WorldWideScience

Sample records for upper troposphere chemistry

  1. The role of chemistry in under-predictions of NO2 in the upper troposphere

    Science.gov (United States)

    Henderson, B. H.; Pinder, R. W.; Goliff, W. S.; Stockwell, W. R.; Fahr, A.; Sarwar, G.; Hutzell, W. T.; Mathur, R.; Vizuete, W.; Cohen, R. C.

    2009-12-01

    Global and regional atmospheric models under-predict upper troposphere NO2 compared to satellite and aircraft observations. The upper tropospheric under-prediction of NO2 could be a function of emissions, transport, chemistry or some combination. Previous researchers have linked poor performance in the model to over-prediction of the OH and under-prediction of the HO2 by chemistry (Olson et al. 2006, Bertram et al. 2007). This study isolates upper tropospheric chemistry to evaluate the chemical contribution to NO2 under-predictions and to diagnose OH and HO2 discrepancies. We use a 0-dimensional time dependent model to evaluate seven chemical mechanisms. Because chamber data representing upper tropospheric conditions does not exist, we evaluate the predictions based against an observation-based aging model. Following Bertram et al (2007), we use the NOx:HNO3 ratio to categorize the chemical age of thousands of 10 second average observations between 8 and 10km. Measurements of 10 inorganics and 32 hydrocarbons are translated to model species for each of seven chemical mechanisms. We chose mechanisms ranging from condensed to semi-explicit. The seven mechanisms' design scopes range from urban to global scale. Results include simulations from Model for OZone And Related chemical Tracers (MOZART), Carbon Bond 05 (CB05), State Air Pollution Research Center (SAPRC) 99, SAPRC 07, GEOS-Chem, Regional Atmospheric Chemical Mechanism version 2, and the LEEDS Master Chemical Mechanism. Results from each chemical mechanism are compared to aircraft observations and to those obtained with other chemical mechanisms. Each mechanism is then further evaluated using integrated reaction rate analysis to identify sources of NO2 bias. We find that the largest contributors to the NO2 bias are over-predictions of PAN and HNO3. The formation of PAN is sensitive to the acetone photolysis rate. The conversion of NOx to HNO3 is most sensitive to hydroxyl radical concentrations. Hydroxyl

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

    Science.gov (United States)

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

    2013-01-01

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

  3. 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

  4. Evaluating Lightning-generated NOx (LNOx) Parameterization based on Cloud Top Height at Resolutions with Partially-resolved Convection for Upper Tropospheric Chemistry Studies

    Science.gov (United States)

    Wong, J.; Barth, M. C.; Noone, D. C.

    2012-12-01

    Lightning-generated nitrogen oxides (LNOx) is an important precursor to tropospheric ozone production. With a meteorological time-scale variability similar to that of the ozone chemical lifetime, it can nonlinearly perturb tropospheric ozone concentration. Coupled with upper-air circulation patterns, LNOx can accumulate in significant amount in the upper troposphere with other precursors, thus enhancing ozone production (see attached figure). While LNOx emission has been included and tuned extensively in global climate models, its inclusions in regional chemistry models are seldom tested. Here we present a study that evaluates the frequently used Price and Rind parameterization based on cloud-top height at resolutions that partially resolve deep convection using the Weather Research and Forecasting model with Chemistry (WRF-Chem) over the contiguous United States. With minor modifications, the parameterization is shown to generate integrated flash counts close to those observed. However, the modeled frequency distribution of cloud-to-ground flashes do not represent well for storms with high flash rates, bringing into question the applicability of the intra-cloud/ground partitioning (IC:CG) formulation of Price and Rind in some studies. Resolution dependency also requires attention when sub-grid cloud-tops are used instead of the originally intended grid-averaged cloud-top. LNOx passive tracers being gathered by monsoonal upper tropospheric anticyclone.

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

    Science.gov (United States)

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

    2013-06-01

    Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short lifetime and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere, where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) version 3.0 data set. We report observations of PAN in boreal biomass burning plumes recorded during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) campaign (12 July to 3 August 2011). The retrieval method employed by incorporating laboratory-recorded absorption cross sections into version 3.0 of the ACE-FTS forward model and retrieval software is described in full detail. The estimated detection limit for ACE-FTS PAN is 5 pptv, and the total systematic error contribution to the ACE-FTS PAN retrieval is ~ 16%. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) Environmental Satellite (ENVISAT). The MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN, where the measured VMR values are well within the associated measurement errors for both instruments and comparative

  6. Factors controlling upper tropospheric relative humidity

    Directory of Open Access Journals (Sweden)

    B. Kärcher

    2004-03-01

    Full Text Available Factors controlling the distribution of relative humidity in the absence of clouds are examined, with special emphasis on relative humidity over ice (RHI under upper tropospheric and lower stratospheric conditions. Variations of temperature are the key determinant for the distribution of RHI, followed by variations of the water vapor mixing ratio. Multiple humidity modes, generated by mixing of different air masses, may contribute to the overall distribution of RHI, in particular below ice saturation. The fraction of air that is supersaturated with respect to ice is mainly determined by the distribution of temperature. The nucleation of ice in cirrus clouds determines the highest relative humdity that can be measured outside of cirrus clouds. While vertical air motion and ice microphysics determine the slope of the distributions of RHI, as shown in a separate study companion (Haag et al., 2003, clouds are not required to explain the main features of the distributions of RHI below the ice nucleation threshold. Key words. Atmospheric composition and structure (pressure, density and temperature; troposphere – composition and chemistry; general or miscellaneous

  7. Factors controlling upper tropospheric relative humidity

    Directory of Open Access Journals (Sweden)

    B. Kärcher

    2004-03-01

    Full Text Available Factors controlling the distribution of relative humidity in the absence of clouds are examined, with special emphasis on relative humidity over ice (RHI under upper tropospheric and lower stratospheric conditions. Variations of temperature are the key determinant for the distribution of RHI, followed by variations of the water vapor mixing ratio. Multiple humidity modes, generated by mixing of different air masses, may contribute to the overall distribution of RHI, in particular below ice saturation. The fraction of air that is supersaturated with respect to ice is mainly determined by the distribution of temperature. The nucleation of ice in cirrus clouds determines the highest relative humdity that can be measured outside of cirrus clouds. While vertical air motion and ice microphysics determine the slope of the distributions of RHI, as shown in a separate study companion (Haag et al., 2003, clouds are not required to explain the main features of the distributions of RHI below the ice nucleation threshold.

    Key words. Atmospheric composition and structure (pressure, density and temperature; troposphere – composition and chemistry; general or miscellaneous

  8. On the impact of aircraft emitted NO{sub x} on upper troposphere photochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Wahner, A; Rohrer, F; Ehhalt, D H [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

    1998-12-31

    The enhanced nitrogen oxide concentrations influence the photochemical production of ozone as well as the steady state concentrations of hydroxyl radicals, OH, in the upper troposphere. That increase is small compared to the impact of NO{sub x} from fossil fuel combustion on boundary layer ozone. A simple quasi 2-D model was used for the latitude band 40 deg - 50 deg N to analyze the reasons for that. The model includes a simplified CH{sub 4} - CO chemistry and the salient sources of upper tropospheric NO{sub x}, namely lightning, stratospheric input, aircraft emissions and fast upward transport of surface emissions. It is shown that the maximum of net O{sub 3} production and OH concentrations occur at much lower NO{sub x} mixing ratios than in the lower troposphere. (author)

  9. On the impact of aircraft emitted NO{sub x} on upper troposphere photochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Wahner, A.; Rohrer, F.; Ehhalt, D.H. [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

    1997-12-31

    The enhanced nitrogen oxide concentrations influence the photochemical production of ozone as well as the steady state concentrations of hydroxyl radicals, OH, in the upper troposphere. That increase is small compared to the impact of NO{sub x} from fossil fuel combustion on boundary layer ozone. A simple quasi 2-D model was used for the latitude band 40 deg - 50 deg N to analyze the reasons for that. The model includes a simplified CH{sub 4} - CO chemistry and the salient sources of upper tropospheric NO{sub x}, namely lightning, stratospheric input, aircraft emissions and fast upward transport of surface emissions. It is shown that the maximum of net O{sub 3} production and OH concentrations occur at much lower NO{sub x} mixing ratios than in the lower troposphere. (author)

  10. The global warming potential of methane reassessed with combined stratosphere and troposphere chemistry

    Science.gov (United States)

    Holmes, C. D.; Archibald, A. T.; Eastham, S. D.; Søvde, O. A.

    2017-12-01

    Methane is a direct and indirect greenhouse gas. The direct greenhouse effect comes from the radiation absorbed and emitted by methane itself. The indirect greenhouse effect comes from radiatively active gases that are produced during methane oxidation: principally O3, H2O, and CO2. Methane also suppresses tropospheric OH, which indirectly affects numerous greenhouses gases and aerosols. Traditionally, the methane global warming potential (GWP) has included the indirect effects on tropospheric O3 and OH and stratospheric H2O, with these effects estimated independently from unrelated tropospheric and stratospheric chemistry models and observations. Using this approach the CH4 is about 28 over 100 yr (without carbon cycle feedbacks, IPCC, 2013). Here we present a comprehensive analysis of the CH4 GWP in several 3-D global atmospheric models capable of simulating both tropospheric and stratospheric chemistry (GEOS-Chem, Oslo CTM3, UKCA). This enables us to include, for the first time, the indirect effects of CH4 on stratospheric O3 and stratosphere-troposphere coupling. We diagnose the GWP from paired simulations with and without a 5% perturbation to tropospheric CH4 concentrations. Including stratospheric chemistry nearly doubles the O3 contribution to CH4 GWP because of O3 production in the lower stratosphere and because CH4 inhibits Cl-catalyzed O3 loss in the upper stratosphere. In addition, stratosphere-troposphere coupling strengthens the chemical feedback on its own lifetime. In the stratosphere, this feedback operates by a CH4 perturbation thickening the stratospheric O3 layer, which impedes UV-driven OH production in the troposphere and prolongs the CH4 lifetime. We also quantify the impact of CH4-derived H2O on the stratospheric HOx cycles but these effects are small. Combining all of the above, these models suggest that the 100-yr GWP of CH4 is over 33.5, a 20% increase over the latest IPCC assessment.

  11. Stratospheric ozone transboundary transport to upper troposphere North Africa

    CSIR Research Space (South Africa)

    Ture, K

    2011-09-01

    Full Text Available will identify the causes and sources of MOZAIC ozone enhancements at upper tropospheric North Africa (20-350 N). In addition the paper will address the modes of transport of ozone rich airmass sampled by MOZAIC at mid latitude and North Africa....

  12. Comparisons of Upper Tropospheric Humidity Retrievals from TOVS and METEOSAT

    Science.gov (United States)

    Escoffier, C.; Bates, J.; Chedin, A.; Rossow, W. B.; Schmetz, J.

    1999-01-01

    Two different methods for retrieving Upper Tropospheric Humidities (UTH) from the TOVS (TIROS Operational Vertical Sounder) instruments aboard NOAA polar orbiting satellites are presented and compared. The first one, from the Environmental Technology Laboratory, computed by J. Bates and D. Jackson (hereafter BJ method), estimates UTH from a simplified radiative transfer analysis of the upper tropospheric infrared water vapor channel at wavelength measured by HIRS (6.3 micrometer). The second one results from a neural network analysis of the TOVS (HIRS and MSU) data developed at, the Laboratoire de Meteorologie Dynamique (hereafter the 3I (Improved Initialization Inversion) method). Although the two methods give very similar retrievals in temperate regions (30-60 N and S), an absolute bias up to 16% appears in the convective zone of the tropics. The two datasets have also been compared with UTH retrievals from infrared radiance measurements in the 6.3 micrometer channel from the geostationary satellite METEOSAT (hereafter MET method). The METEOSAT retrievals are systematically drier than the TOVS-based results by an absolute bias between 5 and 25%. Despite the biases, the spatial and temporal correlations are very good. The purpose of this study is to explain the deviations observed between the three datasets. The sensitivity of UTH to air temperature and humidity profiles is analysed as are the clouds effects. Overall, the comparison of the three retrievals gives an assessment of the current uncertainties in water vapor amounts in the upper troposphere as determined from NOAA and METEOSAT satellites.

  13. Troc: a proposed tropospheric sounder for chemistry and climate

    Science.gov (United States)

    Camy-Peyret, C.

    TROC has been submitted to ESA in the last call for proposals of the Earth Explorer Opportunity Missions and its focus is on tropospheric composition and chemistry-climate interactions. The mission objectives of TROC cover four research subjects. Global tropospheric chemistry: perform global measurements from space of tropospheric composition in order to improve our understanding and to constrain models of tropospheric chemistry with emphasis on tropospheric ozone. Pollution: establish the impact of mega cities of industrialised or developing countries by monitoring their pollution plumes. Biomass burning: monitor the chemical species and aerosols injected in the free troposphere during major burning episodes in the intertropical region as well as by major forest fires at other latitudes. Chemistry-climate interactions: quantify on a global scale the distributions and the sources of greenhouse gases like CO2, CH4, O3, N2O and the CFCs. Contribute to demonstration studies for monitoring from space how Montreal and Kyoto protocols are enforced as far as human impacts on atmospheric chemistry and climate are concerned. To fulfil these objectives, passive remote sensing of the troposphere has been selected as the best compromise between technical maturity and multi-species coverage. The main elements of TROC are a Fourier transform infrared (FTIR) instrument and an ultraviolet-visible (UV-vis) spectrometer, both operating in the downward-looking geometry with a 10 km diameter footprint at nadir. An ``intelligent'' pointing mirror coupled to an infrared imager is used to optimise day/night sounding down to the surface. The FTIR instrument covers at 0.1 cm-1 apodised spectral resolution 3 bands from 14 to 3.3 μ m in thermal emission and one band in solar reflected light around 2.3 μ m. The UV-vis instrument covers the regions 290-490 nm (1 nm resolution) and 520-1030 nm (2.5 nm resolution) with 43 array detectors (2 bands × 2 polarizations) in reflected

  14. The Impact of Upper Tropospheric Humidity from Microwave Limb Sounder on the Midlatitude Greenhouse Effect

    Science.gov (United States)

    Hu, Hua; Liu, W. Timothy

    1998-01-01

    This paper presents an analysis of upper tropospheric humidity, as measured by the Microwave Limb Sounder, and the impact of the humidity on the greenhouse effect in the midlatitudes. Enhanced upper tropospheric humidity and an enhanced greenhouse effect occur over the storm tracks in the North Pacific and North Atlantic. In these areas, strong baroclinic activity and the large number of deep convective clouds transport more water vapor to the upper troposphere, and hence increase greenhouse trapping. The greenhouse effect increases with upper tropospheric humidity in areas with a moist upper troposphere (such as areas over storm tracks), but it is not sensitive to changes in upper tropospheric humidity in regions with a dry upper troposphere, clearly demonstrating that there are different mechanisms controlling the geographical distribution of the greenhouse effect in the midlatitudes.

  15. New Particle Formation in the Mid-Latitude Upper Troposphere

    Science.gov (United States)

    Axisa, Duncan

    Primary aerosol production due to new particle formation (NPF) in the upper troposphere and the impact that this might have on cloud condensation nuclei (CCN) concentration can be of sufficient magnitude to contribute to the uncertainty in radiative forcing. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Therefore, new particle formation must be accurately defined, parametrized and accounted for in models. This research involved the deployment of instruments, data analysis and interpretation of particle formation events during the Mid-latitude Airborne Cirrus Properties Experiment (MACPEX) campaign. The approach combined field measurements and observations with extensive data analysis and modeling to study the process of new particle formation and growth to CCN active sizes. Simultaneous measurements of O3, CO, ultrafine aerosol particles and surface area from a high-altitude research aircraft were used to study tropospheric-stratospheric mixing as well as the frequency and location of NPF. It was found that the upper troposphere was an active region in the production of new particles by gas-to-particle conversion, that nucleation was triggered by convective clouds and mixing processes, and that NPF occurred in regions with high relative humidity and low surface area. In certain cases, mesoscale and synoptic features enhanced mixing and facilitated the formation of new particles in the northern mid-latitudes. A modeling study of particle growth and CCN formation was done based on measured aerosol size distributions and modeled growth. The results indicate that when SO2 is of sufficient concentration NPF is a significant source of potential CCN in the upper troposphere. In conditions where convective cloud outflow eject high concentrations of SO2, a large number of new particles can form especially in the instance when the preexisting surface area is low. The fast growth of nucleated clusters produces a

  16. Reanalysis comparisons of upper tropospheric-lower stratospheric jets and multiple tropopauses

    Science.gov (United States)

    Manney, Gloria L.; Hegglin, Michaela I.; Lawrence, Zachary D.; Wargan, Krzysztof; Millán, Luis F.; Schwartz, Michael J.; Santee, Michelle L.; Lambert, Alyn; Pawson, Steven; Knosp, Brian W.; Fuller, Ryan A.; Daffer, William H.

    2017-09-01

    The representation of upper tropospheric-lower stratospheric (UTLS) jet and tropopause characteristics is compared in five modern high-resolution reanalyses for 1980 through 2014. Climatologies of upper tropospheric jet, subvortex jet (the lowermost part of the stratospheric vortex), and multiple tropopause frequency distributions in MERRA (Modern-Era Retrospective analysis for Research and Applications), ERA-I (ERA-Interim; the European Centre for Medium-Range Weather Forecasts, ECMWF, interim reanalysis), JRA-55 (the Japanese 55-year Reanalysis), and CFSR (the Climate Forecast System Reanalysis) are compared with those in MERRA-2. Differences between alternate products from individual reanalysis systems are assessed; in particular, a comparison of CFSR data on model and pressure levels highlights the importance of vertical grid spacing. Most of the differences in distributions of UTLS jets and multiple tropopauses are consistent with the differences in assimilation model grids and resolution - for example, ERA-I (with coarsest native horizontal resolution) typically shows a significant low bias in upper tropospheric jets with respect to MERRA-2, and JRA-55 (the Japanese 55-year Reanalysis) a more modest one, while CFSR (with finest native horizontal resolution) shows a high bias with respect to MERRA-2 in both upper tropospheric jets and multiple tropopauses. Vertical temperature structure and grid spacing are especially important for multiple tropopause characterizations. Substantial differences between MERRA and MERRA-2 are seen in mid- to high-latitude Southern Hemisphere (SH) winter upper tropospheric jets and multiple tropopauses as well as in the upper tropospheric jets associated with tropical circulations during the solstice seasons; some of the largest differences from the other reanalyses are seen in the same times and places. Very good qualitative agreement among the reanalyses is seen between the large-scale climatological features in UTLS jet and

  17. Application of ion chemistry to tropospheric VOC measurements

    International Nuclear Information System (INIS)

    Hansel, A.; Wisthaler, A.; Graus, M.; Grabmer, W.

    2002-01-01

    The main interest in tropospheric volatile organic compounds (VOCs) originating from biogenic sources such as forests and anthropogenic sources such as cities is because these reactive trace gases can have a significant impact on levels of oxidants such as ozone (O 3 ) and the hydroxyl radical (OH). The proton-transfer-reaction mass-spectrometry (PTR-MS) technique developed by Werner Lindingers Laboratory, utilizes positive ion chemistry to measure trace neutral concentrations in air. It has been applied in food research, medicine and environmental studies to gain gas phase information about VOCs at parts per trillion (pptv) levels.The real-time method relies on proton transfer reactions between H 3 O + primary ions and VOCs which have a higher proton affinity than water molecules. Organic trace gases such as hydrocarbons, carbonyls, alcohols, acetonitrile, and others can be monitored on-line.Results on tropospheric VOCs measurements in tropical regions and in cities are discussed. (nevyjel)

  18. 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.

  19. 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

  20. Upper-tropospheric CO and O3 budget during the Asian summer monsoon

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    B. Barret

    2016-07-01

    Full Text Available During the Asian summer monsoon, the circulation in the upper troposphere/lower stratosphere (UTLS is dominated by the Asian monsoon anticyclone (AMA. Pollutants convectively uplifted to the upper troposphere are trapped within this anticyclonic circulation that extends from the Pacific Ocean to the Eastern Mediterranean basin. Among the uplifted pollutants are ozone (O3 and its precursors, such as carbon monoxide (CO and nitrogen oxides (NOx. Many studies based on global modeling and satellite data have documented the source regions and transport pathways of primary pollutants (CO, HCN into the AMA. Here, we aim to quantify the O3 budget by taking into consideration anthropogenic and natural sources. We first use CO and O3 data from the MetOp-A/IASI sensor to document their tropospheric distributions over Asia, taking advantage of the useful information they provide on the vertical dimension. These satellite data are used together with MOZAIC tropospheric profiles recorded in India to validate the distributions simulated by the global GEOS-Chem chemistry transport model. Over the Asian region, UTLS monthly CO and O3 distributions from IASI and GEOS-Chem display the same large-scale features. UTLS CO columns from GEOS-Chem are in agreement with IASI, with a low bias of 11 ± 9 % and a correlation coefficient of 0.70. For O3, the model underestimates IASI UTLS columns over Asia by 14 ± 26 % but the correlation between both is high (0.94. GEOS-Chem is further used to quantify the CO and O3 budget through sensitivity simulations. For CO, these simulations confirm that South Asian anthropogenic emissions have a more important impact on enhanced concentrations within the AMA (∼  25 ppbv than East Asian emissions (∼  10 ppbv. The correlation between enhanced emissions over the Indo-Gangetic Plain and monsoon deep convection is responsible for this larger impact. Consistently, South Asian anthropogenic NOx emissions also

  1. Generation of layering in the upper arctic troposphere away from the jet stream

    Directory of Open Access Journals (Sweden)

    A. Karpetchko

    Full Text Available Ozone sounding databases for two stations, So-dankylä (67° N, 27° E and Ny-Ålesund (79° N, 12° E were used in order to investigate the generation of layering in the upper and middle troposphere of the Arctic. We concentrated on dry, ozone-rich and stable layers observed below the thermal tropopause under light wind conditions. This condition ensures that the observed layer is not a tropopause fold, a well-known phenomenon that develops within frontal zones near the jet stream. Selection criteria for ozone, humidity and stability anomalies of the tropopause fold detection algorithm were used here to pick out for detailed studies the most pronounced examples of laminae. For all these cases the meteorological situations were investigated in order to establish the origin of the observed layers. We found that layers could be classified into two groups. Laminae of the first group were observed equatorward of the jet stream and those of a second group were observed poleward of the jet. The meteorological situation for the first group resembles that for equatorward stratospheric streamer propagation. It was found that this group accounts for only a small fraction of the layers observed at Sodankylä and for none of those observed at Ny-Ålesund during the period investigated. A large case-to-case variability in the synoptic situation was observed for the second group of laminae, which were detected northward of the jet stream. Nevertheless, in about half of the cases, streamers of tropospheric air were found in the vicinity of the stations on the isentropic surfaces just above the detected stratospheric layers. Back trajectory analyses showed that these layers originated in the vicinity of the polar jet stream. We suppose that laminae-like structures in the troposphere were caused, in both groups, by equatorward (poleward advection of the stratospheric (tropospheric air, together with differential vertical shear. Forward-trajectory calculations

  2. Generation of layering in the upper arctic troposphere away from the jet stream

    Directory of Open Access Journals (Sweden)

    A. Karpetchko

    2003-07-01

    Full Text Available Ozone sounding databases for two stations, So-dankylä (67° N, 27° E and Ny-Ålesund (79° N, 12° E were used in order to investigate the generation of layering in the upper and middle troposphere of the Arctic. We concentrated on dry, ozone-rich and stable layers observed below the thermal tropopause under light wind conditions. This condition ensures that the observed layer is not a tropopause fold, a well-known phenomenon that develops within frontal zones near the jet stream. Selection criteria for ozone, humidity and stability anomalies of the tropopause fold detection algorithm were used here to pick out for detailed studies the most pronounced examples of laminae. For all these cases the meteorological situations were investigated in order to establish the origin of the observed layers. We found that layers could be classified into two groups. Laminae of the first group were observed equatorward of the jet stream and those of a second group were observed poleward of the jet. The meteorological situation for the first group resembles that for equatorward stratospheric streamer propagation. It was found that this group accounts for only a small fraction of the layers observed at Sodankylä and for none of those observed at Ny-Ålesund during the period investigated. A large case-to-case variability in the synoptic situation was observed for the second group of laminae, which were detected northward of the jet stream. Nevertheless, in about half of the cases, streamers of tropospheric air were found in the vicinity of the stations on the isentropic surfaces just above the detected stratospheric layers. Back trajectory analyses showed that these layers originated in the vicinity of the polar jet stream. We suppose that laminae-like structures in the troposphere were caused, in both groups, by equatorward (poleward advection of the stratospheric (tropospheric air, together with differential vertical shear. Forward-trajectory calculations

  3. Water vapour and ozone profiles in the midlatitude upper troposphere

    Directory of Open Access Journals (Sweden)

    G. Vaughan

    2005-01-01

    Full Text Available We present an investigation of upper tropospheric humidity profiles measured with a standard radiosonde, the Vaisala RS80-A, and a commercial frost-point hygrometer, the Snow White. Modifications to the Snow White, to enable the mirror reflectivity and Peltier cooling current to be monitored during flight, were found to be necessary to determine when the instrument was functioning correctly; a further modification to prevent hydrometeors entering the inlet was also implemented. From 23 combined flights of an ozonesonde, radiosonde and Snow White between September 2001 and July 2002, clear agreement was found between the two humidity sensors, with a mean difference of <2% in relative humidity from 2 to 10km, and 2.2% between 10 and 13km. This agreement required a correction to the radiosonde humidity, as described by Miloshevich et al. (2001. Using this result, the dataset of 324 ozonesonde/RS80-A profiles measured from Aberystwyth between 1991 and 2002 was examined to derive statistics for the distribution of water vapour and ozone. Supersaturation with respect to ice was frequently seen at the higher levels - 24% of the time in winter between 8 and 10km. The fairly uniform distribution of relative humidity persisted to 120% in winter, but decreased rapidly above 100% in summer.

  4. Observational evidence for aerosols increasing upper tropospheric humidity

    Directory of Open Access Journals (Sweden)

    L. Riuttanen

    2016-11-01

    Full Text Available Aerosol–cloud interactions are the largest source of uncertainty in the radiative forcing of the global climate. A phenomenon not included in the estimates of the total net forcing is the potential increase in upper tropospheric humidity (UTH by anthropogenic aerosols via changes in the microphysics of deep convection. Using remote sensing data over the ocean east of China in summer, we show that increased aerosol loads are associated with an UTH increase of 2.2 ± 1.5 in units of relative humidity. We show that humidification of aerosols or other meteorological covariation is very unlikely to be the cause of this result, indicating relevance for the global climate. In tropical moist air such an UTH increase leads to a regional radiative effect of 0.5 ± 0.4 W m−2. We conclude that the effect of aerosols on UTH should be included in future studies of anthropogenic climate change and climate sensitivity.

  5. Global distribution of upper tropospheric formic acid from the ACE-FTS

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    G. González Abad

    2009-10-01

    Full Text Available We present the first near global upper tropospheric distribution of formic acid (HCOOH observed from space using solar occultation measurements from the Fourier transform spectrometer (FTS on board the Atmospheric Chemistry Experiment (ACE satellite. Using a new set of spectroscopic line parameters recently published for formic acid by Vander Auwera et al. (2007 and Perrin and Vander Auwera (2007, we have retrieved the concentrations of HCOOH between 5 km and the tropopause for ACE-FTS observations from February 2004 to September 2007. We observe a significant seasonal dependence for the HCOOH concentrations related to vegetation growth and biomass burning. We estimate an emission ratio of 0.0051±0.0015 for HCOOH relative to CO for tropical South American fires using a selected set of data for September 2004. Results from the balloon-borne MkIV Fourier transform spectrometer are also presented and compared with the ACE measurements.

  6. Aqueous aerosol may build up large upper tropospheric ice supersaturation

    Science.gov (United States)

    Bogdan, Anatoli; Molina, Mario J.

    2010-05-01

    Keywords: ice supersaturation, upper tropospheric cirrus clouds, freezing of aqueous aerosol. Observations often reveal enhanced and persistent upper tropospheric (UT) ice supersaturation, Si up to 100%, independently of whether cirrus ice clouds are present or not (Krämer et al., 2009; Lawson et al., 2008). However, a water activity criterion (WAC) (Koop et al., 2000) does not allow the formation of Si > ~67% by the homogeneous freezing of aqueous droplets even at the lowest atmospheric temperature of ~185 K. For aqueous aerosol the WAC predicts the existence of a so called homogeneous ice nucleation threshold which, being expressed as Si, is between ~52 and 67% in the temperature range of ~220 - 185 K. The nature of the formation of large Si remains unclear. Since water vapor is the dominant greenhouse gas it is important to know the nature of the accumulation and persistence of water vapor in the UT. We studied the freezing behavior of micrometer-scaled 3-, 4-, and 5-component droplets, which contain different weight fractions of H2O, H2SO4, HNO3, (NH4)2SO4, (NH4)HSO4, NH4NO3, and (NH4)3H(SO4)2. The study was performed between 133 and 278 K at cooling rates of 3, 0.1, and 0.05 K/min using differential scanning calorimetry (DSC) (Bogdan and Molina, 2010). The cooling rates of 0.1 and 0.05 K/min (6 and 3 K/h) are similar to the smallest reported synoptic temperature change of ~2 K/h (Carslaw et al., 1998). Using the measured freezing temperature of ice, Ti, and the thermodynamic E-AIM model of the system of H+ - NH4+ - SO42-- NO3-- H2O (Clegg et al., 1998), we calculated the corresponding clear-sky Si which would be built up immediately prior to the formation of ice cirrus clouds by the homogeneous freezing of aqueous aerosol of similar composition. We found that our calculated values of Si are both larger and smaller than the homogeneous ice nucleation threshold. For example, for the droplets of compositions of 15/10 and 20/10 wt % (NH4)3H(SO4)2/H2SO4, which

  7. A distribution law for relative humidity in the upper troposphere and lower stratosphere derived from three years of MOZAIC measurements

    Directory of Open Access Journals (Sweden)

    K. Gierens

    1999-09-01

    Full Text Available Data from three years of MOZAIC measurements made it possible to determine a distribution law for the relative humidity in the upper troposphere and lower stratosphere. Data amounting to 13.5% of the total were obtained in regions with ice supersaturation. Troposphere and stratosphere are distinguished by an ozone concentration of 130 ppbv as threshold. The probability of measuring a certain amount of ice supersaturation in the troposphere decreases exponentially with the degree of ice supersaturation. The probability of measuring a certain relative humidity in the stratosphere (both with respect to water and ice decreases exponentially with the relative humidity. A stochastic model that naturally leads to the exponential distribution is provided. Mean supersaturation in the troposphere is about 15%, whereas ice nucleation requires 30% supersaturation on the average. This explains the frequency of regions in which aircraft induce persistent contrails but which are otherwise free of clouds. Ice supersaturated regions are 3-4 K colder and contain more than 50% more vapour than other regions in the upper troposphere. The stratospheric air masses sampled are dry, as expected, having mean relative humidity over water of 12% and over ice of 23%, respectively. However, 2% of the stratospheric data indicate ice supersaturation. As the MOZAIC measurements have been obtained on commercial flights mainly between Europe and North America, the data do not provide a complete global picture, but the exponential character of the distribution laws found is probably valid globally. Since water vapour is the most important greenhouse gas and since it might enhance the anthropogenic greenhouse effects via positive feedback mechanisms, it is important to represent its distribution correctly in climate models. The discovery of the distribution law of the relative humidity makes possible simple tests to show whether the hydrological cycle in climate models is

  8. Relationship between changes in the upper and lower tropospheric water vapor: A revisit

    Science.gov (United States)

    Yang, M.; Sun, D. Z.; Zhang, G. J.

    2017-12-01

    Upper tropospheric water vapor response to enhanced greenhouse gas forcing is as important as the lower tropospheric water vapor response in determining climate sensitivity. Early studies using older versions of climate models have suggested that the upper- and lower-troposphere water vapor changes are more strongly coupled in the climate models than in the observations. Here we reexamine this issue using a state-of-the-art climate model—the NCAR community model CAM5. Specifically, we have calculated the correlations between interannual variations of specific humidity in all levels of the troposphere with that at the surface in CAM5 and in the observations (as represented by the updated ERA-Interim and NCEP reanalysis). It is found that the previously noted biases in how strongly upper tropospheric water vapor and lower troposphere water vapor are linked still exist in CAM5—the change in the tropical averaged upper tropospheric water vapor is more strongly correlated with the change in the surface. However, this bias disappears in the averaged correlation obtained by averaging the point-by-point correlations over the tropics. The spatial pattern of the point-by-point correlations reveals that the better agreement between the model and the observations is related to the opposite model biases in different regions: the correlation is weaker in the model in the western Pacific, but stronger in the central and eastern Pacific. Further analysis of precipitation fields suggests that the weaker (stronger) coupling between tropospheric water vapor and surface moisture over western (central-eastern) Pacific in model is related to weaker (stronger) simulated convective activities in these regions. More specifically, during El Nino, the model has excessive deep convection in the central Pacific, but too littler deep convection in western Pacific. Implications of the results are discussed in the context of climate change as well as in the context of how to improve the model

  9. Satellite observations and modeling of transport in the upper troposphere through the lower mesosphere during the 2006 major stratospheric sudden warming

    Directory of Open Access Journals (Sweden)

    W. H. Daffer

    2009-07-01

    Full Text Available An unusually strong and prolonged stratospheric sudden warming (SSW in January 2006 was the first major SSW for which globally distributed long-lived trace gas data are available covering the upper troposphere through the lower mesosphere. We use Aura Microwave Limb Sounder (MLS, Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS data, the SLIMCAT Chemistry Transport Model (CTM, and assimilated meteorological analyses to provide a comprehensive picture of transport during this event. The upper tropospheric ridge that triggered the SSW was associated with an elevated tropopause and layering in trace gas profiles in conjunction with stratospheric and tropospheric intrusions. Anomalous poleward transport (with corresponding quasi-isentropic troposphere-to-stratosphere exchange at the lowest levels studied in the region over the ridge extended well into the lower stratosphere. In the middle and upper stratosphere, the breakdown of the polar vortex transport barrier was seen in a signature of rapid, widespread mixing in trace gases, including CO, H2O, CH4 and N2O. The vortex broke down slightly later and more slowly in the lower than in the middle stratosphere. In the middle and lower stratosphere, small remnants with trace gas values characteristic of the pre-SSW vortex lingered through the weak and slow recovery of the vortex. The upper stratospheric vortex quickly reformed, and, as enhanced diabatic descent set in, CO descended into this strong vortex, echoing the fall vortex development. Trace gas evolution in the SLIMCAT CTM agrees well with that in the satellite trace gas data from the upper troposphere through the middle stratosphere. In the upper stratosphere and lower mesosphere, the SLIMCAT simulation does not capture the strong descent of mesospheric CO and H2O values into the reformed vortex; this poor CTM performance in the upper stratosphere and lower mesosphere results

  10. Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

    Science.gov (United States)

    Wennberg, P. O.; Hanisco, T. F.; Jaegle, L.; Jacob, D. J.; Hintsa, E. J.; Lanzendorf, E. J.; Anderson, J. G.; Gao, R.-S.; Keim, E. R.; Donnelly, S. G.; hide

    1998-01-01

    The concentrations of the hydrogen radicals OH and HO2 in the middle and upper troposphere were measured simultaneously with those of NO, O3, CO, H2O, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O3, in this region of the atmosphere. Comparison of the measured concentrations of OH and HO2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HO(x) required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production of 03 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO2 and NO) is calculated to be about 1 part per billion by volume each day.This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more 03 than expected.

  11. Hydrogen Cyanide in the Upper Troposphere: GEM-AQ Simulation and Comparison with ACE-FTS Observations

    Science.gov (United States)

    Lupu, A.; Kaminski, J. W.; Neary, L.; McConnell, J. C.; Toyota, K.; Rinsland, C. P.; Bernath, P. F.; Walker, K. A.; Boone, C. D.; Nagahama, Y.; hide

    2009-01-01

    We investigate the spatial and temporal distribution of hydrogen cyanide (HCN) in the upper troposphere through numerical simulations and comparison with observations from a space-based instrument. To perform the simulations, we used the Global Environmental Multiscale Air Quality model (GEM-AQ), which is based on the threedimensional Gobal multiscale model developed by the Meteorological Service of Canada for operational weather forecasting. The model was run for the period 2004-2006 on a 1.5deg x 1.5deg global grid with 28 hybrid vertical levels from the surface up to 10 hPa. Objective analysis data from the Canadian Meteorological Centre were used to update the meteorological fields every 24 h. Fire emission fluxes of gas species were generated by using year-specific inventories of carbon emissions with 8-day temporal resolution from the Global Fire Emission Database (GFED) version 2. The model output is compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument onboard the Canadian SCISAT-1 satellite. High values of up to a few ppbv are observed in the tropics in the Southern Hemisphere; the enhancement in HCN volume mixing ratios in the upper troposphere is most prominent in October. Low upper-tropospheric mixing ratios of less than 100 pptv are mostly recorded at middle and high latitudes in the Southern Hemisphere in May-July. Mixing ratios in Northern Hemisphere peak in the boreal summer. The amplitude of the seasonal variation is less pronounced than in the Southern Hemisphere. The comparison with the satellite data shows that in the upper troposphere GEM-AQ perform7s well globally for all seasons, except at northern hi gh and middle latitudes in surnmer, where the model has a large negative bias, and in the tropics in winter and spring, where it exhibits large positive bias. This may reflect inaccurate emissions or possible inaccuracies in the emission profile. The model is able to

  12. Sulfur dioxide (SO2 from MIPAS in the upper troposphere and lower stratosphere 2002–2012

    Directory of Open Access Journals (Sweden)

    M. Höpfner

    2015-06-01

    Full Text Available Vertically resolved distributions of sulfur dioxide (SO2 with global coverage in the height region from the upper troposphere to ~20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70–100 pptv and by a vertical resolution ranging from 3 to 5 km. Comparison with observations by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS revealed a slightly varying bias with altitude of −20 to 50 pptv for the MIPAS data set in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within −10 to 20 pptv in the altitude range of 10–20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS data set with in situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than 30 volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS. Emitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period – Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 – derived lifetimes of SO2 for the altitude ranges 10–14, 14–18 and 18–22 km are 13.3 ± 2.1, 23.6 ± 1.2 and 32.3 ± 5.5 days respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual

  13. Hydrogen Radicals, Nitrogen Radicals, and the Production of Ozone in the Middle and Upper Troposphere

    Science.gov (United States)

    Bui, T. P.

    1997-01-01

    The concentrations of hydrogen radicals, OH and HO2, in the middle and upper troposphere were measured simultaneously with those of NO, O3,CO, H20, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field.

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

    Science.gov (United States)

    Haase, S.; Matthes, K. B.

    2017-12-01

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

  15. Tropospheric Bromine Chemistry: Implications for Present and Pre-industrial Ozone and Mercury

    Science.gov (United States)

    Parella, J. P.; Jacob, D. J.; Liang, Q.; Zhang, Y.; Mickley, L. J.; Miller, B.; Evans, M. J.; Yang, X.; Pyle, J. A.; Theys, N.; hide

    2012-01-01

    We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

  16. The Effect of Cirrus Clouds on Water Vapor Transport in the Upper Troposphere and Lower Stratosphere

    Science.gov (United States)

    Lei, L.; McCormick, M. P.; Anderson, J.

    2017-12-01

    Water vapor plays an important role in the Earth's radiation budget and stratospheric chemistry. It is widely accepted that a large percentage of water vapor entering the stratosphere travels through the tropical tropopause and is dehydrated by the cold tropopause temperature. The vertical transport of water vapor is also affected by the radiative effects of cirrus clouds in the tropical tropopause layer. This latter effect of cirrus clouds was investigated in this research. The work focuses on the tropical and mid-latitude region (50N-50S). Water vapor data from the Microwave Limb Sounder (MLS) and cirrus cloud data from the Cloud-Aerosol Lidar and Infrared pathfinder Satellite Observation (CALIPSO) instruments were used to investigate the relationship between the water vapor and the occurrence of cirrus cloud. A 10-degree in longitude by 10-degree in latitude resolution was chosen to bin the MLS and CALIPSO data. The result shows that the maximum water vapor in the upper troposphere (below 146 hPa) is matched very well with the highest frequency of cirrus cloud occurrences. Maximum water vapor in the lower stratosphere (100 hPa) is partly matched with the maximum cirrus cloud occurrence in the summer time. The National Oceanic and Atmospheric Administration Interpolated Outgoing Longwave Radiation data and NCEP-DOE Reanalysis 2 wind data were used also to investigate the relationship between the water vapor entering the stratosphere, deep convection, and wind. Results show that maximum water vapor at 100 hPa coincides with the northern hemisphere summer-time anticyclone. The effects from both single-layer cirrus clouds and cirrus clouds above the anvil top on the water vapor entering the stratosphere were also studied and will be presented.

  17. A comparison of lightning and aircraft sources of NO{sub x} in the upper troposphere

    Energy Technology Data Exchange (ETDEWEB)

    Penner, J E; Walton, J J [Michigan Univ., Ann Arbor, MI (United States). Dept. of Atmospheric, Oceanic and Space Physics; Bergmann, D J; Kinnison, D; Rotman, D [Lawrence Livermore National Lab., CA (United States). Atmospheric Science Div.; Price, C [Tel Aviv Univ. (Israel). Dept. of Geophysics and Planetary Sciences; Prather, M J [California Univ., Irvine, CA (United States). Dept. of Earth System Science; Pickering, K E [Maryland Univ., College Park, MD (United States). Dept. of Meteorology; Baughcum, S L [Boeing Commerial Airplane Group, Seatlle, WA (United States)

    1998-12-31

    Uncertainties in the assessment of the contribution of aircraft to upper tropospheric NO{sub x} arise from uncertainties in model treatment of transport, uncertainties in source strengths, and uncertainties in chemical rates and reactions determining the partitioning between NO{sub x} and NO{sub y}. Two different chemical transport models are used to examine the range of uncertainty in the contribution of aircraft to upper tropospheric NO{sub x} from model representations of transport. Uncertainties caused by uncertainties in the rate of production of NO{sub x} from lightning and uncertainties from the range of background concentrations of HNO{sub 3} are also examined. Uncertainties in the treatment of vertical transport and uncertainties in the source strength from lightning contribute to a large range in model results for background NO{sub x}. (author) 18 refs.

  18. A comparison of lightning and aircraft sources of NO{sub x} in the upper troposphere

    Energy Technology Data Exchange (ETDEWEB)

    Penner, J.E.; Walton, J.J. [Michigan Univ., Ann Arbor, MI (United States). Dept. of Atmospheric, Oceanic and Space Physics; Bergmann, D.J.; Kinnison, D.; Rotman, D. [Lawrence Livermore National Lab., CA (United States). Atmospheric Science Div.; Price, C. [Tel Aviv Univ. (Israel). Dept. of Geophysics and Planetary Sciences; Prather, M.J. [California Univ., Irvine, CA (United States). Dept. of Earth System Science; Pickering, K.E. [Maryland Univ., College Park, MD (United States). Dept. of Meteorology; Baughcum, S.L. [Boeing Commerial Airplane Group, Seatlle, WA (United States)

    1997-12-31

    Uncertainties in the assessment of the contribution of aircraft to upper tropospheric NO{sub x} arise from uncertainties in model treatment of transport, uncertainties in source strengths, and uncertainties in chemical rates and reactions determining the partitioning between NO{sub x} and NO{sub y}. Two different chemical transport models are used to examine the range of uncertainty in the contribution of aircraft to upper tropospheric NO{sub x} from model representations of transport. Uncertainties caused by uncertainties in the rate of production of NO{sub x} from lightning and uncertainties from the range of background concentrations of HNO{sub 3} are also examined. Uncertainties in the treatment of vertical transport and uncertainties in the source strength from lightning contribute to a large range in model results for background NO{sub x}. (author) 18 refs.

  19. Upper tropospheric cloud systems determined from IR Sounders and their influence on the atmosphere

    Science.gov (United States)

    Stubenrauch, Claudia; Protopapadaki, Sofia; Feofilov, Artem; Velasco, Carola Barrientos

    2017-02-01

    Covering about 30% of the Earth, upper tropospheric clouds play a key role in the climate system by modulating the Earth's energy budget and heat transport. Infrared Sounders reliably identify cirrus down to an IR optical depth of 0.1. Recently LMD has built global cloud climate data records from AIRS and IASI observations, covering the periods from 2003-2015 and 2008-2015, respectively. Upper tropospheric clouds often form mesoscale systems. Their organization and properties are being studied by (1) distinguishing cloud regimes within 2° × 2° regions and (2) applying a spatial composite technique on adjacent cloud pressures, which estimates the horizontal extent of the mesoscale cloud systems. Convective core, cirrus anvil and thin cirrus of these systems are then distinguished by their emissivity. Compared to other studies of tropical mesoscale convective systems our data include also the thinner anvil parts, which make out about 30% of the area of tropical mesoscale convective systems. Once the horizontal and vertical structure of these upper tropospheric cloud systems is known, we can estimate their radiative effects in terms of top of atmosphere and surface radiative fluxes and by computing their heating rates.

  20. Interactive chemistry in the Laboratoire de Météorologie Dynamique general circulation model: model description and impact analysis of biogenic hydrocarbons on tropospheric chemistry

    Directory of Open Access Journals (Sweden)

    G. A. Folberth

    2006-01-01

    Full Text Available We present a description and evaluation of LMDz-INCA, a global three-dimensional chemistry-climate model, pertaining to its recently developed NMHC version. In this substantially extended version of the model a comprehensive representation of the photochemistry of non-methane hydrocarbons (NMHC and volatile organic compounds (VOC from biogenic, anthropogenic, and biomass-burning sources has been included. The tropospheric annual mean methane (9.2 years and methylchloroform (5.5 years chemical lifetimes are well within the range of previous modelling studies and are in excellent agreement with estimates established by means of global observations. The model provides a reasonable simulation of the horizontal and vertical distribution and seasonal cycle of CO and key non-methane VOC, such as acetone, methanol, and formaldehyde as compared to observational data from several ground stations and aircraft campaigns. LMDz-INCA in the NMHC version reproduces tropospheric ozone concentrations fairly well throughout most of the troposphere. The model is applied in several sensitivity studies of the biosphere-atmosphere photochemical feedback. The impact of surface emissions of isoprene, acetone, and methanol is studied. These experiments show a substantial impact of isoprene on tropospheric ozone and carbon monoxide concentrations revealing an increase in surface O3 and CO levels of up to 30 ppbv and 60 ppbv, respectively. Isoprene also appears to significantly impact the global OH distribution resulting in a decrease of the global mean tropospheric OH concentration by approximately 0.7×105 molecules cm-3 or roughly 8% and an increase in the global mean tropospheric methane lifetime by approximately seven months. A global mean ozone net radiative forcing due to the isoprene induced increase in the tropospheric ozone burden of 0.09 W m-2 is found. The key role of isoprene photooxidation in the global tropospheric redistribution of NOx is demonstrated. LMDz

  1. Surface measurements of upper tropospheric water vapor isotopic composition on the Chajnantor Plateau, Chile

    Science.gov (United States)

    Galewsky, Joseph; Rella, Christopher; Sharp, Zachary; Samuels, Kimberly; Ward, Dylan

    2011-09-01

    Simultaneous, real-time measurements of atmospheric water vapor mixing ratio and isotopic composition (δD and δ18O) were obtained using cavity ringdown spectroscopy on the arid Chajnantor Plateau in the subtropical Chilean Andes (elevation 5080 m or 550 hPa; latitude 23°S) during July and August 2010. The measurements show surface water vapor mixing ratio as low as 215 ppmv, δD values as low as -540‰, and δ18O values as low as -68‰, which are the lowest atmospheric water vapor δ values reported from Earth's surface. The results are consistent with previous measurements from the base of the tropical tropopause layer (TTL) and suggest large-scale subsidence of air masses from the upper troposphere to the Earth's surface. The range of measurements is consistent with condensation under conditions of ice supersaturation and mixing with moister air from the lower troposphere that has been processed through shallow convection. Diagnostics using reanalysis data show that the extreme aridity of the Chajnantor Plateau is controlled by condensation in the upper tropical troposphere.

  2. Influence of isentropic transport on seasonal ozone variations in the lower stratosphere and subtropical upper troposphere

    Science.gov (United States)

    Jing, P.; Cunnold, D. M.; Yang, E.-S.; Wang, H.-J.

    2005-01-01

    The isentropic cross-tropopause ozone transport has been estimated in both hemispheres in 1999 based on the potential vorticity mapping of Stratospheric Aerosol and Gas Experiment 11 ozone measurements and contour advection calculations using the NASA Goddard Space Flight Center Global and Modeling Assimilation Office analysis. The estimated net isentropic stratosphere-to-troposphere ozone flux is approx.118 +/- 61 x 10(exp9)kg/yr globally within the layer between 330 and 370 K in 1999; 60% of it is found in the Northern Hemisphere, and 40% is found in the Southern Hemisphere. The monthly average ozone fluxes are strongest in summer and weakest in winter in both hemispheres. The seasonal variations of ozone in the lower stratosphere (LS) and upper troposphere (UT) have been analyzed using ozonesonde observations from ozonesonde stations in the extratropics and subtropics, respectively. It is shown that observed ozone levels increase in the UT over subtropical ozonesonde stations and decrease in the LS over extratropical stations in late spring/early summer and that the ozone increases in the summertime subtropical UT are unlikely to be explained by photochemical ozone production and diabatic transport alone. We conclude that isentropic transport is a significant contributor to ozone levels in the subtropical upper troposphere, especially in summer.

  3. Tropospheric chemistry over the lower Great Plains of the United States. 2. Trace gas profiles and distributions

    Science.gov (United States)

    Luke, Winston T.; Dickerson, Russell R.; Ryan, William F.; Pickering, Kenneth E.; Nunnermacker, Linda J.

    1992-12-01

    Convective clouds and thunderstorms redistribute air pollutants vertically, and by altering the chemistry and radiative balance of the upper troposphere, these local actions can have global consequences. To study these effects, measurements of trace gases ozone, O3, carbon monoxide, CO, and odd nitrogen were made aboard the NCAR Sabreliner on 18 flights over the southern Great Plains during June 1985. To demonstrate chemical changes induced by vertical motions in the atmosphere and to facilitate comparison with computer model calculations, these data were categorized according to synoptic flow patterns. Part 1 of this two-part paper details the alternating pulses of polar and maritime air masses that dominate the vertical mixing in this region. In this paper, trace gas measurements are presented as altitude profiles (0-12 km) with statistical distributions of mixing ratios for each species in each flow pattern. The polar flow regime is characterized by northwesterly winds, subsiding air, and convective stability. Concentrations of CO and total odd nitrogen (NOy) are relatively high in the shallow planetary boundary layer (PBL) but decrease rapidly with altitude. Ozone, on the other hand, is uniformly distributed, suggesting limited photochemical production; in fact, nitric oxide, NO, mixing ratios fell below 10 ppt (parts per 1012 by volume) in the midtroposphere. The maritime regime is characterized by southerly surface winds, convective instability, and a deep PBL; uniformly high concentrations of trace gases were found up to 4 km on one flight. Severe storms occur in maritime flow, especially when capped by a dry layer, and they transport large amounts of CO, O3, and NOy into the upper troposphere. Median NO levels at high altitude exceeded 300 ppt. Lightning produces spikes of NO (but not CO) with mixing ratios sometimes exceeding 1000 ppt. This flow pattern tends to leave the midtroposphere relatively clean with concentrations of trace gases similar to those

  4. Upper Troposphere Lower Stratosphere structure during convective systems using GPS radio occultations

    DEFF Research Database (Denmark)

    Biondi, Riccardo

    The deep convective systems play a fundamental role in atmospheric circulation and climate. Thunderstorms and meso-scale convective systems produce fast vertical transport, redistributing water vapor and trace gases and influencing the thermal structure of the upper troposphere and lower...... stratosphere (UTLS) contributing to the troposphere-stratosphere transport and affecting the Earth global circulation and the climate changes. The Global Positioning System (GPS) Radio Occultation (RO) technique enables measurement of atmospheric density structure in any meteorological condition...... to the analysis of tropical storms for the future mission ACES will also be evaluated. Using data from the past and ongoing GPS RO missions we have defined an algorithm to detect the clouds top of the convective systems and their thermal structure. Other satellite and in-situ measurements co-located with GPS ROs...

  5. The Ozone Budget in the Upper Troposphere from Global Modeling Initiative (GMI)Simulations

    Science.gov (United States)

    Rodriquez, J.; Duncan, Bryan N.; Logan, Jennifer A.

    2006-01-01

    Ozone concentrations in the upper troposphere are influenced by in-situ production, long-range tropospheric transport, and influx of stratospheric ozone, as well as by photochemical removal. Since ozone is an important greenhouse gas in this region, it is particularly important to understand how it will respond to changes in anthropogenic emissions and changes in stratospheric ozone fluxes.. This response will be determined by the relative balance of the different production, loss and transport processes. Ozone concentrations calculated by models will differ depending on the adopted meteorological fields, their chemical scheme, anthropogenic emissions, and treatment of the stratospheric influx. We performed simulations using the chemical-transport model from the Global Modeling Initiative (GMI) with meteorological fields from (It)h e NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM), (2) the atmospheric GCM from NASA's Global Modeling and Assimilation Office(GMAO), and (3) assimilated winds from GMAO . These simulations adopt the same chemical mechanism and emissions, and adopt the Synthetic Ozone (SYNOZ) approach for treating the influx of stratospheric ozone -. In addition, we also performed simulations for a coupled troposphere-stratosphere model with a subset of the same winds. Simulations were done for both 4degx5deg and 2degx2.5deg resolution. Model results are being tested through comparison with a suite of atmospheric observations. In this presentation, we diagnose the ozone budget in the upper troposphere utilizing the suite of GMI simulations, to address the sensitivity of this budget to: a) the different meteorological fields used; b) the adoption of the SYNOZ boundary condition versus inclusion of a full stratosphere; c) model horizontal resolution. Model results are compared to observations to determine biases in particular simulations; by examining these comparisons in conjunction with the derived budgets, we may pinpoint

  6. First detection of ammonia (NH3 in the Asian summer monsoon upper troposphere

    Directory of Open Access Journals (Sweden)

    M. Höpfner

    2016-11-01

    Full Text Available Ammonia (NH3 has been detected in the upper troposphere by the analysis of averaged MIPAS (Michelson Interferometer for Passive Atmospheric Sounding infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian summer monsoon at 12–15 km altitude. Three-monthly, 10° longitude  ×  10° latitude average profiles reaching maximum mixing ratios of around 30 pptv in this altitude range have been retrieved, with a vertical resolution of 3–8 km and estimated errors of about 5 pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aerosol layer by the formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5 pptv. This upper bound helps to constrain global model simulations.

  7. Tropospheric chemistry research in the U.S.: 1991-1994

    Science.gov (United States)

    Penner, Joyce E.; Atherton, Cynthia S.; Dignon, Jane

    1995-07-01

    The troposphere is chemically complex. Many of the important species in the troposphere are short-lived, with lifetimes less than or of order of a month. Hence, the composition of the troposphere is regionally diverse, leading to regionally diverse chemical processes which control that composition. With the advent of three-dimensional models and regionally-specific estimates of emissions, however, it has become clear that human activity has perturbed the composition of even short-lived species over vast regions of the globe. The list of short-lived species of concern includes the reactive nitrogen oxides, reactive sulfur, ozone, nonmethane hydrocarbons and carbon monoxide. Observations have established that increases in the long-lived species such as carbon dioxide, methane, nitrous oxide, and the chlorofluorocarbons are taking place with important resulting impacts on stratospheric chemistry. Further, there is some indication that carbonyl sulfide (a major precursor to stratospheric aerosols) may have an important anthropogenic source. Growth of pollutants such as these are of concern because they act as greenhouse gases or aerosol precursors (CO2, CH4, O3, N2O, chlorofluorocarbons, carbonyl sufide, reactive sulfur), as agents for depletion of stratospheric ozone (N2O, chlorofluorocarbons), are harmful to vegetation (O3, acids) or act as nutrients (nitrate, sulfate, trace metals). The chemical interactions are important to understand, because the build up of pollutants depends not only on the rates of their release into the troposphere but on their rate of removal in the troposphere. Removal rates depend on processes which determine the rate of oxidation of the component (which for most species proceeds mainly by reaction with the hydroxyl radical) or through precipitation scavenging or dissolution in the ocean (which requires that the pollutant or its oxidation product(s) be soluble in water).

  8. Commentary on using equivalent latitude in the upper troposphere and lower stratosphere

    Directory of Open Access Journals (Sweden)

    L. L. Pan

    2012-10-01

    Full Text Available We discuss the use of potential vorticity (PV based equivalent latitude (EqLat and potential temperature (θ coordinates in the upper troposphere and lower stratosphere (UTLS for chemical transport studies. The main objective is to provide a cautionary note on using EqLat-θ coordinates for aggregating chemical tracers in the UTLS. Several examples are used to show 3-D distributions of EqLat together with chemical constituents for a range of θ. We show that the use of PV-θ coordinates may not be suitable for several reasons when tropospheric processes are an important part of a study. Due to the different static stability structures between the stratosphere and troposphere, the use of θ as a vertical coordinate does not provide equal representations of the UT and LS. Since the θ surfaces in the troposphere often intersect the surface of the Earth, the θ variable does not work well distinguishing the UT from the boundary layer when used globally as a vertical coordinate. We further discuss the duality of PV/EqLat as a tracer versus as a coordinate variable. Using an example, we show that while PV/EqLat serves well as a transport tracer in the UTLS region, it may conceal the chemical structure associated with wave breaking when used as a coordinate to average chemical tracers. Overall, when choosing these coordinates, considerations need to be made not only based on the time scale of PV being a conservative tracer, but also the specific research questions to be addressed.

  9. submitter Technical Note: Using DEG-CPCs at upper tropospheric temperatures

    CERN Document Server

    Wimmer, D; Nieminen, T; Duplissy, J; Ehrhart, S; Almeida, J; Rondo, L; Franchin, A; Kreissl, F; Bianchi, F; Manninen, H E; Kulmala, M; Curtius, J; Petäjä, T

    2015-01-01

    Over the last few years, several condensation particle counters (CPCs) capable of measuring in the sub-3 nm size range have been developed. Here we study the performance of CPCs based on diethylene glycol (DEG) at different temperatures during Cosmics Leaving OUtdoor Droplets (CLOUD) measurements at CERN. The data shown here are the first set of verification measurements for sub-3 nm CPCs under upper tropospheric temperatures using atmospherically relevant aerosol particles. To put the results in perspective we calibrated the DEG-CPC at room temperature, resulting in a cut-off diameter of 1.4 nm. All diameters refer to mobility equivalent diameters in this paper. At upper tropospheric temperatures ranging from 246.15 K to 207.15 K, we found cut-off sizes relative to a particle size magnifier in the range of 2.5 to 2.8 nm. Due to low number concentration after size classification, the cut-off diameters have a high uncertainty (±0.3 nm) associated with them. Operating two laminar flow DEG-CPCs with different c...

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

    Directory of Open Access Journals (Sweden)

    A. Gaudel

    2018-05-01

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

  11. Predicting tropospheric ozone and hydroxyl radical in a global, three-dimensional, chemistry, transport, and deposition model

    Energy Technology Data Exchange (ETDEWEB)

    Atherton, C.S.

    1995-01-05

    Two of the most important chemically reactive tropospheric gases are ozone (O{sub 3}) and the hydroxyl radical (OH). Although ozone in the stratosphere is a necessary protector against the sun`s radiation, tropospheric ozone is actually a pollutant which damages materials and vegetation, acts as a respiratory irritant, and is a greenhouse gas. One of the two main sources of ozone in the troposphere is photochemical production. The photochemistry is initiated when hydrocarbons and carbon monoxide (CO) react with nitrogen oxides (NO{sub x} = NO + NO{sub 2}) in the presence of sunlight. Reaction with the hydroxyl radical, OH, is the main sink for many tropospheric gases. The hydroxyl radical is highly reactive and has a lifetime on the order of seconds. Its formation is initiated by the photolysis of tropospheric ozone. Tropospheric chemistry involves a complex, non-linear set of chemical reactions between atmospheric species that vary substantially in time and space. To model these and other species on a global scale requires the use of a global, three-dimensional chemistry, transport, and deposition (CTD) model. In this work, I developed two such three dimensional CTD models. The first model incorporated the chemistry necessary to model tropospheric ozone production from the reactions of nitrogen oxides with carbon monoxide (CO) and methane (CH{sub 4}). The second also included longer-lived alkane species and the biogenic hydrocarbon isoprene, which is emitted by growing plants and trees. The models` ability to predict a number of key variables (including the concentration of O{sub 3}, OH, and other species) were evaluated. Then, several scenarios were simulated to understand the change in the chemistry of the troposphere since preindustrial times and the role of anthropogenic NO{sub x} on present day conditions.

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

    Energy Technology Data Exchange (ETDEWEB)

    Han, K.M.; Park, R.S. [School of Environmental Science and Engineering, Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of); Advanced Environmental Monitoring Research Center (ADEMRC), Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of); Kim, H.K.; Woo, J.H. [Department of Advanced Technology Fusion, Konkuk University, 1 Hwayang dong, Gwangjin-gu, Seoul, 143-701 (Korea, Republic of); Kim, J. [Department of Atmospheric Sciences, Yonsei University, 134 Sinchon-dong, Seodaemoon-gu, Seoul, 120-749 (Korea, Republic of); Song, C.H., E-mail: chsong@gist.ac.kr [School of Environmental Science and Engineering, Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of); Advanced Environmental Monitoring Research Center (ADEMRC), Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of)

    2013-10-01

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

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

    International Nuclear Information System (INIS)

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

    2013-01-01

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

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

    Science.gov (United States)

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

    2013-10-01

    In this study, the accuracy of biogenic isoprene emission fluxes over East Asia during two summer months (July and August) was examined by comparing two tropospheric HCHO columns (ΩHCHO) obtained from the SCIAMACHY sensor and the Community Multi-scale Air Quality (CMAQ v4.7.1) model simulations, using three available biogenic isoprene emission inventories over East Asia: i) GEIA, ii) MEGAN and iii) MOHYCAN. From this comparative analysis, the tropospheric HCHO columns from the CMAQ model simulations, using the MEGAN and MOHYCAN emission inventories (Ω(CMAQ, MEGAN) and Ω(CMAQ, MOHYCAN)), were found to agree well with the tropospheric HCHO columns from the SCIAMACHY observations (Ω(SCIA)). Secondly, the propagation of such uncertainties in the biogenic isoprene emission fluxes to the levels of atmospheric oxidants (e.g., OH and HO2) and other atmospheric gaseous/particulate species over East Asia during the two summer months was also investigated. As the biogenic isoprene emission fluxes decreased from the GEIA to the MEGAN emission inventories, the levels of OH radicals increased by factors of 1.39 and 1.75 over Central East China (CEC) and South China, respectively. Such increases in the OH radical mixing ratios subsequently influence the partitioning of HO(y) species. For example, the HO2/OH ratios from the CMAQ model simulations with GEIA isoprene emissions were 2.7 times larger than those from the CMAQ model simulations based on MEGAN isoprene emissions. The large HO2/OH ratios from the CMAQ model simulations with the GEIA biogenic emission were possibly due to the overestimation of GEIA biogenic isoprene emissions over East Asia. It was also shown that such large changes in HO(x) radicals created large differences on other tropospheric compounds (e.g., NO(y) chemistry) over East Asia during the summer months. Copyright © 2013 The Authors. Published by Elsevier B.V. All rights reserved.

  15. Evidence of a 50-year increase in tropospheric ozone in Upper Bavaria

    Directory of Open Access Journals (Sweden)

    M. Schmidt

    Full Text Available In a series of ozone-sonde soundings at the Hohenpeißenberg observatory, starting in 1967, the most striking features are increases of sim2.2% per year in all tropospheric heights up to 8 km during the past 24 years. These facts have recently been published and discussed by several authors. In this paper, we present some evidence for the increase of tropospheric ozone concentrations during the past 50 years 1940-1990 in the territory of the northern edge of the Bavarian Alps, including the Hohenpeißenberg data. In December 1940 and August 1942, probably the first exact wet-chemical vertical soundings of ozone up to 9 km height were made by an aircraft in the region mentioned. These results were published in the earlier literature. We have converted the results of the flights on 4 days in December 1940 and on 6 days in August 1942 to modern units and have compared them with the Hohenpeißenberg ozone-sonde data of the December and August months. We also compared the data at the ground with the August results of Paris-Montsouris 1886-1898. Our results show an increase of ozone concentration at all tropospheric heights in Upper Bavaria during the past 50 years, compared with the Montsouris data in August during the past 105 years. In the recently published papers, the increases since 1967 were approximated linearly.Our results, extended to the past, show non-linear trends, with steeper increases since 1975-1979. Possible reasons for these findings are discussed. Quite recently (in case of the December months since 1986/87, the August months since 1990, the ozone mixing ratios at and above Hohenpeißenberg seem to have decreased.

  16. Evidence of a 50-year increase in tropospheric ozone in Upper Bavaria

    Directory of Open Access Journals (Sweden)

    M. Schmidt

    1994-12-01

    Full Text Available In a series of ozone-sonde soundings at the Hohenpeißenberg observatory, starting in 1967, the most striking features are increases of \\sim2.2% per year in all tropospheric heights up to 8 km during the past 24 years. These facts have recently been published and discussed by several authors. In this paper, we present some evidence for the increase of tropospheric ozone concentrations during the past 50 years 1940-1990 in the territory of the northern edge of the Bavarian Alps, including the Hohenpeißenberg data. In December 1940 and August 1942, probably the first exact wet-chemical vertical soundings of ozone up to 9 km height were made by an aircraft in the region mentioned. These results were published in the earlier literature. We have converted the results of the flights on 4 days in December 1940 and on 6 days in August 1942 to modern units and have compared them with the Hohenpeißenberg ozone-sonde data of the December and August months. We also compared the data at the ground with the August results of Paris-Montsouris 1886-1898. Our results show an increase of ozone concentration at all tropospheric heights in Upper Bavaria during the past 50 years, compared with the Montsouris data in August during the past 105 years. In the recently published papers, the increases since 1967 were approximated linearly.Our results, extended to the past, show non-linear trends, with steeper increases since 1975-1979. Possible reasons for these findings are discussed. Quite recently (in case of the December months since 1986/87, the August months since 1990, the ozone mixing ratios at and above Hohenpeißenberg seem to have decreased.

  17. CARIBIC observations of gaseous mercury in the upper troposphere and lower stratosphere

    Directory of Open Access Journals (Sweden)

    Slemr F.

    2013-04-01

    Full Text Available A unique set of gaseous mercury measurements in the upper troposphere and lower stratosphere (UT/LS has been obtained during the monthly CARIBIC (www.caribic-atmospheric.com flights since May 2005. The passenger Airbus 340-600 of Lufthansa covered routes to the Far East, North America, India, and the southern hemisphere. The accompanying measurements of CO, O3, NOy, H2O, aerosols, halocarbons, hydrocarbons, greenhouse gases, and several other parameters as well as backward trajectories enable a detailed analysis of these measurements. Speciation tests have shown that the CARIBIC measurements represent a good approximation of total gaseous mercury (TGM concentrations. Above the tropopause TGM always decrease with increasing potential vorticity (PV and O3 which implies its conversion to particle bound mercury. The observation of the lowest TGM concentrations at the highest particle concentrations in the stratosphere provides further evidence for such conversion. We will show how a seasonally dependent conversion rate could be derived using concomitantly measured SF6 mixing ratios as a timer. Tropospheric mercury data suggest the existence of a decreasing trend in the northern hemisphere whose size is comparable with the trend derived from long-term measurements by ship cruises, at Cape Point (South Africa and Mace Head (Ireland.

  18. Large differences in reanalyses of diabatic heating in the tropical upper troposphere and lower stratosphere

    Directory of Open Access Journals (Sweden)

    J. S. Wright

    2013-09-01

    Full Text Available We present the time mean heat budgets of the tropical upper troposphere (UT and lower stratosphere (LS as simulated by five reanalysis models: the Modern-Era Retrospective Analysis for Research and Applications (MERRA, European Reanalysis (ERA-Interim, Climate Forecast System Reanalysis (CFSR, Japanese 25-yr Reanalysis and Japan Meteorological Agency Climate Data Assimilation System (JRA-25/JCDAS, and National Centers for Environmental Prediction/National Center for Atmospheric Research (NCEP/NCAR Reanalysis 1. The simulated diabatic heat budget in the tropical UTLS differs significantly from model to model, with substantial implications for representations of transport and mixing. Large differences are apparent both in the net heat budget and in all comparable individual components, including latent heating, heating due to radiative transfer, and heating due to parameterised vertical mixing. We describe and discuss the most pronounced differences. Discrepancies in latent heating reflect continuing difficulties in representing moist convection in models. Although these discrepancies may be expected, their magnitude is still disturbing. We pay particular attention to discrepancies in radiative heating (which may be surprising given the strength of observational constraints on temperature and tropospheric water vapour and discrepancies in heating due to turbulent mixing (which have received comparatively little attention. The largest differences in radiative heating in the tropical UTLS are attributable to differences in cloud radiative heating, but important systematic differences are present even in the absence of clouds. Local maxima in heating and cooling due to parameterised turbulent mixing occur in the vicinity of the tropical tropopause.

  19. Large differences in reanalyses of diabatic heating in the tropical upper troposphere and lower stratosphere

    Science.gov (United States)

    Wright, J. S.; Fueglistaler, S.

    2013-09-01

    We present the time mean heat budgets of the tropical upper troposphere (UT) and lower stratosphere (LS) as simulated by five reanalysis models: the Modern-Era Retrospective Analysis for Research and Applications (MERRA), European Reanalysis (ERA-Interim), Climate Forecast System Reanalysis (CFSR), Japanese 25-yr Reanalysis and Japan Meteorological Agency Climate Data Assimilation System (JRA-25/JCDAS), and National Centers for Environmental Prediction/National Center for Atmospheric Research (NCEP/NCAR) Reanalysis 1. The simulated diabatic heat budget in the tropical UTLS differs significantly from model to model, with substantial implications for representations of transport and mixing. Large differences are apparent both in the net heat budget and in all comparable individual components, including latent heating, heating due to radiative transfer, and heating due to parameterised vertical mixing. We describe and discuss the most pronounced differences. Discrepancies in latent heating reflect continuing difficulties in representing moist convection in models. Although these discrepancies may be expected, their magnitude is still disturbing. We pay particular attention to discrepancies in radiative heating (which may be surprising given the strength of observational constraints on temperature and tropospheric water vapour) and discrepancies in heating due to turbulent mixing (which have received comparatively little attention). The largest differences in radiative heating in the tropical UTLS are attributable to differences in cloud radiative heating, but important systematic differences are present even in the absence of clouds. Local maxima in heating and cooling due to parameterised turbulent mixing occur in the vicinity of the tropical tropopause.

  20. Top-of-atmosphere radiative forcing affected by brown carbon in the upper troposphere

    Science.gov (United States)

    Zhang, Yuzhong; Forrister, Haviland; Liu, Jiumeng; Dibb, Jack; Anderson, Bruce; Schwarz, Joshua P.; Perring, Anne E.; Jimenez, Jose L.; Campuzano-Jost, Pedro; Wang, Yuhang; Nenes, Athanasios; Weber, Rodney J.

    2017-07-01

    Carbonaceous aerosols affect the global radiative balance by absorbing and scattering radiation, which leads to warming or cooling of the atmosphere, respectively. Black carbon is the main light-absorbing component. A portion of the organic aerosol known as brown carbon also absorbs light. The climate sensitivity to absorbing aerosols rapidly increases with altitude, but brown carbon measurements are limited in the upper troposphere. Here we present aircraft observations of vertical aerosol distributions over the continental United States in May and June 2012 to show that light-absorbing brown carbon is prevalent in the troposphere, and absorbs more short-wavelength radiation than black carbon at altitudes between 5 and 12 km. We find that brown carbon is transported to these altitudes by deep convection, and that in-cloud heterogeneous processing may produce brown carbon. Radiative transfer calculations suggest that brown carbon accounts for about 24% of combined black and brown carbon warming effect at the tropopause. Roughly two-thirds of the estimated brown carbon forcing occurs above 5 km, although most brown carbon is found below 5 km. The highest radiative absorption occurred during an event that ingested a wildfire plume. We conclude that high-altitude brown carbon from biomass burning is an unappreciated component of climate forcing.

  1. Multi-station synthesis of early twentieth century surface atmospheric electricity measurements for upper tropospheric properties

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    R. G. Harrison

    2007-07-01

    Full Text Available The vertical columnar current density in the global atmospheric electrical circuit depends on the local columnar resistance. A simple model for the columnar resistance is suggested, which separates the local boundary layer component from the upper troposphere cosmic ray component, and calculates the boundary layer component from a surface measurement of air conductivity. This theory is shown to provide reasonable agreement with observations. One application of the simple columnar model theory is to provide a basis for the synthesis of surface atmospheric electrical measurements made simultaneously at several European sites. Assuming the ionospheric potential to be common above all the sites, the theoretical air-earth current density present in the absence of a boundary layer columnar resistance can be found by extrapolation. This is denoted the free troposphere limit air-earth current density, J0. Using early surface data from 1909 when no ionospheric potential data are available for corroboration, J0 is found to be ~6 pA m−2, although this is subject to uncertainties in the data and limitations in the theory. Later (1966–1971 European balloon and surface data give J0=2.4 pA m−2.

  2. Quasi-biweekly oscillations of the South Asian monsoon and its co-evolution in the upper and lower troposphere

    Science.gov (United States)

    Ortega, Sebastián; Webster, Peter J.; Toma, Violeta; Chang, Hai-Ru

    2017-11-01

    The Upper Tropospheric Quasi-Biweekly Oscillation (UQBW) of the South Asian monsoon is studied using the potential vorticity field on the 370 K isentrope. The UQBW is shown to be a common occurrence in the upper troposphere during the monsoon, and its typical evolution is described. We suggest that the UQBW is a phenomenon of both the middle and tropical latitudes, owing its existence to the presence of the planetary-scale upper-tropospheric monsoon anticyclone. The UQBW is first identified as Rossby waves originating in the northern flank of the monsoon anticyclone. These Rossby waves break when reaching the Pacific Ocean, and their associated cyclonic PV anomalies move southward to the east of Asia and then westward across the Indian Ocean and Africa advected by the monsoon anticyclone. A strong correlation, or co-evolution, between the UQBW and quasi-biweekly oscillations in the lower troposphere (QBW) is also found. In particular, analysis of vertically-integrated horizontal moisture transport, 850 hPa geopotential, and outgoing long-wave radiation show that the UQBW is usually observed at the same time as, and co-evolves with, the lower tropospheric QBW over South Asia. We discuss the nature of the UQBW, and its possible physical link with the QBW.

  3. Observed OH and HO2 concentrations in the upper troposphere inside and outside of Asian monsoon influenced air.

    Science.gov (United States)

    Marno, D. R.; Künstler, C.; Hens, K.; Tatum Ernest, C.; Broch, S.; Fuchs, H.; Martinez, M.; Bourtsoukidis, E.; Williams, J.; Holland, F.; Hofzumahaus, A.; Tomsche, L.; Fischer, H.; Klausner, T.; Schlager, H.; Eirenschmalz, L.; Stratmann, G.; Stock, P.; Ziereis, H.; Roiger, A.; Bohn, B.; Zahn, A.; Wahner, A.; Lelieveld, J.; Harder, H.

    2016-12-01

    The Asian monsoon convectively transports pollutants like volatile organic compounds (VOCs), NOx, and SO2 from the boundary layer over South Asia into the upper troposphere where they can potentially enter the stratosphere, or be dispersed globally. Therefore, it is crucial to understand the oxidizing capacity of this system regarding the rate of aerosol formation, and conversion of pollutants into compounds that have much shorter atmospheric lifetimes. OH plays a central role in this oxidation process. During the OMO-ASIA campaign in the summer of 2015, OH and HO2 were measured onboard the High Altitude Long-Range (HALO) Research Aircraft. Two laser-induced fluorescence instruments based on the fluorescence assay by gas expansion technique (LIF-FAGE) had been deployed, the AIR-LIF instrument from Forschungszentrum Jülich GmbH and the HORUS instrument from the Max Planck Institute for Chemistry, Mainz. To measure the chemical background of OH potentially produced inside the HORUS instrument from highly oxidized VOCs, atmospheric OH is scavenged by an Inlet Pre-injector (IPI) system. This was the first time an IPI system was implemented within an airborne LIF-FAGE instrument measuring OH and HO2. Throughout this campaign OH and HO2 were measured at 12 to 15km within the Asian monsoon anticyclone. These measurements have been contrasted by probing air outside the anticyclone in air masses influenced by North American emissions, and in very clean air masses originated from the southern hemisphere.

  4. Oxalic acid as a heterogeneous ice nucleus in the upper troposphere and its indirect aerosol effect

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    B. Zobrist

    2006-01-01

    Full Text Available Heterogeneous ice freezing points of aqueous solutions containing various immersed solid dicarboxylic acids (oxalic, adipic, succinic, phthalic and fumaric have been measured with a differential scanning calorimeter. The results show that only the dihydrate of oxalic acid (OAD acts as a heterogeneous ice nucleus, with an increase in freezing temperature between 2 and 5 K depending on solution composition. In several field campaigns, oxalic acid enriched particles have been detected in the upper troposphere with single particle aerosol mass spectrometry. Simulations with a microphysical box model indicate that the presence of OAD may reduce the ice particle number density in cirrus clouds by up to ~50% when compared to exclusively homogeneous cirrus formation without OAD. Using the ECHAM4 climate model we estimate the global net radiative effect caused by this heterogeneous freezing to result in a cooling as high as −0.3 Wm−2.

  5. The Origins of Air Parcels Uplifted in a Two Dimensional Gravity Wave in the Tropical Upper Troposphere During the NASA Stratosphere Troposphere Exchange Project (STEP)

    Science.gov (United States)

    Selkirk, Henry B.; Pfister, Leonhard; Chan, K. Roland; Kritz, Mark; Kelly, Ken

    1989-01-01

    During January and February 1987, as part of the Stratosphere-Troposphere Exchange Project, the NASA ER-2 made 11 flights from Darwin, Australia to investigate dehydration mechanisms in the vicinity of the tropical tropopause. After the monsoon onset in the second week of January, steady easterly flow of 15-25 ms (exp -1) was established in the upper troposphere and lower stratosphere over northern Australia and adjacent seas. Penetrating into this regime were elements of the monsoon convection such as overshooting convective turrets and extensive anvils including cyclone cloud shields. In cases of the latter, the resulting flow obstructions tended to produce mesoscale gravity waves. In several instances the ER- 2 meteorological and trace constituent measurements provide a detailed description of the structure of these gravity waves. Among these was STEP Flight 6, 22-23 January. It is of particular interest to STEP because of the close proximity of ice-laden and dehydrated air on the same isentropic surfaces. Convective events inject large amounts of ice into the upper troposphere and lower stratosphere which may not be completely removed by local precipitation processes. In the present instance, a gravity wave for removed from the source region appears to induce relativity rapid upward motion in the ice-laden air and subsequent dessication. Potential mechanisms for such a localized removal process are under investigation.

  6. Mercury oxidation from bromine chemistry in the free troposphere over the southeastern US

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    S. Coburn

    2016-03-01

    Full Text Available The elevated deposition of atmospheric mercury over the southeastern United States is currently not well understood. Here we measure partial columns and vertical profiles of bromine monoxide (BrO radicals, a key component of mercury oxidation chemistry, to better understand the processes and altitudes at which mercury is being oxidized in the atmosphere. We use data from a ground-based MAX-DOAS instrument located at a coastal site ∼  1 km from the Gulf of Mexico in Gulf Breeze, FL, where we had previously detected tropospheric BrO (Coburn et al., 2011. Our profile retrieval assimilates information about stratospheric BrO from the WACCM chemical transport model (CTM, and uses only measurements at moderately low solar zenith angles (SZAs to estimate the BrO slant column density contained in the reference spectrum (SCDRef. The approach has 2.6 degrees of freedom, and avoids spectroscopic complications that arise at high SZA; knowledge about SCDRef further helps to maximize sensitivity in the free troposphere (FT. A cloud-free case study day with low aerosol load (9 April 2010 provided optimal conditions for distinguishing marine boundary layer (MBL: 0–1 km and free-tropospheric (FT: 1–15 km BrO from the ground. The average daytime tropospheric BrO vertical column density (VCD of ∼  2.3  ×  1013 molec cm−2 (SZA  <  70° is consistent with our earlier reports on other days. The vertical profile locates essentially all tropospheric BrO above 4 km, and shows no evidence for BrO inside the MBL (detection limit  <  0.5 pptv. BrO increases to  ∼  3.5 pptv at 10–15 km altitude, consistent with recent aircraft observations. Our case study day is consistent with recent aircraft studies, in that the oxidation of gaseous elemental mercury (GEM by bromine radicals to form gaseous oxidized mercury (GOM is the dominant pathway for GEM oxidation throughout the troposphere above Gulf

  7. Interrelated variations of O3, CO and deep convection in the tropical/subtropical upper troposphere observed by the Aura Microwave Limb Sounder (MLS during 2004–2011

    Directory of Open Access Journals (Sweden)

    L. Froidevaux

    2013-01-01

    Full Text Available The interrelated geographic and temporal variability seen in more than seven years of tropical and subtropical upper tropospheric (215 hPa ozone, carbon monoxide and cloud ice water content (IWC observations by the Aura Microwave Limb Sounder (MLS are presented. Observed ozone abundances and their variability (geographic and temporal agree to within 10–15 ppbv with records from sonde observations. MLS complements these (and other observations with global coverage and simultaneous measurements of related parameters. Previously-reported phenomena such as the ozone "wave one" feature are clearly seen in the MLS observations, as is a double peak in ozone abundance over tropical East Africa, with enhanced abundances in both May to June and September to November. While repeatable seasonal cycles are seen in many regions, they are often accompanied by significant interannual variability. Ozone seasonal cycles in the southern tropics and subtropics tend to be more distinct (i.e., annually repeatable than in the northern. By contrast, carbon monoxide shows distinct seasonal cycles in many northern subtropical regions, notably from India to the Eastern Pacific. Deep convection (as indicated by large values of IWC is typically associated with reductions in upper tropospheric ozone. Convection over polluted regions is seen to significantly enhance upper tropospheric carbon monoxide. While some regions show statistically significant correlations among ozone, carbon monoxide and IWC, simple correlations fall well short of accounting for the observed variability. The observed interrelated variations and metrics of annual and interannual variability described here represent a new resource for validation of atmospheric chemistry models.

  8. The Vertical Structure of Relative Humidity and Ozone in the Tropical Upper Troposphere: Intercomparisons Among In Situ Observations, A-Train Measurements and Large-Scale Models

    Science.gov (United States)

    Selkirk, Henry B.; Manyin, Michael; Douglass, Anne R.; Oman, Luke; Pawson, Steven; Ott, Lesley; Benson, Craig; Stolarski, Richard

    2010-01-01

    In situ measurements in the tropics have shown that in regions of active convection, relative humidity with respect to ice in the upper troposphere is typically close to saturation on average, and supersaturations greater than 20% are not uncommon. Balloon soundings with the cryogenic frost point hygrometer (CFH) at Costa Rica during northern summer, for example, show this tendency to be strongest between 11 and 15.5 km (345-360 K potential temperature, or approximately 250-120 hPa). this is the altitude range of deep convective detrainment. Additionally, simultaneous ozonesonde measurements show that stratospheric air (O3 greater than 150 ppbv) can be found as low as approximately 14 km (350 K/150 hPa). In contrast, results from northern winter show a much drier upper troposphere and little penetration of stratospheric air below the tropopause at 17.5 km (approximately 383 K). We show that these results are consistent with in situ measurements from the Measurement of Ozone and water vapor by Airbus In-service airCraft (MOZAIC) program which samples a wider, though still limited, range of tropical locations. To generalize to the tropics as a whole, we compare our insitu results to data from two A-Train satellite instruments, the Atmospheric Infrared Sounder (AIRS) and the Microwave Limb Sounder (MLS) on the Aqua and Aura satellites respectively. Finally, we examine the vertical structure of water vapor, relative humidity and ozone in the NASA Goddard MERRA analysis, an assimilation dataset, and a new version of the GEOS CCM, a free-running chemistry-climate model. We demonstrate that conditional probability distributions of relative humidity and ozone are a sensitive diagnostic for assessing the representation of deep convection and upper troposphere/lower stratosphere mixing processes in large-scale analyses and climate models.

  9. On the Climate Impacts of Upper Tropospheric and Lower Stratospheric Ozone

    Science.gov (United States)

    Xia, Yan; Huang, Yi; Hu, Yongyun

    2018-01-01

    The global warming simulations of the general circulation models (GCMs) are generally performed with different ozone prescriptions. We find that the differences in ozone distribution, especially in the upper tropospheric and lower stratospheric (UTLS) region, account for important model discrepancies shown in the ozone-only historical experiment of the Coupled Model Intercomparison Project Phase 5 (CMIP5). These discrepancies include global high cloud fraction, stratospheric temperature, and stratospheric water vapor. Through a set of experiments conducted by an atmospheric GCM with contrasting UTLS ozone prescriptions, we verify that UTLS ozone not only directly radiatively heats the UTLS region and cools the upper parts of the stratosphere but also strongly influences the high clouds due to its impact on relative humidity and static stability in the UTLS region and the stratospheric water vapor due to its impact on the tropical tropopause temperature. These consequences strongly affect the global mean effective radiative forcing of ozone, as noted in previous studies. Our findings suggest that special attention should be paid to the UTLS ozone when evaluating the climate effects of ozone depletion in the 20th century and recovery in the 21st century. UTLS ozone difference may also be important for understanding the intermodel discrepancy in the climate projections of the CMIP6 GCMs in which either prescribed or interactive ozone is used.

  10. Particulate sulfur in the upper troposphere and lowermost stratosphere – sources and climate forcing

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    B. G. Martinsson

    2017-09-01

    Full Text Available This study is based on fine-mode aerosol samples collected in the upper troposphere (UT and the lowermost stratosphere (LMS of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8–12 km altitude of the IAGOS-CARIBIC platform in the time period 1999–2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission and PESA (particle elastic scattering analysis. Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL. Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of

  11. On the origin of subvisible cirrus clouds in the tropical upper troposphere

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    M. Reverdy

    2012-12-01

    Full Text Available Spaceborne lidar observations have recently revealed a previously undetected significant population of Subvisible Cirrus (SVC. We show them to be colder than −74 °, with an optical depth below 0.0015 on average. The formation and persistence over time of this new cloud population could be related to several atmospheric phenomena. In this paper, we investigate if these clouds follow the same formation mechanisms as the general tropical cirrus population (including convection and in-situ ice nucleation, or if specific nucleation sites and trace species play a role in their formation. The importance of three scenarios in the formation of the global SVC population is investigated through different approaches that include comparisons with data imaging from several spaceborne instruments and back-trajectories that document the history and behavior of air masses leading to the point in time and space where subvisible cirrus were detected. In order to simplify the study of their formation, we singled out SVC with coherent temperature histories (mean variance lower than 4 K according to back-trajectories along 5, 10 or 15 days (respectively 58, 25 and 11% of SVC. Our results suggest that external processes, including local increases in liquid and hygroscopic aerosol concentration (either through biomass burning or volcanic injection forming sulfate-based aerosols in the troposphere or the stratosphere have very limited short-term or mid-term impact on the SVC population. On the other hand, we find that ~20% of air masses leading to SVC formation interacted with convective activity 5 days before they led to cloud formation and detection, a number that climbs to 60% over 15 days. SVC formation appears especially linked to convection over Africa and Central America, more so during JJA than DJF. These results support the view that the SVC population observed by CALIOP is an extension of the general upper tropospheric ice clouds population with its extreme

  12. Retrieval of global upper tropospheric and stratospheric formaldehyde (H2CO distributions from high-resolution MIPAS-Envisat spectra

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    G. P. Stiller

    2008-02-01

    Full Text Available The Fourier transform spectrometer MIPAS (Michelson Interferometer for Passive Atmospheric Sounding on Envisat measures infrared emission of the Earth's atmosphere in a limb viewing mode. High spectral resolution measurements of MIPAS are sensitive to formaldehyde from the upper troposphere to the stratopause. Single profile retrievals of formaldehyde are dominated by a 60% noise error; however zonal mean values for 30 days of data during 8 September 2003 and 1 December 2003 reduces this error by a factor of 20 or more. The number of degrees of freedom for single profile retrieval ranges from 2 to 4.5 depending on latitude and number of cloud-free tangent altitudes. In the upper tropical troposphere zonal mean values of about 70 parts per trillion by volume (pptv were found, which have been attributed to biomass burning emissions. In the stratosphere, formaldehyde values are determined by photochemical reactions. In the upper tropical stratosphere, formaldehyde zonal mean maximum values can reach 130 pptv. Diurnal variations in this region can be up to 50 pptv. Comparisons with other satellite instruments show generally good agreement in the region of upper troposphere and lower stratosphere as well as in the upper stratosphere.

  13. 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

  14. Met UM Upper-tropospheric summer jet teleconnections: A model assessment

    Science.gov (United States)

    Joao Carvalho, Maria; Rodriguez, Jose; Milton, Sean

    2017-04-01

    The upper tropospheric jet stream has been documented to act as a waveguide (Hoskins and Ambrizzi, 1993) and supporting quasi-stationary Rossby waves (Schubert et al. 2011). These have been associated with remote effects in surface level weather such as rainfall anomalies in the East Asian Summer Monsoon as well as extreme temperature events. The goal of this work was to analyse the intraseasonal to interannual upper level boreal summer jet variability and its coupling with low level atmospheric dynamics within the Met Office Unified Model using climate runs. Using the Wallace and Gutzler (1981) proposed approach to find teleconnection patterns on the 200 hPa level wind, lead-lag correlation and Empirical Orthogonal Function analysis on the upper-level jet and relating the results with surface weather variables as well as dynamical variables, it was found that the model presents too strong jet variability, particularly in the tropical region and. In addition, the model presents high teleconnectivity hotspots with higher importance in areas such as the Mediterranean and Caspian Sea which are important source areas for Rossby Waves. Further to this, the model was found to produce an area of teleconnectivity between the tropical Atlantic and western Africa which is not observed in the reanalysis but coexists with long lasting precipitation biases. As comparison for the model results, ERA-Interim circulation and wind data and the TRMM precipitation dataset were used. In order to assess the relative importance of relevant model parameters in the biases and process errors, work is currently underway using perturbed model parameter ensembles.

  15. Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

    Science.gov (United States)

    Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; Amorim Holanda, Bruna; Artaxo, Paulo; Barbosa, Henrique M. J.; Borrmann, Stephan; Cecchini, Micael A.; Costa, Anja; Dollner, Maximilian; Fütterer, Daniel; Järvinen, Emma; Jurkat, Tina; Klimach, Thomas; Konemann, Tobias; Knote, Christoph; Krämer, Martina; Krisna, Trismono; Machado, Luiz A. T.; Mertes, Stephan; Minikin, Andreas; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; Rosenfeld, Daniel; Sauer, Daniel; Schlager, Hans; Schnaiter, Martin; Schneider, Johannes; Schulz, Christiane; Spanu, Antonio; Sperling, Vinicius B.; Voigt, Christiane; Walser, Adrian; Wang, Jian; Weinzierl, Bernadett; Wendisch, Manfred; Ziereis, Helmut

    2018-01-01

    Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September-October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles ( 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable

  16. Concentrations of ethane (C2H6) in the lower stratosphere and upper troposphere and acetylene (C2H2) in the upper troposphere deduced from Atmospheric Trace Molecule Spectroscopy/Spacelab 3 spectra

    Science.gov (United States)

    Rinsland, C. P.; Russell, J. M., III; Zander, R.; Farmer, C. B.; Norton, R. H.

    1987-01-01

    This paper reports the results of the spectroscopic analysis of C2H6 and C2H2 absorption spectra obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument flown on the Shuttle as part of the Spacelab 3 mission. The spectra were recorded during sunset occultations occurring between 25 deg N and 31 deg N latitudes, yielding volume-mixing ratio profiles of C2H6 in the lower stratosphere and the upper troposphere, and an upper tropospheric profile of C2H2. These results compare well with previous in situ and remote sounding data obtained at similar latitudes and with model calculations. The results demonstrate the feasibility of the ATMOS instrument to sound the lower atmosphere from space.

  17. The representation of tropical upper tropospheric water in EC Earth V2

    Energy Technology Data Exchange (ETDEWEB)

    Johnston, M.S. [Chalmers University of Technology, Department of Earth and Space Sciences, Goeteburg (Sweden); Swedish Meteorological and Hydrological Institute (SMHI), Norrkoeping (Sweden); Eriksson, P.; Murtagh, D.P. [Chalmers University of Technology, Department of Earth and Space Sciences, Goeteburg (Sweden); Eliasson, S. [Luleaa University of Technology, Department of Computer Science, Electrical and Space Engineering, Kiruna (Sweden); Jones, C.G. [Swedish Meteorological and Hydrological Institute (SMHI), Norrkoeping (Sweden); Forbes, R.M. [ECMWF, Reading, Berkshire (United Kingdom)

    2012-12-15

    Tropical upper tropospheric humidity, clouds, and ice water content, as well as outgoing longwave radiation (OLR), are evaluated in the climate model EC Earth with the aid of satellite retrievals. The Atmospheric Infrared Sounder and Microwave Limb Sounder together provide good coverage of relative humidity. EC Earth's relative humidity is in fair agreement with these observations. CloudSat and CALIPSO data are combined to provide cloud fractions estimates throughout the altitude region considered (500-100 hPa). EC Earth is found to overestimate the degree of cloud cover above 200 hPa and underestimate it below. Precipitating and non-precipitating EC Earth ice definitions are combined to form a complete ice water content. EC Earth's ice water content is below the uncertainty range of CloudSat above 250 hPa, but can be twice as high as CloudSat's estimate in the melting layer. CERES data show that the model underestimates the impact of clouds on OLR, on average with about 9 W m{sup -2}. Regionally, EC Earth's outgoing longwave radiation can be {proportional_to}20 W m{sup -2} higher than the observation. A comparison to ERA-Interim provides further perspectives on the model's performance. Limitations of the satellite observations are emphasised and their uncertainties are, throughout, considered in the analysis. Evaluating multiple model variables in parallel is a more ambitious approach than is customary. (orig.)

  18. Seasonality of Peroxyacetyl nitrate (PAN in the upper troposphere and lower stratosphere using the MIPAS-E instrument

    Directory of Open Access Journals (Sweden)

    D. P. Moore

    2010-07-01

    Full Text Available The Michelson Interferometer for Passive Atmospheric Sounding onboard ENVISAT (MIPAS–E offers the opportunity to detect and spectrally resolve many atmospheric minor constituents affecting atmospheric chemistry. In this paper, we retrieve global, seasonal PAN volume mixing ratio (vmr data from MIPAS-E measurements made in January, March, August and October 2003 and present results from this scheme between approximately 300 and 150 hPa. The total error on a single PAN retrieval is better than 20% outside the tropics and better than 50% in the tropics where uncertainties in water vapor dominate the total error budget. We observe clear differences in the seasonal cycle of PAN in our data, linked closely to biomass burning regions and growing seasons. Highest Northern Hemisphere mid-latitude PAN vmrs were observed in August (300–600 pptv on average compared with the January and October data (less than 250 pptv on average. In the March 2003 data we observe highest PAN vmrs in the tropics with evidence of vmrs between 600 and 1000 pptv over Eastern Asia and over the Central Pacific at 333 hPa. The vertical distribution of PAN as a function of latitude (i.e. the zonal mean highlights the strong inter-annual variability of PAN in the upper troposphere and lower stratosphere (UTLS, most pronounced poleward of 40° N (up to 400 pptv over the year. The variability of PAN in the tropical UTLS is also significant and we derive a variability of up to 250 pptv in the averages between January and October 2003. These results represent the first seasonal observations of PAN in the UTLS.

  19. Chemistry and dynamics of the lower troposphere over North America and the North Atlantic Ocean in fall 1997 observed using an airborne UV DIAL system

    Science.gov (United States)

    Grant, William B.; Butler, Carolyn F.; Fenn, Marta A.; Kooi, Susan A.; Browell, Edward V.; Fuelberg, Henry

    1998-01-01

    The NASA Langley Research Center's airborne UV Differential Absorption Lidar (DIAL) system participated in the Subsonic Assessment, Ozone and Nitrogen Oxide Experiment (SONEX) mission from October 13 to November 12, 1997. The purpose of the mission was to study the upper troposphere/lower stratosphere in and near the North Atlantic flight corridor to better understand this region of the atmosphere and how civilian air travel in the corridor might be affecting the atmospheric chemistry. Bases of operations included NASA Ames, California (37.4 deg N, 122.1 deg W); Bangor, Maine (44.8 deg N, 68.8 deg W); Shannon, Ireland (52.7 deg N, 8.9 deg W); and Lajes, Terceira Island, Azores (38.8 deg N, 27.1 deg W). Since the UV DIAL system observes in the nadir as well as the zenith, aerosol and ozone data were obtained from near the Earth's surface to the lower stratosphere. A number of interesting features were noted relating to both chemistry and dynamics of the troposphere, which are reported here.

  20. Retrieval of water vapor vertical distributions in the upper troposphere and the lower stratosphere from SCIAMACHY limb measurements

    OpenAIRE

    Rozanov, A.; Weigel, K.; Bovensmann, H.; Dhomse, S.; Eichmann, K.-U.; Kivi, R.; Rozanov, V.; Vömel, H.; Weber, M.; Burrows, J. P.

    2011-01-01

    This study describes the retrieval of water vapor vertical distributions in the upper troposphere and lower stratosphere (UTLS) altitude range from space-borne observations of the scattered solar light made in limb viewing geometry. First results using measurements from SCIAMACHY (Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY) aboard ENVISAT (Environmental Satellite) are presented here. In previous publications, the retrieval of water vapor vertical ...

  1. Summertime mid-to-upper tropospheric nitrous oxide over the Mediterranean as a footprint of Indian emissions

    Science.gov (United States)

    Kangah, Yannick; Ricaud, Philippe; Attié, Jean-Luc; Saitoh, Naoko; Hauglustaine, Didier; El Amraoui, Laaziz; Zbinden, Regina; Delon, Claire

    2016-04-01

    We used global scale thermal infrared measurements of mid-to-upper tropospheric nitrous oxide (N2O) from the Greenhouse gases Observing SATellite (GOSAT) and outputs from the 3D Chemical Transport Model LMDz-OR-INCA to assess the impact of the Indian subcontinent N2O emissions on the N2O field over the eastern Mediterranean Basin (MB) during summer. The use of nitrogen fertilizer coupled with high soil humidity during summer monsoon period produce high emissions of N2O in many south Asian countries and especially the Indian subcontinent. N2O is transported to the upper troposphere by updrafts associated to the monsoon and redistributed westward to the eastern Mediterranean via the Asian Monsoon Anticyclone. This summertime (June-July-August) enrichment in N2O in the eastern Mediterranean produces a maximum in the east-west difference of MB mid-to-upper tropospheric N2O anomaly representative for the period 2010-2013 with a maximum in July and a peak-to-peak amplitude of ~1.0 ± 0.3 ppbv observed by GOSAT consistently with LMDz-OR-INCA but less intense (~0.5 ppbv). This summertime enrichment of N2O over the eastern Mediterranean is consistent with the increase of the surface emissions and the convective precipitations over the Indian subcontinent during the summer monsoon period. N2O over the eastern Mediterranean can therefore be considered as a footprint of Indian summertime emissions.

  2. Towards a Model Climatology of Relative Humidity in the Upper Troposphere for Estimation of Contrail and Contrail-Induced Cirrus

    Science.gov (United States)

    Selkirk, Henry B.; Manyin, M.; Ott, L.; Oman, L.; Benson, C.; Pawson, S.; Douglass, A. R.; Stolarski, R. S.

    2011-01-01

    The formation of contrails and contrail cirrus is very sensitive to the relative humidity of the upper troposphere. To reduce uncertainty in an estimate of the radiative impact of aviation-induced cirrus, a model must therefore be able to reproduce the observed background moisture fields with reasonable and quantifiable fidelity. Here we present an upper tropospheric moisture climatology from a 26-year ensemble of simulations using the GEOS CCM. We compare this free-running model's moisture fields to those obtained from the MLS and AIRS satellite instruments, our most comprehensive observational databases for upper tropospheric water vapor. Published comparisons have shown a substantial wet bias in GEOS-5 assimilated fields with respect to MLS water vapor and ice water content. This tendency is clear as well in the GEOS CCM simulations. The GEOS-5 moist physics in the GEOS CCM uses a saturation adjustment that prevents supersaturation, which is unrealistic when compared to in situ moisture observations from MOZAIC aircraft and balloon sondes as we will show. Further, the large-scale satellite datasets also consistently underestimate super-saturation when compared to the in-situ observations. We place these results in the context of estimates of contrail and contrail cirrus frequency.

  3. Does acetone react with HO2 in the upper-troposphere?

    Directory of Open Access Journals (Sweden)

    J. Lelieveld

    2012-02-01

    Full Text Available Recent theoretical calculations showed that reaction with HO2 could be an important sink for acetone (CH3C(OCH3 and source of acetic acid (CH3C(OOH in cold parts of the atmosphere (e.g. the tropopause region. This work details studies of HO2 + CH3C(OCH3 (CH32C(OHOO (R1 in laboratory-based and theoretical chemistry experiments; the atmospheric significance of Reaction (R1 was assessed in a global 3-D chemical model. Pulsed laser-kinetic experiments were conducted, for the first time, at the low-temperatures representative of the tropopause. Reaction with NO converted HO2 to OH for detection by laser induced fluorescence. Reduced yields of OH at T 2 by CH3C(OCH3 with a forward rate coefficient greater than 2 × 10−12 cm3 molecule−1 s−1. No evidence for Reaction (R1 was observed at T > 230 K, probably due to rapid thermal dissociation back to HO2 + CH3C(OCH3. Numerical simulations of the data indicate that these experiments were sensitive to only (R1a HO2-CH3C(OCH3 complex formation, the first step in (R1. Rearrangement (R1b of the complex to form peroxy radicals, and hence the atmospheric significance of (R1 has yet to be rigorously verified by experiment. Results from new quantum chemical calculations indicate that K1 is characterised by large uncertainties of at least an order of magnitude at T 3C(OCH3 near the tropopause, it cannot explain observations of CH3C(OOH throughout the troposphere.

  4. Large-scale tropospheric transport in the Chemistry-Climate Model Initiative (CCMI) simulations

    Science.gov (United States)

    Orbe, Clara; Yang, Huang; Waugh, Darryn W.; Zeng, Guang; Morgenstern, Olaf; Kinnison, Douglas E.; Lamarque, Jean-Francois; Tilmes, Simone; Plummer, David A.; Scinocca, John F.; Josse, Beatrice; Marecal, Virginie; Jöckel, Patrick; Oman, Luke D.; Strahan, Susan E.; Deushi, Makoto; Tanaka, Taichu Y.; Yoshida, Kohei; Akiyoshi, Hideharu; Yamashita, Yousuke; Stenke, Andreas; Revell, Laura; Sukhodolov, Timofei; Rozanov, Eugene; Pitari, Giovanni; Visioni, Daniele; Stone, Kane A.; Schofield, Robyn; Banerjee, Antara

    2018-05-01

    Understanding and modeling the large-scale transport of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. Here we show that there are large differences in the global-scale atmospheric transport properties among the models participating in the IGAC SPARC Chemistry-Climate Model Initiative (CCMI). Specifically, we find up to 40 % differences in the transport timescales connecting the Northern Hemisphere (NH) midlatitude surface to the Arctic and to Southern Hemisphere high latitudes, where the mean age ranges between 1.7 and 2.6 years. We show that these differences are related to large differences in vertical transport among the simulations, in particular to differences in parameterized convection over the oceans. While stronger convection over NH midlatitudes is associated with slower transport to the Arctic, stronger convection in the tropics and subtropics is associated with faster interhemispheric transport. We also show that the differences among simulations constrained with fields derived from the same reanalysis products are as large as (and in some cases larger than) the differences among free-running simulations, most likely due to larger differences in parameterized convection. Our results indicate that care must be taken when using simulations constrained with analyzed winds to interpret the influence of meteorology on tropospheric composition.

  5. The chemical effects on the summertime ozone in the upper troposphere and lower stratosphere over the Tibetan Plateau and the South Asian monsoon region

    Science.gov (United States)

    Gu, Yixuan; Liao, Hong; Xu, Jianming; Zhou, Guangqiang

    2018-01-01

    We use the global three-dimensional Goddard Earth Observing System chemical transport model with the Universal tropospheric-stratospheric Chemistry eXtension mechanism to examine the contributions of the chemical processes to summertime O3 in the upper troposphere and lower stratosphere (UTLS) over the Tibetan Plateau and the South Asian monsoon region (TP/SASM). Simulated UTLS O3 concentrations are evaluated by comparisons with Microwave Limb Sounder products and net chemical production of O3 (NPO3) are evaluated by comparisons with model results in previous studies. Simulations show that the chemical processes lead to an increase in O3 concentration, which is opposite to the effect of O3 transport in the UTLS over the TP/SASM region throughout the boreal summer. NPO3 in UTLS over the TP/SASM region is the largest in summer. Elevated values (0.016-0.020 Tg year-1) of the seasonal mean NPO3 are simulated to locate at 100 hPa in the TP/SASM region, where the mixing ratios of O3 are low and those of O3 precursors (NO x , VOCs, and CO) are high. The high concentrations of O3 precursors (NO x , VOCs, and CO) together with the active photochemical reactions of NO2 in the UTLS over the TP/SASM region during summertime could be important reasons for the enhancement of {NP}_{{{O}3 }} over the studied region.

  6. Two-dimensional performance of MIPAS observation modes in the upper-troposphere/lower-stratosphere

    Directory of Open Access Journals (Sweden)

    M. Carlotti

    2011-02-01

    Full Text Available In this paper we analyze the performance of the three MIPAS (Michelson Interferometer for Passive Atmospheric Sounding observation modes that sound the Upper-Troposphere/Lower-Stratosphere (UT/LS region. The two-dimensional (2-D tomographic retrieval approach is assumed to derive the atmospheric field of geophysical parameters. For each observation mode we have calculated the 2-D distribution of the information load quantifier relative to the main MIPAS targets. The performance of the observation modes has been evaluated in terms of strength and spatial coverage of the information-load distribution along the full orbit. The indications of the information-load analysis has been validated with simulated retrievals based on the observational parameters of real orbits. In the simulation studies we have assessed the precision and the spatial (both horizontal and vertical resolution of the retrieval products. The performance of the three observation modes has been compared for the MIPAS main products in both the UT/LS and the extended altitude range. This study shows that the two observation modes that were specifically designed for the UT/LS region are actually competitive with the third one, designed for the whole stratosphere, up to altitudes that far exceed the UT/LS. In the UT/LS the performance of the two specific observation modes is comparable even if the best performance in terms of horizontal resolution is provided by the observation mode that was excluded by the European Space Agency (ESA from the current MIPAS duty cycle. This paper reports the first application of the information-load analysis and highlights the worthiness of this approach to make qualitative considerations about retrieval potential and selection of retrieval grid.

  7. NOAA Climate Data Record for Mean Layer Temperature (Upper Troposphere & Lower Stratosphere) from UCAR, Version 2

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — The Temperatures of Troposphere / Stratosphere (TTS) (AMSU channel 7 and MSU channel 3) CDR is generated by using National Oceanic and Atmospheric Administration...

  8. Evaluation of Satellite-Based Upper Troposphere Cloud Top Height Retrievals in Multilayer Cloud Conditions During TC4

    Science.gov (United States)

    Chang, Fu-Lung; Minnis, Patrick; Ayers, J. Kirk; McGill, Matthew J.; Palikonda, Rabindra; Spangenberg, Douglas A.; Smith, William L., Jr.; Yost, Christopher R.

    2010-01-01

    Upper troposphere cloud top heights (CTHs), restricted to cloud top pressures (CTPs) less than 500 hPa, inferred using four satellite retrieval methods applied to Twelfth Geostationary Operational Environmental Satellite (GOES-12) data are evaluated using measurements during the July August 2007 Tropical Composition, Cloud and Climate Coupling Experiment (TC4). The four methods are the single-layer CO2-absorption technique (SCO2AT), a modified CO2-absorption technique (MCO2AT) developed for improving both single-layered and multilayered cloud retrievals, a standard version of the Visible Infrared Solar-infrared Split-window Technique (old VISST), and a new version of VISST (new VISST) recently developed to improve cloud property retrievals. They are evaluated by comparing with ER-2 aircraft-based Cloud Physics Lidar (CPL) data taken during 9 days having extensive upper troposphere cirrus, anvil, and convective clouds. Compared to the 89% coverage by upper tropospheric clouds detected by the CPL, the SCO2AT, MCO2AT, old VISST, and new VISST retrieved CTPs less than 500 hPa in 76, 76, 69, and 74% of the matched pixels, respectively. Most of the differences are due to subvisible and optically thin cirrus clouds occurring near the tropopause that were detected only by the CPL. The mean upper tropospheric CTHs for the 9 days are 14.2 (+/- 2.1) km from the CPL and 10.7 (+/- 2.1), 12.1 (+/- 1.6), 9.7 (+/- 2.9), and 11.4 (+/- 2.8) km from the SCO2AT, MCO2AT, old VISST, and new VISST, respectively. Compared to the CPL, the MCO2AT CTHs had the smallest mean biases for semitransparent high clouds in both single-layered and multilayered situations whereas the new VISST CTHs had the smallest mean biases when upper clouds were opaque and optically thick. The biases for all techniques increased with increasing numbers of cloud layers. The transparency of the upper layer clouds tends to increase with the numbers of cloud layers.

  9. Acetylene C2H 2 retrievals from MIPAS data and regions of enhanced upper tropospheric concentrations in August 2003

    Directory of Open Access Journals (Sweden)

    V. P. Kanawade

    2011-10-01

    Full Text Available Acetylene (C2H2 volume mixing ratios (VMRs have been successfully retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS Level 1B radiances during August 2003, providing the first global map of such data and ratios to CO in the literature. The data presented here contain most information between 300 hPa and 100 hPa with systematic errors less than 10% at the upper levels. Random errors per point are less than 15% at lower levels and are closer to 30% at 100 hPa. Global distributions of the C2H2 and C2H2/CO ratio confirm significant features associated with both the Asian monsoon anticyclone and biomass burning for this important hydrocarbon in a characteristic summer month (August 2003, showing tight correlations regionally, particularly at lower to medium values, but globally emphasising the differences between sources and lifetimes of CO and C2H2. The correlations are seen to be particularly disturbed in the regions of highest C2H2 concentrations, indicating variability in the surface emissions or fast processing. A strong isolation of C2H2 within the Asian monsoon anticyclone is observed, evidencing convective transport into the upper troposphere, horizontal advection within the anticyclone at 200 hPa, distinct gradients at the westward edge of the vortex and formation of a secondary dynamical feature from the eastward extension of the anticyclone outflow over the Asian Pacific. Ratios of C2H2/CO are consistent with the evidence from the cross-sections that the C2H2 is uplifted rapidly in convection. Observations are presented of enhanced C2H2 associated with the injection from biomass burning into the upper troposphere and the outflow from Africa at 200 hPa into both the Atlantic and Indian Oceans. In the biomass burning regions, C2H2 and CO are well correlated, but the uplift is less marked and peaks at lower altitudes compared to the strong effects observed in the Asian monsoon anticyclone. Ratios of C2H2/CO

  10. How predictable is the northern hemisphere summer upper-tropospheric circulation?

    Energy Technology Data Exchange (ETDEWEB)

    Lee, June-Yi; Wang, Bin [University of Hawaii/IPRC, International Pacific Research Center, Honolulu, HI (United States); Ding, Q. [University of Washington, Department of Earth and Space Sciences and Quaternary Research Center, Seattle, WA (United States); Ha, K.J.; Ahn, J.B. [Pusan National University, Division of Earth Environmental System, Busan (Korea, Republic of); Kumar, A. [NCEP/CPC, Camp Springs, MD (United States); Stern, B. [Princeton University, NOAA/GFDL, Princeton, NJ (United States); Alves, O. [Bureau of Meteorology, Centre for Australia Weather and Climate Research (CAWCR), Melbourne, VIC (Australia)

    2011-09-15

    The retrospective forecast skill of three coupled climate models (NCEP CFS, GFDL CM2.1, and CAWCR POAMA 1.5) and their multi-model ensemble (MME) is evaluated, focusing on the Northern Hemisphere (NH) summer upper-tropospheric circulation along with surface temperature and precipitation for the 25-year period of 1981-2005. The seasonal prediction skill for the NH 200-hPa geopotential height basically comes from the coupled models' ability in predicting the first two empirical orthogonal function (EOF) modes of interannual variability, because the models cannot replicate the residual higher modes. The first two leading EOF modes of the summer 200-hPa circulation account for about 84% (35.4%) of the total variability over the NH tropics (extratropics) and offer a hint of realizable potential predictability. The MME is able to predict both spatial and temporal characteristics of the first EOF mode (EOF1) even at a 5-month lead (January initial condition) with a pattern correlation coefficient (PCC) skill of 0.96 and a temporal correlation coefficient (TCC) skill of 0.62. This long-lead predictability of the EOF1 comes mainly from the prolonged impacts of El Nino-Southern Oscillation (ENSO) as the EOF1 tends to occur during the summer after the mature phase of ENSO. The second EOF mode (EOF2), on the other hand, is related to the developing ENSO and also the interdecadal variability of the sea surface temperature over the North Pacific and North Atlantic Ocean. The MME also captures the EOF2 at a 5-month lead with a PCC skill of 0.87 and a TCC skill of 0.67, but these skills are mainly obtained from the zonally symmetric component of the EOF2, not the prominent wavelike structure, the so-called circumglobal teleconnection (CGT) pattern. In both observation and the 1-month lead MME prediction, the first two leading modes are accompanied by significant rainfall and surface air temperature anomalies in the continental regions of the NH extratropics. The MME

  11. Mid-upper tropospheric methane retrieval from IASI and its validation

    Directory of Open Access Journals (Sweden)

    X. Xiong

    2013-09-01

    Full Text Available Mid-upper tropospheric methane (CH4, as an operational product at NOAA's (National Oceanic and Atmospheric Administration Comprehensive Large Array-data Stewardship System (CLASS, has been retrieved from the Infrared Atmospheric Sounding Interferometer (IASI since 2008. This paper provides a description of the retrieval method and the validation using 596 CH4 vertical profiles from aircraft measurements by the HIAPER Pole-to-Pole Observations (HIPPO program over the Pacific Ocean. The number of degrees of freedom for the CH4 retrieval is mostly less than 1.5, and it decreases under cloudy conditions. The retrievals show greatest sensitivity between 100–600 hPa in the tropics and 200–750 hPa in the mid- to high latitude. Validation is accomplished using aircraft measurements (convolved by applying the monthly mean averaging kernels collocated with all the retrieved profiles within 200 km and on the same day, and the results show that, on average, a larger error of CH4 occurs at 300–500 hPa. The bias in the trapezoid of 374–477 hPa is −1.74% with a residual standard deviation of 1.20%, and at layer 596–753 hPa the bias is −0.69% with a residual standard deviation of 1.07%. The retrieval error is relatively larger in the high northern latitude regions and/or under cloudy conditions. The main reasons for this negative bias include the uncertainty in the spectroscopy near the methane Q branch and/or the empirical bias correction, plus residual cloud contamination in the cloud-cleared radiances. It is expected for NOAA to generate the CH4 product for 20 + years using a similar algorithm from three similar thermal infrared sensors: Atmospheric Infrared Sounder (AIRS, IASI and the Cross-track Infrared Sounder (CrIS. Such a unique product will provide a supplementary to the current ground-based observation network, particularly in the Arctic, for monitoring the CH4 cycle, its transport and trend associated with climate change.

  12. Transport of Formaldehyde to the Upper Troposphere In Deep Convective Storms During the 2012 DC3 Study

    Science.gov (United States)

    Fried, A.; Weibring, P.; Richter, D.; Walega, J.; Olson, J. R.; Crawford, J. H.; Barth, M. C.; Apel, E. C.; Hornbrook, R. S.; Bela, M. M.; Toon, O. B.; Blake, D. R.; Blake, N. J.; Luo, Z. J.

    2014-12-01

    The Deep Convective Clouds and Chemistry (DC3) campaign in the summer of 2012 provided an opportunity to study the impacts of deep convection on reactive and soluble precursors of ozone and HOx radicals, including CH2O, in the upper troposphere and lower stratosphere (UTLS) over North America. Formaldehyde measurements were acquired in the inflow and outflow of numerous storms on the NASA DC-8 and NSF/NCAR GV-aircraft employing fast, sensitive, and accurate difference frequency generation infrared absorption spectrometers. Since our Fall 2013 AGU Meeting poster, we have developed an improved methodology based upon 3 independent approaches, to determine the amount of CH2O that is scavenged by deep convective storms. The first approach is based upon WRF-Chem model simulations, which provides greater confidence in the determination of CH2O scavenging efficiencies and allows the estimation of CH2O ice retention factors.The second approach is a modified mixing model employing 4 non-reactive passive tracers (n,i-butane, n,i-pentane) to estimate altitude-dependent lateral entrainment rates. This information is coupled with time-dependent measurements in the outflow of various storms, which when extrapolated to time zero in the storm core, results in estimates of CH2O scavenging efficiencies. This analysis includes estimates of photochemically produced CH2O in the storm core. A third approach is based upon CH2O/n-butane ratio comparisons in both the storm inflow and outflow. Results from various storms over Oklahoma, Colorado, and Alabama will be presented. However, the analysis will primarily focus on the May 29, 2012 supercell storm in Oklahoma. During this storm, the 4 passive tracers produced a very consistent lateral entrainment rate of 0.083 ± 0.008 km-1, a value that broadly agrees with entrainment rates determined previously from analyzing moist static energy profiles (Luo et al., Geophys. Res. Lett., 2010). For this storm, the 3-independent approaches give CH2O

  13. The Relative Importance of Random Error and Observation Frequency in Detecting Trends in Upper Tropospheric Water Vapor

    Science.gov (United States)

    Whiteman, David N.; Vermeesch, Kevin C.; Oman, Luke D.; Weatherhead, Elizabeth C.

    2011-01-01

    Recent published work assessed the amount of time to detect trends in atmospheric water vapor over the coming century. We address the same question and conclude that under the most optimistic scenarios and assuming perfect data (i.e., observations with no measurement uncertainty) the time to detect trends will be at least 12 years at approximately 200 hPa in the upper troposphere. Our times to detect trends are therefore shorter than those recently reported and this difference is affected by data sources used, method of processing the data, geographic location and pressure level in the atmosphere where the analyses were performed. We then consider the question of how instrumental uncertainty plays into the assessment of time to detect trends. We conclude that due to the high natural variability in atmospheric water vapor, the amount of time to detect trends in the upper troposphere is relatively insensitive to instrumental random uncertainty and that it is much more important to increase the frequency of measurement than to decrease the random error in the measurement. This is put in the context of international networks such as the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) and the Network for the Detection of Atmospheric Composition Change (NDACC) that are tasked with developing time series of climate quality water vapor data.

  14. Inertia gravity waves in the upper troposphere during the MaCWAVE winter campaign. Part I. Observations with collocated radars

    Energy Technology Data Exchange (ETDEWEB)

    Hoffmann, P.; Serafimovich, A.; Peters, D.; Latteck, R. [Leibniz-Inst. fuer Atmosphaerenphysik, Kuehlungsborn (Germany); Dalin, P. [Swedish Inst. of Space Physics, Kiruna (Sweden); Goldberg, R. [NASA/Goddard Space Flight Center, Greenbelt, MD (United States)

    2006-07-01

    During the MaCWAVE campaign, combined rocket, radiosonde and ground-based measurements have been performed at the Norwegian Andoeya rocket range (ARR) near Andenes and the Swedish rocket range (ESRANGE) near Kiruna in January 2003 to study gravity waves in the vicinity of the Scandinavian mountain ridge. The investigations presented here are mainly based on the evaluation of continuous radar measurements with the ALWIN VHP radar in the upper troposphere/ lower stratosphere at Andenes (69.3 N, 16.0 E) and the ESRAD VHP radar near Kiruna (67.9 N, 21.9 E). Both radars are separated by about 260 km. Based on wavelet transformations of both data sets, the strongest activity of inertia gravity waves in the upper troposphere has been detected during the first period from 24-26 January 2003 with dominant vertical wavelengths of about 4-5 km as well as with dominant observed periods of about 13-14 h for the altitude range between 5 and 8 km under the additional influence of mountain waves. The results show the appearance of dominating inertia gravity waves with characteristic horizontal wavelengths of {proportional_to}200 km moving in the opposite direction than the mean background wind. The results show the appearance of dominating inertia gravity waves with intrinsic periods in the order of {proportional_to}5 h and with horizontal wavelengths of 200 km, moving in the opposite direction than the mean background wind. From the derived downward energy propagation it is supposed, that these waves are likely generated by a jet streak in the upper troposphere. The parameters of the jet-induced gravity waves have been estimated at both sites separately. The identified gravity waves are coherent at both locations and show higher amplitudes on the east-side of the Scandinavian mountain ridge, as expected by the influence of mountains. (orig.)

  15. 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.

  16. Long-term changes in lower tropospheric baseline ozone concentrations: Comparing chemistry-climate models and observations at northern midlatitudes

    Science.gov (United States)

    Parrish, D. D.; Lamarque, J.-F.; Naik, V.; Horowitz, L.; Shindell, D. T.; Staehelin, J.; Derwent, R.; Cooper, O. R.; Tanimoto, H.; Volz-Thomas, A.; Gilge, S.; Scheel, H.-E.; Steinbacher, M.; Fröhlich, M.

    2014-05-01

    Two recent papers have quantified long-term ozone (O3) changes observed at northern midlatitude sites that are believed to represent baseline (here understood as representative of continental to hemispheric scales) conditions. Three chemistry-climate models (NCAR CAM-chem, GFDL-CM3, and GISS-E2-R) have calculated retrospective tropospheric O3 concentrations as part of the Atmospheric Chemistry and Climate Model Intercomparison Project and Coupled Model Intercomparison Project Phase 5 model intercomparisons. We present an approach for quantitative comparisons of model results with measurements for seasonally averaged O3 concentrations. There is considerable qualitative agreement between the measurements and the models, but there are also substantial and consistent quantitative disagreements. Most notably, models (1) overestimate absolute O3 mixing ratios, on average by 5 to 17 ppbv in the year 2000, (2) capture only 50% of O3 changes observed over the past five to six decades, and little of observed seasonal differences, and (3) capture 25 to 45% of the rate of change of the long-term changes. These disagreements are significant enough to indicate that only limited confidence can be placed on estimates of present-day radiative forcing of tropospheric O3 derived from modeled historic concentration changes and on predicted future O3 concentrations. Evidently our understanding of tropospheric O3, or the incorporation of chemistry and transport processes into current chemical climate models, is incomplete. Modeled O3 trends approximately parallel estimated trends in anthropogenic emissions of NOx, an important O3 precursor, while measured O3 changes increase more rapidly than these emission estimates.

  17. Modeling and observational constraints on the sulfur cycle in the marine troposphere: a focus on reactive halogens and multiphase chemistry

    Science.gov (United States)

    Chen, Q.; Breider, T.; Schmidt, J.; Sherwen, T.; Evans, M. J.; Xie, Z.; Quinn, P.; Bates, T. S.; Alexander, B.

    2017-12-01

    The radiative forcing from marine boundary layer clouds is still highly uncertain, which partly stems from our poor understanding of cloud condensation nuclei (CCN) formation. The oxidation of dimethyl sulfide (DMS) and subsequent chemical evolution of its products (e.g. DMSO) are key processes in CCN formation, but are generally very simplified in large-scale models. Recent research has pointed out the importance of reactive halogens (e.g. BrO and Cl) and multiphase chemistry in the tropospheric sulfur cycle. In this study, we implement a series of sulfur oxidation mechanisms into the GEOS-Chem global chemical transport model, involving both gas-phase and multiphase oxidation of DMS, DMSO, MSIA and MSA, to improve our understanding of the sulfur cycle in the marine troposphere. DMS observations from six locations around the globe and MSA/nssSO42- ratio observations from two ship cruises covering a wide range of latitudes and longitudes are used to assess the model. Preliminary results reveal the important role of BrO for DMS oxidation at high latitudes (up to 50% over Southern Ocean). Oxidation of DMS by Cl radicals is small in the model (within 10% in the marine troposphere), probably due to an underrepresentation of Cl sources. Multiphase chemistry (e.g. oxidation by OH and O3 in cloud droplets) is not important for DMS oxidation but is critical for DMSO oxidation and MSA production and removal. In our model, about half of the DMSO is oxidized in clouds, leading to the formation of MSIA, which is further oxidized to form MSA. Overall, with the addition of reactive halogens and multiphase chemistry, the model is able to better reproduce observations of seasonal variations of DMS and MSA/nssSO42- ratios.

  18. A large impact of tropical biomass burning on CO and CO{sub 2} in the upper troposphere

    Energy Technology Data Exchange (ETDEWEB)

    Hidekazu Matsueda; Shoichi Taguchi; Hisayuki Y; Inoue & Masao Ishii [Meteorological Research Institute, Tsukuba-shi (Japan). Geochemical Research Department

    2002-07-01

    A large interannual variation of biomass burning emissions from Southeast Asia is associated with the ENSO events. During 1997/98 and 1994 El Nino years, uncontrolled wildfires of tropical rainforests and peat lands in Indonesia were enlarged due to a long drought. Enhanced CO injection into the upper troposphere from the intense Indonesian fires was clearly observed in the 8-year measurements from a regular flask sampling over the western Pacific using a JAL airliner between Australia and Japan. This airliner observation also revealed that upper tropospheric CO{sub 2} cycle largely changed during the 1997 El Nio year due partly to the biomass burning emissions. Widespread pollution from the biomass burnings in Southeast Asia was simulated using a CO tracer driven by a 3D global chemical transport model. This simulation indicates that tropical deep convections connected to rapid advection by the subtropical jet play a significant role in dispersing biomass-burning emissions from Southeast Asia on a global scale.

  19. An upper tropospheric ‘ozone river’ from Africa to India during the 2008 Asian post-monsoon season

    Directory of Open Access Journals (Sweden)

    Flore Tocquer

    2015-03-01

    Full Text Available We have used ozone data from the Infrared Atmospheric Sounding Interferometer to follow an event of ozone-enriched air-masses in the upper troposphere from eastern Africa to northern India. The ozone transport (hereafter called ‘ozone river’ or O3R occurred during the Asian post-monsoon season in 2008 and was associated with Rossby wave propagation. The persistence of the O3R in a narrow channel was confirmed by MOZAIC airborne data over the northwestern Indian coast. The regions of origin of the O3R were identified by a transport analysis based on the Lagrangian model FLEXPART. The Lagrangian simulations combined with potential vorticity fields indicate that stratospheric intrusions are not likely to be the most important contributor to the observed O3 enhancements. A high-resolution Eulerian model, Meso-NH, with tagged tracers was used to discriminate between African biomass burning, lightnings and Indian anthropogenic pollution as potential sources of precursors for the O3R. Lightning NOx emissions, associated with convective clouds over Africa, were found to be the principal contributor to the ozone enhancement over the Indian Ocean taking advantage of a northeastward jet. This case study illustrates African lightning emissions as an important source for enhanced O3 in the upper troposphere over the Indian Ocean region during the post-monsoon season.

  20. Regular in situ measurements of HDO/H216O in the northern and southern hemispherical upper troposphere reveal tropospheric transport processes.

    Science.gov (United States)

    Christner, Emanuel; Dyroff, Christoph; Sanati, Shahrokh; Brenninkmeijer, Carl; Zahn, Andreas

    2013-04-01

    influence of convection on the isotopic composition of water in the upper troposphere. This finding is consistent with the well-known regions of deep convection over Africa, Malaysia and South America.

  1. Sub-seasonal temperature variability in the tropical upper troposphere and lower stratosphere observed with GPS radio occultation

    Science.gov (United States)

    Scherllin-Pirscher, Barbara; Randel, William J.; Kim, Joowan

    2017-04-01

    We investigate sub-seasonal temperature variability in the tropical upper troposphere and lower stratosphere (UTLS) region using daily gridded fields of GPS radio occultation measurements. The unprecedented vertical resolution (from about 100 m in the troposphere to about 1.5 km in the stratosphere) and high accuracy and precision (0.7 K to 1 K between 8 km and 25 km) make these data ideal for characterizing temperature oscillations with short vertical wavelengths. Long-term behavior of sub-seasonal temperature variability is investigated using the entire RO record from January 2002 to December 2014 (13 years of data). Transient sub-seasonal waves including eastward-propagating Kelvin waves (isolated with space-time spectral analysis) dominate large-scale zonal temperature variability in the tropical tropopause region and in the lower stratosphere. Above 20 km, Kelvin waves are strongly modulated by the quasi-biennial oscillation (QBO). Enhanced wave activity can be found during the westerly shear phase of the QBO. In the tropical tropopause region, however, sub-seasonal waves are highly transient in time. Several peaks of Kelvin-wave activity coincide with short-term fluctuations in tropospheric deep convection, but other episodes are not evidently related. Also, there are no obvious relationships with zonal winds or stability fields near the tropical tropopause. Further investigations of convective forcing and atmospheric background conditions along the waves' trajectories are needed to better understand sub-seasonal temperature variability near the tropopause. For more details, see Scherllin-Pirscher, B., Randel, W. J., and Kim, J.: Tropical temperature variability and Kelvin-wave activity in the UTLS from GPS RO measurements, Atmos. Chem. Phys., 17, 793-806, doi:10.5194/acp-17-793-2017, 2017. http://www.atmos-chem-phys.net/17/793/2017/acp-17-793-2017.html

  2. A simple climatology of westerly jet streams in global reanalysis datasets part 1: mid-latitude upper tropospheric jets

    Science.gov (United States)

    Rikus, Lawrie

    2018-04-01

    A simple closed contour object identification scheme has been applied to the zonal mean monthly mean zonal wind fields from nine global reanalysis data sets for 31 years of the satellite era (1979-2009) to identify objects corresponding to westerly jet streams. The results cluster naturally into six individual jet streams but only the mid-latitude upper-tropospheric jets are considered here. The time series of the jet properties from all reanalyses are decomposed into seasonal means and anomalies, and correlations between variables are evaluated, with the aim of identifying robust features which can form the basis of evaluation metrics for climate model simulations of the twentieth century. There is substantial agreement between all the reanalyses for all jet properties although there are some systematic differences with particular data sets. Some of the results from the object identification applied to the reanalyses are used in a simple example of a model evaluation score for the zonal mean jet seasonal cycle.

  3. A modelling study of the impact of cirrus clouds on the moisture budget of the upper troposphere

    Directory of Open Access Journals (Sweden)

    S. Fueglistaler

    2006-01-01

    Full Text Available We present a modelling study of the effect of cirrus clouds on the moisture budget of the layer wherein the cloud formed. Our framework simplifies many aspects of cloud microphysics and collapses the problem of sedimentation onto a 0-dimensional box model, but retains essential feedbacks between saturation mixing ratio, particle growth, and water removal through particle sedimentation. The water budget is described by two coupled first-order differential equations for dimensionless particle number density and saturation point temperature, where the parameters defining the system (layer depth, reference temperature, amplitude and time scale of temperature perturbation and inital particle number density, which may or may not be a function of reference temperature and cooling rate are encapsulated in a single coefficient. This allows us to scale the results to a broad range of atmospheric conditions, and to test sensitivities. Results of the moisture budget calculations are presented for a range of atmospheric conditions (T: 238–205 K; p: 325–180 hPa and a range of time scales τT of the temperature perturbation that induces the cloud formation. The cirrus clouds are found to efficiently remove water for τT longer than a few hours, with longer perturbations (τT≳10 h required at lower temperatures (T≲210 K. Conversely, we find that temperature perturbations of duration order 1 h and less (a typical timescale for e.g., gravity waves do not efficiently dehydrate over most of the upper troposphere. A consequence is that (for particle densities typical of current cirrus clouds the assumption of complete dehydration to the saturation mixing ratio may yield valid predictions for upper tropospheric moisture distributions if it is based on the large scale temperature field, but this assumption is not necessarily valid if it is based on smaller scale temperature fields.

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

    Science.gov (United States)

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

    2018-03-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-11-01

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

  6. Large-scale upper tropospheric pollution observed by MIPAS HCN and C2H6 global distributions

    Science.gov (United States)

    Glatthor, N.; von Clarmann, T.; Stiller, G. P.; Funke, B.; Koukouli, M. E.; Fischer, H.; Grabowski, U.; Höpfner, M.; Kellmann, S.; Linden, A.

    2009-12-01

    We present global upper tropospheric HCN and C2H6 amounts derived from MIPAS/ENVISAT limb emission spectra. HCN and C2H6 are retrieved in the spectral regions 715.5-782.7 cm-1 and 811.5-835.7 cm-1, respectively. The datasets consist of 54 days between September 2003 and March 2004. This period covers the peak and decline of the southern hemispheric biomass burning period and some months thereafter. HCN is a nearly unambiguous tracer of biomass burning with an assumed tropospheric lifetime of several months. Indeed, the most significant feature in the MIPAS HCN dataset is an upper tropospheric plume of enhanced values caused by southern hemispheric biomass burning, which in September and October 2003 extended from tropical South America over Africa, Australia to the Southern Pacific. The spatial extent of this plume agrees well with the MOPITT CO distribution of September 2003. Further there is good agreement with the shapes and mixing ratios of the southern hemispheric HCN and C2H6 fields measured by the ACE experiment between September and November 2005. The MIPAS HCN plume extended from the lowermost observation height of 8 km up to about 16 km altitude, with maximum values of 500-600 pptv in October 2003. It was still clearly visible in December 2003, but had strongly decreased by March 2004, confirming the assumed tropospheric lifetime. The main sources of C2H6 are production and transmission of fossil fuels, followed by biofuel use and biomass burning. The C2H6 distribution also clearly reflected the southern hemispheric biomass burning plume and its seasonal variation, with maximum amounts of 600-700 pptv. Generally there was good spatial overlap between the southern hemispheric distributions of both pollution tracers, except for the region between Peru and the mid-Pacific. Here C2H6was considerably enhanced, whereas the HCN amounts were low. Backward trajectory calculations suggested that industrial pollution was responsible for the elevated C2H6

  7. Large-scale upper tropospheric pollution observed by MIPAS HCN and C2H6 global distributions

    Directory of Open Access Journals (Sweden)

    A. Linden

    2009-12-01

    Full Text Available We present global upper tropospheric HCN and C2H6 amounts derived from MIPAS/ENVISAT limb emission spectra. HCN and C2H6 are retrieved in the spectral regions 715.5–782.7 cm−1 and 811.5–835.7 cm−1, respectively. The datasets consist of 54 days between September 2003 and March 2004. This period covers the peak and decline of the southern hemispheric biomass burning period and some months thereafter. HCN is a nearly unambiguous tracer of biomass burning with an assumed tropospheric lifetime of several months. Indeed, the most significant feature in the MIPAS HCN dataset is an upper tropospheric plume of enhanced values caused by southern hemispheric biomass burning, which in September and October 2003 extended from tropical South America over Africa, Australia to the Southern Pacific. The spatial extent of this plume agrees well with the MOPITT CO distribution of September 2003. Further there is good agreement with the shapes and mixing ratios of the southern hemispheric HCN and C2H6 fields measured by the ACE experiment between September and November 2005. The MIPAS HCN plume extended from the lowermost observation height of 8 km up to about 16 km altitude, with maximum values of 500–600 pptv in October 2003. It was still clearly visible in December 2003, but had strongly decreased by March 2004, confirming the assumed tropospheric lifetime. The main sources of C2H6 are production and transmission of fossil fuels, followed by biofuel use and biomass burning. The C2H6 distribution also clearly reflected the southern hemispheric biomass burning plume and its seasonal variation, with maximum amounts of 600–700 pptv. Generally there was good spatial overlap between the southern hemispheric distributions of both pollution tracers, except for the region between Peru and the mid-Pacific. Here C2H6was considerably enhanced, whereas the HCN amounts were low. Backward trajectory calculations suggested that industrial pollution was responsible

  8. Assessment of upper tropospheric and stratospheric water vapor and ozone in reanalyses as part of S-RIP

    Science.gov (United States)

    Davis, Sean M.; Hegglin, Michaela I.; Fujiwara, Masatomo; Dragani, Rossana; Harada, Yayoi; Kobayashi, Chiaki; Long, Craig; Manney, Gloria L.; Nash, Eric R.; Potter, Gerald L.; Tegtmeier, Susann; Wang, Tao; Wargan, Krzysztof; Wright, Jonathon S.

    2017-10-01

    Reanalysis data sets are widely used to understand atmospheric processes and past variability, and are often used to stand in as "observations" for comparisons with climate model output. Because of the central role of water vapor (WV) and ozone (O3) in climate change, it is important to understand how accurately and consistently these species are represented in existing global reanalyses. In this paper, we present the results of WV and O3 intercomparisons that have been performed as part of the SPARC (Stratosphere-troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The comparisons cover a range of timescales and evaluate both inter-reanalysis and observation-reanalysis differences. We also provide a systematic documentation of the treatment of WV and O3 in current reanalyses to aid future research and guide the interpretation of differences amongst reanalysis fields.The assimilation of total column ozone (TCO) observations in newer reanalyses results in realistic representations of TCO in reanalyses except when data coverage is lacking, such as during polar night. The vertical distribution of ozone is also relatively well represented in the stratosphere in reanalyses, particularly given the relatively weak constraints on ozone vertical structure provided by most assimilated observations and the simplistic representations of ozone photochemical processes in most of the reanalysis forecast models. However, significant biases in the vertical distribution of ozone are found in the upper troposphere and lower stratosphere in all reanalyses.In contrast to O3, reanalysis estimates of stratospheric WV are not directly constrained by assimilated data. Observations of atmospheric humidity are typically used only in the troposphere, below a specified vertical level at or near the tropopause. The fidelity of reanalysis stratospheric WV products is therefore mainly dependent on the reanalyses' representation of the physical drivers that

  9. Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

    Directory of Open Access Journals (Sweden)

    D. M. Lienhard

    2015-12-01

    secondary organic aerosol (SOA material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA, levoglucosan, levoglucosan/NH4HSO4, raffinose are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous ice nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.

  10. A new cavity ring-down instrument for airborne monitoring of N2O5, NO3, NO2 and O3 in the upper troposphere lower stratosphere

    Science.gov (United States)

    Ruth, Albert A.; Brown, Steven S.; Dinesan, Hemanth; Dubé, William P.; Goulette, Marc; Hübler, Gerhard; Orphal, Johannes; Zahn, Andreas

    2016-04-01

    The chemistry of NO3 and N2O5 is important to the regulation of both tropospheric and stratospheric ozone. In situ detection of NO3 and N2O5 in the upper troposphere lower stratosphere (UTLS) represents a new scientific direction as the only previous measurements of these species in this region of the atmosphere has been via remote sensing techniques. Because both the sources and the sinks for NO3 and N2O5 are potentially stratified spatially, their mixing ratios, and their influence on nitrogen oxide and ozone transport and loss at night can show large variability as a function of altitude. Aircraft-based measurements of heterogeneous N2O5 uptake in the lower troposphere have uncovered a surprising degree of variability in the uptake coefficient [1], but there are no corresponding high altitude measurements.The UTLS is routinely sampled by the IAGOS-CARIBIC program (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container, www.caribic-atmospheric.com), a European infrastructural program with the aim of studying the chemistry and transport across this part of the atmosphere. An airfreight container with 15 different automated instruments from 8 European research partners is utilized on board a commercial Lufthansa airbus 340-600 to monitor ~ 100 atmospheric species (trace gases and aerosol parameters) in the UTLS. The instrumentation in the CARIBIC container is now to be supplemented by a new cavity ring-down device for monitoring nitrogen oxides, jointly developed by researchers from Cork (Ireland), Boulder (USA) and Karlsruhe (Germany). The compact and light-weight instrument is designed to monitor not only NO3 and N2O5, but also NO2 and O3. The detection is based on 4 high-finesse optical cavities (cavity length ~ 44 cm). Two cavities are operated at 662 nm (maximum absorption of NO3), the other two at 405 nm (maximum absorption of NO2). The inlet to one of the (662)-cavities is heated in order to thermally decompose N2O5

  11. The influence of tropospheric static stability on upper-level frontogenesis

    OpenAIRE

    Saute, Marcel

    2011-01-01

    Upper-level frontogenesis in an inviscid, dry and adiabatic fluid forced by confluence is investigated by means of a two-dimensional semi-geostrophic model using the specific volume as an isentropic vertical coordinate. The initial conditions are specified given an analytical continuous potential vorticity field in the presence of a temperature contrast at the ground, the lower boundary condition requiring an appropriate treatment because the ground intersects the first levels of the model. T...

  12. Quantifying the influence of boreal biomass burning emissions on tropospheric oxidant chemistry over the North Atlantic using BORTAS measurements

    Science.gov (United States)

    Parrington, Mark; Palmer, Paul I.; Rickard, Andrew; Young, Jennifer; Lewis, Ally; Lee, James; Henze, Daven; Tarasick, David; Hyer, Edward; Yantosca, Robert; Bowman, Kevin; Worden, John; Griffin, Debora; Franklin, Jonathan; Helmig, Detlev

    2013-04-01

    We use the GEOS-Chem chemistry transport model to quantify the impact of boreal biomass burning on tropospheric oxidant chemistry over the North Atlantic region during summer of 2011. The GEOS-Chem model is used at a spatial resolution of 1/2 degree latitude by 2/3 degree longitude for a domain covering eastern North America, the North Atlantic Ocean and western Europe. We initialise the model with biomass burning emissions from the Fire Locating and Monitoring of Burning Emissions (FLAMBE) inventory and use a modified chemical mechanism providing a detailed description of ozone photochemistry in boreal biomass burning outflow derived from the Master Chemical Mechanism (MCM). We evaluate the 3-D model distribution of ozone and tracers associated with biomass burning against measurements made by the UK FAAM BAe-146 research aircraft, ozonesondes, ground-based and satellite instruments as part of the BORTAS experiment between 12 July and 3 August 2011. We also use the GEOS-Chem model adjoint to fit the model to BORTAS measurements to analyse the sensitivity of the model chemical mechanism and ozone distribution to wildfire emissions in central Canada.

  13. Overview and sample applications of SMILES and Odin-SMR retrievals of upper tropospheric humidity and cloud ice mass

    Directory of Open Access Journals (Sweden)

    P. Eriksson

    2014-12-01

    Full Text Available Retrievals of cloud ice mass and humidity from the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES and the Odin-SMR (Sub-Millimetre Radiometer limb sounder are presented and example applications of the data are given. SMILES data give an unprecedented view of the diurnal variation of cloud ice mass. Mean regional diurnal cycles are reported and compared to some global climate models. Some improvements in the models regarding diurnal timing and relative amplitude were noted, but the models' mean ice mass around 250 hPa is still low compared to the observations. The influence of the ENSO (El Niño–Southern Oscillation state on the upper troposphere is demonstrated using 12 years of Odin-SMR data. The same retrieval scheme is applied for both sensors, and gives low systematic differences between the two data sets. A special feature of this Bayesian retrieval scheme, of Monte Carlo integration type, is that values are produced for all measurements but for some atmospheric states retrieved values only reflect a priori assumptions. However, this "all-weather" capability allows a direct statistical comparison to model data, in contrast to many other satellite data sets. Another strength of the retrievals is the detailed treatment of "beam filling" that otherwise would cause large systematic biases for these passive cloud ice mass retrievals. The main retrieval inputs are spectra around 635/525 GHz from tangent altitudes below 8/9 km for SMILES/Odin-SMR, respectively. For both sensors, the data cover the upper troposphere between 30° S and 30° N. Humidity is reported as both relative humidity and volume mixing ratio. The vertical coverage of SMILES is restricted to a single layer, while Odin-SMR gives some profiling capability between 300 and 150 hPa. Ice mass is given as the partial ice water path above 260 hPa, but for Odin-SMR ice water content, estimates are also provided. Besides a smaller contrast between most dry and wet

  14. Effects of regional-scale and convective transports on tropospheric ozone chemistry revealed by aircraft observations during the wet season of the AMMA campaign

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    G. Ancellet

    2009-01-01

    Full Text Available The African Monsoon Multidisciplinary Analyses (AMMA fourth airborne campaign was conducted in July–August 2006 to study the chemical composition of the middle and upper troposphere in West Africa with the major objective to better understand the processing of chemical emissions by the West African Monsoon (WAM and its associated regional-scale and vertical transports. In particular, the french airborne experiment was organized around two goals. The first was to characterize the impact of Mesoscale Convective Systems (MCSs on the ozone budget in the upper troposphere and the evolution of the chemical composition of these convective plumes as they move westward toward the Atlantic Ocean. The second objective was to discriminate the impact of remote sources of pollution over West Africa, including transport from the middle east, Europe, Asia and from southern hemispheric fires. Observations of O3, CO, NOx, H2O and hydroperoxide above West Africa along repeated meridional transects were coupled with transport analysis based on the FLEXPART lagrangian model. The cross analysis of trace gas concentrations and transport pathways revealed 5 types of air masses: convective uplift of industrial and urban emissions, convective uplift of biogenic emissions, slow advection from Cotonou polluted plumes near the coast, meridional transport of upper tropospheric air from the subtropical barrier region, and meridional transport of Southern Hemisphere (SH biomass burning emissions. O3/CO correlation plots and the correlation plots of H2O2 with a OH proxy revealed not only a control of the trace gas variability by transport processes but also significant photochemical reactivity in the mid- and upper troposphere. The study of four MCSs outflow showed contrasted chemical composition and air mass origins depending on the MCSs lifetime and latitudinal position. Favorables conditions for ozone

  15. The Composition and Chemistry of the Deep Tropospheres of Saturn and Uranus from Ground-Based Radio Observations

    Science.gov (United States)

    Hofstadter, M. D.; Adumitroaie, V.; Atreya, S. K.; Butler, B.

    2017-12-01

    Ground-based radio observations of the giant planets at wavelengths from 1 millimeter to 1 meter have long been the primary means to study the deep tropospheres of both gas- and ice-giant planets (e.g. de Pater and Massie 1985, Icarus 62; Hofstadter and Butler 2003, Icarus 165). Most recently, radiometers aboard the Cassini and Juno spacecraft at Saturn and Jupiter, respectively, have demonstrated the ability of spaceborne systems to study composition and weather beneath the visible cloud tops with high spatial resolution (Janssen et al. 2013, Icarus 226; Bolton et al. 2016, this meeting). Ground-based observations remain, however, an excellent way to study the tropospheres of the ice giants, particularly the temporal and spatial distribution of condensible species, and to study the deep troposphere of Saturn in the region of the water cloud. This presentation focuses on two ground-based data sets, one for Uranus and one for Saturn. The Uranus data were all collected near the 2007 equinox, and span wavelengths from 0.1 to 20 cm. These data provide a snapshot of atmospheric composition at a single season. The Saturn observations were recently made with the EVLA observatory at wavelengths from 3 to 90 cm, augmented by published observations at shorter and longer wavelengths. It is expected that these data will allow us to constrain conditions in the water cloud region on Saturn. At the time of this writing, both data sets are being analyzed using an optimal estimation retrieval algorithm fed with the latest published information on the chemical and electrical properties of relevant atmospheric species (primarily H2O, NH3, H2S, PH3, and free electrons). At Uranus, we find that—consistent with previously published work—ammonia in the 1 to 50-bar range is strongly depleted from solar values. The relative volume mixing ratios of the above species satisfy PH3 < NH3 < H2S < H2O, which is interesting because based on cosmic abundances one would expect H2S < NH3. At the

  16. Impact of enhanced ozone deposition and halogen chemistry on tropospheric ozone over the Northern Hemisphere

    Science.gov (United States)

    Fate of ozone in marine environments has been receiving increased attention due to the tightening of ambient air quality standards. The role of deposition and halogen chemistry is examined through incorporation of an enhanced ozone deposition algorithm and inclusion of halogen ch...

  17. An Aircraft-Based Upper Troposphere Lower Stratosphere O3, CO, and H2O Climatology for the Northern Hemisphere

    Science.gov (United States)

    Tilmes, S.; Pan, L. L.; Hoor, P.; Atlas, E.; Avery, M. A.; Campos, T.; Christensen, L. E.; Diskin, G. S.; Gao, R.-S.; Herman, R. L.; hide

    2010-01-01

    We present a climatology of O3, CO, and H2O for the upper troposphere and lower stratosphere (UTLS), based on a large collection of high ]resolution research aircraft data taken between 1995 and 2008. To group aircraft observations with sparse horizontal coverage, the UTLS is divided into three regimes: the tropics, subtropics, and the polar region. These regimes are defined using a set of simple criteria based on tropopause height and multiple tropopause conditions. Tropopause ]referenced tracer profiles and tracer ]tracer correlations show distinct characteristics for each regime, which reflect the underlying transport processes. The UTLS climatology derived here shows many features of earlier climatologies. In addition, mixed air masses in the subtropics, identified by O3 ]CO correlations, show two characteristic modes in the tracer ]tracer space that are a result of mixed air masses in layers above and below the tropopause (TP). A thin layer of mixed air (1.2 km around the tropopause) is identified for all regions and seasons, where tracer gradients across the TP are largest. The most pronounced influence of mixing between the tropical transition layer and the subtropics was found in spring and summer in the region above 380 K potential temperature. The vertical extent of mixed air masses between UT and LS reaches up to 5 km above the TP. The tracer correlations and distributions in the UTLS derived here can serve as a reference for model and satellite data evaluation

  18. Ozone sonde cell current measurements and implications for observations of near-zero ozone concentrations in the tropical upper troposphere

    Directory of Open Access Journals (Sweden)

    H. Vömel

    2010-04-01

    Full Text Available Laboratory measurements of the Electrochemical Concentration Cell (ECC ozone sonde cell current using ozone free air as well as defined amounts of ozone reveal that background current measurements during sonde preparation are neither constant as a function of time, nor constant as a function of ozone concentration. Using a background current, measured at a defined timed after exposure to high ozone may often overestimate the real background, leading to artificially low ozone concentrations in the upper tropical troposphere, and may frequently lead to operator dependent uncertainties. Based on these laboratory measurements an improved cell current to partial pressure conversion is proposed, which removes operator dependent variability in the background reading and possible artifacts in this measurement. Data from the Central Equatorial Pacific Experiment (CEPEX have been reprocessed using the improved background treatment based on these laboratory measurements. In the reprocessed data set near-zero ozone events no longer occur. At Samoa, Fiji, Tahiti, and San Cristóbal, nearly all near-zero ozone concentrations occur in soundings with larger background currents. To a large extent, these events are no longer observed in the reprocessed data set using the improved background treatment.

  19. A Laser-Induced Fluorescence Instrument for Aircraft Measurements of Sulfur Dioxide in the Upper Troposphere and Lower Stratosphere

    Science.gov (United States)

    Rollins, Andrew W.; Thornberry, Troy D.; Ciciora, Steven J.; McLaughlin, Richard J.; Watts, Laurel A.; Hanisco, Thomas F.; Baumann, Esther; Giorgetta, Fabrizio R.; Bui, Thaopaul V.; Fahey, David W.

    2016-01-01

    This work describes the development and testing of a new instrument for in situ measurements of sulfur dioxide (SO2) on airborne platforms in the upper troposphere and lower stratosphere (UTLS). The instrument is based on the laser-induced fluorescence technique and uses the fifth harmonic of a tunable fiber-amplified semiconductor diode laser system at 1084.5 nm to excite SO2 at 216.9 nm. Sensitivity and background checks are achieved in flight by additions of SO2 calibration gas and zero air, respectively. Aircraft demonstration was performed during the NASA Volcano Plume Investigation Readiness and Gas-Phase and Aerosol Sulfur (VIRGAS) experiment, which was a series of flights using the NASA WB-57F during October 2015 based at Ellington Field and Harlingen, Texas. During these flights, the instrument successfully measured SO2 in the UTLS at background (non-volcanic) conditions with a precision of 2 ppt at 10 s and an overall uncertainty determined primarily by instrument drifts of +/- (16% + 0.9 ppt).

  20. Retrieval of water vapor vertical distributions in the upper troposphere and the lower stratosphere from SCIAMACHY limb measurements

    Directory of Open Access Journals (Sweden)

    A. Rozanov

    2011-05-01

    Full Text Available This study describes the retrieval of water vapor vertical distributions in the upper troposphere and lower stratosphere (UTLS altitude range from space-borne observations of the scattered solar light made in limb viewing geometry. First results using measurements from SCIAMACHY (Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY aboard ENVISAT (Environmental Satellite are presented here. In previous publications, the retrieval of water vapor vertical distributions has been achieved exploiting either the emitted radiance leaving the atmosphere or the transmitted solar radiation. In this study, the scattered solar radiation is used as a new source of information on the water vapor content in the UTLS region. A recently developed retrieval algorithm utilizes the differential absorption structure of the water vapor in 1353–1410 nm spectral range and yields the water vapor content in the 11–25 km altitude range. In this study, the retrieval algorithm is successfully applied to SCIAMACHY limb measurements and the resulting water vapor profiles are compared to in situ balloon-borne observations. The results from both satellite and balloon-borne instruments are found to agree typically within 10 %.

  1. Isocyanic acid in a global chemistry transport model: Tropospheric distribution, budget, and identification of regions with potential health impacts

    Science.gov (United States)

    Young, Paul. J.; Emmons, Louisa K.; Roberts, James M.; Lamarque, Jean-FrançOis; Wiedinmyer, Christine; Veres, Patrick; Vandenboer, Trevor C.

    2012-05-01

    This study uses a global chemical transport model to estimate the distribution of isocyanic acid (HNCO). HNCO is toxic, and concentrations exceeding 1 ppbv have been suggested to have negative health effects. Based on fire studies, HNCO emissions were scaled to those of hydrogen cyanide (30%), resulting in yearly total emissions of 1.5 Tg for 2008, from both anthropogenic and biomass burning sources. Loss processes included heterogeneous uptake (pH dependent), dry deposition (like formic acid), and reaction with the OH radical (k = 1 × 10-15 molecule-1 cm3 s-1). Annual mean surface HNCO concentrations were highest over parts of China (maximum of 470 pptv), but episodic fire emissions gave much higher levels, exceeding 4 ppbv in tropical Africa and the Amazon, and exceeding 10 ppbv in Southeast Asia and Siberia. This suggests that large biomass burning events could result in deleterious health effects for populations in these regions. For the tropospheric budget, using the model-calculated pH the HNCO lifetime was 37 days, with the split between dry deposition and heterogeneous loss being 95%:5%. Fixing the heterogeneous loss rate at pH = 7 meant that this process dominated, accounting for ˜70% of the total loss, giving a lifetime of 6 days, and resulting in upper tropospheric concentrations that were essentially zero. However, changing the pH does not notably impact the high concentrations found in biomass burning regions. More observational data is needed to evaluate the model, as well as a better representation of the likely underestimated biofuel emissions, which could mean more populations exposed to elevated HNCO concentrations.

  2. Nitric acid particles in cold thick ice clouds observed at global scale: Link with lightning, temperature, and upper tropospheric water vapor

    Science.gov (United States)

    Chepfer, H.; Minnis, P.; Dubuisson, P.; Chiriaco, M.; Sun-Mack, S.; RivièRe, E. D.

    2007-03-01

    Signatures of nitric acid particles (NAP) in cold thick ice clouds have been derived from satellite observations. Most NAP are detected in the tropics (9 to 20% of clouds with T < 202.5 K). Higher occurrences were found in the rare midlatitudes very cold clouds. NAP occurrence increases as cloud temperature decreases, and NAP are more numerous in January than July. Comparisons of NAP and lightning distributions show that lightning seems to be the main source of the NOx, which forms NAP in cold clouds over continents. Qualitative comparisons of NAP with upper tropospheric humidity distributions suggest that NAP may play a role in the dehydration of the upper troposphere when the tropopause is colder than 195 K.

  3. MIPAS measurements of upper tropospheric C2H6 and O3 during the southern hemispheric biomass burning season in 2003

    Directory of Open Access Journals (Sweden)

    T. Steck

    2007-11-01

    Full Text Available Under cloud free conditions, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS provides measurements of spectrally resolved limb radiances down to the upper troposphere. These are used to infer global distributions of mixing ratios of atmospheric constituents in the upper troposphere and the stratosphere. From 21 October to 12 November 2003, MIPAS observed enhanced amounts of upper tropospheric C2H6 (up to about 400 pptv and ozone (up to about 80 ppbv. The absolute values of C2H6, however, may be systematically low by about 30% due to uncertainties of the spectroscopic data used. By means of trajectory calculations, the enhancements observed in the southern hemisphere are, at least partly, attributed to a biomass burning plume, which covers wide parts of the Southern hemisphere, from South America, the Atlantic Ocean, Africa, the Indian Ocean to Australia. The chemical composition of the part of the plume-like pollution belt associated with South American fires, where rainforest burning is predominant appears different from the part of the plume associated with southern African savanna burning. In particular, African savanna fires lead to a larger ozone enhancement than equatorial American fires. In this analysis, MIPAS observations of high ozone were disregarded where low CFC-11 (below 245 pptv was observed, because this hints at a stratospheric component in the measured signal. Different type of vegetation burning (flaming versus smouldering combustion has been identified as a candidate explanation for the different plume compositions.

  4. Estimates of the changes in tropospheric chemistry which result from human activity and their dependence on NO(x) emissions and model resolution

    Science.gov (United States)

    Kanakidou, Maria; Crutzen, Paul J.; Zimmermann, Peter H.

    1994-01-01

    As a consequence of the non-linear behavior of the chemistry of the atmosphere and because of the short lifetime of nitrogen oxides (NO(x)), two-dimensional models do not give an adequate description of the production and destruction rates of NO(x) and their effects on the distributions of the concentration of ozone and hydroxyl radical. In this study, we use a three-dimensional model to evaluate the contribution of increasing NO(x) emissions from industrial activity and biomass burning to changes in the chemical composition of the troposphere. By comparing results obtained from longitudinally-uniform and longitudinally-varying emissions of NO(x), we demonstrate that the geographical representation of the NO(x) emissions is crucial in simulating tropospheric chemistry.

  5. Upper-Level Undergraduate Chemistry Students' Goals for Their Laboratory Coursework

    Science.gov (United States)

    DeKorver, Brittland K.; Towns, Marcy H.

    2016-01-01

    Efforts to reform undergraduate chemistry laboratory coursework typically focus on the curricula of introductory-level courses, while upper-level courses are bypassed. This study used video-stimulated recall to interview 17 junior- and senior- level chemistry majors after they carried out an experiment as part of a laboratory course. It is assumed…

  6. A framework for teaching scientific inquiry in upper secondary school chemistry

    NARCIS (Netherlands)

    van Rens, L.; Pilot, A.; van der Schee, J.A.

    2010-01-01

    A framework for teaching scientific inquiry in upper secondary chemistry education was constructed in a design research consisting of two research cycles. First, in a pilot study a hypothetical framework was enriched in collaboration with five chemistry teachers. Second, a main study in this

  7. Chemistry: content, context and choices : towards students' higher order problem solving in upper secondary school

    OpenAIRE

    Broman, Karolina

    2015-01-01

    Chemistry is often claimed to be difficult, irrelevant, and uninteresting to school students. Even students who enjoy doing science often have problems seeing themselves as being scientists. This thesis explores and challenges the negative perception of chemistry by investigating upper secondary students’ views on the subject. Based on students’ ideas for improving chemistry education to make the subject more interesting and meaningful, new learning approaches rooted in context-based learning...

  8. Transport pathways of CO in the African upper troposphere during the monsoon season: a study based upon the assimilation of spaceborne observations

    Directory of Open Access Journals (Sweden)

    B. Barret

    2008-06-01

    Full Text Available The transport pathways of carbon monoxide (CO in the African Upper Troposphere (UT during the West African Monsoon (WAM is investigated through the assimilation of CO observations by the Aura Microwave Limb Sounder (MLS in the MOCAGE Chemistry Transport Model (CTM. The assimilation setup, based on a 3-D First Guess at Assimilation Time (3-D-FGAT variational method is described. Comparisons between the assimilated CO fields and in situ airborne observations from the MOZAIC program between Europe and both Southern Africa and Southeast Asia show an overall good agreement around the lowermost pressure level sampled by MLS (~215 hPa. The 4-D assimilated fields averaged over the month of July 2006 have been used to determine the main dynamical processes responsible for the transport of CO in the African UT. The studied period corresponds to the second AMMA (African Monsoon Multidisciplinary Analyses aircraft campaign. At 220 hPa, the CO distribution is characterized by a latitudinal maximum around 5° N mostly driven by convective uplift of air masses impacted by biomass burning from Southern Africa, uplifted within the WAM region and vented predominantly southward by the upper branch of the winter hemisphere Hadley cell. Above 150 hPa, the African CO distribution is characterized by a broad maximum over northern Africa. This maximum is mostly controlled by the large scale UT circulation driven by the Asian Summer Monsoon (ASM and characterized by the Asian Monsoon Anticyclone (AMA centered at 30° N and the Tropical Easterly Jet (TEJ on the southern flank of the anticyclone. Asian pollution uplifted to the UT over large region of Southeast Asia is trapped within the AMA and transported by the anticyclonic circulation over Northeast Africa. South of the AMA, the TEJ is responsible for the tranport of CO-enriched air masses from India and Southeast Asia over Africa. Using the high time resolution provided by the 4-D assimilated fields, we give evidence

  9. Observations of HO{sub x}, NO{sub x}, NO{sub y}, and CO. NO{sub x} control of the photochemical production and removal of ozone in the upper troposphere

    Energy Technology Data Exchange (ETDEWEB)

    Wennberg, P O; Hanisco, T F; Lanzendorf, E L; Jaegle, L Y; Jacob, D J; Cohen, R C; Anderson, J G [Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry; [Dept. of Earth and Planetary Sciences; Fahey, D W; Gao, R S; Keim, E R [National Oceanic and Atmospheric Administration, Boulder, CO (United States). Aeronomy Lab.; others, and

    1998-12-31

    In-situ measurements from the NASA ER2 aircraft provide the first observations of the odd-hydrogen radicals in the upper troposphere. A new photochemical model was constructed to explain the observations. Based on the model, the way of NO{sub x} influence on the photochemistry of ozone was determined. The measurements also explain why high NO{sub x}/NO{sub y} ratios are sustained in the upper troposphere. (R.P.)

  10. Observations of HO{sub x}, NO{sub x}, NO{sub y}, and CO. NO{sub x} control of the photochemical production and removal of ozone in the upper troposphere

    Energy Technology Data Exchange (ETDEWEB)

    Wennberg, P.O.; Hanisco, T.F.; Lanzendorf, E.L.; Jaegle, L.Y.; Jacob, D.J.; Cohen, R.C.; Anderson, J.G. [Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry]|[Dept. of Earth and Planetary Sciences; Fahey, D.W.; Gao, R.S.; Keim, E.R. [National Oceanic and Atmospheric Administration, Boulder, CO (United States). Aeronomy Lab.; and others

    1997-12-31

    In-situ measurements from the NASA ER2 aircraft provide the first observations of the odd-hydrogen radicals in the upper troposphere. A new photochemical model was constructed to explain the observations. Based on the model, the way of NO{sub x} influence on the photochemistry of ozone was determined. The measurements also explain why high NO{sub x}/NO{sub y} ratios are sustained in the upper troposphere. (R.P.)

  11. The effects of deep convection on the concentration and size distribution of aerosol particles within the upper troposphere: A case study

    Science.gov (United States)

    Yin, Yan; Chen, Qian; Jin, Lianji; Chen, Baojun; Zhu, Shichao; Zhang, Xiaopei

    2012-11-01

    A cloud resolving model coupled with a spectral bin microphysical scheme was used to investigate the effects of deep convection on the concentration and size distribution of aerosol particles within the upper troposphere. A deep convective storm that occurred on 1 December, 2005 in Darwin, Australia was simulated, and was compared with available radar observations. The results showed that the radar echo of the storm in the developing stage was well reproduced by the model. Sensitivity tests for aerosol layers at different altitudes were conducted in order to understand how the concentration and size distribution of aerosol particles within the upper troposphere can be influenced by the vertical transport of aerosols as a result of deep convection. The results indicated that aerosols originating from the boundary layer can be more efficiently transported upward, as compared to those from the mid-troposphere, due to significantly increased vertical velocity through the reinforced homogeneous freezing of droplets. Precipitation increased when aerosol layers were lofted at different altitudes, except for the case where an aerosol layer appeared at 5.4-8.0 km, in which relatively more efficient heterogeneous ice nucleation and subsequent Wegener-Bergeron-Findeisen process resulted in more pronounced production of ice crystals, and prohibited the formation of graupel particles via accretion. Sensitivity tests revealed, at least for the cases considered, that the concentration of aerosol particles within the upper troposphere increased by a factor of 7.71, 5.36, and 5.16, respectively, when enhanced aerosol layers existed at 0-2.2 km, 2.2-5.4 km, and 5.4-8.0 km, with Aitken mode and a portion of accumulation mode (0.1-0.2μm) particles being the most susceptible to upward transport.

  12. ATom observations of new particle formation in the tropical upper troposphere. The role of convection and nucleation mechanisms

    Science.gov (United States)

    Kupc, A.; Williamson, C.; Hodshire, A. L.; Pierce, J. R.; Ray, E. A.; Froyd, K. D.; Richardson, M.; Weinzierl, B.; Dollner, M.; Erdesz, F.; Bui, T. V.; Diskin, G. S.; Brock, C. A.

    2017-12-01

    Measurements of size distributions during the Atmospheric Tomography Mission (ATom) reveal high number concentrations (>>1000 cm-3) of nucleation mode particles at high altitudes in the tropics and subtropics under low condensation sink conditions and are associated with upwelling in convective clouds. The broad spatial extent of these newly formed particles shows that the upper free troposphere (FT) of the tropics and subtropics is a globally significant source. In this study, we investigate the link between convection and new particle formation (NPF) by exploring the processes that govern NPF and growth in the tropical and subtropical FT of the Pacific and Atlantic Oceans. We use measurements of the size distributions made with a suite of fast-response instruments on board of a NASA DC-8 aircraft during ATom mission. ATom maps the remote atmosphere over the Pacific and Atlantic basins ( 80 °N and 65 °S) in continuous ascents and descents (0.2 and 13 km), providing the latitudinal and vertical information on the greenhouse gases, reactive and tracer species and aerosol properties and their seasonal variability. We couple measurements of size distributions between 0.003 and 4.8 µm and potential aerosol precursor vapors measured on ATom (August 2016 and February 2017) with calculated air mass back trajectories and the TwO-Moment Aerosol Sectional (TOMAS) box model. The back trajectories identify air masses potentially influenced by recent convection. We then use TOMAS to model particle nucleation, condensation and coagulation along that trajectory to investigate the link between convection and NPF. Through TOMAS, we explore the influence of different nucleation mechanisms (such as binary, ternary or the one with organics) and gas-phase aerosol precursors (such as sulfur dioxide) on observed particle size distributions. We discuss similarities and differences in NPF over the Pacific and Atlantic Oceans and their relationship to convection, examine particle

  13. Laboratory studies on tropospheric iodine chemistry: bridging the atomic, molecular and particle scale

    Science.gov (United States)

    Gomez Martin, J.; Saunders, R. W.; Blitz, M. A.; Mahajan, A. S.; Plane, J. M.

    2008-12-01

    High mixing ratios of the iodine oxides IO and OIO have been observed in the polar, mid-latitude and tropical marine boundary layer (MBL). The impact of the iodine chemistry on the oxidizing capacity of the MBL is well documented. Moreover, there is evidence showing that the bursts of new particles measured in coastal regions are produced by the biogenic emission of iodine containing precursors, followed by the photochemical production and condensation of iodine oxide vapours. Airborne measurements of particle growth rates show that these particles can reach significant sizes where they can contribute to the regional aerosol loading, thus suggesting a potential impact on climate on a regional or global scale. Within the frame of the INSPECT project (INorganic Secondary Particle Evolution, Chemistry and Transport) we wish to understand at a fundamental level the tendency for the iodine oxides formed from IO and OIO recombination to condense into particles. Elemental analysis of iodine oxide particles (IOP) made in the laboratory shows that they have the empirical formula I2O5. The major question is how this happens: through formation of I2O5 in the gas phase, followed by polymerization, or by condensation of various IxOy to form amorphous iodine oxides, which subsequently rearrange to I2O5. We are studying the gas phase photochemistry leading to nucleation of IOP, their growth kinetics, aspects of their heterogeneous chemistry, and their properties as ice condensation nuclei. In order to bridge the molecular and the particle scales, a wide variety of techniques are being used, including CRDS, ARAS, LIF, UV-VIS spectroscopy, PI-TOF-MS and mobility particle size scanning. The results obtained so far provide new and interesting insights to the problem. From the gas phase point of view, a unit iodine atom quantum yield from OIO photolysis has been now established across its strong visible spectral bands. This result implies a short lifetime of OIO and explains why in

  14. Observations of fine-scale transport structure in the upper troposphere from the High-performance Instrumented Airborne Platform for Environmental Research

    Science.gov (United States)

    Bowman, Kenneth P.; Pan, Laura L.; Campos, Teresa; Gao, Rushan

    2007-09-01

    The Progressive Science Mission in December 2005 was the first research use of the new NCAR High-performance Instrumented Airborne Platform for Environmental Research (HIAPER) aircraft. The Stratosphere-Troposphere Analyses of Regional Transport (START) component of the mission was designed to investigate the dynamical and chemical structure of the upper troposphere and lower stratosphere. Flight 5 of the Progressive Science mission was a START flight that sampled near the tropopause in an area between the main jet stream and a large, quasi-stationary, cutoff low. The large-scale flow in this region was characterized by a hyperbolic (saddle) point. In this study the in situ measurements by HIAPER are combined with flow analyses and satellite data to investigate the quasi-isentropic stirring of trace species in the upper troposphere. As expected from theoretical considerations, strong stretching and folding deformation of the flow near the hyperbolic point resulted in rapid filamentation of air masses and sharp gradients of constituents. Calculations of the stirring using operational meteorological analyses from the NCEP Global Forecast System model produced excellent agreement with HIAPER and satellite observations of trace species. Back trajectories indicate that elevated ozone levels in some filaments likely came from a large stratospheric intrusion that occurred upstream in the jet over the north Pacific Ocean. The methods presented here can be used with operational forecasts for future flight planning.

  15. Impact of West African Monsoon convective transport and lightning NOx production upon the upper tropospheric composition: a multi-model study

    Directory of Open Access Journals (Sweden)

    H. Schlager

    2010-06-01

    Full Text Available Within the African Monsoon Multidisciplinary Analysis (AMMA, we investigate the impact of nitrogen oxides produced by lightning (LiNOx and convective transport during the West African Monsoon (WAM upon the composition of the upper troposphere (UT in the tropics. For this purpose, we have performed simulations with 4 state-of-the-art chemistry transport models involved within AMMA, namely MOCAGE, TM4, LMDz-INCA and p-TOMCAT. The model intercomparison is complemented with an evaluation of the simulations based on both spaceborne and airborne observations. The baseline simulations show important differences between the UT CO and O3 distributions simulated by each of the 4 models when compared to measurements from the MOZAIC program and fom the Aura/MLS spaceborne sensor. We show that such model discrepancies can be explained by differences in the convective transport parameterizations and, more particularly, the altitude reached by convective updrafts (ranging between ~200–125 hPa. Concerning UT O3, the models exhibit a good agreement with the main observed features. Nevertheless the majority of models simulate low O3 concentrations compared to both MOZAIC and Aura/MLS observations south of the equator, and rather high concentrations in the Northern Hemisphere. Sensitivity studies are performed to quantify the effect of deep convective transport and the influence of LiNOx production on the UT composition. These clearly indicate that the CO maxima and the elevated O3 concentrations south of the equator are due to convective uplift of air masses impacted by Southern African biomass burning, in agreement with previous studies. Moreover, during the WAM, LiNOx from Africa are responsible for the highest UT O3 enhancements (10–20 ppbv over the tropical Atlantic between 10° S–20° N. Differences between models are primarily due to the performance of the parameterizations used to simulate lightning activity which are evaluated using spaceborne

  16. Inertia gravity waves in the upper troposphere during the MaCWAVE winter campaign – Part I: Observations with collocated radars

    Directory of Open Access Journals (Sweden)

    P. Hoffmann

    2006-11-01

    Full Text Available During the {MaCWAVE} campaign, combined rocket, radiosonde and ground-based measurements have been performed at the Norwegian Andøya Rocket Range (ARR near Andenes and the Swedish Rocket Range (ESRANGE near Kiruna in January 2003 to study gravity waves in the vicinity of the Scandinavian mountain ridge. The investigations presented here are mainly based on the evaluation of continuous radar measurements with the ALWIN VHF radar in the upper troposphere/ lower stratosphere at Andenes (69.3° N, 16.0° E and the ESRAD VHF radar near Kiruna (67.9° N, 21.9° E. Both radars are separated by about 260 km. Based on wavelet transformations of both data sets, the strongest activity of inertia gravity waves in the upper troposphere has been detected during the first period from 24–26 January 2003 with dominant vertical wavelengths of about 4–5 km as well as with dominant observed periods of about 13–14 h for the altitude range between 5 and 8 km under the additional influence of mountain waves. The results show the appearance of dominating inertia gravity waves with characteristic horizontal wavelengths of ~200 km moving in the opposite direction than the mean background wind. The results show the appearance of dominating inertia gravity waves with intrinsic periods in the order of ~5 h and with horizontal wavelengths of 200 km, moving in the opposite direction than the mean background wind. From the derived downward energy propagation it is supposed, that these waves are likely generated by a jet streak in the upper troposphere. The parameters of the jet-induced gravity waves have been estimated at both sites separately. The identified gravity waves are coherent at both locations and show higher amplitudes on the east-side of the Scandinavian mountain ridge, as expected by the influence of mountains.

  17. Correction Technique for Raman Water Vapor Lidar Signal-Dependent Bias and Suitability for Water Wapor Trend Monitoring in the Upper Troposphere

    Science.gov (United States)

    Whiteman, D. N.; Cadirola, M.; Venable, D.; Calhoun, M.; Miloshevich, L; Vermeesch, K.; Twigg, L.; Dirisu, A.; Hurst, D.; Hall, E.; hide

    2012-01-01

    The MOHAVE-2009 campaign brought together diverse instrumentation for measuring atmospheric water vapor. We report on the participation of the ALVICE (Atmospheric Laboratory for Validation, Interagency Collaboration and Education) mobile laboratory in the MOHAVE-2009 campaign. In appendices we also report on the performance of the corrected Vaisala RS92 radiosonde measurements during the campaign, on a new radiosonde based calibration algorithm that reduces the influence of atmospheric variability on the derived calibration constant, and on other results of the ALVICE deployment. The MOHAVE-2009 campaign permitted the Raman lidar systems participating to discover and address measurement biases in the upper troposphere and lower stratosphere. The ALVICE lidar system was found to possess a wet bias which was attributed to fluorescence of insect material that was deposited on the telescope early in the mission. Other sources of wet biases are discussed and data from other Raman lidar systems are investigated, revealing that wet biases in upper tropospheric (UT) and lower stratospheric (LS) water vapor measurements appear to be quite common in Raman lidar systems. Lower stratospheric climatology of water vapor is investigated both as a means to check for the existence of these wet biases in Raman lidar data and as a source of correction for the bias. A correction technique is derived and applied to the ALVICE lidar water vapor profiles. Good agreement is found between corrected ALVICE lidar measurments and those of RS92, frost point hygrometer and total column water. The correction is offered as a general method to both quality control Raman water vapor lidar data and to correct those data that have signal-dependent bias. The influence of the correction is shown to be small at regions in the upper troposphere where recent work indicates detection of trends in atmospheric water vapor may be most robust. The correction shown here holds promise for permitting useful upper

  18. Inertia gravity waves in the upper troposphere during the MaCWAVE winter campaign. Part II. Radar investigations and modelling studies

    Energy Technology Data Exchange (ETDEWEB)

    Serafimovich, A.; Zuelicke, C.; Hoffmann, P.; Peters, D.; Singer, W. [Leibniz-Inst. fuer Atmosphaerenphysik, Kuehlungsborn (Germany); Dalin, P. [Swedish Inst. of Space Physics, Kiruna (Sweden)

    2006-07-01

    We present an experimental and modelling study of a strong gravity wave event in the upper troposphere/lower stratosphere near the Scandinavian mountain ridge. Continuous VHP radar measurements during the MaCWAVE rocket and ground-based measurement campaign were performed at the Norwegian Andoya rocket range (ARR) near Andenes (69.3 N, 16 E) in January 2003. Detailed gravity wave investigations based on PSU/NCAR fifth-generation mesoscale model (MM5) data have been used for comparison with experimentally obtained results. The model data show the presence of a mountain wave and of an inertia gravity wave generated by a jet streak near the tropopause region. Temporal and spatial dependencies of jet induced inertia gravity waves with dominant observed periods of about 13 h and vertical wavelengths of {proportional_to}4.5-5 km are investigated with wavelet transform applied on radar measurements and model data. The jet induced wave packet is observed to move upstream and downward in the upper troposphere. The model data agree with the experimentally obtained results fairly well. Possible reasons for the observed differences, e.g. in the time of maximum of the wave activity, are discussed. Finally, the vertical fluxes of horizontal momentum are estimated with different methods and provide similar amplitudes. We found indications that the derived positive vertical flux of the horizontal momentum corresponds to the obtained parameters of the jet-induced inertia gravity wave, but only at the periods and heights of the strongest wave activity. (orig.)

  19. Redox Models in Chemistry Textbooks for the Upper Secondary School: Friend or Foe?

    Science.gov (United States)

    Osterlund, Lise-Lotte; Berg, Anders; Ekborg, Margareta

    2010-01-01

    We have investigated how chemistry textbooks use models of redox reactions in different subject areas, how they change models between and within the topics, and how they deal with specific learning difficulties identified in the literature. The textbooks examined were published for use in the natural science programme in Swedish upper secondary…

  20. Reactive Nitrogen, Ozone and Ozone Production in the Arctic Troposphere and the Impact of Stratosphere-Troposphere Exchange

    Science.gov (United States)

    Liang, Q.; Rodriquez, J. M.; Douglass, A. R.; Crawford, J. H.; Apel, E.; Bian, H.; Blake, D. R.; Brune, W.; Chin, M.; Colarco, P. R.; hide

    2011-01-01

    and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

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

    Directory of Open Access Journals (Sweden)

    D. Wang

    2013-07-01

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

  2. Potential impact of carbonaceous aerosol on the upper troposphere and lower stratosphere (UTLS) and precipitation during Asian summer monsoon in a global model simulation

    KAUST Repository

    Fadnavis, Suvarna

    2017-09-28

    Recent satellite observations show efficient vertical transport of Asian pollutants from the surface to the upper-level anticyclone by deep monsoon convection. In this paper, we examine the transport of carbonaceous aerosols, including black carbon (BC) and organic carbon (OC), into the monsoon anticyclone using of ECHAM6-HAM, a global aerosol climate model. Further, we investigate impacts of enhanced (doubled) carbonaceous aerosol emissions on the upper troposphere and lower stratosphere (UTLS), underneath monsoon circulation and precipitation from sensitivity simulations. The model simulation shows that boundary layer aerosols are transported into the monsoon anticyclone by the strong monsoon convection from the Bay of Bengal, southern slopes of the Himalayas and the South China Sea. Doubling of emissions of both BC and OC aerosols over Southeast Asia (10° S–50° N, 65–155° E) shows that lofted aerosols produce significant warming (0.6–1 K) over the Tibetan Plateau (TP) near 400–200 hPa and instability in the middle/upper troposphere. These aerosols enhance radiative heating rates (0.02–0.03 K day−1) near the tropopause. The enhanced carbonaceous aerosols alter aerosol radiative forcing (RF) at the surface by −4.74 ± 1.42 W m−2, at the top of the atmosphere (TOA) by +0.37 ± 0.26 W m−2 and in the atmosphere by +5.11 ± 0.83 W m−2 over the TP and Indo-Gangetic Plain region (15–35° N, 80–110° E). Atmospheric warming increases vertical velocities and thereby cloud ice in the upper troposphere. Aerosol induced anomalous warming over the TP facilitates the relative strengthening of the monsoon Hadley circulation and increases moisture inflow by strengthening the cross-equatorial monsoon jet. This increases precipitation amounts over India (1–4 mm day−1) and eastern China (0.2–2 mm day−1). These results are significant at the 99 % confidence level.

  3. Continental outflow from the US to the upper troposphere over the North Atlantic during the NASA INTEX-NA Airborne Campaign

    Directory of Open Access Journals (Sweden)

    S. Y. Kim

    2008-04-01

    Full Text Available A case of continental outflow from the United States (US was examined using airborne measurements from NASA DC-8 flight 13 during the Intercontinental Chemical Transport Experiment – North America (INTEX-NA. Mixing ratios of methane (CH4 and carbon monoxide (CO at 8–11 km altitude over the North Atlantic were elevated to 1843 ppbv and 134 ppbv respectively, while those of carbon dioxide (CO2 and carbonyl sulfide (COS were reduced to 372.4 ppmv and 411 pptv respectively. In this region, urban and industrial influences were evidenced by elevated mixing ratios and good linear relationships between urban and industrial tracers compared to North Atlantic background air. Moreover, low mixing ratios and a good correlation between COS and CO2 showed a fingerprint of terrestrial uptake and minimal dilution during rapid transport over a 1–2 day time period. Analysis of synoptic conditions, backward trajectories, and photochemical aging estimates based on C3H8/C2H6 strongly suggested that elevated anthropogenic tracers in the upper troposphere of the flight region were the result of transport via convection and warm conveyor belt (WCB uplifting of boundary layer air over the southeastern US. This mechanism is supported by the similar slope values of linear correlations between long-lived (months anthropogenic tracers (e.g., C2Cl4 and CHCl3 from the flight region and the planetary boundary layer in the southeastern US. In addition, the aircraft measurements suggest that outflow from the US augmented the entire tropospheric column at mid-latitudes over the North Atlantic. Overall, the flight 13 data demonstrate a pervasive impact of US anthropogenic emissions on the troposphere over the North Atlantic.

  4. First airborne water vapor lidar measurements in the tropical upper troposphere and mid-latitudes lower stratosphere: accuracy evaluation and intercomparisons with other instruments

    Directory of Open Access Journals (Sweden)

    C. Schiller

    2008-09-01

    Full Text Available In the tropics, deep convection is the major source of uncertainty in water vapor transport to the upper troposphere and into the stratosphere. Although accurate measurements in this region would be of first order importance to better understand the processes that govern stratospheric water vapor concentrations and trends in the context of a changing climate, they are sparse because of instrumental shortcomings and observational challenges. Therefore, the Falcon research aircraft of the Deutsches Zentrum für Luft- und Raumfahrt (DLR flew a zenith-viewing water vapor differential absorption lidar (DIAL during the Tropical Convection, Cirrus and Nitrogen Oxides Experiment (TROCCINOX in 2004 and 2005 in Brazil. The measurements were performed alternatively on three water vapor absorption lines of different strength around 940 nm. These are the first aircraft DIAL measurements in the tropical upper troposphere and in the mid-latitudes lower stratosphere. Sensitivity analyses reveal an accuracy of 5% between altitudes of 8 and 16 km. This is confirmed by intercomparisons with the Fast In-situ Stratospheric Hygrometer (FISH and the Fluorescent Advanced Stratospheric Hygrometer (FLASH onboard the Russian M-55 Geophysica research aircraft during five coordinated flights. The average relative differences between FISH and DIAL amount to −3%±8% and between FLASH and DIAL to −8%±14%, negative meaning DIAL is more humid. The average distance between the probed air masses was 129 km. The DIAL is found to have no altitude- or latitude-dependent bias. A comparison with the balloon ascent of a laser absorption spectrometer gives an average difference of 0%±19% at a distance of 75 km. Six tropical DIAL under-flights of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS on board ENVISAT reveal a mean difference of −8%±49% at an average distance of 315 km. While the comparison with MIPAS is somewhat less significant due to poorer

  5. How well can global chemistry models calculate the reactivity of short-lived greenhouse gases in the remote troposphere, knowing the chemical composition

    Directory of Open Access Journals (Sweden)

    M. J. Prather

    2018-05-01

    Full Text Available We develop a new protocol for merging in situ measurements with 3-D model simulations of atmospheric chemistry with the goal of integrating these data to identify the most reactive air parcels in terms of tropospheric production and loss of the greenhouse gases ozone and methane. Presupposing that we can accurately measure atmospheric composition, we examine whether models constrained by such measurements agree on the chemical budgets for ozone and methane. In applying our technique to a synthetic data stream of 14 880 parcels along 180° W, we are able to isolate the performance of the photochemical modules operating within their global chemistry-climate and chemistry-transport models, removing the effects of modules controlling tracer transport, emissions, and scavenging. Differences in reactivity across models are driven only by the chemical mechanism and the diurnal cycle of photolysis rates, which are driven in turn by temperature, water vapor, solar zenith angle, clouds, and possibly aerosols and overhead ozone, which are calculated in each model. We evaluate six global models and identify their differences and similarities in simulating the chemistry through a range of innovative diagnostics. All models agree that the more highly reactive parcels dominate the chemistry (e.g., the hottest 10 % of parcels control 25–30 % of the total reactivities, but do not fully agree on which parcels comprise the top 10 %. Distinct differences in specific features occur, including the spatial regions of maximum ozone production and methane loss, as well as in the relationship between photolysis and these reactivities. Unique, possibly aberrant, features are identified for each model, providing a benchmark for photochemical module development. Among the six models tested here, three are almost indistinguishable based on the inherent variability caused by clouds, and thus we identify four, effectively distinct, chemical models. Based on this

  6. How well can global chemistry models calculate the reactivity of short-lived greenhouse gases in the remote troposphere, knowing the chemical composition

    Science.gov (United States)

    Prather, Michael J.; Flynn, Clare M.; Zhu, Xin; Steenrod, Stephen D.; Strode, Sarah A.; Fiore, Arlene M.; Correa, Gustavo; Murray, Lee T.; Lamarque, Jean-Francois

    2018-05-01

    We develop a new protocol for merging in situ measurements with 3-D model simulations of atmospheric chemistry with the goal of integrating these data to identify the most reactive air parcels in terms of tropospheric production and loss of the greenhouse gases ozone and methane. Presupposing that we can accurately measure atmospheric composition, we examine whether models constrained by such measurements agree on the chemical budgets for ozone and methane. In applying our technique to a synthetic data stream of 14 880 parcels along 180° W, we are able to isolate the performance of the photochemical modules operating within their global chemistry-climate and chemistry-transport models, removing the effects of modules controlling tracer transport, emissions, and scavenging. Differences in reactivity across models are driven only by the chemical mechanism and the diurnal cycle of photolysis rates, which are driven in turn by temperature, water vapor, solar zenith angle, clouds, and possibly aerosols and overhead ozone, which are calculated in each model. We evaluate six global models and identify their differences and similarities in simulating the chemistry through a range of innovative diagnostics. All models agree that the more highly reactive parcels dominate the chemistry (e.g., the hottest 10 % of parcels control 25-30 % of the total reactivities), but do not fully agree on which parcels comprise the top 10 %. Distinct differences in specific features occur, including the spatial regions of maximum ozone production and methane loss, as well as in the relationship between photolysis and these reactivities. Unique, possibly aberrant, features are identified for each model, providing a benchmark for photochemical module development. Among the six models tested here, three are almost indistinguishable based on the inherent variability caused by clouds, and thus we identify four, effectively distinct, chemical models. Based on this work, we suggest that water vapor

  7. Tropospheric chemistry of natural hydrocarbons, aldehydes, and peroxy radicals: Their connections to sulfuric acid production and climate effects

    International Nuclear Information System (INIS)

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

    1993-05-01

    Recent work has shown that natural hydrocarbon emissions can significantly affect the levels of urban and regional tropospheric ozone. We report on the reactivities of these biogenic trace gases, particularly isoprene, focusing on their importance in the production of aldehydes and peroxy radicals, leading to increased levels of hydrogen over regional forests. Hydrogen peroxide can lead to the wet oxidation of sulfur dioxide to acidic sulfate in aerosols, fogs, and clouds. In turn, acidic sulfate can act to as a light scattering aerosol and a source of cloud condensation nuclei (CCN), potentially leading to global cooling. Aerosol sulfate and other dissolved organic and inorganic compounds can also play important roles as a greenhouse species in the lower troposphere

  8. Potential impact of carbonaceous aerosol on the upper troposphere and lower stratosphere (UTLS) and precipitation during Asian summer monsoon in a global model simulation

    KAUST Repository

    Fadnavis, Suvarna; Kalita, Gayatry; Kumar, K. Ravi; Gasparini, Blaž; Li, Jui-Lin Frank

    2017-01-01

    The model simulation shows that boundary layer aerosols are transported into the monsoon anticyclone by the strong monsoon convection from the Bay of Bengal, southern slopes of the Himalayas and the South China Sea. Doubling of emissions of both BC and OC aerosols over Southeast Asia (10° S–50° N, 65–155° E) shows that lofted aerosols produce significant warming (0.6–1 K) over the Tibetan Plateau (TP) near 400–200 hPa and instability in the middle/upper troposphere. These aerosols enhance radiative heating rates (0.02–0.03 K day−1) near the tropopause. The enhanced carbonaceous aerosols alter aerosol radiative forcing (RF) at the surface by −4.74 ± 1.42 W m−2, at the top of the atmosphere (TOA) by +0.37 ± 0.26 W m−2 and in the atmosphere by +5.11 ± 0.83 W m−2 over the TP and Indo-Gangetic Plain region (15–35° N, 80–110° E). Atmospheric warming increases vertical velocities and thereby cloud ice in the upper troposphere. Aerosol induced anomalous warming over the TP facilitates the relative strengthening of the monsoon Hadley circulation and increases moisture inflow by strengthening the cross-equatorial monsoon jet. This increases precipitation amounts over India (1–4 mm day−1) and eastern China (0.2–2 mm day−1). These results are significant at the 99 % confidence level.

  9. NASA Goddard Earth Sciences Graduate Student Program. [FIRE CIRRUS-II examination of coupling between an upper tropospheric cloud system and synoptic-scale dynamics

    Science.gov (United States)

    Ackerman, Thomas P.

    1994-01-01

    The evolution of synoptic-scale dynamics associated with a middle and upper tropospheric cloud event that occurred on 26 November 1991 is examined. The case under consideration occurred during the FIRE CIRRUS-II Intensive Field Observing Period held in Coffeyville, KS during Nov. and Dec., 1991. Using data from the wind profiler demonstration network and a temporally and spatially augmented radiosonde array, emphasis is given to explaining the evolution of the kinematically-derived ageostrophic vertical circulations and correlating the circulation with the forcing of an extensively sampled cloud field. This is facilitated by decomposing the horizontal divergence into its component parts through a natural coordinate representation of the flow. Ageostrophic vertical circulations are inferred and compared to the circulation forcing arising from geostrophic confluence and shearing deformation derived from the Sawyer-Eliassen Equation. It is found that a thermodynamically indirect vertical circulation existed in association with a jet streak exit region. The circulation was displaced to the cyclonic side of the jet axis due to the orientation of the jet exit between a deepening diffluent trough and building ridge. The cloud line formed in the ascending branch of the vertical circulation with the most concentrated cloud development occurring in conjunction with the maximum large-scale vertical motion. The relationship between the large scale dynamics and the parameterization of middle and upper tropospheric clouds in large-scale models is discussed and an example of ice water contents derived from a parameterization forced by the diagnosed vertical motions and observed water vapor contents is presented.

  10. Inertia gravity waves in the upper troposphere during the MaCWAVE winter campaign – Part II: Radar investigations and modelling studies

    Directory of Open Access Journals (Sweden)

    A. Serafimovich

    2006-11-01

    Full Text Available We present an experimental and modelling study of a strong gravity wave event in the upper troposphere/lower stratosphere near the Scandinavian mountain ridge. Continuous VHF radar measurements during the MaCWAVE rocket and ground-based measurement campaign were performed at the Norwegian Andoya Rocket Range (ARR near Andenes (69.3° N, 16° E in January 2003. Detailed gravity wave investigations based on PSU/NCAR Fifth-Generation Mesoscale Model (MM5 data have been used for comparison with experimentally obtained results. The model data show the presence of a mountain wave and of an inertia gravity wave generated by a jet streak near the tropopause region. Temporal and spatial dependencies of jet induced inertia gravity waves with dominant observed periods of about 13 h and vertical wavelengths of ~4.5–5 km are investigated with wavelet transform applied on radar measurements and model data. The jet induced wave packet is observed to move upstream and downward in the upper troposphere. The model data agree with the experimentally obtained results fairly well. Possible reasons for the observed differences, e.g. in the time of maximum of the wave activity, are discussed. Finally, the vertical fluxes of horizontal momentum are estimated with different methods and provide similar amplitudes. We found indications that the derived positive vertical flux of the horizontal momentum corresponds to the obtained parameters of the jet-induced inertia gravity wave, but only at the periods and heights of the strongest wave activity.

  11. Investigation of inertia-gravity waves in the upper troposphere/lower stratosphere over Northern Germany observed with collocated VHF/UHF radars

    Directory of Open Access Journals (Sweden)

    A. Serafimovich

    2005-01-01

    Full Text Available A case study to investigate the properties of inertia-gravity waves in the upper troposphere/lower stratosphere has been carried out over Northern Germany during the occurrence of an upper tropospheric jet in connection with a poleward Rossby wave breaking event from 17-19 December 1999. The investigations are based on the evaluation of continuous radar measurements with the OSWIN VHF radar at Kühlungsborn (54.1 N, 11.8 E and the 482 MHz UHF wind profiler at Lindenberg (52.2 N, 14.1 E. Both radars are separated by about 265 km. Based on wavelet transformations of both data sets, the dominant vertical wavelengths of about 2-4 km for fixed times as well as the dominant observed periods of about 11 h and weaker oscillations with periods of  6 h for the altitude range between 5 and 8 km are comparable. Gravity wave parameters have been estimated at both locations separately and by a complex cross-spectral analysis of the data of both radars. The results show the appearance of dominating inertia-gravity waves with characteristic horizontal wavelengths of  300 km moving in the opposite direction than the mean background wind and a secondary less pronounced wave with a horizontal wavelength in the order of about 200 km moving with the wind. Temporal and spatial differences of the observed waves are discussed.

  12. The governing processes and timescales of stratosphere-to-troposphere transport and its contribution to ozone in the Arctic troposphere

    Science.gov (United States)

    Liang, Q.; Douglass, A. R.; Duncan, B. N.; Stolarski, R. S.; Witte, J. C.

    2009-05-01

    We used the seasonality of a combination of atmospheric trace gases and idealized tracers to examine stratosphere-to-troposphere transport and its influence on tropospheric composition in the Arctic. Maximum stratosphere-to-troposphere transport of CFCs and O3 occurs in April as driven by the Brewer-Dobson circulation. Stratosphere-troposphere exchange (STE) occurs predominantly between 40° N to 80° N with stratospheric influx in the mid-latitudes (30-70° N) accounting for 67-81% of the air of stratospheric origin in the Northern Hemisphere extratropical troposphere. Transport from the lower stratosphere to the lower troposphere (LT) takes three months on average, one month to cross the tropopause, the second month to travel from the upper troposphere (UT) to the middle troposphere (MT), and the third month to reach the LT. During downward transport, the seasonality of a trace gas can be greatly impacted by wet removal and chemistry. A comparison of idealized tracers with varying lifetimes suggests that when initialized with the same concentrations and seasonal cycles at the tropopause, trace gases that have shorter lifetimes display lower concentrations, smaller amplitudes, and earlier seasonal maxima during transport to the LT. STE contributes to O3 in the Arctic troposphere directly from the transport of O3 and indirectly from the transport of NOy. Direct transport of O3 from the stratosphere accounts for 78% of O3 in the Arctic UT with maximum contributions occurring from March to May. The stratospheric contribution decreases significantly in the MT/LT (20-25% of total O3) and shows a very weak March-April maximum. Our NOx budget analysis in the Arctic UT shows that during spring and summer, the stratospheric injection of NOy-rich air increases NOx concentrations above the 20 pptv threshold level, thereby shifting the Arctic UT from a regime of net photochemical ozone loss to one of net production with rates as high as +16 ppbv/month.

  13. Tropospheric Ozone as a Short-lived Chemical Climate Forcer

    Science.gov (United States)

    Pickering, Kenneth E.

    2012-01-01

    Tropospheric ozone is the third most important greenhouse gas according to the most recent IPCC assessment. However, tropospheric ozone is highly variable in both space and time. Ozone that is located in the vicinity of the tropopause has the greatest effect on climate forcing. Nitrogen oxides (NOx) are the most important precursors for ozone In most of the troposphere. Therefore, pollution that is lofted upward in thunderstorm updrafts or NOx produced by lightning leads to efficient ozone production in the upper troposphere, where ozone is most important climatically. Global and regional model estimates of the impact of North American pollution and lightning on ozone radiative forcing will be presented. It will be shown that in the Northern Hemisphere summer, the lightning effect on ozone radiative forcing can dominate over that of pollution, and that the radiative forcing signal from North America extends well into Europe and North Africa. An algorithm for predicting lightning flash rates and estimating lightning NOx emissions is being incorporated into the NASA GEOS-5 Chemistry and Climate Model. Changes in flash rates and emissions over an ENSO cycle and in future climates will be assessed, along with the resulting changes in upper tropospheric ozone. Other research on the production of NOx per lightning flash and its distribution in the vertical based on cloud-resolving modeling and satellite observations will be presented. Distributions of NO2 and O3 over the Middle East from the OMI instrument on NASA's Aura satellite will also be shown.

  14. Mercury Plumes in the Global Upper Troposphere Observed during Flights with the CARIBIC Observatory from May 2005 until June 2013

    Directory of Open Access Journals (Sweden)

    Franz Slemr

    2014-05-01

    Full Text Available Tropospheric sections of flights with the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrumented Container observatory from May 2005 until June 2013, are investigated for the occurrence of plumes with elevated Hg concentrations. Additional information on CO, CO2, CH4, NOy, O3, hydrocarbons, halocarbons, acetone and acetonitrile enable us to attribute the plumes to biomass burning, urban/industrial sources or a mixture of both. Altogether, 98 pollution plumes with elevated Hg concentrations and CO mixing ratios were encountered, and the Hg/CO emission ratios for 49 of them could be calculated. Most of the plumes were found over East Asia, in the African equatorial region, over South America and over Pakistan and India. The plumes encountered over equatorial Africa and over South America originate predominantly from biomass burning, as evidenced by the low Hg/CO emission ratios and elevated mixing ratios of acetonitrile, CH3Cl and particle concentrations. The backward trajectories point to the regions around the Rift Valley and the Amazon Basin, with its outskirts, as the source areas. The plumes encountered over East Asia and over Pakistan and India are predominantly of urban/industrial origin, sometimes mixed with products of biomass/biofuel burning. Backward trajectories point mostly to source areas in China and northern India. The Hg/CO2 and Hg/CH4 emission ratios for several plumes are also presented and discussed.

  15. Methane from the Tropospheric Emission Spectrometer (TES)

    Science.gov (United States)

    Payne, Vivienne; Worden, John; Kulawik, Susan; Frankenberg, Christian; Bowman, Kevin; Wecht, Kevin

    2012-01-01

    TES V5 CH4 captures latitudinal gradients, regional variability and interannual variation in the free troposphere. V5 joint retrievals offer improved sensitivity to lower troposphere. Time series extends from 2004 to present. V5 reprocessing in progress. Upper tropospheric bias. Mitigated by N2O correction. Appears largely spatially uniform, so can be corrected. How to relate free-tropospheric values to surface emissions.

  16. 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

  17. 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.

  18. Numerical simulations on the effect of aerosols on tropospheric chemistry and range of sight; Numerische Simulationen zur Wirkung des Aerosols auf die troposphaerische Chemie und die Sichtweite

    Energy Technology Data Exchange (ETDEWEB)

    Riemer, N.

    2002-05-01

    In this study the mesoscale KAMM/DRAS model system was extended by an MADE aerosol module with a view to studying tropospheric aerosols in terms of composition and size distribution in the greatest possible detail. In particular, the MADE aerosol module was supplemented by a routine for soot. This routine involves the parameterisation of the ageing process of soot through coagulation of soot particles with soluble particles and condensation of sulphuric acid on the soot particles. This transforms the soot from an external into an internal mixture and changes its hygroscopic properties. Thus extended the model system was used to study two aspects of the effects of aerosols on the physical and chemical environment of the troposphere. The first of these two tasks was to quantify the influence of heterogeneous hydrolysis of dinitrogen pentoxide (N{sub 2}O{sub 5}) on tropospheric chemistry under summer smog conditions. The second was to study the optical properties of aerosols. The paper shows a way of deriving extinction coefficients from the calculated aerosol distributions. This is then used as a starting point for developing a method for determining range of sight. [German] Das mesoskalige Modellsystem KAMM/DRAIS wird im Rahmen dieser Arbeit um das Aerosolmodul MADE erweitert, um das troposphaerische Aerosol sowohl bezueglich seiner Zusammensetzung als auch bezueglich seiner Groessenverteilung moeglichst detailliert zu behandeln. Insbesondere wird das Aerosolmodul MADE um die Behandlung der Substanz Russ ergaenzt. Hierbei wird der Alterungsprozess von Russ durch Koagulation der Russteilchen mit loeslichen Partikeln und durch Kondensation von Schwefelsaeure auf den Russpartikeln, wodurch der Russ von einer externen in eine interne Mischung uebergeht und seine hygroskopischen Eigenschaften aendert, parametrisiert. Mit dem so erweiterten Modellsystem wird fuer zwei Themenschwerpunkte die Wirkung des Aerosols auf die physikalischen und chemischen Bedingungen in der

  19. Focal plane subsystem design and performance for atmospheric chemistry from geostationary orbit tropospheric emissions monitoring of pollution

    Science.gov (United States)

    Gilmore, A. S.; Philbrick, R. H.; Funderburg, J.

    2017-09-01

    Remote sensing of pollutants are enabled from a satellite in a geostationary orbit containing an imaging spectrometer encompassing the wavelength ranges of 290 - 490 nm and 540 - 740 nm. As the first of NASA's Earth Venture Instrument Program, the Tropospheric Emissions: Monitoring of Pollution (TEMPO) program will utilize this instrument to measure hourly air quality over a large portion of North America. The focal plane subsystem (FPS) contains two custom designed and critically aligned full frame transfer charge coupled devices (active area: 1028 x 2048, 18 μm) within a focal plane array package designed for radiation tolerance and space charging rejection. In addition, the FPS contains custom distributed focal plane electronics that provide all necessary clocks and biases to the sensors, receives all analog data from the sensors and performs 14 bit analog to digital conversion for upstream processing. Finally, the FPS encompasses custom low noise cables connecting the focal plane array and associated electronics. This paper discusses the design and performance of this novel focal plane subsystem with particular emphasis on the optical performance achieved including alignment, quantum efficiency, and modulation transfer function.

  20. Spatial Heterodyne Observations of Water (SHOW) vapour in the upper troposphere and lower stratosphere from a high altitude aircraft: Modelling and sensitivity analysis

    Science.gov (United States)

    Langille, J. A.; Letros, D.; Zawada, D.; Bourassa, A.; Degenstein, D.; Solheim, B.

    2018-04-01

    A spatial heterodyne spectrometer (SHS) has been developed to measure the vertical distribution of water vapour in the upper troposphere and the lower stratosphere with a high vertical resolution (∼500 m). The Spatial Heterodyne Observations of Water (SHOW) instrument combines an imaging system with a monolithic field-widened SHS to observe limb scattered sunlight in a vibrational band of water (1363 nm-1366 nm). The instrument has been optimized for observations from NASA's ER-2 aircraft as a proof-of-concept for a future low earth orbit satellite deployment. A robust model has been developed to simulate SHOW ER-2 limb measurements and retrievals. This paper presents the simulation of the SHOW ER-2 limb measurements along a hypothetical flight track and examines the sensitivity of the measurement and retrieval approach. Water vapour fields from an Environment and Climate Change Canada forecast model are used to represent realistic spatial variability along the flight path. High spectral resolution limb scattered radiances are simulated using the SASKTRAN radiative transfer model. It is shown that the SHOW instrument onboard the ER-2 is capable of resolving the water vapour variability in the UTLS from approximately 12 km - 18 km with ±1 ppm accuracy. Vertical resolutions between 500 m and 1 km are feasible. The along track sampling capability of the instrument is also discussed.

  1. EOF analysis of COSMIC observations on the global zonal mean temperature structure of the Upper Troposphere and Lower Stratosphere from 2007 to 2013

    Science.gov (United States)

    Salinas, Cornelius Csar Jude H.; Chang, Loren C.

    2018-06-01

    This work presents the results of a Conventional Empirical Orthogonal Function Analysis on daily global zonal mean temperature profiles in the Upper Troposphere and Lower Stratosphere (15-35 km), as measured by the FORMOSAT-3/COSMIC mission from January 2007 to June 2013. For validation, results were compared with ERA-Interim reanalysis. Results show that, the leading global EOF mode (27%) from COSMIC is consistent with temperature anomalies due to the tropical cooling associated with boreal winter Sudden Stratospheric Warmings (SSW). The second global EOF mode from COSMIC (15.3%) is consistent with temperature anomalies due to the Quasi-biennial Oscillation (QBO). The third global mode from COSMIC (10.9%) is consistent with temperature anomalies due to the El Nino Southern Oscillation. This work also shows that the second northern hemisphere EOF mode from COSMIC (16.8%) is consistent with temperature anomalies due Rossby-wave breaking (RWB) which is expected to only be resolved by a high vertical and temporal resolution dataset like COSMIC. Our work concludes that the use of a high vertical and temporal resolution dataset like COSMIC yields non-seasonal EOF modes that are consistent with relatively more intricate temperature anomalies due to the SSW, QBO, ENSO and RWB.

  2. Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities.

    Science.gov (United States)

    Van Wyngarden, A L; Pérez-Montaño, S; Bui, J V H; Li, E S W; Nelson, T E; Ha, K T; Leong, L; Iraci, L T

    Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40-80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H 2 SO 4 ) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance-Fourier transform infrared (ATR-FTIR) and 1 H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal

  3. Upper tropospheric ozone production from lightning NOx-impacted convection: Smoke ingestion case study from the DC3 campaign

    Science.gov (United States)

    Apel, E. C.; Hornbrook, R. S.; Hills, A. J.; Blake, N. J.; Barth, M. C.; Weinheimer, A.; Cantrell, C.; Rutledge, S. A.; Basarab, B.; Crawford, J.; Diskin, G.; Homeyer, C. R.; Campos, T.; Flocke, F.; Fried, A.; Blake, D. R.; Brune, W.; Pollack, I.; Peischl, J.; Ryerson, T.; Wennberg, P. O.; Crounse, J. D.; Wisthaler, A.; Mikoviny, T.; Huey, G.; Heikes, B.; O'Sullivan, D.; Riemer, D. D.

    2015-03-01

    As part of the Deep Convective Cloud and Chemistry (DC3) experiment, the National Science Foundation/National Center for Atmospheric Research (NCAR) Gulfstream-V (GV) and NASA DC-8 research aircraft probed the chemical composition of the inflow and outflow of two convective storms (north storm, NS, south storm, SS) originating in the Colorado region on 22 June 2012, a time when the High Park wildfire was active in the area. A wide range of trace species were measured on board both aircraft including biomass burning (BB) tracers hydrogen cyanide (HCN) and acetonitrile (ACN). Acrolein, a much shorter lived tracer for BB, was also quantified on the GV. The data demonstrated that the NS had ingested fresh smoke from the High Park fire and as a consequence had a higher VOC OH reactivity than the SS. The SS lofted aged fire tracers along with other boundary layer ozone precursors and was more impacted by lightning NOx (LNOx) than the NS. The NCAR master mechanism box model was initialized with measurements made in the outflow of the two storms. The NS and SS were predicted to produce 11 and 14 ppbv of O3, respectively, downwind of the storm over 2 days. Sensitivity tests revealed that the ozone production potential of the SS was highly dependent on LNOx. Normalized excess mixing ratios, ΔX/ΔCO, for HCN and ACN were determined in both the fire plume and the storm outflow and found to be 7.0 ± 0.5 and 2.3 ± 0.5 pptv ppbv-1, respectively, and 1.4 ± 0.3 pptv ppbv-1 for acrolein in the outflow only.

  4. Parameterization of the middle and upper tropospheric water vapor from ATOVS observations over a tropical climate region

    Science.gov (United States)

    Makama, Ezekiel Kaura; Lim, Hwee San; Abdullah, Khiruddin

    2018-01-01

    Precipitable water vapor (PWV) is a highly variable, but important greenhouse gas that regulates the radiation budget of the earth. Its variability in time and space makes it difficult to quantify. Knowledge of its vertical distribution, in particular, is crucial for many reasons. In this study, empirical relationships between isobaric layers of PWV over Peninsular Malaysia are examined. Analysis of variance (ANOVA) technique on Advanced Television and Infrared Observation Satellite Operational Vertical Sounder (ATOVS) observations, from 2005 to 2011, has been used to propose a relationship of the form, W=α(WL)β for the middle (MW) and upper (UW) layers PWV. W is either MW or UW with α and β as regression coefficients, which are functions of latitude. Coefficients of determination (R2) and root mean square error (RMSE) of respective values between 0.75-0.86 and 1.65-2.38 mm, across the zones, were obtained for both the MW and UW predictions, with a mean bias (MB) below ±1 mm.The predicted and observed PWV presented a better agreement northerly. Initial predictability test for each model was done on two independent data sets: ATOVS (2012-2015), and radiosonde (2010-2011) at Penang, Kuantan and Sepang stations, with very good outcomes. The results of the tests revealed remarkable performances, when compared with two previously reported models. The inclusion of variable regression coefficients, and the utilization of satellite-derived data, which provide soundings of data-void regions between radiosonde networks, proved to have optimized the results.

  5. Tropospheric jet response to Antarctic ozone depletion: An update with Chemistry-Climate Model Initiative (CCMI) models

    Science.gov (United States)

    Son, Seok-Woo; Han, Bo-Reum; Garfinkel, Chaim I.; Kim, Seo-Yeon; Park, Rokjin; Abraham, N. Luke; Akiyoshi, Hideharu; Archibald, Alexander T.; Butchart, N.; Chipperfield, Martyn P.; Dameris, Martin; Deushi, Makoto; Dhomse, Sandip S.; Hardiman, Steven C.; Jöckel, Patrick; Kinnison, Douglas; Michou, Martine; Morgenstern, Olaf; O’Connor, Fiona M.; Oman, Luke D.; Plummer, David A.; Pozzer, Andrea; Revell, Laura E.; Rozanov, Eugene; Stenke, Andrea; Stone, Kane; Tilmes, Simone; Yamashita, Yousuke; Zeng, Guang

    2018-05-01

    The Southern Hemisphere (SH) zonal-mean circulation change in response to Antarctic ozone depletion is re-visited by examining a set of the latest model simulations archived for the Chemistry-Climate Model Initiative (CCMI) project. All models reasonably well reproduce Antarctic ozone depletion in the late 20th century. The related SH-summer circulation changes, such as a poleward intensification of westerly jet and a poleward expansion of the Hadley cell, are also well captured. All experiments exhibit quantitatively the same multi-model mean trend, irrespective of whether the ocean is coupled or prescribed. Results are also quantitatively similar to those derived from the Coupled Model Intercomparison Project phase 5 (CMIP5) high-top model simulations in which the stratospheric ozone is mostly prescribed with monthly- and zonally-averaged values. These results suggest that the ozone-hole-induced SH-summer circulation changes are robust across the models irrespective of the specific chemistry-atmosphere-ocean coupling.

  6. A model study of ozone in the eastern Mediterranean free troposphere during MINOS (August 2001

    Directory of Open Access Journals (Sweden)

    G. J. Roelofs

    2003-01-01

    Full Text Available A coupled tropospheric chemistry-climate model is used to analyze tropospheric ozone distributions observed during the MINOS campaign in the eastern Mediterranean region (August, 2001. Modeled ozone profiles are generally in good agreement with the observations. Our analysis shows that the atmospheric dynamics in the region are strongly influenced by the occurrence of an upper tropospheric anti-cyclone, associated with the Asian summer monsoon and centered over the Tibetan Plateau. The anti-cyclone affects the chemical composition of the upper troposphere, where ozone concentrations of about 50 ppbv were measured, through advection of boundary layer air from South-East Asia. A layer between 4-6 km thickness was present beneath, containing up to 120 ppbv of ozone with substantial contributions by transport from the stratosphere and through lightning NOx. Additionally, pollutant ozone from North America was mixed in. Ozone in the lower troposphere originated mainly from the European continent. The stratospheric influence may be overestimated due to too strong vertical diffusion associated with the relatively coarse vertical resolution. The estimated tropospheric ozone column over the eastern Mediterranean is ~50 DU in summer, to which ozone from recent stratospheric origin contributes about 30%, ozone from lightning 13%, and from South-East Asia, North America and Europe about 7%, 8% and 14%, respectively, adding to a long-term hemispheric background of 25% of the column.

  7. Trace gas composition in the free and upper troposphere over Asia: Examining the influence of long-range transport and convection of local pollution

    Science.gov (United States)

    Baker, A. K.; Traud, S.; Brenninkmeijer, C. A.; Hoor, P. M.; Neumaier, M.; Oram, D.; Rauthe-Schöch, A.; Schloegl, S.; Sprung, D.; Slemr, F.; van Velthoven, P.; Wernli, H.; Zahn, A.; Ziereis, H.

    2013-12-01

    Between May 2005 and March 2008 the CARIBIC observatory (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) was deployed to make atmospheric observations during 21 round-trip flights between Frankfurt, Germany and Manila, the Philippines with a stopover in Guangzhou, China. This nearly 3 year flight series provides us with information about atmospheric composition in the free and upper troposphere over Asia during all seasons and was used to investigate seasonal and regional differences in trace gas distributions and the relative influences of long range transport and convected local air masses on composition. The flight route was separated into three different regions having unique characteristics in transport and composition; these were Western Asia (5°E to 70°E), Central Asia (70°E to 100°E) and East Asia (100°E to 125°E). The region over Western Asia was heavily influenced by long range transport of air masses from North America and had elevated levels of NOy and acetone, while the region over East Asia was mostly influenced by convected local (South East Asian) pollution, particularly from biomass/biofuel burning as indicated by high levels of acetonitrile and carbon monoxide. Air masses over Central Asia were found to be influenced by both recently convected air masses from the Indian subcontinent and mid-range transport from Eastern Europe and the Middle East. Elevated levels of propane and other non-methane hydrocarbons, both with and without concommitant elevations in other trace gases (i.e. carbon monoxide, acetonitrile) were a persisent feature of this region in all seasons except summer, and were particularly prominent in fall. Influences on composition over Central Asia were investigated more thoroughly in a case study from a series of flights in October 2006, and elevated levels of pollutants were found to be the result of convective transport of both biomass/biofuel burning and urban emissions from

  8. Airborne differential absorption lidar for water vapour measurements in the upper troposphere and lower stratosphere in the spectral region around 940 nm

    Energy Technology Data Exchange (ETDEWEB)

    Poberaj, G.

    2000-07-01

    Two all-solid-state laser systems were developed and studied in detail to optimise their performance for an airborne water vapour differential absorption lidar (DIAL). Their special features are high average output powers and excellent spectral properties in the 940-nm spectral region relevant for monitoring very low water vapour contents in the upper troposphere and lower stratosphere. One system is an injection-seeded pulsed Ti:sapphire ring laser with a spectral bandwidth of 105 MHz and an average power of 1.1 W. The other system is an injection-seeded optical parametric oscillator (OPO) in a ring configuration. Using KTP as nonlinear crystal, a signal output with a spectral bandwidth of 140 MHz and an average power of 1.2 W was achieved. Both systems, the Ti:sapphire ring laser and the KTP OPO, possess spectral purity values higher than 99%. The pump source for these systems is a frequency doubled diode-pumped Nd:YAG laser operating at a repetition rate of 100 Hz. The KTP OPO system has been used as a transmitter in a new airborne water vapour DIAL instrument. For the first time, measurements of two-dimensional water vapour distributions with a high vertical (500 m) and horizontal (20 km) resolution across several potential vorticity streamers were performed. Very low water vapour mixing ratios (10-50 ppmv) and strong gradients were observed in the tropopause region. The sensitivity of the DIAL instrument in the centre of a stratospheric intrusion ranges from 3% in the near field to 12% in the far field (4 km). The first comparison experiments with in situ measuring instruments show a good agreement. Considerable differences are found between DIAL measurements and data obtained from the ECMWF operational analyses and a mesoscale numerical model. (orig.)

  9. Methyl chloride in the upper troposphere observed by the CARIBIC passenger aircraft observatory: Large-scale distributions and Asian summer monsoon outflow

    Science.gov (United States)

    Umezawa, T.; Baker, A. K.; Oram, D.; Sauvage, C.; O'Sullivan, D.; Rauthe-Schöch, A.; Montzka, S. A.; Zahn, A.; Brenninkmeijer, C. A. M.

    2014-05-01

    We present spatial and temporal variations of methyl chloride (CH3Cl) in the upper troposphere (UT) observed mainly by the Civil Aircraft for Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) passenger aircraft for the years 2005-2011. The CH3Cl mixing ratio in the UT over Europe was higher than that observed at a European surface baseline station throughout the year, indicative of a persistent positive vertical gradient at Northern Hemisphere midlatitudes. A series of flights over Africa and South Asia show that CH3Cl mixing ratios increase toward tropical latitudes, and the observed UT CH3Cl level over these two regions and the Atlantic was higher than that measured at remote surface sites. Strong emissions of CH3Cl in the tropics combined with meridional air transport through the UT may explain such vertical and latitudinal gradients. Comparisons with carbon monoxide (CO) data indicate that noncombustion sources in the tropics dominantly contribute to forming the latitudinal gradient of CH3Cl in the UT. We also observed elevated mixing ratios of CH3Cl and CO in air influenced by biomass burning in South America and Africa, and the enhancement ratios derived for CH3Cl to CO in those regions agree with previous observations. In contrast, correlations indicate a high CH3Cl to CO ratio of 2.9 ± 0.5 ppt ppb-1 in the Asian summer monsoon anticyclone and domestic biofuel emissions in South Asia are inferred to be responsible. We estimated the CH3Cl emission in South Asia to be 134 ± 23 Gg Cl yr-1, which is higher than a previous estimate due to the higher CH3Cl to CO ratio observed in this study.

  10. Measurement of low-ppm mixing ratios of water vapor in the upper troposphere and lower stratosphere using chemical ionization mass spectrometry

    Directory of Open Access Journals (Sweden)

    T. D. Thornberry

    2013-06-01

    Full Text Available A chemical ionization mass spectrometer (CIMS instrument has been developed for the fast, precise, and accurate measurement of water vapor (H2O at low mixing ratios in the upper troposphere and lower stratosphere (UT/LS. A low-pressure flow of sample air passes through an ionization volume containing an α-particle radiation source, resulting in a cascade of ion-molecule reactions that produce hydronium ions (H3O+ from ambient H2O. The production of H3O+ ions from ambient H2O depends on pressure and flow through the ion source, which were tightly controlled in order to maintain the measurement sensitivity independent of changes in the airborne sampling environment. The instrument was calibrated every 45 min in flight by introducing a series of H2O mixing ratios between 0.5 and 153 parts per million (ppm, 10−6 mol mol−1 generated by Pt-catalyzed oxidation of H2 standards while overflowing the inlet with dry synthetic air. The CIMS H2O instrument was deployed in an unpressurized payload area aboard the NASA WB-57F high-altitude research aircraft during the Mid-latitude Airborne Cirrus Properties Experiment (MACPEX mission in March and April 2011. The instrument performed successfully during seven flights, measuring H2O mixing ratios below 5 ppm in the lower stratosphere at altitudes up to 17.7 km, and as low as 3.5 ppm near the tropopause. Data were acquired at 10 Hz and reported as 1 s averages. In-flight calibrations demonstrated a typical sensitivity of 2000 Hz ppm−1 at 3 ppm with a signal to noise ratio (2 σ, 1 s greater than 32. The total measurement uncertainty was 9 to 11%, derived from the uncertainty in the in situ calibrations.

  11. 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.

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

    Science.gov (United States)

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

    2012-04-01

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

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

    Directory of Open Access Journals (Sweden)

    T. von Clarmann

    2010-10-01

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

  14. In-situ BrO measurements in the upper troposphere / lower stratosphere. Validation of the ENVISAT satellite measurements and photochemical model studies

    Energy Technology Data Exchange (ETDEWEB)

    Hrechanyy, S.

    2007-04-15

    Inorganic bromine species form the second most important halogen family affecting stratospheric ozone (WMO, 2003). Although the stratospheric bromine mixing ratio is about two orders of magnitude lower than the chlorine one, bromine has much higher ozone depleting potential (factor of about 45) compared to chlorine. This study reports and discusses atmospheric bromine monoxide, BrO, measurements in the altitude range 15-30 km performed by the balloon-borne instrument TRIPLE and aircraft instrument HALOX employing the chemical conversion resonance fluorescence technique, which is the only proven in-situ technique for the measurements of BrO. 57 HALOX flights have been performed in the frame of five field campaigns ranging from the Arctic to tropics. Three TRIPLE flights were carried out at high and mid latitudes in the frame of the SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) validation. Calibration, consistency checks, data analysis, and error assessment for the in-situ measurements are described. The balloon measurements have yielded vertical profiles of BrO between 15 and 30 km altitude at northern mid- and at arctic latitudes. From the aircraft measurements a meridional BrO distribution from tropical to the arctic latitudes between 15 and 20 km altitude was obtained. In order to check the reliability of the bromine chemistry in the CLaMS model the BrO profile measured by TRIPLE on June 9, 2003 in Arctic spring/summer conditions was compared to a simulated BrO profile. For the simulation the model was initialized with appropriate satellite and balloon measurements and with a total stratospheric bromine of 18.4 pptv. Very good agreement between the TRIPLE measurements and model results was found. Measurements of BrO in the tropical tropopause layer (TTL) are well suited to investigate the contribution of very short-lived bromine species (VSLS) to the inorganic bromine, Bry. Since tropical HALOX BrO measurements from TROCCINOX

  15. Synthesis of 10-Ethyl Flavin: A Multistep Synthesis Organic Chemistry Laboratory Experiment for Upper-Division Undergraduate Students

    Science.gov (United States)

    Sichula, Vincent A.

    2015-01-01

    A multistep synthesis of 10-ethyl flavin was developed as an organic chemistry laboratory experiment for upper-division undergraduate students. Students synthesize 10-ethyl flavin as a bright yellow solid via a five-step sequence. The experiment introduces students to various hands-on experimental organic synthetic techniques, such as column…

  16. Modeling Human Serum Albumin Tertiary Structure to Teach Upper-Division Chemistry Students Bioinformatics and Homology Modeling Basics

    Science.gov (United States)

    Petrovic, Dus?an; Zlatovic´, Mario

    2015-01-01

    A homology modeling laboratory experiment has been developed for an introductory molecular modeling course for upper-division undergraduate chemistry students. With this experiment, students gain practical experience in homology model preparation and assessment as well as in protein visualization using the educational version of PyMOL…

  17. Evidence of Convective Redistribution of Carbon Monoxide in Aura Tropospheric Emission Sounder (TES) and Microwave Limb Sounder (MLS) Observations

    Science.gov (United States)

    Manyin, Michael; Douglass, Anne; Schoeberl, Mark

    2010-01-01

    Vertical convective transport is a key element of the tropospheric circulation. Convection lofts air from the boundary layer into the free troposphere, allowing surface emissions to travel much further, and altering the rate of chemical processes such as ozone production. This study uses satellite observations to focus on the convective transport of CO from the boundary layer to the mid and upper troposphere. Our hypothesis is that strong convection associated with high rain rate regions leads to a correlation between mid level and upper level CO amounts. We first test this hypothesis using the Global Modeling Initiative (GMI) chemistry and transport model. We find the correlation is robust and increases as the precipitation rate (the strength of convection) increases. We next examine three years of CO profiles from the Tropospheric Emission Sounder (TES) and Microwave Limb Sounder (MLS) instruments aboard EOS Aura. Rain rates are taken from the Tropical Rainfall Measuring Mission (TRMM) 3B-42 multi-satellite product. Again we find a correlation between mid-level and upper tropospheric CO, which increases with rain rate. Our result shows the critical importance of tropical convection in coupling vertical levels of the troposphere in the transport of trace gases. The effect is seen most clearly in strong convective regions such as the Inter-tropical Convergence Zone.

  18. Tropospheric Aerosols

    Science.gov (United States)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    within the atmosphere. Therefore, the few existing approaches to chemical transformation and aerosol evolution rest heavily on assumptions, for example, that particles are adequately represented as spheres and are homogeneous in composition as a function of particle size, although both assumptions are known to be inaccurate (e.g., Buseck and Pósfai, 1999; Buseck et al., 2002).This chapter provides an overview of the loading, geographical distribution, and chemical and physical properties of both natural and anthropogenic atmospheric aerosols and of the processes controlling their production, reaction, transport, and ultimate removal - the "life cycle" of tropospheric aerosols. More detailed treatment may be found in texts by Junge (1963), Friedlander (1977), Twomey (1977), Hinds (1982, 1999), Seinfeld and Pandis (1998), and Jacob (1999). We highlight here the effects of aerosols on climate. The effects of aerosols on health, visibility, heterogeneous chemistry, and ozone are examined by Heintzenberg et al. (2003), Jacob (2000), Kreidenweis (1995), Anastasio and Martin (2001), Pósfai and Molnár (2000), and Prospero et al. (2002). A detailed overview of tropospheric aerosols and their environmental effects is given by EPA (2002). Kaufman et al. (2002) provide an overview of satellite measurement of aerosols pertinent to climate change.

  19. Homepage for the Global Tropospheric Experiment

    Science.gov (United States)

    Ward, Eugene

    1995-01-01

    The objective of my NASA summer research project was to create a homepage to describe and present results from the NASA Global Tropospheric Experiment (GTE). The GTE is a major component of NASA's Tropospheric Chemistry Program and is managed in the Atmospheric Studies Branch, Atmospheric Sciences Division at the NASA Langley Research Center.

  20. HALIPP. Photocatalysis of tropospheric chemistry by sea salt. Final report; HALIPP. Photokatalyse der Luftchemie durch Seesalz-Aerosole. Abschlussbericht

    Energy Technology Data Exchange (ETDEWEB)

    Zetzsch, C; Scheer, V; Krueger, H U; Behnke, W

    1994-12-31

    The reactions of gaseous NO{sub 2} and N{sub 2}O{sub 5} with humidified NaCl-aerosol and humidified mixed NaCl/NaNO{sub 3}- and NaCl/Na{sub 2}SO{sub 4} -aerosols and of gaseous O{sub 3} with humidified sea-salt aerosol were investigated. An upper limit of <10{sup 4} was estimated for the uptake coefficient of NO{sub 2} from our measurements, the uptake coefficient of N{sub 2}O{sub 5} was determined to be 0.032{+-}0.003 (stated error: {+-}2{sigma}). Instead of NOCl reported as a product from NaCl in the literature, HONO is formed from the reaction of NO{sub 2} with deliquescent NaCl aerosol. Gaseaous N{sub 2}O{sub 5} is converted to gaseous CINO{sub 2} below relative humidities of 94%. Only at much higher humidities the formation of 2 HNO{sub 3} increases. No precursors of atomic Cl are observed to be formed from gaseous ozone and pure NaCl-aerosol. Only in the presence of seal-salt aerosols a formation of Cl{sub 2} is found (although not yet quantified). (orig.) [Deutsch] Es wurde die Reaktion von gasfoermigem NO{sub 2} und N{sub 2}O{sub 5} mit feuchtem NaCl- und gemischtem NaCl/NaNO{sub 3}- und NaCl/Na{sub 2}SO{sub 4}- Aerosol sowie von gasfoermigem O{sub 3} mit feuchtem Seesalzaerosol untersucht. Der Uptake-Koeffizient von NO{sub 2} wurde mit kleiner 10{sup -4} abgeschaetzt, der von N{sub 2}O{sub 5} mit 0.032{+-}0.003 (2{sigma}-Fehler) bestimmt. In Gegenwart von NO{sub 2} bildet sich anstelle des in der Literatur angegebenen NOCl gasfoermigs HONO und in Gegenwart von N{sub 2}O{sub 5} unterhalb einer relativen Feuchte von 94% hauptsaechlich gasfoermiges ClNO{sub 2}. Erst in Gegenwart wesentlich hoeherer Feuchten nimmt die Bildung von 2HNO{sub 3} zu. In Gegenwart von Ozon und reinem NaCl-Aerosol bilden sich keine Chloratomvorlaeufer. Erst in Gegenwart von Seesalzaerosolen kommt es zur Bildung von Cl{sub 2}. Eine Quantifizierung dieser letzteren Ergebnisse wurde noch nicht durchgefuehrt. (orig.)

  1. The Role of Convection in Redistributing Formaldehyde to the Upper Troposphere Over North America and the North Atlantic during the Summer 2004 INTEX Campaign

    Science.gov (United States)

    Fried, Alan; Olson, Jennifer R.; Walega, Jim; Crawford, Jim H.; Chen, Gao; Weibring, Petter; Richter, Dirk; Roller, Chad; Tittel, Frank; Porter, Michael; hide

    2007-01-01

    Measurements of CH2O from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 during the summer 2004 INTEX-NA (Intercontinental Chemical Transport Experiment - North America) campaign to test our understanding of convection and production mechanisms in the upper troposphere (UT, 6-12-km) over continental North America and the North Atlantic Ocean. Point-by-point comparisons with box model calculations, when MHP (CH3OOH) measurements were available for model constraint, resulted in a median CH2O measurement/model ratio of 0.91 in the UT. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46% of the TDLAS measurements fell within the latter category. At least 66% to 73% of these elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. This distinction is important, since the effects from the former can last for over a week or more compared to one day or less in the case of convective transport of CH2O itself. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from MHP, methanol, PAN type compounds, and ketones, in descending order of their contribution. In the presence of elevated NO from lightning and potentially from the stratosphere, there was a definite trend in the CH2O discrepancy, which for the highest NO mixing ratios produced a median CH2O measurement/model ratio of 3.9 in the 10-12-km range. Discrepancies in CH2O and HO2 in the UT with NO were highly correlated and this provided further information as to the possible mechanism(s) responsible. These discrepancies with NO are consistent with additional production sources of both gases involving CH3O2 + NO reactions, most likely caused by unmeasured hydrocarbons.

  2. Model study of the impacts of emissions, chemical and dynamical processes on the CO variability in the tropical upper troposphere and lower stratosphere

    Directory of Open Access Journals (Sweden)

    Chunxiao Wang

    2015-07-01

    Full Text Available The Whole Atmosphere Community Climate Model (WACCM is used to investigate the relative importance of CO emissions, chemical and dynamical processes on temporal variations of CO in the tropical upper troposphere (UT and the lower stratosphere (LS. The semi-annual oscillation (SAO in the tropical UT and the annual oscillation (AO in the tropical LS detected in the MLS CO observations can be well captured by the model. The model simulations reveal that the CO surface emissions explain most of the SAO signals in the tropical UT, with the remainder being attributed to dynamical and chemical processes. The CO AO in the LS primarily results from combined effects of dynamical and chemical processes while the dynamical and chemical processes make opposite contributions to the CO AO signals, consistent with the previous findings. Our analysis further reveals that CO surface emissions tend to weaken the amplitude of the CO annual cycle in the tropical LS, while the annual variations in the meridional component of the Brewer–Dobson (BD circulation can amplify the annual variations of CO above 30 hPa. The model simulations also indicate that the CO annual cycle in the LS has a mixed behaviour with the annual variations of tropical upwelling reflected in CO between ~70 and ~50 hPa and a standard tape-recorder signal above 50 hPa. Moreover, the AO signals of CO exist up to 10 hPa when the chemical processes are switched off. The temporal and spatial variations of CO in the UT and near the tropopause are mainly driven by the upward transport of CO by tropical deep convection and the Asian summer monsoon circulation. In the early stage of the South Asian summer monsoon over the Bay of Bengal and the South China in the late spring and early summer, the transport of the CO surface emissions over Southeast Asia by the South Asian summer monsoon leads to an increase in the tropical CO, but the horizontal transport from the extratropics into the tropics (termed in

  3. Carbon monoxide distributions from the upper troposphere to the mesosphere inferred from 4.7 μm non-local thermal equilibrium emissions measured by MIPAS on Envisat

    Directory of Open Access Journals (Sweden)

    B. Funke

    2009-04-01

    Full Text Available We present global distributions of carbon monoxide (CO from the upper troposphere to the mesosphere observed by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS on Envisat. Vertically resolved volume mixing ratio profiles have been retrieved from 4.7 μm limb emission spectra under consideration of non-local thermodynamic equilibrium. The precision of individual CO profiles is typically 5–30 ppbv (15–40% for altitudes greater than 40 km and lower than 15 km and 30–90% within 15–40 km. Estimated systematic errors are in the order of 8–15%. Below 60 km, the vertical resolution is 4–7 km. The data set which covers 54 days from September 2003 to March 2004 has been derived with an improved retrieval version including (i the retrieval of log(vmr, (ii the consideration of illumination-dependent vibrational population gradients along the instrument's line of sight, and (iii joint-fitted vmr horizontal gradients in latitudinal and longitudinal directions. A detailed analysis of spatially resolved CO distributions during the 2003/2004 Northern Hemisphere major warming event demonstrate the potential of MIPAS CO observations to obtain new information on transport processes during dynamical active episodes, particularly on those acting in the vertical. From the temporal evolution of zonally averaged CO abundances, we derived extraordinary polar winter descent velocities of 1200 m per day inside the recovered polar vortex in January 2004. Middle stratospheric CO abundances show a well established correlation with the chemical source CH4, particularly in the tropics. In the upper troposphere, a moderate CO decrease from September 2003 to March 2004 was observed. Upper tropospheric CO observations provide a detailed picture of long-range transport of polluted air masses and uplift events. MIPAS observations taken on 9–11 September 2003 confirm the trapping of convective outflow of polluted CO-rich air from

  4. The Governing Processes and Timescales of Stratosphere-to-Troposphere Transport and its Contribution to Ozone in the Arctic Troposphere

    Science.gov (United States)

    Liang, Q.; Douglass, A. R.; Duncan, B. N.; Stolarski, R. S.; Witte, J. C.

    2009-01-01

    We used the seasonality of a combination of atmospheric trace gases and idealized tracers to examine stratosphere-to-troposphere transport and its influence on tropospheric composition in the Arctic. Maximum stratosphere-to-troposphere transport of CFCs and O3 occurs in April as driven by the Brewer-Dobson circulation. Stratosphere-troposphere exchange (STE) occurs predominantly between 40 deg N to 80 deg N with stratospheric influx in the mid-latitudes (30-70 deg N) accounting for 67.81 percent of the air of stratospheric origin in the Northern Hemisphere extratropical troposphere. Transport from the lower stratosphere to the lower troposphere (LT) takes three months on average, one month to cross the tropopause, the second month to travel from the upper troposphere (UT) to the middle troposphere (MT), and the third month to reach the LT. During downward transport, the seasonality of a trace gas can be greatly impacted by wet removal and chemistry. A comparison of idealized tracers with varying lifetimes suggests that when initialized with the same concentrations and seasonal cycles at the tropopause, trace gases that have shorter lifetimes display lower concentrations, smaller amplitudes, and earlier seasonal maxima during transport to the LT. STE contributes to O3 in the Arctic troposphere directly from the transport of O3 and indirectly from the transport of NOy . Direct transport of O3 from the stratosphere accounts for 78 percent of O3 in the Arctic UT with maximum contributions occurring from March to May. The stratospheric contribution decreases significantly in the MT/LT (20.25 percent of total O3) and shows a very weak March.April maximum. Our NOx budget analysis in the Arctic UT shows that during spring and summer, the stratospheric injection of NO y-rich air increases NOx concentrations above the 20 pptv threshold level, thereby shifting the Arctic UT from a regime of net photochemical ozone loss to one of net production with rates as high as +16 ppbv/month.

  5. Model Calculations of Changes in Tropospheric Ozone Over Europe and the Role of Surface Sources and Aircraft Emissions

    Energy Technology Data Exchange (ETDEWEB)

    Hov, Oe [Bergen Univ. (Norway)

    1996-01-01

    This conference paper deals with a study of the impact of various sources of NO{sub x} on the ozone production in the free troposphere. A comprehensive two-dimensional zonally averaged chemistry/transport model and a three-dimensional meso-scale chemical transport (MCT) model are used in the study. Using the two-dimensional model, three surches of NO{sub x} in the upper troposphere were examined covering NO{sub x} produced by lightening, NO{sub x} (and NO{sub y}) brought to the upper troposphere from the planetary boundary layer by rapid vertical transport processes, and NO{sub x} emitted from aircraft. 4 refs.

  6. The effect of clouds on photolysis rates and ozone formation in the unpolluted troposphere

    Science.gov (United States)

    Thompson, A. M.

    1984-01-01

    The photochemistry of the lower atmosphere is sensitive to short- and long-term meteorological effects; accurate modeling therefore requires photolysis rates for trace gases which reflect this variability. As an example, the influence of clouds on the production of tropospheric ozone has been investigated, using a modification of Luther's two-stream radiation scheme to calculate cloud-perturbed photolysis rates in a one-dimensional photochemical transport model. In the unpolluted troposphere, where stratospheric inputs of odd nitrogen appear to represent the photochemical source of O3, strong cloud reflectance increases the concentration of NO in the upper troposphere, leading to greatly enhanced rates of ozone formation. Although the rate of these processes is too slow to verify by observation, the calculation is useful in distinguishing some features of the chemistry of regions of differing mean cloudiness.

  7. Controls on Surface Water Chemistry in the Upper Merced River Basin, Yosemite National Park, California

    Science.gov (United States)

    Clow, David W.; Alisa Mast, M.; Campbell, Donald H.

    1996-05-01

    Surface water draining granitic bedrock in Yosemite National Park exhibits considerable variability in chemical composition, despite the relative homogeneity of bedrock chemistry. Other geological factors, including the jointing and distribution of glacial till, appear to exert strong controls on water composition. Chemical data from three surface water surveys in the upper Merced River basin conducted in August 1981, June 1988 and August 1991 were analysed and compared with mapped geological, hydrological and topographic features to identify the solute sources and processes that control water chemistry within the basin during baseflow. Water at most of the sampling sites was dilute, with alkalinities ranging from 26 to 77 equiv. l-1. Alkalinity was much higher in two subcatchments, however, ranging from 51 to 302 equiv. l-1. Base cations and silica were also significantly higher in these two catchments than in the rest of the watershed. Concentrations of weathering products in surface water were correlated to the fraction of each subcatchment underlain by surficial material, which is mostly glacial till. Silicate mineral weathering is the dominant control on concentrations of alkalinity, silica and base cations, and ratios of these constituents in surface water reflect the composition of local bedrock. Chloride concentrations in surface water samples varied widely, ranging from <1 to 96 equiv. l-1. The annual volume-weighted mean chloride concentration in the Merced River at the Happy Isles gauge from 1968 to 1990 was 26 equiv. l-1, which was five times higher than in atmospheric deposition (4-5 equiv. l-1), suggesting that a source of chloride exists within the watershed. Saline groundwater springs, whose locations are probably controlled by vertical jointing in the bedrock, are the most likely source of the chloride. Sulphate concentrations varied much less than most other solutes, ranging from 3 to 14 equiv. l-1. Concentrations of sulphate in quarterly samples

  8. In situ measurements of tropical cloud properties in the West African Monsoon: upper tropospheric ice clouds, Mesoscale Convective System outflow, and subvisual cirrus

    Directory of Open Access Journals (Sweden)

    W. Frey

    2011-06-01

    Full Text Available In situ measurements of ice crystal size distributions in tropical upper troposphere/lower stratosphere (UT/LS clouds were performed during the SCOUT-AMMA campaign over West Africa in August 2006. The cloud properties were measured with a Forward Scattering Spectrometer Probe (FSSP-100 and a Cloud Imaging Probe (CIP operated aboard the Russian high altitude research aircraft M-55 Geophysica with the mission base in Ouagadougou, Burkina Faso. A total of 117 ice particle size distributions were obtained from the measurements in the vicinity of Mesoscale Convective Systems (MCS. Two to four modal lognormal size distributions were fitted to the average size distributions for different potential temperature bins. The measurements showed proportionately more large ice particles compared to former measurements above maritime regions. With the help of trace gas measurements of NO, NOy, CO2, CO, and O3 and satellite images, clouds in young and aged MCS outflow were identified. These events were observed at altitudes of 11.0 km to 14.2 km corresponding to potential temperature levels of 346 K to 356 K. In a young outflow from a developing MCS ice crystal number concentrations of up to (8.3 ± 1.6 cm−3 and rimed ice particles with maximum dimensions exceeding 1.5 mm were found. A maximum ice water content of 0.05 g m−3 was observed and an effective radius of about 90 μm. In contrast the aged outflow events were more diluted and showed a maximum number concentration of 0.03 cm−3, an ice water content of 2.3 × 10−4 g m−3, an effective radius of about 18 μm, while the largest particles had a maximum dimension of 61 μm.

    Close to the tropopause subvisual cirrus were encountered four times at altitudes of 15 km to 16.4 km. The mean ice particle number concentration of these encounters was 0.01 cm−3 with maximum particle sizes of 130

  9. Observing Tropospheric Ozone From Space

    Science.gov (United States)

    Fishman, Jack

    2000-01-01

    The importance of tropospheric ozone embraces a spectrum of relevant scientific issues ranging from local environmental concerns, such as damage to the biosphere and human health, to those that impact global change questions, Such is climate warming. From an observational perspective, the challenge is to determine the tropospheric ozone global distribution. Because its lifetime is short compared with other important greenhouse gases that have been monitored over the past several decades, the distribution of tropospheric ozone cannot be inferred from a relatively small set of monitoring stations. Therefore, the best way to obtain a true global picture is from the use of space-based instrumentation where important spatial gradients over vast ocean expanses and other uninhabited areas can be properly characterized. In this paper, the development of the capability to measure tropospheric ozone from space over the past 15 years is summarized. Research in the late 1980s successfully led to the determination of the climatology of tropospheric ozone as a function of season; more recently, the methodology has improved to the extent where regional air pollution episodes can be characterized. The most recent modifications now provide quasi-global (50 N) to 50 S) maps on a daily basis. Such a data set would allow for the study of long-range (intercontinental) transport of air pollution and the quantification of how regional emissions feed into the global tropospheric ozone budget. Future measurement capabilities within this decade promise to offer the ability to provide Concurrent maps of the precursors to the in situ formation of tropospheric ozone from which the scientific community will gain unprecedented insight into the processes that control global tropospheric chemistry

  10. A Lagrangian model of air-mass photochemistry and mixing using a trajectory ensemble: the Cambridge Tropospheric Trajectory model of Chemistry And Transport (CiTTyCAT version 4.2

    Directory of Open Access Journals (Sweden)

    T. A. M. Pugh

    2012-01-01

    Full Text Available A Lagrangian model of photochemistry and mixing is described (CiTTyCAT, stemming from the Cambridge Tropospheric Trajectory model of Chemistry And Transport, which is suitable for transport and chemistry studies throughout the troposphere. Over the last five years, the model has been developed in parallel at several different institutions and here those developments have been incorporated into one "community" model and documented for the first time. The key photochemical developments include a new scheme for biogenic volatile organic compounds and updated emissions schemes. The key physical development is to evolve composition following an ensemble of trajectories within neighbouring air-masses, including a simple scheme for mixing between them via an evolving "background profile", both within the boundary layer and free troposphere. The model runs along trajectories pre-calculated using winds and temperature from meteorological analyses. In addition, boundary layer height and precipitation rates, output from the analysis model, are interpolated to trajectory points and used as inputs to the mixing and wet deposition schemes. The model is most suitable in regimes when the effects of small-scale turbulent mixing are slow relative to advection by the resolved winds so that coherent air-masses form with distinct composition and strong gradients between them. Such air-masses can persist for many days while stretching, folding and thinning. Lagrangian models offer a useful framework for picking apart the processes of air-mass evolution over inter-continental distances, without being hindered by the numerical diffusion inherent to global Eulerian models. The model, including different box and trajectory modes, is described and some output for each of the modes is presented for evaluation. The model is available for download from a Subversion-controlled repository by contacting the corresponding authors.

  11. Source attribution of tropospheric ozone

    Science.gov (United States)

    Butler, T. M.

    2015-12-01

    Tropospheric ozone is a harmful pollutant with adverse effects on human health and ecosystems. As well as these effects, tropospheric ozone is also a powerful greenhouse gas, with an anthropogenic radiative forcing one quarter of that of CO2. Along with methane and atmospheric aerosol, tropospheric ozone belongs to the so-called Short Lived Climate forcing Pollutants, or SLCP. Recent work has shown that efforts to reduce concentrations of SLCP in the atmosphere have the potential to slow the rate of near-term climate change, while simultaneously improving public health and reducing crop losses. Unlike many other SLCP, tropospehric ozone is not directly emitted, but is instead influenced by two distinct sources: transport of air from the ozone-rich stratosphere; and photochemical production in the troposphere from the emitted precursors NOx (oxides of nitrogen), CO (Carbon Monoxide), and VOC (volatile organic compounds, including methane). Better understanding of the relationship between ozone production and the emissions of its precursors is essential for the development of targeted emission reduction strategies. Several modeling methods have been employed to relate the production of tropospheric ozone to emissions of its precursors; emissions perturbation, tagging, and adjoint sensitivity methods all deliver complementary information about modelled ozone production. Most studies using tagging methods have focused on attribution of tropospheric ozone production to emissions of NOx, even though perturbation methods have suggested that tropospheric ozone is also sensitive to VOC, particularly methane. In this study we describe the implementation into a global chemistry-climate model of a scheme for tagging emissions of NOx and VOC with an arbitrary number of labels, which are followed through the chemical reactions of tropospheric ozone production in order to perform attribution of tropospehric ozone to its emitted precursors. Attribution is performed to both

  12. Chemical processes related to net ozone tendencies in the free troposphere

    Science.gov (United States)

    Bozem, Heiko; Butler, Tim M.; Lawrence, Mark G.; Harder, Hartwig; Martinez, Monica; Kubistin, Dagmar; Lelieveld, Jos; Fischer, Horst

    2017-09-01

    Ozone (O3) is an important atmospheric oxidant, a greenhouse gas, and a hazard to human health and agriculture. Here we describe airborne in situ measurements and model simulations of O3 and its precursors during tropical and extratropical field campaigns over South America and Europe, respectively. Using the measurements, net ozone formation/destruction tendencies are calculated and compared to 3-D chemistry-transport model simulations. In general, observation-based net ozone tendencies are positive in the continental boundary layer and the upper troposphere at altitudes above ˜ 6 km in both environments. On the other hand, in the marine boundary layer and the middle troposphere, from the top of the boundary layer to about 6-8 km altitude, net O3 destruction prevails. The ozone tendencies are controlled by ambient concentrations of nitrogen oxides (NOx). In regions with net ozone destruction the available NOx is below the threshold value at which production and destruction of O3 balance. While threshold NO values increase with altitude, in the upper troposphere NOx concentrations are generally higher due to the integral effect of convective precursor transport from the boundary layer, downward transport from the stratosphere and NOx produced by lightning. Two case studies indicate that in fresh convective outflow of electrified thunderstorms net ozone production is enhanced by a factor 5-6 compared to the undisturbed upper tropospheric background. The chemistry-transport model MATCH-MPIC generally reproduces the pattern of observation-based net ozone tendencies but mostly underestimates the magnitude of the net tendency (for both net ozone production and destruction).

  13. The behaviour of stratospheric and upper tropospheric ozone in high and mid latitudes; the role of ozone as a climate gas

    Energy Technology Data Exchange (ETDEWEB)

    Kyroe, M.; Rummukainen, M.; Kivi, R.; Turunen, T.; Karhu, J. [Finnish Meteorological Inst., Sodankylae (Finland); Taalas, P. [Finnish Meteorological Inst., Helsinki (Finland)

    1996-12-31

    During the past few years, the dual role that ozone plays in climate change has been becoming increasingly obvious. First, continuous thinning of the ozone layer has been evident, even in the high and middle latitudes in the northern hemisphere. Secondly, ozone is also a greenhouse gas, affecting radiative transfer. Increases in tropospheric ozone have a positive forcing, whereas decreases in stratospheric ozone cause a negative forcing. During the last six years, measurements on total ozone and the vertical distribution of ozone have been performed at the Sodankylae Observatory. At Jokioinen Observatory, measurements on total ozone have been performed since 1990 and measurements on the vertical distribution of ozone since 1993. The overall project has focused on extending the national data series on total ozone and the vertical distribution of ozone. At the same time, the study has contributed to the study of interannual variability of the ozone layer. This SILMU project took part in the large-scale research activities, in addition to performing national studies. The results confirm that there has been fast chemical ozone destruction in the high latitudes in the northern hemisphere. This was particularly evident in the last two winters, 1994/95 and 1995/96. The new data also allows better trend analyses to be made on ozone in high and mid latitudes

  14. The behaviour of stratospheric and upper tropospheric ozone in high and mid latitudes; the role of ozone as a climate gas

    Energy Technology Data Exchange (ETDEWEB)

    Kyroe, M; Rummukainen, M; Kivi, R; Turunen, T; Karhu, J [Finnish Meteorological Inst., Sodankylae (Finland); Taalas, P [Finnish Meteorological Inst., Helsinki (Finland)

    1997-12-31

    During the past few years, the dual role that ozone plays in climate change has been becoming increasingly obvious. First, continuous thinning of the ozone layer has been evident, even in the high and middle latitudes in the northern hemisphere. Secondly, ozone is also a greenhouse gas, affecting radiative transfer. Increases in tropospheric ozone have a positive forcing, whereas decreases in stratospheric ozone cause a negative forcing. During the last six years, measurements on total ozone and the vertical distribution of ozone have been performed at the Sodankylae Observatory. At Jokioinen Observatory, measurements on total ozone have been performed since 1990 and measurements on the vertical distribution of ozone since 1993. The overall project has focused on extending the national data series on total ozone and the vertical distribution of ozone. At the same time, the study has contributed to the study of interannual variability of the ozone layer. This SILMU project took part in the large-scale research activities, in addition to performing national studies. The results confirm that there has been fast chemical ozone destruction in the high latitudes in the northern hemisphere. This was particularly evident in the last two winters, 1994/95 and 1995/96. The new data also allows better trend analyses to be made on ozone in high and mid latitudes

  15. Secondary ozone peaks in the troposphere over the Himalayas

    Directory of Open Access Journals (Sweden)

    N. Ojha

    2017-06-01

    Full Text Available Layers with strongly enhanced ozone concentrations in the middle–upper troposphere, referred to as secondary ozone peaks (SOPs, have been observed in different regions of the world. Here we use the global ECHAM5/MESSy atmospheric chemistry model (EMAC to (i investigate the processes causing SOPs, (ii explore both their frequency of occurrence and seasonality, and (iii assess their effects on the tropospheric ozone budget over the Himalayas. The vertical profiles of potential vorticity (PV and a stratospheric ozone tracer (O3s in EMAC simulations, in conjunction with the structure of SOPs, suggest that SOPs over the Himalayas are formed by stratosphere-to-troposphere transport (STT of ozone. The spatial distribution of O3s further shows that such effects are in general most pronounced in the northern part of India. Model simulated ozone distributions and backward air trajectories show that ozone rich air masses, associated with STT, originate as far as northern Africa and the North Atlantic Ocean, the Middle East, as well as in nearby regions in Afghanistan and Pakistan, and are rapidly (within 2–3 days transported to the Himalayas. Analysis of a 15-year (2000–2014 EMAC simulation shows that the frequency of SOPs is highest during the pre-monsoon season (e.g. 11 % of the time in May, while no intense SOP events are found during the July–October period. The SOPs are estimated to enhance the tropospheric column ozone (TCO over the central Himalayas by up to 21 %.

  16. Variations of tropospheric methane over Japan during 1988–2010

    Directory of Open Access Journals (Sweden)

    Taku Umezawa

    2014-05-01

    Full Text Available We present observations of CH4 concentrations from the lower to upper troposphere (LT and UT over Japan during 1988–2010 based on aircraft measurements from the Tohoku University (TU. The analysis is aided by simulation results using an atmospheric chemistry transport model (i.e. ACTM. Tropospheric CH4 over Japan shows interannual and seasonal variations that are dependent on altitudes, primarily reflecting differences in air mass origins at different altitudes. The long-term trend and interannual variation of CH4 in the LT are consistent with previous reports of measurements at surface baseline stations in the northern hemisphere. However, those in the UT show slightly different features from those in the LT. In the UT, CH4 concentrations show a seasonal maximum in August due to efficient transport of air masses influenced by continental CH4 sources, while LT CH4 reaches its seasonal minimum during summer due to enhanced chemical loss. Vertical profiles of the CH4 concentrations also vary with season, reflecting the seasonal cycles at the respective altitudes. In summer, transport of CH4-rich air from Asian regions elevates UT CH4 levels, forming a uniform vertical profile above the mid-troposphere. On the other hand, CH4 decreases nearly monotonically with altitude in winter–spring. The ACTM simulations with different emission scenarios reproduce general features of the tropospheric CH4 variations over Japan. Tagged tracer simulations using the ACTM indicate substantial contributions of CH4 sources in South Asia and East Asia to the summertime high CH4 values observed in the UT. This suggests that our observations over Japan are highly sensitive to CH4 emission signals particularly from Asia.

  17. Aerosol indirect effect on tropospheric ozone via lightning

    Science.gov (United States)

    Yuan, T.; Remer, L. A.; Bian, H.; Ziemke, J. R.; Albrecht, R. I.; Pickering, K. E.; Oreopoulos, L.; Goodman, S. J.; Yu, H.; Allen, D. J.

    2012-12-01

    Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. The unresolved difference between modeled and observed natural background O3 concentrations is a key source of the uncertainty. Here we demonstrate remarkable sensitivity of lightning activity to aerosol loading with lightning activity increasing more than 30 times per unit of aerosol optical depth over our study area. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses suggest O3 is increased as a result of aerosol-induced increase in lightning and lightning produced NOx. Model simulations with prescribed lightning change corroborate the satellite data analysis. This aerosol-O3 connection is achieved via aerosol increasing lightning and thus lightning produced nitrogen oxides. This aerosol-lightning-ozone link provides a potential physical mechanism that may account for a part of the model-observation difference in background O3 concentration. More importantly, O3 production increase from this link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. Both of these implications suggest a stronger O3 historical radiative forcing. This introduces a new pathway, through which increasing in aerosols from pre-industrial time to present day enhances tropospheric O3 production. Aerosol forcing thus has a warming component via its effect on O3 production. Sensitivity simulations suggest that 4-8% increase of tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications

  18. Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

    Directory of Open Access Journals (Sweden)

    B. Newsome

    2017-12-01

    Full Text Available Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global, use these rate constants. Expert panels evaluate laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the Jet Propulsion Laboratory (JPL and International Union of Pure and Applied Chemistry (IUPAC evaluations we assess the influence of 50 mainly inorganic rate constants and 10 photolysis rates on tropospheric composition through the use of the GEOS-Chem chemistry transport model. We assess the impact on four standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH →M  HNO3 and O3 + NO  →  NO2 + O2 are the two largest sources of uncertainty in these metrics. The absolute magnitude of the change in the metrics is similar if rate constants are increased or decreased by their σ values. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 10, 11, 16 and 16 %, respectively. These are larger than the spread between models in recent model intercomparisons. Remote

  19. Mid-infrared spectroscopy of Uranus from the Spitzer Infrared Spectrometer: 1. Determination of the mean temperature structure of the upper troposphere and stratosphere

    Science.gov (United States)

    Orton, Glenn S.; Fletcher, Leigh N.; Moses, Julianne I.; Mainzer, Amy K.; Hines, Dean; Hammel, Heidi B.; Martin-Torres, F. Javier; Burgdorf, Martin; Merlet, Cecile; Line, Michael R.

    2014-11-01

    On 2007 December 16-17, spectra were acquired of the disk of Uranus by the Spitzer Infrared Spectrometer (IRS), ten days after the planet's equinox, when its equator was close to the sub-Earth point. This spectrum provides the highest-resolution broad-band spectrum ever obtained for Uranus from space, allowing a determination of the disk-averaged temperature and molecule composition to a greater degree of accuracy than ever before. The temperature profiles derived from the Voyager radio occultation experiment by Lindal et al. (Lindal, G.F., Lyons, J.R., Sweetnam, D.N., Eshleman, V.R., Hinson, D.P. [1987]. J. Geophys. Res. 92, 14987-15001) and revisions suggested by Sromovsky et al. (Sromovsky, L.A., Fry, P.A., Kim, J.H. [2011]. Icarus 215, 292-312) that match these data best are those that assume a high abundance of methane in the deep atmosphere. However, none of these model profiles provides a satisfactory fit over the full spectral range sampled. This result could be the result of spatial differences between global and low-latitudinal regions, changes in time, missing continuum opacity sources such as stratospheric hazes or unknown tropospheric constituents, or undiagnosed systematic problems with either the Voyager radio-occultation or the Spitzer IRS data sets. The spectrum is compatible with the stratospheric temperatures derived from the Voyager ultraviolet occultations measurements by Herbert et al. (Herbert, F. et al. [1987]. J. Geophys. Res. 92, 15093-15109), but it is incompatible with the hot stratospheric temperatures derived from the same data by Stevens et al. (Stevens, M.H., Strobel, D.F., Herbert, F.H. [1993]. Icarus 101, 45-63). Thermospheric temperatures determined from the analysis of the observed H2 quadrupole emission features are colder than those derived by Herbert et al. at pressures less than ∼1 μbar. Extrapolation of the nominal model spectrum to far-infrared through millimeter wavelengths shows that the spectrum arising solely from H2

  20. Chemistry

    International Nuclear Information System (INIS)

    Ferris, L.M.

    1975-01-01

    The chemical research and development efforts related to the design and ultimate operation of molten-salt breeder reactor systems are concentrated on fuel- and coolant-salt chemistry, including the development of analytical methods for use in these systems. The chemistry of tellurium in fuel salt is being studied to help elucidate the role of this element in the intergranular cracking of Hastelloy N. Studies were continued of the effect of oxygen-containing species on the equilibrium between dissolved UF 3 and dissolved UF 4 , and, in some cases, between the dissolved uranium fluorides and graphite, and the UC 2 . Several aspects of coolant-salt chemistry are under investigation. Hydroxy and oxy compounds that could be formed in molten NaBF 4 are being synthesized and characterized. Studies of the chemistry of chromium (III) compounds in fluoroborate melts were continued as part of a systematic investigation of the corrosion of structural alloys by coolant salt. An in-line voltammetric method for determining U 4+ /U 3+ ratios in fuel salt was tested in a forced-convection loop over a six-month period. (LK)

  1. Observations of primary and secondary emissions in a B747 exhaust plume in the upper troposphere and inferred engine exit plane OH concentrations

    Energy Technology Data Exchange (ETDEWEB)

    Schlager, H; Schulte, P; Tremmel, H G; Ziereis, H [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Wessling (Germany). Inst. fuer Physik der Atmosphaere; Arnold, F; Droste-Franke, B; Klemm, M; Schneider, J [Max-Planck-Inst. fuer Kernphysik, Heidelberg (Germany)

    1998-12-31

    The speciation of NO{sub y} exhaust emissions in the near-field plume of a B747 cruising at 9.2 km was measured in situ using the DLR Falcon research aircraft instrumented with a chemical ionisation mass spectrometer of MPI-K and a chemiluminescence NO detector of DLR. In addition, CO{sub 2} was measured providing a dilution factor for the exhaust species. Observed maximum peak concentrations above background in the plume 60 s after emission were 25.4 ppmv (CO{sub 2}), 184 ppbv (NO), 2.6 ppbv (HNO{sub 2}), and 1.3 ppbv (HNO{sub 3}). The observations were used to infer the initial OH concentration (15.4 ppmv) and NO{sub 2}/NO{sub x} ratio (0.08) at the engine exit by back calculations using a chemistry box model. (author) 20 refs.

  2. Observations of primary and secondary emissions in a B747 exhaust plume in the upper troposphere and inferred engine exit plane OH concentrations

    Energy Technology Data Exchange (ETDEWEB)

    Schlager, H.; Schulte, P.; Tremmel, H.G.; Ziereis, H. [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Wessling (Germany). Inst. fuer Physik der Atmosphaere; Arnold, F.; Droste-Franke, B.; Klemm, M.; Schneider, J. [Max-Planck-Inst. fuer Kernphysik, Heidelberg (Germany)

    1997-12-31

    The speciation of NO{sub y} exhaust emissions in the near-field plume of a B747 cruising at 9.2 km was measured in situ using the DLR Falcon research aircraft instrumented with a chemical ionisation mass spectrometer of MPI-K and a chemiluminescence NO detector of DLR. In addition, CO{sub 2} was measured providing a dilution factor for the exhaust species. Observed maximum peak concentrations above background in the plume 60 s after emission were 25.4 ppmv (CO{sub 2}), 184 ppbv (NO), 2.6 ppbv (HNO{sub 2}), and 1.3 ppbv (HNO{sub 3}). The observations were used to infer the initial OH concentration (15.4 ppmv) and NO{sub 2}/NO{sub x} ratio (0.08) at the engine exit by back calculations using a chemistry box model. (author) 20 refs.

  3. Distribution of tropical tropospheric water vapor

    Science.gov (United States)

    Sun, De-Zheng; Lindzen, Richard S.

    1993-01-01

    Utilizing a conceptual model for tropical convection and observational data for water vapor, the maintenance of the vertical distribution of the tropical tropospheric water vapor is discussed. While deep convection induces large-scale subsidence that constrains the turbulent downgradient mixing to within the convective boundary layer and effectively dries the troposphere through downward advection, it also pumps hydrometeors into the upper troposphere, whose subsequent evaporation appears to be the major source of moisture for the large-scale subsiding motion. The development of upper-level clouds and precipitation from these clouds may also act to dry the outflow, thus explaining the low relative humidity near the tropopause. A one-dimensional model is developed to simulate the mean vertical structure of water vapor in the tropical troposphere. It is also shown that the horizontal variation of water vapor in the tropical troposphere above the trade-wind boundary layer can be explained by the variation of a moisture source that is proportional to the amount of upper-level clouds. Implications for the nature of water vapor feedback in global warming are discussed.

  4. 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.

  5. Determination of the Acid Dissociation Constant of a Phenolic Acid by High Performance Liquid Chromatography: An Experiment for the Upper Level Analytical Chemistry Laboratory

    Science.gov (United States)

    Raboh, Ghada

    2018-01-01

    A high performance liquid chromatography (HPLC) experiment for the upper level analytical chemistry laboratory is described. The students consider the effect of mobile-phase composition and pH on the retention times of ionizable compounds in order to determine the acid dissociation constant, K[subscript a], of a phenolic acid. Results are analyzed…

  6. Kinetics programs for simulation of tropospheric photochemistry on the global scale

    International Nuclear Information System (INIS)

    Elliott, S.; Kao, C.Y.J.; Turco, R.P.; Zhao, X.P.

    1993-08-01

    The study of tropospheric kinetics underlies global change because key greenhouse gases are photochemically active. Modeling of tropospheric chemistry on a global scale is essential because some indirect greenhouse gases are short-lived and interact in a non-linear fashion. It is also extremely challenging, however; the global change grid is extensive in both the physical and temporal domains, and critical lower atmospheric species include the organics and their oxidized derivatives, which are numerous. Several types of optimization may be incorporated into kinetics modules to enhance their ability to simulate the complete lower atmospheric gas phase chemical system. (1) The photochemical integrator can be accelerated by avoiding matrix and iterative solutions and by establishing families. Accuracy and mass conservation are sacrificed in the absence of iteration, but atom balancing is restorable post hoc. (2) Chemistry can be arranged upon the massive grid to exploit parallel processing, and solutions to its continuity equations can be automated to permit experimentation with species and reaction lists or family definitions. Costs in programming effort will be incurred in these cases. (3) Complex hydrocarbon decay sequences can be streamlined either through structural lumping methods descended from smog investigations, which require considerable calibration, or by defining surrogates for classes of compounds, with a loss in constituent detail. From among the available options, the most advantageous permutations will vary with the specific nature of any eventual global scale study, and there is likely to be demand for many approaches. Tracer transport codes serve as a foundation upon which tropospheric chemistry packages will be tested. Encroachment of the NO x sphere of influence upon tropical rain forests and the upper free troposphere are two examples of specific problems to which full three-dimensional chemical simulations might be applied

  7. Effects of elevated concentrations of atmospheric CO{sub 2} and tropospheric O{sub 3} on leaf litter production and chemistry in trembling aspen and paper birch communities

    Energy Technology Data Exchange (ETDEWEB)

    Liu, L.; King, J.S. [Michigan Technological Univ., Houghton, MI (United States). School of Forest Resources and Environmental Science; Giardina, C.P. [United States Dept. of Agriculture Forest Service, Houghton, MI (United States)

    2005-12-01

    This study examined the effects of elevated carbon dioxide (CO{sub 2}) and elevated ozone (O{sub 3}) on the quantity and timing of nutrient release to plants and on soil carbon formation rates, and how they are influenced by the combined change in litter quality and quantity. The changes in leaf litter in response to environmental changes was characterized in order to understand the influence of global change on forests. Free-air CO{sub 2} enrichment (FACE) technology was used to examine leaf litter production and biochemical input to soil in response to elevated CO{sub 2} and O{sub 3} treatments. The study involved collecting litter from aspen and birch-aspen communities that had been exposed to FACE and O{sub 3} treatments for 6 years. The hypothesis of growth differentiation balance was used as the basis to develop other hypotheses regarding litter chemistry responses to elevated levels of carbon dioxide and ozone. It was assumed that environmental factors that increase the net balance of plant carbon sources relative to growth sinks will increase the allocation of photosynthate to the production of carbon-based secondary compounds. Litter was analyzed for concentrations of carbon, nitrogen, soluble sugars, lipids, lignin, cellulose, hemicellulose and carbon-based defensive compounds such as soluble phenolics and condensed tannins. The study showed that high levels of ozone greatly increased litter concentrations of soluble sugars, soluble phenolics and condensed tannins, but there were no major effects of elevated carbon dioxide or elevated ozone on the concentrations of individual carbon structural carbon hydrates such as cellulose, hemicellulose and lignin. It was concluded that in the future, the inputs of nitrogen, soluble sugars, condensed tannins, soluble phenolics, cellulose and lignin to forest soils can change as a result of small changes in litter chemistry resulting from elevated CO{sub 2}, tropospheric O{sub 3}, and changes in litter biomass

  8. Effect of some climatic parameters on tropospheric and total ozone ...

    Indian Academy of Sciences (India)

    carbon, carbon monoxide, nitrogen dioxide, and sulphur dioxide) that are collected from India Meteo- rological Department .... and the upper troposphere is not only able to absorb ... lar traffic, thermal power plants, very busy ports, small and ...

  9. Chemistry

    International Nuclear Information System (INIS)

    Ferris, L.M.

    1976-01-01

    Research progress is reported in programs on fuel-salt chemistry, properties of compounds in the Li--Te system, Te spectroscopy UF 4 --H equilibria, porous electrode studies of molten salts, fuel salt-coolant salt reactions, thermodynamic properties of transition-metal fluorides, and properties of sodium fluoroborate. Developmental work on analytical methods is summarized including in-line analysis of molten MSBR fuel, analysis of coolant-salts for tritium, analysis of molten LiF--BeF 2 --ThF 4 for Fe and analysis of LiF--BeF--ThF 4 for Te

  10. Applications of Satellite Observations of Tropospheric Composition

    Science.gov (United States)

    Monks, Paul S.; Beirle, Steffen

    A striking feature of the field of tropospheric composition is the sheer number of chemical species that have been detected and measured with satellite instruments. The measurements have found application both in atmospheric chemistry itself, providing evidence, for example, of unexpected cryochemistry in the Arctic regions, and also in environmental monitoring with, for example, the observed growth in NO2 emissions over eastern Asia. Chapter 8 gives an overview of the utility of satellite observations for measuring tropospheric composition, dealing with each of the many compounds seen in detail. A comprehensive compound by compound table of the many studies performed is a most useful feature.

  11. Impact of climate variability on tropospheric ozone

    International Nuclear Information System (INIS)

    Grewe, Volker

    2007-01-01

    A simulation with the climate-chemistry model (CCM) E39/C is presented, which covers both the troposphere and stratosphere dynamics and chemistry during the period 1960 to 1999. Although the CCM, by its nature, is not exactly representing observed day-by-day meteorology, there is an overall model's tendency to correctly reproduce the variability pattern due to an inclusion of realistic external forcings, like observed sea surface temperatures (e.g. El Nino), major volcanic eruption, solar cycle, concentrations of greenhouse gases, and Quasi-Biennial Oscillation. Additionally, climate-chemistry interactions are included, like the impact of ozone, methane, and other species on radiation and dynamics, and the impact of dynamics on emissions (lightning). However, a number of important feedbacks are not yet included (e.g. feedbacks related to biogenic emissions and emissions due to biomass burning). The results show a good representation of the evolution of the stratospheric ozone layer, including the ozone hole, which plays an important role for the simulation of natural variability of tropospheric ozone. Anthropogenic NO x emissions are included with a step-wise linear trend for each sector, but no interannual variability is included. The application of a number of diagnostics (e.g. marked ozone tracers) allows the separation of the impact of various processes/emissions on tropospheric ozone and shows that the simulated Northern Hemisphere tropospheric ozone budget is not only dominated by nitrogen oxide emissions and other ozone pre-cursors, but also by changes of the stratospheric ozone budget and its flux into the troposphere, which tends to reduce the simulated positive trend in tropospheric ozone due to emissions from industry and traffic during the late 80s and early 90s. For tropical regions the variability in ozone is dominated by variability in lightning (related to ENSO) and stratosphere-troposphere exchange (related to Northern Hemisphere Stratospheric

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

    Science.gov (United States)

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

    1995-01-01

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

  13. Tropospheric VOC measurements by PTR-MS

    International Nuclear Information System (INIS)

    Hansel, A.; Wisthaler, A.; Graus, M.; Grabmer, W.

    2002-01-01

    Full text: O 3 is formed photochemically from the photolysis of NO 2 , and because O 3 reacts rapidly with NO these reactions result in a photoequilibrium between NO, NO 2 with no net formation or loss of O 3 , However, in the presence of volatile organic compounds (VOCs), the degradation reactions of VOCs lead to the formation of intermediate peroxy radicals which react with NO, converting NO to NO 2 , which then photolyze to form O 3 . Thus, in order to understand quantitatively tropospheric ozone chemistry, it is necessary to know the VOC distribution within the troposphere as well as VOC fluxes from individual sources. Examples will be presented how the use of Proton Transfer Reaction Mass Spectrometry (PTR-MS) has enhanced our understanding of anthropogenic VOC emissions, biosphere-atmosphere exchange processes, and photochemical processing of both anthropogenic and biogenic VOCs in the troposphere. (author)

  14. Evaluation of 1,3,5 trimethylbenzene degradation in the detailed tropospheric chemistry mechanism, MCMv3.1, using environmental chamber data

    Directory of Open Access Journals (Sweden)

    A. Metzger

    2008-11-01

    Full Text Available The degradation mechanism of 1,3,5-trimethyl- benzene (TMB as implemented in the Master Chemical Mechanism version 3.1 (MCM was evaluated using data from the environmental chamber at the Paul Scherrer Institute. The results show that the MCM provides a consistent description of the photo-oxidation of TMB/NOx mixtures for a range of conditions. In all cases the agreement between the measurement and the simulation decreases with decreasing VOC-NOx ratio and in addition with increasing precursor concentration. A significant underestimation of the decay rate of TMB and thus underestimation of reactivity in the system, consistent with results from previous appraisals of the MCM, was observed.

    Much higher nitrous acid (HONO concentrations compared to simulations and expected from chamber characterization experiments were measured during these smog chamber experiments. A light induced NO2 to HONO conversion at the chamber walls is suggested to occur. This photo-enhanced NO2 to HONO conversion with subsequent HONO photolysis enhances the reactivity of the system. After the implementation of this reaction in the model it describes the decay of TMB properly. Nevertheless, the model still over-predicts ozone at a later stage of the experiment. This can be attributed to a too slow removal of NO2. It is also shown that this photo-enhanced HONO formation is not restricted to TMB photo-oxidation but also occurs in other chemical systems (e.g. α-pinene. However, the influence of HONO as a source of OH radicals is less important in these more reactive systems and therefore the importance of the HONO chemistry is less obvious.

  15. Negative chlorine ion chemistry in the upper stratosphere and its application to an artificially created dense electron cloud

    Directory of Open Access Journals (Sweden)

    S. S. Prasad

    Full Text Available This paper discusses new potential reactions of chlorine-bearing anions (negative ions in the upper stratosphere. These reactions are then applied to the negative-ion chemistry following the injection of an electron cloud of very high density, of the order of 106-107 e- cm-3, in the 40-45-km region. The idea is to evaluate the recently proposed scheme to mitigate ozone depletion by converting the reactive chlorine atoms at these altitudes into Cl- ions which are unreactive towards ozone, i.e., electron scavenging of Cl. We find that the previously neglected photodetachment from Cl- is fast. For an overhead sun, this process may have a rate coefficient of 0.08 s-1 when multiple scattering is included. The rate could be even higher, depending on the ground albedo. Switching reaction between Cl-·H2O and HCl might lead to the formation of Cl-·HCl anion. Possible reactions of Cl-·H2O and Cl-·HCl with O atoms could produce ClO- and Cl-2. The production of ClO- in this manner is significant because Cl- having a high photodetachment rate constant would be regenerated in the very likely reactions of ClO- with O. When these possibilities are considered, then it is found that the chlorine anions may not be the major ions inside the electron cloud due to the rapid photodetachment from Cl-. Furthermore, in such a cloud, there may be the hazard that the Cl--Cl-·H2O-ClO--Cl- cycle amounts to catalytic destruction of two O atoms. Thus, the scheme could be risky if practised in the altitude region where atomic oxygen is an important constituent. Similar conclusions apply even if the ClO- species forms ClO-3 by three-body association with O2

  16. Negative chlorine ion chemistry in the upper stratosphere and its application to an artificially created dense electron cloud

    Directory of Open Access Journals (Sweden)

    S. S. Prasad

    1995-03-01

    Full Text Available This paper discusses new potential reactions of chlorine-bearing anions (negative ions in the upper stratosphere. These reactions are then applied to the negative-ion chemistry following the injection of an electron cloud of very high density, of the order of 106-107 e- cm-3, in the 40-45-km region. The idea is to evaluate the recently proposed scheme to mitigate ozone depletion by converting the reactive chlorine atoms at these altitudes into Cl- ions which are unreactive towards ozone, i.e., electron scavenging of Cl. We find that the previously neglected photodetachment from Cl- is fast. For an overhead sun, this process may have a rate coefficient of 0.08 s-1 when multiple scattering is included. The rate could be even higher, depending on the ground albedo. Switching reaction between Cl-·H2O and HCl might lead to the formation of Cl-·HCl anion. Possible reactions of Cl-·H2O and Cl-·HCl with O atoms could produce ClO- and Cl-2. The production of ClO- in this manner is significant because Cl- having a high photodetachment rate constant would be regenerated in the very likely reactions of ClO- with O. When these possibilities are considered, then it is found that the chlorine anions may not be the major ions inside the electron cloud due to the rapid photodetachment from Cl-. Furthermore, in such a cloud, there may be the hazard that the Cl--Cl-·H2O-ClO--Cl- cycle amounts to catalytic destruction of two O atoms. Thus, the scheme could be risky if practised in the altitude region where atomic oxygen is an important constituent. Similar conclusions apply even if the ClO- species forms ClO-3 by three-body association with O2, instead of reacting with O. It must be emphasized that the present study is speculative at this time, because none of the relevant reactions have been investigated in the laboratory as yet. Nevertheless, it is very safe to say that the scheme of ozone preservation by electron scavenging of the upper stratospheric Cl is

  17. Chemistry

    International Nuclear Information System (INIS)

    Ferris, L.M.

    1975-01-01

    Research and development activities dealing with the chemical problems related to design and ultimate operation of molten-salt reactor systems are described. An experimental test stand was constructed to expose metallurgical test specimens to Te 2 vapor at defined temperatures and deposition rates. To better define the chemistry of fluoroborate coolant, several aspects are being investigated. The behavior of hydroxy and oxy compounds in molten NaBF 4 is being investigated to define reactions and compounds that may be involved in corrosion and/or could be involved in methods for trapping tritium. Two corrosion products of Hastelloy N, Na 3 CrF 6 and Na 5 Cr 3 F 14 , were identified from fluoroborate systems. The evaluation of fluoroborate and alternate coolants continued. Research on the behavior of hydrogen and its isotopes is summarized. The solubilities of hydrogen, deuterium, and helium in Li 2 BeF 4 are very low. The sorption of tritium on graphite was found to be significant (a few milligrams of tritium per kilogram of graphite), possibly providing a means of sequestering a portion of the tritium produced. Development of analytical methods continued with emphasis on voltammetric and spectrophotometric techniques for the in-line analysis of corrosion products such as Fe 2+ and Cr 3+ and the determination of the U 3+ /U 4+ ratio in MSBR fuel salt. Similar studies were conducted with the NaBF 4 --NaF coolant salt. Information developed during the previous operation of the CSTF has been assessed and used to formulate plans for evaluation of in-line analytical methods in future CSTF operations. Electroanalytical and spectrophotometric research suggests that an electroactive protonic species is present in molten NaBF 4 --NaF, and that this species rapidly equilibrates with a volatile proton-containing species. Data obtained from the CSTF indicated that tritium was concentrated in the volatile species. (JGB)

  18. 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

  19. UPPER TROPOSPHERIC ND STR TOSPHERIC OZONE OVER ...

    African Journals Online (AJOL)

    USER

    2015-03-26

    Mar 26, 2015 ... site free of anthropogenic emissions, can be representative ... et al., 2009).The reduction in production of ... over Nairobi are small, light instruments attached on a .... pollutants from the city of Nairobi. The ... transport. Figure 9 ...

  20. Uncertainty in the Future Distribution of Tropospheric Ozone over West Africa due to Variability in Anthropogenic Emissions Estimates between 2025 and 2050

    Directory of Open Access Journals (Sweden)

    J. E. Williams

    2011-01-01

    Full Text Available Particle and trace gas emissions due to anthropogenic activity are expected to increase significantly in West Africa over the next few decades due to rising population and more energy intensive lifestyles. Here we perform 3D global chemistry-transport model calculations for 2025 and 2050 using both a “business-as-usual” (A1B and “clean economy” (B1 future anthropogenic emission scenario to focus on the changes in the distribution and uncertainties associated with tropospheric O3 due to the various projected emission scenarios. When compared to the present-day troposphere we find that there are significant increases in tropospheric O3 for the A1B emission scenario, with the largest increases being located in the lower troposphere near the source regions and into the Sahel around 15–20°N. In part this increase is due to more efficient NOx re-cycling related to increases in the background methane concentrations. Examining the uncertainty across different emission inventories reveals that there is an associated uncertainty of up to ~20% in the predicted increases at 2025 and 2050. For the upper troposphere, where increases in O3 have a more pronounced impact on radiative forcing, the uncertainty is influenced by transport of O3 rich air from Asia on the Tropical Easterly Jet.

  1. Sulfate Aerosols from Non-Explosive Volcanoes: Chemical-Radiative Effects in the Troposphere and Lower Stratosphere

    Directory of Open Access Journals (Sweden)

    Giovanni Pitari

    2016-06-01

    Full Text Available SO2 and H2S are the two most important gas-phase sulfur species emitted by volcanoes, with a global amount from non-explosive emissions of the order 10 Tg-S/yr. These gases are readily oxidized forming SO42− aerosols, which effectively scatter the incoming solar radiation and cool the surface. They also perturb atmospheric chemistry by enhancing the NOx to HNO3 heterogeneous conversion via hydrolysis on the aerosol surface of N2O5 and Br-Cl nitrates. This reduces formation of tropospheric O3 and the OH to HO2 ratio, thus limiting the oxidation of CH4 and increasing its lifetime. In addition to this tropospheric chemistry perturbation, there is also an impact on the NOx heterogeneous chemistry in the lower stratosphere, due to vertical transport of volcanic SO2 up to the tropical tropopause layer. Furthermore, the stratospheric O3 formation and loss, as well as the NOx budget, may be slightly affected by the additional amount of upward diffused solar radiation and consequent increase of photolysis rates. Two multi-decadal time-slice runs of a climate-chemistry-aerosol model have been designed for studying these chemical-radiative effects. A tropopause mean global net radiative flux change (RF of −0.23 W·m−2 is calculated (including direct and indirect aerosol effects with a 14% increase of the global mean sulfate aerosol optical depth. A 5–15 ppt NOx decrease is found in the mid-troposphere subtropics and mid-latitudes and also from pole to pole in the lower stratosphere. The tropospheric NOx perturbation triggers a column O3 decrease of 0.5–1.5 DU and a 1.1% increase of the CH4 lifetime. The surface cooling induced by solar radiation scattering by the volcanic aerosols induces a tropospheric stabilization with reduced updraft velocities that produce ice supersaturation conditions in the upper troposphere. A global mean 0.9% decrease of the cirrus ice optical depth is calculated with an indirect RF of −0.08 W·m−2.

  2. Sensitivity of stomatal conductance to soil moisture: implications for tropospheric ozone

    Directory of Open Access Journals (Sweden)

    A. Anav

    2018-04-01

    Full Text Available Soil moisture and water stress play a pivotal role in regulating stomatal behaviour of plants; however, in the last decade, the role of water availability has often been neglected in atmospheric chemistry modelling studies as well as in integrated risk assessments, despite the fact that plants remove a large amount of atmospheric compounds from the lower troposphere through stomata. The main aim of this study is to evaluate, within the chemistry transport model CHIMERE, the effect of soil water limitation on stomatal conductance and assess the resulting changes in atmospheric chemistry testing various hypotheses of water uptake by plants in the rooting zone. Results highlight how dry deposition significantly declines when soil moisture is used to regulate the stomatal opening, mainly in the semi-arid environments: in particular, over Europe the amount of ozone removed by dry deposition in one year without considering any soil water limitation to stomatal conductance is about 8.5 TgO3, while using a dynamic layer that ensures that plants maximize the water uptake from soil, we found a reduction of about 10 % in the amount of ozone removed by dry deposition ( ∼  7.7 TgO3. Although dry deposition occurs from the top of canopy to ground level, it affects the concentration of gases remaining in the lower atmosphere, with a significant impact on ozone concentration (up to 4 ppb extending from the surface to the upper troposphere (up to 650 hPa. Our results shed light on the importance of improving the parameterizations of processes occurring at plant level (i.e. from the soil to the canopy as they have significant implications for concentration of gases in the lower troposphere and resulting risk assessments for vegetation or human health.

  3. Sensitivity of stomatal conductance to soil moisture: implications for tropospheric ozone

    Science.gov (United States)

    Anav, Alessandro; Proietti, Chiara; Menut, Laurent; Carnicelli, Stefano; De Marco, Alessandra; Paoletti, Elena

    2018-04-01

    Soil moisture and water stress play a pivotal role in regulating stomatal behaviour of plants; however, in the last decade, the role of water availability has often been neglected in atmospheric chemistry modelling studies as well as in integrated risk assessments, despite the fact that plants remove a large amount of atmospheric compounds from the lower troposphere through stomata. The main aim of this study is to evaluate, within the chemistry transport model CHIMERE, the effect of soil water limitation on stomatal conductance and assess the resulting changes in atmospheric chemistry testing various hypotheses of water uptake by plants in the rooting zone. Results highlight how dry deposition significantly declines when soil moisture is used to regulate the stomatal opening, mainly in the semi-arid environments: in particular, over Europe the amount of ozone removed by dry deposition in one year without considering any soil water limitation to stomatal conductance is about 8.5 TgO3, while using a dynamic layer that ensures that plants maximize the water uptake from soil, we found a reduction of about 10 % in the amount of ozone removed by dry deposition ( ˜ 7.7 TgO3). Although dry deposition occurs from the top of canopy to ground level, it affects the concentration of gases remaining in the lower atmosphere, with a significant impact on ozone concentration (up to 4 ppb) extending from the surface to the upper troposphere (up to 650 hPa). Our results shed light on the importance of improving the parameterizations of processes occurring at plant level (i.e. from the soil to the canopy) as they have significant implications for concentration of gases in the lower troposphere and resulting risk assessments for vegetation or human health.

  4. Interpretation of TOMS Observations of Tropical Tropospheric Ozone with a Global Model and In Situ Observations

    Science.gov (United States)

    Martin, Randall V.; Jacob, Daniel J.; Logan, Jennifer A.; Bey, Isabelle; Yantosca, Robert M.; Staudt, Amanda C.; Fiore, Arlene M.; Duncan, Bryan N.; Liu, Hongyu; Ginoux, Paul

    2004-01-01

    We interpret the distribution of tropical tropospheric ozone columns (TTOCs) from the Total Ozone Mapping Spectrometer (TOMS) by using a global three-dimensional model of tropospheric chemistry (GEOS-CHEM) and additional information from in situ observations. The GEOS-CHEM TTOCs capture 44% of the variance of monthly mean TOMS TTOCs from the convective cloud differential method (CCD) with no global bias. Major discrepancies are found over northern Africa and south Asia where the TOMS TTOCs do not capture the seasonal enhancements from biomass burning found in the model and in aircraft observations. A characteristic feature of these northern topical enhancements, in contrast to southern tropical enhancements, is that they are driven by the lower troposphere where the sensitivity of TOMS is poor due to Rayleigh scattering. We develop an efficiency correction to the TOMS retrieval algorithm that accounts for the variability of ozone in the lower troposphere. This efficiency correction increases TTOC's over biomass burning regions by 3-5 Dobson units (DU) and decreases them by 2-5 DU over oceanic regions, improving the agreement between CCD TTOCs and in situ observations. Applying the correction to CCD TTOCs reduces by approximately DU the magnitude of the "tropical Atlantic paradox" [Thompson et al, 2000], i.e. the presence of a TTOC enhancement over the southern tropical Atlantic during the northern African biomass burning season in December-February. We reproduce the remainder of the paradox in the model and explain it by the combination of upper tropospheric ozone production from lightning NOx, peristent subsidence over the southern tropical Atlantic as part of the Walker circulation, and cross-equatorial transport of upper tropospheric ozone from northern midlatitudes in the African "westerly duct." These processes in the model can also account for the observed 13-17 DU persistent wave-1 pattern in TTOCs with a maximum above the tropical Atlantic and a minimum

  5. Tropospheric Ozone and Photochemical Smog

    Science.gov (United States)

    Sillman, S.

    2003-12-01

    emitted species, in a process that is driven by sunlight and is accelerated by warm temperatures. This smog is largely the product of gasoline-powered engines (especially automobiles), although coal-fired industry can also generate photochemical smog. The process of photochemical smog formation was first identified by Haagen-Smit and Fox (1954) in association with Los Angeles, a city whose geography makes it particularly susceptible to this type of smog formation. Sulfate aerosols and organic particulates are often produced concurrently with ozone, giving rise to a characteristic milky-white haze associated with this type of air pollution.Today ozone and particulates are recognized as the air pollutants that are most likely to affect human health adversely. In the United States, most major metropolitan areas have periodic air pollution events with ozone in excess of government health standards. Violations of local health standards also occur in major cities in Canada and in much of Europe. Other cities around the world (especially Mexico City) also experience very high ozone levels. In addition to urban-scale events, elevated ozone occurs in region-wide events in the eastern USA and in Western Europe, with excess ozone extending over areas of 1,000 km2 or more. Ozone plumes of similar extent are found in the tropics (especially in Central Africa) at times of high biomass burning (e.g., Jenkins et al., 1997; Chatfield et al., 1998). In some cases ozone associated with biomass burning has been identified at distances up to 104 km from its sources (Schultz et al., 1999).Ozone also has a significant impact on the global troposphere, and ozone chemistry is a major component of global tropospheric chemistry. Global background ozone concentrations are much lower than urban or regional concentrations during pollution events, but there is evidence that the global background has increased as a result of human activities (e.g., Wang and Jacob, 1998; Volz and Kley, 1988). A rise in

  6. Impact of the new HNO3-forming channel of the HO2+NO reaction on tropospheric HNO3, NOx, HOx and ozone

    Directory of Open Access Journals (Sweden)

    A. Kukui

    2008-07-01

    Full Text Available We have studied the impact of the recently observed reaction NO+HO2→HNO3 on atmospheric chemistry. A pressure and temperature-dependent parameterisation of this minor channel of the NO+HO2→NO2+OH reaction has been included in both a 2-D stratosphere-troposphere model and a 3-D tropospheric chemical transport model (CTM. Significant effects on the nitrogen species and hydroxyl radical concentrations are found throughout the troposphere, with the largest percentage changes occurring in the tropical upper troposphere (UT. Including the reaction leads to a reduction in NOx everywhere in the troposphere, with the largest decrease of 25% in the tropical and Southern Hemisphere UT. The tropical UT also has a corresponding large increase in HNO3 of 25%. OH decreases throughout the troposphere with the largest reduction of over 20% in the tropical UT. The mean global decrease in OH is around 13%, which is very large compared to the impact that typical photochemical revisions have on this modelled quantity. This OH decrease leads to an increase in CH4 lifetime of 5%. Due to the impact of decreased NOx on the OH:HO2 partitioning, modelled HO2 actually increases in the tropical UT on including the new reaction. The impact on tropospheric ozone is a decrease in the range 5 to 12%, with the largest impact in the tropics and Southern Hemisphere. Comparison with observations shows that in the region of largest changes, i.e. the tropical UT, the inclusion of the new reaction tends to degrade the model agreement. Elsewhere the model comparisons are not able to critically assess the impact of including this reaction. Only small changes are calculated in the minor species distributions in the stratosphere.

  7. Test of numerical methods for the integration of kinetic equations in tropospheric chemistry; Confronto di metodi numerici per l'integrazione di sistemi di equazioni differenziali ordinarie di tipo STIFF inserite nel modello fotochimico Calgrid

    Energy Technology Data Exchange (ETDEWEB)

    Lorenzini, R.; Passoni, L. [ENEA, Centro Ricerche Ezio Clementel, Bologna (Italy). Dipt. Ambiente

    1999-07-01

    The integration of ordinary differential equations systems (ODEs) is of significant concern to tropospheric and stratospheric chemistry modelers. The solution of the ODEs requires a large computational effort because of their stiff nature; in a three-dimensional photochemical model the solution of the ODEs required at least 70% of the total CPU time. Several numerical integration techniques exist which attempt to provide accurate and computationally efficient solutions. In this work it is presented a comparison of some of the techniques in terms of solution accuracy and required computational time. It has been compared the Hybrid Solver (Young and Boris, 1977), the Quasi Steady-State Approximation method (Hesstvedt et al., 1978) and the Chemical Solver for Ordinary Differential Equations (Aro, 1996), by using the CALGRID photochemical model. The accuracy is evaluated by comparing the results of every method with the solutions obtained by the Livermore Solver for Ordinary Differential Equations (Hindmarsh, 1980). The comparison has been made varing the parameters of the error tolerances, and taking into account the trade-off between solution accuracy and computational efficiency. [Italian] L'integrazione di sistemi di equazioni differenziali ordinarie (ODEs), e' un problema significativo per i modellisti della chimica troposferica e stratosferica. A causa della loro natura stiff la soluzione degli ODEs richiese un notevole sforzo computazionale; in un modello fotochimico tridimensionale la soluzione degli ODEs richiede almeno il 70% del tempo totale di CPU. Esistono diverse tecniche di integrazione numerica che possono fornire soluzioni accurate e computazionalmente efficienti: in questo lavoro presentiamo un confronto fra alcune tecniche in termini di accuratezza della soluzione e tempo computazionale richiesto. Si sono confrontati il Solver Ibrido (Young and Boris, 1977), il metodo Quasi Steady-State Approximation (Hesstvedt et al., 1978) ed il Chemical

  8. Characteristics of intercontinental transport of tropospheric ozone from Africa to Asia

    Science.gov (United States)

    Han, Han; Liu, Jane; Yuan, Huiling; Zhuang, Bingliang; Zhu, Ye; Wu, Yue; Yan, Yuhan; Ding, Aijun

    2018-03-01

    In this study, we characterize the transport of ozone from Africa to Asia through the analysis of the simulations of a global chemical transport model, GEOS-Chem, from 1987 to 2006. The receptor region Asia is defined within 5-60° N and 60-145° E, while the source region Africa is within 35° S-15° N and 20° W-55° E and within 15-35° N and 20° W-30° E. The ozone generated in the African troposphere from both natural and anthropogenic sources is tracked through tagged ozone simulation. Combining this with analysis of trajectory simulations using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, we find that the upper branch of the Hadley cell connects with the subtropical westerlies in the Northern Hemisphere (NH) to form a primary transport pathway from Africa to Asia in the middle and upper troposphere throughout the year. The Somali jet that runs from eastern Africa near the equator to the Indian subcontinent in the lower troposphere is the second pathway that appears only in NH summer. The influence of African ozone mainly appears over Asia south of 40° N. The influence shows strong seasonality, varying with latitude, longitude, and altitude. In the Asian upper troposphere, imported African ozone is largest from March to May around 30° N (12-16 ppbv) and lowest during July-October around 10° N ( ˜ 2 ppbv). In the Asian middle and lower troposphere, imported African ozone peaks in NH winter between 20 and 25° N. Over 5-40° N, the mean fractional contribution of imported African ozone to the overall ozone concentrations in Asia is largest during NH winter in the middle troposphere ( ˜ 18 %) and lowest in NH summer throughout the tropospheric column ( ˜ 6 %). This seasonality mainly results from the collective effects of the ozone precursor emissions in Africa and meteorology and chemistry in Africa, in Asia and along the transport pathways. The seasonal swing of the Hadley circulation and subtropical westerlies along the

  9. The influence of biogenic emissions from Africa on tropical tropospheric ozone during 2006: a global modeling study

    Directory of Open Access Journals (Sweden)

    J. E. Williams

    2009-08-01

    Full Text Available We have performed simulations using a 3-D global chemistry-transport model to investigate the influence that biogenic emissions from the African continent exert on the composition of the troposphere in the tropical region. For this purpose we have applied two recently developed biogenic emission inventories provided for use in large-scale global models (Granier et al., 2005; Lathière et al., 2006 whose seasonality and temporal distribution for biogenic emissions of isoprene, other volatile organic compounds and NO is markedly different. The use of the 12 year average values for biogenic emissions provided by Lathière et al. (2006 results in an increase in the amount of nitrogen sequestrated into longer lived reservoir compounds which contributes to the reduction in the tropospheric ozone burden in the tropics. The associated re-partitioning of nitrogen between PAN, HNO3 and organic nitrates also results in a ~5% increase in the loss of nitrogen by wet deposition. At a global scale there is a reduction in the oxidizing capacity of the model atmosphere which increases the atmospheric lifetimes of CH4 and CO by ~1.5% and ~4%, respectively. Comparisons against a range of different measurements indicate that applying the 12 year average of Lathière et al. (2006 improves the performance of TM4_AMMA for 2006 in the tropics. By the use of sensitivity studies we show that the release of NO from soils in Africa accounts for between ~2–45% of tropospheric ozone in the African troposphere, ~10% in the upper troposphere and between ~5–20% of the tropical tropospheric ozone column over the tropical Atlantic Ocean. The subsequent reduction in OH over the source regions allows enhanced transport of CO out of the region. For biogenic volatile organic C1 to C3 species released from Africa, the effects on tropical tropospheric ozone are rather limited, although this source contributes to the global burden of VOC by between ~2–4% and

  10. A model study of ozone in the eastern Mediterranean free troposphere during MINOS (August 2001)

    NARCIS (Netherlands)

    Roelofs, GJ; Scheeren, HA; Heland, J; Ziereis, H; Lelieveld, J

    2003-01-01

    A coupled tropospheric chemistry-climate model is used to analyze tropospheric ozone distributions observed during the MINOS campaign in the eastern Mediterranean region ( August, 2001). Modeled ozone profiles are generally in good agreement with the observations. Our analysis shows that the

  11. Stratosphere-troposphere exchange in a summertime extratropical low: analysis

    Directory of Open Access Journals (Sweden)

    J. Brioude

    2006-01-01

    Full Text Available Ozone and carbon monoxide measurements sampled during two commercial flights in airstreams of a summertime midlatitude cyclone are analysed with a Lagrangian-based study (backward trajectories and a Reverse Domain Filling technique to gain a comprehensive understanding of transport effects on trace gas distributions. The study demonstrates that summertime cyclones can be associated with deep stratosphere-troposphere transport. A tropopause fold is sampled twice in its life cycle, once in the lower troposphere (O3≃100 ppbv; CO≃90 ppbv in the dry airstream of the cyclone, and again in the upper troposphere (O3≃200 ppbv; CO≃90 ppbv on the northern side of the large scale potential vorticity feature associated with baroclinic development. In agreement with the maritime development of the cyclone, the chemical composition of the anticyclonic portion of the warm conveyor belt outflow (O3≃40 ppbv; CO≃85 ppbv corresponds to the lowest mixing ratios of both ozone and carbon monoxide in the upper tropospheric airborne observations. The uncertain degree of confidence of the Lagrangian-based technique applied to a 100 km segment of upper level airborne observations with high ozone (200 ppbv and relatively low CO (80 ppbv observed northwest of the cyclone prevents identification of the ozone enrichment process of air parcels embedded in the cyclonic part of the upper level outflow of the warm conveyor belt. Different hypotheses of stratosphere-troposphere exchange are discussed.

  12. Surface-Enhanced Resonance Raman Scattering and Visible Extinction Spectroscopy of Copper Chlorophyllin: An Upper Level Chemistry Experiment

    Science.gov (United States)

    Schnitzer, Cheryl S.; Reim, Candace Lawson; Sirois, John J.; House, Paul G.

    2010-01-01

    Advanced chemistry students are introduced to surface-enhanced resonance Raman scattering (SERRS) by studying how sodium copper chlorophyllin (CuChl) adsorbs onto silver colloids (CuChl/Ag) as a function of pH. Using both SERRS and visible extinction spectroscopy, the extent of CuChl adsorption and colloidal aggregation are monitored. Initially at…

  13. Tropospheric Emissions: Monitoring of Pollution (TEMPO)

    Science.gov (United States)

    Zoogman, P.; Liu, X.; Suleiman, R. M.; Pennington, W. F.; Flittner, D. E.; Al-Saadi, J. A.; Hilton, B. B.; Nicks, D. K.; Newchurch, M. J.; Carr, J. L.; hide

    2016-01-01

    TEMPO (Tropospheric Emissions: Monitoring of Pollution) was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021. It will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO observes from Mexico City, Cuba, and the Bahamas to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution (approximately 2.1 kilometers N/S by 4.4 kilometers E/W at 36.5 degrees N, 100 degrees W). TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry, as well as contributing to carbon cycle knowledge. Measurements are made hourly from geostationary (GEO) orbit, to capture the high variability present in the diurnal cycle of emissions and chemistry that are unobservable from current low-Earth orbit (LEO) satellites that measure once per day. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a commercial GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve ozone (O3), nitrogen dioxide (NO2), sulfur dioxide (SO2), formaldehyde (H2CO), glyoxal (C2H2O2), bromine monoxide (BrO), IO (iodine monoxide),water vapor, aerosols, cloud parameters, ultraviolet radiation, and foliage properties. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions. TEMPO quantifies and tracks the evolution of aerosol loading. It provides these near-real-time air quality products that will be made publicly available. TEMPO will launch at a prime time to be the

  14. Tropospheric Emissions: Monitoring of Pollution (TEMPO)

    Science.gov (United States)

    Chance, Kelly; Liu, Xiong; Suleiman, Raid M.; Flittner, David E.; Al-Saadi, Jassim; Janz, Scott J.

    2014-06-01

    TEMPO, selected by NASA as the first Earth Venture Instrument, will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO measures from Mexico City to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution. TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry. Measurements are from geostationary (GEO) orbit, to capture the inherent high variability in the diurnal cycle of emissions and chemistry. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a GEO host spacecraft to provide a modest-cost mission that measures the spectra required to retrieve O3, NO2, SO2, H2CO, C2H2O2, H2O, aerosols, cloud parameters, and UVB radiation. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, reducing uncertainty in air quality predictions by 50 %. TEMPO quantifies and tracks the evolution of aerosol loading. It provides near-real-time air quality products that will be made widely, publicly available. TEMPO makes the first tropospheric trace gas measurements from GEO, by building on the heritage of five spectrometers flown in low-earth-orbit (LEO). These LEO instruments measure the needed spectra, although at coarse spatial and temporal resolutions, to the precisions required for TEMPO and use retrieval algorithms developed for them by TEMPO Science Team members and currently running in operational environments. This makes TEMPO an innovative use of a well-proven technique, able to produce a revolutionary data set. TEMPO provides much of the atmospheric measurement

  15. New capability for ozone dial profiling measurements in the troposphere and lower stratosphere from aircraft

    Science.gov (United States)

    Hair, Johnathan; Hostetler, Chris; Cook, Anthony; Harper, David; Notari, Anthony; Fenn, Marta; Newchurch, Mike; Wang, Lihua; Kuang, Shi; Knepp, Travis; Burton, Sharon; Ferrare, Richard; Butler, Carolyn; Collins, Jim; Nehrir, Amin

    2018-04-01

    Recently, we successfully demonstrated a new compact and robust ozone DIAL lidar for smaller aircraft such as the NASA B200 and the ER-2 high-altitude aircraft. This is the first NASA airborne lidar to incorporate advanced solid-state lasers to produce the required power at the required ultraviolet wavelengths, and is compact and robust enough to operate nearly autonomously on the high-altitude ER-2 aircraft. This technology development resulted in the first new NASA airborne ozone DIAL instrument in more than 15 years. The combined ozone, aerosol, and clouds measurements provide valuable information on the chemistry, radiation, and dynamics of the atmosphere. In particular, from the ER-2 it offers a unique capability to study the upper troposphere and lower stratosphere.

  16. New capability for ozone dial profiling measurements in the troposphere and lower stratosphere from aircraft

    Directory of Open Access Journals (Sweden)

    Hair Johnathan

    2018-01-01

    Full Text Available Recently, we successfully demonstrated a new compact and robust ozone DIAL lidar for smaller aircraft such as the NASA B200 and the ER-2 high-altitude aircraft. This is the first NASA airborne lidar to incorporate advanced solid-state lasers to produce the required power at the required ultraviolet wavelengths, and is compact and robust enough to operate nearly autonomously on the high-altitude ER-2 aircraft. This technology development resulted in the first new NASA airborne ozone DIAL instrument in more than 15 years. The combined ozone, aerosol, and clouds measurements provide valuable information on the chemistry, radiation, and dynamics of the atmosphere. In particular, from the ER-2 it offers a unique capability to study the upper troposphere and lower stratosphere.

  17. Impact of NO2 Profile Shape in OMI Tropospheric NO2 Retrievals

    Science.gov (United States)

    Lamsal, Lok; Krotkov, Nickolay A.; Pickering, K.; Schwartz, W. H.; Celarier, E. A.; Bucsela, E. J.; Gleason, J. F.; Philip, S.; Nowlan, C.; Martin, R. V.; hide

    2013-01-01

    Nitrogen oxides (NOx NO + NO2) are key actors in air quality and climate change. Tropospheric NO2 columns from the nadir-viewing satellite sensors have been widely used to understand sources and chemistry of NOx. We have implemented several improvements to the operational algorithm developed at NASA GSFC and retrieved tropospheric NO2 columns. We present tropospheric NO2 validation studies of the new OMI Standard Product version 2.1 using ground-based and in-situ aircraft measurements. We show how vertical profile of scattering weight and a-priori NO2 profile shapes, which are taken from chemistry-transport models, affect air mass factor (AMF) and therefore tropospheric NO2 retrievals. Users can take advantage of scattering weights information that is made available in the operational NO2 product. Improved tropospheric NO2 data retrieved using thoroughly evaluated high spatial resolution NO2 profiles are helpful to test models.

  18. Evaluation of the Cloud Fields in the UK Met Office HadGEM3-UKCA Model Using the CCCM Satellite Data Product to Advance Our Understanding of the Influence of Clouds on Tropospheric Composition and Chemistry

    Science.gov (United States)

    Varma, Sunil; Voulgarakis, Apostolos; Liu, Hongyu; Crawford, James H.; White, James

    2016-01-01

    To determine the role of clouds in driving inter-annual and inter-seasonal variability of trace gases in the troposphere and lower stratosphere with a particular focus on the importance of cloud modification of photolysis. To evaluate the cloud fields and their vertical distribution in the HadGEM3 model utilizing CCCM, a unique 3-D cloud data product merged from multiple A-Train satellites (CERES, CloudSat, CALIPSO, and MODIS) developed at the NASA Langley Research Center.

  19. Tropospheric ozone trend over Beijing from 2002–2010: ozonesonde measurements and modeling analysis

    Directory of Open Access Journals (Sweden)

    Y. Wang

    2012-09-01

    Full Text Available Using a combination of ozonesonde data and numerical simulations of the Chemical Lagrangian Model of the Stratosphere (CLaMS, the trend of tropospheric ozone (O3 during 2002–2010 over Beijing was investigated. Tropospheric ozone over Beijing shows a winter minimum and a broad summer maximum with a clear positive trend in the maximum summer ozone concentration over the last decade. The observed significant trend of tropospheric column ozone is mainly caused by photochemical production (3.1% yr−1 for a mean level of 52 DU. This trend is close to the significant trend of partial column ozone in the lower troposphere (0–3 km resulting from the enhanced photochemical production during summer (3.0% yr−1 for a mean level of 23 DU. Analysis of the CLaMS simulation shows that transport rather than chemistry drives most of the seasonality of tropospheric ozone. However, dynamical processes alone cannot explain the trend of tropospheric ozone in the observational data. Clearly enhanced ozone values and a negative vertical ozone gradient in the lower troposphere in the observational data emphasize the importance of photochemistry within the troposphere during spring and summer, and suggest that the photochemistry within the troposphere significantly contributes to the tropospheric ozone trend over Beijing during the last decade.

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

    International Nuclear Information System (INIS)

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

    2009-01-01

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

  1. Airborne measurement of peroxy radicals in the lower troposphere

    Science.gov (United States)

    Andrés Hernández, Maria Dolores; Horstjann, Markus; Kartal, Deniz; Krebsbach, Marc; Linke, Christian; Lichtenstern, Michael; Andrey, Javier; Burrows, John P.

    2013-04-01

    The importance of peroxy radicals in the tropospheric chemistry is well recognized in the scientific literature. Hydroxy- and organic peroxy radicals (HO2 and RO2, R being an organic chain) are key intermediates in the OH radical initiated oxidation of CO and SO2, of volatile organic compounds (VOC), in the ozonolysis of alkenes and photo-oxidation of carbonyl species. Peroxy radicals are responsible for the ozone production in the troposphere, the formation of peroxides and other oxidants. Although radical chemistry in the troposphere has been subject of intensive research in the past three decades, it is still very few known about the vertical distribution of peroxy radicals. Airborne observations are scarce in spite of their particular importance to improve the understanding of the tropospheric chemistry and the oxidising capacity of the atmosphere at different altitudes. In situ trace gas measurements were carried out in summer 2010 on board of the INTA (Instituto Nacional de Técnicas Aeroespaciales) C212 aircraft over Spain in the frame of the EUFAR project VERDRILLT (VERtical Distribution of Radicals In the Lower Layers of the Troposphere), and in cooperation with the DLR (Deutsches Zentrum für Luft- und Raumfahrt), the University of Wuppertal, the CEAM (Centro de Estudios Ambientales del Mediterráneo) and the UPV-EHU University in Bilbao. VERDRILLT aimed at getting a deeper understanding of the vertical distribution of peroxy radicals in the lower layers of the troposphere. Measurements were taken over urban areas and extensions of different vegetation under meteorological conditions favouring active photochemistry and convection from the ground into close atmospheric layers. Results and main findings will be presented and discussed.

  2. Tropospheric emissions: Monitoring of pollution (TEMPO)

    Science.gov (United States)

    Zoogman, P.; Liu, X.; Suleiman, R. M.; Pennington, W. F.; Flittner, D. E.; Al-Saadi, J. A.; Hilton, B. B.; Nicks, D. K.; Newchurch, M. J.; Carr, J. L.; Janz, S. J.; Andraschko, M. R.; Arola, A.; Baker, B. D.; Canova, B. P.; Chan Miller, C.; Cohen, R. C.; Davis, J. E.; Dussault, M. E.; Edwards, D. P.; Fishman, J.; Ghulam, A.; González Abad, G.; Grutter, M.; Herman, J. R.; Houck, J.; Jacob, D. J.; Joiner, J.; Kerridge, B. J.; Kim, J.; Krotkov, N. A.; Lamsal, L.; Li, C.; Lindfors, A.; Martin, R. V.; McElroy, C. T.; McLinden, C.; Natraj, V.; Neil, D. O.; Nowlan, C. R.; O`Sullivan, E. J.; Palmer, P. I.; Pierce, R. B.; Pippin, M. R.; Saiz-Lopez, A.; Spurr, R. J. D.; Szykman, J. J.; Torres, O.; Veefkind, J. P.; Veihelmann, B.; Wang, H.; Wang, J.; Chance, K.

    2017-01-01

    TEMPO was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021. It will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO observes from Mexico City, Cuba, and the Bahamas to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution ( 2.1 km N/S×4.4 km E/W at 36.5°N, 100°W). TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry, as well as contributing to carbon cycle knowledge. Measurements are made hourly from geostationary (GEO) orbit, to capture the high variability present in the diurnal cycle of emissions and chemistry that are unobservable from current low-Earth orbit (LEO) satellites that measure once per day. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a commercial GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve ozone (O3), nitrogen dioxide (NO2), sulfur dioxide (SO2), formaldehyde (H2CO), glyoxal (C2H2O2), bromine monoxide (BrO), IO (iodine monoxide), water vapor, aerosols, cloud parameters, ultraviolet radiation, and foliage properties. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions. TEMPO quantifies and tracks the evolution of aerosol loading. It provides these near-real-time air quality products that will be made publicly available. TEMPO will launch at a prime time to be the North American component of the global geostationary constellation of pollution monitoring

  3. Tropospheric Emissions: Monitoring of Pollution Overview

    Science.gov (United States)

    Chance, Kelly; Liu, Xiong; Suleiman, Raid M.; Flittner, David; Al-Saadi, Jay; Janz, Scott

    2015-01-01

    TEMPO is now well into its implementation phase, having passed both its Key Decision Point C and the Critical Design Review (CDR) for the instrument. The CDR for the ground systems will occur in March 2016 and the CDR for the Mission component at a later date, after the host spacecraft has been selected. TEMPO is on schedule to measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO measures from Mexico City to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution. TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry. Measurements are from geostationary (GEO) orbit, to capture the inherent high variability in the diurnal cycle of emissions and chemistry. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve O3, NO2, SO2, H2CO, C2H2O2, H2O, aerosols, cloud parameters, and UVB radiation. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions by 50 percent. TEMPO quantifies and tracks the evolution of aerosol loading. It provides near-real-time air quality products that will be made widely, publicly available. TEMPO provides much of the atmospheric measurement capability recommended for GEO-CAPE in the 2007 National Research Council Decadal Survey, Earth Science and Applications from Space: National Imperatives for the Next Decade and Beyond. Instruments from Europe (Sentinel 4) and Asia (GEMS) will

  4. A Raman lidar at La Reunion (20.8° S, 55.5° E for monitoring water vapour and cirrus distributions in the subtropical upper troposphere: preliminary analyses and description of a future system

    Directory of Open Access Journals (Sweden)

    C. Hoareau

    2012-06-01

    Full Text Available A ground-based Rayleigh lidar has provided continuous observations of tropospheric water vapour profiles and cirrus cloud using a preliminary Raman channels setup on an existing Rayleigh lidar above La Reunion over the period 2002–2005. With this instrument, we performed a first measurement campaign of 350 independent water vapour profiles. A statistical study of the distribution of water vapour profiles is presented and some investigations concerning the calibration are discussed. Analysis regarding the cirrus clouds is presented and a classification has been performed showing 3 distinct classes. Based on these results, the characteristics and the design of a future lidar system, to be implemented at the new Reunion Island altitude observatory (2200 m for long-term monitoring, is presented and numerical simulations of system performance have been realised to compare both instruments.

  5. Photochemistry and transport of tropospheric ozone and its precursors in urban and remote environments

    Science.gov (United States)

    Anderson, Daniel Craig

    Tropospheric ozone (O3) adversely affects human health, reduces crop yields, and contributes to climate forcing. To limit these effects, the processes controlling O3 abundance as well as that of its precursor molecules must be fully characterized. Here, I examine three facets of O 3 production, both in heavily polluted and remote environments. First, using in situ observations from the DISCOVER-AQ field campaign in the Baltimore/Washington region, I evaluate the emissions of the O 3 precursors CO and NOx (NOx = NO + NO2) in the National Emissions Inventory (NEI). I find that CO/NOx emissions ratios derived from observations are 21% higher than those predicted by the NEI. Comparisons to output from the CMAQ model suggest that CO in the NEI is accurate within 15 +/- 11%, while NOx emissions are overestimated by 51-70%, likely due to errors in mobile sources. These results imply that ambient ozone concentrations will respond more efficiently to NOx controls than current models suggest. I then investigate the source of high O3 and low H2O structures in the Tropical Western Pacific (TWP). A combination of in situ observations, satellite data, and models show that the high O3 results from photochemical production in biomass burning plumes from fires in tropical Southeast Asia and Central Africa; the low relative humidity results from large-scale descent in the tropics. Because these structures have frequently been attributed to mid-latitude pollution, biomass burning in the tropics likely contributes more to the radiative forcing of climate than previously believed. Finally, I evaluate the processes controlling formaldehyde (HCHO) in the TWP. Convective transport of near surface HCHO leads to a 33% increase in upper tropospheric HCHO mixing ratios; convection also likely increases upper tropospheric CH 3OOH to ~230 pptv, enough to maintain background HCHO at ~75 pptv. The long-range transport of polluted air, with NO four times the convectively controlled background

  6. Trends and seasonality in stream water chemistry in two moorland catchments of the Upper River Wye, Plynlimon

    Directory of Open Access Journals (Sweden)

    B. Reynolds

    1997-01-01

    Full Text Available Stream water chemistry in the Cyff and Gwy subcatchments within the headwaters of the River Wye has been monitored regularly since 1980. In the Gwy, which is a predominantly semi-natural grassland catchment, land use has remained relatively static over the monitoring period, whilst the Cyff catchment is more buffered because of base cation inputs from agricultural improvement and ground water sources. Using a variety of statistical techniques, the long-term data are examined for evidence of trends after eliminating seasonal effects. The results highlight some of the difficulties associated with the analysis of longterm water quality data which show considerable variability over a variety of timescales. Some of this variability can be explained in terms of hydrochemical responses to climatic extremes and episodic events such as large atmospheric inputs of seasalts. The long-term fluctuations in solute concentration underline the continuing need for maintaining consistent long-term monitoring at sensitive upland sites if underlying trends related to gradual changes in pollutant deposition or climate are to be detected with any certainty.

  7. Groundwater chemistry characterization using multi-criteria approach: The upper Samalá River basin (SW Guatemala)

    Science.gov (United States)

    Bucci, Arianna; Franchino, Elisa; De Luca, Domenico Antonio; Lasagna, Manuela; Malandrino, Mery; Bianco Prevot, Alessandra; Hernández Sac, Humberto Osvaldo; Coyoy, Israel Macario; Sac Escobar, Edwin Osvaldo; Hernández, Ardany

    2017-10-01

    Improving understanding on groundwater chemistry is a key priority for water supply from groundwater resources, especially in developing countries. A hydrochemical study was performed in an area of SW Guatemala (Samalà River basin), where water supply to population is groundwater-based and no systematic studies on its groundwater resources have been performed so far. Traditional hydrochemical analyses on major ions and some trace elements metals coupled with chemometric approach were performed, including principal component analysis and hierarchical clustering analysis. Results evidence that chemical differentiation is linked to the spatial distribution of sampled waters. The most common hydrochemical facies, bicarbonate calcium and magnesium, is linked to infiltration of meteoric waters in recharge areas represented by highlands surrounding Xela caldera, a wide plateau where most of population is concentrated. This trend undergoes chemical evolution in proximity of active volcanic complexes in the southern area, with enrichment in sulphate, chloride and magnesium. Chemical evolution also occurs towards the centre of Xela caldera due to slow circulation in aquifer and consequent sodium enrichment due to ion exchange with the porous medium. Water quality did not reveal severe concerns, even though some sources of contamination could be identified; in particular, agriculture and urban wastewater could be responsible for observed threshold exceedances in nitrate and lead. This integrated multi-approach to hydrochemical data interpretation yielded to the achievement of important information that poses the basis for future groundwater protection in an area where main water features were almost unknown.

  8. Origins of Tropospheric Ozone Interannual Variation (IAV) over Reunion: A Model Investigation

    Science.gov (United States)

    Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Francoise

    2016-01-01

    Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Reunion Island (21.1 degrees South Latitude, 55.5 degrees East Longitude) in June-August. Here we examine possible causes of the observed ozone variation at Reunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Reunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange. Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Reunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Reunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited tothe lower troposphere near the surface in August-September.

  9. Troposphere - ionosphere interaction during tropospheric MCC events

    International Nuclear Information System (INIS)

    Manzano, J.R.; Zossi Artigas, M.M. de; Filippi Manzano, A.N. de; Cosio Ragone, A.H. de

    1995-09-01

    The present paper describes the investigation of possible effects of the type of large meteorological events known as Mesoscale Convective Complexes (MCC) on the F-region of the ionosphere over Argentina. These warm-season weather systems of huge size are present in the United States (Maddox, 1980) and in South Americal (Velasco and Fritsch, 1987). Their extension can be as large as 1,300,000 Km 2 and they tend to move in different directions over the earth surface. It is expected that these meteorological events should leave its signature in the upper region of the atmosphere. 13 refs, 12 figs, 1 tab

  10. Tropospheric NO2 over China

    NARCIS (Netherlands)

    A, van der R.J.; Peters, D.H.M.U.; Kuenen, J.J.P.; Eskes, H.J.; Boersma, K.F.; Roozendael, Van M.; Smedt, de I.; Zhang, P.; Kelder, H.M.; Lacoste, H.; Ouwehand, L.

    2006-01-01

    The results are presented of a study to tropospheric NO2 over China, based on measurements from the satellite instruments GOME and SCIAMACHY. A data set of 10 year tropospheric NO2 has been processed from GOME and SCIAMACHY observations using a combined retrieval/assimilation approach. This approach

  11. Diurnal variation of tropospheric temperature at a tropical station

    Directory of Open Access Journals (Sweden)

    K. Revathy

    2001-08-01

    Full Text Available The vertical velocity in the troposphere-lower stratosphere region measured using MST radar has been utilized to evaluate the temperature profile in the region. The diurnal variation of the tropospheric temperature on one day in August 1998 at the tropical station Gadanki (13.5° N, 79.2° E has been studied using the MST radar technique. The diurnal variation of the temperature revealed a prominent diurnal variation with the peak in the afternoon hours increasingly delayed in altitude. The tropopause temperature and altitude exhibited a clear diurnal cycle.Key words. Atmospheric composition and structure (pressure, density and temperature; troposphere - composition and chemistry; instruments and technique

  12. Lidar investigations on the optical and dynamical properties of cirrus clouds in the upper troposphere and lower stratosphere regions at a tropical station, Gadanki, India (13.5°N, 79.2°E)

    Science.gov (United States)

    Krishnakumar, Vasudevannair; Satyanarayana, Malladi; Radhakrishnan, Soman R.; Dhaman, Reji K.; Jayeshlal, Glory Selvan; Motty, Gopinathan Nair S.; Pillai, Vellara P. Mahadevan; Raghunath, Karnam; Ratnam, Madineni Venkat; Rao, Duggirala Ramakrishna; Sudhakar, Pindlodi

    2014-01-01

    High altitude cirrus clouds are composed mainly of ice crystals with a variety of sizes and shapes. They have a large influence on Earth's energy balance and global climate. Recent studies indicate that the formation, dissipation, life time, optical, and micro-physical properties are influenced by the dynamical conditions of the surrounding atmosphere like background aerosol, turbulence, etc. In this work, an attempt has been made to quantify some of these characteristics by using lidar and mesosphere-stratosphere-troposphere (MST) radar. Mie lidar and 53 MHz MST radar measurements made over 41 nights during the period 2009 to 2010 from the tropical station, Gadanki, India (13.5°N, 79.2°E). The optical and microphysical properties along with the structure and dynamics of the cirrus are presented as observed under different atmospheric conditions. The study reveals the manifestation of different forms of cirrus with a preferred altitude of formation in the 13 to 14 km altitude. There are considerable differences in the properties obtained among 2009 and 2010 showing significant anomalous behavior in 2010. The clouds observed during 2010 show relatively high asymmetry and large multiple scattering effects. The anomalies found during 2010 may be attributed to the turbulence noticed in the surrounding atmosphere. The results show a clear correlation between the crystal morphology in the clouds and the dynamical conditions of the prevailing atmosphere during the observational period.

  13. Retrieval of tropospheric carbon monoxide for the MOPITT experiment

    Science.gov (United States)

    Pan, Liwen; Gille, John C.; Edwards, David P.; Bailey, Paul L.; Rodgers, Clive D.

    1998-12-01

    A retrieval method for deriving the tropospheric carbon monoxide (CO) profile and column amount under clear sky conditions has been developed for the Measurements of Pollution In The Troposphere (MOPITT) instrument, scheduled for launch in 1998 onboard the EOS-AM1 satellite. This paper presents a description of the method along with analyses of retrieval information content. These analyses characterize the forward measurement sensitivity, the contribution of a priori information, and the retrieval vertical resolution. Ensembles of tropospheric CO profiles were compiled both from aircraft in situ measurements and from chemical model results and were used in retrieval experiments to characterize the method and to study the sensitivity to different parameters. Linear error analyses were carried out in parallel with the ensemble experiments. Results of these experiments and analyses indicate that MOPITT CO column measurements will have better than 10% precision, and CO profile measurement will have approximately three pieces of independent information that will resolve 3-5 tropospheric layers to approximately 10% precision. These analyses are important for understanding MOPITT data, both for application of data in tropospheric chemistry studies and for comparison with in situ measurements.

  14. Study on the regional and global rise in NO{sub x} and non-methane hydrocarbon concentrations in the upper troposphere and lower stratosphere as a consequence of airplane emissions. Final report; Untersuchungen zur regionalen und globalen Erhoehung der NO{sub x}- und Nichtmethankohlenwasserstoff-Konzentrationen in der oberen Troposphaere und der unteren Stratosphaere infolge Flugzeugemissionen. Abschlussbericht

    Energy Technology Data Exchange (ETDEWEB)

    Rohrer, F

    1996-01-05

    In this project a chemical mechanism was developed for the upper troposphere which permits examining the photochemical formation of ozone. Using this mechanism it was found that at medium latitudes (at 10 km altitude in June) hydroxyl radical concentration and the rate of photochemical ozone formation to which it is coupled depend on NO{sub x} concentrations in a strongly non-linear manner, peaking at 110 ppt NO{sub x} and 200 pp NO{sub x}, respectively. Regarding the assessment of the effects of air traffic it was thus shown that in attempting to forecast changes in ozone concentration one must not only take aviation-related changes in NO{sub x} concentrations into account but also the forecasted absolute concentrations of NO{sub x}. The measured data were interpreted by combining a simplified model of NO{sub x} reactions with an existing three-dimensional transport model and comparing the measured and the calculated vertical NO profiles. It can be said that the 3D chemical transport model supplies realistic tropospheric NO{sub x} ratios at least for medium latitudes (49 to 56 N) in the months of May, June, July, December, and January. At these latitudes the tropospheric NO{sub x} budget is mainly governed by anthropogenic emissions. (orig./KW) [Deutsch] In diesem Projekt wurde ein Chemiemechanismus fuer die obere Troposphaere entwickelt, der es erlaubt, die photochemische Ozonbildung zu untersuchen. Mit diesem Mechanismus konnte fuer mittlere noerdliche Breiten (fuer 10 km Hoehe, Juni) gezeigt werden, dass die Hydroxylradikalkonzentration und die damit gekoppelte photochemische Ozonbildungsrate in stark nichtlinearer Weise von der Stickoxidkonzentration abhaengen und bei etwa 110 ppt NO{sub x} (bezw. 200 ppt NO{sub x} fuer die Ozonbildungsrate) ein Maximum durchlaufen. Fuer die Beurteilung der Auswirkungen des Flugverkehrs konnte deswegen gezeigt werden, dass die Voraussagen ueber Ozonveraenderungen nicht nur von der Aenderung der Stickoxidkonzentration durch den

  15. Thermodynamic constraint on the depth of the global tropospheric circulation.

    Science.gov (United States)

    Thompson, David W J; Bony, Sandrine; Li, Ying

    2017-08-01

    The troposphere is the region of the atmosphere characterized by low static stability, vigorous diabatic mixing, and widespread condensational heating in clouds. Previous research has argued that in the tropics, the upper bound on tropospheric mixing and clouds is constrained by the rapid decrease with height of the saturation water vapor pressure and hence radiative cooling by water vapor in clear-sky regions. Here the authors contend that the same basic physics play a key role in constraining the vertical structure of tropospheric mixing, tropopause temperature, and cloud-top temperature throughout the globe. It is argued that radiative cooling by water vapor plays an important role in governing the depth and amplitude of large-scale dynamics at extratropical latitudes.

  16. Impact of land convection on troposphere-stratosphere exchange in the tropics

    Directory of Open Access Journals (Sweden)

    P. Ricaud

    2007-11-01

    Full Text Available The mechanism of troposphere-stratosphere exchange in the tropics was investigated from space-borne observations of the horizontal distributions of tropospheric-origin long-lived species, nitrous oxide (N2O, methane (CH4 and carbon monoxide (CO, from 150 to 70 hPa in March-April-May by the ODIN/Sub-Millimeter Radiometer (SMR, the Upper Atmosphere Research Satellite (UARS/Halogen Occultation Experiment (HALOE and the TERRA/Measurements Of Pollution In The Troposphere (MOPITT instruments in 2002–2004, completed by recent observations of the AURA/Microwave Limb Sounder (MLS instrument during the same season in 2005. The vertical resolution of the satellite measurements ranges from 2 to 4 km. The analysis has been performed on isentropic surfaces: 400 K (lower stratosphere for all the species and 360 K (upper troposphere only for CO. At 400 K (and 360 K for CO, all gases show significant longitudinal variations with peak-to-trough values of ~5–11 ppbv for N2O, 0.07–0.13 ppmv for CH4, and ~10 ppbv for CO (~40 ppbv at 360 K. The maximum amounts are primarily located over Africa and, depending on the species, secondary more or less pronounced maxima are reported above northern South America and South-East Asia. The lower stratosphere over the Western Pacific deep convective region where the outgoing longwave radiation is the lowest, the tropopause the highest and the coldest, appears as a region of minimum concentration of tropospheric trace species. The possible impact on trace gas concentration at the tropopause of the inhomogeneous distribution and intensity of the sources, mostly continental, of the horizontal and vertical transports in the troposphere, and of cross-tropopause transport was explored with the MOCAGE Chemistry Transport Model. In the simulations, significant longitudinal variations were found on the medium-lived CO (2-month lifetime with peak-to-trough value of ~20 ppbv at 360 K and

  17. Aerosol indirect effects on lightning in the generation of induced NOx and tropospheric ozone over an Indian urban metropolis

    Science.gov (United States)

    Saha, Upal; Maitra, Animesh; Talukdar, Shamitaksha; Jana, Soumyajyoti

    increase in lightning activity is caused by the indirect influx of aerosols, especially in the upper troposphere. This is due to the warming-effect of aerosol forcing via its effect on tropospheric ozone production. Due to the increased production of O3 by lightning-induced NOx and high aerosol loading in the pre-monsoon and monsoon months, the positive climate feedback indicates a warmer climate. As a consequence, convective activity as well as lightning flashes may increase due to this indirect effect of AOD over the region. The generation of induced NOx has a positive correlation (r = 0.723) with the LFR during 2001-2012 over Kolkata. Thus, our results have significant implications for understanding the tropospheric ozone forcing by investigating the coupled aerosol-cloud-chemistry system on the generation of lightning and lightning-induced NOx over the urban metropolis.

  18. Two case studies on the interaction of large-scale transport, mesoscale photochemistry, and boundary-layer processes on the lower tropospheric ozone dynamics in early spring

    Directory of Open Access Journals (Sweden)

    S. Brönnimann

    2001-04-01

    Full Text Available The vertical distribution of ozone in the lower troposphere over the Swiss Plateau is investigated in detail for two episodes in early spring (February 1998 and March 1999. Profile measurements of boundary-layer ozone performed during two field campaigns with a tethered balloon sounding system and a kite are investigated using regular aerological and ozone soundings from a nearby site, measurements from monitoring stations at various altitudes, backward trajectories, and synoptic analyses of meteorological fields. Additionally, the effect of in situ photochemistry was estimated for one of the episodes employing the Metphomod Eulerian photochemical model. Although the meteorological situations were completely different, both cases had elevated layers with high ozone concentrations, which is not untypical for late winter and early spring. In the February episode, the highest ozone concentrations of 55 to 60 ppb, which were found at around 1100 m asl, were partly advected from Southern France, but a considerable contribution of in situ photochemistry is also predicted by the model. Below that elevation, the local chemical sinks and surface deposition probably overcompensated chemical production, and the vertical ozone distribution was governed by boundary-layer dynamics. In the March episode, the results suggest that ozone-rich air parcels, probably of stratospheric or upper tropospheric origin, were advected aloft the boundary layer on the Swiss Plateau.Key words. Atmospheric composition and structure (pollution – urban and regional; troposphere – composition and  chemistry – Meteorology and atmospheric dynamics (mesoscale meteorology

  19. Tropospheric Emission Spectrometer (TES) Data

    Data.gov (United States)

    National Aeronautics and Space Administration — TES focuses on the troposphere, the layer of atmosphere that stretches from the ground to the altitude at which airplanes fly. With very high spectral resolution,...

  20. Physics of the tropospheric radiopropagation

    International Nuclear Information System (INIS)

    Ajayi, G.O.

    1989-02-01

    The physics of the tropospheric radiopropagation is presented considering the atmospheric radio refractive index and taking into account the influence of precipitation and the attenuation due to the atmospheric gases. 35 refs, 20 figs, 3 tabs

  1. An assessment of 10-year NOAA aircraft-based tropospheric ozone profiling in Colorado

    Science.gov (United States)

    Leonard, Mark; Petropavlovskikh, Irina; Lin, Meiyun; McClure-Begley, Audra; Johnson, Bryan J.; Oltmans, Samuel J.; Tarasick, David

    2017-06-01

    The Global Greenhouse Gas Reference Network Aircraft Program at NOAA has sampled ozone and other atmospheric trace constituents in North America for over a decade (2005-present). The method to derive tropospheric ozone climatology from the light aircraft measurements equipped with the 2B Technology instruments is described in this paper. Since ozone instruments at most of aircraft locations are flown once a month, this raises the question of whether the sampling frequency allows for deriving a climatology that can adequately represent ozone seasonal and vertical variability over various locations. Here we interpret the representativeness of the tropospheric ozone climatology derived from these under-sampled observations using hindcast simulations conducted with the Geophysical Fluid Dynamics Laboratory chemistry-climate model (GFDL-AM3). We first focus on ozone measurements from monthly aircraft profiles over the Front Range of Colorado and weekly ozonesondes launched in Boulder, Colorado. The climatology is presented as monthly values separated in 5th, 25th, 50th, 75th, 95th percentiles, and averaged at three vertical layers: lower (1.6-3 km), middle (3-6 km), and upper (6-8 km) troposphere. The aircraft-based climatology is compared to the climatology derived from the nearest located ozonesondes launched from Boulder, Colorado, from GFDL-AM3 co-sampled in time with in-situ observations, and from GFDL-AM3 continuous 3-h samples. Based on these analyses, we recommend the sampling frequency to obtain adequate representation of ozone climatology in the free troposphere. The 3-h sampled AM3 model is used as a benchmark reference for the under-sampled time series. We find that the minimal number of soundings required per month for the all altitude bins (1.6-3, 3-6, and 6-8 km) to sufficiently match the 95% confidence level of the fully sampled monthly ozone means vary between 3 and 5 sounding per month, except in August with a minimum of 6 soundings per month. The

  2. A new diagnostic for tropospheric ozone production

    Science.gov (United States)

    Edwards, Peter M.; Evans, Mathew J.

    2017-11-01

    Tropospheric ozone is important for the Earth's climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain-like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model-model comparisons to better identify the root causes of model differences.

  3. A new diagnostic for tropospheric ozone production

    Directory of Open Access Journals (Sweden)

    P. M. Edwards

    2017-11-01

    Full Text Available Tropospheric ozone is important for the Earth's climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain-like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model–model comparisons to better identify the root causes of model differences.

  4. A tropospheric ozone maximum over the equatorial Southern Indian Ocean

    Directory of Open Access Journals (Sweden)

    L. Zhang

    2012-05-01

    Full Text Available We examine the distribution of tropical tropospheric ozone (O3 from the Microwave Limb Sounder (MLS and the Tropospheric Emission Spectrometer (TES by using a global three-dimensional model of tropospheric chemistry (GEOS-Chem. MLS and TES observations of tropospheric O3 during 2005 to 2009 reveal a distinct, persistent O3 maximum, both in mixing ratio and tropospheric column, in May over the Equatorial Southern Indian Ocean (ESIO. The maximum is most pronounced in 2006 and 2008 and less evident in the other three years. This feature is also consistent with the total column O3 observations from the Ozone Mapping Instrument (OMI and the Atmospheric Infrared Sounder (AIRS. Model results reproduce the observed May O3 maximum and the associated interannual variability. The origin of the maximum reflects a complex interplay of chemical and dynamic factors. The O3 maximum is dominated by the O3 production driven by lightning nitrogen oxides (NOx emissions, which accounts for 62% of the tropospheric column O3 in May 2006. We find the contribution from biomass burning, soil, anthropogenic and biogenic sources to the O3 maximum are rather small. The O3 productions in the lightning outflow from Central Africa and South America both peak in May and are directly responsible for the O3 maximum over the western ESIO. The lightning outflow from Equatorial Asia dominates over the eastern ESIO. The interannual variability of the O3 maximum is driven largely by the anomalous anti-cyclones over the southern Indian Ocean in May 2006 and 2008. The lightning outflow from Central Africa and South America is effectively entrained by the anti-cyclones followed by northward transport to the ESIO.

  5. Implementation of Tropospheric Emissions: Monitoring of Pollution (TEMPO)

    Science.gov (United States)

    Chance, K.; Liu, X.; Suleiman, R. M.; Flittner, D. E.; Al-Saadi, J. A.; Janz, S. J.

    2014-12-01

    The updated status of TEMPO, as it proceeds from formulation phase into implementation phase is presented. TEMPO, the first NASA Earth Venture Instrument, will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO measures from Mexico City to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution. TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry. Measurements are from geostationary (GEO) orbit, to capture the inherent high variability in the diurnal cycle of emissions and chemistry. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve O3, NO2, SO2, H2CO, C2H2O2, H2O, aerosols, cloud parameters, and UVB radiation. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, reducing uncertainty in air quality predictions by 50%. TEMPO quantifies and tracks the evolution of aerosol loading. It provides near-real-time air quality products that will be made widely, publicly available. TEMPO provides much of the atmospheric measurement capability recommended for GEO-CAPE in the 2007 National Research Council Decadal Survey, Earth Science and Applications from Space: National Imperatives for the Next Decade and Beyond. GEO-CAPE is not planned for implementation this decade. However, instruments from Europe (Sentinel 4) and Asia (GEMS) will form parts of a global GEO constellation for pollution monitoring later this decade, with a major focus on intercontinental

  6. The Radiative Role of Free Tropospheric Aerosols and Marine Clouds over the Central North Atlantic

    Energy Technology Data Exchange (ETDEWEB)

    Mazzoleni, Claudio [Michigan Technological Univ., Houghton, MI (United States); Kumar, Sumit [Michigan Technological Univ., Houghton, MI (United States); Wright, Kendra [Michigan Technological Univ., Houghton, MI (United States); Kramer, Louisa [Michigan Technological Univ., Houghton, MI (United States); Mazzoleni, Lynn [Michigan Technological Univ., Houghton, MI (United States); Owen, Robert [Michigan Technological Univ., Houghton, MI (United States); Helmig, Detlev [Univ. of Colorado, Boulder, CO (United States)

    2014-12-09

    microscope – were often very compacted, suggesting cloud processing and exhibiting different optical properties from fresh emissions. In addition, black carbon was found to be sometimes mixed with mineral dust, affecting its optical properties and potential forcing. c) Some aerosols collected at PMO acted as ice nuclei, potentially contributing to cirrus cloud formation during their transport in the upper free troposphere. Identified good ice nuclei were often mineral dust particles. d) The free tropospheric aerosols studied at PMO have relevance to low level marine clouds due, for example, to synoptic subsidence entraining free tropospheric aerosols into the marine boundary layer. This has potentially large consequences on cloud condensation nuclei concentrations and compositions in the marine boundary layer; therefore, having an effect on the marine stratus clouds, with potentially important repercussions on the radiative forcing. The scientific products of this project currently include contributions to two papers published in the Nature Publishing group (Nature Communications and Scientific Reports), one paper under revision for Atmospheric Chemistry and Physics, one in review in Geophysical Research Letters and one recently submitted to Atmospheric Chemistry and Physics Discussion. In addition, four manuscripts are in advanced state of preparation. Finally, twenty-eight presentations were given at international conferences, workshops and seminars.

  7. Tropospheric ozone annual variation and possible troposphere-stratosphere coupling in the Arctic and Antarctic as derived from ozone soundings at Resolute and Amundsen-Scott stations

    Energy Technology Data Exchange (ETDEWEB)

    Gruzdev, A.N.; Sitnov, S.A. (Russian Academy of Sciences, Moscow (Russian Federation). Inst. of Atmospheric Physics)

    1993-01-01

    The tropospheric ozone annual variation in the northern and southern polar regions is analyzed from ozone sounding data obtained at Resolute during a 15-year period and Amundsen-Scott during a 7-year period. The phase of ozone annual variation above Resolute changes (increases) gradually from the stratosphere across the tropopause to the middle troposphere. Unlike this, the phase of the Antarctic ozone annual harmonic has a discontinuity in the layer of the changing tropopause level, so that the annual harmonic in the upper troposphere, lower stratosphere is 4-to-5 months out of phase (earlier) to that above and beneath. Above both the Arctic and Antarctic stations, the ozone mixing ratio and its vertical gradient evolve in a similar manner in the wide layer from the lower stratosphere to the middle troposphere. This likely points out that ozone in this layer is controlled from above. An indication of the stratospheric-tropospheric ozone exchange above Resolute is noted from mid-winter to spring. The analysis of columnar tropospheric ozone changes gives a lower estimate of the cross-tropopause ozone flux up to 5x10[sup 10] mol cm[sup -2] s[sup -1]. Above the South Pole, the cross-tropopause ozone flux is not usually large. There is also some evidence that early in the spring, when the stratospheric ozone 'hole' is developed, the stratospheric-tropospheric exchange conducts the influence of the 'hole' into the upper troposphere, where the integrated ozone destruction is estimated to be 8x10[sup 10] mol cm[sup -2] s[sup -1]. Correlation analysis gives no ozone-tropopause correlation in the Antarctic in winter, while in other seasons as well as during all seasons in the Arctic, there are negative correlation peaks just above the tropopause. (19 refs., 6 figs.).

  8. Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone

    Directory of Open Access Journals (Sweden)

    B. Sauvage

    2007-01-01

    Full Text Available We use a global chemical transport model (GEOS-Chem to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS satellite instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning NOx and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flashes improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 6±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils and VOCs (biomass burning. The top-down biomass burning inventory is larger than the bottom-up inventory by a factor of 2 for HCHO and alkenes, and by a factor of 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4 is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv

  9. A New Retrieval Algorithm for OMI NO2: Tropospheric Results and Comparisons with Measurements and Models

    Science.gov (United States)

    Swartz, W. H.; Bucesla, E. J.; Lamsal, L. N.; Celarier, E. A.; Krotkov, N. A.; Bhartia, P, K,; Strahan, S. E.; Gleason, J. F.; Herman, J.; Pickering, K.

    2012-01-01

    Nitrogen oxides (NOx =NO+NO2) are important atmospheric trace constituents that impact tropospheric air pollution chemistry and air quality. We have developed a new NASA algorithm for the retrieval of stratospheric and tropospheric NO2 vertical column densities using measurements from the nadir-viewing Ozone Monitoring Instrument (OMI) on NASA's Aura satellite. The new products rely on an improved approach to stratospheric NO2 column estimation and stratosphere-troposphere separation and a new monthly NO2 climatology based on the NASA Global Modeling Initiative chemistry-transport model. The retrieval does not rely on daily model profiles, minimizing the influence of a priori information. We evaluate the retrieved tropospheric NO2 columns using surface in situ (e.g., AQS/EPA), ground-based (e.g., DOAS), and airborne measurements (e.g., DISCOVER-AQ). The new, improved OMI tropospheric NO2 product is available at high spatial resolution for the years 200S-present. We believe that this product is valuable for the evaluation of chemistry-transport models, examining the spatial and temporal patterns of NOx emissions, constraining top-down NOx inventories, and for the estimation of NOx lifetimes.

  10. Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis

    Directory of Open Access Journals (Sweden)

    K. Tsigaridis

    2003-01-01

    Full Text Available A global 3-dimensional chemistry/transport model able to describe O3, NOx, Volatile Organic Compounds (VOC, sulphur and NH3 chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere focusing on Secondary Organic Aerosol (SOA formation. A number of global simulations have been performed to determine a possible range of annual global SOA production and investigate uncertainties associated with the model results. The studied uncertainties in the SOA budget have been evaluated to be in decreasing importance: the potentially irreversible sticking of the semi-volatile compounds on aerosols, the enthalpy of vaporization of these compounds, the partitioning of SOA on non-carbonaceous aerosols, the conversion of aerosols from hydrophobic to hydrophilic, the emissions of primary carbonaceous aerosols, the chemical fate of the first generation products and finally the activity coefficient of the condensable species. The large uncertainties associated with the emissions of VOC and the adopted simplification of chemistry have not been investigated in this study. Although not all sources of uncertainties have been investigated, according to our calculations, the above factors within the experimental range of variations could result to an overall uncertainty of about a factor of 20 in the global SOA budget. The global annual SOA production from biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or sea-salt, together with the partitioning and the dissociation of the semi-volatile products in aerosol water has been neglected. Comparison of model results to observations, where available, shows a better agreement for the upper budget estimates than for the

  11. Ozone in the Tropical Troposphere

    NARCIS (Netherlands)

    Peters, Wouter

    2002-01-01

    The aim of the research presented here is to acquire knowledge of the past, present, and future composition, stability, sensitivity, and variability of the troposphere. We focus mostly on the tropical regions because it has received little attention so far, measurements here are scarce, and large

  12. Impacts of stratospheric sulfate geoengineering on tropospheric ozone

    Science.gov (United States)

    Xia, Lili; Nowack, Peer J.; Tilmes, Simone; Robock, Alan

    2017-10-01

    A range of solar radiation management (SRM) techniques has been proposed to counter anthropogenic climate change. Here, we examine the potential effects of stratospheric sulfate aerosols and solar insolation reduction on tropospheric ozone and ozone at Earth's surface. Ozone is a key air pollutant, which can produce respiratory diseases and crop damage. Using a version of the Community Earth System Model from the National Center for Atmospheric Research that includes comprehensive tropospheric and stratospheric chemistry, we model both stratospheric sulfur injection and solar irradiance reduction schemes, with the aim of achieving equal levels of surface cooling relative to the Representative Concentration Pathway 6.0 scenario. This allows us to compare the impacts of sulfate aerosols and solar dimming on atmospheric ozone concentrations. Despite nearly identical global mean surface temperatures for the two SRM approaches, solar insolation reduction increases global average surface ozone concentrations, while sulfate injection decreases it. A fundamental difference between the two geoengineering schemes is the importance of heterogeneous reactions in the photochemical ozone balance with larger stratospheric sulfate abundance, resulting in increased ozone depletion in mid- and high latitudes. This reduces the net transport of stratospheric ozone into the troposphere and thus is a key driver of the overall decrease in surface ozone. At the same time, the change in stratospheric ozone alters the tropospheric photochemical environment due to enhanced ultraviolet radiation. A shared factor among both SRM scenarios is decreased chemical ozone loss due to reduced tropospheric humidity. Under insolation reduction, this is the dominant factor giving rise to the global surface ozone increase. Regionally, both surface ozone increases and decreases are found for both scenarios; that is, SRM would affect regions of the world differently in terms of air pollution. In conclusion

  13. Impacts of stratospheric sulfate geoengineering on tropospheric ozone

    Directory of Open Access Journals (Sweden)

    L. Xia

    2017-10-01

    Full Text Available A range of solar radiation management (SRM techniques has been proposed to counter anthropogenic climate change. Here, we examine the potential effects of stratospheric sulfate aerosols and solar insolation reduction on tropospheric ozone and ozone at Earth's surface. Ozone is a key air pollutant, which can produce respiratory diseases and crop damage. Using a version of the Community Earth System Model from the National Center for Atmospheric Research that includes comprehensive tropospheric and stratospheric chemistry, we model both stratospheric sulfur injection and solar irradiance reduction schemes, with the aim of achieving equal levels of surface cooling relative to the Representative Concentration Pathway 6.0 scenario. This allows us to compare the impacts of sulfate aerosols and solar dimming on atmospheric ozone concentrations. Despite nearly identical global mean surface temperatures for the two SRM approaches, solar insolation reduction increases global average surface ozone concentrations, while sulfate injection decreases it. A fundamental difference between the two geoengineering schemes is the importance of heterogeneous reactions in the photochemical ozone balance with larger stratospheric sulfate abundance, resulting in increased ozone depletion in mid- and high latitudes. This reduces the net transport of stratospheric ozone into the troposphere and thus is a key driver of the overall decrease in surface ozone. At the same time, the change in stratospheric ozone alters the tropospheric photochemical environment due to enhanced ultraviolet radiation. A shared factor among both SRM scenarios is decreased chemical ozone loss due to reduced tropospheric humidity. Under insolation reduction, this is the dominant factor giving rise to the global surface ozone increase. Regionally, both surface ozone increases and decreases are found for both scenarios; that is, SRM would affect regions of the world differently in terms of air

  14. Influence of the Gulf Stream on the troposphere.

    Science.gov (United States)

    Minobe, Shoshiro; Kuwano-Yoshida, Akira; Komori, Nobumasa; Xie, Shang-Ping; Small, Richard Justin

    2008-03-13

    The Gulf Stream transports large amounts of heat from the tropics to middle and high latitudes, and thereby affects weather phenomena such as cyclogenesis and low cloud formation. But its climatic influence, on monthly and longer timescales, remains poorly understood. In particular, it is unclear how the warm current affects the free atmosphere above the marine atmospheric boundary layer. Here we consider the Gulf Stream's influence on the troposphere, using a combination of operational weather analyses, satellite observations and an atmospheric general circulation model. Our results reveal that the Gulf Stream affects the entire troposphere. In the marine boundary layer, atmospheric pressure adjustments to sharp sea surface temperature gradients lead to surface wind convergence, which anchors a narrow band of precipitation along the Gulf Stream. In this rain band, upward motion and cloud formation extend into the upper troposphere, as corroborated by the frequent occurrence of very low cloud-top temperatures. These mechanisms provide a pathway by which the Gulf Stream can affect the atmosphere locally, and possibly also in remote regions by forcing planetary waves. The identification of this pathway may have implications for our understanding of the processes involved in climate change, because the Gulf Stream is the upper limb of the Atlantic meridional overturning circulation, which has varied in strength in the past and is predicted to weaken in response to human-induced global warming in the future.

  15. The Tropospheric Ozone Assessment Report (TOAR): A community-wide effort to quantify tropospheric ozone in a rapidly changing world

    Science.gov (United States)

    Cooper, O. R.; Schultz, M.; Paoletti, E.; Galbally, I. E.; Naja, M. K.; Tarasick, D. W.; Evans, M. J.; Thompson, A. M.

    2017-12-01

    Tropospheric ozone is a greenhouse gas and pollutant detrimental to human health and crop and ecosystem productivity. Since 1990 a large portion of the anthropogenic emissions that react in the atmosphere to produce ozone has shifted from North America and Europe to Asia. This rapid shift, coupled with limited ozone monitoring in developing nations, left scientists unable to answer the most basic questions: Which regions of the world have the greatest human and plant exposure to ozone pollution? Is ozone continuing to decline in nations with strong emissions controls? To what extent is ozone increasing in the developing world? How can the atmospheric sciences community facilitate access to the ozone metrics necessary for quantifying ozone's impact on human health and crop/ecosystem productivity? To answer these questions the International Global Atmospheric Chemistry Project (IGAC) initiated the Tropospheric Ozone Assessment Report (TOAR). With over 220 member scientists and air quality specialists from 36 nations, TOAR's mission is to provide the research community with an up-to-date scientific assessment of tropospheric ozone's global distribution and trends from the surface to the tropopause. TOAR has also built the world's largest database of surface ozone observations and generated ozone exposure and dose metrics at thousands of measurement sites around the world, freely accessible for research on the global-scale impact of ozone on climate, human health and crop/ecosystem productivity. Plots of these metrics show the regions of the world with the greatest ozone exposure for humans and crops/ecosystems, at least in areas where observations are available. The results also highlight regions where air quality is improving and where it has degraded. TOAR has also conducted the first intercomparison of tropospheric column ozone from ozonesondes and multiple satellite instruments, which provide similar estimates of the present-day tropospheric ozone burden.

  16. The distribution and speciation of mercury in the free troposphere of the Pacific Northwest

    Science.gov (United States)

    Swartzendruber, Philip C.

    2009-12-01

    Mercury (Hg) is a potent neurotoxin which has accumulated in aquatic ecosystems and has led to increased neurological and developmental health risks for wildlife and humans worldwide. This dissertation aims to improve our understanding of the global mercury cycle by investigating its distribution and chemistry in the free troposphere. A Hg speciation system was deployed at the summit station of Mt. Bachelor, OR (2.7 km asl) (MBO). It measured gaseous elemental mercury (GEM), reactive gaseous mercury (RGM), and particulate mercury (PHg) from May-Aug 2005. The system detected RGM up to 600 pg/m3, or 40% of the total airborne Hg. The high RGM was not due to anthropogenic emissions, but was produced in situ. The GEOS-Chem chemical transport model (CTM) was unable to reproduce the magnitude of the highest RGM concentrations using the assumed OH and ozone oxidation mechanisms. The vertical distribution of mercury in the Pacific Northwest was investigated with an aircraft campaign in 2006 during the INTEX-B campaign. Three of the eight flights observed significant enhancements of GEM and CO in the free troposphere. The enhancement ratios (0.0067 (+/-0.0027) ng/m3 /ppb) were consistent with previous observations of Asian industrial influence at MBO and in Okinawa, Japan. Backtrajectories and GEOS-Chem CTM simulations supported Asian long range transport as the source of the influence. A technique was developed to measure RGM in an aircraft. In this technique, RGM is measured by difference and simultaneously is directly collected on a denuder. The system was tested in the laboratory with an RGM proxy, (HgCl 2 at ˜500 pg/m3), and the agreement of the denuder-difference techniques was 15% (+/-13%, relative percent difference). The instrument was tested in five flights from the surface to 5 km. A linear correlation of all denuder-difference data had a slope of 0.41. RGM enhancements (200-500 pg/m3) were observed with varying relationships to ozone and water vapor which

  17. Tropospheric Ozone Assessment Report: Assessment of global-scale model performance for global and regional ozone distributions, variability, and trends

    Directory of Open Access Journals (Sweden)

    P. J. Young

    2018-01-01

    Full Text Available The goal of the Tropospheric Ozone Assessment Report (TOAR is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for

  18. Multimodel ensemble simulations of of present-day and near-future tropospheric ozone

    NARCIS (Netherlands)

    Stevenson, D.S.; Dentener, F.J.; van Noije, T.P.C.; Eskes, H.J.; Krol, M.C.

    2006-01-01

    Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions

  19. Multimodel ensemble simulations of present-day and near-future tropospheric ozone

    NARCIS (Netherlands)

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

    2006-01-01

    Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions

  20. THEORETICAL STUDY OF THE REMOVAL OF THE TROPOSPHERIC FORMALDEHYDE BY REACTION WITH OH* AND NH3* RADICALS

    OpenAIRE

    Cjuno H., Jesús A.; Arroyo C., Juan; Cubas C., Roger

    2014-01-01

    In the context of atmospheric chemistry, two reactions radical-molecule of hydrogen abstraction have been studied. These are the OH' and NO3: radical (oxidizers agents in the troposphere) with formaldehyde in gas-phase. The calculations were carried out using the PM3 and . Ab initio methods of the UHF type. The results have allowed us to estimate the corresponding times of tropospheric permanency and the implications of these reactions in the removal of forrnaldehyde and similars from the low...

  1. Uncertainties in models of tropospheric ozone based on Monte Carlo analysis: Tropospheric ozone burdens, atmospheric lifetimes and surface distributions

    Science.gov (United States)

    Derwent, Richard G.; Parrish, David D.; Galbally, Ian E.; Stevenson, David S.; Doherty, Ruth M.; Naik, Vaishali; Young, Paul J.

    2018-05-01

    Recognising that global tropospheric ozone models have many uncertain input parameters, an attempt has been made to employ Monte Carlo sampling to quantify the uncertainties in model output that arise from global tropospheric ozone precursor emissions and from ozone production and destruction in a global Lagrangian chemistry-transport model. Ninety eight quasi-randomly Monte Carlo sampled model runs were completed and the uncertainties were quantified in tropospheric burdens and lifetimes of ozone, carbon monoxide and methane, together with the surface distribution and seasonal cycle in ozone. The results have shown a satisfactory degree of convergence and provide a first estimate of the likely uncertainties in tropospheric ozone model outputs. There are likely to be diminishing returns in carrying out many more Monte Carlo runs in order to refine further these outputs. Uncertainties due to model formulation were separately addressed using the results from 14 Atmospheric Chemistry Coupled Climate Model Intercomparison Project (ACCMIP) chemistry-climate models. The 95% confidence ranges surrounding the ACCMIP model burdens and lifetimes for ozone, carbon monoxide and methane were somewhat smaller than for the Monte Carlo estimates. This reflected the situation where the ACCMIP models used harmonised emissions data and differed only in their meteorological data and model formulations whereas a conscious effort was made to describe the uncertainties in the ozone precursor emissions and in the kinetic and photochemical data in the Monte Carlo runs. Attention was focussed on the model predictions of the ozone seasonal cycles at three marine boundary layer stations: Mace Head, Ireland, Trinidad Head, California and Cape Grim, Tasmania. Despite comprehensively addressing the uncertainties due to global emissions and ozone sources and sinks, none of the Monte Carlo runs were able to generate seasonal cycles that matched the observations at all three MBL stations. Although

  2. On the use of mass-conserving wind fields in chemistry-transport models

    Directory of Open Access Journals (Sweden)

    B. Bregman

    2003-01-01

    Full Text Available A new method has been developed that provides mass-conserving wind fields for global chemistry-transport models. In previous global Eulerian modeling studies a mass-imbalance was found between the model mass transport and the surface pressure tendencies. Several methods have been suggested to correct for this imbalance, but so far no satisfactory solution has been found. Our new method solves these problems by using the wind fields in a spherical harmonical form (divergence and vorticity by mimicing the physics of the weather forecast model as closely as possible. A 3-D chemistry-transport model was used to show that the calculated ozone fields with the new processing method agree remarkably better with ozone observations in the upper troposphere and lower stratosphere. In addition, the calculated age of air in the lower stratosphere show better agreement with observations, although the air remains still too young in the extra-tropical stratosphere.

  3. Improvement of OMI Ozone Profile Retrievals in the Troposphere and Lower Troposphere by the Use of the Tropopause-Based Ozone Profile Climatology

    Science.gov (United States)

    Bak, Juseon; Liu, X.; Wei, J.; Kim, J. H.; Chance, K.; Barnet, C.

    2011-01-01

    An advance algorithm based on the optimal estimation technique has beeen developed to derive ozone profile from GOME UV radiances and have adapted it to OMI UV radiances. OMI vertical resolution : 7-11 km in the troposphere and 10-14 km in the stratosphere. Satellite ultraviolet measurements (GOME, OMI) contain little vertical information for the small scale of ozone, especially in the upper troposphere (UT) and lower stratosphere (LS) where the sharp O3 gradient across the tropopause and large ozone variability are observed. Therefore, retrievals depend greatly on the a-priori knowledge in the UTLS

  4. Forecasting tropical cyclone recurvature with upper tropospheric winds

    Science.gov (United States)

    Gentry, R. C.

    1983-01-01

    Data from 17 tropical cyclones during the 1974 through 1979 hurricane seasons are used to investigate whether the high level winds far to the northwest, north and northeast of the hurricane center can be used to predict hurricane track recurvature. When the man 200-mb winds 1500 to 2000 km northwest and north of the storm center equal or exceed 20 m/s, 80 per cent of the storms recurved before traveling as much as 12 degrees of longitude farther west. The high winds were also used to predict change in direction of forward motion during the next 72 hours. The regression equations developed explain up to 41 per cent of the variance in future direction. In addition to the geostrophic winds used, winds were also obtained by tracking clouds with successive satellite imagery. The u-components of the satellite winds are highly correlated with the geostrophic winds at 200-mb and could probably be used instead of them when available. The v-components are less highly correlated.

  5. Interactive ozone and methane chemistry in GISS-E2 historical and future climate simulations

    Directory of Open Access Journals (Sweden)

    D. T. Shindell

    2013-03-01

    Full Text Available The new generation GISS climate model includes fully interactive chemistry related to ozone in historical and future simulations, and interactive methane in future simulations. Evaluation of ozone, its tropospheric precursors, and methane shows that the model captures much of the large-scale spatial structure seen in recent observations. While the model is much improved compared with the previous chemistry-climate model, especially for ozone seasonality in the stratosphere, there is still slightly too rapid stratospheric circulation, too little stratosphere-to-troposphere ozone flux in the Southern Hemisphere and an Antarctic ozone hole that is too large and persists too long. Quantitative metrics of spatial and temporal correlations with satellite datasets as well as spatial autocorrelation to examine transport and mixing are presented to document improvements in model skill and provide a benchmark for future evaluations. The difference in radiative forcing (RF calculated using modeled tropospheric ozone versus tropospheric ozone observed by TES is only 0.016 W m−2. Historical 20th Century simulations show a steady increase in whole atmosphere ozone RF through 1970 after which there is a decrease through 2000 due to stratospheric ozone depletion. Ozone forcing increases throughout the 21st century under RCP8.5 owing to a projected recovery of stratospheric ozone depletion and increases in methane, but decreases under RCP4.5 and 2.6 due to reductions in emissions of other ozone precursors. RF from methane is 0.05 to 0.18 W m−2 higher in our model calculations than in the RCP RF estimates. The surface temperature response to ozone through 1970 follows the increase in forcing due to tropospheric ozone. After that time, surface temperatures decrease as ozone RF declines due to stratospheric depletion. The stratospheric ozone depletion also induces substantial changes in surface winds and the Southern Ocean circulation, which may play a role in

  6. Sensitivity of simulated convection-driven stratosphere-troposphere exchange in WRF-Chem to the choice of physical and chemical parameterization

    Science.gov (United States)

    Phoenix, Daniel B.; Homeyer, Cameron R.; Barth, Mary C.

    2017-08-01

    Tropopause-penetrating convection is capable of rapidly transporting air from the lower troposphere to the upper troposphere and lower stratosphere (UTLS), where it can have important impacts on chemistry, the radiative budget, and climate. However, obtaining in situ measurements of convection and convective transport is difficult and such observations are historically rare. Modeling studies, on the other hand, offer the advantage of providing output related to the physical, dynamical, and chemical characteristics of storms and their environments at fine spatial and temporal scales. Since these characteristics of simulated convection depend on the chosen model design, we examine the sensitivity of simulated convective transport to the choice of physical (bulk microphysics or BMP and planetary boundary layer or PBL) and chemical parameterizations in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). In particular, we simulate multiple cases where in situ observations are available from the recent (2012) Deep Convective Clouds and Chemistry (DC3) experiment. Model output is evaluated using ground-based radar observations of each storm and in situ trace gas observations from two aircraft operated during the DC3 experiment. Model results show measurable sensitivity of the physical characteristics of a storm and the transport of water vapor and additional trace gases into the UTLS to the choice of BMP. The physical characteristics of the storm and transport of insoluble trace gases are largely insensitive to the choice of PBL scheme and chemical mechanism, though several soluble trace gases (e.g., SO2, CH2O, and HNO3) exhibit some measurable sensitivity.

  7. Using Raman Spectroscopy and Surface-Enhanced Raman Scattering to Identify Colorants in Art: An Experiment for an Upper-Division Chemistry Laboratory

    Science.gov (United States)

    Mayhew, Hannah E.; Frano, Kristen A.; Svoboda, Shelley A.; Wustholz, Kristin L.

    2015-01-01

    Surface-enhanced Raman scattering (SERS) studies of art represent an attractive way to introduce undergraduate students to concepts in nanoscience, vibrational spectroscopy, and instrumental analysis. Here, we present an undergraduate analytical or physical chemistry laboratory wherein a combination of normal Raman and SERS spectroscopy is used to…

  8. Analysis of CO in the tropical troposphere using Aura satellite data and the GEOS-Chem model: insights into transport characteristics of the GEOS meteorological products

    Directory of Open Access Journals (Sweden)

    Junhua Liu

    2010-12-01

    Full Text Available We use the GEOS-Chem chemistry-transport model (CTM to interpret the spatial and temporal variations of tropical tropospheric CO observed by the Microwave Limb Sounder (MLS and the Tropospheric Emission Spectrometer (TES. In so doing, we diagnose and evaluate transport in the GEOS-4 and GEOS-5 assimilated meteorological fields that drive the model, with a particular focus on vertical mixing at the end of the dry season when convection moves over the source regions. The results indicate that over South America, deep convection in both GEOS-4 and GEOS-5 decays at too low an altitude early in the wet season, and the source of CO from isoprene in the model (MEGAN v2.1 is too large, causing a lag in the model's seasonal maximum of CO compared to MLS CO in the upper troposphere (UT. TES and MLS data reveal problems with excessive transport of CO to the eastern equatorial Pacific and lofting in the ITCZ in August and September, particularly in GEOS-4. Over southern Africa, GEOS-4 and GEOS-5 simulations match the phase of the observed CO variation from the lower troposphere (LT to the UT fairly well, although the magnitude of the seasonal maximum is underestimated considerably due to low emissions in the model. A sensitivity run with increased emissions leads to improved agreement with observed CO in the LT and middle troposphere (MT, but the amplitude of the seasonal variation is too high in the UT in GEOS-4. Difficulty in matching CO in the LT and UT implies there may be overly vigorous vertical mixing in GEOS-4 early in the wet season. Both simulations and observations show a time lag between the peak in fire emissions (July and August and in CO (September and October. We argue that it is caused by the prevailing subsidence in the LT until convection moves south in September, as well as the low sensitivity of TES data in the LT over the African Plateau. The MLS data suggest that too much CO has been transported from fires in northern Africa to the UT

  9. Greenhouse Observations of the Stratosphere and Troposphere (GHOST): a novel shortwave infrared spectrometer developed for the Global Hawk unmanned aerial vehicle

    Science.gov (United States)

    Humpage, Neil; Boesch, Hartmut; Palmer, Paul; Parr-Burman, Phil; Vick, Andy; Bezawada, Naidu; Black, Martin; Born, Andy; Pearson, David; Strachan, Jonathan; Wells, Martyn

    2014-05-01

    The tropospheric distribution of greenhouse gases (GHGs) is dependent on surface flux variations, atmospheric chemistry and transport processes over a wide range of spatial and temporal scales. Errors in assumed atmospheric transport can adversely affect surface flux estimates inferred from surface, aircraft or satellite observations of greenhouse gas concentrations using inverse models. We present a novel, compact shortwave infrared spectrometer (GHOST) for installation on the NASA Global Hawk unmanned aerial vehicle to provide tropospheric column observations of CO2, CO, CH4, H2O and HDO over the ocean to address the need for large-scale, simultaneous, finely resolved measurements of key GHGs. These species cover a range of lifetimes and source processes, and measurements of their tropospheric columns will reflect the vertically integrated signal of their vertical and horizontal transport within the troposphere. The primary science objectives of GHOST are to: 1) provide observations which can be used to test atmospheric transport models; 2) validate satellite observations of GHG column observations over oceans, thus filling a critical gap in current validation capabilities; and 3) complement in-situ tropopause transition layer tracer observations from other instrumentation on board the Global Hawk to provide a link between upper and lower troposphere concentration measurements. The GHOST spectrometer system comprises a target acquisition module (TAM), a fibre slicer and feed system, and a multiple order spectrograph. The TAM design utilises a gimbal behind an optical dome, which is programmed to direct solar radiation reflected by the ocean surface into a fibre optic bundle. The fibre slicer and feed system then splits the light into the four spectral bands using order sorting filters. The fibres corresponding to each band are arranged with a small sideways offset to correctly centre each spectrum on the detector array. The spectrograph design is unique in that a

  10. Tropospheric ozone climatology at two Southern Hemisphere tropical/subtropical sites, (Reunion Island and Irene, South Africa from ozonesondes, LIDAR, and in situ aircraft measurements

    Directory of Open Access Journals (Sweden)

    G. Clain

    2009-03-01

    Full Text Available This paper presents a climatology and trends of tropospheric ozone in the Southwestern Indian Ocean (Reunion Island and South Africa (Irene and Johannesburg. This study is based on a multi-instrumental dataset: PTU-O3 ozonesondes, DIAL LIDAR and MOZAIC airborne instrumentation.

    The seasonal profiles of tropospheric ozone at Reunion Island have been calculated from two different data sets: ozonesondes and LIDAR. The two climatological profiles are similar, except in austral summer when the LIDAR profiles show greater values in the free troposphere, and in the upper troposphere when the LIDAR profiles show lower values during all seasons. These results show that the climatological value of LIDAR profiles must be discussed with care since LIDAR measurements can be performed only under clear sky conditions, and the upper limit of the profile depends on the signal strength.

    In addition, linear trends have been calculated from ozonesonde data at Reunion and Irene. Considering the whole tropospheric column, the trend is slightly positive for Reunion, and more clearly positive for Irene. Trend calculations have also been made separating the troposphere into three layers, and separating the dataset into seasons. Results show that the positive trend for Irene is governed by the lower layer that is affected by industrial pollution and biomass burning. On the contrary, for Reunion Island, the strongest trends are observed in the upper troposphere, and in winter when stratosphere-troposphere exchange is more frequently expected.

  11. Evidence of a tropospheric aerosol backscatter background mode

    Science.gov (United States)

    Rothermel, Jeffry; Bowdle, David A.; Vaughan, J. Michael; Post, Madison J.

    1989-01-01

    Vertical profiles of atmospheric aerosol backscatter coefficients at 10.6 microns obtained with airborne and ground-based lidar are compared. Both sets of profiles show a high frequency of occurrence of low backscatter over a limited range of values in the middle and upper troposphere. It is suggested that this narrow range indicates a ubiquitous background mode for atmospheric backscatter around the globe. Implications of such a mode for global scale aerosol models and for the design of satellite-borne lidar-based sensors are discussed.

  12. Tropospheric aerosol backscatter background mode at CO2 wavelengths

    Science.gov (United States)

    Rothermel, Jeffry; Bowdle, David A.; Menzies, Robert T.; Post, Madison J.; Vaughan, J. Michael

    1989-01-01

    A comparison is made between three climatologies of backscatter measurements in the troposphere and lower stratosphere at CO2 wavelengths. These were obtained from several locations using ground-based and airborne lidar systems. All three measurement sets show similar features, specifically, a high frequency of occurrence of low backscatter over a limited range of values in the middle and upper atmosphere (the 'background mode'). This background mode is important for the design and performance simulation of the prospective satellite sensors that rely on atmospheric aerosols as scattering targets.

  13. Investigating Quantum Mechanical Tunneling at the Nanoscale via Analogy: Development and Assessment of a Teaching Tool for Upper-Division Chemistry

    Science.gov (United States)

    Muniz, Marc N.; Oliver-Hoyo, Maria T.

    2014-01-01

    We report a novel educational activity designed to teach quantum mechanical tunneling to upper-division undergraduate students in the context of nanochemistry. The activity is based on a theoretical framework for analogy and is split into three parts that are linked pedagogically through the framework: classical ball-and-ramp system, tunneling…

  14. Instrumentation for tropospheric aerosol characterization

    Energy Technology Data Exchange (ETDEWEB)

    Shi, Z.; Young, S.E.; Becker, C.H.; Coggiola, M.J. [SRI International, Menlo Park, CA (United States); Wollnik, H. [Giessen Univ. (Germany)

    1997-12-31

    A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

  15. Instrumentation for tropospheric aerosol characterization

    Energy Technology Data Exchange (ETDEWEB)

    Shi, Z; Young, S E; Becker, C H; Coggiola, M J [SRI International, Menlo Park, CA (United States); Wollnik, H [Giessen Univ. (Germany)

    1998-12-31

    A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

  16. Analysis of the summertime buildup of tropospheric ozone abundances over the Middle East and North Africa as observed by the Tropospheric Emission Spectrometer instrument

    Science.gov (United States)

    Liu, Jane J.; Jones, Dylan B. A.; Worden, John R.; Noone, David; Parrington, Mark; Kar, Jay

    2009-03-01

    We use the GEOS-Chem chemical transport model to interpret observations of tropospheric ozone from the Tropospheric Emission Spectrometer (TES) satellite instrument in summer 2005. Observations from TES reveal elevated ozone in the middle troposphere (500-400 hPa) across North Africa and the Middle East. Observed ozone abundances in the middle troposphere are at a maximum in summer and a minimum in winter, consistent with the previously predicted summertime "Middle East ozone maximum." This summertime enhancement in ozone is associated with the Arabian and Sahara anticyclones, centered over the Zagros and Atlas Mountains, respectively. These anticyclones isolate the middle troposphere over northeast Africa and the Middle East, with westerlies to the north and easterlies to the south, facilitating the buildup of ozone. Over the Middle East, we find that in situ production and transport from Asia provides comparable contributions of 30-35% to the ozone buildup. Over North Africa, in situ production is dominant (at about 20%), with transport from Asia, North America, and equatorial Africa each contributing about 10-15% to the total ozone. We find that although the eastern Mediterranean is characterized by strong descent in the middle and upper troposphere in summer, transport from the boundary layer accounts for about 25% of the local Middle Eastern contribution to the ozone enhancement in the middle troposphere. This upward transport of boundary layer air is associated with orographic lifting along the Zagros Mountains in Iran and the Asir and Hijaz Mountain ranges in Saudi Arabia, and is consistent with TES observations of deuterated water.

  17. Two case studies on the interaction of large-scale transport, mesoscale photochemistry, and boundary-layer processes on the lower tropospheric ozone dynamics in early spring

    Directory of Open Access Journals (Sweden)

    S. Brönnimann

    Full Text Available The vertical distribution of ozone in the lower troposphere over the Swiss Plateau is investigated in detail for two episodes in early spring (February 1998 and March 1999. Profile measurements of boundary-layer ozone performed during two field campaigns with a tethered balloon sounding system and a kite are investigated using regular aerological and ozone soundings from a nearby site, measurements from monitoring stations at various altitudes, backward trajectories, and synoptic analyses of meteorological fields. Additionally, the effect of in situ photochemistry was estimated for one of the episodes employing the Metphomod Eulerian photochemical model. Although the meteorological situations were completely different, both cases had elevated layers with high ozone concentrations, which is not untypical for late winter and early spring. In the February episode, the highest ozone concentrations of 55 to 60 ppb, which were found at around 1100 m asl, were partly advected from Southern France, but a considerable contribution of in situ photochemistry is also predicted by the model. Below that elevation, the local chemical sinks and surface deposition probably overcompensated chemical production, and the vertical ozone distribution was governed by boundary-layer dynamics. In the March episode, the results suggest that ozone-rich air parcels, probably of stratospheric or upper tropospheric origin, were advected aloft the boundary layer on the Swiss Plateau.

    Key words. Atmospheric composition and structure (pollution – urban and regional; troposphere – composition and  chemistry – Meteorology and atmospheric dynamics (mesoscale meteorology

  18. 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

  19. Tropospheric effects of energy conversion

    International Nuclear Information System (INIS)

    Derwent, R.G.

    1992-01-01

    The tropospheric concentrations of a number of trace gases are increasing due to man's activities. For some trace gases, their atmospheric life cycles are not fully understood and it is difficult to be certain about the role of man's activities. Emissions from the energy industries and energy conversion processes represent an important subset of source terms in these life cycles, along with agriculture, deforestation, cement manufacture, biomass burning, process industries and natural biospheric processes. Global Warming Potentials (GWPs) allow the tropospheric effects of a range of climate forcing trace gases to be assessed on a comparable basis. If a short term view of the commitment to global warming is adopted then the contribution from other trace gases may approach and exceed that of carbon dioxide, itself. Over longer time horizons, the long atmospheric lifetime of carbon dioxide shows through as a major influence and the contributions from the other trace gases appear to be much smaller, representing an additional 13-18% contribution on top of that from CO 2 itself

  20. Radiation chemistry

    International Nuclear Information System (INIS)

    Rodgers, F.; Rodgers, M.A.

    1987-01-01

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

  1. Performance Evaluation of Blind Tropospheric Delay correction ...

    African Journals Online (AJOL)

    lekky

    and Temperature 2 wet (GPT2w) models) for tropospheric delay correction, ... In practice, a user often employs a certain troposphere model based on the popularity ... comparisons between some of the models have been carried out in the past for .... prediction of meteorological parameter values, which are then used to ...

  2. Sequence stratigraphy, organic petrology and chemistry applied to the upper and lower coal seams in the Candiota Coalfield, Parana Basin, RS, Brazil

    Energy Technology Data Exchange (ETDEWEB)

    Oliveira, J.S. de; Kalkreuth, W. [Instituto de Geociencias, UFRGS, Porto Alegre (Brazil)

    2010-12-01

    The Permian age coal seams in the Candiota Coalfield represent the largest coal deposit of the country. Currently two seams are mined, called ''Camada Candiota Superior'' and ''Camada Candiota Inferior''. The other coal seams of the coalfield, seams S1-S9 (upper seams) and I1-I5 (lower seams) have as yet not been exploited. The objective of this paper is to perform a detailed sequence stratigraphic, petrologic and chemical study of the upper and lower coal seams, thereby generating data for assisting in the development and better use of the coal-bearing interval. The methodology includes application of the concepts of sequence stratigraphy, which includes the lithological interpretation of the core to establish the depositional environments and genetic correlation between facies associations to define parasequences and bounding surfaces; coal petrology (analysis of the reflectance of vitrinite, determination of the petrographic composition of the coals by maceral analyses), and chemical analyses such as sulphur determination, proximate analyses (ash, moisture, volatile matter, and fixed carbon), and elemental analyses. Three main depositional systems were so far identified: alluvial fan, fluvial system, lagoonal estuary system. This study shows that coal development was controlled by accommodation/accumulation rates, with coal seams with greater thickness and lateral continuity being formed within the transgressive systems tract (lagoonal depositional system) of parasequence 2 (PS2), indicating that the accumulation rates of the peat and distribution of the coal seams were controlled by stratigraphic setting. Vitrinite reflectances for the upper and lower coal seams are indicative of subbituminous rank (Rrandom = 0.36-0.47%), with evidence that anomalously low reflectance values are related to high mineral-matter contents. Maceral composition is highly variable, with some coal seams being extremely rich in inertinite (up to

  3. Effects of Aircraft Wake Dynamics on Measured and Simulated NO(x) and HO(x) Wake Chemistry. Appendix B

    Science.gov (United States)

    Lewellen, D. C.; Lewellen, W. S.

    2001-01-01

    High-resolution numerical large-eddy simulations of the near wake of a B757 including simplified NOx and HOx chemistry were performed to explore the effects of dynamics on chemistry in wakes of ages from a few seconds to several minutes. Dilution plays an important basic role in the NOx-O3 chemistry in the wake, while a more interesting interaction between the chemistry and dynamics occurs for the HOx species. These simulation results are compared with published measurements of OH and HO2 within a B757 wake under cruise conditions in the upper troposphere taken during the Subsonic Aircraft Contrail and Cloud Effects Special Study (SUCCESS) mission in May 1996. The simulation provides a much finer grained representation of the chemistry and dynamics of the early wake than is possible from the 1 s data samples taken in situ. The comparison suggests that the previously reported discrepancy of up to a factor of 20 - 50 between the SUCCESS measurements of the [HO2]/[OH] ratio and that predicted by simplified theoretical computations is due to the combined effects of large mixing rates around the wake plume edges and averaging over volumes containing large species fluctuations. The results demonstrate the feasibility of using three-dimensional unsteady large-eddy simulations with coupled chemistry to study such phenomena.

  4. 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.

  5. Verification of an immunoturbidimetric assay for heart-type fatty acid-binding protein (H-FABP) on a clinical chemistry platform and establishment of the upper reference limit.

    Science.gov (United States)

    Da Molin, Simona; Cappellini, Fabrizio; Falbo, Rosanna; Signorini, Stefano; Brambilla, Paolo

    2014-11-01

    Heart-type fatty acid-binding protein (H-FABP) is an early biomarker of cardiac injury. Randox Laboratories developed an immunoturbidimetric H-FABP assay for non-proprietary automated clinical chemistry analysers that could be useful in the emergency department. We verified the analytical performances claimed by Randox Laboratories on Roche Cobas 6000 clinical chemistry platform in use in our laboratory, and we defined our own 99th percentile upper reference limit for H-FABP. For the verification of method performances, we used pools of spared patient samples from routine and two levels of quality control material, while samples for the reference value study were collected from 545 blood donors. Following CLSI guidelines we verified limit of blank (LOB), limit of detection (LOD), limit of quantitation (LOQ), repeatability and within-laboratory precision, trueness, linearity, and the stability of H-FABP in EDTA over 24h. The LOQ (3.19 μg/L) was verified with a CV% of 10.4. The precision was verified for the low (mean 5.88 μg/L, CV=6.7%), the medium (mean 45.28 μg/L, CV=3.0%), and the high concentration (mean 88.81 μg/L, CV=4.0%). The trueness was verified as well as the linearity over the indicated measurement interval of 0.747-120 μg/L. The H-FABP in EDTA samples is stable throughout 24h both at room temperature and at 4 °C. The H-FABP 99th percentile upper reference limit for all subjects (3.60 μg/L, 95% CI 3.51-3.77) is more appropriate than gender-specific ones that are not statistically different. Copyright © 2014 The Canadian Society of Clinical Chemists. Published by Elsevier Inc. All rights reserved.

  6. Why are models unable to reproduce multi-decadal trends in lower tropospheric baseline ozone levels?

    Science.gov (United States)

    Hu, L.; Liu, J.; Mickley, L. J.; Strahan, S. E.; Steenrod, S.

    2017-12-01

    Assessments of tropospheric ozone radiative forcing rely on accurate model simulations. Parrish et al (2014) found that three chemistry-climate models (CCMs) overestimate present-day O3 mixing ratios and capture only 50% of the observed O3 increase over the last five decades at 12 baseline sites in the northern mid-latitudes, indicating large uncertainties in our understanding of the ozone trends and their implications for radiative forcing. Here we present comparisons of outputs from two chemical transport models (CTMs) - GEOS-Chem and the Global Modeling Initiative model - with O3 observations from the same sites and from the global ozonesonde network. Both CTMs are driven by reanalysis meteorological data (MERRA or MERRA2) and thus are expected to be different in atmospheric transport processes relative to those freely running CCMs. We test whether recent model developments leading to more active ozone chemistry affect the computed ozone sensitivity to perturbations in emissions. Preliminary results suggest these CTMs can reproduce present-day ozone levels but fail to capture the multi-decadal trend since 1980. Both models yield widespread overpredictions of free tropospheric ozone in the 1980s. Sensitivity studies in GEOS-Chem suggest that the model estimate of natural background ozone is too high. We discuss factors that contribute to the variability and trends of tropospheric ozone over the last 30 years, with a focus on intermodel differences in spatial resolution and in the representation of stratospheric chemistry, stratosphere-troposphere exchange, halogen chemistry, and biogenic VOC emissions and chemistry. We also discuss uncertainty in the historical emission inventories used in models, and how these affect the simulated ozone trends.

  7. Study of stratosphere-troposphere exchange via 10Be/7Be isotope ratios

    International Nuclear Information System (INIS)

    Priller, A.; Berger, M.; Golser, R.; Kutschera, W.; Steier, P.; Vockenhuber, C.; Wild, E.M.

    2001-01-01

    Full text: The present study is part of the European project STACCATO (influence of stratosphere-troposphere exchange in a changing climate on atmospheric transport and oxidation capacity). Stratosphere-troposphere exchange (STE) is one of the key factors controlling the budgets of ozone, water vapor and other substances in both the troposphere and the lower stratosphere. However, its contribution to their ozone budget relative to photo-chemical ozone formation from natural and anthropogenic precursor emissions is still uncertain. An international effort is made to estimate the strength of STE and its impact on tropospheric chemistry. The two cosmogenic radioisotopes of beryllium, 10 Be and 7 Be have very different half-lives of 1.51 Ma and 53.4 d, respectively. The combination of production rates, half-lives and different residence times in the stratosphere and troposphere, respectively, results in 10 Be/ 7 Be isotope ratios which can be used as fingerprints for STE. This ratio helps to give a much improved estimate of STE. However, only few 10 Be measurements exist, because its detection requires the rather elaborate method of accelerator mass spectrometry (AMS). At the AMS facility VERA we are now measuring the 10 Be content of air filters from the high-alpine stations 'Hoher Sonnblick', Austria, and 'Zugspitze', Germany. The TBe content is measured separately by decay counting. In this presentation, we want to describe the method of measuring 10 Be with AMS, and to discuss the results of first 10 Be/ 7 Be ratios. (author)

  8. 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.)

  9. Tropospheric radiowave propagation beyond the horizon

    CERN Document Server

    Du Castel, François

    1966-01-01

    Tropospheric Radiowave Propagation Beyond the Horizon deals with developments concerning the tropospheric propagation of ultra-short radio waves beyond the horizon, with emphasis on the relationship between the theoretical and the experimental. Topics covered include the general conditions of propagation in the troposphere; general characteristics of propagation beyond the horizon; and attenuation in propagation. This volume is comprised of six chapters and begins with a brief historical look at the various stages that have brought the technique of transhorizon links to its state of developmen

  10. Stratospheric Ozone Distribution and Tropospheric General Circulation: Interconnections in the UTLS Region

    Science.gov (United States)

    Barodka, S.; Krasovsky, A.; Shalamyansky, A.

    2014-12-01

    The height of the tropopause, which divided the stratosphere and the troposphere, is a result of two rival categories of processes: the tropospheric vertical convection and the radiative heating of the stratosphere resulting from the ozone cycle. Hence, it is natural that tropospheric and stratospheric phenomena can have effect each other in manifold processes of stratosphere-troposphere interactions. In the present study we focus our attention to the "top-down" side of the interaction: the impact of stratospheric ozone distribution on the features of tropospheric circulation and the associated weather patterns and regional climate conditions. We proceed from analyzes of the observational data performed at the A.I. Voeikov Main Geophysical Observatory, which suggest a distinct correlation between stratospheric ozone distribution, synoptic formations and air-masses boundaries in the upper troposphere and the temperature field of the lower stratosphere [1]. Furthermore, we analyze local features of atmospheric general circulation and stratospheric ozone distribution from the atmospheric reanalyses and general circulation model data, focusing our attention to instantaneous positions of subtropical and polar stationary atmospheric fronts, which define regional characteristics of the general circulation cells in the troposphere and separate global tropospheric air-masses, correspond to distinct meteorological regimes in the TOC field [2, 3]. We assume that by altering the tropopause height, stratospheric ozone-related processes can have an impact on the location of the stationary atmospheric fronts, thereby exerting influence on circulation processes in troposphere and lower stratosphere. For midlatitudes, the tropopause height controls the position of the polar stationary front, which has a direct impact on the trajectory of motion of active vortices on synoptic tropospheric levels, thereby controlling weather patterns in that region and the regional climate. This

  11. 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...

  12. Unconventional Constraints on Nitrogen Chemistry using DC3 Observations and Trajectory-based Chemical Modeling

    Science.gov (United States)

    Shu, Q.; Henderson, B. H.

    2017-12-01

    Chemical transport models underestimate nitrogen dioxide observations in the upper troposphere (UT). Previous research in the UT succeeded in combining model predictions with field campaign measurements to demonstrate that the nitric acid formation rate (HO + NO2 → HNO3 (R1)) is overestimated by 22% (Henderson et al., 2012). A subsequent publication (Seltzer et al., 2015) demonstrated that single chemical constraint alters ozone and aerosol formation/composition. This work attempts to replicate previous chemical constraints with newer observations and a different modeling framework. We apply the previously successful constraint framework to Deep Convection Clouds and Chemistry (DC3). DC3 is a more recent field campaign where simulated nitrogen imbalances still exist. Freshly convected air parcels, identified in the DC3 dataset, as initial coordinates to initiate Lagrangian trajectories. Along each trajectory, we simulate the air parcel chemical state. Samples along the trajectories will form ensembles that represent possible realizations of UT air parcels. We then apply Bayesian inference to constrain nitrogen chemistry and compare results to the existing literature. Our anticipated results will confirm overestimation of HNO3 formation rate in previous work and provide further constraints on other nitrogen reaction rate coefficients that affect terminal products from NOx. We will particularly focus on organic nitrate chemistry that laboratory literature has yet to fully address. The results will provide useful insights into nitrogen chemistry that affects climate and human health.

  13. The use of satellite data to determine the distribution of ozone in the troposphere

    Science.gov (United States)

    Fishman, Jack; Watson, Catherine E.; Brackett, Vincent G.; Fakhruzzaman, Khan; Veiga, Robert E.

    1991-01-01

    Measurements from two independent satellite data sets have been used to derive the climatology of the integrated amount of ozone in the troposphere. These data have led to the finding that large amounts of ozone pollution are generated by anthropogenic activity originating from both the industrialized regions of the Northern Hemisphere and from the southern tropical regions of Africa. To verify the existence of this ozone anomaly at low latitudes, an ozonesonde capability has been established at Ascension Island (8 deg S, 15 deg W) since July 1990. According to the satellite analyses, Ascension Island is located downwind of the primary source region of this ozone pollution, which likely results from the photochemical oxidation of emissions emanating from the widespread burning of savannas and other biomass. These in situ measurements confirm the existence of large amounts of ozone in the lower atmosphere. A summary of these ozonesonde data to date will be presented. In addition, we will present some ozone profile measurements from SAGE II which can be used to provide upper tropospheric ozone measurements directly in the tropical troposphere. A preliminary comparison between the satellite observations and the ozonesonde profiles in the upper troposphere and lower stratosphere will also be presented.

  14. Concentration variations of the tropospheric carbon dioxide over the Antarctic region

    Directory of Open Access Journals (Sweden)

    Shohei Murayama

    1997-03-01

    Full Text Available Aircraft measurements of the atmospheric CO_2 concentration have been made over Syowa Station, Antarctica since 1983. The minimum concentration of the average seasonal CO_2 cycle appears in March throughout the troposphere, while the maximum concentration occurs in mid-August in the upper troposphere and in late September in the middle and lower troposphere. The peak-to-peak amplitude of the seasonal cycle decreases with height. The CO_2 concentration increases with height during most of the year; however, this height dependency is larger from summer to early winter than in the remaining seasons. The average concentration difference between the upper troposphere and the ground surface is about 0.3ppmv. From comparisons with the results of the ground-based and aircraft measurements at southern middle and high latitudes and trajectory analysis, it is hypothesized that the seasonal cycle of height-dependent atmospheric transport processes could influence the seasonal cycle and the vertical distribution of the CO_2 concentration over Syowa Station.

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

    Science.gov (United States)

    Sekiya, T.; Sudo, K.

    2014-04-01

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

  16. 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

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

    Science.gov (United States)

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

    1997-01-01

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

  18. The global impact of biomass burning on tropospheric reactive nitrogen

    International Nuclear Information System (INIS)

    Levy, H. II; Moxim, W.J.; Kasibhatla, P.S.; Logan, J.A.

    1991-01-01

    In this chapter the authors first review their current understanding of both the anthropogenic and natural sources of reactive nitrogen compounds in the troposphere. Then the available observations of both surface concentration and wet deposition are summarized for regions with significant sources, for locations downwind of strong sources, and for remote sites. The obvious sparsity of the data leads to the next step: an attempt to develop a more complete global picture of surface concentrations and deposition of NO y with the help of global chemistry transport model (GCTM). The available source data are inserted into the GCTM and the resulting simulations compared with surface observations. The impact of anthropogenic sources, both downwind and at remote locations, is discussed and the particular role of biomass burning is identified

  19. Connections among soil, ground, and surface water chemistries characterize nitrogen loss from an agricultural landscape in the upper Missouri River Basin

    Science.gov (United States)

    Sigler, W. Adam; Ewing, Stephanie A.; Jones, Clain A.; Payn, Robert A.; Brookshire, E. N. Jack; Klassen, Jane K.; Jackson-Smith, Douglas; Weissmann, Gary S.

    2018-01-01

    Elevated nitrate in shallow aquifers is common in agricultural areas and remediation requires an understanding of nitrogen (N) leaching at a variety of spatial scales. Characterization of the drivers of nitrate leaching at the mesoscale level (102-103 km2) is needed to bridge from field-scale observations to the landscape-scale context, allowing informed water resource management decisions. Here we explore patterns in nitrate leaching rates across a depositional landform in the northern Great Plains within the Upper Missouri Basin, where the predominant land use is non-irrigated small grain production, and nitrate-N concentrations above 10 mg L-1 are common. The shallow Moccasin terrace (260 km2) aquifer is bounded in vertical extent by underlying shale and is isolated from mountain front stream recharge, such that aquifer recharge is dominated by infiltration of precipitation through agricultural soils. This configuration presents a simple landform-scale water balance that we leveraged to estimate leaching rates using groundwater nitrate concentrations and surface water discharge, and quantify uncertainty using a Monte Carlo approach based on spatial variation in observations of groundwater nitrate concentrations. A participatory research approach allowed local farmer knowledge of the landscape to be incorporated into the study design, improved selection of and access to sample sites, and enhanced prospects for addressing nitrate leaching through collaborative understanding of system hydrology. Mean landform-scale nitrate-N leaching rates were 11 and 18 kg ha-1 yr-1 during the 2012-2014 study for the two largest catchments draining the terrace. Over a standard three-year crop rotation, these leaching rates represent 19-31% of typical fertilizer N application rates; however, leaching losses are likely derived not only from fertilizer but also from soil organic N mineralization, and are apparently higher during the post-fallow phase of the crop rotation. Groundwater

  20. Sr evolution in the Upper Permian and Lower Triassic carbonates, northeast Sichuan basin, China: Constraints from chemistry, isotope and fluid inclusions

    International Nuclear Information System (INIS)

    Li, Kaikai; Cai, Chunfang; Jiang, Lei; Cai, Liulu; Jia, Lianqi; Zhang, Bing; Xiang, Lei; Yuan, Yuyang

    2012-01-01

    Petrographic features, C, O and Sr isotopes, rare earth and trace elements were determined, and fluid inclusions were analyzed on various stages of interparticle cements and vug-fillings from the Upper Permian and Lower Triassic sour reservoirs in northeastern Sichuan basin. The aim was to assess the origin and evolution of palaeo-waters in the carbonates. The original water was contemporary seawater, from which marine cements precipitated with slightly high Sr contents (mean 1911 ppm), 87 Sr/ 86 Sr ratios from 0.7067 to 0.7082 and nonluminescent CL. The palaeo-seawater was diluted by meteoric water, as indicated by bright cathodoluminescence (CL) and Sr-depletion (0–516 ppm) in low-temperature calcite. When buried to temperatures of about 60–90 °C during Middle to Late Triassic, the palaeo-water was enriched in Sr released from the transformation of precursor aragonite and calcite to dolomite, resulting in precipitation of substantial pre-bitumen Sr-rich minerals (SrSO 4 and SrCO 3 ). For un-dolomitized limestone sections, aragonite neomorphism may have contributed Sr to the precipitation of small amounts of Sr-bearing minerals and calcite crystals with elevated homogenization temperatures (HTs, mainly from 90 to 130 °C) and wide Sr contents (from 34 to 3825 ppm), as recorded in stage III calcite. Since the Middle Jurassic, almost all of the early stage celestite and significant amounts of solid CaSO 4 have been consumed by reactions with hydrocarbons (i.e., TSR), resulting in water enriched in isotopically light CO 2 and HCO 3 - ,Sr 2+ ,Ba 2+ and Eu 2+ , as recorded in calcite with low δ 13 C values (down to −18.9‰), 87 Sr/ 86 Sr ratios from 0.7072 to 0.7076, high HTs (mainly 110–198 °C), positive Eu anomalies and high Sr and Ba contents. Subsequently, the water was uplifted and cooled down to about 115 °C, celestite and strontianite were precipitated with the occurrence of natural elemental S immiscible inclusions. TSR may have produced

  1. Bad chemistry

    OpenAIRE

    Petsko, Gregory A

    2004-01-01

    General chemistry courses haven't changed significantly in forty years. Because most basic chemistry students are premedical students, medical schools have enormous influence and could help us start all over again to create undergraduate chemistry education that works.

  2. Spatial variability of the structure of the lower troposphere over north western Indian Ocean during 1983 summer monsoon

    Digital Repository Service at National Institute of Oceanography (India)

    RameshKumar, M.R.; Sadhuram, Y.; Michael, G.S.; Rao, L.V.G.

    The spatial variability of the structure of the lower troposphere over the north western Indian Ocean during the period 12th July to 2nd September, 1983 has been studied using the upper air data collected during the first scientific cruise of @i...

  3. Impact of aircraft emissions on the atmospheric chemistry

    Energy Technology Data Exchange (ETDEWEB)

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

    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.

  4. Impact of aircraft emissions on the atmospheric chemistry

    Energy Technology Data Exchange (ETDEWEB)

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

    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.

  5. Origin of oxidized mercury in the summertime free troposphere over the southeastern US

    Directory of Open Access Journals (Sweden)

    V. Shah

    2016-02-01

    Full Text Available We collected mercury observations as part of the Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS aircraft campaign over the southeastern US between 1 June and 15 July 2013. We use the GEOS-Chem chemical transport model to interpret these observations and place new constraints on bromine radical initiated mercury oxidation chemistry in the free troposphere. We find that the model reproduces the observed mean concentration of total atmospheric mercury (THg (observations: 1.49 ± 0.16 ng m−3, model: 1.51 ± 0.08 ng m−3, as well as the vertical profile of THg. The majority (65 % of observations of oxidized mercury (Hg(II were below the instrument's detection limit (detection limit per flight: 58–228 pg m−3, consistent with model-calculated Hg(II concentrations of 0–196 pg m−3. However, for observations above the detection limit we find that modeled Hg(II concentrations are a factor of 3 too low (observations: 212 ± 112 pg m−3, model: 67 ± 44 pg m−3. The highest Hg(II concentrations, 300–680 pg m−3, were observed in dry (RH  <  35 % and clean air masses during two flights over Texas at 5–7 km altitude and off the North Carolina coast at 1–3 km. The GEOS-Chem model, back trajectories and observed chemical tracers for these air masses indicate subsidence and transport from the upper and middle troposphere of the subtropical anticyclones, where fast oxidation of elemental mercury (Hg(0 to Hg(II and lack of Hg(II removal lead to efficient accumulation of Hg(II. We hypothesize that the most likely explanation for the model bias is a systematic underestimate of the Hg(0 + Br reaction rate. We find that sensitivity simulations with tripled bromine radical concentrations or a faster oxidation rate constant for Hg(0 + Br, result in 1.5–2 times higher modeled Hg(II concentrations and improved agreement with the observations. The modeled

  6. Northern Winter Climate Change: Assessment of Uncertainty in CMIP5 Projections Related to Stratosphere-Troposphere Coupling

    Science.gov (United States)

    Manzini, E.; Karpechko, A.Yu.; Anstey, J.; Shindell, Drew Todd; Baldwin, M.P.; Black, R.X.; Cagnazzo, C.; Calvo, N.; Charlton-Perez, A.; Christiansen, B.; hide

    2014-01-01

    Future changes in the stratospheric circulation could have an important impact on northern winter tropospheric climate change, given that sea level pressure (SLP) responds not only to tropospheric circulation variations but also to vertically coherent variations in troposphere-stratosphere circulation. Here we assess northern winter stratospheric change and its potential to influence surface climate change in the Coupled Model Intercomparison Project-Phase 5 (CMIP5) multimodel ensemble. In the stratosphere at high latitudes, an easterly change in zonally averaged zonal wind is found for the majority of the CMIP5 models, under the Representative Concentration Pathway 8.5 scenario. Comparable results are also found in the 1% CO2 increase per year projections, indicating that the stratospheric easterly change is common feature in future climate projections. This stratospheric wind change, however, shows a significant spread among the models. By using linear regression, we quantify the impact of tropical upper troposphere warming, polar amplification, and the stratospheric wind change on SLP. We find that the intermodel spread in stratospheric wind change contributes substantially to the intermodel spread in Arctic SLP change. The role of the stratosphere in determining part of the spread in SLP change is supported by the fact that the SLP change lags the stratospheric zonally averaged wind change. Taken together, these findings provide further support for the importance of simulating the coupling between the stratosphere and the troposphere, to narrow the uncertainty in the future projection of tropospheric circulation changes.

  7. Impact of climate change on tropospheric ozone and its global budgets

    Directory of Open Access Journals (Sweden)

    G. Zeng

    2008-01-01

    Full Text Available We present the chemistry-climate model UMCAM in which a relatively detailed tropospheric chemical module has been incorporated into the UK Met Office's Unified Model version 4.5. We obtain good agreements between the modelled ozone/nitrogen species and a range of observations including surface ozone measurements, ozone sonde data, and some aircraft campaigns.

    Four 2100 calculations assess model responses to projected changes of anthropogenic emissions (SRES A2, climate change (due to doubling CO2, and idealised climate change-associated changes in biogenic emissions (i.e. 50% increase of isoprene emission and doubling emissions of soil-NOx. The global tropospheric ozone burden increases significantly for all the 2100 A2 simulations, with the largest response caused by the increase of anthropogenic emissions. Climate change has diverse impacts on O3 and its budgets through changes in circulation and meteorological variables. Increased water vapour causes a substantial ozone reduction especially in the tropical lower troposphere (>10 ppbv reduction over the tropical ocean. On the other hand, an enhanced stratosphere-troposphere exchange of ozone, which increases by 80% due to doubling CO2, contributes to ozone increases in the extratropical free troposphere which subsequently propagate to the surface. Projected higher temperatures favour ozone chemical production and PAN decomposition which lead to high surface ozone levels in certain regions. Enhanced convection transports ozone precursors more rapidly out of the boundary layer resulting in an increase of ozone production in the free troposphere. Lightning-produced NOx increases by about 22% in the doubled CO2 climate and contributes to ozone production.

    The response to the increase of isoprene emissions shows that the change of ozone is largely determined by background NOx levels: high

  8. Effects of 1997-1998 El Nino on Tropospheric Ozone and Water Vapor

    Science.gov (United States)

    Chandra, S.; Ziemke, J. R.; Min, W.; Read, W. G.

    1998-01-01

    This paper analyzes the impact of the 1997-1998 El Nino on tropospheric column ozone and tropospheric water vapor derived respectively from the Total Ozone Mapping Spectrometer (TOMS) on Earth Probe and the Microwave Limb Scanning instrument on the Upper Atmosphere Research Satellite. The 1997-1998 El Nino, characterized by an anomalous increase in sea-surface temperature (SST) across the eastern and central tropical Pacific Ocean, is one of the strongest El Nino Southern Oscillation (ENSO) events of the century, comparable in magnitude to the 1982-1983 episode. The major impact of the SST change has been the shift in the convection pattern from the western to the eastern Pacific affecting the response of rain-producing cumulonimbus. As a result, there has been a significant increase in rainfall over the eastern Pacific and a decrease over the western Pacific and Indonesia. The dryness in the Indonesian region has contributed to large-scale burning by uncontrolled wildfires in the tropical rainforests of Sumatra and Borneo. Our study shows that tropospheric column ozone decreased by 4-8 Dobson units (DU) in the eastern Pacific and increased by about 10-20 DU in the western Pacific largely as a result of the eastward shift of the tropical convective activity as inferred from National Oceanic and Atmospheric Administration (NOAA) outgoing longwave radiation (OLR) data. The effect of this shift is also evident in the upper tropospheric water vapor mixing ratio which varies inversely as ozone (O3). These conclusions are qualitatively consistent with the changes in atmospheric circulation derived from zonal and vertical wind data obtained from the Goddard Earth Observing System data assimilation analyses. The changes in tropospheric column O3 during the course of the 1997-1998 El Nino appear to be caused by a combination of large-scale circulation processes associated with the shift in the tropical convection pattern and surface/boundary layer processes associated with

  9. A Global Climatology of Tropospheric and Stratospheric Ozone Derived from Aura OMI and MLS Measurements

    Science.gov (United States)

    Ziemke, J.R.; Chandra, S.; Labow, G.; Bhartia, P. K.; Froidevaux, L.; Witte, J. C.

    2011-01-01

    A global climatology of tropospheric and stratospheric column ozone is derived by combining six years of Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) ozone measurements for the period October 2004 through December 2010. The OMI/MLS tropospheric ozone climatology exhibits large temporal and spatial variability which includes ozone accumulation zones in the tropical south Atlantic year-round and in the subtropical Mediterranean! Asia region in summer months. High levels of tropospheric ozone in the northern hemisphere also persist in mid-latitudes over the eastern North American and Asian continents extending eastward over the Pacific Ocean. For stratospheric ozone climatology from MLS, largest ozone abundance lies in the northern hemisphere in the latitude range 70degN-80degN in February-April and in the southern hemisphere around 40degS-50degS during months August-October. The largest stratospheric ozone abundances in the northern hemisphere lie over North America and eastern Asia extending eastward across the Pacific Ocean and in the southern hemisphere south of Australia extending eastward across the dateline. With the advent of many newly developing 3D chemistry and transport models it is advantageous to have such a dataset for evaluating the performance of the models in relation to dynamical and photochemical processes controlling the ozone distributions in the troposphere and stratosphere.

  10. A Review of Low Frequency Electromagnetic Wave Phenomena Related to Tropospheric-Ionospheric Coupling Mechanisms

    Science.gov (United States)

    Simoes, Fernando; Pfaff, Robert; Berthelier, Jean-Jacques; Klenzing, Jeffrey

    2012-01-01

    Investigation of coupling mechanisms between the troposphere and the ionosphere requires a multidisciplinary approach involving several branches of atmospheric sciences, from meteorology, atmospheric chemistry, and fulminology to aeronomy, plasma physics, and space weather. In this work, we review low frequency electromagnetic wave propagation in the Earth-ionosphere cavity from a troposphere-ionosphere coupling perspective. We discuss electromagnetic wave generation, propagation, and resonance phenomena, considering atmospheric, ionospheric and magnetospheric sources, from lightning and transient luminous events at low altitude to Alfven waves and particle precipitation related to solar and magnetospheric processes. We review in situ ionospheric processes as well as surface and space weather phenomena that drive troposphere-ionosphere dynamics. Effects of aerosols, water vapor distribution, thermodynamic parameters, and cloud charge separation and electrification processes on atmospheric electricity and electromagnetic waves are reviewed. We also briefly revisit ionospheric irregularities such as spread-F and explosive spread-F, sporadic-E, traveling ionospheric disturbances, Trimpi effect, and hiss and plasma turbulence. Regarding the role of the lower boundary of the cavity, we review transient surface phenomena, including seismic activity, earthquakes, volcanic processes and dust electrification. The role of surface and atmospheric gravity waves in ionospheric dynamics is also briefly addressed. We summarize analytical and numerical tools and techniques to model low frequency electromagnetic wave propagation and solving inverse problems and summarize in a final section a few challenging subjects that are important for a better understanding of tropospheric-ionospheric coupling mechanisms.

  11. Supplemental Instruction in Physical Chemistry I

    Science.gov (United States)

    Toby, Ellen; Scott, Timothy P.; Migl, David; Kolodzeji, Elizabeth

    2016-01-01

    Physical chemistry I at Texas A&M University is an upper division course requiring mathematical and analytical skills. As such, this course poses a major problem for many Chemistry, Engineering, Biochemistry and Genetics majors. Comparisons between participants and non-participants in Supplemental Instruction for physical chemistry were made…

  12. Upper-Level Waves of Synoptic Scale at Midlatitudes

    Science.gov (United States)

    Rivest, Chantal

    1990-01-01

    Upper-level waves of synoptic scale are important dynamical entities at midlatitudes. They often induce surface cyclogenesis (cf. Peterssen and Smebye, 1971), and their life duration is typically longer than time scales for disruption by the ambient shear (Sanders, 1988). The objectives of the present thesis are to explain the maintenance and genesis of upper-level synoptic-scale waves in the midlatitude flow. We develop an analytical model of waves on generalized Eady basic states that have uniform tropospheric and stratospheric potential vorticity, but allow for the decay of density with height. The Eady basic state represents the limiting case of infinite stratospheric stability and constant density. We find that the Eady normal mode characteristics hold in the presence of realistic tropopause and stratosphere. In particular, the basic states studied support at the synoptic scale upper-level normal modes. These modes provide simple models for the dynamics of upper-level synoptic-scale waves, as waves supported by the large latitudinal gradients of potential vorticity at the tropopause. In the presence of infinitesimal positive tropospheric gradients of potential vorticity, the upper-level normal mode solutions no longer exist, as was demonstrated in Green (1960). Disappearance of the normal mode solution when a parameter changes slightly represents a dilemma that we seek to understand. We examine what happens to the upper-level normal modes in the presence of tropospheric gradients of potential vorticity in a series of initial -value experiments. Our results show that the normal modes become slowly decaying quasi-modes. Mathematically the quasi-modes consist of a superposition of singular modes sharply peaked in the phase speed domain, and their decay proceeds as the modes interfere with one another. We repeat these experiments in basic states with a smooth tropopause in the presence of tropospheric and stratospheric gradients, and similar results are obtained

  13. Complex chemistry

    International Nuclear Information System (INIS)

    Kim, Bong Gon; Kim, Jae Sang; Kim, Jin Eun; Lee, Boo Yeon

    2006-06-01

    This book introduces complex chemistry with ten chapters, which include development of complex chemistry on history coordination theory and Warner's coordination theory and new development of complex chemistry, nomenclature on complex with conception and define, chemical formula on coordination compound, symbol of stereochemistry, stereo structure and isomerism, electron structure and bond theory on complex, structure of complex like NMR and XAFS, balance and reaction on solution, an organo-metallic chemistry, biology inorganic chemistry, material chemistry of complex, design of complex and calculation chemistry.

  14. The global distribution of tropospheric NO{sub x} estimated by a 3-D chemical tracer model

    Energy Technology Data Exchange (ETDEWEB)

    Kraus, A B; Rohrer, F; Ehhalt, D H [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

    1998-12-31

    The global distribution of NO{sub x} in the troposphere is calculated using a three-dimensional chemical tracer model with a simplified chemistry scheme for the tracers NO{sub x} {identical_to} NO + NO{sub 2} and HNO{sub 3}. At northern mid- and high latitudes, the calculated tropospheric NO{sub x} content is dominated by the surface source fossil fuel combustion. In the tropical free troposphere lightning discharges provide about 80% of the total NO{sub x} throughout the year. The zonally averaged fractional contribution of aircraft emissions strongly depends on season. The NO mixing ratios determined by the model show good overall agreement with corresponding zonal mean values observed during the STRATOZ III aircraft campaign in June. Over Canada, mixing ratios as high as 0.5-1.0 ppbv NO were measured during TROPOZ II, the origin of which is not yet understood. (author) 8 refs.

  15. The global distribution of tropospheric NO{sub x} estimated by a 3-D chemical tracer model

    Energy Technology Data Exchange (ETDEWEB)

    Kraus, A.B.; Rohrer, F.; Ehhalt, D.H. [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

    1997-12-31

    The global distribution of NO{sub x} in the troposphere is calculated using a three-dimensional chemical tracer model with a simplified chemistry scheme for the tracers NO{sub x} {identical_to} NO + NO{sub 2} and HNO{sub 3}. At northern mid- and high latitudes, the calculated tropospheric NO{sub x} content is dominated by the surface source fossil fuel combustion. In the tropical free troposphere lightning discharges provide about 80% of the total NO{sub x} throughout the year. The zonally averaged fractional contribution of aircraft emissions strongly depends on season. The NO mixing ratios determined by the model show good overall agreement with corresponding zonal mean values observed during the STRATOZ III aircraft campaign in June. Over Canada, mixing ratios as high as 0.5-1.0 ppbv NO were measured during TROPOZ II, the origin of which is not yet understood. (author) 8 refs.

  16. Mathematical Chemistry

    OpenAIRE

    Trinajstić, Nenad; Gutman, Ivan

    2002-01-01

    A brief description is given of the historical development of mathematics and chemistry. A path leading to the meeting of these two sciences is described. An attempt is made to define mathematical chemistry, and journals containing the term mathematical chemistry in their titles are noted. In conclusion, the statement is made that although chemistry is an experimental science aimed at preparing new compounds and materials, mathematics is very useful in chemistry, among other things, to produc...

  17. Stratospheric ozone intrusion events and their impacts on tropospheric ozone in the Southern Hemisphere

    Directory of Open Access Journals (Sweden)

    J. W. Greenslade

    2017-09-01

    Full Text Available Stratosphere-to-troposphere transport (STT provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the Southern Hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality of STT events and quantify the ozone transported across the tropopause over Davis (69° S, 2006–2013, Macquarie Island (54° S, 2004–2013, and Melbourne (38° S, 2004–2013. STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile and an analysis of the Brunt–Väisälä frequency. Using a bandpass filter on 7–9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter for all three sites. The majority of tropospheric ozone enhancements owing to STT events occur within 2.5 and 3 km of the tropopause at Davis and Macquarie Island respectively. Events are more spread out at Melbourne, occurring frequently up to 6 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is  ∼ 1. 0–3. 5 % at each site; however, during individual events, over 10 % of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low-pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, which are apparent during austral winter and spring and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely

  18. Spectropolarimetric Measurements of Scattered Sunlight in the Huggins Bands: Retrieval of Tropospheric Ozone Profiles

    Science.gov (United States)

    Fu, D.; Sander, S. P.; Stutz, J.; Pongetti, T. J.; Yung, Y. L.; Wong, M.; Natraj, V.; Li, K.; Shia, R.

    2009-12-01

    Ozone concentrations in the troposphere have increased over the past century as a result of anthropogenic emissions of NOx and volatile organic compounds. In addition to being harmful to human health and plant life, ozone is an important greenhouse gas, especially in the middle and upper troposphere. Therefore, accurate monitoring of tropospheric ozone vertical distributions is crucial for a better understanding of air quality and climate change. Simulations of vector radiative transfer in the near ultraviolet region have shown that tropospheric ozone profiles can be retrieved using polarization measurements. However, to date there has been no experimental test of this method. A new compact, portable spectropolarimeter has been built for atmospheric remote sensing. The first comprehensive description of the configuration and performance of this instrument for ground-based operation is provided and sample atmospheric scattered sunlight spectra are shown. Using optimal estimation retrieval theory we study the information content of polarization spectra in the Huggins band and uncertainties in the retrieval associated with the measurement parameters, such as aerosol scattering.

  19. 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.

  20. Drivers of the tropospheric ozone budget throughout the 21st century under the medium-high climate scenario RCP 6.0

    Science.gov (United States)

    Revell, L. E.; Tummon, F.; Stenke, A.; Sukhodolov, T.; Coulon, A.; Rozanov, E.; Garny, H.; Grewe, V.; Peter, T.

    2015-05-01

    Because tropospheric ozone is both a greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry-climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NOx), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change (including methane effects) and stratospheric ozone recovery on the tropospheric ozone budget, in a simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0 (a medium-high, and reasonably realistic climate scenario). Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximizes in the early 21st century at 23% compared to 1960. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70-year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally averaged northern midlatitude ozone because of increasing emissions from Asia, together with the long lifetime of ozone in the troposphere. A simulation with fixed anthropogenic ozone precursor emissions of NOx, CO and non-methane VOCs at 1960 conditions shows a 6% increase in global-mean tropospheric ozone by the end of the 21st century, with an 11 % increase at northern midlatitudes. This increase maximizes in the 2080s and is mostly caused by methane, which maximizes in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its

  1. Results from the July 1981 Workshop on Passive Remote Sensing of the Troposphere

    International Nuclear Information System (INIS)

    Keafer, L.S. Jr.; Reichle, H.G. Jr.

    1982-01-01

    Potential roles of passive remote sensors in the study of the chemistry and related dynamics of the lower atmosphere were defined by a Tropospheric Passive Remote Sensing Workshop, and technology advances required to implement these roles were identified. A promising role is in making global-scale, multilayer measurements of the more abundant trace tropospheric gaseous species (e.g., O 3 , CO, CH 4 , HNO 3 ) and of aerosol thickness and size distribution. It includes both nadirand limb-viewing measurements. Technology advances focus on both scanning- and fixed-spectra, nadir-viewing techniques with resolutions of 0.1 kaysers or better. Balloon- and Shuttle-borne experiments should be performed to study the effects of instrument noise and background fluctuations on data inversion and to determine the utility of simultaneously obtained nadir- and limb-viewing data

  2. Tropospheric Ozone from the TOMS TDOT (TOMS-Direct-Ozone-in-Troposphere) Technique During SAFARI-2000

    Science.gov (United States)

    Stone, J. B.; Thompson, A. M.; Frolov, A. D.; Hudson, R. D.; Bhartia, P. K. (Technical Monitor)

    2002-01-01

    There are a number of published residual-type methods for deriving tropospheric ozone from TOMS (Total Ozone Mapping Spectrometer). The basic concept of these methods is that within a zone of constant stratospheric ozone, the tropospheric ozone column can be computed by subtracting stratospheric ozone from the TOMS Level 2 total ozone column, We used the modified-residual method for retrieving tropospheric ozone during SAFARI-2000 and found disagreements with in-situ ozone data over Africa in September 2000. Using the newly developed TDOT (TOMS-Direct-Ozone-in-Troposphere) method that uses TOMS radiances and a modified lookup table based on actual profiles during high ozone pollution periods, new maps were prepared and found to compare better to soundings over Lusaka, Zambia (15.5 S, 28 E), Nairobi and several African cities where MOZAIC aircraft operated in September 2000. The TDOT technique and comparisons are described in detail.

  3. Performance Evaluation of Blind Tropospheric Delay correction ...

    African Journals Online (AJOL)

    This report represents an appraisal of the performance of the GPT2w and UNB3M models with accurate International GNSS Service (IGS)- tropospheric estimations for fifteen IGS stations over a period of 1 year on the Africa continent. Both models perform significantly better at low latitudes than higher latitudes. There was ...

  4. Tropospheric ozone. Formation, properties, effects. Expert opinion

    International Nuclear Information System (INIS)

    Elstner, E.F.

    1996-01-01

    The formation and dispersion of tropospheric ozone are discussed only marginally in this expert opinion; the key interest is in the effects of ground level ozone on plants, animals, and humans. The expert opinion is based on an analysis of the available scientific publications. (orig./MG) [de

  5. TROPOSPHERIC AEROSOL PROGRAM, PROGRAM PLAN, MARCH 2001

    Energy Technology Data Exchange (ETDEWEB)

    SCHWARTZ,S.E.; LUNN,P.

    2001-03-01

    The goal of Tropospheric Aerosol Program (TAP) will be to develop the fundamental scientific understanding required to construct tools for simulating the life cycle of tropospheric aerosols--the processes controlling their mass loading, composition, and microphysical properties, all as a function of time, location, and altitude. The TAP approach to achieving this goal will be by conducting closely linked field, modeling, laboratory, and theoretical studies focused on the processes controlling formation, growth, transport, and deposition of tropospheric aerosols. This understanding will be represented in models suitable for describing these processes on a variety of geographical scales; evaluation of these models will be a key component of TAP field activities. In carrying out these tasks TAP will work closely with other programs in DOE and in other Federal and state agencies, and with the private sector. A forum to directly work with our counterparts in industry to ensure that the results of this research are translated into products that are useful to that community will be provided by NARSTO (formerly the North American Research Strategy on Tropospheric Ozone), a public/private partnership, whose membership spans government, the utilities, industry, and university researchers in Mexico, the US, and Canada.

  6. Impact of biogenic terpene emissions from Brassica napus on tropospheric ozone over Saxony (Germany): numerical investigation.

    Science.gov (United States)

    Renner, Eberhard; Münzenberg, Annette

    2003-01-01

    The role of biogenic emissions in tropospheric ozone production is currently under discussion and major aspects are not well understood yet. This study aims towards the estimation of the influence of biogenic emissions on tropospheric ozone concentrations over Saxony in general and of biogenic emissions from brassica napus in special. MODELLING TOOLS: The studies are performed by utilizing a coupled numerical modelling system consisting of the meteorological model METRAS and the chemistry transport model MUSCAT. For the chemical part, the Euro-RADM algorithm is used. EMISSIONS: Anthropogenic and biogenic emissions are taken into account. The anthropogenic emissions are introduced by an emission inventory. Biogenic emissions, VOC and NO, are calculated within the chemical transport model MUSCAT at each time step and in each grid cell depending on land use type and on the temperature. The emissions of hydrocarbons from forest areas as well as biogenic NO especially from agricultural grounds are considered. Also terpene emissions from brassica napus fields are estimated. SIMULATION SETUP AND METEOROLOGICAL CONDITIONS: The simulations were performed over an area with an extension of 160 x 140 km2 which covers the main parts of Saxony and neighboring areas of Brandenburg, Sachsen-Anhalt and Thuringia. Summer smog with high ozone concentrations can be expected during high pressure conditions on hot summer days. Typical meteorological conditions for such cases were introduced in an conceptual way. It is estimated that biogenic emissions change tropospheric ozone concentrations in a noticeable way (up to 15% to 20%) and, therefore, should not be neglected in studies about tropospheric ozone. Emissions from brassica napus do have a moderate potential to enhance tropospheric ozone concentrations, but emissions are still under consideration and, therefore, results vary to a high degree. Summing up, the effect of brassica napus terpene emissions on ozone concentrations is

  7. The influence of African air pollution on regional and global tropospheric ozone

    Directory of Open Access Journals (Sweden)

    A. M. Aghedo

    2007-01-01

    Full Text Available We investigate the influence of African biomass burning, biogenic, lightning and anthropogenic emissions on the tropospheric ozone over Africa and globally using a coupled global chemistry climate model. Our model studies indicate that surface ozone concentration may rise by up to 50 ppbv in the burning region during the biomass burning seasons. Biogenic emissions yield between 5–30 ppbv increase in the near surface ozone concentration over tropical Africa. The impact of lightning on surface ozone is negligible, while anthropogenic emissions yield a maximum of 7 ppbv increase in the annual-mean surface ozone concentration over Nigeria, South Africa and Egypt. Our results show that biogenic emissions are the most important African emission source affecting total tropospheric ozone. The influence of each of the African emissions on the global tropospheric ozone burden (TOB of 384 Tg yields about 9.5 Tg, 19.6 Tg, 9.0 Tg and 4.7 Tg for biomass burning, biogenic, lightning and anthropogenic emissions emitted in Africa respectively. The impact of each of these emission categories on African TOB of 33 Tg is 2.5 Tg, 4.1 Tg, 1.75 Tg and 0.89 Tg respectively, which together represents about 28% of the total TOB calculated over Africa. Our model calculations also suggest that more than 70% of the tropospheric ozone produced by each of the African emissions is found outside the continent, thus exerting a noticeable influence on a large part of the tropical troposphere. Apart from the Atlantic and Indian Ocean, Latin America experiences the largest impact of African emissions, followed by Oceania, the Middle East, Southeast and south-central Asia, northern North America (i.e. the United States and Canada, Europe and north-central Asia, for all the emission categories.

  8. Quantifying the causes of differences in tropospheric OH within global models

    Science.gov (United States)

    Nicely, Julie M.; Salawitch, Ross J.; Canty, Timothy; Anderson, Daniel C.; Arnold, Steve R.; Chipperfield, Martyn P.; Emmons, Louisa K.; Flemming, Johannes; Huijnen, Vincent; Kinnison, Douglas E.; Lamarque, Jean-François; Mao, Jingqiu; Monks, Sarah A.; Steenrod, Stephen D.; Tilmes, Simone; Turquety, Solene

    2017-02-01

    The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (τCH4) between these models. Annual average τCH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in τCH4 (ΔτCH4) result from variations in chemical mechanisms (ΔτCH4 = 0.46 years), the photolysis frequency (J) of O3 → O(1D) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The ΔτCH4 due to CTM differences in NOx (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NOx. Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.

  9. Momentum flux associated with gravity waves in the low-latitude troposphere

    Directory of Open Access Journals (Sweden)

    S. R. Prabhakaran Nayar

    Full Text Available The vertical fluxes of horizontal momentum at tropospheric heights are calculated for four days, 25–28 August 1999. The mean zonal wind during these days show the presence of strong westward wind at the upper troposphere. Both the symmetric beam radar method and the power spectral method of evaluation of vertical flux of zonal and meridional momentum shows nearly the same result for quiet conditions. The temporal evolution of the momentum flux is estimated for a day with strong zonal shear and convection. These results indicate that on 28 August 1999, the strong downward vertical wind in the lower altitude range is associated with upward vertical flux of zonal momentum, and strong upward vertical wind is associated with downward vertical flux. Similarly, the strong shear in zonal wind is associated with the increase in negative values in vertical flux in the upper troposphere. Analysis of the role of wave periods in the transport of momentum flux indicates that the vertical momentum flux magnitude is not evenly distributed in all wave periods, but instead it peaks at certain wave periods in the range 10 to 100 min.

    Key words. Meteorology and atmospheric dynamics (convective process; tropical meteorology; precipitation

  10. Assimilation of IASI partial tropospheric columns with an Ensemble Kalman Filter over Europe

    Directory of Open Access Journals (Sweden)

    A. Coman

    2012-03-01

    Full Text Available Partial lower tropospheric ozone columns provided by the IASI (Infrared Atmospheric Sounding Interferometer instrument have been assimilated into a chemistry-transport model at continental scale (CHIMERE using an Ensemble Square Root Kalman Filter (EnSRF. Analyses are made for the month of July 2007 over the European domain. Launched in 2006, aboard the MetOp-A satellite, IASI shows high sensitivity for ozone in the free troposphere and low sensitivity at the ground; therefore it is important to evaluate if assimilation of these observations can improve free tropospheric ozone, and possibly surface ozone. The analyses are validated against independent ozone observations from sondes, MOZAIC1 aircraft and ground based stations (AIRBASE – the European Air quality dataBase and compared with respect to the free run of CHIMERE. These comparisons show a decrease in error of 6 parts-per-billion (ppb in the free troposphere over the Frankfurt area, and also a reduction of the root mean square error (respectively bias at the surface of 19% (33% for more than 90% of existing ground stations. This provides evidence of the potential of data assimilation of tropospheric IASI columns to better describe the tropospheric ozone distribution, including surface ozone, despite the lower sensitivity.

    The changes in concentration resulting from the observational constraints were quantified and several geophysical explanations for the findings of this study were drawn. The corrections were most pronounced over Italy and the Mediterranean region, we noted an average reduction of 8–9 ppb in the free troposphere with respect to the free run, and still a reduction of 5.5 ppb at ground, likely due to a longer residence time of air masses in this part associated to the general circulation pattern (i.e. dominant western circulation and to persistent anticyclonic conditions over the Mediterranean basin. This is an important geophysical result, since the

  11. Chemistry Notes

    Science.gov (United States)

    School Science Review, 1976

    1976-01-01

    Described are eight chemistry experiments and demonstrations applicable to introductory chemistry courses. Activities include: measure of lattice enthalpy, Le Chatelier's principle, decarboxylation of soap, use of pocket calculators in pH measurement, and making nylon. (SL)

  12. Chemistry Dashboard

    Science.gov (United States)

    The Chemistry Dashboard is part of a suite of dashboards developed by EPA to help evaluate the safety of chemicals. The Chemistry Dashboard provides access to a variety of information on over 700,000 chemicals currently in use.

  13. Ground-based remote sensing of tropospheric water vapour isotopologues within the project MUSICA

    Directory of Open Access Journals (Sweden)

    M. Schneider

    2012-12-01

    Full Text Available Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water, long-term tropospheric water vapour isotopologue data records are provided for ten globally distributed ground-based mid-infrared remote sensing stations of the NDACC (Network for the Detection of Atmospheric Composition Change. We present a new method allowing for an extensive and straightforward characterisation of the complex nature of such isotopologue remote sensing datasets. We demonstrate that the MUSICA humidity profiles are representative for most of the troposphere with a vertical resolution ranging from about 2 km (in the lower troposphere to 8 km (in the upper troposphere and with an estimated precision of better than 10%. We find that the sensitivity with respect to the isotopologue composition is limited to the lower and middle troposphere, whereby we estimate a precision of about 30‰ for the ratio between the two isotopologues HD16O and H216O. The measurement noise, the applied atmospheric temperature profiles, the uncertainty in the spectral baseline, and the cross-dependence on humidity are the leading error sources. We introduce an a posteriori correction method of the cross-dependence on humidity, and we recommend applying it to isotopologue ratio remote sensing datasets in general. In addition, we present mid-infrared CO2 retrievals and use them for demonstrating the MUSICA network-wide data consistency. In order to indicate the potential of long-term isotopologue remote sensing data if provided with a well-documented quality, we present a climatology and compare it to simulations of an isotope incorporated AGCM (Atmospheric General Circulation Model. We identify differences in the multi-year mean and seasonal cycles that significantly exceed the estimated errors, thereby indicating deficits in the modeled atmospheric water cycle.

  14. Ground-based remote sensing of tropospheric water vapour isotopologues within the project MUSICA

    Science.gov (United States)

    Schneider, M.; Barthlott, S.; Hase, F.; González, Y.; Yoshimura, K.; García, O. E.; Sepúlveda, E.; Gomez-Pelaez, A.; Gisi, M.; Kohlhepp, R.; Dohe, S.; Blumenstock, T.; Wiegele, A.; Christner, E.; Strong, K.; Weaver, D.; Palm, M.; Deutscher, N. M.; Warneke, T.; Notholt, J.; Lejeune, B.; Demoulin, P.; Jones, N.; Griffith, D. W. T.; Smale, D.; Robinson, J.

    2012-12-01

    Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water), long-term tropospheric water vapour isotopologue data records are provided for ten globally distributed ground-based mid-infrared remote sensing stations of the NDACC (Network for the Detection of Atmospheric Composition Change). We present a new method allowing for an extensive and straightforward characterisation of the complex nature of such isotopologue remote sensing datasets. We demonstrate that the MUSICA humidity profiles are representative for most of the troposphere with a vertical resolution ranging from about 2 km (in the lower troposphere) to 8 km (in the upper troposphere) and with an estimated precision of better than 10%. We find that the sensitivity with respect to the isotopologue composition is limited to the lower and middle troposphere, whereby we estimate a precision of about 30‰ for the ratio between the two isotopologues HD16O and H216O. The measurement noise, the applied atmospheric temperature profiles, the uncertainty in the spectral baseline, and the cross-dependence on humidity are the leading error sources. We introduce an a posteriori correction method of the cross-dependence on humidity, and we recommend applying it to isotopologue ratio remote sensing datasets in general. In addition, we present mid-infrared CO2 retrievals and use them for demonstrating the MUSICA network-wide data consistency. In order to indicate the potential of long-term isotopologue remote sensing data if provided with a well-documented quality, we present a climatology and compare it to simulations of an isotope incorporated AGCM (Atmospheric General Circulation Model). We identify differences in the multi-year mean and seasonal cycles that significantly exceed the estimated errors, thereby indicating deficits in the modeled atmospheric water cycle.

  15. Combinatorial chemistry

    DEFF Research Database (Denmark)

    Nielsen, John

    1994-01-01

    An overview of combinatorial chemistry is presented. Combinatorial chemistry, sometimes referred to as `irrational drug design,' involves the generation of molecular diversity. The resulting chemical library is then screened for biologically active compounds.......An overview of combinatorial chemistry is presented. Combinatorial chemistry, sometimes referred to as `irrational drug design,' involves the generation of molecular diversity. The resulting chemical library is then screened for biologically active compounds....

  16. Aquatic Chemistry

    International Nuclear Information System (INIS)

    Kim, Dong Yeun; Kim, Oh Sik; Kim, Chang Guk; Park, Cheong Gil; Lee, Gwi Hyeon; Lee, Cheol Hui

    1987-07-01

    This book deals aquatic chemistry, which treats water and environment, chemical kinetics, chemical balance like dynamical characteristic, and thermodynamics, acid-base chemistry such as summary, definition, kinetics, and PH design for mixture of acid-base chemistry, complex chemistry with definition, and kinetics, precipitation and dissolution on summary, kinetics of precipitation and dissolution, and balance design oxidation and resolution with summary, balance of oxidation and resolution.

  17. Positronium chemistry

    CERN Document Server

    Green, James

    1964-01-01

    Positronium Chemistry focuses on the methodologies, reactions, processes, and transformations involved in positronium chemistry. The publication first offers information on positrons and positronium and experimental methods, including mesonic atoms, angular correlation measurements, annihilation spectra, and statistical errors in delayed coincidence measurements. The text then ponders on positrons in gases and solids. The manuscript takes a look at the theoretical chemistry of positronium and positronium chemistry in gases. Topics include quenching, annihilation spectrum, delayed coincidence

  18. Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures

    CERN Document Server

    Kürten, Andreas; Almeida, Joao; Kupiainen-Määttä, Oona; Dunne, Eimear M.; Duplissy, Jonathan; Williamson, Christina; Barmet, Peter; Breitenlechner, Martin; Dommen, Josef; Donahue, Neil M.; Flagan, Richard C.; Franchin, Alessandro; Gordon, Hamish; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Ickes, Luisa; Jokinen, Tuija; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Kupc, Agnieszka; Lehtipalo, Katrianne; Leiminger, Markus; Makhmutov, Vladimir; Onnela, Antti; Ortega, Ismael K.; Petäjä, Tuukka; Praplan, Arnaud P.; Riccobono, Francesco; Rissanen, Matti P.; Rondo, Linda; Schnitzhofer, Ralf; Schobesberger, Siegfried; Smith, James N.; Steiner, Gerhard; Stozhkov, Yuri; Tomé, António; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Wagner, Paul E.; Wimmer, Daniela; Ye, Penglin; Baltensperger, Urs; Carslaw, Ken; Kulmala, Markku; Curtius, Joachim

    2016-01-01

    Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia arethought to be the dominant processes responsible for new particle formation (NPF) in the cold temperaturesof the middle and upper troposphere. Ions are also thought to be important for particle nucleation inthese regions. However, global models presently lack experimentally measured NPF rates under controlledlaboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here withdata obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets)chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. Theconditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrationsbet ween 5 × 105and 1 × 109cm3, and ammonia mixing ratios from zero added ammonia, i.e., nominally purebinary, to a maximum of ~1400 parts per trillion by volume (pptv). We performed nucleation s...

  19. Iodine's impact on tropospheric oxidants: a global model study in GEOS-Chem

    Directory of Open Access Journals (Sweden)

    T. Sherwen

    2016-02-01

    Full Text Available We present a global simulation of tropospheric iodine chemistry within the GEOS-Chem chemical transport model. This includes organic and inorganic iodine sources, standard gas-phase iodine chemistry, and simplified higher iodine oxide (I2OX, X = 2, 3, 4 chemistry, photolysis, deposition, and parametrized heterogeneous reactions. In comparisons with recent iodine oxide (IO observations, the simulation shows an average bias of  ∼ +90 % with available surface observations in the marine boundary layer (outside of polar regions, and of  ∼ +73 % within the free troposphere (350 hPa  <  p  <  900 hPa over the eastern Pacific. Iodine emissions (3.8 Tg yr−1 are overwhelmingly dominated by the inorganic ocean source, with 76 % of this emission from hypoiodous acid (HOI. HOI is also found to be the dominant iodine species in terms of global tropospheric IY burden (contributing up to 70 %. The iodine chemistry leads to a significant global tropospheric O3 burden decrease (9.0 % compared to standard GEOS-Chem (v9-2. The iodine-driven OX loss rate1 (748 Tg OX yr−1 is due to photolysis of HOI (78 %, photolysis of OIO (21 %, and reaction between IO and BrO (1 %. Increases in global mean OH concentrations (1.8 % by increased conversion of hydroperoxy radicals exceeds the decrease in OH primary production from the reduced O3 concentration. We perform sensitivity studies on a range of parameters and conclude that the simulation is sensitive to choices in parametrization of heterogeneous uptake, ocean surface iodide, and I2OX (X = 2, 3, 4 photolysis. The new iodine chemistry combines with previously implemented bromine chemistry to yield a total bromine- and iodine-driven tropospheric O3 burden decrease of 14.4 % compared to a simulation without iodine and bromine chemistry in the model, and a small increase in OH (1.8 %. This is a significant impact and so halogen chemistry needs to be

  20. Problems in global atmospheric chemistry

    Science.gov (United States)

    Crutzen, Paul J.

    1993-02-01

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

  1. 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

  2. Ozone Depletion in Tropospheric Volcanic Plumes: From Halogen-Poor to Halogen-Rich Emissions

    Directory of Open Access Journals (Sweden)

    Tjarda J. Roberts

    2018-02-01

    Full Text Available Volcanic halogen emissions to the troposphere undergo a rapid plume chemistry that destroys ozone. Quantifying the impact of volcanic halogens on tropospheric ozone is challenging, only a few observations exist. This study presents measurements of ozone in volcanic plumes from Kīlauea (HI, USA, a low halogen emitter. The results are combined with published data from high halogen emitters (Mt Etna, Italy; Mt Redoubt, AK, USA to identify controls on plume processes. Ozone was measured during periods of relatively sustained Kīlauea plume exposure, using an Aeroqual instrument deployed alongside Multi-Gas SO2 and H2S sensors. Interferences were accounted for in data post-processing. The volcanic H2S/SO2 molar ratio was quantified as 0.03. At Halema‘uma‘u crater-rim, ozone was close to ambient in the emission plume (at 10 ppmv SO2. Measurements in grounding plume (at 5 ppmv SO2 about 10 km downwind of Pu‘u ‘Ō‘ō showed just slight ozone depletion. These Kīlauea observations contrast with substantial ozone depletion reported at Mt Etna and Mt Redoubt. Analysis of the combined data from these three volcanoes identifies the emitted Br/S as a strong but non-linear control on the rate of ozone depletion. Model simulations of the volcanic plume chemistry highlight that the proportion of HBr converted into reactive bromine is a key control on the efficiency of ozone depletion. This underlines the importance of chemistry in the very near-source plume on the fate and atmospheric impacts of volcanic emissions to the troposphere.

  3. Multidecadal Changes in the UTLS Ozone from the MERRA-2 Reanalysis and the GMI Chemistry Model

    Science.gov (United States)

    Wargan, Krzysztof; Orbe, Clara; Pawson, Steven; Ziemke, Jerald R.; Oman, Luke; Olsen, Mark; Coy, Lawrence; Knowland, Emma

    2018-01-01

    Long-term changes of ozone in the UTLS (Upper Troposphere / Lower Stratosphere) reflect the response to decreases in the stratospheric concentrations of ozone-depleting substances as well as changes in the stratospheric circulation induced by climate change. To date, studies of UTLS ozone changes and variability have relied mainly on satellite and in-situ observations as well as chemistry-climate model simulations. By comparison, the potential of reanalysis ozone data remains relatively untapped. This is despite evidence from recent studies, including detailed analyses conducted under SPARC (Scalable Processor Architecture) Reanalysis Intercomparison Project (S-RIP), that demonstrate that stratospheric ozone fields from modern atmospheric reanalyses exhibit good agreement with independent data while delineating issues related to inhomogeneities in the assimilated observations. In this presentation, we will explore the possibility of inferring long-term geographically and vertically resolved behavior of the lower stratospheric (LS) ozone from NASA's MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications -2) reanalysis after accounting for the few known discontinuities and gaps in its assimilated input data. This work builds upon previous studies that have documented excellent agreement between MERRA-2 ozone and ozonesonde observations in the LS. Of particular importance is a relatively good vertical resolution of MERRA-2 allowing precise separation of tropospheric and stratospheric ozone contents. We also compare the MERRA-2 LS ozone results with the recently completed 37-year simulation produced using Goddard Earth Observing System in "replay"� mode coupled with the GMI (Global Modeling Initiative) chemistry mechanism. Replay mode dynamically constrains the model with the MERRA-2 reanalysis winds, temperature, and pressure. We will emphasize the areas of agreement of the reanalysis and replay and interpret differences between them in the context

  4. Forensic Chemistry

    Science.gov (United States)

    Bell, Suzanne

    2009-07-01

    Forensic chemistry is unique among chemical sciences in that its research, practice, and presentation must meet the needs of both the scientific and the legal communities. As such, forensic chemistry research is applied and derivative by nature and design, and it emphasizes metrology (the science of measurement) and validation. Forensic chemistry has moved away from its analytical roots and is incorporating a broader spectrum of chemical sciences. Existing forensic practices are being revisited as the purview of forensic chemistry extends outward from drug analysis and toxicology into such diverse areas as combustion chemistry, materials science, and pattern evidence.

  5. Nitrogen oxides in the troposphere – What have we learned from satellite measurements?

    Directory of Open Access Journals (Sweden)

    Richter A.

    2009-02-01

    Full Text Available Nitrogen oxides are key species in the troposphere where they are linked to ozone formation and acid rain. The sources of nitrogen oxides are anthropogenic to large extend, mainly through combustion of fossil fuels. Satellite observations of NO2 provide global measurements of nitrogen oxides since summer 1995, and these data have been applied for many studies on the emission sources and strengths, the chemistry and the transport of NOx. In this paper, an overview will be given on satellite measurements of NO2 , some examples of typical applications and an outlook on future prospects.

  6. Tropospheric Delay from VLBI and GNSS Measurements

    Science.gov (United States)

    Gubanov, V. S.

    2018-02-01

    Using an updated version of the QUASAR software package developed at the Institute of Applied Astronomy of the Russian Academy of Sciences, we have processed the VLBI observations within the international CONT14 program (May 6-20, 2014), in which a global network of 17 stations was involved (a total of 250 000 observations). The package update concerned the optimization of data structure and the refinement of stochastic models for the random variations in wet tropospheric delay and atomic clock difference. The main goal of this paper is to compare the VLBI determinations of the tropospheric delay with its independent determinations using global navigation satellite systems (GNSS). We show that both these determinations agree well between themselves only in the case of a global analysis of the VLBI observations, where the VLBI station coordinates are also refined, along with the tropospheric delay and the clock synchronization and Earth orientation parameters. If, alternatively, the station coordinates are insufficiently accurate and are not refined from VLBI observations, then it is appropriate not to determine the tropospheric delay from these observations, but to take it from the publicly accessible independent GNSS data. However, this requires that the VLBI and GNSS techniques operate simultaneously at a common observing site. We have established the shortcomings of the universally accepted method of stabilizing the global solution associated with the absence of a criterion for choosing reference stations and radio sources. Two ways of their elimination are proposed: (i) introducing a coordinated list of weight factors for the errors in the coordinates of such stations and sources into the stabilization algorithm and (ii) adopting a coordinated list of stations and sources the refinement of whose coordinates is not required at all for a certain time.

  7. Radon concentration inversions in the troposphere

    International Nuclear Information System (INIS)

    Pereira, E.B.

    1987-07-01

    Vertical concentrations of radon in the lower troposphere were obtained in Southern Brazil up to 7Km high and have shown unexpected inverted profiles. The presence of low pressure center systems southwest to the flight path suggested that inversions might have been originated by a vertical transport mechanism based on the large scale circulation of developing synoptic systems. A simple friction-driven circulation model was contructed and the transport equation was solved. (author) [pt

  8. Tropospheric radiative forcing of CH4

    International Nuclear Information System (INIS)

    Grossman, A.S.; Grant, K.E.

    1994-04-01

    We have evaluated the tropospheric radiative forcing of CH 4 in the 0-3000 cm -1 wavenumber range and compared this with prior published calculations. The atmospheric test cases involved perturbed methane scenarios in both a McClatchey mid latitude, summer, clear sky approximation, model atmosphere, as well as a globally and seasonally averaged model atmosphere containing a representative cloud distribution. The scenarios involved pure CH 4 radiative forcing and CH 4 plus a mixture of H 2 O, CO 2 , O 3 , and N 2 O. The IR radiative forcing was calculated using a correlated k-distribution transmission model. The major purposes of this paper are to first, use the correlated k-distribution model to calculate the tropospheric radiative forcing for CH 4 , as the only radiatively active gas, and in a mixture with H 2 O, CO 2 , O 3 , and N 2 O, for a McClatchey mid-latitude summer, clear-sky model atmosphere, and to compare the results to those obtained in the studies mentioned above. Second, we will calculate the tropospheric methane forcing in a globally and annually averaged atmosphere with and without a representative cloud distribution in order to validate the conjecture given in IPCC (1990) that the inclusion of clouds in the forcing calculations results in forcing values which are approximately 20 percent less than those obtained using clear sky approximations

  9. Tropospheric Enhancement of Ozone over the UAE

    Science.gov (United States)

    Abbasi, Naveed Ali; Majeed, Tariq; Iqbal, Mazhar; Kaminski, Jacek; Struzewska, Joanna; Durka, Pawel; Tarasick, David; Davies, Jonathan

    2015-04-01

    We use the Global Environmental Multiscale - Air Quality (GEM-AQ) model to interpret the vertical profiles of ozone acquired with ozone sounding experiments at the meteorological site located at the Abu Dhabi airport. The purpose of this study is to gain insight into the chemical and dynamical structures in the atmosphere of this unique subtropical location (latitude 24.45N; longitude 54.22E). Ozone observations for years 2012 - 2013 reveal elevated ozone abundances in the range from 70 ppbv to 120 ppbv near 500-400 hPa during summer. The ozone abundances in other seasons are much lower than these values. The preliminary results indicate that summertime enhancement in ozone is associated with the Arabian anticyclones centered over the Zagros Mountains in Iran and the Asir and Hijaz Mountain ranges in Saudi Arabia, and is consistent with TES observations of deuterated water. The model also shows considerable seasonal variation in the tropospheric ozone which is transported from the stratosphere by dynamical processes. The domestic production of ozone in the middle troposphere is estimated and compared GEM-AQ model. It is estimated that about 40-50% of ozone in the UAE is transported from the neighbouring petrochemical industries in the Gulf region. We will present ozone sounding data and GEM-AQ results including a discussion on the high levels of the tropospheric ozone responsible for contaminating the air quality in the UAE. This work is supported by National Research Foundation, UAE.

  10. A Lagrangian analysis of the impact of transport and transformation on the ozone stratification observed in the free troposphere during the ESCOMPTE campaign

    Directory of Open Access Journals (Sweden)

    A. Colette

    2006-01-01

    Full Text Available The ozone variability observed by tropospheric ozone lidars during the ESCOMPTE campaign is analyzed by means of a hybrid-Lagrangian modeling study. Transport processes responsible for the formation of ozone-rich layers are identified using a semi-Lagrangian analysis of mesoscale simulations to identify the planetary boundary layer (PBL footprint in the free troposphere. High ozone concentrations are related to polluted air masses exported from the Iberian PBL. The chemical composition of air masses coming from the PBL and transported in the free troposphere is evaluated using a Lagrangian chemistry model. The initial concentrations are provided by a model of chemistry and transport. Different scenarios are tested for the initial conditions and for the impact of mixing with background air in order to perform a quantitative comparison with the lidar observations. For this meteorological situation, the characteristic mixing time is of the order of 2 to 6 days depending on the initial conditions. Ozone is produced in the free troposphere within most air masses exported from the Iberian PBL at an average rate of 0.2 ppbv h−1, with a maximum ozone production of 0.4 ppbv h−1. Transport processes from the PBL are responsible for an increase of 13.3 ppbv of ozone concentrations in the free troposphere compared to background levels; about 45% of this increase is attributed to in situ production during the transport rather than direct export of ozone.

  11. A Lagrangian analysis of the impact of transport and transformation on the ozone stratification observed in the free troposphere during the ESCOMPTE campaign

    Science.gov (United States)

    Colette, A.; Ancellet, G.; Menut, L.; Arnold, S. R.

    2006-08-01

    The ozone variability observed by tropospheric ozone lidars during the ESCOMPTE campaign is analyzed by means of a hybrid-Lagrangian modeling study. Transport processes responsible for the formation of ozone-rich layers are identified using a semi-Lagrangian analysis of mesoscale simulations to identify the planetary boundary layer (PBL) footprint in the free troposphere. High ozone concentrations are related to polluted air masses exported from the Iberian PBL. The chemical composition of air masses coming from the PBL and transported in the free troposphere is evaluated using a Lagrangian chemistry model. The initial concentrations are provided by a model of chemistry and transport. Different scenarios are tested for the initial conditions and for the impact of mixing with background air in order to perform a quantitative comparison with the lidar observations. For this meteorological situation, the characteristic mixing time is of the order of 2 to 6 days depending on the initial conditions. Ozone is produced in the free troposphere within most air masses exported from the Iberian PBL at an average rate of 0.2 ppbv h-1, with a maximum ozone production of 0.4 ppbv h-1. Transport processes from the PBL are responsible for an increase of 13.3 ppbv of ozone concentrations in the free troposphere compared to background levels; about 45% of this increase is attributed to in situ production during the transport rather than direct export of ozone.

  12. Quantification of topographic venting of boundary layer air to the free troposphere

    Directory of Open Access Journals (Sweden)

    S. Henne

    2004-01-01

    Full Text Available Net vertical air mass export by thermally driven flows from the atmospheric boundary layer (ABL to the free troposphere (FT above deep Alpine valleys was investigated. The vertical export of pollutants above mountainous terrain is presently poorly represented in global chemistry transport models (GCTMs and needs to be quantified. Air mass budgets were calculated using aircraft observations obtained in deep Alpine valleys. The results show that on average 3 times the valley air mass is exported vertically per day under fair weather conditions. During daytime the type of valleys investigated in this study can act as an efficient 'air pump' that transports pollutants upward. The slope wind system within the valley plays an important role in redistributing pollutants. Nitrogen oxide emissions in mountainous regions are efficiently injected into the FT. This could enhance their ozone (O3 production efficiency and thus influences tropospheric pollution budgets. Once lifted to the FT above the Alps pollutants are transported horizontally by the synoptic flow and are subject to European pollution export. Forward trajectory studies show that under fair weather conditions two major pathways for air masses above the Alps dominate. Air masses moving north are mixed throughout the whole tropospheric column and further transported eastward towards Asia. Air masses moving south descend within the subtropical high pressure system above the Mediterranean.

  13. Prediction of ozone tropospheric degradation rate constant of organic compounds by using artificial neural networks

    International Nuclear Information System (INIS)

    Fatemi, M.H.

    2006-01-01

    Ozone tropospheric degradation of organic compound is very important in environmental chemistry. The lifetime of organic chemicals in the atmosphere can be calculated from the knowledge of the rate constant of their reaction with free radicals such as OH and NO 3 or O 3 . In the present work, the rate constant for the tropospheric degradation of 137 organic compounds by reaction with ozone, the least widely and successfully modeled degradation process, are predicted by quantitative structure activity relationships modeling based on a variety of theoretical descriptors, which screened and selected by genetic algorithm variable subset selection procedure. These descriptors which can be used as inputs for generated artificial neural networks are; HOMO-LUMO gap, number of double bonds, number of single bonds, maximum net charge on C atom, minimum (>0.1) bond order of C atom and Minimum e-e repulsion of H atom. After generation, optimization and training of artificial neural network, network was used for the prediction of log KO 3 for the validation set. The root mean square error for the neural network calculated log KO 3 for training, prediction and validation set are 0.357, 0.460 and 0.481, respectively, which are smaller than those obtained by multiple linear regressions model (1.217, 0.870 and 0.968, respectively). Results obtained reveal the reliability and good predictivity of neural network model for the prediction of ozone tropospheric degradations rate constant of organic compounds

  14. PM2.5 and tropospheric ozone in China: overview of situation and responses

    Science.gov (United States)

    Zhang, Hua

    This work reviewed the observational status of PM2.5 and tropospheric ozone in China. It told us the observational facts on the ratios of typical types of aerosol components to the total PM2.5/PM10, and daily and seasonal change of near surface ozone concentration at different cities of China; the global concentration distribution of tropospheric ozone observed by satellite in 2010-2013 was also given for comparison; the PM2.5 concentration distribution and their seasonal change in China region were simulated by an aerosol chemistry-global climate modeling system. Different contribution from five kinds of aerosols to the simulated PM2.5 was analyzed. Then, it linked the emissions of aerosol and greenhouse gases and their radiative forcing and thus gave their climatic effect by reducing their emissions on the basis of most recently published IPCC AR5. Finally it suggested policies on reducing emissions of short-lived climate pollutants (SLCPs) (such as PM2.5 and tropospheric ozone) in China from protecting both climate and environment.

  15. Seasonal Changes in Tropospheric Ozone Concentrations over South Korea and Its Link to Ozone Precursors

    Science.gov (United States)

    Jung, H. C.; Moon, B. K.; Wie, J.

    2017-12-01

    Concentration of tropospheric ozone over South Korea has steadily been on the rise in the last decades, mainly due to rapid industrializing and urbanizing in the Eastern Asia. To identify the characteristics of tropospheric ozone in South Korea, we fitted a sine function to the surface ozone concentration data from 2005 to 2014. Based on fitted sine curves, we analyzed the shifts in the dates on which ozone concentration reached its peak in the calendar year. Ozone monitoring sites can be classified into type types: where the highest annual ozone concentration kept occurring sooner (Esites) and those that kept occurring later (Lsites). The seasonal analysis shows that the surface ozone had increased more rapidly in Esites than in Lsites in the past decade during springtime and vice-versa during summertime. We tried to find the reason for the different seasonal trends with the relationship between ozone and ozone precursors. As a result, it was found that the changes in the ground-level ozone concentration in the spring and summer times are considerably influenced by changes in nitrogen dioxide concentration, and this is closely linked to the destruction (production) process of ozone by nitrogen dioxide in spring (summer). The link between tropospheric ozone and nitrogen dioxide discussed in this study will have to be thoroughly examined through climate-chemistry modeling in the future. Acknowledgements This research was supported by the Korea Ministry of Environment (MOE) as "Climate Change Correspondence Program."

  16. Transport mechanisms for synoptic, seasonal and interannual SF6 variations and "age" of air in troposphere

    Directory of Open Access Journals (Sweden)

    K. Miyazaki

    2009-02-01

    Full Text Available We use an atmospheric general circulation model (AGCM driven chemistry-transport model (ACTM to simulate the evolution of sulfur hexafluoride (SF6 in the troposphere. The model results are compared with continuous measurements at 6 sites over 71° N–90° S. These comparisons demonstrate that the ACTM simulations lie within the measurement uncertainty over the analysis period (1999–2006 and capture salient features of synoptic, seasonal and interannual SF6 variability. To understand transport timescales of SF6 within the troposphere, transport times of air parcels from the surface to different regions of the troposphere ("age" are estimated from a simulation of an idealized tracer. The age estimation error and its sensitivity to the selection of reanalysis meteorology for ACTM nudging or the tracer transport by deep cumulus convection as represented in the model are discussed. Monthly-mean, 2-box model exchange times (τex are calculated from both the observed and simulated SF6 time series at the 6 observing sites and show favorable agreement, suggesting that the ACTM adequately represents large-scale interhemispheric transport. The simulated SF6 variability is further investigated through decomposition of the mixing ratio time-tendency into advective, convective, and vertical diffusive components. The transport component analysis illustrates the role of each process in SF6 synoptic variability at the site level and provides insight into the seasonality of τex.

  17. Impact of solar versus volcanic activity variations on tropospheric temperatures and precipitation during the Dalton Minimum

    Science.gov (United States)

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

    2014-05-01

    The aim of this work is to elucidate the impact of changes in solar irradiance and energetic particles versus volcanic eruptions on tropospheric global climate during the Dalton Minimum (DM, AD 1780-1840). Separate variations in the (i) solar irradiance in the UV-C with wavelengths λ 250 nm, (iii) in energetic particle spectrum, and (iv) volcanic aerosol forcing were analyzed separately, and (v) in combination, by means of small ensemble calculations using a coupled atmosphere-ocean chemistry-climate model. Global and hemispheric mean surface temperatures show a significant dependence on solar irradiance at λ > 250 nm. Also, powerful volcanic eruptions in 1809, 1815, 1831 and 1835 significantly decreased global mean temperature by up to 0.5 K for 2-3 years after the eruption. However, while the volcanic effect is clearly discernible in the Southern Hemispheric mean temperature, it is less significant in the Northern Hemisphere, partly because the two largest volcanic eruptions occurred in the SH tropics and during seasons when the aerosols were mainly transported southward, partly because of the higher northern internal variability. In the simulation including all forcings, temperatures are in reasonable agreement with the tree ring-based temperature anomalies of the Northern Hemisphere. Interestingly, the model suggests that solar irradiance changes at λ Dalton Minimum. This downscales the importance of top-down processes (stemming from changes at λ 250 nm). Reduction of irradiance at λ > 250 nm leads to a significant (up to 2%) decrease in the ocean heat content (OHC) between 0 and 300 m in depth, whereas the changes in irradiance at λ < 250 nm or in energetic particles have virtually no effect. Also, volcanic aerosol yields a very strong response, reducing the OHC of the upper ocean by up to 1.5%. In the simulation with all forcings, the OHC of the uppermost levels recovers after 8-15 years after volcanic eruption, while the solar signal and the different

  18. Impact of solar vs. volcanic activity variations on tropospheric temperatures and precipitation during the Dalton Minimum

    Science.gov (United States)

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

    2013-11-01

    The aim of this work is to elucidate the impact of changes in solar irradiance and energetic particles vs. volcanic eruptions on tropospheric global climate during the Dalton Minimum (DM, 1780-1840 AD). Separate variations in the (i) solar irradiance in the UV-C with wavelengths λ 250 nm, (iii) in energetic particle spectrum, and (iv) volcanic aerosol forcing were analyzed separately, and (v) in combination, by means of small ensemble calculations using a coupled atmosphere-ocean chemistry-climate-model. Global and hemispheric mean surface temperatures show a significant dependence on solar irradiance at λ > 250 nm. Also, powerful volcanic eruptions in 1809, 1815, 1831 and 1835 significantly decrease global mean temperature by up to 0.5 K for 2-3 yr after the eruption. However, while the volcanic effect is clearly discernible in the southern hemispheric mean temperature, it is less significant in the Northern Hemisphere, partly because the two largest volcanic eruptions occurred in the SH tropics and during seasons when the aerosols were mainly transported southward, partly because of the higher northern internal variability. In the simulation including all forcings, temperatures are in reasonable agreement with the tree-ring-based temperature anomalies of the Northern Hemisphere. Interestingly, the model suggests that solar irradiance changes at λ Dalton Minimum. This downscales the importance of top-down processes (stemming from changes at λ 250 nm). Reduction of irradiance at λ > 250 nm leads to a significant (up to 2%) decrease of the ocean heat content (OHC) between the 0 and 300 m of depth, whereas the changes in irradiance at λ < 250 nm or in energetic particle have virtually no effect. Also, volcanic aerosol yields a very strong response, reducing the OHC of the upper ocean by up to 1.5%. In the simulation with all forcings, the OHC of the uppermost levels recovers after 8-15 yr after volcanic eruption, while the solar signal and the different

  19. Chemical and climatic drivers of radiative forcing due to changes in stratospheric and tropospheric ozone over the 21st century

    Science.gov (United States)

    Banerjee, Antara; Maycock, Amanda C.; Pyle, John A.

    2018-02-01

    The ozone radiative forcings (RFs) resulting from projected changes in climate, ozone-depleting substances (ODSs), non-methane ozone precursor emissions and methane between the years 2000 and 2100 are calculated using simulations from the UM-UKCA chemistry-climate model (UK Met Office's Unified Model containing the United Kingdom Chemistry and Aerosols sub-model). Projected measures to improve air-quality through reductions in non-methane tropospheric ozone precursor emissions present a co-benefit for climate, with a net global mean ozone RF of -0.09 W m-2. This is opposed by a positive ozone RF of 0.05 W m-2 due to future decreases in ODSs, which is driven by an increase in tropospheric ozone through stratosphere-to-troposphere transport of air containing higher ozone amounts. An increase in methane abundance by more than a factor of 2 (as projected by the RCP8.5 scenario) is found to drive an ozone RF of 0.18 W m-2, which would greatly outweigh the climate benefits of non-methane tropospheric ozone precursor reductions. A small fraction (˜ 15 %) of the ozone RF due to the projected increase in methane results from increases in stratospheric ozone. The sign of the ozone RF due to future changes in climate (including the radiative effects of greenhouse gases, sea surface temperatures and sea ice changes) is shown to be dependent on the greenhouse gas emissions pathway, with a positive RF (0.05 W m-2) for RCP4.5 and a negative RF (-0.07 W m-2) for the RCP8.5 scenario. This dependence arises mainly from differences in the contribution to RF from stratospheric ozone changes. Considering the increases in tropopause height under climate change causes only small differences (≤ |0.02| W m-2) for the stratospheric, tropospheric and whole-atmosphere RFs.

  20. Global budget of tropospheric ozone: Evaluating recent model advances with satellite (OMI), aircraft (IAGOS), and ozonesonde observations

    Science.gov (United States)

    Hu, Lu; Jacob, Daniel J.; Liu, Xiong; Zhang, Yi; Zhang, Lin; Kim, Patrick S.; Sulprizio, Melissa P.; Yantosca, Robert M.

    2017-10-01

    The global budget of tropospheric ozone is governed by a complicated ensemble of coupled chemical and dynamical processes. Simulation of tropospheric ozone has been a major focus of the GEOS-Chem chemical transport model (CTM) over the past 20 years, and many developments over the years have affected the model representation of the ozone budget. Here we conduct a comprehensive evaluation of the standard version of GEOS-Chem (v10-01) with ozone observations from ozonesondes, the OMI satellite instrument, and MOZAIC-IAGOS commercial aircraft for 2012-2013. Global validation of the OMI 700-400 hPa data with ozonesondes shows that OMI maintained persistent high quality and no significant drift over the 2006-2013 period. GEOS-Chem shows no significant seasonal or latitudinal bias relative to OMI and strong correlations in all seasons on the 2° × 2.5° horizontal scale (r = 0.88-0.95), improving on previous model versions. The most pronounced model bias revealed by ozonesondes and MOZAIC-IAGOS is at high northern latitudes in winter-spring where the model is 10-20 ppbv too low. This appears to be due to insufficient stratosphere-troposphere exchange (STE). Model updates to lightning NOx, Asian anthropogenic emissions, bromine chemistry, isoprene chemistry, and meteorological fields over the past decade have overall led to gradual increase in the simulated global tropospheric ozone burden and more active ozone production and loss. From simulations with different versions of GEOS meteorological fields we find that tropospheric ozone in GEOS-Chem v10-01 has a global production rate of 4960-5530 Tg a-1, lifetime of 20.9-24.2 days, burden of 345-357 Tg, and STE of 325-492 Tg a-1. Change in the intensity of tropical deep convection between these different meteorological fields is a major factor driving differences in the ozone budget.

  1. Anthropogenic influence on the distribution of tropospheric sulphate aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Langner, J; Rodhe, H; Crutzen, P J; Zimmermann, P [Swedish Meteorological and Hydrological Institute, Norrkoeping (Sweden)

    1992-10-22

    Human activities have increased global emissions of sulphur gases by about a factor of three during the past century, leading to increased sulphate aerosol concentrations, mainly in the Northern Hemisphere. Sulphate aerosols can affect the climate directly, by increasing the backscattering of solar radiation in cloud-free air, and indirectly, by providing additional cloud condensation nuclei. Here a global transport-chemistry model is used to estimate the changes in the distribution of tropospheric sulphate aerosol and deposition of non-seasalt sulphur that have occurred since pre-industrial times. The increase in sulphate aerosol concentration is small over the Southern Hemisphere oceans, but reaches a factor of 100 over northern Europe in winter. Calculations indicate, however, that at most 6% of the anthropogenic sulphur emissions is available for the formation of new aerosol particles. This is because about one-half of the sulphur dioxide is deposited on the Earth's surface, and most of the remainder is oxidized in cloud droplets so that the sulphate becomes associated with pre-existing particles. Even so, the rate of formation of new sulphate particles may have doubled since pre-industrial times. 18 refs., 3 figs.

  2. Stratospheric impact on tropospheric ozone variability and trends: 1990–2009

    Directory of Open Access Journals (Sweden)

    P. G. Hess

    2013-01-01

    Full Text Available The influence of stratospheric ozone on the interannual variability and trends in tropospheric ozone is evaluated between 30 and 90° N from 1990–2009 using ozone measurements and a global chemical transport model, the Community Atmospheric Model with chemistry (CAM-chem. Long-term measurements from ozonesondes, at 150 and 500 hPa, and the Measurements of OZone and water vapour by in-service Airbus aircraft programme (MOZAIC, at 500 hPa, are analyzed over Japan, Canada, the Eastern US and Northern and Central Europe. The measurements generally emphasize northern latitudes, although the simulation suggests that measurements over the Canadian, Northern and Central European regions are representative of the large-scale interannual ozone variability from 30 to 90° N at 500 hPa. CAM-chem is run with input meteorology from the National Center for Environmental Prediction; a tagging methodology is used to identify the stratospheric contribution to tropospheric ozone concentrations. A variant of the synthetic ozone tracer (synoz is used to represent stratospheric ozone. Both the model and measurements indicate that on large spatial scales stratospheric interannual ozone variability drives significant tropospheric variability at 500 hPa and the surface. In particular, the simulation and the measurements suggest large stratospheric influence at the surface sites of Mace Head (Ireland and Jungfraujoch (Switzerland as well as many 500 hPa measurement locations. Both the measurements and simulation suggest the stratosphere has contributed to tropospheric ozone trends. In many locations between 30–90° N 500 hPa ozone significantly increased from 1990–2000, but has leveled off since (from 2000–2009. The simulated global ozone budget suggests global stratosphere-troposphere exchange increased in 1998–1999 in association with a global ozone anomaly. Discrepancies between the simulated and measured ozone budget include a large underestimation of

  3. Atmospheric chemistry and transport modeling in the outer solar system

    Science.gov (United States)

    Lee, Yuan-Tai (Anthony)

    2001-11-01

    This thesis consists of 1-D and 2-D photochemical- dynamical modeling in the upper atmospheres of outer planets. For 1-D modeling, a unified hydrocarbon photochemical model has been studied in Jupiter, Saturn, Uranus, Neptune, and Titan, by comparing with the Voyager observations, and the recent measurements of methyl radicals by ISO in Saturn and Neptune. The CH3 observation implies a kinetically sensitive test to the measured and estimated hydrocarbon rate constants at low temperatures. We identify the key reactions that control the concentrations of CH3 in the model, such as the three-body recombination reaction, CH3 + CH3 + M --> C 2H6 + M, and the recycling reaction H + CH3 + M --> CH4 + M. The results show reasonable agreement with ISO values. In Chapter 4, the detection of PH3 in the lower stratosphere and upper troposphere of Jupiter has provided a photochemical- dynamical coupling model to derive the eddy diffusion coefficient in the upper troposphere of Jupiter. Using a two-layers photochemical model with updated photodissociation cross-sections and chemical rate constants for NH3 and PH 3, we find that the upper tropospheric eddy diffusion coefficient 106 cm2 sec-1, are required to match the derived PH3 vertical profile by the observation. The best-fit functional form derivation of eddy diffusion coefficient in the upper troposphere of Jupiter above 400 mbar is K = 2.0 × 104 (n/2.2 × 1019)-0.5 cm 2 sec-1. On the other hand, Chapter 5 demonstrates a dynamical-only 2-D model of C2H6 providing a complete test for the current 2-D transport models in Jovian lower stratosphere and upper troposphere (270 to 0.1 mbar pressure levels). Different combinations of residual advection, horizontal eddy dispersion, and vertical eddy mixing are examined at different latitudes.

  4. Organic chemistry

    International Nuclear Information System (INIS)

    2003-08-01

    This book with sixteen chapter explains organic chemistry on linkage isomerism such as alkane, cycloalkane, alkene, aromatic compounds, stereo selective isomerization, aromatic compounds, stereo selective isomerization, organic compounds, stereo selective isomerization, organic halogen compound, alcohol, ether, aldehyde and ketone, carboxylic acid, dicarboxylic acid, fat and detergent, amino, carbohydrate, amino acid and protein, nucleotide and nucleic acid and spectroscopy, a polymer and medical chemistry. Each chapter has introduction structure and characteristic and using of organic chemistry.

  5. Radiation chemistry

    Energy Technology Data Exchange (ETDEWEB)

    None

    1973-07-01

    Research progress is reported on radiation chemistry of heavy elements that includes the following topics: radiation chemistry of plutonium in nitric acid solutions (spectrophotometric analysis and gamma radiolysis of Pu(IV) and Pu(VI) in nitric acid solution); EPR studies of intermediates formed in radiolytic reactions with aqueous medium; two-phase radiolysis and its effect on the distribution coefficient of plutonium; and radiation chemistry of nitric acid. (DHM)

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

    Science.gov (United States)

    Scattergood, Thomas W.

    1987-01-01

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

  7. SWIFT: Semi-empirical and numerically efficient stratospheric ozone chemistry for global climate models

    OpenAIRE

    Kreyling, Daniel; Wohltmann, Ingo; Lehmann, Ralph; Rex, Markus

    2015-01-01

    The SWIFT model is a fast yet accurate chemistry scheme for calculating the chemistry of stratospheric ozone. It is mainly intended for use in Global Climate Models (GCMs), Chemistry Climate Models (CCMs) and Earth System Models (ESMs). For computing time reasons these models often do not employ full stratospheric chem- istry modules, but use prescribed ozone instead. This can lead to insufficient representation between stratosphere and troposphere. The SWIFT stratospheric ozone chem...

  8. Technetium chemistry

    International Nuclear Information System (INIS)

    Burns, C.; Bryan, J.; Cotton, F.; Ott, K.; Kubas, G.; Haefner, S.; Barrera, J.; Hall, K.; Burrell, A.

    1996-01-01

    Technetium chemistry is a young and developing field. Despite the limited knowledge of its chemistry, technetium is the workhorse for nuclear medicine. Technetium is also a significant environmental concern because it is formed as a byproduct of nuclear weapons production and fission-power generators. Development of new technetium radio-pharmaceuticals and effective environmental control depends strongly upon knowledge of basic technetium chemistry. The authors performed research into the basic coordination and organometallic chemistry of technetium and used this knowledge to address nuclear medicine and environmental applications. This is the final report of a three-year Laboratory-Directed Research and Development (LDRD) project at the Los Alamos National Laboratory (LANL)

  9. Chemistry Technology

    Data.gov (United States)

    Federal Laboratory Consortium — Chemistry technology experts at NCATS engage in a variety of innovative translational research activities, including:Design of bioactive small molecules.Development...

  10. Overview of the Deep Convective Clouds and Chemistry Experiment

    Science.gov (United States)

    Barth, M. C.; Brune, W. H.; Cantrell, C. A.; Rutledge, S. A.; Crawford, J. H.; Flocke, F. M.; Huntrieser, H.

    2012-12-01

    The Deep Convective Clouds and Chemistry (DC3) project conducted a 7-week field campaign during May and June 2012 to study thunderstorm dynamical, physical, and electrical characteristics, as well as their effects on the atmosphere's composition, especially ozone and particles in the climate-sensitive upper troposphere near the thunderstorm tops. The NSF/NCAR Gulfstream V (GV) and the NASA DC-8 aircraft flew 17 coordinated flights to sample low-level inflow and upper troposphere outflow air near thunderstorms and to sample convective outflow air as it chemically aged during the next 24 hours. The DLR Falcon aircraft observed the fresh storm outflow and also obtained measurements of aged outflow. In total, 19 cases of active thunderstorms and over 6 cases of photochemical aging were flown. The DC3 aircraft, based in Salina, Kansas, were equipped with instruments to measure a variety of gases, aerosols, and cloud particle characteristics in situ as well as the NASA DC-8 measuring the ozone and aerosol distribution by lidar. The aircraft targeted storms predicted to occur within range of coverage by ground-based radar pairs, lightning mapping arrays (LMAs), and frequent launches of balloon-borne instruments that could measure the storm's physical, kinematic, and lightning characteristics. This coverage occurred in three regions: 1) northeastern Colorado, 2) central Oklahoma to western Texas, and 3) northern Alabama. DC3 demonstrated that it is possible to sample with two aircraft the inflow and outflow of storms, which were simultaneously sampled by the ground radars, LMAs, and soundings. The DC3 data set is extensive and rich. This presentation will summarize the overall statistics of the DC3 measurements giving a general idea of storm characteristics, transport of trace gases, and photochemical aging of species. Examples will be given of specific thunderstorm cases, including a Colorado case where a biomass-burning plume was ingested by a storm, and of sampling a

  11. Tropospheric Ozone Climatology over Irene, South Africa, From 1990-1994 and 1998-2002

    Science.gov (United States)

    Diab, R. D.; Thompson, A. M.; Marl, K.; Ramsay, L.; Coetzee, G. J. R.

    2004-01-01

    This paper describes ozone profiles from sonde data during the period of NASA s TRACE-A and the more recent SHADOZ (Southern Hemisphere Additional Ozonesondes) period. The data were taken by the South African Weather Service at the Irene (25 deg.54 min S; 28 deg. 13 min. E) station near Pretoria, South Africa, an area that is a unique mixture of local industry, heavy biofuels use and importation of biomass burning ozone from neighboring countries to the north. The main findings are: (1) With its geographical position at the edge of the subtropical transition zone, mid- latitude dynamical influences are evident at Irene, predominantly in winter when upper tropospheric ozone is enhanced as a result of stratospheric-tropospheric exchange. (2) There has been an increase in the near-surface ozone amount between the early 1990s and a decade later, presumably due to an influx of rural population toward the Johannesburg-Pretoria area, as well as with industrial growth and development. (3) Most significant for developing approaches for satellite ozone profile climatologies, cluster analysis has enabled the delineation of a background and "most polluted" profile. Enhancements of at least 30% occur throughout the troposphere in spring and in certain layers increases of 100 % are observed.

  12. Sources of tropospheric ozone along the Asian Pacific Rim: An analysis of ozonesonde observations

    Science.gov (United States)

    Liu, Hongyu; Jacob, Daniel J.; Chan, Lo Yin; Oltmans, Samuel J.; Bey, Isabelle; Yantosca, Robert M.; Harris, Joyce M.; Duncan, Bryan N.; Martin, Randall V.

    2002-11-01

    The sources contributing to tropospheric ozone over the Asian Pacific Rim in different seasons are quantified by analysis of Hong Kong and Japanese ozonesonde observations with a global three-dimensional (3-D) chemical transport model (GEOS-CHEM) driven by assimilated meteorological observations. Particular focus is placed on the extensive observations available from Hong Kong in 1996. In the middle-upper troposphere (MT-UT), maximum Asian pollution influence along the Pacific Rim occurs in summer, reflecting rapid convective transport of surface pollution. In the lower troposphere (LT) the season of maximum Asian pollution influence shifts to summer at midlatitudes from fall at low latitudes due to monsoonal influence. The UT ozone minimum and high variability observed over Hong Kong in winter reflects frequent tropical intrusions alternating with stratospheric intrusions. Asian biomass burning makes a major contribution to ozone at pollution influence (pollution influence exceeds European influence in the UT-MT, reflecting the uplift from convection and the warm conveyor belts over the eastern seaboard of North America. African outflow makes a major contribution to ozone in the low-latitude MT-UT over the Pacific Rim during November-April. Lightning influence over the Pacific Rim is minimum in summer due to westward UT transport at low latitudes associated with the Tibetan anticyclone. The Asian outflow flux of ozone to the Pacific is maximum in spring and fall and includes a major contribution from Asian anthropogenic sources year-round.

  13. Current organic chemistry

    National Research Council Canada - National Science Library

    1997-01-01

    Provides in depth reviews on current progress in the fields of asymmetric synthesis, organometallic chemistry, bioorganic chemistry, heterocyclic chemistry, natural product chemistry, and analytical...

  14. Global impacts of tropospheric halogens (Cl, Br, I on oxidants and composition in GEOS-Chem

    Directory of Open Access Journals (Sweden)

    T. Sherwen

    2016-09-01

    Full Text Available We present a simulation of the global present-day composition of the troposphere which includes the chemistry of halogens (Cl, Br, I. Building on previous work within the GEOS-Chem model we include emissions of inorganic iodine from the oceans, anthropogenic and biogenic sources of halogenated gases, gas phase chemistry, and a parameterised approach to heterogeneous halogen chemistry. Consistent with Schmidt et al. (2016 we do not include sea-salt debromination. Observations of halogen radicals (BrO, IO are sparse but the model has some skill in reproducing these. Modelled IO shows both high and low biases when compared to different datasets, but BrO concentrations appear to be modelled low. Comparisons to the very sparse observations dataset of reactive Cl species suggest the model represents a lower limit of the impacts of these species, likely due to underestimates in emissions and therefore burdens. Inclusion of Cl, Br, and I results in a general improvement in simulation of ozone (O3 concentrations, except in polar regions where the model now underestimates O3 concentrations. Halogen chemistry reduces the global tropospheric O3 burden by 18.6 %, with the O3 lifetime reducing from 26 to 22 days. Global mean OH concentrations of 1.28  ×  106 molecules cm−3 are 8.2 % lower than in a simulation without halogens, leading to an increase in the CH4 lifetime (10.8 % due to OH oxidation from 7.47 to 8.28 years. Oxidation of CH4 by Cl is small (∼  2 % but Cl oxidation of other VOCs (ethane, acetone, and propane can be significant (∼  15–27 %. Oxidation of VOCs by Br is smaller, representing 3.9 % of the loss of acetaldehyde and 0.9 % of the loss of formaldehyde.

  15. 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)

  16. Nuclear chemistry

    International Nuclear Information System (INIS)

    Vertes, A.; Kiss, I.

    1987-01-01

    This book is an introduction to the application of nuclear science in modern chemistry. The first group of chapters discuss the basic phenomena and concepts of nuclear physics with emphasis on their relation to chemical problems, including the main properties and the composition of atomic nuclei, nuclear reactions, radioactive decay and interactions of radiation with matter. These chapters provide the basis for understanding the following chapters which encompass the wide scope of nuclear chemistry. The methods of the investigation of chemical structure based on the interaction of nuclear radiation with matter including positronium chemistry and other exotic atoms is elaborated in particular detail. Separate chapters are devoted to the use of radioactive tracers, the chemical consequences of nuclear processes (i.e. hot atom chemistry), radiation chemistry, isotope effects and their applications, and the operation of nuclear reactors

  17. Nuclear chemistry

    International Nuclear Information System (INIS)

    Vertes, A.; Kiss, I.

    1987-01-01

    This book is an introduction to the application of nuclear science in modern chemistry. The first group of chapters discuss the basic phenomena and concepts of nuclear physics with emphasis on their relation to chemical problems, including the main properties and the composition of atomic nuclei, nuclear reactions, radioactive decay and interactions of radiation with matter. These chapters provide the basis for understanding the following chapters which encompass the wide scope of nuclear chemistry. The methods of the investigation of chemical structure based on the interaction of nuclear radiation with matter including positronium chemistry and other exotic atoms is elaborated in particular detail. Separate chapters are devoted to the use of radioactive tracers, the chemical consequences of nuclear processes (i.e. hot atom chemistry), radiation chemistry, isotope effects and their applications, and the operation of nuclear reactors. (Auth.)

  18. Characteristics of tropospheric ozone depletion events in the Arctic spring: analysis of the ARCTAS, ARCPAC, and ARCIONS measurements and satellite BrO observations

    Directory of Open Access Journals (Sweden)

    J.-H. Koo

    2012-10-01

    Full Text Available Arctic ozone depletion events (ODEs are caused by halogen catalyzed ozone loss. In situ chemistry, advection of ozone-poor air mass, and vertical mixing in the lower troposphere are important factors affecting ODEs. To better characterize the ODEs, we analyze the combined set of surface, ozonesonde, and aircraft in situ measurements of ozone and bromine compounds during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS, the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC, and the Arctic Intensive Ozonesonde Network Study (ARCIONS experiments (April 2008. Tropospheric BrO columns retrieved from satellite measurements and back trajectory calculations are also used to investigate the characteristics of observed ODEs. In situ observations from these field experiments are inadequate to validate tropospheric BrO columns derived from satellite measurements. In view of this difficulty, we construct an ensemble of tropospheric column BrO estimates from two satellite (OMI and GOME-2 measurements and with three independent methods of calculating stratospheric BrO columns. Furthermore, we select analysis methods that do not depend on the absolute magnitude of column BrO, such as time-lagged correlation analysis of ozone and tropospheric column BrO, to understand characteristics of ODEs. Time-lagged correlation analysis between in situ (surface and ozonesonde measurements of ozone and satellite derived tropospheric BrO columns indicates that the ODEs are due to either local halogen-driven ozone loss or short-range (∼1 day transport from nearby regions with ozone depletion. The effect of in situ ozone loss is also evident in the diurnal variation difference between low (10th and 25th percentiles and higher percentiles of surface ozone concentrations at Alert, Canada. Aircraft observations indicate low-ozone air mass transported from adjacent high-BrO regions. Correlation analyses of ozone

  19. Evaluating the lower-tropospheric COSMIC GPS radio occultation sounding quality over the Arctic

    Science.gov (United States)

    Yu, Xiao; Xie, Feiqin; Ao, Chi O.

    2018-04-01

    Lower-tropospheric moisture and temperature measurements are crucial for understanding weather prediction and climate change. Global Positioning System radio occultation (GPS RO) has been demonstrated as a high-quality observation technique with high vertical resolution and sub-kelvin temperature precision from the upper troposphere to the stratosphere. In the tropical lower troposphere, particularly the lowest 2 km, the quality of RO retrievals is known to be degraded and is a topic of active research. However, it is not clear whether similar problems exist at high latitudes, particularly over the Arctic, which is characterized by smooth ocean surface and often negligible moisture in the atmosphere. In this study, 3-year (2008-2010) GPS RO soundings from COSMIC (Constellation Observing System for Meteorology, Ionosphere, and Climate) over the Arctic (65-90° N) show uniform spatial sampling with average penetration depth within 300 m above the ocean surface. Over 70 % of RO soundings penetrate deep into the lowest 300 m of the troposphere in all non-summer seasons. However, the fraction of such deeply penetrating profiles reduces to only about 50-60 % in summer, when near-surface moisture and its variation increase. Both structural and parametric uncertainties of GPS RO soundings were also analyzed. The structural uncertainty (due to different data processing approaches) is estimated to be within ˜ 0.07 % in refractivity, ˜ 0.72 K in temperature, and ˜ 0.05 g kg-1 in specific humidity below 10 km, which is derived by comparing RO retrievals from two independent data processing centers. The parametric uncertainty (internal uncertainty of RO sounding) is quantified by comparing GPS RO with near-coincident radiosonde and European Centre for Medium-Range Weather Forecasts (ECMWF) ERA-Interim profiles. A systematic negative bias up to ˜ 1 % in refractivity below 2 km is only seen in the summer, which confirms the moisture impact on GPS RO quality.

  20. Effects of anthropogenic emissions on tropospheric ozone and its radiative forcing

    Energy Technology Data Exchange (ETDEWEB)

    Berntsen, T.; Isaksen, I.S.A.; Fuglestvedt, J.S.; Myhre, G.; Larsen, T. Alsvik; Stordal, F.; Freckleton, R.S.; Shine, K.P.

    1997-12-31

    As described in this report, changes in tropospheric ozone since pre-industrial times due to changes in emissions have been calculated by the University of Oslo global three-dimensional photochemical model. The radiative forcing caused by the increase in ozone has been calculated by means of two independent radiative transfer models: the University of Reading model (Reading), and the University of Oslo/Norwegian Institute for Air Research model (OsloRad). Significant increases in upper tropospheric ozone concentrations are found at northern mid-latitudes at about 10 km altitude. In the tropical regions the largest increase is found at about 15 km altitude. The increase is found to be caused mainly by enhanced in situ production due to transport of precursors from the boundary layer, with a smaller contribution from increased transport of ozone produced in the boundary layer. The lifetime of ozone in the troposphere decreased by about 35% as a result of enhanced concentrations of HO{sub 2}. The calculated increase in surface ozone in Europe is in good agreement with observations. The calculations of radiative forcing include the effect of clouds and allow for thermal adjustment in the stratosphere. The global and annual averaged radiative forcing at the tropopause from both models are in the lower part of the Intergovernmental Panel on Climate Change estimated range. The calculated radiative forcing is similar in magnitude to the negative radiative forcing by sulfate aerosols, but displaced southward in source regions at northern mid-latitudes. The increase in tropospheric ozone is calculated to have cooled the lower stratosphere by up to 0.9 K, with possibly half of this cooling occurring in the past 2 to 3 decades. 76 refs., 16 figs., 9 tabs.

  1. 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.

  2. Comment on "Tropospheric temperature response to stratospheric ozone recovery in the 21st century" by Hu et al. (2011

    Directory of Open Access Journals (Sweden)

    C. McLandress

    2012-03-01

    Full Text Available In a recent paper Hu et al. (2011 suggest that the recovery of stratospheric ozone during the first half of this century will significantly enhance free tropospheric and surface warming caused by the anthropogenic increase of greenhouse gases, with the effects being most pronounced in Northern Hemisphere middle and high latitudes. These surprising results are based on a multi-model analysis of CMIP3 model simulations with and without prescribed stratospheric ozone recovery. Hu et al. suggest that in order to properly quantify the tropospheric and surface temperature response to stratospheric ozone recovery, it is necessary to run coupled atmosphere-ocean climate models with stratospheric ozone chemistry. The results of such an experiment are presented here, using a state-of-the-art chemistry-climate model coupled to a three-dimensional ocean model. In contrast to Hu et al., we find a much smaller Northern Hemisphere tropospheric temperature response to ozone recovery, which is of opposite sign. We suggest that their result is an artifact of the incomplete removal of the large effect of greenhouse gas warming between the two different sets of models.

  3. Rapid increases in tropospheric ozone production and export from China

    NARCIS (Netherlands)

    Verstraeten, W.W.; Neu, J.L.; Williams, J.E.; Bowman, K.W.; Worden, J.R.; Boersma, K.F.

    2015-01-01

    Rapid population growth and industrialization have driven substantial increases in Asian ozone precursor emissions over the past decade1, with highly uncertain impacts on regional and global tropospheric ozone levels. According to ozonesonde measurements2, 3, tropospheric ozone concentrations at two

  4. Quantum chemistry

    CERN Document Server

    Lowe, John P

    1993-01-01

    Praised for its appealing writing style and clear pedagogy, Lowe's Quantum Chemistry is now available in its Second Edition as a text for senior undergraduate- and graduate-level chemistry students. The book assumes little mathematical or physical sophistication and emphasizes an understanding of the techniques and results of quantum chemistry, thus enabling students to comprehend much of the current chemical literature in which quantum chemical methods or concepts are used as tools. The book begins with a six-chapter introduction of standard one-dimensional systems, the hydrogen atom,

  5. Atmospheric and aerosol chemistry

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-09-01

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

  6. 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.

  7. Materials Chemistry

    CERN Document Server

    Fahlman, Bradley D

    2011-01-01

    The 2nd edition of Materials Chemistry builds on the strengths that were recognized by a 2008 Textbook Excellence Award from the Text and Academic Authors Association (TAA). Materials Chemistry addresses inorganic-, organic-, and nano-based materials from a structure vs. property treatment, providing a suitable breadth and depth coverage of the rapidly evolving materials field. The 2nd edition continues to offer innovative coverage and practical perspective throughout. After briefly defining materials chemistry and its history, seven chapters discuss solid-state chemistry, metals, semiconducting materials, organic "soft" materials, nanomaterials, and materials characterization. All chapters have been thoroughly updated and expanded with, for example, new sections on ‘soft lithographic’ patterning, ‘click chemistry’ polymerization, nanotoxicity, graphene, as well as many biomaterials applications. The polymer and ‘soft’ materials chapter represents the largest expansion for the 2nd edition. Each ch...

  8. Analytical chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Jae Seong

    1993-02-15

    This book is comprised of nineteen chapters, which describes introduction of analytical chemistry, experimental error and statistics, chemistry equilibrium and solubility, gravimetric analysis with mechanism of precipitation, range and calculation of the result, volume analysis on general principle, sedimentation method on types and titration curve, acid base balance, acid base titration curve, complex and firing reaction, introduction of chemical electro analysis, acid-base titration curve, electrode and potentiometry, electrolysis and conductometry, voltammetry and polarographic spectrophotometry, atomic spectrometry, solvent extraction, chromatograph and experiments.

  9. Analytical chemistry

    International Nuclear Information System (INIS)

    Choi, Jae Seong

    1993-02-01

    This book is comprised of nineteen chapters, which describes introduction of analytical chemistry, experimental error and statistics, chemistry equilibrium and solubility, gravimetric analysis with mechanism of precipitation, range and calculation of the result, volume analysis on general principle, sedimentation method on types and titration curve, acid base balance, acid base titration curve, complex and firing reaction, introduction of chemical electro analysis, acid-base titration curve, electrode and potentiometry, electrolysis and conductometry, voltammetry and polarographic spectrophotometry, atomic spectrometry, solvent extraction, chromatograph and experiments.

  10. Analytical chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Chae, Myeong Hu; Lee, Hu Jun; Kim, Ha Seok

    1989-02-15

    This book give explanations on analytical chemistry with ten chapters, which deal with development of analytical chemistry, the theory of error with definition and classification, sample and treatment gravimetry on general process of gravimetry in aqueous solution and non-aqueous solution, precipitation titration about precipitation reaction and types, complexometry with summary and complex compound, oxidation-reduction equilibrium on electrode potential and potentiometric titration, solvent extraction and chromatograph and experiment with basic operation for chemical experiment.

  11. Analytical chemistry

    International Nuclear Information System (INIS)

    Chae, Myeong Hu; Lee, Hu Jun; Kim, Ha Seok

    1989-02-01

    This book give explanations on analytical chemistry with ten chapters, which deal with development of analytical chemistry, the theory of error with definition and classification, sample and treatment gravimetry on general process of gravimetry in aqueous solution and non-aqueous solution, precipitation titration about precipitation reaction and types, complexometry with summary and complex compound, oxidation-reduction equilibrium on electrode potential and potentiometric titration, solvent extraction and chromatograph and experiment with basic operation for chemical experiment.

  12. Green Chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Collison, Melanie

    2011-05-15

    Green chemistry is the science of chemistry used in a way that will not use or create hazardous substances. Dr. Rui Resendes is working in this field at GreenCentre Canada, an offshoot of PARTEQ Innovations in Kingston, Ontario. GreenCentre's preliminary findings suggest their licensed product {sup S}witchable Solutions{sup ,} featuring 3 classes of solvents and a surfactant, may be useful in bitumen oil sands extraction.

  13. Efficient transport of tropospheric aerosol into the stratosphere via the Asian summer monsoon anticyclone

    Science.gov (United States)

    Yu, Pengfei; Rosenlof, Karen H.; Liu, Shang; Telg, Hagen; Thornberry, Troy D.; Rollins, Andrew W.; Portmann, Robert W.; Bai, Zhixuan; Ray, Eric A.; Duan, Yunjun; Pan, Laura L.; Toon, Owen B.; Bian, Jianchun; Gao, Ru-Shan

    2017-07-01

    An enhanced aerosol layer near the tropopause over Asia during the June-September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (˜15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (˜35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.

  14. Tropospheric trace gas measurement by tunable diode laser spectroscopy. Final report. Messung troposphaerischer Spurengase mittels Dioden-Laser-Spektroskopie. Abschlussbericht

    Energy Technology Data Exchange (ETDEWEB)

    Burrows, J P; Crutzen, P J; Harris, G W; Klemp, D; Johnson, T J; Perner, D; Wienhold, F G; Zenker, T

    1991-01-01

    This final report is concerned with tropospheric trace gas measurements by Tunable Diode Laser Spectroscopy (TDLAS). A TDLAS instrument was built which simultaneously measures four selected trace gases and is sufficiently sensitive for use in 'clean' air conditions. The instrument is the first of its kind to be used for measurements aboard ship platforms in clean marine air. In order to guarantee that the instrument function continuously for several weeks at a time under the difficult conditions encountered at sea, a variety of innovative technical developments were necessary. The TDLAS instrument was used to investigate boundary layer tropospheric chemistry in one engineering test and four field campaigns. Three of the field campaigns took place on board the German research vessels. The measurements on board the research vessels enabled different types of tropospheric air to be investigated: (i) clean maritime air; (ii) maritime regions influenced by continental sources of trace gases and pollutants, in particular the coastal region around the west coast of Africa was thoroughly investigated under downwind conditions. A large set of data of simultaneous measurements of key tropospheric trace gases (NO{sub 2}, CO, HCHO, H{sub 2}O{sub 2} and O{sub 3}) were obtained which help paint a more complete picture of tropospheric oxidation cycles. The first measurements of H{sub 2}O{sub 2} in the remote marine boundary layer are reported. In selected regions successful TDLAS measurements of HCl and COS were obtained, results in themselves of importance. Intercomparisons of TDLAS and other measurement techniques were successfully undertaken. (orig./BBR).

  15. Global tropospheric ozone modeling: Quantifying errors due to grid resolution

    Science.gov (United States)

    Wild, Oliver; Prather, Michael J.

    2006-06-01

    Ozone production in global chemical models is dependent on model resolution because ozone chemistry is inherently nonlinear, the timescales for chemical production are short, and precursors are artificially distributed over the spatial scale of the model grid. In this study we examine the sensitivity of ozone, its precursors, and its production to resolution by running a global chemical transport model at four different resolutions between T21 (5.6° × 5.6°) and T106 (1.1° × 1.1°) and by quantifying the errors in regional and global budgets. The sensitivity to vertical mixing through the parameterization of boundary layer turbulence is also examined. We find less ozone production in the boundary layer at higher resolution, consistent with slower chemical production in polluted emission regions and greater export of precursors. Agreement with ozonesonde and aircraft measurements made during the NASA TRACE-P campaign over the western Pacific in spring 2001 is consistently better at higher resolution. We demonstrate that the numerical errors in transport processes on a given resolution converge geometrically for a tracer at successively higher resolutions. The convergence in ozone production on progressing from T21 to T42, T63, and T106 resolution is likewise monotonic but indicates that there are still large errors at 120 km scales, suggesting that T106 resolution is too coarse to resolve regional ozone production. Diagnosing the ozone production and precursor transport that follow a short pulse of emissions over east Asia in springtime allows us to quantify the impacts of resolution on both regional and global ozone. Production close to continental emission regions is overestimated by 27% at T21 resolution, by 13% at T42 resolution, and by 5% at T106 resolution. However, subsequent ozone production in the free troposphere is not greatly affected. We find that the export of short-lived precursors such as NOx by convection is overestimated at coarse resolution.

  16. Experimental and modeling study of the impact of vertical transport processes from the boundary-layer on the variability and the budget of tropospheric ozone

    International Nuclear Information System (INIS)

    Colette, A.

    2005-12-01

    Closing the tropospheric ozone budget requires a better understanding of the role of transport processes from the major reservoirs: the planetary boundary layer and the stratosphere. Case studies lead to the identification of mechanisms involved as well as their efficiency. However, their global impact on the budget must be addressed on a climatological basis. This manuscript is thus divided in two parts. First, we present case studies based on ozone LIDAR measurements performed during the ESCOMPTE campaign. This work consists in a data analysis investigation by means of a hybrid - Lagrangian study involving: global meteorological analyses, Lagrangian particle dispersion computation, and mesoscale, chemistry - transport, and Lagrangian photochemistry modeling. Our aim is to document the amount of observed ozone variability related to transport processes and, when appropriate, to infer the role of tropospheric photochemical production. Second, we propose a climatological analysis of the respective impact of transport from the boundary-layer and from the tropopause region on the tropospheric ozone budget. A multivariate analysis is presented and compared to a trajectography approach. Once validated, this algorithm is applied to the whole database of ozone profiles collected above Europe during the past 30 years in order to discuss the seasonal, geographical and temporal variability of transport processes as well as their impact on the tropospheric ozone budget. The variability of turbulent mixing and its impact on the persistence of tropospheric layers will also be discussed. (author)

  17. Measuring tropospheric wind with microwave sounders

    Science.gov (United States)

    Lambrigtsen, B.; Su, H.; Turk, J.; Hristova-Veleva, S. M.; Dang, V. T.

    2017-12-01

    In its 2007 "Decadal Survey" of earth science missions for NASA the U.S. National Research Council recommended that a Doppler wind lidar be developed for a three-dimensional tropospheric winds mission ("3D-Winds"). The technology required for such a mission has not yet been developed, and it is expected that the next Decadal Survey, planned to be released by the end of 2017, will put additional emphasis on the still pressing need for wind measurements from space. The first Decadal Survey also called for a geostationary microwave sounder (GMS) on a Precipitation and All-weather Temperature and Humidity (PATH) mission, which could be used to measure wind from space. Such a sounder, the Geostationary Synthetic Thinned Aperture Radiometer (GeoSTAR), has been developed at the Jet Propulsion Laboratory (JPL). The PATH mission has not yet been funded by NASA, but a low-cost subset of PATH, GeoStorm has been proposed as a hosted payload on a commercial communications satellite. Both PATH and GeoStorm would obtain frequent (every 15 minutes of better) measurements of tropospheric water vapor profiles, and they can be used to derive atmospheric motion vector (AMV) wind profiles, even in the presence of clouds. Measurement of wind is particularly important in the tropics, where the atmosphere is largely not in thermal balance and wind estimates cannot generally be derived from temperature and pressure fields. We report on simulation studies of AMV wind vectors derived from a GMS and from a cluster of low-earth-orbiting (LEO) small satellites (e.g., CubeSats). The results of two separate simulation studies are very encouraging and show that a ±2 m/s wind speed precision is attainable, which would satisfy WMO requirements. A GMS observing system in particular, which can be implemented now, would enable significant progress in the study of atmospheric dynamics. Copyright 2017 California Institute of Technology. Government sponsorship acknowledged

  18. Future Climate Impacts of Direct Radiative Forcing Anthropogenic Aerosols, Tropospheric Ozone, and Long-lived Greenhouse Gases

    Science.gov (United States)

    Chen, Wei-Ting; Liao, Hong; Seinfeld, John H.

    2007-01-01

    Long-lived greenhouse gases (GHGs) are the most important driver of climate change over the next century. Aerosols and tropospheric ozone (O3) are expected to induce significant perturbations to the GHG-forced climate. To distinguish the equilibrium climate responses to changes in direct radiative forcing of anthropogenic aerosols, tropospheric ozone, and GHG between present day and year 2100, four 80-year equilibrium climates are simulated using a unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies (GISS) general circulation model (GCM) 110. Concentrations of sulfate, nitrate, primary organic (POA) carbon, secondary organic (SOA) carbon, black carbon (BC) aerosols, and tropospheric ozone for present day and year 2100 are obtained a priori by coupled chemistry-aerosol GCM simulations, with emissions of aerosols, ozone, and precursors based on the Intergovernmental Panel on Climate Change (IPCC) Special Report on Emissions Scenario (SRES) A2. Changing anthropogenic aerosols, tropospheric ozone, and GHG from present day to year 2100 is predicted to perturb the global annual mean radiative forcing by +0.18 (considering aerosol direct effects only), +0.65, and +6.54 W m(sup -2) at the tropopause, and to induce an equilibrium global annual mean surface temperature change of +0.14, +0.32, and +5.31 K, respectively, with the largest temperature response occurring at northern high latitudes. Anthropogenic aerosols, through their direct effect, are predicted to alter the Hadley circulation owing to an increasing interhemispheric temperature gradient, leading to changes in tropical precipitation. When changes in both aerosols and tropospheric ozone are considered, the predicted patterns of change in global circulation and the hydrological cycle are similar to those induced by aerosols alone. GHG-induced climate changes, such as amplified warming over high latitudes, weakened Hadley circulation, and increasing precipitation over the

  19. Upper atmosphere research at INPE

    International Nuclear Information System (INIS)

    Clemesha, B.R.

    1984-01-01

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

  20. Top-down NOX Emissions of European Cities Derived from Modelled and Spaceborne Tropospheric NO2 Columns

    Science.gov (United States)

    Verstraeten, W. W.; Boersma, K. F.; Douros, J.; Williams, J. E.; Eskes, H.; Delcloo, A. W.

    2017-12-01

    High nitrogen oxides (NOX = NO + NO2) concentrations near the surface impact humans and ecosystems badly and play a key role in tropospheric chemistry. NO2 is an important precursor of tropospheric ozone (O3) which in turn affects the production of the hydroxyl radical controlling the chemical lifetime of key atmospheric pollutants and reactive greenhouse gases. Combustion from industrial, traffic and household activities in large and densely populated urban areas result in high NOX emissions. Accurate mapping of these emissions is essential but hard to do since reported emissions factors may differ from real-time emissions in order of magnitude. Modelled NO2 levels and lifetimes also have large associated uncertainties and overestimation in the chemical lifetime which may mask missing NOX chemistry in current chemistry transport models (CTM's). The simultaneously estimation of both the NO2 lifetime and as well as the concentrations by applying the Exponentially Modified Gaussian (EMG) method on tropospheric NO2 columns lines densities should improve the surface NOX emission estimates. Here we evaluate if the EMG methodology applied on the tropospheric NO2 columns simulated by the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) CTM can reproduce the NOX emissions used as model input. First we process both the modelled tropospheric NO2 columns for the period April-September 2013 for 21 selected European urban areas under windy conditions (averaged vertical wind speeds between surface and 500 m from ECMWF > 2 m s-1) as well as the accompanying OMI (Ozone Monitoring Instrument) data providing us with real-time observation-based estimates of midday NO2 columns. Then we compare the top-down derived surface NOX emissions with the 2011 MACC-III emission inventory, used in the CTM as input to simulate the NO2 columns. For cities where NOX emissions can be assumed as originating from one large source good agreement is found between the top-down derived

  1. Estimates of Free-tropospheric NO2 Abundance from the Aura Ozone Monitoring Instrument (OMI) Using Cloud Slicing Technique

    Science.gov (United States)

    Choi, S.; Joiner, J.; Krotkov, N. A.; Choi, Y.; Duncan, B. N.; Celarier, E. A.; Bucsela, E. J.; Vasilkov, A. P.; Strahan, S. E.; Veefkind, J. P.; Cohen, R. C.; Weinheimer, A. J.; Pickering, K. E.

    2013-12-01

    Total column measurements of NO2 from space-based sensors are of interest to the atmospheric chemistry and air quality communities; the relatively short lifetime of near-surface NO2 produces satellite-observed hot-spots near pollution sources including power plants and urban areas. However, estimates of NO2 concentrations in the free-troposphere, where lifetimes are longer and the radiative impact through ozone formation is larger, are severely lacking. Such information is critical to evaluate chemistry-climate and air quality models that are used for prediction of the evolution of tropospheric ozone and its impact of climate and air quality. Here, we retrieve free-tropospheric NO2 volume mixing ratio (VMR) using the cloud slicing technique. We use cloud optical centroid pressures (OCPs) as well as collocated above-cloud vertical NO2 columns (defined as the NO2 column from top of the atmosphere to the cloud OCP) from the Ozone Monitoring Instrument (OMI). The above-cloud NO2 vertical columns used in our study are retrieved independent of a priori NO2 profile information. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud optical centroid pressure is proportional to the NO2 volume mixing ratio (VMR) for a given pressure (altitude) range. We retrieve NO2 volume mixing ratios and compare the obtained NO2 VMRs with in-situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is good when proper data screening is applied. In addition, the OMI cloud slicing reports a high NO2 VMR where the aircraft reported lightning NOx during the Deep Convection Clouds and Chemistry (DC3) campaign in 2012. We also provide a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the

  2. Transport and build-up of tropospheric trace gases during the MINOS campaign: comparision of GOME, in situ aircraft measurements and MATCH-MPIC-data

    Directory of Open Access Journals (Sweden)

    A. Ladstätter-Weißenmayer

    2003-01-01

    Full Text Available The MINOS (Mediterranean INtensive Oxidant Study campaign was an international, multi-platform field campaign to measure long-range transport of air-pollution and aerosols from South East Asia and Europe towards the Mediterranean basin during August 2001. High pollution events were observed during this campaign. For the Mediterranean region enhanced tropospheric nitrogen dioxide (NO2 and formaldehyde (HCHO, which are precursors of tropospheric ozone (O3, were detected by the satellite based GOME (Global Ozone Monitoring Experiment instrument and compared with airborne in situ measurements as well as with the output from the global 3D photochemistry-transport model MATCH-MPIC (Model of Atmospheric Transport and CHemistry - Max Planck Institute for Chemistry. The increase of pollution in that region leads to severe air quality degradation with regional and global implications.

  3. Is tropospheric weather influenced by solar wind through atmospheric vertical coupling downward control?

    Science.gov (United States)

    Prikryl, Paul; Tsukijihara, Takumi; Iwao, Koki; Muldrew, Donald B.; Bruntz, Robert; Rušin, Vojto; Rybanský, Milan; Turňa, Maroš; Šťastný, Pavel; Pastirčák, Vladimír

    2017-04-01

    More than four decades have passed since a link between solar wind magnetic sector boundary structure and mid-latitude upper tropospheric vorticity was discovered (Wilcox et al., Science, 180, 185-186, 1973). The link has been later confirmed and various physical mechanisms proposed but apart from controversy, little attention has been drawn to these results. To further emphasize their importance we investigate the occurrence of mid-latitude severe weather in the context of solar wind coupling to the magnetosphere-ionosphere-atmosphere (MIA) system. It is observed that significant snowstorms, windstorms and heavy rain, particularly if caused by low pressure systems in winter, tend to follow arrivals of high-speed solar wind. Previously published statistical evidence that explosive extratropical cyclones in the northern hemisphere tend to occur after arrivals of high-speed solar wind streams from coronal holes (Prikryl et al., Ann. Geophys., 27, 1-30, 2009; Prikryl et al., J. Atmos. Sol.-Terr. Phys., 149, 219-231, 2016) is corroborated for the southern hemisphere. A physical mechanism to explain these observations is proposed. The leading edge of high-speed solar wind streams is a locus of large-amplitude magneto-hydrodynamic waves that modulate Joule heating and/or Lorentz forcing of the high-latitude lower thermosphere generating medium-scale atmospheric gravity waves that propagate upward and downward through the atmosphere. Simulations of gravity wave propagation in a model atmosphere using the Transfer Function Model (Mayr et al., Space Sci. Rev., 54, 297-375, 1990) show that propagating waves originating in the thermosphere can excite a spectrum of gravity waves in the lower atmosphere. In spite of significantly reduced amplitudes but subject to amplification upon reflection in the upper troposphere, these gravity waves can provide a lift of unstable air to release instabilities in the troposphere thus initiating convection to form cloud/precipitation bands

  4. Tropospheric mercury vertical profiles between 500 and 10 000 m in central Europe

    Directory of Open Access Journals (Sweden)

    A. Weigelt

    2016-03-01

    Full Text Available The knowledge of the vertical distribution of atmospheric mercury (Hg plays an important role in determining the transport and cycling of mercury. However, measurements of the vertical distribution are rare, because airborne measurements are expensive and labour intensive. Consequently, only a few vertical Hg profile measurements have been reported since the 1970s. Besides the Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC observations, the latest vertical profile over Europe was measured in 1996. Within the Global Mercury Observation System (GMOS project, four vertical profiles were taken on board research aircraft (CASA-212 in August 2013 in background air over different locations in Slovenia and Germany. Each vertical profile consists of at least seven 5 min horizontal flight sections from 500 m above ground to 3000 m a.s.l. Gaseous elemental mercury (GEM and total gaseous mercury (TGM were measured with Tekran 2537X and Tekran 2537B analysers. In addition to the mercury measurements, SO2, CO, O3, NO, and NO2, basic meteorological parameters (pressure, temperature, relative humidity have been measured. Additional ground-based mercury measurements at the GMOS master site in Waldhof, Germany and measurements onboard the CARIBIC passenger aircraft were used to extend the profile to the ground and upper troposphere respectively. No vertical gradient was found inside the well-mixed boundary layer (variation of less than 0.1 ng m−3 at different sites, with GEM varying from location to location between 1.4 and 1.6 ng m−3 (standard temperature and pressure, STP: T  =  273.15 K, p  =  1013.25 hPa. At all locations GEM dropped to 1.3 ng m−3 (STP when entering the free troposphere and remained constant at higher altitudes. The combination of the vertical profile, measured on 21 August 2013 over Leipzig, Germany, with the CARIBIC measurements during ascent and descent to

  5. Chemical and aerosol characterisation of the troposphere over West Africa during the monsoon period as part of AMMA

    Directory of Open Access Journals (Sweden)

    C. E. Reeves

    2010-08-01

    Full Text Available During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons and points to some of the important findings discussed in more detail in other papers in this special issue.

    The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow.

    Mineral dust was found to be the most abundant and ubiquitous aerosol type in the

  6. General chemistry

    International Nuclear Information System (INIS)

    Kwon, Yeong Sik; Lee, Dong Seop; Ryu, Haung Ryong; Jang, Cheol Hyeon; Choi, Bong Jong; Choi, Sang Won

    1993-07-01

    The book concentrates on the latest general chemistry, which is divided int twenty-three chapters. It deals with basic conception and stoichiometry, nature of gas, structure of atoms, quantum mechanics, symbol and structure of an electron of ion and molecule, chemical thermodynamics, nature of solid, change of state and liquid, properties of solution, chemical equilibrium, solution and acid-base, equilibrium of aqueous solution, electrochemistry, chemical reaction speed, molecule spectroscopy, hydrogen, oxygen and water, metallic atom; 1A, IIA, IIIA, carbon and atom IVA, nonmetal atom and an inert gas, transition metals, lanthanons, and actinoids, nuclear properties and radioactivity, biochemistry and environment chemistry.

  7. Radiation chemistry

    International Nuclear Information System (INIS)

    Swallow, A.J.

    1983-01-01

    The subject is covered in chapters, entitled: introduction (defines scope of article as dealing with the chemistry of reactive species, (e.g. excess electrons, excited states, free radicals and inorganic ions in unusual valency states) as studied using radiation with radiation chemistry in its traditional sense and with biological and industrial applications); gases; water and simple inorganic systems; aqueous metallo-organic compounds and metalloproteins; small organic molecules in aqueous solution; microheterogeneous systems; non-aqueous liquids and solutions; solids; biological macromolecules; synthetic polymers. (U.K.)

  8. 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....

  9. Impact of sampling frequency in the analysis of tropospheric ozone observations

    Directory of Open Access Journals (Sweden)

    M. Saunois

    2012-08-01

    Full Text Available Measurements of ozone vertical profiles are valuable for the evaluation of atmospheric chemistry models and contribute to the understanding of the processes controlling the distribution of tropospheric ozone. The longest record of ozone vertical profiles is provided by ozone sondes, which have a typical frequency of 4 to 12 profiles a month. Here we quantify the uncertainty introduced by low frequency sampling in the determination of means and trends. To do this, the high frequency MOZAIC (Measurements of OZone, water vapor, carbon monoxide and nitrogen oxides by in-service AIrbus airCraft profiles over airports, such as Frankfurt, have been subsampled at two typical ozone sonde frequencies of 4 and 12 profiles per month. We found the lowest sampling uncertainty on seasonal means at 700 hPa over Frankfurt, with around 5% for a frequency of 12 profiles per month and 10% for a 4 profile-a-month frequency. However the uncertainty can reach up to 15 and 29% at the lowest altitude levels. As a consequence, the sampling uncertainty at the lowest frequency could be higher than the typical 10% accuracy of the ozone sondes and should be carefully considered for observation comparison and model evaluation. We found that the 95% confidence limit on the seasonal mean derived from the subsample created is similar to the sampling uncertainty and suggest to use it as an estimate of the sampling uncertainty. Similar results are found at six other Northern Hemisphere sites. We show that the sampling substantially impacts on the inter-annual variability and the trend derived over the period 1998–2008 both in magnitude and in sign throughout the troposphere. Also, a tropical case is discussed using the MOZAIC profiles taken over Windhoek, Namibia between 2005 and 2008. For this site, we found that the sampling uncertainty in the free troposphere is around 8 and 12% at 12 and 4 profiles a month respectively.

  10. SO2 over Central China: Measurements, Numerical Simulations and the Tropospheric Sulfur Budget

    Science.gov (United States)

    He, Hao; Li, Can; Loughner, Christopher P.; Li, Zhangqing; Krotkov, Nickolay A.; Yang, Kai; Wang, Lei; Zheng, Youfei; Bao, Xiangdong; Zhao, Guoqiang; hide

    2012-01-01

    SO2 in central China was measured in situ from an aircraft and remotely using the Ozone Monitoring Instrument (OMI) from the Aura satellite; results were used to develop a numerical tool for evaluating the tropospheric sulfur budget - sources, sinks, transformation and transport. In April 2008, measured ambient SO2 concentrations decreased from approx.7 ppbv near the surface to approx. 1 ppbv at 1800 m altitude (an effective scale height of approx.800 m), but distinct SO2 plumes were observed between 1800 and 4500 m, the aircraft's ceiling. These free tropospheric plumes play a major role in the export of SO2 and in the accuracy of OMI retrievals. The mean SO2 column contents from aircraft measurements (0.73 DU, Dobson Units) and operational OMI SO2 products (0.63+/-0.26 DU) were close. The OMI retrievals were well correlated with in situ measurements (r = 0.84), but showed low bias (slope = 0.54). A new OMI retrieval algorithm was tested and showed improved agreement and bias (r = 0.87, slope = 0.86). The Community Multiscale Air Quality (CMAQ) model was used to simulate sulfur chemistry, exhibiting reasonable agreement (r = 0.62, slope = 1.33) with in situ SO2 columns. The mean CMAQ SO2 loading over central and eastern China was 54 kT, approx.30% more than the estimate from OMI SO2 products, 42 kT. These numerical simulations, constrained by observations, indicate that ",50% (35 to 61 %) of the anthropogenic sulfur emissions were transported downwind, and the overall lifetime of tropospheric SO2 was 38+/-7 h.

  11. Vertical distribution and sources of tropospheric ozone over South China in spring 2004: Ozonesonde measurements and modeling analysis

    Science.gov (United States)

    Zhang, Y.; Liu, H.; Crawford, J. H.; Considine, D. B.; Chan, C.; Scientific Team Of Tapto

    2010-12-01

    The Transport of Air Pollutant and Tropospheric Ozone over China (TAPTO-China) science initiative is a two-year (TAPTO 2004 and 2005) field measurement campaign to help improve our understanding of the physical and chemical processes that control the tropospheric ozone budget over the Chinese subcontinent (including the Asian Pacific rim) and its surrounding SE Asia. In this paper, we use two state-of-the-art 3-D global chemical transport models (GEOS-Chem and Global Modeling Initiative or GMI) to examine the characteristics of vertical distribution and quantify the sources of tropospheric ozone by analysis of TAPTO in-situ ozonesonde data obtained at five stations in South China during spring (April and May) 2004: Lin’an (30.30N, 119.75E), Tengchong (25.01N, 98.30E), Taipei (25.0N, 121.3E), Hong Kong (22.21N, 114.30E) and Sanya (18.21N, 110.31E). The observed tropospheric ozone concentrations show strong spatial and temporal variability, which is largely captured by the models. The models simulate well the observed vertical gradients of tropospheric ozone at higher latitudes but are too low at lower latitudes. Model tagged ozone simulations suggest that stratosphere has a large impact on the upper and middle troposphere (UT/MT) at Lin’an and Tengchong. Continental SE Asian biomass burning emissions are maximum in March but still contribute significantly to the photochemical production of tropopheric ozone in South China in early April. Asian anthropogenic emissions are the major contribution to lower tropospheric ozone at all stations. On the other hand, there are episodes of influence from European/North American anthropogenic emissions. For example, model tagged ozone simulations show that over Lin’an in April 2004, stratosphere contributes 20% (13 ppbv) at 5 km, Asian boundary layer contributes 70% (46 ppbv) to ozone in the boundary layer, European boundary layer contributes 5% (3-4 ppbv) at 1.2 km, and North American boundary layer contributes 4.5% (3

  12. Exploring the Production of NOx by Lightning and Its Impact on Tropospheric Ozone

    Science.gov (United States)

    Gillani, Noor; Koshak, William; Biazar, Arastoo; Doty, Kevin; Mahon, Robert; Newchurch, Michael; Byun, Daewon; Emmons, Louisa

    2006-01-01

    Our quantitative understanding of free tropospheric (FT) chemistry is quite poor. State-of-the-art regional air quality models (e.g., US EPA's CMAQ) perform very poorly in simulating FT chemistry, with Uniform ozone around 70 ppb throughout the FT in summer, while ozonesonde data show much higher levels of ozone and much spatial-temporal structure. Such models completely neglect lightning-NOx (LNOx) emissions (the most significant source of NOx in the FT), and also contain large uncertainties in the specifications of intercontinental transport, stratosphere-troposphere exchange (STE) and PBLFT exchange (PFTE). Global air chemistry models include LNOx, but in very crude fashion, with the frequency and distribution of lightning being based on modeled cloud parameters (hence large uncertainty), lightning energetics being assumed to be constant for all flashes (literature value, while in reality there is at least a two-orders of magnitude variability from flash-to-flash), and the production of NOx in the surrounding heated air, per Joule of heating, being assumed to be constant also (literature value, while in fact it is a non-linear function of the dissipated heat and local air density, p). This situation is commonly blamed on paucity of pertinent observational data, but for the USA, there is now a wealth of surface- and satellite-based data of lightning available to permit much improved observation-based estimation of LNOx emissions. In the FT, such NOx has a long residence time, and also the ozone production efficiency from NOx there is considerably higher than in the PBL. It is, therefore, of critical importance in FT chemistry. This paper will describe the approach and data products of an ongoing NSSTC project aimed at a much-improved quantification of not only LNOx production on the scale of continental USA based on local and regional lightning observations, but also of intercontinental transport, STE and PFTE, all in upgraded simulations of tropospheric

  13. Analysis of the tropospheric water distribution during FIRE 2

    Science.gov (United States)

    Westphal, Douglas L.

    1993-01-01

    The Penn State/NCAR mesoscale model, as adapted for use at ARC, was used as a testbed for the development and validation of cloud models for use in General Circulation Models (GCM's). This modeling approach also allows us to intercompare the predictions of the various cloud schemes within the same dynamical framework. The use of the PSU/NCAR mesoscale model also allows us to compare our results with FIRE-II (First International Satellite Cloud Climatology Project Regional Experiment) observations, instead of climate statistics. Though a promising approach, our work to date revealed several difficulties. First, the model by design is limited in spatial coverage and is only run for 12 to 48 hours at a time. Hence the quality of the simulation will depend heavily on the initial conditions. The poor quality of upper-tropospheric measurements of water vapor is well known and the situation is particularly bad for mid-latitude winter since the coupling with the surface is less direct than in summer so that relying on the model to spin-up a reasonable moisture field is not always successful. Though one of the most common atmospheric constituents, water vapor is relatively difficult to measure accurately, especially operationally over large areas. The standard NWS sondes have little sensitivity at the low temperatures where cirrus form and the data from the GOES 6.7 micron channel is difficult to quantify. For this reason, the goals of FIRE Cirrus II included characterizing the three-dimensional distribution of water vapor and clouds. In studying the data from FIRE Cirrus II, it was found that no single special observation technique provides accurate regional distributions of water vapor. The Raman lidar provides accurate measurements, but only at the Hub, for levels up to 10 km, and during nighttime hours. The CLASS sondes are more sensitive to moisture at low temperatures than are the NWS sondes, but the four stations only cover an area of two hundred kilometers on a side

  14. Handbook of heterocyclic chemistry

    National Research Council Canada - National Science Library

    Katritzky, Alan R

    2010-01-01

    ... Heterocyclic Chemistry I (1984) Comprehensive Heterocyclic Chemistry II (1996) Comprehensive Heterocyclic Chemistry III (2008) Comprehensive Organic Functional Group Transformations I (1995) Compreh...

  15. Variable influence on the equatorial troposphere associated with ...

    Indian Academy of Sciences (India)

    sphere to the stratosphere due to the uneven land profile (Matsuno ... an impact of the North Atlantic ocean-atmosphere heat flux, Eurasian ... convective clouds in the stratosphere–troposphere dynamics ..... modeling benchmarks; J. Clim.

  16. Verification and Validation of Tropospheric Model/Database

    National Research Council Canada - National Science Library

    Junho, choi

    1998-01-01

    A verification and validation of tropospheric models and databases has been performed based on ray tracing algorithm, statistical analysis, test on real time system operation, and other technical evaluation process...

  17. MSU (Microwave Sounding Unit) Daily Troposphere Temperatures and Precipitation

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — This data set consists of two MSU tropospheric temperatures levels and precipitation which are described in detail below. The NOAA satellites contributing to this...

  18. Reinventing Chemistry

    OpenAIRE

    Whitesides, George McClelland

    2015-01-01

    Chemistry is in a period of change, from an era focused on molecules and reactions, to one in which manipulations of systems of molecules and reactions will be essential parts of controlling larger systems. This Essay traces paths from the past to possible futures.

  19. Chemistry Notes

    Science.gov (United States)

    School Science Review, 1972

    1972-01-01

    Short articles on the kinetics of the hydrogen peroxide-iodide ion reaction, simulation of fluidization catalysis, the use of Newman projection diagrams to represent steric relationships in organic chemistry, the use of synthetic substrates for proteolytic enzyme reactions, and two simple clock reactions"--hydrolysis of halogenoalkanes and…

  20. Measurements and estimation of the columnar optical depth of tropospheric aerosols in the UV spectral region

    Directory of Open Access Journals (Sweden)

    V. E. Cachorro

    2002-04-01

    Full Text Available We report values of the columnar tropospheric aerosol optical depth at UV wavelengths based on experimental measurements of the direct spectral irradiances carried out by a commercial spectroradiometer (Li1800 of Licor company covering the range from 300–1100 nm at two stations with different climate characteristics in Spain. The first station is located in a rural site in north central Spain with continental climate. The data extend from March to the end of October of 1995. The other station is a coastal site in the Gulf of Cádiz (southwest Spain of maritime climate type. This study is mainly focused on the capability of estimating aerosol optical depth values in the UV region based on the extracted information in the visible and near infrared ranges. A first method has been used based on the Ångström turbidity parameters. However, since this method requires detailed spectral information, a second method has also been used, based on the correlation between wavelengths. A correlation has been established between the experimental aerosol optical depth values at 350 nm and 500 nm wavelengths. Although the type of aerosol seems to be the key factor that determines the quality of these estimations, the evaluation of the associated error is necessary to know the behaviour of these estimations in each area of study.Key words. Atmospheric composition and structure (aerosols and particles; transmission and scattering of radiation; troposphere – composition and chemistry

  1. Measurements and estimation of the columnar optical depth of tropospheric aerosols in the UV spectral region

    Directory of Open Access Journals (Sweden)

    V. E. Cachorro

    Full Text Available We report values of the columnar tropospheric aerosol optical depth at UV wavelengths based on experimental measurements of the direct spectral irradiances carried out by a commercial spectroradiometer (Li1800 of Licor company covering the range from 300–1100 nm at two stations with different climate characteristics in Spain. The first station is located in a rural site in north central Spain with continental climate. The data extend from March to the end of October of 1995. The other station is a coastal site in the Gulf of Cádiz (southwest Spain of maritime climate type. This study is mainly focused on the capability of estimating aerosol optical depth values in the UV region based on the extracted information in the visible and near infrared ranges. A first method has been used based on the Ångström turbidity parameters. However, since this method requires detailed spectral information, a second method has also been used, based on the correlation between wavelengths. A correlation has been established between the experimental aerosol optical depth values at 350 nm and 500 nm wavelengths. Although the type of aerosol seems to be the key factor that determines the quality of these estimations, the evaluation of the associated error is necessary to know the behaviour of these estimations in each area of study.

    Key words. Atmospheric composition and structure (aerosols and particles; transmission and scattering of radiation; troposphere – composition and chemistry

  2. Eleven years of tropospheric NO2 measured by GOME, SCIAMACHY and OMI