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- ItemCharacterization of Saharan dust, marine aerosols and mixtures of biomass-burning aerosols and dust by means of multi-wavelength depolarization and Raman lidar measurements during SAMUM 2(Milton Park : Taylor & Francis, 2017) Groß, Silke; Tesche, Matthias; Freudenthaler, Volker; Toledano, Carlos; Wiegner, Matthias; Ansmann, Albert; Althausen, Dietrich; Seefeldner, MeinhardThe particle linear depolarization ratio δp of Saharan dust, marine aerosols and mixtures of biomass-burning aerosols from southern West Africa and Saharan dust was determined at three wavelengths with three lidar systems during the SAharan Mineral dUst experiMent 2 at the airport of Praia, Cape Verde, between 22 January and 9 February 2008. The lidar ratio Sp of these major types of tropospheric aerosols was analysed at two wavelengths. For Saharan dust, we find wavelength dependent mean particle linear depolarization ratios δp of 0.24–0.27 at 355 nm, 0.29–0.31 at 532 nm and 0.36–0.40 at 710 nm, and wavelength independent mean lidar ratios Sp of 48–70 sr. Mixtures of biomass-burning aerosols and dust show wavelength independent values of δp and Sp between 0.12–0.23 and 57–98 sr, respectively. The mean values of marine aerosols range independent of wavelength for δp from 0.01 to 0.03 and for Sp from 14 to 24 sr.
- ItemDust mobilization and aerosol transport from West Africa to Cape Verde - a meteorological overview of SAMUM-2(Milton Park : Taylor & Francis, 2017) Knippertz, Peter; Tesche, Matthias; Heinold, Bernd; Kandler, Konrad; Toledano, Carlos; Esselborn, MichaelThe second field campaign of the SAharan Mineral dUst experiMent (SAMUM-2) was performed between 15 January and 14 February 2008 at the airport of Praia, Cape Verde, and provided valuable information to study the westward transport of Saharan dust and the mixing with biomass-burning smoke and sea-salt aerosol. Here lidar, meteorological, and particle measurements at Praia, together with operational analyses, trajectories, and satellite and synoptic station data are used to give an overview of the meteorological conditions and to place other SAMUM-2 measurements into a large-scale context. It is demonstrated that wintertime dust conditions at Cape Verde are closely related to the movement and intensification of mid-latitude high-pressure systems and the associated pressure gradients at their southern flanks. These cause dust emission over Mauritania, Mali, and Niger, and subsequent westward transport to Cape Verde within about 1–5 d. Dust emissions often peak around midday, suggesting a relation to daytime mixing of momentum from nocturnal low-level jets to the surface. The dust layer over Cape Verde is usually restricted to the lowest 1.5 km of the atmosphere. During periods with near-surface wind speeds about 5.5 ms−1, a maritime aerosol layer develops which often mixes with dust from above. On most days, the middle levels up to about 5 km additionally contain smoke that can be traced back to sources in southernWest Africa. Above this layer, clean air masses are transported to Cape Verde with the westerly flow at the southern side of the subtropical jet. The penetration of extra-tropical disturbances to low latitudes can bring troposphere-deep westerly flow and unusually clean conditions to the region.
- ItemOne 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%.
- ItemLong-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.
- ItemMulti-wavelength Raman lidar, sun photometric and aircraft measurements in combination with inversion models for the estimation of the aerosol optical and physico-chemical properties over Athens, Greece(München : European Geopyhsical Union, 2012) Mamouri, R.E.; Papayannis, A.; Amiridis, V.; Müller, D.; Kokkalis, P.; Rapsomanikis, S.; Karageorgos, E.T.; Tsaknakis, G.; Nenes, A.; Kazadzis, S.; Remoundaki, E.A novel procedure has been developed to retrieve, simultaneously, the optical, microphysical and chemical properties of tropospheric aerosols with a multi-wavelength Raman lidar system in the troposphere over an urban site (Athens, Greece: 37.9° N, 23.6° E, 200 m a.s.l.) using data obtained during the European Space Agency (ESA) THERMOPOLIS project, which took place between 15–31 July 2009 over the Greater Athens Area (GAA). We selected to apply our procedure for a case study of intense aerosol layers that occurred on 20–21 July 2009. The National Technical University of Athens (NTUA) EOLE 6-wavelength Raman lidar system has been used to provide the vertical profiles of the optical properties of aerosols (extinction and backscatter coefficients, lidar ratio) and the water vapor mixing ratio. An inversion algorithm was used to derive the mean aerosol microphysical properties (mean effective radius (reff), single-scattering albedo ω) and mean complex refractive index (m)) at selected heights in the 2–3 km height region. We found that reff was 0.14–0.4 (±0.14) μm, ω was 0.63–0.88 (±0.08) (at 532 nm) and m ranged from 1.44 (±0.10) + 0.01 (±0.01)i to 1.55 (±0.12) + 0.06 (±0.02)i, in good agreement (only for the reff values) with in situ aircraft measurements. The water vapor and temperature profiles were incorporated into the ISORROPIA II model to propose a possible in situ aerosol composition consistent with the retrieved m and ω values. The retrieved aerosol chemical composition in the 2–3 km height region gave a variable range of sulfate (0–60%) and organic carbon (OC) content (0–50%), although the OC content increased (up to 50%) and the sulfate content dropped (up to 30%) around 3 km height; the retrieved low ω value (0.63), indicates the presence of absorbing biomass burning smoke mixed with urban haze. Finally, the retrieved aerosol microphysical properties were compared with column-integrated sun photometer CIMEL data.
- ItemPolarization lidar: An extended three-signal calibration approach(Katlenburg-Lindau : Copernicus, 2019) Jimenez, Cristofer; Ansmann, Albert; Engelmann, Ronny; Haarig, Moritz; Schmidt, Jörg; Wandinger, UllaWe present a new formalism to calibrate a threesignal polarization lidar and to measure highly accurate height profiles of the volume linear depolarization ratios under realistic experimental conditions. The methodology considers elliptically polarized laser light, angular misalignment of the receiver unit with respect to the main polarization plane of the laser pulses, and cross talk among the receiver channels. A case study of a liquid-water cloud observation demonstrates the potential of the new technique. Long-term observations of the calibration parameters corroborate the robustness of the method and the long-term stability of the three-signal polarization lidar. A comparison with a second polarization lidar shows excellent agreement regarding the derived volume linear polarization ratios in different scenarios: A biomass burning smoke event throughout the troposphere and the lower stratosphere up to 16 km in height, a dust case, and also a cirrus cloud case. © Author(s) 2019.
- ItemMercury distribution in the upper troposphere and lowermost stratosphere according to measurements by the IAGOS-CARIBIC observatory: 2014-2016(Katlenburg-Lindau : EGU, 2018) Slemr, Franz; Weigelt, Andreas; Ebinghaus, Ralf; Bieser, Johannes; Brenninkmeijer, Carl A. M.; Rauthe-Schöch, Armin; Hermann, Markus; Martinsson, Bengt G.; van Velthoven, Peter; Bönisch, Harald; Neumaier, Marco; Zahn, Andreas; Ziereis, HelmutMercury was measured onboard the IAGOS-CARIBIC passenger aircraft from May 2005 until February 2016 during near monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Increased upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Speciation experiments suggest comparable TM and gaseous elementary mercury (GEM) concentrations at and below the tropopause leaving little space for Hg2+ (TM-thinsp;GEM) being the dominating component of TM here. In the stratosphere significant GEM concentrations were found to exist up to 4 km altitude above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72±37 and 74±27 years for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation and cloud scavenging processes.
- ItemPollution events observed during CARIBIC flights in the upper troposphere between South China and the Philippines(München : European Geopyhsical Union, 2010) Lai, S.C.; Baker, A.K.; Schuck, T.J.; van Velthoven, P.; Oram, D.E.; Zahn, A.; Hermann, M.; Weigelt, A.; Slemr, F.; Brenninkmeijer, C.A.M.; Ziereis, H.A strong pollution episode in the upper troposphere between South China and the Philippines was observed during CARIBIC flights in April 2007. Five pollution events were observed, where enhancements in aerosol and trace gas concentrations including CO, CO2, CH4, non-methane hydrocarbons (NMHCs) and halocarbons were observed along the flight tracks during four sequential flights. The importance of the contribution of biomass/biofuel burning was investigated using chemical tracers, emission factor analysis, back-trajectory analysis and satellite images. The Indochinese peninsula was identified as the probable source region of biomass/biofuel burning. However, enhancements in the urban/industrial tracer C2Cl4 during the events also indicate a substantial contribution from urban anthropogenic emissions. An estimation of the contribution of fossil fuel versus biomass/biofuel to the CO enhancement was made, indicating a biomass/biofuel burning contribution of ~54 to ~92% of the observed CO enhancements. Biomass/biofuel burning was found to be the most important source category during the sampling period.
- ItemVertical aerosol distribution in the southern hemispheric midlatitudes as observed with lidar in Punta Arenas, Chile (53.2° and 70.9° W), during ALPACA(Katlenburg-Lindau : EGU, 2019) Foth, Andreas; Kanitz, Thomas; Engelmann, Ronny; Baars, Holger; Radenz, Martin; Seifert, Patric; Barja, Boris; Fromm, Michael; Kalesse, Heike; Ansmann, AlbertWithin this publication, lidar observations of the vertical aerosol distribution above Punta Arenas, Chile (53.2 S and 70.9 W), which have been performed with the Raman lidar PollyXT from December 2009 to April 2010, are presented. Pristine marine aerosol conditions related to the prevailing westerly circulation dominated the measurements. Lofted aerosol layers could only be observed eight times during the whole measurement period. Two case studies are presented showing long-range transport of smoke from biomass burning in Australia and regionally transported dust from the Patagonian Desert, respectively. The aerosol sources are identified by trajectory analyses with the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) and FLEXible PARTicle dispersion model (FLEXPART). However, seven of the eight analysed cases with lofted layers show an aerosol optical thickness of less than 0.05. From the lidar observations, a mean planetary boundary layer (PBL) top height of 1150 350m was determined. An analysis of particle backscatter coefficients confirms that the majority of the aerosol is attributed to the PBL, while the free troposphere is characterized by a very low background aerosol concentration. The ground-based lidar observations at 532 and 1064 nm are supplemented by the Aerosol Robotic Network (AERONET) Sun photometers and the space-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). The averaged aerosol optical thickness (AOT) determined by CALIOP was 0:02 0:01 in Punta Arenas from 2009 to 2010. © Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
- ItemMolecular distributions of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls in PM2.5 collected at the top of Mt. Tai, North China, during the wheat burning season of 2014(Katlenburg-Lindau : EGU, 2018) Zhu, Yanhong; Yang, Lingxiao; Chen, Jianmin; Kawamura, Kimitaka; Sato, Mamiko; Tilgner, Andreas; van Pinxteren, Dominik; Chen, Ying; Xue, Likun; Wang, Xinfeng; Simpson, Isobel J.; Herrmann, Hartmut; Blake, Donald R.; Wang, WenxingFine particulate matter (PM2.5) samples collected at Mount (Mt.) Tai in the North China Plain during summer 2014 were analyzed for dicarboxylic acids and related compounds (oxocarboxylic acids and α-dicarbonyls) (DCRCs). The total concentration of DCRCs was 1050±580 and 1040±490ng m-3 during the day and night, respectively. Although these concentrations were about 2 times lower than similar measurements in 2006, the concentrations reported here were about 1-13 times higher than previous measurements in other major cities in the world. Molecular distributions of DCRCs revealed that oxalic acid (C2) was the dominant species (50%), followed by succinic acid (C4) (12%) and malonic acid (C3) (8%). WRF modeling revealed that Mt. Tai was mostly in the free troposphere during the campaign and long-range transport was a major factor governing the distributions of the measured compounds at Mt. Tai. A majority of the samples (79%) had comparable concentrations during the day and night, with their day-night concentration ratios between 0.9 and 1.1. Multi-day transport was considered an important reason for the similar concentrations. Correlation analyses of DCRCs and their gas precursors and between C2 and sulfate indicated precursor emissions and aqueous-phase oxidations during long-range transport also likely play an important role, especially during the night. Source identification indicated that anthropogenic activities followed by photochemical aging accounted for about 60% of the total variance and were the dominant source at Mt. Tai. However, biomass burning was only important during the first half of the measurement period. Measurements of potassium (K+) and DCRCs were about 2 times higher than those from the second half of the measurement period. The concentration of levoglucosan, a biomass burning tracer, decreased by about 80% between 2006 and 2014, indicating that biomass burning may have decreased between 2006 and 2014.