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Doppler lidar studies of heat island effects on vertical mixing of aerosols during SAMUM-2

2017, Engelmann, Ronny, Ansmann, Albert, Horn, Stefan, Seifert, Patric, Althausen, Dietrich, Tesche, Matthias, Esselborn, Michael, Fruntke, Julia, Lieke, Kirsten, Freudenthaler, Volker, Gross, Silke

A wind Doppler lidar was deployed next to three aerosol lidars during the SAMUM–2 campaign on the main island of Cape Verde. The effects of the differential heating of the island and the surrounding ocean and the orographic impact of the capital island Santiago and the small island on its luv side, Maio, are investigated. Horizontal and vertical winds were measured in the disturbed maritime boundary layer and compared to local radiosoundings. Lidar measurements from the research aircraft Falcon and a 3-D Large Eddy Simulation (LES) model were used in addition to study the heating effects on the scale of the islands. Indications are found that these effects can widely control the downward mixing from greater heights to the surface of African aerosols, mainly Saharan dust and biomass-burning smoke, which were detected in a complex layering over the Cape Verde region.

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Size distribution, mass concentration, chemical and mineralogical composition and derived optical parameters of the boundary layer aerosol at Tinfou, Morocco, during SAMUM 2006

2017, Kandler, K., Schütz, L., Deutscher, C., Ebert, M., Hofmann, H., Jäckel, S., Jaenicke, R., Knippertz, P., Lieke, K., Massling, A., Petzold, A., Schladitz, A., Weinzierl, B., Wiedensohler, A., Zorn, S., Weinbruch, S.

During the SAMUM 2006 field campaign in southern Morocco, physical and chemical properties of desert aerosols were measured. Mass concentrations ranging from 30μgm−3 for PM2.5 under desert background conditions up to 300 000μgm−3 for total suspended particles (TSP) during moderate dust storms were measured. TSP dust concentrations are correlated with the local wind speed, whereasPM10 andPM2.5 concentrations are determined by advection from distant sources. Size distributions were measured for particles with diameter between 20 nm and 500μm (parametrizations are given). Two major regimes of the size spectrum can be distinguished. For particles smaller than 500 nm diameter, the distributions show maxima around 80 nm, widely unaffected of varying meteorological and dust emission conditions. For particles larger than 500 nm, the range of variation may be up to one order of magnitude and up to three orders of magnitude for particles larger than 10μm. The mineralogical composition of aerosol bulk samples was measured by X-ray powder diffraction. Major constituents of the aerosol are quartz, potassium feldspar, plagioclase, calcite, hematite and the clay minerals illite, kaolinite and chlorite. A small temporal variability of the bulk mineralogical composition was encountered. The chemical composition of approximately 74 000 particles was determined by electron microscopic single particle analysis. Three size regimes are identified: for smaller than 500 nm in diameter, the aerosol consists of sulphates and mineral dust. For larger than 500 nm up to 50μm, mineral dust dominates, consisting mainly of silicates, and—to a lesser extent—carbonates and quartz. For diameters larger than 50μm, approximately half of the particles consist of quartz. Time series of the elemental composition show a moderate temporal variability of the major compounds. Calcium-dominated particles are enhanced during advection from a prominent dust source in Northern Africa (Chott El Djerid and surroundings). The particle aspect ratio was measured for all analysed particles. Its size dependence reflects that of the chemical composition. For larger than 500 nm particle diameter, a median aspect ratio of 1.6 is measured. Towards smaller particles, it decreases to about 1.3 (parametrizations are given). From the chemical/mineralogical composition, the aerosol complex refractive index was determined for several wavelengths from ultraviolet to near-infrared. Both real and imaginary parts show lower values for particles smaller than 500 nm in diameter (1.55–2.8 × 10−3i at 530 nm) and slightly higher values for larger particles (1.57–3.7 × 10−3i at 530 nm).

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Horizontal homogeneity and vertical extent of new particle formation events

2017, Wehner, Birgit, Siebert, Holger, Stratmann, Frank, Tuch, Thomas, Wiedensohler, Alfred, PetäJä, Tuukka, Dal Maso, Miikka, Kulmala, Markku

During the SATURN campaign 2002, new particle formation, i.e. the occurrence of ultrafine particles was investigated simultaneously at four ground-based measurement sites. The maximum distance between the sites was 50 km. Additionally, vertical profiles of aerosol particles from 5–10 nm have been measured by a tethered-balloonborne system at one of the sites. In general, two different scenarios have been found: (i) new particle formation was measured at all sites nearly in parallel with subsequent particle growth (homogeneous case) and (ii) new particle formation was observed at one to three sites irregularly (inhomogeneous case) where subsequent particle growth was often interrupted. The homogeneous case was connected with stable synoptical conditions, i.e. the region was influenced by a high pressure system. Here, the horizontal extent of the phenomenon has been estimated to be 400 km at maximum. In the vertical dimension, the ultrafine particles are well mixed within the entire boundary layer. In the inhomogeneous case the new particle formation depends mainly on the incoming solar radiation and was often interrupted due the occurrence of clouds. Thus, single point measurements are not representative for a larger region in that case.

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A simple non-linear analytical relationship between aerosol accumulation number and sub-micron volume, explaining their observed ratio in the clean and polluted marine boundary layer

2016, Van Dingenen, Rita, Virkkula, Aki O., Raes, Frank, Bates, Timothy S., Wiedensohler, Alfred

We propose an analytical expression for the relation between aerosol accumulation number and sub-micron volume over the marine boundary layer (MBL), based on a simple balance equation. By providing appropriate source and sink terms which account for entrainment, coagulation, in-cloud scavenging and condensational growth, the model is able to reproduce the observed ratio between MBL particles larger than 80 nm diameter (as a proxy for accumulation mode number) and submicron aerosol volume, from freshly polluted to background conditions. Entrainment and coagulation are essential in predicting the observed ratio. Budget and lifetime calculations show that, due to relatively low source rates of oceanic non-sea-salt-sulfate and sea-salt, the anthropogenic signature in aerosol volume remains significant even after 8 days of MBL transport.

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Characterization of the planetary boundary layer during SAMUM-2 by means of lidar measurements

2017, Groß, Silke, Gasteiger, Josef, Freudenthaler, Volker, Wiegner, Matthias, Geiß, Alexander, Schladitz, Alexander, Toledano, Carlos, Kandler, Konrad, Tesche, Matthias, Ansmann, Albert, Wiedensohler, Alfred

Measurements with two Raman-depolarization lidars of the Meteorological Institute of the Ludwig-Maximilians- Universit¨at, M¨unchen, Germany, performed during SAMUM-2, were used to characterize the planetary boundary layer (PBL) over Praia, Cape Verde. A novel approach was used to determine the volume fraction of dust υd in the PBL. This approach primarily relies on accurate measurements of the linear depolarization ratio. Comparisons with independent in situ measurements showed the reliability of this approach. Based on our retrievals, two different phases could be distinguished within the measurement period of almost one month. The first (22–31 January 2008) was characterized by high aerosol optical depth (AOD) in the PBL and large υd > 95%. During the second phase, the AOD in the PBL was considerably lower and υd less than ∼40%. These findings were in very good agreement with ground based in situ measurements, when ambient volume fractions are considered that were calculated from the actual measurements of the dry volume fraction. Only in cases when dust was not the dominating aerosol component (second phase), effects due to hygroscopic growth became important.

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Aerosol physical properties and processes in the lower marine boundary layer: A comparison of shipboard sub-micron data from ACE-1 and ACE-2

2016, Bates, Timothy S., Quinn, Patricia K., Covert, David S., Coffman, Derek J., Johnson, James E., Wiedensohler, Alfred

The goals of the IGAC Aerosol Characterization Experiments (ACE) are to determine and understand the properties and controlling processes of the aerosol in a globally representative range of natural and anthropogenically perturbed environments. ACE-1 was conducted in the remote marine atmosphere south of Australia while ACE-2 was conducted in the anthropogenically modified atmosphere of the Eastern North Atlantic. In-situ shipboard measurements from the RV Discoverer(ACE-1) and the RV Professor Vodyanitskiy(ACE-2), combined with calculated back trajectories can be used to define the physical properties of the sub-micron aerosol in marine boundary layer (MBL) air masses from the remote Southern Ocean, Western Europe, the Iberian coast, the Mediterranean and the background Atlantic Ocean. The differences in these aerosol properties, combined with dimethylsulfide, sulfur dioxide and meteorological measurements provide a means to assess processes that affect the aerosol distribution. The background sub-micron aerosol measured over the Atlantic Ocean during ACE-2 was more abundant (number and volume) and appeared to be more aged than that measured over the Southern Ocean during ACE-1. Based on seawater DMS measurements and wind speed, the oceanic source of non-sea-salt sulfur and sea-salt to the background marine atmosphere during ACE-1 and ACE-2 was similar. However, the synoptic meteorological pattern was quite different during ACE-1 and ACE-2. The frequent frontal passages during ACE-1 resulted in the mixing of nucleation mode particles into the marine boundary layer from the free troposphere and relatively short aerosol residence times. In the more stable meteorological setting of ACE-2, a significant nucleation mode aerosol was observed in the MBL only for a half day period associated with a weak frontal system. As a result of the longer MBL aerosol residence times, the average background ACE-2 accumulation mode aerosol had a larger diameter and higher number concentration than during ACE-1. The sub-micron aerosol number size distributions in the air masses that passed over Western Europe, the Mediterranean, and coastal Portugal were distinctly different from each other and the background aerosol. The differences can be attributed to the age of the air mass and the degree of cloud processing.

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An overview of the ACE-2 clear sky column closure experiment (CLEARCOLUMN)

2016, Russell, Philip B., Heintzenberg, Jost

As 1 of 6 focused ACE-2 activities, a clear sky column closure experiment (CLEARCOLUMN) took place in June/July 1997 at the southwest corner of Portugal, in the Canary Islands, and over the eastern Atlantic Ocean surrounding and linking those sites. Overdetermined sets of volumetric, vertical profile and columnar aerosol data were taken from the sea surface to~5 km asl by samplers and sensors at land sites (20–3570 m asl), on a ship, and on 4 aircraft. In addition, 5 satellites measured upwelling radiances used to derive properties of the aerosol column. Measurements were made in a wide range of conditions and locations (e.g., the marine boundary layer with and without continental pollution, the free troposphere with and without African dust). Numerous tests of local and column closure, using unidisciplinary and multidisciplinary approaches, were conducted. This paper summarizes the methodological approach, the experiment sites and platforms, the types of measurements made on each, the types of analyses conducted, and selected key results, as a guide to the more complete results presented in other papers in this special issue and elsewhere. Example results include determinations of aerosol single scattering albedo by several techniques, measurements of hygroscopic effects on particle light scattering and size, and a wide range in the degree of agreement found in closure tests. In general, the smallest discrepancies were found in comparisons among (1) different techniques to measure an optical property of the ambient, unperturbed aerosol (e.g., optical depth, extinction, or backscatter by sunphotometer, lidar, and/or satellite) or (2) different techniques to measure an aerosol that had passed through a common sampling process (e.g., nephelometer and size spectrometer measurements with the same or similar inlets, humidities and temperatures). Typically, larger discrepancies were found between techniques that measure the ambient, unperturbed aerosol and those that must reconstruct the ambient aerosol by accounting for (a) processes that occur during sampling (e.g., aerodynamic selection, evaporation of water and other volatile material) or ( b) calibrations that depend on aerosol characteristics (e.g., sizedependent density or refractive index). A primary reason for the discrepancies in such cases is the lack of validated hygroscopic growth models covering the necessary range of particle sizes and compositions. Other common reasons include (1) using analysis or retrieval techniques that assume aerosol properties (e.g., density, single scattering albedo, shape) that do not apply in all cases and (2) using surface measurements to estimate column properties. Taken together, the ACE-2 CLEARCOLUMN data set provides a large collection of new information on the properties of the aerosol over the northeast Atlantic Ocean. CLEARCOLUMN studies have also pointed to improved techniques for analyzing current and future data sets (including satellite data sets) which will provide a more accurate and comprehensive description of the Atlantic–European–African aerosol. Thus they set the stage for an improved regional quantification of radiative forcing by anthropogenic aerosols.