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- ItemLong-term cloud condensation nuclei number concentration, particle number size distribution and chemical composition measurements at regionally representative observatories(Katlenburg-Lindau : EGU, 2018) Schmale, Julia; Henning, Silvia; Decesari, Stefano; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Pöhlker, Mira L.; Brito, Joel; Bougiatioti, Aikaterini; Kristensson, Adam; Kalivitis, Nikos; Stavroulas, Iasonas; Carbone, Samara; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Iwamoto, Yoko; Aalto, Pasi; Äijälä, Mikko; Bukowiecki, Nicolas; Ehn, Mikael; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Herrmann, Erik; Herrmann, Hartmut; Holzinger, Rupert; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Nenes, Athanasios; O'Dowd, Colin; Petäjä, Tuukka; Picard, David; Pöhlker, Christopher; Pöschl, Ulrich; Poulain, Laurent; Prévôt, André Stephan Henry; Swietlicki, Erik; Andreae, Meinrat O.; Artaxo, Paulo; Wiedensohler, Alfred; Ogren, John; Matsuki, Atsushi; Yum, Seong Soo; Stratmann, Frank; Baltensperger, Urs; Gysel, MartinAerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set - ready to be used for model validation - of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles 20nm) across the range of 0.1 to 1.0% supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2-0.3). We performed closure studies based on -Köhler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of . The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating migrating-CCNCs to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved.
- ItemRegional modelling of Saharan dust and biomass-burning smoke, Part 2: Direct radiative forcing and atmospheric dynamic response(Milton Park : Taylor & Francis, 2017) Heinold, Bernd; Tegen, Ina; Bauer, Stefan; Wendisch, ManfredThe direct radiative forcing and dynamic atmospheric response due to Saharan dust and biomass-burning aerosol particles are presented for a case study during the SAMUM-2 field campaign in January and February 2008. The regional model system COSMO-MUSCAT is used. It allows online interaction of the computed dust and smoke load with the solar and terrestrial radiation and with the model dynamics. Model results of upward solar irradiances are evaluated against airborne radiation measurements in the Cape Verde region. The comparison shows a good agreement for the case of dust and smoke mixture. Dust and smoke particles influence the atmospheric dynamics by changing the radiative heating rates. The related pressure perturbations modify local and synoptic scale air-flow patterns. In the radiative feedback simulations, the Hadley circulation is enhanced and convergence zones occur along the Guinea coast. Thus, the smoke particles spread more than 5◦ further north and the equatorward transport is reduced. Within the convergence zones, Saharan dust and biomass-burning material are more effectively advected towards the Cape Verdes. Given the model uncertainties, the agreement between the modelled and observed aerosol distribution is locally improved when aerosol–radiation interaction is considered.
- ItemCollocated observations of cloud condensation nuclei, particle size distributions, and chemical composition(London : Nature Publ. Group, 2017) Schmale, Julia; Henning, Silvia; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Bougiatioti, Aikaterini; Kalivitis, Nikos; Stavroulas, Iasonas; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Kristensson, Adam; Iwamoto, Yoko; Pringle, Kirsty; Reddington, Carly; Aalto, Pasi; Äijälä, Mikko; Baltensperger, Urs; Bialek, Jakub; Birmili, Wolfram; Bukowiecki, Nicolas; Ehn, Mikael; Fjæraa, Ann Mari; Fiebig, Markus; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Furuya, Masaki; Hammer, Emanuel; Heikkinen, Liine; Herrmann, Erik; Holzinger, Rupert; Hyono, Hiroyuki; Kanakidou, Maria; Kiendler-Scharr, Astrid; Kinouchi, Kento; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Motos, Ghislain; Nenes, Athanasios; O’Dowd, Colin; Paramonov, Mikhail; Petäjä, Tuukka; Picard, David; Poulain, Laurent; Prévôt, André Stephan Henry; Slowik, Jay; Sonntag, Andre; Swietlicki, Erik; Svenningsson, Birgitta; Tsurumaru, Hiroshi; Wiedensohler, Alfred; Wittbom, Cerina; Ogren, John A.; Matsuki, Atsushi; Yum, Seong Soo; Myhre, Cathrine Lund; Carslaw, Ken; Stratmann, Frank; Gysel, MartinCloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.
- ItemSolar radiative effects of a Saharan dust plume observed during SAMUM assuming spheroidal model particles(Milton Park : Taylor & Francis, 2017) Otto, Sebastian; Bierwirth, Eike; Weinzierl, Bernadett; Kandler, Konrad; Esselborn, Michael; Tesche, Matthias; Schladitz, Alexander; Wendisch, Manfred; Trautmann, ThomasThe solar optical properties of Saharan mineral dust observed during the Saharan Mineral Dust Experiment (SAMUM) were explored based on measured size-number distributions and chemical composition. The size-resolved complex refractive index of the dust was derived with real parts of 1.51–1.55 and imaginary parts of 0.0008–0.006 at 550 nm wavelength. At this spectral range a single scattering albedo ωo and an asymmetry parameter g of about 0.8 were derived. These values were largely determined by the presence of coarse particles. Backscatter coefficients and lidar ratios calculated with Mie theory (spherical particles) were not found to be in agreement with independently measured lidar data. Obviously the measured Saharan mineral dust particles were of non-spherical shape. With the help of these lidar and sun photometer measurements the particle shape as well as the spherical equivalence were estimated. It turned out that volume equivalent oblate spheroids with an effective axis ratio of 1:1.6 matched these data best. This aspect ratio was also confirmed by independent single particle analyses using a scanning electron microscope. In order to perform the non-spherical computations, a database of single particle optical properties was assembled for oblate and prolate spheroidal particles. These data were also the basis for simulating the non-sphericity effects on the dust optical properties: ωo is influenced by up to a magnitude of only 1% and g is diminished by up to 4% assuming volume equivalent oblate spheroids with an axis ratio of 1:1.6 instead of spheres. Changes in the extinction optical depth are within 3.5%. Non-spherical particles affect the downwelling radiative transfer close to the bottom of the atmosphere, however, they significantly enhance the backscattering towards the top of the atmosphere: Compared to Mie theory the particle non-sphericity leads to forced cooling of the Earth-atmosphere system in the solar spectral range for both dust over ocean and desert.