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Sökning: L773:1680 7316 > (2012)

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1.
  • Aas, W., et al. (författare)
  • Lessons learnt from the first EMEP intensive measurement periods
  • 2012
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:17, s. 8073-8094
  • Tidskriftsartikel (refereegranskat)abstract
    • The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.
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2.
  • Abbatt, J. P. D., et al. (författare)
  • Halogen activation via interactions with environmental ice and snow in the polar lower troposphere and other regions
  • 2012
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:14, s. 6237-6271
  • Tidskriftsartikel (refereegranskat)abstract
    • The role of ice in the formation of chemically active halogens in the environment requires a full understanding because of its role in atmospheric chemistry, including controlling the regional atmospheric oxidizing capacity in specific situations. In particular, ice and snow are important for facilitating multiphase oxidative chemistry and as media upon which marine algae live. This paper reviews the nature of environmental ice substrates that participate in halogen chemistry, describes the reactions that occur on such substrates, presents the field evidence for ice-mediated halogen activation, summarizes our best understanding of ice-halogen activation mechanisms, and describes the current state of modeling these processes at different scales. Given the rapid pace of developments in the field, this paper largely addresses advances made in the past five years, with emphasis given to the polar boundary layer. The integrative nature of this field is highlighted in the presentation of work from the molecular to the regional scale, with a focus on understanding fundamental processes. This is essential for developing realistic parameterizations and descriptions of these processes for inclusion in larger scale models that are used to determine their regional and global impacts.
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3.
  • Achtert, Peggy, 1982-, et al. (författare)
  • On the linkage between tropospheric and Polar Stratospheric clouds in the Arctic as observed by space-borne lidar
  • 2012
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:8, s. 3791-3798
  • Tidskriftsartikel (refereegranskat)abstract
    • The type of Polar stratospheric clouds (PSCs) as well as their temporal and spatial extent are important for the occurrence of heterogeneous reactions in the polar stratosphere. The formation of PSCs depends strongly on temperature. However, the mechanisms of the formation of solid PSCs are still poorly understood. Recent satellite studies of Antarctic PSCs have shown that their formation can be associated with deep-tropospheric clouds which have the ability to cool the lower stratosphere radiatively and/or adiabatically. In the present study, lidar measurements aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite were used to investigate whether the formation of Arctic PSCs can be associated with deep-tropospheric clouds as well. Deep-tropospheric cloud systems have a vertical extent of more than 6.5 km with a cloud top height above 7 km altitude. PSCs observed by CALIPSO during the Arctic winter 2007/2008 were classified according to their type (STS, NAT, or ice) and to the kind of underlying tropospheric clouds. Our analysis reveals that 172 out of 211 observed PSCs occurred in connection with tropospheric clouds. 72% of these 172 observed PSCs occurred above deep-tropospheric clouds. We also find that the type of PSC seems to be connected to the characteristics of the underlying tropospheric cloud system. During the Arctic winter 2007/2008 PSCs consisting of ice were mainly observed in connection with deep-tropospheric cloud systems while no ice PSC was detected above cirrus. Furthermore, we find no correlation between the occurrence of PSCs and the top temperature of tropospheric clouds. Thus, our findings suggest that Arctic PSC formation is connected to adiabatice cooling, i.e. dynamic effects rather than radiative cooling.
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4.
  • Ansmann, A., et al. (författare)
  • Profiling of fine and coarse particle mass : case studies of Saharan dust and Eyjafjallajokull/Grimsvotn volcanic plumes
  • 2012
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:20, s. 9399-9415
  • Tidskriftsartikel (refereegranskat)abstract
    • The polarization lidar photometer networking (POLIPHON) method introduced to separate coarse-mode and fine-mode particle properties of Eyjafjallajokull volcanic aerosols in 2010 is extended to cover Saharan dust events as well. Furthermore, new volcanic dust observations performed after the Grimsvotn volcanic eruptions in 2011 are presented. The retrieval of particle mass concentrations requires mass-specific extinction coefficients. Therefore, a review of recently published mass-specific extinction coefficients for Saharan dust and volcanic dust is given. Case studies of four different scenarios corroborate the applicability of the profiling technique: (a) Saharan dust outbreak to central Europe, (b) Saharan dust plume mixed with biomass-burning smoke over Cape Verde, and volcanic aerosol layers originating from (c) the Eyjafjallajokull eruptions in 2010 and (d) the Grimsvotn eruptions in 2011. Strong differences in the vertical aerosol layering, aerosol mixing, and optical properties are observed for the different volcanic events.
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5.
  • Baron, Phillippe, et al. (författare)
  • Observation of horizontal winds in the middle-atmosphere between 30° S and 55° N during the northern winter 2009–2010
  • 2012
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13, s. 6049-6064
  • Tidskriftsartikel (refereegranskat)abstract
    • Although the links between stratospheric dynamics, climate and weather have been demonstrated, direct observations of stratospheric winds are lacking. We report observations of winds between 8 and 0.01 hPa (~35–80 km) from October 2009 to April 2010 by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station. The altitude range covers the region between 35–60 km where previous space-borne wind instruments show a lack of sensitivity. Both zonal and meridional wind components were obtained, though not simultaneously, in the latitude range from 30° S to 55° N and with a single profile precision of 7–9 m s−1 between 8 and 0.6 hPa and better than 20 m s−1 at altitudes above. The vertical resolution is 5–7 km except in the upper part of the retrieval range (10 km at 0.01 hPa). In the region between 1–0.05 hPa, a mean difference <2 m s−1 is found between SMILES profiles retrieved from different spectroscopic lines and instrumental settings. Good agreement (mean difference of ~2 m s−1) is also found with the European Centre for Medium-Range Weather Forecasts (ECMWF) analysis in most of the stratosphere except for the zonal winds over the equator (mean difference of 5–10 m s−1). In the mesosphere, SMILES and ECMWF zonal winds exhibit large differences (> 20 m s−1), especially in the tropics. We illustrate our results by showing daily and monthly zonal wind variations, namely the semi-annual oscillation in the tropics and reversals of the flow direction between 50° N–55° N during sudden stratospheric warmings in the stratosphere. The daily comparison with ECMWF winds reveals that in the beginning of February, a significantly stronger zonal westward flow is measured in the tropics at 2 hPa compared to the flow computed in the analysis (difference of ~20 m s−1). The results show that the comparison between SMILES and ECMWF winds is not only relevant for the quality assessment of the new SMILES winds but it also provides insights on the quality of the ECMWF winds themselves. Although the instrument was not specifically designed for measuring winds, the results demonstrate that space-borne sub-mm wave radiometers have the potential to provide good quality data for improving the stratospheric winds in atmospheric models.
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6.
  • Bergström, Robert, et al. (författare)
  • Modelling of organic aerosols over Europe (2002-2007) using a volatility basis set (VBS) framework: application of different assumptions regarding the formation of secondary organic aerosol
  • 2012
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:18, s. 8499-8527
  • Tidskriftsartikel (refereegranskat)abstract
    • A new organic aerosol module has been implemented into the EMEP chemical transport model. Four different volatility basis set (VBS) schemes have been tested in long-term simulations for Europe, covering the six years 2002-2007. Different assumptions regarding partitioning of primary organic aerosol and aging of primary semi-volatile and intermediate volatility organic carbon (S/IVOC) species and secondary organic aerosol (SOA) have been explored. Model results are compared to filter measurements, aerosol mass spectrometry (AMS) data and source apportionment studies, as well as to other model studies. The present study indicates that many different sources contribute significantly to organic aerosol in Europe. Biogenic and anthropogenic SOA, residential wood combustion and vegetation fire emissions may all contribute more than 10% each over substantial parts of Europe. This study shows smaller contributions from biogenic SOA to organic aerosol in Europe than earlier work, but relatively greater anthropogenic SOA. Simple VBS based organic aerosol models can give reasonably good results for summer conditions but more observational studies are needed to constrain the VBS parameterisations and to help improve emission inventories. The volatility distribution of primary emissions is one important issue for further work. Emissions of volatile organic compounds from biogenic sources are also highly uncertain and need further validation. We can not reproduce winter levels of organic aerosol in Europe, and there are many indications that the present emission inventories substantially underestimate emissions from residential wood combustion in large parts of Europe.
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7.
  • Birch, C. E., et al. (författare)
  • Modelling atmospheric structure, cloud and their response to CCN in the central Arctic : ASCOS case studies
  • 2012
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:7, s. 3419-3435
  • Tidskriftsartikel (refereegranskat)abstract
    • Observations made during late summer in the central Arctic Ocean, as part of the Arctic Summer Cloud Ocean Study (ASCOS), are used to evaluate cloud and vertical temperature structure in the Met Office Unified Model (MetUM). The observation period can be split into 5 regimes; the first two regimes had a large number of frontal systems, which were associated with deep cloud. During the remainder of the campaign a layer of low-level cloud occurred, typical of central Arctic summer conditions, along with two periods of greatly reduced cloud cover. The short-range operational NWP forecasts could not accurately reproduce the observed variations in near-surface temperature. A major source of this error was found to be the temperature-dependant surface albedo parameterisation scheme. The model reproduced the low-level cloud layer, though it was too thin, too shallow, and in a boundary-layer that was too frequently well-mixed. The model was also unable to reproduce the observed periods of reduced cloud cover, which were associated with very low cloud condensation nuclei (CCN) concentrations (< 1 cm(-3)). As with most global NWP models, the MetUM does not have a prognostic aerosol/cloud scheme but uses a constant CCN concentration of 100 cm(-3) over all marine environments. It is therefore unable to represent the low CCN number concentrations and the rapid variations in concentration frequently observed in the central Arctic during late summer. Experiments with a single-column model configuration of the MetUM show that reducing model CCN number concentrations to observed values reduces the amount of cloud, increases the near-surface stability, and improves the representation of both the surface radiation fluxes and the surface temperature. The model is shown to be sensitive to CCN only when number concentrations are less than 10-20 cm(-3).
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8.
  • Buehler, Stefan, et al. (författare)
  • A multi-instrument comparison of integrated water vapour measurements at a high latitude site
  • 2012
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:22, s. 10925-10943
  • Tidskriftsartikel (refereegranskat)abstract
    • We compare measurements of integrated water vapour (IWV) over a subarctic site (Kiruna, Northern Sweden) from five different sensors and retrieval methods: Radiosondes, Global Positioning System (GPS), ground-based Fourier-transform infrared (FTIR) spectrometer, ground-based microwave radiometer, and satellite-based microwave radiometer (AMSU-B). Additionally, we compare also to ERA-Interim model reanalysis data. GPS-based IWV data have the highest temporal coverage and resolution and are chosen as reference data set. All datasets agree reasonably well, but the ground-based microwave instrument only if the data are cloud-filtered. We also address two issues that are general for such intercomparison studies, the impact of different lower altitude limits for the IWV integration, and the impact of representativeness error. We develop methods for correcting for the former, and estimating the random error contribution of the latter. A literature survey reveals that reported systematic differences between different techniques are study-dependent and show no overall consistent pattern. Further improving the absolute accuracy of IWV measurements and providing climate-quality time series therefore remain challenging problems.
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9.
  • Buker, P., et al. (författare)
  • DO3SE modelling of soil moisture to determine ozone flux to forest trees
  • 2012
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:12, s. 5537-5562
  • Tidskriftsartikel (refereegranskat)abstract
    • The DO3SE (Deposition of O-3 for Stomatal Exchange) model is an established tool for estimating ozone (O-3) deposition, stomatal flux and impacts to a variety of vegetation types across Europe. It has been embedded within the EMEP (European Monitoring and Evaluation Programme) photochemical model to provide a policy tool capable of relating the flux-based risk of vegetation damage to O-3 precursor emission scenarios for use in policy formulation. A key limitation of regional flux-based risk assessments has been the assumption that soil water deficits are not limiting O-3 flux due to the unavailability of evaluated methods for modelling soil water deficits and their influence on stomatal conductance (g(sto)), and subsequent O-3 flux. This paper describes the development and evaluation of a method to estimate soil moisture status and its influence on g(sto) for a variety of forest tree species. This DO3SE soil moisture module uses the Penman-Monteith energy balance method to drive water cycling through the soil-plant-atmosphere system and empirical data describing g(sto) relationships with pre-dawn leaf water status to estimate the biological control of transpiration. We trial four different methods to estimate this biological control of the transpiration stream, which vary from simple methods that relate soil water content or potential directly to g(sto), to more complex methods that incorporate hydraulic resistance and plant capacitance that control water flow through the plant system. These methods are evaluated against field data describing a variety of soil water variables, g(sto) and transpiration data for Norway spruce (Picea abies), Scots pine (Pinus sylvestris), birch (Betula pendula), aspen (Populus tremuloides), beech (Fagus sylvatica) and holm oak (Quercus ilex) collected from ten sites across Europe and North America. Modelled estimates of these variables show consistency with observed data when applying the simple empirical methods, with the timing and magnitude of soil drying events being captured well across all sites and reductions in transpiration with the onset of drought being predicted with reasonable accuracy. The more complex methods, which incorporate hydraulic resistance and plant capacitance, perform less well, with predicted drying cycles consistently underestimating the rate and magnitude of water loss from the soil. A sensitivity analysis showed that model performance was strongly dependent upon the local parameterisation of key model drivers such as the maximum g(sto), soil texture, root depth and leaf area index. The results suggest that the simple modelling methods that relate g(sto) directly to soil water content and potential provide adequate estimates of soil moisture and influence on g(sto) such that they are suitable to be used to assess the potential risk posed by O-3 to forest trees across Europe.
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10.
  • Colette, A., et al. (författare)
  • Future air quality in Europe: a multi-model assessment of projected exposure to ozone
  • 2012
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:21, s. 10613-10630
  • Tidskriftsartikel (refereegranskat)abstract
    • In order to explore future air quality in Europe at the 2030 horizon, two emission scenarios developed in the framework of the Global Energy Assessment including varying assumptions on climate and energy access policies are investigated with an ensemble of six regional and global atmospheric chemistry transport models. A specific focus is given in the paper to the assessment of uncertainties and robustness of the projected changes in air quality. The present work relies on an ensemble of chemistry transport models giving insight into the model spread. Both regional and global scale models were involved, so that the ensemble benefits from medium-resolution approaches as well as global models that capture long-range transport. For each scenario a whole decade is modelled in order to gain statistical confidence in the results. A statistical downscaling approach is used to correct the distribution of the modelled projection. Last, the modelling experiment is related to a hind-cast study published earlier, where the performances of all participating models were extensively documented. The analysis is presented in an exposure-based framework in order to discuss policy relevant changes. According to the emission projections, ozone precursors such as NOx will drop down to 30% to 50% of their current levels, depending on the scenario. As a result, annual mean O-3 will slightly increase in NOx saturated areas but the overall O-3 burden will decrease substantially. Exposure to detrimental O-3 levels for health (SOMO35) will be reduced down to 45% to 70% of their current levels. And the fraction of stations where present-day exceedences of daily maximum O-3 is higher than 120 mu g m(-3) more than 25 days per year will drop from 43% down to 2 to 8 %. We conclude that air pollution mitigation measures (present in both scenarios) are the main factors leading to the improvement, but an additional cobenefit of at least 40% (depending on the indicator) is brought about by the climate policy.
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