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  • 11
    Publication Date: 2012-12-05
    Description: Primary marine aerosols (PMA) are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (Tw) range between −1 °C and 15 °C. A sharp decrease in PMA emissions for a Tw increase from −1 °C to 4 °C was followed by a lower rate of change in PMA emissions for Tw up to about 6 °C. Near constant number concentrations for water temperatures between 6 °C to 10 °C and higher were recorded. Even though the total particle number concentrations changes for overlapping Tw ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for Dp 〈 0.125 μm measured during winter conditions were similar (deviation of up to 3%), or lower (up to 70%) than the ones measured during summer conditions (for the same water temperature range). For Dp 〉 0.125 μm, the particle number concentrations during winter were mostly higher than in summer (up to 50%). The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in Tw from −1 °C to 10 °C during winter measurements showed a decrease in the peak of relative particle number concentration at about Dp of 0.180 μm, while an increase was observed for particles with Dp 〉 1 μm. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of Tw in the range 7–11 °C. The differences in the shape of the number size distributions between winter and summer may be caused by different production of organic material in water, different local processes modifying the water masses within the fjord (like sea ice production in winter and increased glacial melt water inflow during summer) and different origin of the dominant sea water mass. Further research is needed regarding the contribution of these factors to the PMA production.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 12
    Publication Date: 2012-06-29
    Description: Sea spray aerosols are an important part of the climate system through their direct and indirect effects. Due to the diminishing sea ice, the Arctic Ocean is one of the most rapidly changing sea spray aerosol source areas. However, the influence of these changes on primary particle production is not known. In laboratory experiments we examined the influence of Arctic Ocean water temperature, salinity and oxygen saturation on primary particle concentration characteristics. Sea water temperature was identified as the most important of these parameters. A strong decrease in sea spray aerosol production with increasing water temperature was observed for water temperatures between −1 °C and 9 °C. Aerosol number concentrations decreased from at least 1400 cm−3 to 350 cm−3. In general, the aerosol number size distribution exhibited a robust shape with one mode close to Dp 0.2 μm with approximately 45% of particles at smaller sizes. Changes in sea water temperature did not result in pronounced change of the shape of the aerosol size distribution, only in the magnitude of the concentrations. Our experiments indicate that changes in aerosol emissions are most likely linked to changes of the physical properties of sea water at low temperatures. The observed strong dependence of sea spray aerosol concentrations on sea water temperature, with a large fraction of the emitted particles in the typical cloud condensation nuclei size range, provide strong arguments for a more careful consideration of this effect in climate models.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 13
    Publication Date: 2010-11-24
    Description: Understanding Arctic climate change requires knowledge of both the external and the local drivers of Arctic climate as well as local feedbacks within the system. An Arctic feedback mechanism relating changes in sea ice extent to an alteration of the emission of sea salt aerosol and the consequent change in radiative balance is examined. A set of idealized climate model simulations were performed to quantify the radiative effects of changes in sea salt aerosol emissions induced by prescribed changes in sea ice extent. The model was forced using sea ice concentrations consistent with present day conditions and projections of sea ice extent for 2100. Sea salt aerosol emissions increase in response to a decrease in sea ice, the model results showing an annual average increase in number emission over the polar cap (70–90° N) of 86×106 m−2 s−1 (mass emission increase of 23 μg m−2 s−1). This in turn leads to an increase in the natural aerosol optical depth of approximately 23%. In response to changes in aerosol optical depth, the natural component of the aerosol direct forcing over the Arctic polar cap is estimated to be between −0.2 and −0.4 W m−2 for the summer months, which results in a negative feedback on the system. The model predicts that the change in first indirect aerosol effect (cloud albedo effect) is approximately a factor of ten greater than the change in direct aerosol forcing although this result is highly uncertain due to the crude representation of Arctic clouds and aerosol-cloud interactions in the model. This study shows that both the natural aerosol direct and first indirect effects are strongly dependent on the surface albedo, highlighting the strong coupling between sea ice, aerosols, Arctic clouds and their radiative effects.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 14
    Publication Date: 2010-09-09
    Description: Unlike exhaust emissions, non-exhaust traffic emissions are completely unregulated and there are large uncertainties in the non-exhaust emission factors required to estimate the emissions of these aerosols. This study provides the first published results of direct measurements of size resolved emission factors for particles in the size range 0.25–2.5 μm using a new approach deriving aerosol emission factors from the CO2 emission fluxes. Because the aerosol and CO2 emissions have a common source and because the CO2 emission per fuel or traffic amount are much less uncertain than the aerosol emissions, this approach has obvious advantages. Therefore aerosol fluxes were measured during one year using the eddy covariance method at the top of a 118 m high communication tower over Stockholm, Sweden. Maximum CO2 and particle fluxes coincides with the wind direction with densest traffic within the footprint area. Negative fluxes (uptake of CO2 and deposition of particles) coincides with an urban forest area. The fluxes of CO2 were used to obtain emission factors for particles by assuming that the CO2 fluxes could converted to amounts of fuel burnt. The estimated emission factors for the fleet mix in the measurement area are, in number 1.4×1011 [particle veh−1 km−1]. Assuming spherical particles of density 1600 kg/m3 this corresponds to 27.5 mg veh−1 km−1. Wind speed influence the emission factor indicating that wind induced turbulence may be important.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 15
    Publication Date: 2005-07-29
    Description: Urban aerosol sources are important due to the health effects of particles and their potential impact on climate. Our aim has been to quantify and parameterise the urban aerosol source number flux F (particles m-2 s-1), in order to help improve how this source is represented in air quality and climate models. We applied an aerosol eddy covariance flux system 118.0 m above the city of Stockholm. This allowed us to measure the aerosol number flux for particles with diameters 〉11 nm. Upward source fluxes dominated completely over deposition fluxes in the collected dataset. Therefore, the measured fluxes were regarded as a good approximation of the aerosol surface sources. Upward fluxes were parameterised using a traffic activity (TA) database, which is based on traffic intensity measurement. The footprint (area on the surface from which sources and sinks affect flux measurements, located at one point in space) of the eddy system covered road and building construction areas, forests and residential areas, as well as roads with high traffic density and smaller streets. We found pronounced diurnal cycles in the particle flux data, which were well correlated with the diurnal cycles in traffic activities, strongly supporting the conclusion that the major part of the aerosol fluxes was due to traffic emissions. The emission factor for the fleet mix in the measurement area EFfm=1.4±0.1×1014 veh-1 km-1 was deduced. This agrees fairly well with other studies, although this study has an advantage of representing the actual effective emission from a mixed vehicle fleet. Emission from other sources, not traffic related, account for a F0=14±18×106 m-2 s-1. The urban aerosol source flux can then be written as F=EFfmTA+F0. In a second attempt to find a parameterisation, the friction velocity U* normalised with the average friction velocity has been included, F=EF. This parameterisation results in a somewhat reduced emission factor, 1.3×1014 veh-1 km-1. When multiple linear regression have been used, two emission factors are found, one for light duty vehicles EFLDV=0.3±0.3×1014 veh-1 km-1 and one for heavy-duty vehicles, EFHDV=19.8±4.0×1014 veh-1 km-1, and F0=18±16×106 m-2 s-1. The results show that during weekdays ~70–80% of the emissions came from HDV.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 16
    Publication Date: 2007-09-12
    Description: Primary marine aerosol fluxes were measured using eddy covariance (EC), a condensation particle counter (CPC) and an optical particle counter (OPC) with a heated inlet. The later was used to discriminate between sea salt and total aerosol. Measurements were made from the 25 m tower at the research station Mace Head at the Irish west coast, May to September 2002. The aerosol fluxes were dominated by upward fluxes, sea spray from bubble bursting at the ocean surface. The sea salt aerosol number emissions increased two orders of magnitude with declining diameter from 1 to 0.1 μm where it peaked at values of 105 to 107 particles m−2s−1. The sea salt emissions increased at all sizes in the wind range 4 to 22 ms−1, in consistency with a power function of the wind speed. The sea salt emission data were compared to three recent sub micrometer sea salt source parameterisations. The best agreement was with Mårtensson et al. (2003), which appear to apply from 0.1 to 1.1 μm diameters in temperate water (12°C) as well as tropical water (25°C). The total aerosol emissions were independent of the wind speed below 10 ms−1, but increased with the wind above 10 ms−1. The aerosol volume emissions were larger for the total aerosol than for the sea salt at all wind speeds, while the sea salt number emissions approached the total number emissions at 15 ms−1. It is speculated that this is caused by organic carbon in the surface water that is depleted at high wind speeds. The data are consistent with an internal aerosol mixture of sea salt, organic carbon and water. Using the aerosol model by Ellison et al. (1999) (a mono-layer of organic carbon surrounding a water-sea-salt brine) we show that the total and sea salt aerosol emissions are consistent. This predict that the organic carbon fraction increase with decreasing diameter from a few % at 1 μm over 50% at about 0.5 μm to about 90% at 0.1 μm, in consistency with simultaneous chemical data by Cavalli et al. (2004). The combined models of Mårtensson et al. (2003) and Ellison et al. (1999) reproduce the observed total aerosol emissions and offer an approach to model the organic sea spray fraction.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 17
    Publication Date: 2009-08-19
    Description: Number fluxes of particles with diameter larger than 10 nm were measured with the eddy covariance method over the Amazon rain forest during the wet season as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) campaign 2008. The primary goal was to investigate whether sources or sinks dominate the aerosol number flux in the tropical rain forest-atmosphere system. During the measurement campaign, from 12 March to 18 May, 60% of the particle fluxes pointed downward, which is a similar fraction to what has been observed over boreal forests. The particle transfer velocity vt increased with increasing friction velocity and the relation is described by the equation vt=2.4×10−3·u∗ where u∗ is the friction velocity. Upward particle fluxes often appeared in the morning hours and seem to a large extent to be an effect of entrainment fluxes into a growing mixed layer rather than primary aerosol emission. In general, primary aerosol emission had a limited impact on the total aerosol number population in this study, possibly because the measured particle number fluxes reflect mostly particles less than approximately 200 nm. The net deposition flux prevailed even in the absolute cleanest atmospheric conditions during the campaign and therefore cannot be explained only by deposition of anthropogenic particles. It seems that a significant contribution of secondary aerosol particles to the aerosol population is the most reasonable explanation for the net downward flux. This is an indication that secondary aerosol particles may dominate the aerosol number population in the Amazon boundary layer and that the contribution of primary aerosol particles may be low in terms of numbers. However, aerosol flux measurements should be repeated in a more remote area of the Amazon with less influence from anthropogenic sources before any final conclusions may be drawn.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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