2011, Asmi, A., Wiedensohler, A., Laj, P., Fjaeraa, A.-M., Sellegri, K., Birmili, W., Weingartner, E., Baltensperger, U., Zdimal, V., Zikova, N., Putaud, J.-P., Marinoni, A., Tunved, P., Hansson, H.-C., Fiebig, M., Kivekäs, N., Lihavainen, H., Asmi, E., Ulevicius, V., Aalto, P.P., Swietlicki, E., Kristensson, A., Mihalopoulos, N., Kalivitis, N., Kalapov, I., Kiss, G., de Leeuw, G., Henzing, B., Harrison, R.M., Beddows, D., O'Dowd, C., Jennings, S.G., Flentje, H., Weinhold, K., Meinhardt, F., Ries, L., Kulmala, M.

Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-\AA lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.

2013, Asmi, A., Collaud Coen, M., Ogren, J.A., Andrews, E., Sheridan, P., Jefferson, A., Weingartner, E., Baltensperger, U., Bukowiecki, N., Lihavainen, H., Kivekäs, N., Asmi, E., Aalto, P.P., Kulmala, M., Wiedensohler, A., Birmili, W., Hamed, A., O'Dowd, C., Jennings, S.G., Weller, R., Flentje, H., Fjaeraa, A.M., Fiebig, M., Myhre, C.L., Hallar, A.G., Swietlicki, E., Kristensson, A., Laj, P.

We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.

2012, Laakso, L., Vakkari, V., Virkkula, A., Laakso, H., Backman, J., Kulmala, M., Beukes, J.P., van Zyl, P.G., Tiitta, P., Josipovic, M., Pienaar, J.J., Chiloane, K., Gilardoni, S., Vignati, E., Wiedensohler, A., Tuch, T., Birmili, W., Piketh, S., Collett, K., Fourie, G.D., Komppula, M., Lihavainen, H., de Leeuw, G., Kerminen, V.-M.

In this paper we introduce new in situ observations of atmospheric aerosols, especially chemical composition, physical and optical properties, on the eastern brink of the heavily polluted Highveld area in South Africa. During the observation period between 11 February 2009 and 31 January 2011, the mean particle number concentration (size range 10–840 nm) was 6310 cm3 and the estimated volume of sub-10 μm particles 9.3 μm3 m−3. The aerosol absorption and scattering coefficients at 637 nm were 8.3 Mm−1 and 49.5 Mm−1, respectively. The mean single-scattering albedo at 637 nm was 0.84 and the Ångström exponent of scattering was 1.5 over the wavelength range 450–635 nm. The mean O3, SO2, NOx and H2S-concentrations were 37.1, 11.5, 15.1 and 3.2 ppb, respectively. The observed range of concentrations was large and attributed to the seasonal variation of sources and regional meteorological effects, especially the anticyclonic re-circulation and strong winter-time inversions. In a global context, the levels of gases and particulates were typical for continental sites with strong anthropogenic influence, but clearly lower than the most polluted areas of south-eastern Asia. Of all pollutants observed at the site, ozone is the most likely to have adverse environmental effects, as the concentrations were high also during the growing season. The measurements presented here will help to close existing gaps in the ground-based global atmosphere observation system, since very little long-term data of this nature is available for southern Africa.

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, 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%.

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.

2015, Sundström, A.-M., Nikandrova, A., Atlaskina, K., Nieminen, 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.

Proxies for estimating nucleation mode number concentrations and further simplification for their use with satellite data have been presented in Kulmala et al. (2011). In this paper we discuss the underlying assumptions for these simplifications and evaluate the resulting proxies over an area in South Africa based on a comparison with a suite of ground-based measurements available from four different stations. The proxies are formulated in terms of sources (concentrations of precursor gases (NO2 and SO2) and UVB radiation intensity near the surface) and a sink term related to removal of the precursor gases due to condensation on pre-existing aerosols. A-Train satellite data are used as input to compute proxies. Both the input data and the resulting proxies are compared with those obtained from ground-based measurements. In particular, a detailed study is presented on the substitution of the local condensation sink (CS) with satellite aerosol optical depth (AOD), which is a column-integrated parameter. One of the main factors affecting the disagreement between CS and AOD is the presence of elevated aerosol layers. Overall, the correlation between proxies calculated from the in situ data and observed nucleation mode particle number concentrations (Nnuc) remained low. At the time of the satellite overpass (13:00–14:00 LT) the highest correlation is observed for SO2/CS (R2 = 0.2). However, when the proxies are calculated using satellite data, only NO2/AOD showed some correlation with Nnuc (R2 = 0.2). This can be explained by the relatively high uncertainties related especially to the satellite SO2 columns and by the positive correlation that is observed between the ground-based SO2 and NO2 concentrations. In fact, results show that the satellite NO2 columns compare better with in situ SO2 concentration than the satellite SO2 column. Despite the high uncertainties related to the proxies calculated using satellite data, the proxies calculated from the in situ data did not better predict Nnuc. Hence, overall improvements in the formulation of the proxies are needed.

2012, Komppula, M., Mielonen, T., Arola, A., Korhonen, K., Lihavainen, H., Hyvärinen, A.-P., Baars, H., Engelmann, R., Althausen, D., Ansmann, A., Müller, D., Panwar, T.S., Hooda, R.K., Sharma, V.P., Kerminen, V.-M., Lehtinen, K.E.J., Viisanen, Y.

One year of multi-wavelength (3 backscatter + 2 extinction + 1 depolarization) Raman lidar measurements at Gual Pahari, close to New Delhi, were analysed. The data was split into four seasons: spring (March–May), summer (June–August), autumn (September–November) and winter (December–February). The vertical profiles of backscatter, extinction, and lidar ratio and their variability during each season are presented. The measurements revealed that, on average, the aerosol layer was at its highest in spring (5.5 km). In summer, the vertically averaged (between 1–3 km) backscatter and extinction coefficients had the highest averages (3.3 Mm−1 sr−1 and 142 Mm−1 at 532 nm, respectively). Aerosol concentrations were slightly higher in summer compared to other seasons, and particles were larger in size. The autumn showed the highest lidar ratio and high extinction-related Ångström exponents (AEext), indicating the presence of smaller probably absorbing particles. The winter had the lowest backscatter and extinction coefficients, but AEext was the highest, suggesting still a large amount of small particles.

2011, Kulmala, M., Asmi, A., Lappalainen, H.K., Carslaw, K.S., Pöschl, U., Baltensperger, U., Hov, Ø., Brenquier, J.-L., Pandis, S.N., Facchini, M.C., Hansson, H.-C., Wiedensohler, A., O'Dowd, C.D., Boers, R., Boucher, O., de Leeuw, G., Denier van der Gon, H.A.C., Feichter, J., Krejci, R., Laj, P., Lihavainen, H., Lohmann, U., McFiggans, G., Mentel, T., Pilinis, C., Riipinen, I., Schulz, M., Stohl, A., Swietlicki, E., Vignati, E., Alves, C., Amann, M., Ammann, M., Arabas, S., Artaxo, P., Baars, H., Beddows, D.C.S., Bergström, R., Beukes, J.P., Bilde, M., Burkhart, J.F., Canonaco, F., Clegg, S.L., Coe, H., Crumeyrolle, S., D'Anna, B., Decesari, S., Gilardoni, S., Fischer, M., Fjaeraa, A.M., Fountoukis, C., George, C., Gomes, L., Halloran, P., Hamburger, T., Harrison, R.M., Herrmann, H., Hoffmann, T., Hoose, C., Hu, M., Hyvärinen, A., Hõrrak, U., Iinuma, Y., Iversen, T., Josipovic, M., Kanakidou, M., Kiendler-Scharr, A., Kirkevåg, A., Kiss, G., Klimont, Z., Kolmonen, P., Komppula, M., Kristjánsson, J.-E., Laakso, L., Laaksonen, A., Labonnote, L., Lanz, V.A., Lehtinen, K.E.J., Rizzo, L.V., Makkonen, R., Manninen, H.E., McMeeking, G., Merikanto, J., Minikin, A., Mirme, S., Morgan, W.T., Nemitz, E., O'Donnell, D., Panwar, T.S., Pawlowska, H., Petzold, A., Pienaar, J.J., Pio, C., Plass-Duelmer, C., Prévôt, A.S.H., Pryor, S., Reddington, C.L., Roberts, G., Rosenfeld, D., Schwarz, J., Seland, Ø., Sellegri, K., Shen, X.J., Shiraiwa, M., Siebert, H., Sierau, B., Simpson, D., Sun, J.Y., Topping, D., Tunved, P., Vaattovaara, P., Vakkari, V., Veefkind, J.P., Visschedijk, A., Vuollekoski, H., Vuolo, R., Wehner, B., Wildt, J., Woodward, S., Worsnop, D.R., van Zadelhoff, G.-J., Zardini, A.A., Zhang, K., van Zyl, P.G., Kerminen, V.-M.

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

2014, Beddows, D.C.S., Dall'Osto, M., Harrison, R.M., Kulmala, M., Asmi, A., Wiedensohler, A., Laj, P., Fjaeraa, A.M., Sellegri, K., Birmili, W., Bukowiecki, N., Weingartner, E., Baltensperger, U., Zdimal, V., Zikova, N., Putaud, J.-P., Marinoni, A., Tunved, P., Hansson, H.-C., Fiebig, M., Kivekäs, N., Swietlicki, E., Lihavainen, H., Asmi, E., Ulevicius, V., Aalto, P.P., Mihalopoulos, N., Kalivitis, N., Kalapov, I., Kiss, G., de Leeuw, G., Henzing, B., O'Dowd, C., Jennings, S.G., Flentje, H., Meinhardt, F., Ries, L., Denier van der Gon, H.A.C., Visschedijk, A.J.H.

Cluster~analysis of particle number size distributions from~background sites across Europe~is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze.~The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected.~These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6–0.9 nm h−1. Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. ~While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.