2015, Crenn, V., Sciare, J., Croteau, P.L., Verlhac, S., Fröhlich, R., Belis, C.A., Aas, W., Äijälä, M., Alastuey, A., Artiñano, B., Baisnée, D., Bonnaire, N., Bressi, M., Canagaratna, M., Canonaco, F., Carbone, C., Cavalli, F., Coz, E., Cubison, M.J., Esser-Gietl, J.K., Green, D.C., Gros, V., Heikkinen, L., Herrmann, H., Lunder, C., Minguillón, M.C., Močnik, G., O'Dowd, C.D., Ovadnevaite, J., Petit, J.-E., Petralia, E., Poulain, L., Priestman, M., Riffault, V., Ripoll, A., Sarda-Estève, R., Slowik, J.G., Setyan, A., Wiedensohler, A., Baltensperger, U., Prévôt, A.S.H., Jayne, J.T., Favez, O.

As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall – early-winter period (November–December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36 % for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some recommendations about best calibration practices, standardized data processing, and data treatment.

2015, Yttri, K.E., Schnelle-Kreis, J., Maenhaut, W., Abbaszade, G., Alves, C., Bjerke, A., Bonnier, N., Bossi, R., Claeys, M., Dye, C., Evtyugina, M., García-Gacio, D., Hillamo, R., Hoffer, A., Hyder, M., Iinuma, Y., Jaffrezo, J.-L., Kasper-Giebl, A., Kiss, G., López-Mahia, P.L., Pio, C., Piot, C., Ramirez-Santa-Cruz, C., Sciare, J., Teinilä, K., Vermeylen, R., Vicente, A., Zimmermann, R.

The monosaccharide anhydrides (MAs) levoglucosan, galactosan and mannosan are products of incomplete combustion and pyrolysis of cellulose and hemicelluloses, and are found to be major constituents of biomass burning (BB) aerosol particles. Hence, ambient aerosol particle concentrations of levoglucosan are commonly used to study the influence of residential wood burning, agricultural waste burning and wildfire emissions on ambient air quality. A European-wide intercomparison on the analysis of the three monosaccharide anhydrides was conducted based on ambient aerosol quartz fiber filter samples collected at a Norwegian urban background site during winter. Thus, the samples' content of MAs is representative for BB particles originating from residential wood burning. The purpose of the intercomparison was to examine the comparability of the great diversity of analytical methods used for analysis of levoglucosan, mannosan and galactosan in ambient aerosol filter samples. Thirteen laboratories participated, of which three applied high-performance anion-exchange chromatography (HPAEC), four used high-performance liquid chromatography (HPLC) or ultra-performance liquid chromatography (UPLC) and six resorted to gas chromatography (GC). The analytical methods used were of such diversity that they should be considered as thirteen different analytical methods. All of the thirteen laboratories reported levels of levoglucosan, whereas nine reported data for mannosan and/or galactosan. Eight of the thirteen laboratories reported levels for all three isomers. The accuracy for levoglucosan, presented as the mean percentage error (PE) for each participating laboratory, varied from −63 to 20%; however, for 62% of the laboratories the mean PE was within ±10%, and for 85% the mean PE was within ±20%. For mannosan, the corresponding range was −60 to 69%, but as for levoglucosan, the range was substantially smaller for a subselection of the laboratories; i.e. for 33% of the laboratories the mean PE was within ±10%. For galactosan, the mean PE for the participating laboratories ranged from −84 to 593%, and as for mannosan 33% of the laboratories reported a mean PE within ±10%. The variability of the various analytical methods, as defined by their minimum and maximum PE value, was typically better for levoglucosan than for mannosan and galactosan, ranging from 3.2 to 41% for levoglucosan, from 10 to 67% for mannosan and from 6 to 364% for galactosan. For the levoglucosan to mannosan ratio, which may be used to assess the relative importance of softwood versus hardwood burning, the variability only ranged from 3.5 to 24 . To our knowledge, this is the first major intercomparison on analytical methods used to quantify monosaccharide anhydrides in ambient aerosol filter samples conducted and reported in the scientific literature. The results show that for levoglucosan the accuracy is only slightly lower than that reported for analysis of SO42- (sulfate) on filter samples, a constituent that has been analysed by numerous laboratories for several decades, typically by ion chromatography and which is considered a fairly easy constituent to measure. Hence, the results obtained for levoglucosan with respect to accuracy are encouraging and suggest that levels of levoglucosan, and to a lesser extent mannosan and galactosan, obtained by most of the analytical methods currently used to quantify monosaccharide anhydrides in ambient aerosol filter samples, are comparable. Finally, the various analytical methods used in the current study should be tested for other aerosol matrices and concentrations as well, the most obvious being summertime aerosol samples affected by wildfires and/or agricultural fires.

2015, Altstädter, B., Platis, A., Wehner, B., Scholtz, A., Wildmann, N., Hermann, M., Käthner, R., Baars, H., Bange, J., Lampert, A.

This paper presents the unmanned research aircraft Carolo P360 "ALADINA" (Application of Light-weight Aircraft for Detecting IN situ Aerosol) for investigating the horizontal and vertical distribution of ultrafine particles in the atmospheric boundary layer (ABL). It has a wingspan of 3.6 m, a maximum take-off weight of 25 kg and is equipped with aerosol instrumentation and meteorological sensors. A first application of the system, together with the unmanned research aircraft MASC (Multi-Purpose Airborne Carrier) of the Eberhard Karls University of Tübingen (EKUT), is described. As small payload for ALADINA, two condensation particle counters (CPC) and one optical particle counter (OPC) were miniaturised by re-arranging the vital parts and composing them in a space-saving way in the front compartment of the airframe. The CPCs are improved concerning the lower detection threshold and the response time to less than 1.3 s. Each system was characterised in the laboratory and calibrated with test aerosols. The CPCs are operated in this study with two different lower detection threshold diameters of 11 and 18 nm. The amount of ultrafine particles, which is an indicator for new particle formation, is derived from the difference in number concentrations of the two CPCs (ΔN). Turbulence and thermodynamic structure of the boundary layer are described by measurements of fast meteorological sensors that are mounted at the aircraft nose. A first demonstration of ALADINA and a feasibility study were conducted in Melpitz near Leipzig, Germany, at the Global Atmosphere Watch (GAW) station of the Leibniz Institute for Tropospheric Research (TROPOS) on 2 days in October 2013. There, various ground-based instruments are installed for long-term atmospheric monitoring. The ground-based infrastructure provides valuable additional background information to embed the flights in the continuous atmospheric context and is used for validation of the airborne results. The development of the boundary layer, derived from backscatter signals of a portable Raman lidar POLLYXT, allows a quick overview of the current vertical structure of atmospheric particles. Ground-based aerosol number concentrations are consistent with the results from flights in heights of a few metres. In addition, a direct comparison of ALADINA aerosol data and ground-based aerosol data, sampling the air at the same location for more than 1 h, shows comparable values within the range of ± 20 %. MASC was operated simultaneously with complementary flight patterns. It is equipped with the same meteorological instruments that offer the possibility to determine turbulent fluxes. Therefore, additional information about meteorological conditions was collected in the lowest part of the atmosphere. Vertical profiles up to 1000 m in altitude indicate a high variability with distinct layers of aerosol, especially for the small particles of a few nanometres in diameter on 1 particular day. The stratification was almost neutral and two significant aerosol layers were detected with total aerosol number concentrations up to 17 000 ± 3400 cm−3 between 180 and 220 m altitude and 14 000 ± 2800 cm−3 between 550 and 650 m. Apart from those layers, the aerosol distribution was well mixed and reached the total number concentration of less than 8000 ± 1600 cm−3. During another day, the distribution of the small particles in the lowermost ABL was related to the stratification, with continuously decreasing number concentrations from 16 000 ± 3200 cm−3 to a minimum of 4000 ± 800 cm−3 at the top of the inversion at 320 m. Above this, the total number concentration was rather constant. In the region of 500 to 600 m altitude, a significant difference of both CPCs was observed. This event occurred during the boundary layer development in the morning and represents a particle burst within the ABL.

2015, Paramonov, M., Kerminen, V.-M., Gysel, M., Aalto, P.P., Andreae, M.O., Asmi, E., Baltensperger, U., Bougiatioti, A., Brus, D., Frank, G.P., Good, N., Gunthe, S.S., Hao, L., Irwin, M., Jaatinen, A., Jurányi, Z., King, S.M., Kortelainen, A., Kristensson, A., Lihavainen, H., Kulmala, M., Lohmann, U., Martin, S.T., McFiggans, G., Mihalopoulos, N., Nenes, A., O'Dowd, C.D., Ovadnevaite, J., Petäjä, T., Pöschl, U., Roberts, G.C., Rose, D., Svenningsson, B., Swietlicki, E., Weingartner, E., Whitehead, J., Wiedensohler, A., Wittbom, C., Sierau, B.

Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (NCCN) to the total number concentration of particles (NCN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations – exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A50 and A100, respectively) renders a much more stable dependence of A on S; A50 and A100 also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter κ decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations κ increased with size. In fact, in Hyytiälä, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5 % significance level. In a boreal environment the assumption of a size-independent κ can lead to a potentially substantial overestimation of NCCN at S levels above 0.6 %. The same is true for other locations where κ was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of NCCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol–cloud interactions in various environments.

2015, Binietoglou, I., Basart, S., Alados-Arboledas, L., Amiridis, V., Argyrouli, A., Baars, H., Baldasano, J.M., Balis, D., Belegante, L., Bravo-Aranda, J.A., Burlizzi, P., Carrasco, V., Chaikovsky, A., Comerón, A., D'Amico, G., Filioglou, M., Granados-Muñoz, M.J., Haefele, A., Hervo, M., Iarlori, M., Kokkalis, P., Lange, D., Mamouri, R.E., Mattis, I., Molero, F., Montoux, N., Muñoz, A., Muñoz Porcar, C., Navas-Guzmán, F., Nicolae, D., Nisantzi, A., Papagiannopoulos, N., Papayannis, A., Pereira, S., Preißler, J., Pujadas, M., Rizi, V., Rocadenbosch, F., Sellegri, K., Simeonov, V., Tsaknakis, G., Wagner, F., Pappalardo, G.

Systematic measurements of dust concentration profiles at a continental scale were recently made possible by the development of synergistic retrieval algorithms using combined lidar and sun photometer data and the establishment of robust remote-sensing networks in the framework of Aerosols, Clouds, and Trace gases Research InfraStructure Network (ACTRIS)/European Aerosol Research Lidar Network (EARLINET). We present a methodology for using these capabilities as a tool for examining the performance of dust transport models. The methodology includes considerations for the selection of a suitable data set and appropriate metrics for the exploration of the results. The approach is demonstrated for four regional dust transport models (BSC-DREAM8b v2, NMMB/BSC-DUST, DREAMABOL, DREAM8-NMME-MACC) using dust observations performed at 10 ACTRIS/EARLINET stations. The observations, which include coincident multi-wavelength lidar and sun photometer measurements, were processed with the Lidar-Radiometer Inversion Code (LIRIC) to retrieve aerosol concentration profiles. The methodology proposed here shows advantages when compared to traditional evaluation techniques that utilize separately the available measurements such as separating the contribution of dust from other aerosol types on the lidar profiles and avoiding model assumptions related to the conversion of concentration fields to aerosol extinction values. When compared to LIRIC retrievals, the simulated dust vertical structures were found to be in good agreement for all models with correlation values between 0.5 and 0.7 in the 1–6 km range, where most dust is typically observed. The absolute dust concentration was typically underestimated with mean bias values of -40 to -20 μg m−3 at 2 km, the altitude of maximum mean concentration. The reported differences among the models found in this comparison indicate the benefit of the systematic use of the proposed approach in future dust model evaluation studies.