in JS is attributable to nitrification of soil organic matter but that NO 3 in OS is derived mostly from manure. Additionally, the contributions of potential anthropogenic sources to the two streams were estimated in more detail by using a plot of δ 34 S SO4 and δ 15 N NO3 . This study suggests that the dual isotope approach for sulfate and nitrate is an excellent additional tool for elucidating the sources and processes controlling the water chemistry of streams draining watersheds having different
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.
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.
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.
Locating the Source of Atmospheric Contamination Based on Data From the Kori Field Tracer Experiment

Directory of Open Access Journals (Sweden)

Piotr Kopka

2015-01-01

Full Text Available Accidental releases of hazardous material into the atmosphere pose high risks to human health and the environment. Thus it would be valuable to develop an emergency reaction system which can recognize the probable location of the source based only on concentrations of the released substance as reported by a network of sensors. We apply a methodology combining Bayesian inference with Sequential Monte Carlo (SMC methods to the problem of locating the source of an atmospheric contaminant. The input data for this algorithm are the concentrations of a given substance gathered continuously in time. We employ this algorithm to locating a contamination source using data from a field tracer experiment covering the Kori nuclear site and conducted in May 2001. We use the second-order Closure Integrated PUFF Model (SCIPUFF of atmospheric dispersion as the forward model to predict concentrations at the sensors' locations. We demonstrate that the source of continuous contamination may be successfully located even in the very complicated, hilly terrain surrounding the Kori nuclear site. (original abstract
Preparative radiation chemistry

International Nuclear Information System (INIS)

Drawe, H.

1978-01-01

Preparative synthesis of compounds with the aid of radiation chemistry is increasingly used in laboratories as well as on a technical scale. A large number of new compounds has been produced with the methods of radiation chemistry. With the increasing number of available radiation sources, also the number of synthesis metods in radiation chemistry has increased. This paper can only briefly mention the many possible ways of synthesis in radiation chemistry. (orig./HK) [de
Radiation Protection Aspects of Primary Water Chemistry and Source-term Management Report

International Nuclear Information System (INIS)

2014-04-01

Since the beginning of the 1990's, occupational exposures in nuclear power plant has strongly decreased, outlining efforts achieved by worldwide nuclear operators in order to reach and maintain occupational exposure as low as reasonably achievable (ALARA) in accordance with international recommendations and national regulations. These efforts have focused on both technical and organisational aspects. According to many radiation protection experts, one of the key features to reach this goal is the management of the primary system water chemistry and the ability to avoid dissemination of radioactivity within the system. It outlines the importance for radiation protection staff to work closely with chemistry staff (as well as operation staff) and thus to have sufficient knowledge to understand the links between chemistry and the generation of radiation field. This report was prepared with the primary objective to provide such knowledge to 'non-chemist'. The publication primarily focuses on three topics dealing with water chemistry, source term management and remediation techniques. One key objective of the report is to provide current knowledge regarding these topics and to address clearly related radiation protection issues. In that mind, the report prepared by the EGWC was also reviewed by radiation protection experts. In order to address various designs, PWRs, VVERs, PHWRs and BWRs are addressed within the document. Additionally, available information addressing current operating units and lessons learnt is outlined with choices that have been made for the design of new plants. Chapter 3 of this report addresses current practices regarding primary chemistry management for different designs, 'how to limit activity in the primary circuit and to minimise contamination'. General information is provided regarding activation, corrosion and transport of activated materials in the primary circuit (background on radiation field generation). Primary chemistry aspects that
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 ).
Carbon monoxide in jupiter's upper atmosphere: An extraplanetary source

International Nuclear Information System (INIS)

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

1978-01-01

Ablation of meteoroidal material in Jupiter's atmosphere may provide substantial quantities of H 2 O. Subsequent photochemistry can convert H 2 O and CH 4 to CO and H 2 . The associated source of CO could account for the observations by Beer, Larson, Fink, and Treffers, and Beer and Taylor, and would explain the relatively low rotational temperatures inferred by Beer and Taylor. Meteoritic debris might also provide spectroscopically detectable concentrations of SiO
Diffusion from a point source in an urban atmosphere

International Nuclear Information System (INIS)

Essa, K.S.M.; El-Otaify, M.S.

2005-01-01

In the present paper, a model for the diffusion of material from a point source in an urban atmosphere is incorporated. The plume is assumed to have a well-defined edge at which the concentration falls to zero. The vertical wind shear is estimated using logarithmic law, by employing most of the available techniques of stability categories. The concentrations estimated from the model were compared favorably with the field observations of other investigators
Source reconciliation of atmospheric gas-phase and particle-phase pollutants during a severe photochemical smog episode.

Science.gov (United States)

Schauer, James J; Fraser, Matthew P; Cass, Glen R; Simoneit, Bernd R T

2002-09-01

A comprehensive organic compound-based receptor model is developed that can simultaneously apportion the source contributions to atmospheric gas-phase organic compounds, semivolatile organic compounds, fine particle organic compounds, and fine particle mass. The model is applied to ambient data collected at four sites in the south coast region of California during a severe summertime photochemical smog episode, where the model determines the direct primary contributions to atmospheric pollutants from 11 distinct air pollution source types. The 11 sources included in the model are gasoline-powered motor vehicle exhaust, diesel engine exhaust, whole gasoline vapors, gasoline headspace vapors, organic solvent vapors, whole diesel fuel, paved road dust, tire wear debris, meat cooking exhaust, natural gas leakage, and vegetative detritus. Gasoline engine exhaust plus whole gasoline vapors are the predominant sources of volatile organic gases, while gasoline and diesel engine exhaust plus diesel fuel vapors dominate the emissions of semivolatile organic compounds from these sources during the episode studied at all four air monitoring sites. The atmospheric fine particle organic compound mass was composed of noticeable contributions from gasoline-powered motor vehicle exhaust, diesel engine exhaust, meat cooking, and paved road dust with smaller but quantifiable contributions from vegetative detritus and tire wear debris. In addition, secondary organic aerosol, which is formed from the low-vapor pressure products of gas-phase chemical reactions, is found to be a major source of fine particle organic compound mass under the severe photochemical smog conditions studied here. The concentrations of secondary organic aerosol calculated in the present study are compared with previous fine particle source apportionment results for less intense photochemical smog conditions. It is shown that estimated secondary organic aerosol concentrations correlate fairly well with the
Global inventory of NOx sources

International Nuclear Information System (INIS)

Delmas, R.; Serca, D.; Jambert, C.

1997-01-01

Nitrogen oxides are key compounds for the oxidation capacity of the troposphere. Their concentration depends on the proximity of sources because of their short atmospheric lifetime. An accurate knowledge of the distribution of their sources and sinks is therefore crucial. At the global scale, the dominant sources of nitrogen oxides - combustion of fossil fuel (about 50%) and biomass burning (about 20%) - are basically anthropogenic. Natural sources, including lightning and microbial activity in soils, represent therefore less than 30% of total emissions. Fertilizer use in agriculture constitutes an anthropogenic perturbation to the microbial source. The methods to estimate the magnitude and distribution of these dominant sources of nitrogen oxides are discussed. Some minor sources which may play a specific role in tropospheric chemistry such as NO x emission from aircraft in the upper troposphere or input from production in the stratosphere from N 2 O photodissociation are also considered
Investigation and Applications of In-Source Oxidation in Liquid Sampling-Atmospheric Pressure Afterglow Microplasma Ionization (LS-APAG) Source.

Science.gov (United States)

Xie, Xiaobo; Wang, Zhenpeng; Li, Yafeng; Zhan, Lingpeng; Nie, Zongxiu

2017-06-01

A liquid sampling-atmospheric pressure afterglow microplasma ionization (LS-APAG) source is presented for the first time, which is embedded with both electrospray ionization (ESI) and atmospheric pressure afterglow microplasma ionization (APAG) techniques. This ion source is capable of analyzing compounds with diverse molecule weights and polarities. An unseparated mixture sample was detected as a proof-of-concept, giving complementary information (both polarities and non-polarities) with the two ionization modes. It should also be noted that molecular mass can be quickly identified by ESI with clean and simple spectra, while the structure can be directly studied using APAG with in-source oxidation. The ionization/oxidation mechanism and applications of the LS-APAG source have been further explored in the analysis of nonpolar alkanes and unsaturated fatty acids/esters. A unique [M + O - 3H] + was observed in the case of individual alkanes (C 5 -C 19 ) and complex hydrocarbons mixture under optimized conditions. Moreover, branched alkanes generated significant in-source fragments, which could be further applied to the discrimination of isomeric alkanes. The technique also facilitates facile determination of double bond positions in unsaturated fatty acids/esters due to diagnostic fragments (the acid/ester-containing aldehyde and acid oxidation products) generated by on-line ozonolysis in APAG mode. Finally, some examples of in situ APAG analysis by gas sampling and surface sampling were given as well. Graphical Abstract ᅟ.
Source apportionment of atmospheric carbonaceous particulate matter based on the radiocarbon

International Nuclear Information System (INIS)

Guang-hua Wang; You-shi Zeng; Jian Yao; Yuan Qian; Ke Liu; Wei Liu; Yan Li; Yu Huang; University of South China, Hunan

2013-01-01

A method was established to quantitatively estimate sources of atmospheric carbonaceous matter, using a combination of radiocarbon technology, linear regression of organic carbon (OC) -K + and elemental carbon (EC) tracer method. Fractional contributions of fossil fuels, biomass burning, biogenic secondary organic carbon (BSOC) and soil dust to the atmospheric size-resolved carbonaceous matters in Shanghai suburb were estimated using this new method. The fossil carbon contributed most of the OC in particles smaller than 0.49 μm, and its fraction decreased with the increase of particle size. Biomass burning contributed 17-28 % to the OC. The BSOC contributed comparable proportions to the OC in particles smaller than 3.0 μm with the biomass burning, but larger in the particles lager than 3.0 μm. The soil dust contributed least fraction to the OC of each size with a proportion of 2-13 %. The biomass burning and fossil sources shared comparable fraction of the EC in all size range. (author)
Southwest Pacific deep water carbonate chemistry linked to high southern latitude climate and atmospheric CO2 during the Last Glacial Termination

Science.gov (United States)

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

2015-08-01

A greater amount of CO2 was stored in the deep sea during glacial periods, likely via greater efficiency of the biologic pump and increased uptake by a more alkaline ocean. Reconstructing past variations in seawater carbonate ion concentration (a major component of alkalinity) enables quantification of the relative roles of different oceanic CO2 storage mechanisms and also places constraints on the timing, magnitude, and location of subsequent deep ocean ventilation. Here, we present a record of deep-water inorganic carbon chemistry since the Last Glacial Maximum (LGM; ∼19-23 ka BP), derived from sediment core RR0503-83 raised from 1627 m in New Zealand's Bay of Plenty. The core site lies within the upper limit of southern-sourced Circumpolar Deep Water (CDW), just below the lower boundary of Antarctic Intermediate Water (AAIW). We reconstruct past changes in bottom water inorganic carbon chemistry from the trace element and stable isotopic composition of calcite shells of the epibenthic foraminifer Cibicidoides wuellerstorfi. A record of ΔCO32-(ΔCO32- = [COCO32-] in situ - [CO32-] saturation) derived from the foraminiferal boron to calcium ratio (B/Ca) provides evidence for greater ice-age storage of respired CO2 and reveals abrupt deglacial shifts in [CO32-] in situ of up to 30 μmol/kg (5 times larger than the difference between average LGM and Holocene values). The rapidity of these changes suggests the influence of changing water mass structure and atmospheric circulation in addition to a decrease in CO2 content of interior waters.
Iodine chemistry effect on source term assessments. A MELCOR 186 YT study of a PWR severe accident sequence

International Nuclear Information System (INIS)

Herranz, Luis E.; Garcia, Monica; Otero, Bernadette

2009-01-01

Level-2 Probabilistic Safety Analysis has demonstrated to be a powerful tool to give insights into multiple aspects concerning severe accidents: phenomena with the greatest potential to lead to containment failure, safety systems performance and, even, to identify any additional accident management that could mitigate the consequences of such an even, etc. A major result of level-2 PSA is iodine content in Source Term since it is the main responsible for the radiological impact during the first few days after a hypothetical severe accident. Iodine chemistry is known to considerably affect iodine behavior and although understanding has improved substantially since the early 90's, a thorough understanding is still missing and most PSA studies do not address it when assessing severe accident scenarios. This paper emphasizes the quantitative and qualitative significance of considering iodine chemistry in level-2 PSA estimates. To do so a cold leg break, low pressure severe accident sequence of an actual pressurized water reactor has been analyzed with the MELCOR 1.8.6 YT code. Two sets of calculations, with and without chemistry, have been carried out and compared. The study shows that iodine chemistry could result in an iodine release to environment about twice higher, most of which would consist of around 60% of iodine in gaseous form. From these results it is concluded that exploratory studies on the potential effect of iodine chemistry on source term estimates should be carried out. (author)
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.
Simple microwave plasma source at atmospheric pressure

International Nuclear Information System (INIS)

Kim, Jeong H.; Hong, Yong C.; Kim, Hyoung S.; Uhm, Han S.

2003-01-01

We have developed a thermal plasma source operating without electrodes. One electrodeless torch is the microwave plasma-torch, which can produce plasmas in large quantities. We can generate plasma at an atmospheric pressure by marking use of the same magnetrons used as commercial microwave ovens. Most of the magnetrons are operated at the frequency of 2.45 GHz; the magnetron power microwave is about 1kW. Electromagnetic waves from the magnetrons propagate through a shorted waveguide. Plasma was generated under a resonant condition, by an auxiliary ignition system. The plasma is stabilized by vortex stabilization. Also, a high-power and high-efficiency microwave plasma-torch has been operated in air by combining two microwave plasma sources with 1kW, 2.45 GHz. They are arranged in series to generate a high-power plasma flame. The second torch adds all its power to the plasma flame of the first torch. Basically, electromagnetic waves in the waveguide were studied by a High Frequency Structure Simulator (HFSS) code and preliminary experiments were conducted

Toward Synchronous Evaluation of Source Apportionments for Atmospheric Concentration and Deposition of Sulfate Aerosol Over East Asia

Science.gov (United States)

Itahashi, S.

2018-03-01

Source apportionments for atmospheric concentration, dry deposition, and wet deposition of sulfate aerosol (SO42-) were synchronously evaluated over East Asia, a main source of anthropogenic sulfur dioxide (SO2) emissions. Estimating dry deposition was difficult owing to the difficulty of measuring deposition velocity directly; therefore, sensitivity simulations using two dry deposition schemes were conducted. Moreover, sensitivity simulations for different emission inventories, the largest uncertainty source in the air quality model, were also conducted. In total, four experimental settings were used. Model performance was verified for atmospheric concentration and wet deposition using a ground-based observation network in China, Korea, and Japan, and all four model settings captured the observations. The underestimation of wet deposition over China was improved by an adjusted approach that linearly scaled the modeled precipitation values to observations. The synchronous evaluation of source apportionments for atmospheric concentration and dry and wet deposition showed the dominant contribution of anthropogenic emissions from China to the atmospheric concentration and deposition in Japan. The contributions of emissions from volcanoes were more important for wet deposition than for atmospheric concentration. Differences in the dry deposition scheme and emission inventory did not substantially influence the relative ratio of source apportionments over Japan. Because the dry deposition was more attributed to local factors, the differences in dry deposition may be an important determinant of the source contributions from China to Japan. Verification of these findings, including the dry deposition velocity, is necessary for better understanding of the behavior of sulfur compound in East Asia.
[Geochemical characteristics and sources of atmospheric particulates in Shanghai during dust storm event].

Science.gov (United States)

Qian, Peng; Zheng, Xiang-min; Zhou, Li-min

2013-05-01

Atmospheric particulates were sampled from three sampling sites of Putuo, Minhang and Qingpu Districts in Shanghai between Oct. , 2009 and Oct. , 2010. In addition, particulate samples were also collected from Nantong, Zhengzhou, Xi'an, and Beijing city where dust storm dust transported along during spring. Element compositions of atmospheric particulates were determined by XRF and ICP-MS. The concentrations of major and trace elements in atmospheric particulates from Putuo, Minhang and Qingpu Districts were similar, indicating their common source. The UCC standardization distribution map showed that the major element composition of dust storm samples was similar to that of loess in northwestern China, indicating that the dust storm dust was mainly derived from Western desert and partly from local area. The REE partition patterns of dust storm dusts among different cities along dust transport route were similar to each other, as well as to those of northern loess, which indicates that the dust storm samples may have the same material source as loess, which mainly comes from crust material. However, the REE partition patterns of non-dust storm particulates were different among the studied cities, and different from those of loess, which suggests that the non-dust storm samples may be mixed with non-crust source material, which is different from dust storm dust and loess. The major element composition and REE partition pattern are effective indicators for source tracing of dust storm dust.
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....
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.
Microplasma discharge vacuum ultraviolet photoionization source for atmospheric pressure ionization mass spectrometry.

Science.gov (United States)

Symonds, Joshua M; Gann, Reuben N; Fernández, Facundo M; Orlando, Thomas M

2014-09-01

In this paper, we demonstrate the first use of an atmospheric pressure microplasma-based vacuum ultraviolet (VUV) photoionization source in atmospheric pressure mass spectrometry applications. The device is a robust, easy-to-operate microhollow cathode discharge (MHCD) that enables generation of VUV photons from Ne and Ne/H(2) gas mixtures. Photons were detected by excitation of a microchannel plate detector and by analysis of diagnostic sample ions using a mass spectrometer. Reactive ions, charged particles, and metastables produced in the discharge were blocked from entering the ionization region by means of a lithium fluoride window, and photoionization was performed in a nitrogen-purged environment. By reducing the output pressure of the MHCD, we observed heightened production of higher-energy photons, making the photoionization source more effective. The initial performance of the MHCD VUV source has been evaluated by ionizing model analytes such as acetone, azulene, benzene, dimethylaniline, and glycine, which were introduced in solid or liquid phase. These molecules represent species with both high and low proton affinities, and ionization energies ranging from 7.12 to 9.7 eV.
Characterization of atmospheric emission sources in lichen from metal and organic contaminant patterns.

Science.gov (United States)

Ratier, Aude; Dron, Julien; Revenko, Gautier; Austruy, Annabelle; Dauphin, Charles-Enzo; Chaspoul, Florence; Wafo, Emmanuel

2018-03-01

Lichen samples from contrasted environments, influenced by various anthropic activities, were investigated focusing on the contaminant signatures according to the atmospheric exposure typologies. Most of the contaminant concentrations measured in the 27 lichen samples, collected around the industrial harbor of Fos-sur-Mer (France), were moderate in rural and urban environments, and reached extreme levels in industrial areas and neighboring cities (Al up to 6567 mg kg -1 , Fe 42,398 mg kg -1 , or ΣPAH 1417 μg kg -1 for example). At the same time, a strong heterogeneity was noticed in industrial samples while urban and rural ones were relatively homogeneous. Several metals could be associated to steel industry (Fe, Mn, Cd), road traffic, and agriculture (Sb, Cu, Sn), or to a distinct chemical installation (Mo). As well, PCDFs dominated in industrial samples while PCDDs prevailed in urban areas. The particularities observed supported the purpose of this work and discriminated the contributions of various atmospheric pollution emission sources in lichen samples. A statistical approach based on principal component analysis (PCA) was applied and resolved these potential singularities into specific component factors. Even if a certain degree of mixing of the factors is pointed out, relevant relationships were observed with several atmospheric emission sources. By this methodology, the contribution of industrial emissions to the atmospheric metal, PAH, PCB, and PCDD/F levels was roughly estimated to be 60.2%, before biomass burning (10.2%) and road traffic (3.8%). These results demonstrate that lichen biomonitoring offers an encouraging perspective of spatially resolved source apportionment studies.
The New Color of Chemistry: Green Chemistry

Directory of Open Access Journals (Sweden)

Zuhal GERÇEK

2012-01-01

Full Text Available Green chemistry which is the new application of chemistry rules provides solutions to problems that mankind is faced with climate changes, sustainable agriculture, energy, toxics, depletion of natural sources e.g. designing new chemicals and processes that production and utilization of hazardous matters. So, it is the indispensible tool for sustainable development. Current and future chemists should consider the human health and ecological issues in their professional life. In order to provide a solution for this requirement, green chemistry rules and under standings should be primarily taken in the university curriculum and at all educational levels.
Basalts as probes of planetary interiors: constraints on the chemistry and mineralogy of their source regions

International Nuclear Information System (INIS)

Bence, A.E.; Grove, T.L.; Papike, J.J.

1980-01-01

Basalt magmas, derived by the partial melting of planetary interiors, have compositions that reflect the pre-accretionary history of the material from which the planet formed, the planets, subsequent evolutionary history, the chemistry and mineralogy of the source regions, and the intensive thermodynamic parameters operating at the source and emplacement sites. Studies of basalt suites from the Earth, its Moon, and the eucrite parent body reveal compositional differences intrinsic to their source regions which are, in turn, a characteristic of the planet and its formational and evolutionary history. (Auth.)
Sources of atmospheric methane from coastal marine wetlands

International Nuclear Information System (INIS)

Harriss, R.C.; Sebacher, D.I.; Bartlett, K.B.; Bartlett, D.S.

1982-01-01

Biological methanogenesis in wetlands is believed to be one of the major sources of global tropospheric methane. The present paper reports measurements of methane distribution in the soils, sediments, water and vegetation of coastal marine wetlands. Measurements, carried out in the salt marshes Bay Tree Creek in Virginia and Panacea in northwest Florida, reveal methane concentrations in soils and sediments to vary with depth below the surface and with soil temperature. The fluxes of methane from marsh soils to the atmosphere at the soil-air interface are estimated to range from -0.00067 g CH 4 /sq m per day (methane sink) to 0.024 g CH 4 /sq m per day, with an average value of 0.0066 g CH 4 /sq m per day. Data also demonstrate the important role of tidal waters percolating through marsh soils in removing methane from the soils and releasing it to the atmosphere. The information obtained, together with previous studies, provides a framework for the design of a program based on in situ and remote sensing measurements to study the global methane cycle
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.
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
Coral reefs - sources or sinks of atmospheric CO[sub 2

Energy Technology Data Exchange (ETDEWEB)

Ware, J R; Smith, S V; Reakakudla, M L [Hawaii University, Honolulu, HI (USA). Dept. of Oceanography

1992-09-01

Because the precipitation of calcium carbonate results in the sequestering of carbon, it frequently has been thought that coral reefs function as sinks of global atmospheric CO[sub 2]. However, the precipitation of calcium carbonate is accompanied by a shift of pH that results in the release of CO[sub 2]. This release of CO[sub 2] is less in buffered sea water than fresh water systems; nevertheless, coral reefs are sources, not sinks, of atmospheric carbon. Using estimated rates of coral reef carbonate production, we compute that coral reefs release 0.02 to 0.08 Gt C as CO[sub 2] annually. This is approximately 0.4% to 1.4% of the current anthropogenic CO[sub 2] production due to fossil fuel combustion.
Quantification of air plasma chemistry for surface disinfection

International Nuclear Information System (INIS)

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

2014-01-01

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

Science.gov (United States)

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

2014-12-01

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

International Nuclear Information System (INIS)

Ferrara, R.; Mazzolai, B.; Edner, H.; Svanberg, S.; Wallinder, E.

1998-01-01

Mt. Amiata, located in southern Tuscany (Italy), is part of the geologic anomaly of the Mediterranean basin, which contains about 65% of the world's cinnabar (HgS) deposits. Atmospheric mercury emissions from the main sources (geothermal power plants, abandoned mine structures and spoil banks of roasted cinnabar ore) were determined by flux chamber and by LIDAR remote sensing. Mercury emissions from five geothermal power plants were on the order of 24 g h -1 for each plant, a value that remains constant throughout the year. In the month of July, the mine spoils (covering an area of =200000 m 2 ) emit a few grams of mercury per hour, while the abandoned mine structures give off 100-110 g h -1 . These two mercury sources were strongly influenced by ambient temperature. The area affected by mercury sources displays an average air mercury concentration of 20 ng m -3 during the summer and 10 ng m -3 in winter
Application of californium-252 neutron sources for analytical chemistry

International Nuclear Information System (INIS)

Ishii, Daido

1976-01-01

The researches made for the application of Cf-252 neutron sources to analytical chemistry during the period from 1970 to 1974 including partly 1975 are reviewed. The first part is the introduction to the above. The second part deals with general review of symposia, publications and the like. Attention is directed to ERDA publishing the periodical ''Californium-252 Progress'' and to a study group of Cf-252 utilization held by Japanese Radioisotope Association in 1974. The third part deals with its application for radio activation analysis. The automated absolute activation analysis (AAAA) of Savannha River is briefly explained. The joint experiment of Savannha River operation office with New Brunswick laboratory is mentioned. Cf-252 radiation source was used for the non-destructive analysis of elements in river water. East neutrons of Cf-252 were used for the quantitative analysis of lead in paints. Many applications for industrial control processes have been reported. Attention is drawn to the application of Cf-252 neutron sources for the field search of neutral resources. For example, a logging sonde for searching uranium resources was developed. the fourth part deals with the application of the analysis with gamma ray by capturing neutrons. For example, a bore hole sonde and the process control analysis of sulfur in fuel utilized capture gamma ray. The prompt gamma ray by capturing neutrons may be used for the nondestructive analysis of enrivonment. (Iwakiri, K.)
Bacteria in atmospheric waters: Detection, characteristics and implications

Science.gov (United States)

Hu, Wei; Niu, Hongya; Murata, Kotaro; Wu, Zhijun; Hu, Min; Kojima, Tomoko; Zhang, Daizhou

2018-04-01

In this review paper, we synthesize the current knowledges about bacteria in atmospheric waters, e.g., cloud, fog, rain, and snow, most of which were obtained very recently. First, we briefly describe the importance of bacteria in atmospheric waters, i.e., the essentiality of studying bacteria in atmospheric waters in understanding aerosol-cloud-precipitation-climate interactions in the Earth system. Next, approaches to collect atmospheric water samples for the detection of bacteria and methods to identify the bacteria are summarized and compared. Then the available data on the abundance, viability and community composition of bacteria in atmospheric waters are summarized. The average bacterial concentration in cloud water was usually on the order 104-105 cells mL-1, while that in precipitation on the order 103-104 cells mL-1. Most of the bacteria were viable or metabolically active. Their community composition was highly diverse and differed at various sites. Factors potentially influencing the bacteria, e.g., air pollution levels and sources, meteorological conditions, seasonal effect, and physicochemical properties of atmospheric waters, are described. After that, the implications of bacteria present in atmospheric waters, including their effect on nucleation in clouds, atmospheric chemistry, ecosystems and public health, are briefly discussed. Finally, based on the current knowledges on bacteria in atmospheric waters, which in fact remains largely unknown, we give perspectives that should be paid attention to in future studies.
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...
Uncertainties in United States agricultural N2O emissions: comparing forward model simulations to atmospheric N2O data.

Science.gov (United States)

Nevison, C. D.; Saikawa, E.; Dlugokencky, E. J.; Andrews, A. E.; Sweeney, C.

2014-12-01

Atmospheric N2O concentrations have increased from 275 ppb in the preindustrial to about 325 ppb in recent years, a ~20% increase with important implications for both anthropogenic greenhouse forcing and stratospheric ozone recovery. This increase has been driven largely by synthetic fertilizer production and other perturbations to the global nitrogen cycle associated with human agriculture. Several recent regional atmospheric inversion studies have quantified North American agricultural N2O emissions using top-down constraints based on atmospheric N2O data from the National Oceanic and Atmospheric Administration (NOAA) Global Greenhouse Gas Reference Network, including surface, aircraft and tall tower platforms. These studies have concluded that global N2O inventories such as EDGAR may be underestimating the true U.S. anthropogenic N2O source by a factor of 3 or more. However, simple back-of-the-envelope calculations show that emissions of this magnitude are difficult to reconcile with the basic constraints of the global N2O budget. Here, we explore some possible reasons why regional atmospheric inversions might overestimate the U.S. agricultural N2O source. First, the seasonality of N2O agricultural sources is not well known, but can have an important influence on inversion results, particularly when the inversions are based on data that are concentrated in the spring/summer growing season. Second, boundary conditions can strongly influence regional inversions but the boundary conditions used may not adequately account for remote influences on surface data such as the seasonal stratospheric influx of N2O-depleted air. We will present a set of forward model simulations, using the Community Land Model (CLM) and two atmospheric chemistry tracer transport models, MOZART and the Whole Atmosphere Community Climate Model (WACCM), that examine the influence of terrestrial emissions and atmospheric chemistry and dynamics on atmospheric variability in N2O at U.S. and
Control of emissions from stationary combustion sources: Pollutant detection and behavior in the atmosphere

International Nuclear Information System (INIS)

Licht, W.; Engel, A.J.; Slater, S.M.

1979-01-01

Stationary combustion resources continue to be significant sources of NOx and SOx pollutants in the ambient atmosphere. This volume considers four problem areas: (1) control of emissions from stationary combustion sources, particularly SOx and NOx (2) pollutant behavior in the atmosphere (3) advances in air pollution analysis and (4) air quality management. Topics of interest include carbon slurries for sulfur dioxide abatement, mass transfer in the Kellogg-Weir air quality control system, oxidation/inhibition of sulfite ion in aqueous solution, some micrometeorological methods of measuring dry deposition rates, Spanish moss as an indicator of airborne metal contamination, and air quality impacts from future electric power generation in Texas

Search for atmospheric muon-neutrinos and extraterrestric neutrino point sources in the 1997 AMANDA-B10 data

International Nuclear Information System (INIS)

Biron von Curland, A.

2002-07-01

The young field of high energy neutrino astronomy can be motivated by the search for the origin of the charged cosmic rays. Large astrophysical objects like AGNs or supernova remnants are candidates to accelerate hadrons which then can interact to eventually produce high energy neutrinos. Neutrino-induced muons can be detected via their emission of Cherenkov light in large neutrino telescopes like AMANDA. More than 10 9 atmospheric muon events and approximately 5000 atmospheric neutrino events were registered by AMANDA-B10 in 1997. Out of these, 223 atmospheric neutrino candidate events have been extracted. This data set contains approximately 15 background events. It allows to confirm the expected sensitivity of the detector towards neutrino events. A second set containing 369 (approximately 270 atmospheric neutrino events and 100 atmospheric muon events) was used to search for extraterrestrial neutrino point sources. Neither a binned search, nor a cluster search, nor a search for preselected sources gave indications for the existence of a strong neutrino point source. Based on this result, flux limits were derived. Assuming E ν -2 spectra, typical flux limits for selected sources of the order of Φ μ limit ∝ 10 -14 cm -2 s -1 for muons and Φ ν limit ∝ 10 -7 cm -2 s -1 for neutrinos have been obtained. (orig.)
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
Characterisation of the photolytic HONO-source in the atmosphere simulation chamber SAPHIR

Directory of Open Access Journals (Sweden)

F. Rohrer

2005-01-01

Full Text Available HONO formation has been proposed as an important OH radical source in simulation chambers for more than two decades. Besides the heterogeneous HONO formation by the dark reaction of NO2 and adsorbed water, a photolytic source has been proposed to explain the elevated reactivity in simulation chamber experiments. However, the mechanism of the photolytic process is not well understood so far. As expected, production of HONO and NOx was also observed inside the new atmospheric simulation chamber SAPHIR under solar irradiation. This photolytic HONO and NOx formation was studied with a sensitive HONO instrument under reproducible controlled conditions at atmospheric concentrations of other trace gases. It is shown that the photolytic HONO source in the SAPHIR chamber is not caused by NO2 reactions and that it is the only direct NOy source under illuminated conditions. In addition, the photolysis of nitrate which was recently postulated for the observed photolytic HONO formation on snow, ground, and glass surfaces, can be excluded in the chamber. A photolytic HONO source at the surface of the chamber is proposed which is strongly dependent on humidity, on light intensity, and on temperature. An empirical function describes these dependencies and reproduces the observed HONO formation rates to within 10%. It is shown that the photolysis of HONO represents the dominant radical source in the SAPHIR chamber for typical tropospheric O3/H2O concentrations. For these conditions, the HONO concentrations inside SAPHIR are similar to recent observations in ambient air.
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.
The New Color of Chemistry: Green Chemistry

OpenAIRE

Zuhal GERÇEK

2012-01-01

Green chemistry which is the new application of chemistry rules provides solutions to problems that mankind is faced with climate changes, sustainable agriculture, energy, toxics, depletion of natural sources e.g. designing new chemicals and processes that production and utilization of hazardous matters. So, it is the indispensible tool for sustainable development. Current and future chemists should consider the human health and ecological issues in their professional life. In order to provid...
Emission of nitrous acid from soil and biological soil crusts as a major source of atmospheric HONO on Cyprus

Science.gov (United States)

Meusel, Hannah; Tamm, Alexandra; Wu, Dianming; Kuhn, Uwe; Leifke, Anna-Lena; Weber, Bettina; Su, Hang; Lelieveld, Jos; Hoffmann, Thorsten; Pöschl, Ulrich; Cheng, Yafang

2017-04-01

Elucidation of the sources and atmospheric chemistry of nitrous acid (HONO) is highly relevant, as HONO is an important precursor of OH radicals. Up to 30% of the OH budget are formed by photolysis of HONO, whereas major fractions of HONO measured in the field derive from yet unidentified sources. Heterogeneous conversion of nitrogen dioxide (NO2) to HONO on a variety of surfaces (soot, humic acid aerosol) is assumed to be a major HONO source (Stemmler et al., 2007, Ammann et al., 1998). In rural regions, however, NO2 concentrations were found to be too low to explain observed HONO concentrations, as e.g., in the case of a recent field study on the Mediterranean island of Cyprus (Meusel et al., 2016). In this study a good correlation between missing sources of HONO and nitrogen oxide (NO) was found indicating a common origin of both reactive nitrogen compounds. Simultaneous emission of HONO and NO from soil was reported earlier (Oswald et al., 2013), and enhanced emission rates were found when soil was covered by biological soil crusts in arid and semi-arid ecosystems (Weber et al., 2015). In the present study we measured HONO and NO emissions of 43 soil and soil crust samples from Cyprus during full wetting and drying cycles under controlled laboratory conditions by means of a dynamic chamber system. The observed range of HONO and NO emissions was in agreement with earlier studies, but unlike the study of Weber et al. (2015), we found highest emission from bare soil, followed by soil covered by light and dark cyanobacteria-dominated biological soil crusts. Emission rates correlated well with the nitrite and nitrate contents of soil and biological soil crust samples, and higher nutrient contents of bare soil samples, as compared to the previous biological soil crust study, explain the higher bare soil emissions. Integrating the emission rates of bare soil and the different types of biological soil crusts, based on their local relative abundance, the calculated
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.
Critical assessment of the current state of scientific knowledge, terminology, and research needs concerning the role of organic aerosols in the atmosphere, climate, and global change

OpenAIRE

Fuzzi, S.; Andreae, M. O.; Huebert, B. J.; Kulmala, M.; Bond, T. C.; Boy, M.; Doherty, S. J.; Guenther, A.; Kanakidou, M.; Kawamura, K.; Kerminen, V.-M.; Lohmann, U.; Russell, L. M.; Pöschl, U.

2006-01-01

International audience; In spite of impressive advances in recent years, our present understanding of organic aerosol (OA) composition, physical and chemical properties, sources and transformation characteristics is still rather limited, and their environmental effects remain highly uncertain. Therefore, the three atmosphere-related projects of the International Geosphere Biosphere Programme (IGBP) ? IGAC (International Global Atmospheric Chemistry Project), iLEAPS (Integrated Land Ecosystem ...
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/
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
Transport of Chemical Vapors from Subsurface Sources to Atmosphere as Affected by Shallow Subsurface and Atmospheric Conditions

Science.gov (United States)

Rice, A. K.; Smits, K. M.; Hosken, K.; Schulte, P.; Illangasekare, T. H.

2012-12-01

Understanding the movement and modeling of chemical vapor through unsaturated soil in the shallow subsurface when subjected to natural atmospheric thermal and mass flux boundary conditions at the land surface is of importance to applications such as landmine detection and vapor intrusion into subsurface structures. New, advanced technologies exist to sense chemical signatures at the land/atmosphere interface, but interpretation of these sensor signals to make assessment of source conditions remains a challenge. Chemical signatures are subject to numerous interactions while migrating through the unsaturated soil environment, attenuating signal strength and masking contaminant source conditions. The dominant process governing movement of gases through porous media is often assumed to be Fickian diffusion through the air phase with minimal or no quantification of other processes contributing to vapor migration, such as thermal diffusion, convective gas flow due to the displacement of air, expansion/contraction of air due to temperature changes, temporal and spatial variations of soil moisture and fluctuations in atmospheric pressure. Soil water evaporation and interfacial mass transfer add to the complexity of the system. The goal of this work is to perform controlled experiments under transient conditions of soil moisture, temperature and wind at the land/atmosphere interface and use the resulting dataset to test existing theories on subsurface gas flow and iterate between numerical modeling efforts and experimental data. Ultimately, we aim to update conceptual models of shallow subsurface vapor transport to include conditionally significant transport processes and inform placement of mobile sensors and/or networks. We have developed a two-dimensional tank apparatus equipped with a network of sensors and a flow-through head space for simulation of the atmospheric interface. A detailed matrix of realistic atmospheric boundary conditions was applied in a series of
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...
Optimizing best management practices to control anthropogenic sources of atmospheric phosphorus deposition to inland lakes.

Science.gov (United States)

Weiss, Lee; Thé, Jesse; Winter, Jennifer; Gharabaghi, Bahram

2018-04-18

Excessive phosphorus loading to inland freshwater lakes around the globe has resulted in nuisance plant growth along the waterfronts, degraded habitat for cold water fisheries, and impaired beaches, marinas and waterfront property. The direct atmospheric deposition of phosphorus can be a significant contributing source to inland lakes. The atmospheric deposition monitoring program for Lake Simcoe, Ontario indicates roughly 20% of the annual total phosphorus load (2010-2014 period) is due to direct atmospheric deposition (both wet and dry deposition) on the lake. This novel study presents a first-time application of the Genetic Algorithm (GA) methodology to optimize the application of best management practices (BMPs) related to agriculture and mobile sources to achieve atmospheric phosphorus reduction targets and restore the ecological health of the lake. The novel methodology takes into account the spatial distribution of the emission sources in the airshed, the complex atmospheric long-range transport and deposition processes, cost and efficiency of the popular management practices and social constraints related to the adoption of BMPs. The optimization scenarios suggest that the optimal overall capital investment of approximately $2M, $4M, and $10M annually can achieve roughly 3, 4 and 5 tonnes reduction in atmospheric P load to the lake, respectively. The exponential trend indicates diminishing returns for the investment beyond roughly $3M per year and that focussing much of this investment in the upwind, nearshore area will significantly impact deposition to the lake. The optimization is based on a combination of the lowest-cost, most-beneficial and socially-acceptable management practices that develops a science-informed promotion of implementation/BMP adoption strategy. The geospatial aspect to the optimization (i.e. proximity and location with respect to the lake) will help land managers to encourage the use of these targeted best practices in areas that
Degradation of the Neonicotinoid Pesticides in the Atmospheric Pressure Ionization Source

Science.gov (United States)

Chai, Yunfeng; Chen, Hongping; Liu, Xin; Lu, Chengyin

2018-02-01

During the analysis of neonicotinoid pesticide standards (thiamethoxam, clothianidin, imidacloprid, acetamiprid, and thiacloprid) by mass spectrometry, the degradation of these pesticides (M-C=N-R is degraded into M-C=O, M is the skeleton moiety, and R is NO2 or CN) was observed in the atmospheric pressure ionization interfaces (ESI and APCI). In APCI, the degradation of all the five neonicotinoid pesticides studied took place, and the primary mechanism was in-source ion/molecule reaction, in which a molecule of water (confirmed by use of H2 18O) attacked the carbon of the imine group accompanying with loss of NH2R (R=NO2, CN). For the nitroguanidine neonicotinoid pesticides (R=NO2, including thiamethoxam, clothianidin, and imidacloprid), higher auxiliary gas heater temperature also contributed to their degradation in APCI due to in-source pyrolysis. The degradation of the five neonicotinoid pesticides studied in ESI was not significant. In ESI, only the nitroguanidine neonicotinoid pesticides could generate the degradation products through in-source fragmentation mechanism. The degradation of cyanoamidine neonicotinoid pesticides (R=CN, including acetamiprid and thiacloprid) in ESI was not observed. The degradation of neonicotinoid pesticides in the ion source of mass spectrometer renders some adverse consequences, such as difficulty interpreting the full-scan mass spectrum, reducing the sensitivity and accuracy of quantitative analysis, and misleading whether these pesticides have degraded in the real samples. Therefore, a clear understanding of these unusual degradation reactions should facilitate the analysis of neonicotinoid pesticides by atmospheric pressure ionization mass spectrometry.
Degradation of the Neonicotinoid Pesticides in the Atmospheric Pressure Ionization Source.

Science.gov (United States)

Chai, Yunfeng; Chen, Hongping; Liu, Xin; Lu, Chengyin

2018-02-01

During the analysis of neonicotinoid pesticide standards (thiamethoxam, clothianidin, imidacloprid, acetamiprid, and thiacloprid) by mass spectrometry, the degradation of these pesticides (M-C=N-R is degraded into M-C=O, M is the skeleton moiety, and R is NO 2 or CN) was observed in the atmospheric pressure ionization interfaces (ESI and APCI). In APCI, the degradation of all the five neonicotinoid pesticides studied took place, and the primary mechanism was in-source ion/molecule reaction, in which a molecule of water (confirmed by use of H 2 18 O) attacked the carbon of the imine group accompanying with loss of NH 2 R (R=NO 2 , CN). For the nitroguanidine neonicotinoid pesticides (R=NO 2 , including thiamethoxam, clothianidin, and imidacloprid), higher auxiliary gas heater temperature also contributed to their degradation in APCI due to in-source pyrolysis. The degradation of the five neonicotinoid pesticides studied in ESI was not significant. In ESI, only the nitroguanidine neonicotinoid pesticides could generate the degradation products through in-source fragmentation mechanism. The degradation of cyanoamidine neonicotinoid pesticides (R=CN, including acetamiprid and thiacloprid) in ESI was not observed. The degradation of neonicotinoid pesticides in the ion source of mass spectrometer renders some adverse consequences, such as difficulty interpreting the full-scan mass spectrum, reducing the sensitivity and accuracy of quantitative analysis, and misleading whether these pesticides have degraded in the real samples. Therefore, a clear understanding of these unusual degradation reactions should facilitate the analysis of neonicotinoid pesticides by atmospheric pressure ionization mass spectrometry. Graphical Abstract.
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.
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
Proposal of a stationary model of dispersion diagnoses of pollutants chemically non-reactivate, applied for mobile sources in Bogota

International Nuclear Information System (INIS)

Ruiz Murcia, Jose Franklln; Pabon Caicedo, Jose Daniel

2002-01-01

The following document presents a semi empirical model to calculate concentrations of monoxide of carbon in surface by mobile sources. This model considers three basic components: meteorology, emissions and atmospheric chemistry. Scientifically, the propose model is sustained en the fact that the quality of the air depends of the weather's conditions and the numbers of source that is emitting
Methods of gas purification and effect on the ion composition in an RF atmospheric pressure plasma jet investigated by mass spectrometry

International Nuclear Information System (INIS)

Grosse-Kreul, Simon; Huebner, Simon; Schneider, Simon; Keudell, Achim von; Benedikt, Jan

2016-01-01

The analysis of the ion chemistry of atmospheric pressure plasmas is essential to evaluate ionic reaction pathways during plasma-surface or plasma-analyte interactions. In this contribution, the ion chemistry of a radio-frequency atmospheric pressure plasma jet (μ-APPJ) operated in helium is investigated by mass spectrometry (MS). It is found, that the ion composition is extremely sensitive to impurities such as N 2 , O 2 and H 2 O. Without gas purification, protonated water cluster ions of the form H + (H 2 O) n are dominating downstream the positive ion mass spectrum. However, even after careful feed gas purification to the sub-ppm level using a molecular sieve trap and a liquid nitrogen trap as well as operation of the plasma in a controlled atmosphere, the positive ion mass spectrum is strongly influenced by residual trace gases. The observations support the idea that species with a low ionization energy serve as a major source of electrons in atmospheric pressure helium plasmas. Similarly, the neutral density of atomic nitrogen measured by MS in a He/N 2 mixture is varying up to a factor 3, demonstrating the significant influence of impurities on the neutral species chemistry as well. (orig.)
Methods of gas purification and effect on the ion composition in an RF atmospheric pressure plasma jet investigated by mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Grosse-Kreul, Simon; Huebner, Simon; Schneider, Simon; Keudell, Achim von; Benedikt, Jan [Ruhr-Universitaet Bochum, Institute for Experimental Physics II, Bochum (Germany)

2016-12-15

The analysis of the ion chemistry of atmospheric pressure plasmas is essential to evaluate ionic reaction pathways during plasma-surface or plasma-analyte interactions. In this contribution, the ion chemistry of a radio-frequency atmospheric pressure plasma jet (μ-APPJ) operated in helium is investigated by mass spectrometry (MS). It is found, that the ion composition is extremely sensitive to impurities such as N{sub 2}, O{sub 2} and H{sub 2}O. Without gas purification, protonated water cluster ions of the form H{sup +}(H{sub 2}O){sub n} are dominating downstream the positive ion mass spectrum. However, even after careful feed gas purification to the sub-ppm level using a molecular sieve trap and a liquid nitrogen trap as well as operation of the plasma in a controlled atmosphere, the positive ion mass spectrum is strongly influenced by residual trace gases. The observations support the idea that species with a low ionization energy serve as a major source of electrons in atmospheric pressure helium plasmas. Similarly, the neutral density of atomic nitrogen measured by MS in a He/N{sub 2} mixture is varying up to a factor 3, demonstrating the significant influence of impurities on the neutral species chemistry as well. (orig.)

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…
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
Seasonal variations in the sources of natural and anthropogenic lead deposited at the East Rongbuk Glacier in the high-altitude Himalayas

International Nuclear Information System (INIS)

Burn-Nunes, Laurie; Vallelonga, Paul; Lee, Khanghyun; Hong, Sungmin; Burton, Graeme; Hou, Shugui; Moy, Andrew; Edwards, Ross; Loss, Robert; Rosman, Kevin

2014-01-01

Lead (Pb) isotopic compositions and concentrations, and barium (Ba) and indium (In) concentrations have been analysed at sub-annual resolution in three sections from a < 110 m ice core dated to the 18th and 20th centuries, as well as snow pit samples dated to 2004/2005, recovered from the East Rongbuk Glacier in the high-altitude Himalayas. Ice core sections indicate that atmospheric chemistry prior to ∼ 1953 was controlled by mineral dust inputs, with no discernible volcanic or anthropogenic contributions. Eighteenth century monsoon ice core chemistry is indicative of dominant contributions from local Himalayan sources; non-monsoon ice core chemistry is linked to contributions from local (Himalayan), regional (Indian/Thar Desert) and long-range (North Africa, Central Asia) sources. Twentieth century monsoon and non-monsoon ice core data demonstrate similar seasonal sources of mineral dust, however with a transition to less-radiogenic isotopic signatures that suggests local and regional climate/environmental change. The snow pit record demonstrates natural and anthropogenic contributions during both seasons, with increased anthropogenic influence during non-monsoon times. Monsoon anthropogenic inputs are most likely sourced to South/South-East Asia and/or India, whereas non-monsoon anthropogenic inputs are most likely sourced to India and Central Asia. - Highlights: • Pb isotopes in ice and snow show seasonality in Mt Everest atmospheric chemistry. • Local (Himalayan) mineral dust inputs are present year round. • Regional and long-range mineral dust inputs are evident during non-monsoon times. • Snow samples indicate increased anthropogenic inputs during non-monsoon times. • Anthropogenic inputs are linked with Indian, South Asian and Central Asian sources
Seasonal variations in the sources of natural and anthropogenic lead deposited at the East Rongbuk Glacier in the high-altitude Himalayas

Energy Technology Data Exchange (ETDEWEB)

Burn-Nunes, Laurie, E-mail: L.Nunes@curtin.edu.au [Department of Imaging and Applied Physics, Curtin University, GPO Box U 1987, Perth 6845, Western Australia (Australia); Vallelonga, Paul [Centre for Ice and Climate, Niels Bohr Institute, University of Copenhagen, Juliane Maries Vej 30, DK-2100 Copenhagen Ø (Denmark); Lee, Khanghyun [Environmental Measurement and Analysis Center, National Institute of Environmental Research, Environmental Research Complex, Kyungseo-dong, Seo-gu, Incheon 404-170 (Korea, Republic of); Hong, Sungmin [Department of Ocean Sciences, Inha University, 100 Inha-ro, Nam-gu, Incheon 402-751 (Korea, Republic of); Burton, Graeme [Department of Imaging and Applied Physics, Curtin University, GPO Box U 1987, Perth 6845, Western Australia (Australia); Hou, Shugui [Key Laboratory of Coast and Island development of Ministry of Education, School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210093 (China); Moy, Andrew [Department of the Environment, Australian Antarctic Division, Channel Highway, Kingston 7050, Tasmania (Australia); Antarctic Climate and Ecosystems Cooperative Research Centre, University of Tasmania, Private Bag 80, Hobart 7001, Tasmania (Australia); Edwards, Ross; Loss, Robert; Rosman, Kevin [Department of Imaging and Applied Physics, Curtin University, GPO Box U 1987, Perth 6845, Western Australia (Australia)

2014-07-01

Lead (Pb) isotopic compositions and concentrations, and barium (Ba) and indium (In) concentrations have been analysed at sub-annual resolution in three sections from a < 110 m ice core dated to the 18th and 20th centuries, as well as snow pit samples dated to 2004/2005, recovered from the East Rongbuk Glacier in the high-altitude Himalayas. Ice core sections indicate that atmospheric chemistry prior to ∼ 1953 was controlled by mineral dust inputs, with no discernible volcanic or anthropogenic contributions. Eighteenth century monsoon ice core chemistry is indicative of dominant contributions from local Himalayan sources; non-monsoon ice core chemistry is linked to contributions from local (Himalayan), regional (Indian/Thar Desert) and long-range (North Africa, Central Asia) sources. Twentieth century monsoon and non-monsoon ice core data demonstrate similar seasonal sources of mineral dust, however with a transition to less-radiogenic isotopic signatures that suggests local and regional climate/environmental change. The snow pit record demonstrates natural and anthropogenic contributions during both seasons, with increased anthropogenic influence during non-monsoon times. Monsoon anthropogenic inputs are most likely sourced to South/South-East Asia and/or India, whereas non-monsoon anthropogenic inputs are most likely sourced to India and Central Asia. - Highlights: • Pb isotopes in ice and snow show seasonality in Mt Everest atmospheric chemistry. • Local (Himalayan) mineral dust inputs are present year round. • Regional and long-range mineral dust inputs are evident during non-monsoon times. • Snow samples indicate increased anthropogenic inputs during non-monsoon times. • Anthropogenic inputs are linked with Indian, South Asian and Central Asian sources.
Non-Darwinian evolution for the source detection of atmospheric releases

Science.gov (United States)

Cervone, Guido; Franzese, Pasquale

2011-08-01

A non-Darwinian evolutionary algorithm is presented as search engine to identify the characteristics of a source of atmospheric pollutants, given a set of concentration measurements. The algorithm drives iteratively a forward dispersion model from tentative sources toward the real source. The solutions of non-Darwinian evolution processes are not generated through pseudo-random operators, unlike traditional evolutionary algorithms, but through a reasoning process based on machine learning rule generation and instantiation. The new algorithm is tested with both a synthetic case and with the Prairie Grass field experiment. To further test the capabilities of the algorithm to work in real-world scenarios, the source identification of all Prairie Grass releases was performed with a decreasing number of sensor measurements, and a relationship is found between the precision of the solution, the number of sensors available, and the levels of concentration measured by the sensors. The proposed methodology can be used for a variety of optimization problems, and is particularly suited for problems where the operations needed for evaluating new candidate solutions are computationally expensive.
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.
Atomic carbon emission from photodissociation of CO2. [planetary atmospheric chemistry

Science.gov (United States)

Wu, C. Y. R.; Phillips, E.; Lee, L. C.; Judge, D. L.

1978-01-01

Atomic carbon fluorescence, C I 1561, 1657, and 1931 A, has been observed from photodissociation of CO2, and the production cross sections have been measured. A line emission source provided the primary photons at wavelengths from threshold to 420 A. The present results suggest that the excited carbon atoms are produced by total dissociation of CO2 into three atoms. The cross sections for producing the O I 1304-A fluorescence through photodissociation of CO2 are found to be less than 0.01 Mb in the wavelength region from 420 to 835 A. The present data have implications with respect to photochemical processes in the atmospheres of Mars and Venus.
Spatial considerations of snow chemistry as a non-point contamination source in Alpine watersheds

International Nuclear Information System (INIS)

Elder, K.; Williams, M.; Dozier, J.

1991-01-01

Alpine watersheds act as a temporary storage basin for large volumes of precipitation as snow. Monitoring these basins for the presence and effects of acid precipitation is important because these areas are often weakly buffered and sensitive to acidification. Study of these sensitive areas may provide early detection of trends resulting form anthropogenic atmospheric inputs. In an intensive study of an alpine watershed in the Sierra Nevada in 1987 and 1988, the authors carefully monitored snow distribution and chemistry through space and time. They found that the volume-weighted mean ionic concentrations within the snowpack did not vary greatly over the basin at peak accumulation. However, the distribution of total snow water equivalence (SWE) was highly variable spatially. Coefficients of variation (CV) for SWE lead to a corresponding high spatial variance in the chemical loading of their study basin. Their results show that to obtain accurate estimates of chemical loading they must measure the chemical and physical snow parameters at a resolution proportional to their individual variances. It is therefore necessary to combine many SWE measurements with fewer carefully obtained chemistry measurements. They used a classification method based on physical parameters to partition the basin into similar zones for estimation of SWE distribution. This technique can also be used for sample design
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
HELIOS–RETRIEVAL: An Open-source, Nested Sampling Atmospheric Retrieval Code; Application to the HR 8799 Exoplanets and Inferred Constraints for Planet Formation

Energy Technology Data Exchange (ETDEWEB)

Lavie, Baptiste; Mendonça, João M.; Malik, Matej; Demory, Brice-Olivier; Grimm, Simon L. [University of Bern, Space Research and Planetary Sciences, Sidlerstrasse 5, CH-3012, Bern (Switzerland); Mordasini, Christoph; Oreshenko, Maria; Heng, Kevin [University of Bern, Center for Space and Habitability, Sidlerstrasse 5, CH-3012, Bern (Switzerland); Bonnefoy, Mickaël [Université Grenoble Alpes, IPAG, F-38000, Grenoble (France); Ehrenreich, David, E-mail: baptiste.lavie@space.unibe.ch, E-mail: kevin.heng@csh.unibe.ch [Observatoire de l’Université de Genève, 51 chemin des Maillettes, 1290, Sauverny (Switzerland)

2017-09-01

We present an open-source retrieval code named HELIOS–RETRIEVAL, designed to obtain chemical abundances and temperature–pressure profiles by inverting the measured spectra of exoplanetary atmospheres. In our forward model, we use an exact solution of the radiative transfer equation, in the pure absorption limit, which allows us to analytically integrate over all of the outgoing rays. Two chemistry models are considered: unconstrained chemistry and equilibrium chemistry (enforced via analytical formulae). The nested sampling algorithm allows us to formally implement Occam’s Razor based on a comparison of the Bayesian evidence between models. We perform a retrieval analysis on the measured spectra of the four HR 8799 directly imaged exoplanets. Chemical equilibrium is disfavored for HR 8799b and c. We find supersolar C/H and O/H values for the outer HR 8799b and c exoplanets, while the inner HR 8799d and e exoplanets have a range of C/H and O/H values. The C/O values range from being superstellar for HR 8799b to being consistent with stellar for HR 8799c and being substellar for HR 8799d and e. If these retrieved properties are representative of the bulk compositions of the exoplanets, then they are inconsistent with formation via gravitational instability (without late-time accretion) and consistent with a core accretion scenario in which late-time accretion of ices occurred differently for the inner and outer exoplanets. For HR 8799e, we find that spectroscopy in the K band is crucial for constraining C/O and C/H. HELIOS–RETRIEVAL is publicly available as part of the Exoclimes Simulation Platform (http://www.exoclime.org).
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
Atmospheric mercury concentration and chemical speciation at a rural site in Beijing, China: implications of mercury emission sources

Directory of Open Access Journals (Sweden)

L. Zhang

2013-10-01

Full Text Available Continuous measurements of atmospheric mercury concentration and speciation play a key role in identifying mercury sources and its behavior in the atmosphere. In this study, speciated atmospheric mercury including gaseous elemental mercury (GEM, reactive gaseous mercury (RGM and particle-bound mercury (PBM were continuously measured at Miyun, a rural site in Beijing, China, from December 2008 to November 2009. The average GEM, RGM and PBM concentrations were found to be 3.22 ± 1.74, 10.1 ± 18.8 and 98.2 ± 112.7 pg m−3, respectively, about 2–20 times higher than the background concentration of the Northern Hemisphere. The results indicated that atmospheric mercury concentrations in northern China were highly affected by anthropogenic emissions. The atmospheric mercury showed obvious seasonal variations, with the highest seasonal average GEM concentration in summer (3.48 ng m−3 and the lowest value in winter (2.66 ng m−3. In autumn and winter a diurnal variation of GEM was observed, with peak levels in the late afternoon till midnight. Most of the high RGM concentration values occurred in the afternoon of all seasons due to the higher oxidation. The PBM concentration was higher in early morning of all seasons because of the the temperature inversion that increases in depth as the night proceeds. The ratio of GEM to CO indicates that residential boilers play an important role in the elevation of GEM in winter. The ratio of RGM to O3 could be an indicator of the contribution of local primary sources. The ratio of PBM to PM2.5 reveals that the air mass from the east and southwest of the site in spring and summer carries more atmospheric mercury. The HYSPLIT back-trajectory analysis indicated that the monitoring site is affected by local, regional and interregional sources simultaneously during heavy pollution episodes. The results from the potential source contribution function (PSCF model indicate that the atmospheric transport
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.
An Atmospheric Atomic Oxygen Source for Cleaning Smoke Damaged Art Objects

Science.gov (United States)

Banks, Bruce A.; Rutledge, Sharon K.; Norris, Mary Jo

1998-01-01

Soot and other carbonaceous combustion products deposited on the surfaces of porous ceramic, stone, ivory and paper can be difficult to remove and can have potentially unsatisfactory results using wet chemical and/or abrasive cleaning techniques. An atomic oxygen source which operates in air at atmospheric pressure, using a mixture of oxygen and helium, has been developed to produce an atomic oxygen beam which is highly effective in oxidizing soot deposited on surfaces by burning candles made of paraffin, oil or rendered animal fat. Atomic oxygen source operating conditions and the results of cleaning soot from paper, gesso, ivory, limestone and water color-painted limestone are presented,
Atmospheric acidification of mineral aerosols: a source of bioavailable phosphorus for the oceans

Directory of Open Access Journals (Sweden)

A. Nenes

2011-07-01

Full Text Available Primary productivity of continental and marine ecosystems is often limited or co-limited by phosphorus. Deposition of atmospheric aerosols provides the major external source of phosphorus to marine surface waters. However, only a fraction of deposited aerosol phosphorus is water soluble and available for uptake by phytoplankton. We propose that atmospheric acidification of aerosols is a prime mechanism producing soluble phosphorus from soil-derived minerals. Acid mobilization is expected to be pronounced where polluted and dust-laden air masses mix. Our hypothesis is supported by the soluble compositions and reconstructed pH values for atmospheric particulate matter samples collected over a 5-yr period at Finokalia, Crete. In addition, at least tenfold increase in soluble phosphorus was observed when Saharan soil and dust were acidified in laboratory experiments which simulate atmospheric conditions. Aerosol acidification links bioavailable phosphorus supply to anthropogenic and natural acidic gas emissions, and may be a key regulator of ocean biogeochemistry.
Carbon (14C,13C) and hydrogen (D) isotope measurements on atmospheric methane and its sources (sinks)

International Nuclear Information System (INIS)

Levin, I.; Doerr, H.

1991-07-01

Concentrations and isotope ratios ( 13 C/ 12 C and D/H) of atmospheric methane and methane from other sources were determined by gas chromatography and mass spectroscopy in specially prepared samples. The results were used for assessing the atmospheric methane inventory. (BBR) [de
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.
Non-LTE H2+ as the source of missing opacity in the solar atmosphere

Science.gov (United States)

Swamy, K. S. K.; Stecher, T. P.

1974-01-01

The population of the various vibrational levels of the H2+ molecule has been calculated from the consideration of formation and destruction mechanisms. The resulting population is used in calculating the total absorption due to H2+ and is compared with the other known sources of opacity at several optical depths of the solar atmosphere. It is shown that the absorption due to H2+ can probably account for the missing ultraviolet opacity in the solar atmosphere.
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
Effects of continental anthropogenic sources on organic aerosols in the coastal atmosphere of East China

International Nuclear Information System (INIS)

Shang, Dongjie; Hu, Min; Guo, Qingfeng; Zou, Qi; Zheng, Jing; Guo, Song

2017-01-01

source data and meteorological parameters. - Highlights: • Molecular and spatial characteristics of particulate organic compounds in coastal atmosphere of East China are reported. • Terrestrial fossil fuels and biomass burning have significant influences on aerosols in coastal atmosphere of East China. • Continental influences are highly dependent on the air mass origins. • Proportion of compounds from photochemical oxidation increased during the long range transport. - Capsule: Influences of continental anthropogenic sources on the composition of organic aerosols in the coastal atmosphere of East China were found to be significant and dependent on the origins of the air masses.

Bootstrap inversion technique for atmospheric trace gas source detection and quantification using long open-path laser measurements

Science.gov (United States)

Alden, Caroline B.; Ghosh, Subhomoy; Coburn, Sean; Sweeney, Colm; Karion, Anna; Wright, Robert; Coddington, Ian; Rieker, Gregory B.; Prasad, Kuldeep

2018-03-01

Advances in natural gas extraction technology have led to increased activity in the production and transport sectors in the United States and, as a consequence, an increased need for reliable monitoring of methane leaks to the atmosphere. We present a statistical methodology in combination with an observing system for the detection and attribution of fugitive emissions of methane from distributed potential source location landscapes such as natural gas production sites. We measure long (> 500 m), integrated open-path concentrations of atmospheric methane using a dual frequency comb spectrometer and combine measurements with an atmospheric transport model to infer leak locations and strengths using a novel statistical method, the non-zero minimum bootstrap (NZMB). The new statistical method allows us to determine whether the empirical distribution of possible source strengths for a given location excludes zero. Using this information, we identify leaking source locations (i.e., natural gas wells) through rejection of the null hypothesis that the source is not leaking. The method is tested with a series of synthetic data inversions with varying measurement density and varying levels of model-data mismatch. It is also tested with field observations of (1) a non-leaking source location and (2) a source location where a controlled emission of 3.1 × 10-5 kg s-1 of methane gas is released over a period of several hours. This series of synthetic data tests and outdoor field observations using a controlled methane release demonstrates the viability of the approach for the detection and sizing of very small leaks of methane across large distances (4+ km2 in synthetic tests). The field tests demonstrate the ability to attribute small atmospheric enhancements of 17 ppb to the emitting source location against a background of combined atmospheric (e.g., background methane variability) and measurement uncertainty of 5 ppb (1σ), when measurements are averaged over 2 min. The
Fundamentals of nuclear chemistry

International Nuclear Information System (INIS)

Matel, L.; Dulanska, S.

2013-01-01

This text-book is an introductory text in nuclear chemistry and radiochemistry, aimed on university undergraduate students in chemistry and related disciplines (physics, nuclear engineering). It covers the key aspects of modern nuclear chemistry. The text begins with basic theories in contemporary physics. It relates nuclear phenomena to key divisions of chemistry such as atomic structure, spectroscopy, equilibria and kinetics. It also gives an introduction to sources of ionizing radiation, detection of ionizing radiation, nuclear power industry and accident on nuclear installations as well as basic knowledge's of radiobiology. This book is essential reading for those taking a first course in nuclear chemistry and is a useful companion to other volumes in physical and analytical chemistry. It will also be of use to those new to working in nuclear chemistry or radiochemistry.
Low frequency acoustic waves from explosive sources in the atmosphere

Science.gov (United States)

Millet, Christophe; Robinet, Jean-Christophe; Roblin, Camille; Gloerfelt, Xavier

2006-11-01

In this study, a perturbative formulation of non linear euler equations is used to compute the pressure variation for low frequency acoustic waves from explosive sources in real atmospheres. Based on a Dispersion-Relation-Preserving (DRP) finite difference scheme, the discretization provides good properties for both sound generation and long range sound propagation over a variety of spatial atmospheric scales. It also assures that there is no wave mode coupling in the numerical simulation The background flow is obtained by matching the comprehensive empirical global model of horizontal winds HWM-93 (and MSISE-90 for the temperature profile) with meteorological reanalysis of the lower atmosphere. Benchmark calculations representing cases where there is downward and upward refraction (including shadow zones), ducted propagation, and generation of acoustic waves from low speed shear layers are considered for validation. For all cases, results show a very good agreement with analytical solutions, when available, and with other standard approaches, such as the ray tracing and the normal mode technique. Comparison of calculations and experimental data from the high explosive ``Misty Picture'' test that provided the scaled equivalent airblast of an 8 kt nuclear device (on May 14, 1987), is also considered. It is found that instability waves develop less than one hour after the wavefront generated by the detonation passes.
Applications of Ground-based Mobile Atmospheric Monitoring: Real-time Characterization of Source Emissions and Ambient Concentrations

Science.gov (United States)

Goetz, J. Douglas

Gas and particle phase atmospheric pollution are known to impact human and environmental health as well as contribute to climate forcing. While many atmospheric pollutants are regulated or controlled in the developed world uncertainty still remains regarding the impacts from under characterized emission sources, the interaction of anthropogenic and naturally occurring pollution, and the chemical and physical evolution of emissions in the atmosphere, among many other uncertainties. Because of the complexity of atmospheric pollution many types of monitoring have been implemented in the past, but none are capable of perfectly characterizing the atmosphere and each monitoring type has known benefits and disadvantages. Ground-based mobile monitoring with fast-response in-situ instrumentation has been used in the past for a number of applications that fill data gaps not possible with other types of atmospheric monitoring. In this work, ground-based mobile monitoring was implemented to quantify emissions from under characterized emission sources using both moving and portable applications, and used in a novel way for the characterization of ambient concentrations. In the Marcellus Shale region of Pennsylvania two mobile platforms were used to estimate emission rates from infrastructure associated with the production and transmission of natural gas using two unique methods. One campaign investigated emissions of aerosols, volatile organic compounds (VOCs), methane, carbon monoxide (CO), nitrogen dioxide (NO2), and carbon dioxide (CO 2) from natural gas wells, well development practices, and compressor stations using tracer release ratio methods and a developed fenceline tracer release correction factor. Another campaign investigated emissions of methane from Marcellus Shale gas wells and infrastructure associated with two large national transmission pipelines using the "Point Source Gaussian" method described in the EPA OTM-33a. During both campaigns ambient concentrations
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
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
Major ion chemistry of the Son River, India

Indian Academy of Sciences (India)

The chemistry of major ions in the surface water of the Son River was studied in detail to determine various source(s) and processes controlling its water chemistry, seasonal and spatial variations in water chemistry, dissolved fluxes and chemical denudation rate (CDR). The study shows that Ca2+, Mg2+ and HCO 3 − are ...
Formation of amino acids and nucleotide bases in a Titan atmosphere simulation experiment.

Science.gov (United States)

Hörst, S M; Yelle, R V; Buch, A; Carrasco, N; Cernogora, G; Dutuit, O; Quirico, E; Sciamma-O'Brien, E; Smith, M A; Somogyi, A; Szopa, C; Thissen, R; Vuitton, V

2012-09-01

The discovery of large (>100 u) molecules in Titan's upper atmosphere has heightened astrobiological interest in this unique satellite. In particular, complex organic aerosols produced in atmospheres containing C, N, O, and H, like that of Titan, could be a source of prebiotic molecules. In this work, aerosols produced in a Titan atmosphere simulation experiment with enhanced CO (N(2)/CH(4)/CO gas mixtures of 96.2%/2.0%/1.8% and 93.2%/5.0%/1.8%) were found to contain 18 molecules with molecular formulae that correspond to biological amino acids and nucleotide bases. Very high-resolution mass spectrometry of isotopically labeled samples confirmed that C(4)H(5)N(3)O, C(4)H(4)N(2)O(2), C(5)H(6)N(2)O(2), C(5)H(5)N(5), and C(6)H(9)N(3)O(2) are produced by chemistry in the simulation chamber. Gas chromatography-mass spectrometry (GC-MS) analyses of the non-isotopic samples confirmed the presence of cytosine (C(4)H(5)N(3)O), uracil (C(5)H(4)N(2)O(2)), thymine (C(5)H(6)N(2)O(2)), guanine (C(5)H(5)N(5)O), glycine (C(2)H(5)NO(2)), and alanine (C(3)H(7)NO(2)). Adenine (C(5)H(5)N(5)) was detected by GC-MS in isotopically labeled samples. The remaining prebiotic molecules were detected in unlabeled samples only and may have been affected by contamination in the chamber. These results demonstrate that prebiotic molecules can be formed by the high-energy chemistry similar to that which occurs in planetary upper atmospheres and therefore identifies a new source of prebiotic material, potentially increasing the range of planets where life could begin.
Hydroxyl and Hydroperoxy Radical Chemistry during the MCMA-2006 Field Campaign: Measurement and Model Comparison

Science.gov (United States)

Dusanter, S.; Vimal, D.; Stevens, P. S.; Volkamer, R.; Molina, L. T.

2007-12-01

The Mexico City Metropolitan Area (MCMA) field campaign, held in March 2006, was a unique opportunity to collect data in one of the most polluted megacities in the world. Such environments exhibit a complex oxidation chemistry involving a strong coupling between odd hydrogen radicals (HOX=OH+HO2) and nitrogen oxides species (NOX=NO+NO2). High levels of volatile organic compounds (VOCs) and NOX control the HOX budget and lead to elevated tropospheric ozone formation. The HOX-NOX coupling can be investigated by comparing measured and model-predicted HOx concentrations. Atmospheric HOX concentrations were measured by the Indiana University laser-induced fluorescence instrument and data were collected at the Instituto Mexicano del Petroleo between 14 and 31 March. Measured hydroxyl radical (OH) concentrations are comparable to that measured in less polluted urban environments and suggest that the OH concentrations are highly buffered under high NOX conditions. In contrast, hydroperoxy radical (HO2) concentrations are more sensitive to the NOX levels and are highly variable between different urban sites. Enhanced levels of OH and HO2 radicals were observed on several days between 9h30-11h00 AM and suggest an additional HOX source for the morning hours and/or a fast HOX cycling under the high NOX conditions of the MCMA. A preliminary investigation of the HOX chemistry occurring in the MCMA urban atmosphere was performed using a photochemical box model based on the Regional Atmospheric Chemistry Mechanism (RACM). Model comparisons will be presented and the agreement between measured and predicted HOX concentrations will be discussed.
BARTTest: Community-Standard Atmospheric Radiative-Transfer and Retrieval Tests

Science.gov (United States)

Harrington, Joseph; Himes, Michael D.; Cubillos, Patricio E.; Blecic, Jasmina; Challener, Ryan C.

2018-01-01

Atmospheric radiative transfer (RT) codes are used both to predict planetary and brown-dwarf spectra and in retrieval algorithms to infer atmospheric chemistry, clouds, and thermal structure from observations. Observational plans, theoretical models, and scientific results depend on the correctness of these calculations. Yet, the calculations are complex and the codes implementing them are often written without modern software-verification techniques. The community needs a suite of test calculations with analytically, numerically, or at least community-verified results. We therefore present the Bayesian Atmospheric Radiative Transfer Test Suite, or BARTTest. BARTTest has four categories of tests: analytically verified RT tests of simple atmospheres (single line in single layer, line blends, saturation, isothermal, multiple line-list combination, etc.), community-verified RT tests of complex atmospheres, synthetic retrieval tests on simulated data with known answers, and community-verified real-data retrieval tests.BARTTest is open-source software intended for community use and further development. It is available at https://github.com/ExOSPORTS/BARTTest. We propose this test suite as a standard for verifying atmospheric RT and retrieval codes, analogous to the Held-Suarez test for general circulation models. This work was supported by NASA Planetary Atmospheres grant NX12AI69G, NASA Astrophysics Data Analysis Program grant NNX13AF38G, and NASA Exoplanets Research Program grant NNX17AB62G.
Source apportionment of atmospheric polycyclic aromatic hydrocarbons (PAHs) in Palm Beach County, Florida.

Science.gov (United States)

Afshar-Mohajer, Nima; Wilson, Christina; Wu, Chang-Yu; Stormer, James E

2016-04-01

Due to concerns about adverse health effects associated with inhalation of atmospheric polycyclic aromatic hydrocarbons (PAHs), 30 ambient air samples were obtained at an air quality monitoring station in Palm Beach County, Florida, from March 2013 to March 2014. The ambient PAH concentration measurements and fractional emission rates of known sources were incorporated into a chemical mass balance model, CMB8.2, developed by EPA, to apportion contributions of three major PAH sources including preharvest sugarcane burning, mobile vehicles, and wildland fires. Strong association between the number of benzene rings and source contribution was found, and mobile vehicles were identified to be the prevailing source (contribution≥56%) for the observed PAHs concentration with lower molecular weights (four or fewer benzene rings) throughout the year. Preharvest sugarcane burning was the primary contributing source for PAHs with relatively higher molecular weights (five or more benzene rings) during the sugarcane burning season (from October to May of the next year). Source contribution of wildland fires varied among PAH compounds but was consistently lower than for sugarcane burning during the sugarcane harvest season. Determining the major sources responsible for ground-level PAHs serves as a tool to improving management strategies for PAH emitting sources and a step toward better protection of the health of residents in terms of exposure to PAHs. The results obtain insight into temporal dominance of PAH polluting sources for those residential areas located near sugarcane burning facilities and have implications beyond Palm Beach County, in areas with high concerns of PAHs and their linked sources. Source apportionment of atmospheric polycyclic hydrocarbons (PAHs) in Palm Beach County, Florida, meant to estimate contributions of major sources in PAH concentrations measured at Belle Glade City of Palm Beach County. Number of benzene rings was found to be the key parameter
Sources of speciated atmospheric mercury at a residential neighborhood impacted by industrial sources.

Science.gov (United States)

Manolopoulos, Helen; Snyder, David C; Schauer, James J; Hill, Jason S; Turner, Jay R; Olson, Mark L; Krabbenhoft, David P

2007-08-15

Speciated measurements of atmospheric mercury plumes were obtained at an industrially impacted residential area of East St. Louis, IL. These plumes were found to result in extremely high mercury concentrations at ground level that were composed of a wide distribution of mercury species. Ground level concentrations as high as 235 ng m(-3) for elemental mercury (Hg0) and 38 300 pg m(-3) for reactive mercury species (reactive gaseous (RGM) plus particulate (PHg) mercury) were measured. The highest mercury concentrations observed during the study were associated with plumes that contained high concentrations of all mercury species (Hg0, RGM, and PHg) and originated from a source located southwest of the sampling site. Variations in proportions of Hg0/RGM/PHg among plumes, with Hg0 dominating some plumes and RGM and/or PHg dominating others, were attributed to differences in emissions from different sources. Correlations between mercury plumes and elevated NO(x) were not observed; however, a correlation between elevated SO2 and mercury plumes was observed during some but not all plume events. Despite the presence of six coal-fired power plants within 60 km of the study site, wind direction data along with Hg/SO2 and Hg/NO(x) ratios suggest that high-concentration mercury plumes impacting the St. Louis-Midwest Particle Matter Supersite are attributable to local point sources within 5 km of the site.
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
Separating contributions from natural and anthropogenic sources in atmospheric methane from the Black Sea region, Romania

International Nuclear Information System (INIS)

Cuna, Stela; Pendall, Elise; Miller, John B.; Tans, Pieter P.; Dlugokencky, Ed; White, James W.C.

2008-01-01

The Danube Delta-Black Sea region of Romania is an important wetland, and this preliminary study evaluates the significance of this region as a source of atmospheric CH 4 . Measurements of the mixing ratio and δ 13 C in CH 4 are reported from air and water samples collected at eight sites in the Danube Delta. High mixing ratios of CH 4 were found in air (2500-14,000 ppb) and dissolved in water samples (∼1-10 μmol L -1 ), demonstrating that the Danube Delta is an important natural source of CH 4 . The intercepts on Keeling plots of about -62 per mille show that the main source of CH 4 in this region is microbial, probably resulting primarily from acetate fermentation. Atmospheric CH 4 and CO data from the NOAA/ESRL (National Oceanic and Atmospheric Administration/Earth System Research Laboratory) were used to make a preliminary estimate of biogenic CH 4 at the Black Sea sampling site at Constanta (BSC). These data were used to calculate ratios of CH 4 /CO in air samples, and using an assumed CH 4 /CO anthropogenic emissions ratio of 0.6, fossil fuel emissions at BSC were estimated. Biogenic CH 4 emissions were then estimated by a simple mass balance approach. Keeling plots of well-mixed air from the BSC site suggested a stronger wetland source in summer and a stronger fossil fuel source in winter
Global-scale combustion sources of organic aerosols: sensitivity to formation and removal mechanisms

Science.gov (United States)

Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos

2017-06-01

Organic compounds from combustion sources such as biomass burning and fossil fuel use are major contributors to the global atmospheric load of aerosols. We analyzed the sensitivity of model-predicted global-scale organic aerosols (OA) to parameters that control primary emissions, photochemical aging, and the scavenging efficiency of organic vapors. We used a computationally efficient module for the description of OA composition and evolution in the atmosphere (ORACLE) of the global chemistry-climate model EMAC (ECHAM/MESSy Atmospheric Chemistry). A global dataset of aerosol mass spectrometer (AMS) measurements was used to evaluate simulated primary (POA) and secondary (SOA) OA concentrations. Model results are sensitive to the emission rates of intermediate-volatility organic compounds (IVOCs) and POA. Assuming enhanced reactivity of semi-volatile organic compounds (SVOCs) and IVOCs with OH substantially improved the model performance for SOA. The use of a hybrid approach for the parameterization of the aging of IVOCs had a small effect on predicted SOA levels. The model performance improved by assuming that freshly emitted organic compounds are relatively hydrophobic and become increasingly hygroscopic due to oxidation.
Selected source term topics. Report to CSNI by an OECD/NEA Group of experts

International Nuclear Information System (INIS)

1987-04-01

CSNI Report 136 summarizes the results of the work performed by the Group of Experts on the Source Term and Environmental Consequences (PWG4) during the period extending from 1983 and 1986. This report is complementary to Part 1, 'Technical Status of the Source Term' of CSNI Report 135, 'Report to CSNI on Source Term Assessment, Containment atmosphere control systems, and accident consequences'; it considers in detail a number of very specific issues thought to be important in the source term area. It consists of: an executive summary (prepared by the Chairman of the Group), a section on conclusions and recommendations, and five technical chapters (fission product chemistry in the primary circuit of a LWR during severe accidents; resuspension/re-entrainment of aerosols in LWRs following a meltdown accident; iodine chemistry under severe accident conditions; effects of combustion, steam explosions and pressurized melt ejection on fission product behaviour; radionuclide removal by pool scrubbing), a technical annex and two appendices
Mercury from combustion sources: a review of the chemical species emitted and their transport in the atmosphere

International Nuclear Information System (INIS)

Carpi, A.

1997-01-01

Different species of mercury have different physical/chemical properties and thus behave quite differentially in air pollution control equipment and in the atmosphere. In general, emission of mercury from coal combustion sources are approximately 20-50% elemental mercury (Hg 0 ) and 50-80% divalent mercury (Hg(II)), which may be predominantly HgCl 2 . Emissions of mercury from waste incinerators are approximately 10-20% Hg 0 and 75-85% Hg(II). The partitioning of mercury in flue gas between the elemental and divalent forms may be dependent on the concentration of particulate carbon, HCl and other pollutants in the stack emissions. The emission of mercury from combustion facilities depends on the species in the exhaust stream and the type of air pollution control equipment used at the source. Air pollution control equipment for mercury removal at combustion facilities includes activated carbon injection, sodium sulfide injection and wet lime/limestone flue gas desulfurization. White Hg(II) is water-soluble and may be removed form the atmosphere by wet and dry deposition close to the combustion sources, the combination of a high vapor pressure and low water-solubility facilitate the long-range transport of Hg 0 in the atmosphere. Background mercury in the atmosphere is predominantly Hg 0 . Elemental mercury is eventually removed from the atmosphere by dry deposition onto surfaces and by wet deposition after oxidation to water-soluble, divalent mercury. 62 refs., 2 figs., 1 tab
Mass spectroscopic analysis of atmospheric particulate matter

International Nuclear Information System (INIS)

Wippel, R.

1997-02-01

Particulate matter (PM) in the atmosphere vary greatly in origin, in their physical and chemical properties and their effects on climate, atmospheric chemistry and health. Aerosol particles with an aerodynamic diameter less than two μm can enter the respiratory tract of humans when inhaled. Bulk analysis of ambient dust particles was performed using an inductively coupled plasma mass spectrometer (ICP-MS). The size-fractionated collected samples were analyzed after a leaching procedure that simulates the solution reactions occurring in the lungs. A disadvantage of bulk analysis is that it gives no information about the distribution of a certain element within the particles under investigation. A Laser-Microprobe-Mass-Analyzer (LAMMA-500) was used to obtain this information. At sampling sites in Austria and in Zimbabwe, Africa, single particles were sampled using a self-made impactor. One of the final aims in environmental analysis is to successfully apply receptor models that relate the chemical and physical properties of a receptor site to a source. The knowledge of the sources of atmospheric particulate matter is essential for environmental policy makers as well as for epidemiological studies. Artificial neural networks (ANN) have a remarkable ability to handle LAMMA-data. Three ANNs were used as a pattern recognition tool for LAMMA mass spectral data: a back-propagation net, a Kohonen network,and a counter-propagation net. Standard source profiles from the United States Environmental Protection Agency were used as training and test data of the different nets. The elemental patterns of the sum of 100 mass spectra of fine dust particles were presented to the trained nets and satisfactory recognition (> 80 %) was obtained. (author)
Top-down estimate of a large source of atmospheric carbon monoxide associated with fuel combustion in Asia

Energy Technology Data Exchange (ETDEWEB)

Kasibhatla, P.; Arellano, A.; Logan, J.A.; Palmer, P.I.; Novelli, P. [Duke University, Durham, NC (United States). Nicholas School of Environmental & Earth Science

2002-10-01

Deriving robust regional estimates of the sources of chemically and radiatively important gases and aerosols to the atmosphere is challenging. Using an inverse modeling methodology, it was found that the source of carbon monoxide from fossil-fuel and biofuel combustion in Asia during 1994 was 350-380 Tg yr{sup -1}, which is 110-140 Tg yr{sup -1} higher than bottom-up estimates derived using traditional inventory-based approaches. This discrepancy points to an important gap in our understanding of the human impact on atmospheric chemical composition.
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

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.
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
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
Pb isotopic composition of the atmosphere of the Sao Paulo city, Brazil, and isotopic characterization of some pollutant sources

International Nuclear Information System (INIS)

Aily, C.; Babinski, M.; Ruiz, I.R.; Sato, K

2001-01-01

Lead isotopes are known to be good tools for surveying lead origin in atmospheric samples (Chow et al., 1975). Lead has four naturally occurring stable isotopes: 206 Pb, 207 Pb, 208 Pb and 204 Pb. The first three isotopes are end products of radioactive decay chains from 238 U, 235 U and 232 Th, respectively, and the last one is non-radiogenic. Therefore, their abundance and the ratios among the four isotopes gradually change with time. Lead in the atmosphere comes from various sources, such as leaded gasoline, industrial emissions and coal combustion. Thus, lead isotope ratios different from those of the mother rock in the region are often observed in the atmosphere (Tatsumoto and Patterson, 1963). Lead is emitted to the atmosphere in fine particles, which can be transported within air masses for very long distances, e. g. from mid latitude regions to the Artic and Antarctica (Sturges and Barrie, 1989). Lead isotopes have been used to trace the pollutant sources in many cities of the world. However, a systematic study using this methodology has not been done in any Brazilian city. The main purpose of the present work is to characterize the Pb isotope composition in the atmosphere in Sao Paulo city, and suggest the possible pollutant sources. For our study lead isotopes were measured in different samples: aerosols and rainwater which would yield the Pb isotope composition of the atmosphere. Samples of gasoline and ethanol, gutter sweepings, soot from vehicle exhaust pipes, and filters containing particulate material from industrial emissions were also analyzed, since they were considered potential pollutant sources of the atmosphere. In order to obtain the local geogenic Pb isotopic composition we also analyzed rock and K-feldspar samples. Lead concentrations were only determined on aerosols and rainwater samples (au)
Source, flux and balance of atmospheric deposition of metals at Ile-de-France; Source, flux et bilan des retombees atmospheriques de metaux en Ile de France

Energy Technology Data Exchange (ETDEWEB)

Azimi, S

2004-07-15

The urban atmosphere is submitted to large inputs of anthropogenic contaminants arising from both stationary (power plants, industries, etc.) and mobile (road traffic) sources. These small particles may be transported over long distances and affect ecosystems. Significant dry and wet atmospheric deposition also occurs locally and contributes to the contamination of urban runoff. The aim of this study is to compare heavy metal and hydrocarbon atmospheric deposition fluxes to other input ways on agricultural and urban areas to assess their importance. Moreover, a source investigation has been done to identify the main origins of these pollutants. Before the quantification of pollutant fluxes, a comparison of several sampling procedures was performed. As a result, the sampling of total atmospheric deposition is not affected by the funnel material (Teflon and polyethylene) or by the sampling duration (7 and 28 days). However, the rinsing step of the funnel walls showed a higher relative importance during short sampling periods. The relative amount contained in these solutions reached 24 to 40 % of the total flux during weekly sampling periods and 8 to 18 % during monthly sampling periods, whatever the element considered. The temporal evolution of atmospheric deposition showed no seasonal influence on flux variations during the 2001-2002 period. Considering an 8-year period behaviour, between 1994 and 2002, a significant decrease of the deposition fluxes of Cd, Cu, Pb and Zn occurred at the Creteil site which is placed in an industrialized area of the Paris suburb. The decreasing factor reached 16, 2.5, 4 and 7.5 for these elements respectively. At the Ile-de-France scale, the deposition flux levels on urban and semi-urban areas were of the same order of magnitude (?20 tonnes per year for Ba, Cu, Pb and Sr). Since semi-urban surface area is four times higher than urban ones, the important influence of anthropogenic activities on atmospheric deposition of urban areas is
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.
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.
Source apportionment and environmental fate of lead chromates in atmospheric dust in arid environments.

Science.gov (United States)

Meza-Figueroa, Diana; González-Grijalva, Belem; Romero, Francisco; Ruiz, Joaquin; Pedroza-Montero, Martín; Rivero, Carlos Ibañez-Del; Acosta-Elías, Mónica; Ochoa-Landin, Lucas; Navarro-Espinoza, Sofía

2018-03-07

The environmental fate of lead derived from traffic paint has been poorly studied in developing countries, mainly in arid zones. For this purpose, a developing city located in the Sonoran desert (Hermosillo, Mexico), was chosen to conduct a study. In this paper the lead chromate (crocoite) sources in atmospheric dust were addressed using a combination of Raman microspectroscopy, X-ray diffraction, scanning electron microscopy (SEM), and Pb isotope measurements. A high concentration of Pb and Cr as micro- and nanostructured pigments of crocoite is reported in yellow traffic paint (n=80), road dust (n=146), settled dust in roofs (n=21), and atmospheric dust (n=20) from a developing city located in the Sonoran Desert. 10 samples of peri-urban soils were collected for local geochemical background. The paint photodegradation and erosion of the asphaltic cover are enhanced by the climate, and the presence of the mineral crocoite (PbCrO 4 ) in road dust with an aerodynamic diameter ranging from 100nm to 2μm suggests its integration into the atmosphere by wind resuspension processes. A positive PbCr correlation (R 2 =0.977) was found for all studied samples, suggesting a common source. The Pb-isotope data show signatures in atmospheric dust as a product of the mixing of two end members: i) local soils and ii) crocoite crystals as pigments in paint. The presence of lead chromates in atmospheric dust has not been previously documented in Latin America, and it represents an unknown health risk to the exposed population because the identified size of crystals can reach the deepest part of lungs. Copyright © 2018 Elsevier B.V. All rights reserved.
Development of computer-based function to estimate radioactive source term by coupling atmospheric model with monitoring data

International Nuclear Information System (INIS)

Akiko, Furuno; Hideyuki, Kitabata

2003-01-01

Full text: The importance of computer-based decision support systems for local and regional scale accidents has been recognized by many countries with the experiences of accidental atmospheric releases of radionuclides at Chernobyl in 1986 in the former Soviet Union. The recent increase of nuclear power plants in the Asian region also necessitates an emergency response system for Japan to predict the long-range atmospheric dispersion of radionuclides due to overseas accident. On the basis of these backgrounds, WSPEEDI (Worldwide version of System for Prediction of Environmental Emergency Dose Information) at Japan Atomic Energy Research Institute is developed to forecast long-range atmospheric dispersions of radionuclides during nuclear emergency. Although the source condition is critical parameter for accurate prediction, it is rarely that the condition can be acquired in the early stage of overseas accident. Thus, we have been developing a computer-based function to estimate radioactive source term, e.g. the release point, time and amount, as a part of WSPEEDI. This function consists of atmospheric transport simulations and statistical analysis for the prediction and monitoring of air dose rates. Atmospheric transport simulations are carried out for the matrix of possible release points in Eastern Asia and possible release times. The simulation results of air dose rates are compared with monitoring data and the best fitted release condition is defined as source term. This paper describes the source term estimation method and the application to Eastern Asia. The latest version of WSPEEDI accommodates following two models: an atmospheric meteorological model MM5 and a particle random walk model GEARN. MM5 is a non-hydrostatic meteorological model developed by the Pennsylvania State University and the National Center for Atmospheric Research (NCAR). MM5 physically calculates more than 40 meteorological parameters with high resolution in time and space based an
Radiation field of an optically finite homogeneous atmosphere with internal sources

International Nuclear Information System (INIS)

Viik, T.

2010-01-01

The equation of radiative transfer in an optically finite homogeneous atmosphere with different internal sources is solved using the method of kernel approximation the essence of which is to approximate the kernel in the equation for the Sobolev resolvent function by a Gauss-Legendre sum. This approximation allows to solve the equation exactly for the resolvent function while the solution is a weighted sum of exponents. Since the resolvent function is closely connected with the Green function of the integral radiative transfer equation, the radiation field for different internal sources can be found by simple integration. In order to simplify the obtained formulas we have defined the x and y functions as the generalization of the well-known Ambarzumian-Chandrasekhar X and Y functions. For some types of internal sources the package of codes in Fortran-77 can be found at (http://www.aai.ee/~viik/HOMOGEN.FOR).
Modeling the biogeochemical impact of atmospheric phosphate deposition from desert dust and combustion sources to the Mediterranean Sea

Science.gov (United States)

Richon, Camille; Dutay, Jean-Claude; Dulac, François; Wang, Rong; Balkanski, Yves

2018-04-01

Daily modeled fields of phosphate deposition to the Mediterranean from natural dust, anthropogenic combustion and wildfires were used to assess the effect of this external nutrient on marine biogeochemistry. The ocean model used is a high-resolution (1/12°) regional coupled dynamical-biogeochemical model of the Mediterranean Sea (NEMO-MED12/PISCES). The input fields of phosphorus are for 2005, which are the only available daily resolved deposition fields from the global atmospheric chemical transport model LMDz-INCA. Traditionally, dust has been suggested to be the main atmospheric source of phosphorus, but the LMDz-INCA model suggests that combustion is dominant over natural dust as an atmospheric source of phosphate (PO4, the bioavailable form of phosphorus in seawater) for the Mediterranean Sea. According to the atmospheric transport model, phosphate deposition from combustion (Pcomb) brings on average 40.5×10-6 mol PO4 m-2 yr-1 over the entire Mediterranean Sea for the year 2005 and is the primary source over the northern part (e.g., 101×10-6 mol PO4 m-2 yr-1 from combustion deposited in 2005 over the north Adriatic against 12.4×10-6 from dust). Lithogenic dust brings 17.2×10-6 mol PO4 m-2 yr-1 on average over the Mediterranean Sea in 2005 and is the primary source of atmospheric phosphate to the southern Mediterranean Basin in our simulations (e.g., 31.8×10-6 mol PO4 m-2 yr-1 from dust deposited in 2005 on average over the south Ionian basin against 12.4×10-6 from combustion). The evaluation of monthly averaged deposition flux variability of Pdust and Pcomb for the 1997-2012 period indicates that these conclusions may hold true for different years. We examine separately the two atmospheric phosphate sources and their respective flux variability and evaluate their impacts on marine surface biogeochemistry (phosphate concentration, chlorophyll a, primary production). The impacts of the different phosphate deposition sources on the biogeochemistry of the
Bootstrap inversion technique for atmospheric trace gas source detection and quantification using long open-path laser measurements

Directory of Open Access Journals (Sweden)

C. B. Alden

2018-03-01

Full Text Available Advances in natural gas extraction technology have led to increased activity in the production and transport sectors in the United States and, as a consequence, an increased need for reliable monitoring of methane leaks to the atmosphere. We present a statistical methodology in combination with an observing system for the detection and attribution of fugitive emissions of methane from distributed potential source location landscapes such as natural gas production sites. We measure long (> 500 m, integrated open-path concentrations of atmospheric methane using a dual frequency comb spectrometer and combine measurements with an atmospheric transport model to infer leak locations and strengths using a novel statistical method, the non-zero minimum bootstrap (NZMB. The new statistical method allows us to determine whether the empirical distribution of possible source strengths for a given location excludes zero. Using this information, we identify leaking source locations (i.e., natural gas wells through rejection of the null hypothesis that the source is not leaking. The method is tested with a series of synthetic data inversions with varying measurement density and varying levels of model–data mismatch. It is also tested with field observations of (1 a non-leaking source location and (2 a source location where a controlled emission of 3.1  ×  10−5 kg s−1 of methane gas is released over a period of several hours. This series of synthetic data tests and outdoor field observations using a controlled methane release demonstrates the viability of the approach for the detection and sizing of very small leaks of methane across large distances (4+ km2 in synthetic tests. The field tests demonstrate the ability to attribute small atmospheric enhancements of 17 ppb to the emitting source location against a background of combined atmospheric (e.g., background methane variability and measurement uncertainty of 5 ppb (1σ, when
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.
Source apportionment of atmospheric bulk deposition in the Belgrade urban area using Positive Matrix factorization

Science.gov (United States)

Tasić, M.; Mijić, Z.; Rajšić, S.; Stojić, A.; Radenković, M.; Joksić, J.

2009-04-01

The primary objective of the present study was to assess anthropogenic impacts of heavy metals to the environment by determination of total atmospheric deposition of heavy metals. Atmospheric depositions (wet + dry) were collected monthly, from June 2002 to December 2006, at three urban locations in Belgrade, using bulk deposition samplers. Concentrations of Fe, Al, Pb, Zn, Cu, Ni, Mn, Cr, V, As and Cd were analyzed using atomic absorption spectrometry. Based upon these results, the study attempted to examine elemental associations in atmospheric deposition and to elucidate the potential sources of heavy metal contaminants in the region by the use of multivariate receptor model Positive Matrix Factorization (PMF).
Source apportionment of atmospheric bulk deposition in the Belgrade urban area using Positive Matrix factorization

International Nuclear Information System (INIS)

Tasic, M; Mijic, Z; Rajsic, S; Stojic, A; Radenkovic, M; Joksic, J

2009-01-01

The primary objective of the present study was to assess anthropogenic impacts of heavy metals to the environment by determination of total atmospheric deposition of heavy metals. Atmospheric depositions (wet + dry) were collected monthly, from June 2002 to December 2006, at three urban locations in Belgrade, using bulk deposition samplers. Concentrations of Fe, Al, Pb, Zn, Cu, Ni, Mn, Cr, V, As and Cd were analyzed using atomic absorption spectrometry. Based upon these results, the study attempted to examine elemental associations in atmospheric deposition and to elucidate the potential sources of heavy metal contaminants in the region by the use of multivariate receptor model Positive Matrix Factorization (PMF).
GPU-accelerated atmospheric chemical kinetics in the ECHAM/MESSy (EMAC) Earth system model (version 2.52)

Science.gov (United States)

Alvanos, Michail; Christoudias, Theodoros

2017-10-01

This paper presents an application of GPU accelerators in Earth system modeling. We focus on atmospheric chemical kinetics, one of the most computationally intensive tasks in climate-chemistry model simulations. We developed a software package that automatically generates CUDA kernels to numerically integrate atmospheric chemical kinetics in the global climate model ECHAM/MESSy Atmospheric Chemistry (EMAC), used to study climate change and air quality scenarios. A source-to-source compiler outputs a CUDA-compatible kernel by parsing the FORTRAN code generated by the Kinetic PreProcessor (KPP) general analysis tool. All Rosenbrock methods that are available in the KPP numerical library are supported.Performance evaluation, using Fermi and Pascal CUDA-enabled GPU accelerators, shows achieved speed-ups of 4. 5 × and 20. 4 × , respectively, of the kernel execution time. A node-to-node real-world production performance comparison shows a 1. 75 × speed-up over the non-accelerated application using the KPP three-stage Rosenbrock solver. We provide a detailed description of the code optimizations used to improve the performance including memory optimizations, control code simplification, and reduction of idle time. The accuracy and correctness of the accelerated implementation are evaluated by comparing to the CPU-only code of the application. The median relative difference is found to be less than 0.000000001 % when comparing the output of the accelerated kernel the CPU-only code.The approach followed, including the computational workload division, and the developed GPU solver code can potentially be used as the basis for hardware acceleration of numerous geoscientific models that rely on KPP for atmospheric chemical kinetics applications.
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.
Revisit the modeling of the Saturnian ring atmosphere and ionosphere from the "Cassini Grand Finale" results

Science.gov (United States)

Tseng, W. L.; Johnson, R. E.; Tucker, O. J.; Perry, M. E.; Ip, W. H.

2017-12-01

During the Cassini Grand Finale mission, this spacecraft, for the first time, has done the in-situ measurements of Saturn's upper atmosphere and its rings and provides critical information for understanding the coupling dynamics between the main rings and the Saturnian system. The ring atmosphere is the source of neutrals (i.e., O2, H2, H; Tseng et al., 2010; 2013a), which is primarily generated by photolytic decomposition of water ice (Johnson et al., 2006), and plasma (i.e., O2+ and H2+; Tseng et al., 2011) in the Saturnian magnetosphere. In addition, the main rings have strong interaction with Saturn's atmosphere and ionosphere (i.e., a source of oxygen into Saturn's upper atmosphere and/or the "ring rain" in O'Donoghue et al., 2013). Furthermore, the near-ring plasma environment is complicated by the neutrals from both the seasonally dependent ring atmosphere and Enceladus torus (Tseng et al., 2013b), and, possibly, from small grains from the main and tenuous F and G rings (Johnson et al.2017). The data now coming from Cassini Grand Finale mission already shed light on the dominant physics and chemistry in this region of Saturn's magnetosphere, for example, the presence of carbonaceous material from meteorite impacts in the main rings and each gas species have similar distribution in the ring atmosphere. We will revisit the details in our ring atmosphere/ionosphere model to study, such as the source mechanism for the organic material and the neutral-grain-plasma interaction processes.
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....
Atmospheric dispersion and inverse modelling for the reconstruction of accidental sources of pollutants

International Nuclear Information System (INIS)

Winiarek, Victor

2014-01-01

Uncontrolled releases of pollutant in the atmosphere may be the consequence of various situations: accidents, for instance leaks or explosions in an industrial plant, or terrorist attacks such as biological bombs, especially in urban areas. In the event of such situations, authorities' objectives are various: predict the contaminated zones to apply first countermeasures such as evacuation of concerned population; determine the source location; assess the long-term polluted areas, for instance by deposition of persistent pollutants in the soil. To achieve these objectives, numerical models can be used to model the atmospheric dispersion of pollutants. We will first present the different processes that govern the transport of pollutants in the atmosphere, then the different numerical models that are commonly used in this context. The choice between these models mainly depends of the scale and the details one seeks to take into account. We will then present several inverse modeling methods to estimate the emission as well as statistical methods to estimate prior errors, to which the inversion is very sensitive. Several case studies are presented, using synthetic data as well as real data such as the estimation of source terms from the Fukushima accident in March 2011. From our results, we estimate the Cesium-137 emission to be between 12 and 19 PBq with a standard deviation between 15 and 65% and the Iodine-131 emission to be between 190 and 380 PBq with a standard deviation between 5 and 10%. Concerning the localization of an unknown source of pollutant, two strategies can be considered. On one hand parametric methods use a limited number of parameters to characterize the source term to be reconstructed. To do so, strong assumptions are made on the nature of the source. The inverse problem is hence to estimate these parameters. On the other hand nonparametric methods attempt to reconstruct a full emission field. Several parametric and nonparametric methods are

Atmospheric cycles of nitrogen oxides and ammonia. [source strengths and destruction rates

Science.gov (United States)

Bottger, A.; Ehhalt, D. H.; Gravenhorst, G.

1981-01-01

The atmospheric cycles of nitrogenous trace compounds for the Northern and Southern Hemispheres are discussed. Source strengths and destruction rates for the nitrogen oxides: NO, NO2 and HNO3 -(NOX) and ammonia (NH3) are given as a function of latitude over continents and oceans. The global amounts of NOX-N and NH3-N produced annually in the period 1950 to 1975 (34 + 5 x one trillion g NOx-N/yr and 29 + or - 6 x one trillion g NH3-N/yr) are much less than previously assumed. Globally, natural and anthropogenic emissions are of similar magnitude. The NOx emission from anthropogenic sources is 1.5 times that from natural processes in the Northern Hemisphere, whereas in the Southern Hemisphere, it is a factor of 3 or 4 less. More than 80% of atmospheric ammonia seems to be derived from excrements of domestic animals, mostly by bulk deposition: 24 + or - 9 x one trillion g NO3 -N/yr and 21 + or - 9 x one trillion g NH4+-N/yr. Another fraction may be removed by absorption on vegetation and soils.
Identifying the change in atmospheric sulfur sources in China using isotopic ratios in mosses

Science.gov (United States)

Xiao, Hua-Yun; Tang, Cong-Guo; Xiao, Hong-Wei; Liu, Xue-Yan; Liu, Cong-Qiang

2009-08-01

A considerable number of studies on rainwater sulfur isotopic ratios (δ34Srain) have been conducted to trace sulfur sources at a large number of sites in the past. If longitudinal studies on the isotope composition of precipitation sulfate were conducted, it is possible to relate that to changes in sulfur emissions. But direct measurement needs considerable labor and time. So, in this study, sulfur isotopic ratios in rainwater and mosses were analyzed at Guiyang and Nanchang to evaluate the possibility of using mosses as a substitute for rainwater. We found that present moss sulfur isotopic ratios were comparable to those of present rainwater. Additionally, we investigated the changes of atmospheric sulfur sources and sulfur concentrations using an isotopic graphic analysis at five industrial cities, two forested areas, and two remote areas in China. Mosses in industrial cities show a wide range of δ34S values, with the highest occurring at Chongqing (+3.9‰) and the lowest at Guiyang (-3.1‰). But as compared to those in forested and remote areas, δ34S values of mosses in all the five industrial cities are lower. On the basis of isotopic comparisons between past rainwater (reported in the literature) and present mosses, in the plot of δ34Smoss versus δ34Srain, six zones indicating different atmospheric sulfur change are separated by the 1:1 line and δ34S values of potential sulfur sources. Our results indicate that atmospheric sulfur pollution in most of the industrial cities decreased, while at the two forested areas, no significant changes were observed, and a new anxiousness coming from new energy sources (e.g., oil) appeared in some cities. Studies on the change of ambient SO2 concentrations support these results.
Sources of Sahelian-Sudan moisture: Insights from a moisture-tracing atmospheric model

Science.gov (United States)

Salih, Abubakr A. M.; Zhang, Qiong; Pausata, Francesco S. R.; Tjernström, Michael

2016-07-01

The summer rainfall across Sahelian-Sudan is one of the main sources of water for agriculture, human, and animal needs. However, the rainfall is characterized by large interannual variability, which has attracted extensive scientific efforts to understand it. This study attempts to identify the source regions that contribute to the Sahelian-Sudan moisture budget during July through September. We have used an atmospheric general circulation model with an embedded moisture-tracing module (Community Atmosphere Model version 3), forced by observed (1979-2013) sea-surface temperatures. The result suggests that about 40% of the moisture comes with the moisture flow associated with the seasonal migration of the Intertropical Convergence Zone (ITCZ) and originates from Guinea Coast, central Africa, and the Western Sahel. The Mediterranean Sea, Arabian Peninsula, and South Indian Ocean regions account for 10.2%, 8.1%, and 6.4%, respectively. Local evaporation and the rest of the globe supply the region with 20.3% and 13.2%, respectively. We also compared the result from this study to a previous analysis that used the Lagrangian model FLEXPART forced by ERA-Interim. The two approaches differ when comparing individual regions, but are in better agreement when neighboring regions of similar atmospheric flow features are grouped together. Interannual variability with the rainfall over the region is highly correlated with contributions from regions that are associated with the ITCZ movement, which is in turn linked to the Atlantic Multidecadal Oscillation. Our result is expected to provide insights for the effort on seasonal forecasting of the rainy season over Sahelian Sudan.
Lead isotopic fingerprinting of aerosols to characterize the sources of atmospheric lead in an industrial city of India

Science.gov (United States)

Sen, Indra S.; Bizimis, Michael; Tripathi, Sachchida Nand; Paul, Debajyoti

2016-03-01

Anthropogenic Pb in the environment is primarily sourced from combustion of fossil fuel and high-temperature industries such as smelters. Identifying the sources and pathways of anthropogenic Pb in the environment is important because Pb toxicity is known to have adverse effects on human health. Pb pollution sources for America, Europe, and China are well documented. However, sources of atmospheric Pb are unknown in India, particularly after leaded gasoline was phased out in 2000. India has a developing economy with a rapidly emerging automobile and high temperature industry, and anthropogenic Pb emission is expected to rise in the next decade. In this study, we report on the Pb-isotope compositions and trace metal ratios of airborne particulates collected in Kanpur, a large city in northern part of India. The study shows that the PM10 aerosols had elevated concentration of Cd, Pb, Zn, As, and Cu in the Kanpur area, however their concentrations are well below the United States Environmental Protection Agency chronic exposure limit. Lead isotopic and trace metal data reveal industrial emission as the plausible source of anthropogenic Pb in the atmosphere in Kanpur. However, Pb isotopic compositions of potential source end-members are required to fully evaluate Pb contamination in India over time. This is the first study that characterizes the isotopic composition of atmospheric Pb in an Indian city after leaded gasoline was phased out by 2000.
Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

Science.gov (United States)

Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

2015-10-06

Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.
Sources of speciated atmospheric mercury at a residential neighborhood impacted by industrial sources

Energy Technology Data Exchange (ETDEWEB)

Helen Manolopoulos; David C. Snyder; James J. Schauer; Jason S. Hill; Jay R. Turner; Mark L. Olson; David P. Krabbenhoft [University of Wisconsin-Madison, Madison, WI (United States). Environmental Chemistry and Technology Program

2007-08-15

Speciated measurements of atmospheric mercury plumes were obtained at an industrially impacted residential area of East St. Louis, IL. These plumes were found to result in extremely high mercury concentrations at ground level that were composed of a wide distribution of mercury species. Ground level concentrations as high as 235 ng m{sup -3} for elemental mercury (Hg{sup 0}) and 38,300 pg m{sup -3} for reactive mercury species (reactive gaseous (RGM) plus particulate (PHg) mercury) were measured. The highest mercury concentrations observed during the study were associated with plumes that contained high concentrations of all mercury species (Hg{sup 0}, RGM, and PHg) and originated from a source located southwest of the sampling site. Variations in proportions of Hg{sup 0}/RGM/PHg among plumes, with Hg{sup 0} dominating some plumes and RGM and/or PHg dominating others, were attributed to differences in emissions from different sources. Correlations between mercury plumes and elevated NOx were not observed; however, a correlation between elevated SO{sub 2} and mercury plumes was observed during some but not all plume events. Despite the presence of six coal-fired power plants within 60 km of the study site, wind direction data along with Hg/SO{sub 2} and Hg/NOx ratios suggest that high-concentration mercury plumes impacting the St. Louis-Midwest Particle Matter Supersite are attributable to local point sources within 5 km of the site. 35 refs., 5 figs.
Further evaluation of wetland emission estimates from the JULES land surface model using SCIAMACHY and GOSAT atmospheric column methane measurements

Science.gov (United States)

Hayman, Garry; Comyn-Platt, Edward; McNorton, Joey; Chipperfield, Martyn; Gedney, Nicola

2016-04-01

The atmospheric concentration of methane began rising again in 2007 after a period of near-zero growth [1,2], with the largest increases observed over polar northern latitudes and the Southern Hemisphere in 2007 and in the tropics since then. The observed inter-annual variability in atmospheric methane concentrations and the associated changes in growth rates have variously been attributed to changes in different methane sources and sinks [2,3]. Wetlands are generally accepted as being the largest, but least well quantified, single natural source of CH4, with global emission estimates ranging from 142-284 Tg yr-1 [3]. The modelling of wetlands and their associated emissions of CH4 has become the subject of much current interest [4]. We have previously used the HadGEM2 chemistry-climate model to evaluate the wetland emission estimates derived using the UK community land surface model (JULES, the Joint UK Land Earth Simulator) against atmospheric observations of methane, including SCIAMACHY total methane columns [5] up to 2007. We have undertaken a series of new HadGEM2 runs using new JULES emission estimates extended in time to the end of 2012, thereby allowing comparison with both SCIAMACHY and GOSAT atmospheric column methane measurements. We will describe the results of these runs and the implications for methane wetland emissions. References [1] Rigby, M., et al.: Renewed growth of atmospheric methane. Geophys. Res. Lett., 35, L22805, 2008; [2] Nisbet, E.G., et al.: Methane on the Rise-Again, Science 343, 493, 2014; [3] Kirschke, S., et al.,: Three decades of global methane sources and sinks, Nature Geosciences, 6, 813-823, 2013; [4] Melton, J. R., et al.: Present state of global wetland extent and wetland methane modelling: conclusions from a model inter-comparison project (WETCHIMP), Biogeosciences, 10, 753-788, 2013; [5] Hayman, G.D., et al.: Comparison of the HadGEM2 climate-chemistry model against in situ and SCIAMACHY atmospheric methane data, Atmos. Chem
History of atmospheric deposition of Cd, Hg, and Pb in North America: Evidence from lake and peat bog sediments

International Nuclear Information System (INIS)

Norton, S.A.; Dillon, P.J.; Evans, R.D.; Mierle, G.; Kahl, J.S.

1990-01-01

The precipitation chemistry and lake and peat sediment chemistry of three metals emitted to the atmosphere in significant amounts as a result of anthropogenic activity are reviewed. The three metals, Cd, Hg, and Pb, have contrasting source terms, atmospheric residence times, and chemical mobility. Lake and ombrotrophic peat bog sediments record increases in the concentrations and accumulation rates of the metals for most of temperate North America for the last 100 years. These increases are largely related to the burning of coal, smelting of nonferrous metals, the transportation industry, and the industrial production of chlorine. Modern atmospheric fluxes of Cd in central North America are about 1,000 times background fluxes; accumulation rates for Cd in sediments have increased two to 3 times above background, beginning about 100 years ago. Global scale Hg pollution off the atmosphere is suggested by concentrations in northern hemisphere air that are double the Hg content of southern hemisphere air. Accumulation rates of Hg in sediment have approximately doubled in the last 100 years. However, these rates are approximately an order of magnitude less than those for Cd. Modern increases in Pb concentrations are ubiquitous for all lakes examines thus far in North America. Input is from multiple sources and thus the timing of increased accumulation rates in sediment varies across the continent. Typical modern accumulation rates reach maxima at 20 to 30 mg/sq-m/yr, or 100 times that of Cd and 1,000 times that off Hg. Recent decreases in atmospheric lead are reflected in decreases in the accumulation rate of Pb in both lake and peat bog sediment in eastern North America
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
Atmospheric observations for quantifying emissions of point-source synthetic greenhouse gases (CF4, NF3 and HFC-23)

Science.gov (United States)

Arnold, Tim; Manning, Alistair J.; Li, Shanlan; Kim, Jooil; Park, Sunyoung; Fraser, Paul J.; Mitrevski, Blagoj; Steele, L. Paul; Krummel, Paul B.; Mühle, Jens; Weiss, Ray F.

2016-04-01

The fluorinated species carbon tetrafluoride (CF4; PFC-14), nitrogen trifluoride (NF3) and trifluoromethane (CHF3; HFC-23) are potent greenhouse gases with 100-year global warming potentials of 6,630, 16,100 and 12,400, respectively. Unlike the majority of CFC-replacement compounds that are emitted from fugitive and mobile emission sources, these gases are largely emitted from large single point sources - semiconductor manufacturing facilities (all three), aluminium smelting plants (CF4) and chlorodifluoromethane factories (HFC-23). In this work we show the potential for atmospheric measurements to understand regional sources of these gases and to highlight emission 'hotspots'. We target our analysis on measurements from two Advanced Global Atmospheric Gases Experiment (AGAGE) long term monitoring sites that are particularly sensitive to regional emissions of these gases: Gosan on Jeju Island in the Republic of Korea and Cape Grim on Tasmania in Australia. These sites measure CF4, NF3 and HFC-23 alongside a suite of greenhouse and stratospheric ozone depleting gases every two hours using automated in situ gas-chromatography mass-spectrometry instrumentation. We couple each measurement to an analysis of air history using the regional atmospheric transport model NAME (Numerical Atmospheric dispersion Modelling Environment) driven by 3D meteorology from the Met Office's Unified Model, and use a Bayesian inverse method (InTEM - Inversion Technique for Emission Modelling) to calculate yearly emission changes over a decade (2005-2015) at high spatial resolution. At present these gases make a small contribution to global radiative forcing, however, given that their impact could rise significantly and that point sources of such gases can be mitigated, atmospheric monitoring could be an important tool for aiding emissions reduction policy.
Atmospheric deposition of polycyclic aromatic hydrocarbons (PAHs) in Shanghai: the spatio-temporal variation and source identification

Science.gov (United States)

Cheng, Chen; Bi, Chunjuan; Wang, Dongqi; Yu, Zhongjie; Chen, Zhenlou

2018-03-01

This study investigated the dry and wet deposition fluxes of atmospheric polycyclic aromatic hydrocarbons (PAHs) in Shanghai, China. The flux sources were traced based on composition and spatio-temporal variation. The results show that wet deposition concentrations of PAHs ranged from 0.07 to 0.67 mg·L-1 and were correlated with temperature ( P<0.05). Dry deposition of PAHs concentrations ranged from 3.60-92.15 mg·L-1 and were higher in winter and spring than in summer and autumn. The annual PAH average fluxes were 0.631 mg·m-2·d-1 and 4.06 mg·m-2·d-1 for wet and dry deposition, respectively. The highest wet deposition of PAH fluxes was observed in summer, while dry deposition fluxes were higher in winter and spring. Atmospheric PAHs were deposited as dry deposition in spring and winter, yet wet deposition was the dominant pathway during summer. Total atmospheric PAH fluxes were higher in the northern areas than in the southern areas of Shanghai, and were also observed to be higher in winter and spring. Annual deposition of atmospheric PAHs was about 10.8 t in across all of Shanghai. Wet deposition of PAHs was primarily composed of two, three, or four rings, while dry deposition of PAHs was composed of four, five, or six rings. The atmospheric PAHs, composed of four, five, or six rings, primarily existed in the form of particulates. Coal combustion and vehicle emissions were the dominant sources of PAH in the observed area of downtown Shanghai. In suburban areas, industrial pollution, from sources such as coke oven, incinerator, and oil fired power plant, was as significant as vehicle emissions in contributing to the deposition of PAHs.
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)
Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol

Energy Technology Data Exchange (ETDEWEB)

Massachusetts Institute of Technology; Kroll, Jesse H.; Donahue, Neil M.; Jimenez, Jose L.; Kessler, Sean H.; Canagaratna, Manjula R.; Wilson, Kevin R.; Altieri, Katye E.; Mazzoleni, Lynn R.; Wozniak, Andrew S.; Bluhm, Hendrik; Mysak, Erin R.; Smith, Jared D.; Kolb, Charles E.; Worsnop, Douglas R.

2010-11-05

A detailed understanding of the sources, transformations, and fates of organic species in the environment is crucial because of the central roles that organics play in human health, biogeochemical cycles, and Earth's climate. However, such an understanding is hindered by the immense chemical complexity of environmental mixtures of organics; for example, atmospheric organic aerosol consists of at least thousands of individual compounds, all of which likely evolve chemically over their atmospheric lifetimes. Here we demonstrate the utility of describing organic aerosol (and other complex organic mixtures) in terms of average carbon oxidation state (OSC), a quantity that always increases with oxidation, and is readily measured using state-of-the-art analytical techniques. Field and laboratory measurements of OSC , using several such techniques, constrain the chemical properties of the organics and demonstrate that the formation and evolution of organic aerosol involves simultaneous changes to both carbon oxidation state and carbon number (nC).
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
Absolute density measurements in the middle atmosphere

Directory of Open Access Journals (Sweden)

M. Rapp

2001-05-01

Full Text Available In the last ten years a total of 25 sounding rockets employing ionization gauges have been launched at high latitudes ( ~ 70° N to measure total atmospheric density and its small scale fluctuations in an altitude range between 70 and 110 km. While the determination of small scale fluctuations is unambiguous, the total density analysis has been complicated in the past by aerodynamical disturbances leading to densities inside the sensor which are enhanced compared to atmospheric values. Here, we present the results of both Monte Carlo simulations and wind tunnel measurements to quantify this aerodynamical effect. The comparison of the resulting ‘ram-factor’ profiles with empirically determined density ratios of ionization gauge measurements and falling sphere measurements provides excellent agreement. This demonstrates both the need, but also the possibility, to correct aerodynamical influences on measurements from sounding rockets. We have determined a total of 20 density profiles of the mesosphere-lower-thermosphere (MLT region. Grouping these profiles according to season, a listing of mean density profiles is included in the paper. A comparison with density profiles taken from the reference atmospheres CIRA86 and MSIS90 results in differences of up to 40%. This reflects that current reference atmospheres are a significant potential error source for the determination of mixing ratios of, for example, trace gas constituents in the MLT region.Key words. Middle atmosphere (composition and chemistry; pressure, density, and temperature; instruments and techniques
Absolute density measurements in the middle atmosphere

Directory of Open Access Journals (Sweden)

M. Rapp

Full Text Available In the last ten years a total of 25 sounding rockets employing ionization gauges have been launched at high latitudes ( ~ 70° N to measure total atmospheric density and its small scale fluctuations in an altitude range between 70 and 110 km. While the determination of small scale fluctuations is unambiguous, the total density analysis has been complicated in the past by aerodynamical disturbances leading to densities inside the sensor which are enhanced compared to atmospheric values. Here, we present the results of both Monte Carlo simulations and wind tunnel measurements to quantify this aerodynamical effect. The comparison of the resulting ‘ram-factor’ profiles with empirically determined density ratios of ionization gauge measurements and falling sphere measurements provides excellent agreement. This demonstrates both the need, but also the possibility, to correct aerodynamical influences on measurements from sounding rockets. We have determined a total of 20 density profiles of the mesosphere-lower-thermosphere (MLT region. Grouping these profiles according to season, a listing of mean density profiles is included in the paper. A comparison with density profiles taken from the reference atmospheres CIRA86 and MSIS90 results in differences of up to 40%. This reflects that current reference atmospheres are a significant potential error source for the determination of mixing ratios of, for example, trace gas constituents in the MLT region.

Key words. Middle atmosphere (composition and chemistry; pressure, density, and temperature; instruments and techniques
Chemical characterisation of atmospheric aerosols during a 2007 summer field campaign at Brasschaat, Belgium: sources and source processes of biogenic secondary organic aerosol

Directory of Open Access Journals (Sweden)

Y. Gómez-González

2012-01-01

Full Text Available Measurements of organic marker compounds and inorganic species were performed on PM_2.5 aerosols from a Belgian forest site that is severely impacted by urban pollution ("De Inslag", Brasschaat, Belgium during a 2007 summer period within the framework of the "Formation mechanisms, marker compounds, and source apportionment for biogenic atmospheric aerosols (BIOSOL" project. The measured organic species included (i low-molecular weight (MW dicarboxylic acids (LMW DCAs, (ii methanesulfonate (MSA, (iii terpenoic acids originating from the oxidation of α-pinene, β-pinene, d-limonene and Δ³-carene, and (iv organosulfates related to secondary organic aerosol from the oxidation of isoprene and α-pinene. The organic tracers explained, on average, 5.3 % of the organic carbon (OC, of which 0.7 % was due to MSA, 3.4 % to LMW DCAs, 0.6 % to organosulfates, and 0.6 % to terpenoic acids. The highest atmospheric concentrations of most species were observed during the first five days of the campaign, which were characterised by maximum day-time temperatures >22 °C. Most of the terpenoic acids and the organosulfates peaked during day-time, consistent with their local photochemical origin. High concentrations of 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA and low concentrations of cis-pinonic acid were noted during the first five days of the campaign, indicative of an aged biogenic aerosol. Several correlations between organic species were very high (r>0.85, high (0.7<r<0.85, or substantial (0.5<r<0.7, suggesting that they are generated through similar formation pathways. Substantial correlations with temperature were found for OC, water-soluble OC, MBTCA, and several other organic species. MBTCA and terebic acid were highly correlated with the temperature (r>0.7 and showed an Arrhenius-type relationship, consistent with their formation through OH radical chemistry.
Traveling-Wave Tube Amplifier Second Harmonic as Millimeter-Wave Beacon Source for Atmospheric Propagation Studies

Science.gov (United States)

Simons, Rainee N.; Wintucky, Edwin G.

2014-01-01

This paper presents the design and test results of a CW millimeter-wave satellite beacon source, based on the second harmonic from a traveling-wave tube amplifier and utilizes a novel waveguide multimode directional coupler. A potential application of the beacon source is for investigating the atmospheric effects on Q-band (37-42 GHz) and V/W-band (71- 76 GHz) satellite-to-ground signals.
Air exposure of coral is a significant source of dimethylsulfide (DMS) to the atmosphere.

Science.gov (United States)

Hopkins, Frances E; Bell, Thomas G; Yang, Mingxi; Suggett, David J; Steinke, Michael

2016-10-31

Corals are prolific producers of dimethylsulfoniopropionate (DMSP). High atmospheric concentrations of the DMSP breakdown product dimethylsulfide (DMS) have been linked to coral reefs during low tides. DMS is a potentially key sulfur source to the tropical atmosphere, but DMS emission from corals during tidal exposure is not well quantified. Here we show that gas phase DMS concentrations (DMS gas ) increased by an order of magnitude when three Indo-Pacific corals were exposed to air in laboratory experiments. Upon re-submersion, an additional rapid rise in DMS gas was observed, reflecting increased production by the coral and/or dissolution of DMS-rich mucus formed by the coral during air exposure. Depletion in DMS following re-submersion was likely due to biologically-driven conversion of DMS to dimethylsulfoxide (DMSO). Fast Repetition Rate fluorometry showed downregulated photosynthesis during air exposure but rapid recovery upon re-submersion, suggesting that DMS enhances coral tolerance to oxidative stress during a process that can induce photoinhibition. We estimate that DMS emission from exposed coral reefs may be comparable in magnitude to emissions from other marine DMS hotspots. Coral DMS emission likely comprises a regular and significant source of sulfur to the tropical marine atmosphere, which is currently unrecognised in global DMS emission estimates and Earth System Models.
The central and eastern Arabian Sea as a perennial source of atmospheric carbon dioxide

Digital Repository Service at National Institute of Oceanography (India)

Sarma, V.V.S.S.; DileepKumar, M.; George, M.D.

circulation and biological production. In all seasons, the pCO sub(2) is higher in surface waters of the Arabian Sea, except along the Indian coast in the southwest monsoon, than that in atmosphere, and thus this region appears to be a perennial source...

Identification of major sources controlling groundwater chemistry ...

Indian Academy of Sciences (India)

The study area Mettur forms an important industrial town situated NW of Salem district. The geology of the area is mainly composed of Archean crystalline metamorphic complexes. To iden- tify the major process activated for controlling the groundwater chemistry an attempt has been made by collecting a total of 46 ...
The kINPen—a review on physics and chemistry of the atmospheric pressure plasma jet and its applications

Science.gov (United States)

Reuter, Stephan; von Woedtke, Thomas; Weltmann, Klaus-Dieter

2018-06-01

The kINPen® plasma jet was developed from laboratory prototype to commercially available non-equilibrium cold plasma jet for various applications in materials research, surface treatment and medicine. It has proven to be a valuable plasma source for industry as well as research and commercial use in plasma medicine, leading to very successful therapeutic results and its certification as a medical device. This topical review presents the different kINPen plasma sources available. Diagnostic techniques applied to the kINPen are introduced. The review summarizes the extensive studies of the physics and plasma chemistry of the kINPen performed by research groups across the world, and closes with a brief overview of the main application fields.
Long-term trends of black carbon and sulphate aerosol in the Arctic: changes in atmospheric transport and source region emissions

Directory of Open Access Journals (Sweden)

D. Hirdman

2010-10-01

Full Text Available As a part of the IPY project POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport and building on previous work (Hirdman et al., 2010, this paper studies the long-term trends of both atmospheric transport as well as equivalent black carbon (EBC and sulphate for the three Arctic stations Alert, Barrow and Zeppelin. We find a general downward trend in the measured EBC concentrations at all three stations, with a decrease of −2.1±0.4 ng m⁻³ yr⁻¹ (for the years 1989–2008 and −1.4±0.8 ng m⁻³ yr⁻¹ (2002–2009 at Alert and Zeppelin respectively. The decrease at Barrow is, however, not statistically significant. The measured sulphate concentrations show a decreasing trend at Alert and Zeppelin of −15±3 ng m⁻³ yr⁻¹ (1985–2006 and −1.3±1.2 ng m⁻³ yr⁻¹ (1990–2008 respectively, while there is no trend detectable at Barrow.

To reveal the contribution of different source regions on these trends, we used a cluster analysis of the output of the Lagrangian particle dispersion model FLEXPART run backward in time from the measurement stations. We have investigated to what extent variations in the atmospheric circulation, expressed as variations in the frequencies of the transport from four source regions with different emission rates, can explain the long-term trends in EBC and sulphate measured at these stations. We find that the long-term trend in the atmospheric circulation can only explain a minor fraction of the overall downward trend seen in the measurements of EBC (0.3–7.2% and sulphate (0.3–5.3% at the Arctic stations. The changes in emissions are dominant in explaining the trends. We find that the highest EBC and sulphate concentrations are associated with transport from Northern Eurasia and decreasing emissions in this region drive the
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.
Mass spectrometric characterization of a pyrolytic radical source using femtosecond ionization

Energy Technology Data Exchange (ETDEWEB)

Frey, H M; Beaud, P; Mischler, B; Radi, P P; Tzannis, A P; Gerber, T [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

1997-06-01

Radicals play, as reactive species, an important role in the chemistry of combustion. In contrast to atmospheric flames where spectra are congested due to high vibrational and rotational excitation, experiments in the cold environment of a molecular beam (MB) yield clean spectra that can be easily attributed to one species by Resonantly Enhanced Multi Photon Ionization (REMP). A pyrolytic radical source has been set up. To characterize the efficiency of the source `soft` ionization with femto second pulses is applied which results in less fragmentation, simplifying the interpretation of the mass spectrum. (author) figs., tabs., refs.
MEAD Marine Effects of Atmospheric Deposition

Science.gov (United States)

Jickells, T.; Spokes, L.

2003-04-01

The coastal seas are one of the most valuable resources on the planet but they are threatened by human activity. We rely on the coastal area for mineral resources, waste disposal, fisheries and recreation. In Europe, high population densities and high levels of industrial activity mean that the pressures arising from these activities are particularly acute. One of the main problems concerning coastal seas is the rapid increase in the amounts of nitrogen-based pollutants entering the water. They come from many sources, the most important ones being traffic, industry and agriculture. These pollutants can be used by algae as nutrients. The increasing concentrations of these nutrients have led to excessive growth of algae, some of which are harmful. When algae die and decay, oxygen in the water is used up and the resulting lower levels of oxygen may lead to fish kills. Human activity has probably doubled the amount of chemically and biologically reactive nitrogen present globally. In Europe the increases have been greater than this, leading to real concern over the health of coastal waters. Rivers have, until recently, been thought to be the most important source of reactive nitrogen to the coastal seas but we now know that inputs from the atmosphere are large and can equal, or exceed, those from the rivers. Our initial hypothesis was that atmospheric inputs are important and potentially different in their effect on coastal ecosystems to riverine inputs and hence require different management strategies. However, we had almost no information on the direct effects of atmospheric deposition on marine ecosystems, though clearly such a large external nitrogen input should lead to enhanced phytoplankton growth The aim of this European Union funded MEAD project has been to determine how inputs of nitrogen from the atmosphere affect the chemistry and biology of coastal waters. To try to answer this, we have conducted field experiments in the Kattegat, an area where we know
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.
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.
Moisture sources of the Atmospheric Rivers making landfall in western Europe

Science.gov (United States)

Trigo, Ricardo M.; Ramos, Alexandre M.; Nieto, Raquel; Tomé, Ricardo; Gimeno, Luis; Liberato, Margarida L. R.; Lavers, David A.

2017-04-01

An automated atmospheric river (AR) detection algorithm is used for the North Atlantic Ocean basin, allowing the identification of the major ARs affecting western European coasts between 1979 and 2012. The entire western coast of Europe was divided into five domains, namely the Iberian Peninsula (9.75W, 36-43.75N), France (4.5W, 43.75-50N), UK (4.5W, 50-59N), southern Scandinavia and the Netherlands (5.25E, 50-59N), and northern Scandinavia (5.25E, 59-70N). Following the identification of the main ARs that made landfall in western Europe, a Lagrangian analysis was then applied in order to identify the main areas where the moisture uptake was anomalous and contributed to the ARs reaching each domain. The Lagrangian data set used was obtained from the FLEXPART model global simulation from 1979 to 2012. The results show that, in general, for all regions considered, the major climatological areas for the anomalous moisture uptake extend along the subtropical North Atlantic, from the Florida Peninsula (northward of 20N) to each sink region, with the nearest coast to each sink region always appearing as a local maximum. In addition, during AR events the Atlantic subtropical source is reinforced and displaced, with a slight northward movement of the sources found when the sink region is positioned at higher latitudes. In conclusion, the results confirm not only the anomalous advection of moisture linked to ARs from subtropical ocean areas but also the existence of a tropical source, together with midlatitude anomaly sources at some locations closer to AR landfalls (Ramos et al., 2016). References: Ramos et al., (2016) Atmospheric rivers moisture sources from a Lagrangian perspective, Earth Syst. Dynam., 7, 371-384. Acknowledgements This work was supported by the project IMDROFLOOD - Improving Drought and Flood Early Warning, Forecasting and Mitigation using real-time hydroclimatic indicators (WaterJPI/0004/2014) funded by Fundação para a Ciência e a Tecnologia
Acoustic-gravity waves generated by atmospheric and near-surface sources

Science.gov (United States)

Kunitsyn, Viacheslav E.; Kholodov, Alexander S.; Krysanov, Boris Yu.; Andreeva, Elena S.; Nesterov, Ivan A.; Vorontsov, Artem M.

2013-04-01

. The ionospheric footprints of atmospheric disturbances are given. The effects of AGW evolution after launching the rockets are studied. One of the possible applications of RT imaging of wavelike disturbances is the study of AGW and TID as probable precursors of the earthquakes. The key difficulty here is to distinguish between the AGW and atmospheric and ionospheric disturbances of non-seismic nature (for example, those caused by the enhanced solar-geomagnetic activity), which can be done by analyzing spatial two-dimensional and three-dimensional structures revealed by tomographic methods. The examples of AGW RT imaging based on the real experimental satellite data measured in regions of the Europe, North America and Asia are demonstrated. The example of AGW and TID generation by the tsunami wave after the Tohoku earthquake is presented. Our results prove the capability of RT methods to detect wavelike disturbances in the ionosphere, which are caused by the near-surface sources, and to distinguish between these disturbances and the influence from the atmosphere and space. The work was supported by the Russian Foundation for Basic Research (grants 11-05-01157 and 13-05-01122 ).
Simulation of preindustrial atmospheric methane to constrain the global source strength of natural wetlands

NARCIS (Netherlands)

Houweling, S; Dentener, F; Lelieveld, J

2000-01-01

Previous attempts to quantify the global source strength of CH4 from natural wetlands have resulted in a range of 90-260 TE(CH4) yr(-1). This relatively uncertain estimate significantly limits our understanding of atmospheric methane. In this study we reduce this uncertainty by simulating
The atmosphere as a source/sink of polychlorinated biphenyls to/from the Lower Duwamish Waterway Superfund site

International Nuclear Information System (INIS)

Apell, Jennifer N.; Gschwend, Philip M.

2017-01-01

Waterbodies polluted with polychlorinated biphenyls (PCBs) may cause the air in the surrounding area to become PCB-contaminated. Conversely, when a waterbody is located in or near an urban area, the deposition of atmospheric PCBs may act as a low-level, ongoing source of PCB contamination to that water. Distinguishing these situations is necessary to be protective of human populations and to guide efforts seeking to cleanup such aquatic ecosystems. To assess the situation at the Lower Duwamish Waterway (LDW) Superfund site, low-density polyethylene passive samplers were deployed in the summer of 2015 to quantify freely dissolved water and gaseous air concentrations of PCBs thereby enabling estimates of the direction and magnitude of air-water exchange of PCB congeners. For the sum of the 27 PCB congeners, average concentrations were 220 pg/m 3 (95% C.I.: 80–610) in the air and 320 pg/L (95% C.I.: 110–960) in the water. The sum of air-water exchange fluxes of these PCB congeners was estimated to be 68 ng/m 2 /day (95% C.I.: 30–148) into the lower atmosphere, contrasting with the reported wet and dry depositional flux of only 5.5 ng/m 2 /day (95% C.I.: 1–38) from the air into the water. Therefore, the atmosphere was ultimately a sink of PCBs from the LDW Superfund site, at least under 2015 summertime conditions. However, we conclude that air-water exchange of PCBs is likely only a minor sink of PCBs from the LDW and only a minor source of contamination to the region's local atmosphere. - Highlights: • Passive samplers were used to estimate air and water concentrations. • At this site, PCBs were being transported from the water into the local atmosphere. • Air-water exchange was likely only a minor sink of PCBs for the LDW site. • The LDW was likely only a minor source of PCBs to the local atmosphere. - Air-water exchange of PCBs from the LDW Superfund site, calculated using passive sampler data, was determined to be a minor sink of PCBs from
Fruit and cereal bioactives: sources, chemistry, and applications

National Research Council Canada - National Science Library

Tokusoglu, Ozlem; Hall, Clifford, III

2011-01-01

"Presenting up-to-date data in an easy-to-use format, this comprehensive overview of the chemistry of bioactive components of fruits and cereals addresses the role of these compounds in determining...
Atmospheric Aerosol Source-Receptor Relationships: The Role of Coal-Fired Power Plants

Energy Technology Data Exchange (ETDEWEB)

Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

2005-12-01

This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of March 2005 through August 2005. Significant progress was made this project period on the source characterization, source apportionment, and deterministic modeling activities. This report highlights new data on road dust, vegetative detritus and motor vehicle emissions. For example, the results show significant differences in the composition in urban and rural road dust. A comparison of the organic of the fine particulate matter in the tunnel with the ambient provides clear evidence of the significant contribution of vehicle emissions to ambient PM. The source profiles developed from this work are being used by the source-receptor modeling activities. The report presents results on the spatial distribution of PMF-factors. The results can be grouped into three different categories: regional sources, local sources, or potentially both regional and local sources. Examples of the regional sources are the sulfate and selenium PMF-factors which most likely-represent coal fired power plants. Examples of local sources are the specialty steel and lead factors. There is reasonable correspondence between these apportionments and data from the EPA TRI and AIRS emission inventories. Detailed comparisons between PMCAMx predictions and measurements by the STN and IMPROVE measurements in the Eastern US are presented. Comparisons were made for the major aerosol components and PM{sub 2.5} mass in July 2001, October 2001, January 2002, and April 2002. The results are encouraging with average fraction biases for most species less than 0.25. The improvement of the model performance during the last two years was mainly due to the comparison of the model predictions with the continuous measurements in the Pittsburgh Supersite. Major improvements have included the descriptions: of ammonia emissions (CMU inventory), night time nitrate chemistry, EC emissions and their diurnal
Atmospheric toxic metals emission inventory and spatial characteristics from anthropogenic sources of Guangdong province, China

Science.gov (United States)

Cher, S.; Menghua, L.; Xiao, X.; Yuqi, W.; Zhuangmin, Z.; Zhijiong, H.; Cheng, L.; Guanglin, J.; Zibing, Y.; Junyu, Z.

2017-12-01

Atmospheric toxic metals (TMs) are part of particulate matters, and may create adverse effects on the environment and human health depending upon their bioavailability and toxicity. Localized emission inventory is fundamental for parsing of toxic metals to identify key sources in order to formulate efficient toxic metals control strategies. With the use of the latest municipal level environment statistical data, this study developed a bottom-up emission inventory of five toxic metals (Hg, As, Pb, Cd, Cr) from anthropogenic activities in Guangdong province for the year of 2014. Major atmospheric toxic metals sources including combustion sources (coal, oil, biomass, municipal solid waste) and industrial process sources (cement production, nonferrous metal smelting, iron and steel industry, battery and fluorescent lamp production) were investigated. Results showed that: (1) The total emissions of Hg, As, Pb, Cd, Cr in Guangdong province were 18.14, 32.59, 411.34, 13.13, 84.16 t, respectively. (2) Different pollutants have obvious characteristics of emission sources. For total Hg emission, 46% comes from combustion sources, of which 32% from coal combustion and 8% from MSW combustion. Other 54% comes from industrial processes, which dominated by the cement (19%), fluorescent lamp (18%) and battery production (13%). Of the total Hg emission, 69% is released as Hg0 , 29% as Hg2+ , and only 2% as Hgp due to strict particulate matters controls policies. For As emissions, coal combustion, nonferrous metal smelting and iron and steel industry contributed approximate 48%, 25% and 24%, respectively. Pb emissions primarily come from battery production (42%), iron and steel industry (21%) and on-road mobile gasoline combustion (17%). Cd and Cr emissions were dominated by nonferrous metal smelting (71%) and iron and steel industry (82%), respectively. (3) In term of the spatial distribution, emissions of atmospheric toxic metals are mainly concentrated in the central region of
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...
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.
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.
An Atmospheric Pressure Plasma Setup to Investigate the Reactive Species Formation.

Science.gov (United States)

Gorbanev, Yury; Soriano, Robert; O'Connell, Deborah; Chechik, Victor

2016-11-03

Non-thermal atmospheric pressure ('cold') plasmas have received increased attention in recent years due to their significant biomedical potential. The reactions of cold plasma with the surrounding atmosphere yield a variety of reactive species, which can define its effectiveness. While efficient development of cold plasma therapy requires kinetic models, model benchmarking needs empirical data. Experimental studies of the source of reactive species detected in aqueous solutions exposed to plasma are still scarce. Biomedical plasma is often operated with He or Ar feed gas, and a specific interest lies in investigation of the reactive species generated by plasma with various gas admixtures (O2, N2, air, H2O vapor, etc.) Such investigations are very complex due to difficulties in controlling the ambient atmosphere in contact with the plasma effluent. In this work, we addressed common issues of 'high' voltage kHz frequency driven plasma jet experimental studies. A reactor was developed allowing the exclusion of ambient atmosphere from the plasma-liquid system. The system thus comprised the feed gas with admixtures and the components of the liquid sample. This controlled atmosphere allowed the investigation of the source of the reactive oxygen species induced in aqueous solutions by He-water vapor plasma. The use of isotopically labelled water allowed distinguishing between the species originating in the gas phase and those formed in the liquid. The plasma equipment was contained inside a Faraday cage to eliminate possible influence of any external field. The setup is versatile and can aid in further understanding the cold plasma-liquid interactions chemistry.
Current sources of carbon tetrachloride (CCl4) in our atmosphere

Science.gov (United States)

Sherry, David; McCulloch, Archie; Liang, Qing; Reimann, Stefan; Newman, Paul A.

2018-02-01

Carbon tetrachloride (CCl4 or CTC) is an ozone-depleting substance whose emissive uses are controlled and practically banned by the Montreal Protocol (MP). Nevertheless, previous work estimated ongoing emissions of 35 Gg year-1 of CCl4 into the atmosphere from observation-based methods, in stark contrast to emissions estimates of 3 (0-8) Gg year-1 from reported numbers to UNEP under the MP. Here we combine information on sources from industrial production processes and legacy emissions from contaminated sites to provide an updated bottom-up estimate on current CTC global emissions of 15-25 Gg year-1. We now propose 13 Gg year-1 of global emissions from unreported non-feedstock emissions from chloromethane and perchloroethylene plants as the most significant CCl4 source. Additionally, 2 Gg year-1 are estimated as fugitive emissions from the usage of CTC as feedstock and possibly up to 10 Gg year-1 from legacy emissions and chlor-alkali plants.

Parsing pyrogenic polycyclic aromatic hydrocarbons: forensic chemistry, receptor models, and source control policy.

Science.gov (United States)

O'Reilly, Kirk T; Pietari, Jaana; Boehm, Paul D

2014-04-01

A realistic understanding of contaminant sources is required to set appropriate control policy. Forensic chemical methods can be powerful tools in source characterization and identification, but they require a multiple-lines-of-evidence approach. Atmospheric receptor models, such as the US Environmental Protection Agency (USEPA)'s chemical mass balance (CMB), are increasingly being used to evaluate sources of pyrogenic polycyclic aromatic hydrocarbons (PAHs) in sediments. This paper describes the assumptions underlying receptor models and discusses challenges in complying with these assumptions in practice. Given the variability within, and the similarity among, pyrogenic PAH source types, model outputs are sensitive to specific inputs, and parsing among some source types may not be possible. Although still useful for identifying potential sources, the technical specialist applying these methods must describe both the results and their inherent uncertainties in a way that is understandable to nontechnical policy makers. The authors present an example case study concerning an investigation of a class of parking-lot sealers as a significant source of PAHs in urban sediment. Principal component analysis is used to evaluate published CMB model inputs and outputs. Targeted analyses of 2 areas where bans have been implemented are included. The results do not support the claim that parking-lot sealers are a significant source of PAHs in urban sediments. © 2013 SETAC.
Study on surface modification of polymer films by using atmospheric plasma jet source

International Nuclear Information System (INIS)

Takemura, Yuichiro; Hara, Tamio; Yamaguchi, Naohiro

2008-01-01

Reactive gas plasma treatments of poly(ethylene terephthalate) (PET) and polyimide (Kapton) have been performed using an atmospheric plasmas jet source. Characteristics of surface modification have been examined by changing the distance between the plasma jet source and the treated sample, and by changing the working gas spaces. Simultaneously, each plasma jet source has been investigated by space-resolving spectroscopy in the UV/visible region. Polymer surfaces have been analyzed by X-ray photoelectron spectroscopy (XPS). A marked improvement in the hydrophilicity of the polymer surfaces has been made by using N 2 or O 2 plasma jet source with a very short exposure time of about 0.01 s, whereas the less improvement has been obtained using on air plasma jet source because of NO x compound production. Changes in the chemical states of C of the polymer surfaces have been observed in XPS spectra after N 2 plasma jet spraying. (author)
Atmospheric mercury emissions in Australia from anthropogenic, natural and recycled sources

Science.gov (United States)

Nelson, Peter F.; Morrison, Anthony L.; Malfroy, Hugh J.; Cope, Martin; Lee, Sunhee; Hibberd, Mark L.; Meyer, C. P. (Mick); McGregor, John

2012-12-01

The United Nations Environment Programme (UNEP) has begun a process of developing a legally binding instrument to manage emissions of mercury from anthropogenic sources. The UNEP Governing Council has concluded that there is sufficient evidence of significant global adverse impacts from mercury to warrant further international action; and that national, regional and global actions should be initiated as soon as possible to identify populations at risk and to reduce human generated releases. This paper describes the development of, and presents results from, a comprehensive, spatially and temporally resolved inventory of atmospheric mercury emissions from the Australian landmass. Results indicate that the best estimate of total anthropogenic emissions of mercury to the atmosphere in 2006 was 15 ± 5 tonnes. Three industrial sectors contribute substantially to Australian anthropogenic emissions: gold smelting (˜50%, essentially from a single site/operation), coal combustion in power plants (˜15%) and alumina production from bauxite (˜12%). A diverse range of other sectors contribute smaller proportions of the emitted mercury, but industrial emissions account for around 90% of total anthropogenic mercury emissions. The other sectors include other industrial sources (mining, smelting, and cement production) and the use of products containing mercury. It is difficult to determine historical trends in mercury emissions given the large uncertainties in the data. Estimates for natural and re-emitted emissions from soil, water, vegetation and fires are made using meteorological models, satellite observations of land cover and soil and vegetation type, fuel loading, fire scars and emission factors which account for the effects of temperature, insolation and other environmental variables. These natural and re-emitted sources comfortably exceed the anthropogenic emissions, and comprise 4-12 tonnes per year from vegetation, 70-210 tonnes per year from soils, and 21-63 tonnes
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...
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.
Heavy Metals in Contaminated Soils: A Review of Sources, Chemistry, Risks and Best Available Strategies for Remediation

OpenAIRE

Wuana, Raymond A.; Okieimen, Felix E.

2011-01-01

Scattered literature is harnessed to critically review the possible sources, chemistry, potential biohazards and best available remedial strategies for a number of heavy metals (lead, chromium, arsenic, zinc, cadmium, copper, mercury and nickel) commonly found in contaminated soils. The principles, advantages and disadvantages of immobilization, soil washing and phytoremediation techniques which are frequently listed among the best demonstrated available technologies for cleaning up heavy met...
Iron Oxide Minerals in Atmospheric Dust and Source Sediments-Studies of Types and Properties to Assess Environmental Effects

Science.gov (United States)

Reynolds, R. L.; Goldstein, H. L.; Moskowitz, B. M.; Till, J. L.; Flagg, C.; Kokaly, R. F.; Munson, S.; Landry, C.; Lawrence, C. R.; Hiza, M. M.; D'Odorico, P.; Painter, T. H.

2011-12-01

Ferric oxide minerals in atmospheric dust can influence atmospheric temperatures, accelerate melting of snow and ice, stimulate marine phytoplankton productivity, and impact human health. Such effects vary depending on iron mineral type, size, surface area, and solubility. Generally, the presence of ferric oxides in dust is seen in the red, orange, or yellow hues of plumes that originate in North Africa, central and southwest Asia, South America, western North America, and Australia. Despite their global importance, these minerals in source sediments, atmospheric dust, and downwind aeolian deposits remain poorly described with respect to specific mineralogy, particle size and surface area, or presence in far-traveled aerosol compounds. The types and properties of iron minerals in atmospheric dust can be better understood using techniques of rock magnetism (measurements at 5-300 K), Mössbauer and high-resolution visible and near-infrared reflectance spectroscopy; chemical reactivity of iron oxide phases; and electron microscopy for observing directly the ferric oxide coatings and particles. These studies can elucidate the diverse environmental effects of iron oxides in dust and can help to identify dust-source areas. Dust-source sediments from the North American Great Basin and Colorado Plateau deserts and the Kalahari Desert, southern Africa, were used to compare average reflectance values with a magnetic parameter (hard isothermal remanent magnetization, HIRM) for ferric oxide abundance. Lower reflectance values correspond strongly with higher HIRM values, indicating that ferric oxides (hematite or goethite, or both) contribute to absorption of solar radiation in these sediments. Dust deposited to snow cover of the San Juan Mountains (Colorado) and Wasatch Mountains (Utah) was used to characterize dust composition compared with properties of sediments exposed in source-areas identified from satellite retrievals. Results from multiple methods indicate that
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
Characterization of an atmospheric pressure air plasma source for polymer surface modification

Science.gov (United States)

Yang, Shujun; Tang, Jiansheng

2013-10-01

An atmospheric pressure air plasma source was generated through dielectric barrier discharge (DBD). It was used to modify polyethyleneterephthalate (PET) surfaces with very high throughput. An equivalent circuit model was used to calculate the peak average electron density. The emission spectrum from the plasma was taken and the main peaks in the spectrum were identified. The ozone density in the down plasma region was estimated by Absorption Spectroscopy. NSF and ARC-ODU
GPU-accelerated atmospheric chemical kinetics in the ECHAM/MESSy (EMAC Earth system model (version 2.52

Directory of Open Access Journals (Sweden)

M. Alvanos

2017-10-01

Full Text Available This paper presents an application of GPU accelerators in Earth system modeling. We focus on atmospheric chemical kinetics, one of the most computationally intensive tasks in climate–chemistry model simulations. We developed a software package that automatically generates CUDA kernels to numerically integrate atmospheric chemical kinetics in the global climate model ECHAM/MESSy Atmospheric Chemistry (EMAC, used to study climate change and air quality scenarios. A source-to-source compiler outputs a CUDA-compatible kernel by parsing the FORTRAN code generated by the Kinetic PreProcessor (KPP general analysis tool. All Rosenbrock methods that are available in the KPP numerical library are supported.Performance evaluation, using Fermi and Pascal CUDA-enabled GPU accelerators, shows achieved speed-ups of 4. 5 × and 20. 4 × , respectively, of the kernel execution time. A node-to-node real-world production performance comparison shows a 1. 75 × speed-up over the non-accelerated application using the KPP three-stage Rosenbrock solver. We provide a detailed description of the code optimizations used to improve the performance including memory optimizations, control code simplification, and reduction of idle time. The accuracy and correctness of the accelerated implementation are evaluated by comparing to the CPU-only code of the application. The median relative difference is found to be less than 0.000000001 % when comparing the output of the accelerated kernel the CPU-only code.The approach followed, including the computational workload division, and the developed GPU solver code can potentially be used as the basis for hardware acceleration of numerous geoscientific models that rely on KPP for atmospheric chemical kinetics applications.
Microbiology and atmospheric processes: an upcoming era of research on bio-meteorology

Science.gov (United States)

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

2008-01-01

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.
A Planar Source of Atmospheric-Pressure Plasma Jet

Science.gov (United States)

Zhdanova, O. S.; Kuznetsov, V. S.; Panarin, V. A.; Skakun, V. S.; Sosnin, E. A.; Tarasenko, V. F.

2018-01-01

In a single-barrier discharge with voltage sharpening and low gas consumption (up to 1 L/min), plane atmospheric pressure plasma jets with a width of up to 3 cm and length of up to 4 cm in air are formed in the slit geometry of the discharge zone. The energy, temperature, and spectral characteristics of the obtained jets have been measured. The radiation spectrum contains intense maxima corresponding to vibrational transitions of the second positive system of molecular nitrogen N2 ( C 3Π u → B 3Π g ) and comparatively weak transition lines of the first positive system of the N 2 + ion ( B 2Σ u + → X 2Σ g ). By an example of inactivation of the Staphylococcus aureus culture (strain ATCC 209), it is shown that plasma is a source of chemically active particles providing the inactivation of microorganisms.
Landfill is an important atmospheric mercury emission source

Institute of Scientific and Technical Information of China (English)

FENG Xinbin; TANG Shunlin; LI Zhonggen; WANG Shaofeng; LIANG Lian

2004-01-01

Since municipal wastes contain refuses with high mercury contents, incineration of municipal wastes becomes the major anthropogenic atmospheric mercury emission source. In China, landfills are however the main way to dispose of municipal wastes. Total gaseous mercury (TGM) concentrations in landfill gas of Gaoyan sanitary landfill located in suburb of Guiyang City were monitored using a high temporal resolved automated mercury analyzer, and mono-methylmercury (MMHg) and dimethylmercury (DMHg) concentrations in landfill gas were also measured using GC coupled with the cold vapor atomic fluorescence (CVAFS) method. Meanwhile, the TGM exchange fluxes between exposed waste and air and the soil surface of the landfill and air, were measured using low Hg blank quartz flux chamber coupled with high temporal resolved automated mercury analyzer technique. TGM concentrations in landfill gas from half year filling area averaged out at 665.52±291.25 ng/m3, which is comparable with TGM concentrations from flue gas of a small coal combustion boiler in Guiyang. The average MMHg and DMHg concentrations averaged out at 2.06±1.82 ng/m3 and 9.50±5.18 ng/m3, respectively. It is proven that mercury emission is the predominant process at the surfaces of both exposed wastes and soil of landfill. Landfills are not only TGM emission source, but also methylmercury emission source to the ambient air. There are two ways to emit mercury to the air from landfills, one is with the landfill gas through landfill gas duct, and the other through soil/air exchange. The Hg emission processes from landfills are controlled by meteorological parameters.
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.
Atmospheric aerosol compositions and sources at two national background sites in northern and southern China

Science.gov (United States)

Zhu, Qiao; He, Ling-Yan; Huang, Xiao-Feng; Cao, Li-Ming; Gong, Zhao-Heng; Wang, Chuan; Zhuang, Xin; Hu, Min

2016-08-01

Although China's severe air pollution has become a focus in the field of atmospheric chemistry and the mechanisms of urban air pollution there have been researched extensively, few field sampling campaigns have been conducted at remote background sites in China, where air pollution characteristics on a larger scale are highlighted. In this study, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), together with an Aethalometer, was deployed at two of China's national background sites in northern (Lake Hongze site; 33.23° N, 118.33° E; altitude 21 m) and southern (Mount Wuzhi site; 18.84° N, 109.49° E; altitude 958 m) China in the spring seasons in 2011 and 2015, respectively, in order to characterize submicron aerosol composition and sources. The campaign-average PM1 concentration was 36.8 ± 19.8 µg m-3 at the northern China background (NCB) site, which was far higher than that at the southern China background (SCB) site (10.9 ± 7.8 µg m-3). Organic aerosol (OA) (27.2 %), nitrate (26.7 %), and sulfate (22.0 %) contributed the most to the PM1 mass at NCB, while OA (43.5 %) and sulfate (30.5 %) were the most abundant components of the PM1 mass at SCB, where nitrate only constituted a small fraction (4.7 %) and might have contained a significant amount of organic nitrates (5-11 %). The aerosol size distributions and organic aerosol elemental compositions all indicated very aged aerosol particles at both sites. The OA at SCB was more oxidized with a higher average oxygen to carbon (O / C) ratio (0.98) than that at NCB (0.67). Positive matrix factorization (PMF) analysis was used to classify OA into three components, including a hydrocarbon-like component (HOA, attributed to fossil fuel combustion) and two oxygenated components (OOA1 and OOA2, attributed to secondary organic aerosols from different source areas) at NCB. PMF analysis at SCB identified a semi-volatile oxygenated component (SV-OOA) and a low-volatility oxygenated
Photoionization mass spectrometer for studies of flame chemistry with a synchrotron light source

International Nuclear Information System (INIS)

Cool, Terrill A.; McIlroy, Andrew; Qi, Fei; Westmoreland, Phillip R.; Poisson, Lionel; Peterka, Darcy S.; Ahmed, Musahid

2005-01-01

A flame-sampling molecular-beam photoionization mass spectrometer, recently designed and constructed for use with a synchrotron-radiation light source, provides significant improvements over previous molecular-beam mass spectrometers that have employed either electron-impact ionization or vacuum ultraviolet laser photoionization. These include superior signal-to-noise ratio, soft ionization, and photon energies easily and precisely tunable [E/ΔE(FWHM)≅250-400] over the 7.8-17-eV range required for quantitative measurements of the concentrations and isomeric compositions of flame species. Mass resolution of the time-of-flight mass spectrometer is m/Δm=400 and sensitivity reaches ppm levels. The design of the instrument and its advantages for studies of flame chemistry are discussed
Seasonal variations in the sources of natural and anthropogenic lead deposited at the East Rongbuk Glacier in the high-altitude Himalayas.

Science.gov (United States)

Burn-Nunes, Laurie; Vallelonga, Paul; Lee, Khanghyun; Hong, Sungmin; Burton, Graeme; Hou, Shugui; Moy, Andrew; Edwards, Ross; Loss, Robert; Rosman, Kevin

2014-07-15

Lead (Pb) isotopic compositions and concentrations, and barium (Ba) and indium (In) concentrations have been analysed at sub-annual resolution in three sections from a snow pit samples dated to 2004/2005, recovered from the East Rongbuk Glacier in the high-altitude Himalayas. Ice core sections indicate that atmospheric chemistry prior to ~1,953 was controlled by mineral dust inputs, with no discernible volcanic or anthropogenic contributions. Eighteenth century monsoon ice core chemistry is indicative of dominant contributions from local Himalayan sources; non-monsoon ice core chemistry is linked to contributions from local (Himalayan), regional (Indian/Thar Desert) and long-range (North Africa, Central Asia) sources. Twentieth century monsoon and non-monsoon ice core data demonstrate similar seasonal sources of mineral dust, however with a transition to less-radiogenic isotopic signatures that suggests local and regional climate/environmental change. The snow pit record demonstrates natural and anthropogenic contributions during both seasons, with increased anthropogenic influence during non-monsoon times. Monsoon anthropogenic inputs are most likely sourced to South/South-East Asia and/or India, whereas non-monsoon anthropogenic inputs are most likely sourced to India and Central Asia. Copyright © 2014 Elsevier B.V. All rights reserved.
The Approximate Bayesian Computation methods in the localization of the atmospheric contamination source

International Nuclear Information System (INIS)

Kopka, P; Wawrzynczak, A; Borysiewicz, M

2015-01-01

In many areas of application, a central problem is a solution to the inverse problem, especially estimation of the unknown model parameters to model the underlying dynamics of a physical system precisely. In this situation, the Bayesian inference is a powerful tool to combine observed data with prior knowledge to gain the probability distribution of searched parameters. We have applied the modern methodology named Sequential Approximate Bayesian Computation (S-ABC) to the problem of tracing the atmospheric contaminant source. The ABC is technique commonly used in the Bayesian analysis of complex models and dynamic system. Sequential methods can significantly increase the efficiency of the ABC. In the presented algorithm, the input data are the on-line arriving concentrations of released substance registered by distributed sensor network from OVER-LAND ATMOSPHERIC DISPERSION (OLAD) experiment. The algorithm output are the probability distributions of a contamination source parameters i.e. its particular location, release rate, speed and direction of the movement, start time and duration. The stochastic approach presented in this paper is completely general and can be used in other fields where the parameters of the model bet fitted to the observable data should be found. (paper)
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
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.

Source apportionment of particulate pollutants in the atmosphere over the Northern Yellow Sea

Science.gov (United States)

Wang, L.; Qi, J. H.; Shi, J. H.; Chen, X. J.; Gao, H. W.

2013-05-01

Atmospheric aerosol samples were collected over the Northern Yellow Sea of China during the years of 2006 and 2007, in which the Total Carbon (TC), Cu, Pb, Cd, V, Zn, Fe, Al, Na+, Ca2+, Mg2+, NH4+, NO3-, SO42-, Cl-, and K+ were measured. The principle components analysis (PCA) and positive matrix factorization (PMF) receptor models were used to identify the sources of particulate matter. The results indicated that seven factors contributed to the atmospheric particles over the Northern Yellow Sea, i.e., two secondary aerosols (sulfate and nitrate), soil dust, biomass burning, oil combustion, sea salt, and metal smelting. When the whole database was considered, secondary aerosol formation contributed the most to the atmospheric particle content, followed by soil dust. Secondary aerosols and soil dust consisted of 65.65% of the total mass of particulate matter. The results also suggested that the aerosols over the North Yellow Sea were heavily influenced by ship emission over the local sea area and by continental agricultural activities in the northern China, indicating by high loading of V in oil combustion and high loading of K+ in biomass burning. However, the contribution of each factor varied greatly over the different seasons. In spring and autumn, soil dust and biomass burning were the dominant factors. In summer, heavy oil combustion contributed the most among these factors. In winter, secondary aerosols were major sources. Backward trajectories analysis indicated the 66% of air mass in summer was from the ocean, while the air mass is mainly from the continent in other seasons.
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...
Isotopic evidence for enhanced fossil fuel sources of aerosol ammonium in the urban atmosphere.

Science.gov (United States)

Pan, Yuepeng; Tian, Shili; Liu, Dongwei; Fang, Yunting; Zhu, Xiaying; Gao, Meng; Gao, Jian; Michalski, Greg; Wang, Yuesi

2018-04-20

The sources of aerosol ammonium (NH 4 + ) are of interest because of the potential of NH 4 + to impact the Earth's radiative balance, as well as human health and biological diversity. Isotopic source apportionment of aerosol NH 4 + is challenging in the urban atmosphere, which has excess ammonia (NH 3 ) and where nitrogen isotopic fractionation commonly occurs. Based on year-round isotopic measurements in urban Beijing, we show the source dependence of the isotopic abundance of aerosol NH 4 + , with isotopically light (-33.8‰) and heavy (0 to +12.0‰) NH 4 + associated with strong northerly winds and sustained southerly winds, respectively. On an annual basis, 37-52% of the initial NH 3 concentrations in urban Beijing arises from fossil fuel emissions, which are episodically enhanced by air mass stagnation preceding the passage of cold fronts. These results provide strong evidence for the contribution of non-agricultural sources to NH 3 in urban regions and suggest that priority should be given to controlling these emissions for haze regulation. This study presents a carefully executed application of existing stable nitrogen isotope measurement and mass-balance techniques to a very important problem: understanding source contributions to atmospheric NH 3 in Beijing. This question is crucial to informing environmental policy on reducing particulate matter concentrations, which are some of the highest in the world. However, the isotopic source attribution results presented here still involve a number of uncertain assumptions and they are limited by the incomplete set of chemical and isotopic measurements of gas NH 3 and aerosol NH 4 + . Further field work and lab experiments are required to adequately characterize endmember isotopic signatures and the subsequent isotopic fractionation process under different air pollution and meteorological conditions. Copyright © 2018 Elsevier Ltd. All rights reserved.
Atmospheric Production of Perchlorate on Earth and Mars

Science.gov (United States)

Claire, M.; Catling, D. C.; Zahnle, K. J.

2009-12-01

Natural production and preservation of perchlorate on Earth occurs only in arid environments. Isotopic evidence suggests a strong role for atmospheric oxidation of chlorine species via pathways including ozone or its photochemical derivatives. As the Martian atmosphere is both oxidizing and drier than the driest places on Earth, we propose an atmospheric origin for the Martian perchlorates measured by NASA's Phoenix Lander. A variety of hypothetical formation pathways can be proposed including atmospheric photochemical reactions, electrostatic discharge, and gas-solid reactions. Here, we investigate gas phase formation pathways using a 1-D photochemical model (Catling et al. 2009, accepted by JGR). Because perchlorate-rich deposits in the Atacama desert are closest in abundance to perchlorate measured at NASA's Phoenix Lander site, we start with a study of the means to produce Atacama perchlorate. We found that perchlorate can be produced in sufficient quantities to explain the abundance of perchlorate in the Atacama from a proposed gas phase oxidation of chlorine volatiles to perchloric acid. These results are sensitive to estimated reaction rates for ClO3 species. The feasibility of gas phase production for the Atacama provides justification for further investigations of gas phase photochemistry as a possible source for Martian perchlorate. In addition to the Atacama results, we will present a preliminary study incorporating chlorine chemistry into an existing Martian photochemical model (Zahnle et al. JGR 2008).
Source-receptor probability of atmospheric long-distance dispersal of viruses to Israel from the eastern Mediterranean area.

Science.gov (United States)

Klausner, Z; Klement, E; Fattal, E

2018-02-01

Viruses that affect the health of humans and farm animals can spread over long distances via atmospheric mechanisms. The phenomenon of atmospheric long-distance dispersal (LDD) is associated with severe consequences because it may introduce pathogens into new areas. The introduction of new pathogens to Israel was attributed to LDD events numerous times. This provided the motivation for this study which is aimed to identify all the locations in the eastern Mediterranean that may serve as sources for pathogen incursion into Israel via LDD. This aim was achieved by calculating source-receptor relationship probability maps. These maps describe the probability that an infected vector or viral aerosol, once airborne, will have an atmospheric route that can transport it to a distant location. The resultant probability maps demonstrate a seasonal tendency in the probability of specific areas to serve as sources for pathogen LDD into Israel. Specifically, Cyprus' season is the summer; southern Turkey and the Greek islands of Crete, Karpathos and Rhodes are associated with spring and summer; lower Egypt and Jordan may serve as sources all year round, except the summer months. The method used in this study can easily be implemented to any other geographic region. The importance of this study is the ability to provide a climatologically valid and accurate risk assessment tool to support long-term decisions regarding preparatory actions for future outbreaks long before a specific outbreak occurs. © 2017 Blackwell Verlag GmbH.
Source-receptor relationships for atmospheric mercury in urban Detroit, Michigan

Science.gov (United States)

Lynam, Mary M.; Keeler, Gerald J.

Speciated hourly mercury measurements were made in Detroit, Michigan during four sampling campaigns from 2000 to 2002. In addition, other chemical and meteorological parameters were measured concurrently. These data were analyzed using principal components analysis (PCA) in order to develop source receptor relationships for mercury species in urban Detroit. Reactive gaseous mercury (RGM) was found to cluster on two main factors; photochemistry and a coal combustion factor. Particulate phase mercury, Hg p, tended to cluster with RGM on the same factor. The photochemistry factor corroborates previous observations of the presence of RGM in highly oxidizing atmospheres and does not point to a specific source emission type. Instead, it likely represents local emissions and regional transport of photochemically processed air masses. The coal combustion factor is indicative of emissions from coal-fired power plants near the receptor site. Elemental mercury was found on a factor for combustion from automobiles and points to the influence these emissions have on the receptor site, which was located proximate to two major interstate highways and the largest border crossing in the United States. This analysis reveals that the receptor site which is located in an industrialized sector of the city of Detroit experienced impacts from both stationary and point sources of mercury that are both local and regional in nature.
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)
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...
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.
Effects of continental anthropogenic sources on organic aerosols in the coastal atmosphere of East China.

Science.gov (United States)

Shang, Dongjie; Hu, Min; Guo, Qingfeng; Zou, Qi; Zheng, Jing; Guo, Song

2017-10-01

Although organic compounds in marine atmospheric aerosols have significant effects on climate and marine ecosystems, they have rarely been studied, especially in the coastal regions of East China. To assess the origins of the organic aerosols in the East China coastal atmosphere, PM 2.5 samples were collected from the atmospheres of the Yellow Sea, the East China Sea, and Changdao Island during the CAPTAIN (Campaign of Air PolluTion At INshore Areas of Eastern China) field campaign in the spring of 2011. The marine atmospheric aerosol samples that were collected were grouped based on the backward trajectories of their air masses. The organic carbon concentrations in the PM 2.5 samples from the marine and Changdao Island atmospheres were 5.5 ± 3.1 μgC/m 3 and 6.9 ± 2.4 μgC/m 3 , respectively, which is higher than in other coastal water atmospheres. The concentration of polycyclic aromatic hydrocarbons (PAHs) in the marine atmospheric PM 2.5 samples was 17.0 ± 20.2 ng/m 3 , indicating significant continental anthropogenic influences. The influences of fossil fuels and biomass burning on the composition of organic aerosols in the coastal atmosphere of East China were found to be highly dependent on the origins of the air masses. Diesel combustion had a strong impact on air masses from the Yangtze River Delta (YRD), and gasoline emissions had a more significant impact on the "North China" marine atmospheric samples. The "Northeast China" marine atmospheric samples were most impacted by biomass burning. Coal combustion contributed significantly to the compositions of all of the atmospheric samples. The proportions of secondary compounds increased as samples aged in the marine atmosphere indicating that photochemical oxidation occured during transport. Our results quantified ecosystem effects on marine atmospheric aerosols and highlighted the uncertainties that arise when modeling marine atmospheric PM 2.5 without considering high spatial resolution source
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.
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.
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.
Oxygenated Organic Chemicals in the Pacific Troposphere: Distribution, Sources and Chemistry

Science.gov (United States)

Singh, Hanwant B.; Salas, L.; Chatfield, R.; Czech, E.; Fried, A.; Evans, M.; Jacob, D. J.; Blake, D.; Heikes, B.; Talbot, R.

2003-01-01

Airborne measurements of a large number of oxygenated organic chemicals (Oxorgs) were carried out in the Pacific troposphere (0.1-12 km) in the Spring of 2001 (Feb. 24-April 10). Specifically these measuremen ts included acetone, methylethyl ketone (MEK), methanol, ethanol, ace taldehyde, propionaldehyde, PANS, and organic nitrates. Complementary measurements of formaldehyde, organic peroxides, and tracers were al so available. Ox-orgs were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Their mixing ratios were typically highest in the lower troposphere and declined toward s the upper troposphere and the lowermost stratosphere. Their total a bundance (Ox-orgs) significantly exceeded that of NMHC (C2-C8 NMHC). A comparison of these data with observations collected some seven yea rs earlier (Feb.-March, 1994), did not reveal any significant changes . Throughout the troposphere mixing ratios of Ox-orgs were strongly c orrelated with each other as well as with tracers of fossil and bioma sshiof'uel combustion. Analysis of the relative enhancement of selected Oxorgs with respect to CH3Cl and CO in twelve sampled plumes, origi nating from fires, is used to assess their primary and secondary sour ces from biomass combustion. The composition of these plumes also ind icates a large shift of reactive nitrogen into the PAN reservoir ther eby limiting ozone formation. The Harvard 3-D photochemical model, th at uses state of the art chemistry and source information, is used to compare simulated and observed mixing ratios of selected species. A 1 -D model is used to explore the chemistry of aldehydes. These results will be presented.
Biogenic non-methane hydrocarbons (NMHC). Nature`s contribution to regional and global atmospheric chemistry

Energy Technology Data Exchange (ETDEWEB)

Klockow, D.; Hoffman, T. [Inst. of Spectrochemistry and Applied Spectroscopy, Dortmund (Germany)

1995-12-31

Terrestrial vegetation provides an important source of volatile hydrocarbons, especially isoprene, monoterpenes and in addition possibly sesquiterpenes as well as oxygenated compounds. Although there exist considerable uncertainties in the estimation of the magnitude of these biogenic NMHC emissions, it is generally accepted that the majority of global NMHC release is from natural and not from anthropogenic sources. Taking into consideration the high reactivity of the mostly unsaturated biogenic emissions, their impact on tropospheric processes can be assumed to be of great importance. Together with anthropogenic NO{sub x} emissions, the highly reactive natural alkenes can act as precursors in photochemical oxidant formation and contribute to regional-scale air pollution. Their oxidation in the atmosphere and the subsequent gas-to-particle conversion of the products lead to the formation of organic aerosols. Because of the formation of phytotoxic compounds, the interaction of the biogenic hydrocarbons with ozone inside or outside the leaves and needles of plants has been suggested to play a role in forest decline. (author)
Biogenic non-methane hydrocarbons (NMHC). Nature`s contribution to regional and global atmospheric chemistry

Energy Technology Data Exchange (ETDEWEB)

Klockow, D; Hoffman, T [Inst. of Spectrochemistry and Applied Spectroscopy, Dortmund (Germany)

1996-12-31

Terrestrial vegetation provides an important source of volatile hydrocarbons, especially isoprene, monoterpenes and in addition possibly sesquiterpenes as well as oxygenated compounds. Although there exist considerable uncertainties in the estimation of the magnitude of these biogenic NMHC emissions, it is generally accepted that the majority of global NMHC release is from natural and not from anthropogenic sources. Taking into consideration the high reactivity of the mostly unsaturated biogenic emissions, their impact on tropospheric processes can be assumed to be of great importance. Together with anthropogenic NO{sub x} emissions, the highly reactive natural alkenes can act as precursors in photochemical oxidant formation and contribute to regional-scale air pollution. Their oxidation in the atmosphere and the subsequent gas-to-particle conversion of the products lead to the formation of organic aerosols. Because of the formation of phytotoxic compounds, the interaction of the biogenic hydrocarbons with ozone inside or outside the leaves and needles of plants has been suggested to play a role in forest decline. (author)
Atmospheric methane isotopic record favors fossil sources flat in 1980s and 1990s with recent increase

Science.gov (United States)

Rice, Andrew L.; Butenhoff, Christopher L.; Teama, Doaa G.; Röger, Florian H.; Khalil, M. Aslam K.; Rasmussen, Reinhold A.

2016-09-01

Observations of atmospheric methane (CH4) since the late 1970s and measurements of CH4 trapped in ice and snow reveal a meteoric rise in concentration during much of the twentieth century. Since 1750, levels of atmospheric CH4 have more than doubled to current globally averaged concentration near 1,800 ppb. During the late 1980s and 1990s, the CH4 growth rate slowed substantially and was near or at zero between 1999 and 2006. There is no scientific consensus on the drivers of this slowdown. Here, we report measurements of the stable isotopic composition of atmospheric CH4 (13C/12C and D/H) from a rare air archive dating from 1977 to 1998. Together with more modern records of isotopic atmospheric CH4, we performed a time-dependent retrieval of methane fluxes spanning 25 y (1984-2009) using a 3D chemical transport model. This inversion results in a 24 [18, 27] Tg y-1 CH4 increase in fugitive fossil fuel emissions since 1984 with most of this growth occurring after year 2000. This result is consistent with some bottom-up emissions inventories but not with recent estimates based on atmospheric ethane. In fact, when forced with decreasing emissions from fossil fuel sources our inversion estimates unreasonably high emissions in other sources. Further, the inversion estimates a decrease in biomass-burning emissions that could explain falling ethane abundance. A range of sensitivity tests suggests that these results are robust.
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.
Sources of atmospheric aerosols controlling PM10 levels in Heraklion, Crete during winter time

Science.gov (United States)

Kalivitis, Nikolaos; Kouvarakis, Giorgos; Stavroulas, Iasonas; Kandilogiannaki, Maria; Vavadaki, Katerina; Mihalopoulos, Nikolaos

2016-04-01

High concentrations of Particulate Matter (PM) in the atmosphere have negative impact to human health. Thresholds for ambient concentrations that are defined by the directive 2008/50/EC are frequently exceeded even at background conditions in the Mediterranean region as shown in earlier studies. The sources of atmospheric particles in the urban environment of a medium size city of eastern Mediterranean are studied in the present work in order to better understand the causes and characteristics of exceedances of the daily mean PM10limit value of 50 μg m-3. Measurements were performed at the atmospheric quality measurement station of the Region of Crete, at the Heraklion city center on Crete island, during the winter/spring period of 2014-2015 and 2015-2016. Special emphasis was given to the study of the contribution of Black Carbon (BC) to the levels of PM10. Continuous measurements were performed using a beta-attenuation PM10monitor and a 7-wavelength Aethalometer with a time resolution of 30 and 5 minutes respectively. For direct comparison to background regional conditions, concurrent routine measurements at the atmospheric research station of University of Crete at Finokalia were used as background reference. Analysis of exceedances in the daily PM10 mass concentration showed that the total of the exceedances was related to long range transport of Saharan dust rather than local sources. However, compared to the Finokalia station it was found that there were 20% more exceedances in Heraklion, the addition of transported dust on the local pollution was the reason for the additional exceedance days. Excluding dust events, it was found that the PM10variability was dependent on the BC abundance, traffic during rush hours in the morning and biomass burning for domestic heating in the evening contributed significantly to PM10levels in Heraklion.
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

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