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    One year of Raman lidar observations of free-tropospheric aerosol layers over South Africa
    (München : European Geopyhsical Union, 2015) Giannakaki, E.; Pfüller, A.; Korhonen, K.; Mielonen, T.; Laakso, L.; Vakkari, V.; Baars, H.; Engelmann, R.; Beukes, J.P.; Van Zyl, P.G.; Josipovic, M.; Tiitta, P.; Chiloane, K.; Piketh, S.; Lihavainen, H.; Lehtinen, K.E.J.; Komppula, M.
    Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46%.
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    Four-dimensional distribution of the 2010 Eyjafjallajökull volcanic cloud over Europe observed by EARLINET
    (München : European Geopyhsical Union, 2013) Pappalardo, G.; Mona, L.; D'Amico, G.; Wandinger, U.; Adam, M.; Amodeo, A.; Ansmann, A.; Apituley, A.; Alados Arboledas, L.; Balis, D.; Boselli, A.; Bravo-Aranda, J.A.; Chaikovsky, A.; Comeron, A.; Cuesta, J.; De Tomasi, F.; Freudenthaler, V.; Gausa, M.; Giannakaki, E.; Giehl, H.; Giunta, A.; Grigorov, I.; Groß, S.; Haeffelin, M.; Hiebsch, A.; Iarlori, M.; Lange, D.; Linné, H.; Madonna, F.; Mattis, I.; Mamouri, R.-E.; McAuliffe, M.A.P.; Mitev, V.; Molero, F.; Navas-Guzman, F.; Nicolae, D.; Papayannis, A.; Perrone, M.R.; Pietras, C.; Pietruczuk, A.; Pisani, G.; Preißler, J.; Pujadas, M.; Rizi, V.; Ruth, A.A.; Schmidt, J.; Schnell, F.; Seifert, P.; Serikov, I.; Sicard, M.; Simeonov, V.; Spinelli, N.; Stebel, K.; Tesche, M.; Trickl, T.; Wang, X.; Wagner, F.; Wiegner, M.; Wilson, K.M.
    The eruption of the Icelandic volcano Eyjafjallajökull in April–May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April–26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org. During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5–15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area. The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events.
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    Long-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela – Sources, impacts and interannual variability
    (München : European Geopyhsical Union, 2013) Hamburger, T.; Matisāns, M.; Tunved, P.; Ström, J.; Calderon, S.; Hoffmann, P.; Hochschild, G.; Gross, J.; Schmeissner, T.; Wiedensohler, A.; Krejci, R.
    First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4±1.3 μm3 cm−3, refractory particle number concentrations (at 300 °C) 510±420 cm−3 and the absorption coefficient 0.91±1.2 Mm−1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19±0.25 μm3 cm−3, 150±94 cm−3 and 0.15±0.26 Mm−1. A decrease of particle concentrations during the dry seasons from 2007–2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño–Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.
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    Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation
    (München : European Geopyhsical Union, 2010) Spracklen, D.V.; Carslaw, K.S.; Merikanto, J.; Mann, G.W.; Reddington, C.L.; Pickering, S.; Ogren, J.A.; Andrews, E.; Baltensperger, U.; Weingartner, E.; Boy, M.; Kulmala, M.; Laakso, L.; Lihavainen, H.; Kivekäs, N.; Komppula, M.; Mihalopoulos, N.; Kouvarakis, G.; Jennings, S.G.; O'Dowd, C.; Birmili, W.; Wiedensohler, A.; Weller, R.; Gras, J.; Laj, P.; Sellegri, K.; Bonn, B.; Krejci, R.; Laaksonen, A.; Hamed, A.; Minikin, A.; Harrison, R.M.; Talbot, R.; Sun, J.
    We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
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    Overview of the synoptic and pollution situation over Europe during the EUCAARI-LONGREX field campaign
    (München : European Geopyhsical Union, 2011) Hamburger, T.; McMeeking, G.; Minikin, A.; Birmili, W.; Dall'Osto, M.; O'Dowd, C.; Flentje, H.; Henzing, B.; Junninen, H.; Kristensson, A.; de Leeuw, G.; Stohl, A.; Burkhart, J.F.; Coe, H.; Krejci, R.; Petzold, A.
    In May 2008 the EUCAARI-LONGREX aircraft field campaign was conducted within the EUCAARI intensive observational period. The campaign aimed at studying the distribution and evolution of air mass properties on a continental scale. Airborne aerosol and trace gas measurements were performed aboard the German DLR Falcon 20 and the British FAAM BAe-146 aircraft. This paper outlines the meteorological situation over Europe during May 2008 and the temporal and spatial evolution of predominantly anthropogenic particulate pollution inside the boundary layer and the free troposphere. Time series data of six selected ground stations are used to discuss continuous measurements besides the single flights. The observations encompass total and accumulation mode particle number concentration (0.1–0.8 μm) and black carbon mass concentration as well as several meteorological parameters. Vertical profiles of total aerosol number concentration up to 10 km are compared to vertical profiles probed during previous studies. During the first half of May 2008 an anticyclonic blocking event dominated the weather over Central Europe. It led to increased pollutant concentrations within the centre of the high pressure inside the boundary layer. Due to long-range transport the accumulated pollution was partly advected towards Western and Northern Europe. The measured aerosol number concentrations over Central Europe showed in the boundary layer high values up to 14 000 cm−3 for particles in diameter larger 10 nm and 2300 cm−3 for accumulation mode particles during the high pressure period, whereas the middle free troposphere showed rather low concentrations of particulates. Thus a strong negative gradient of aerosol concentrations between the well mixed boundary layer and the clean middle troposphere occurred.