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- ItemVariations in tropospheric submicron particle size distributions across the European continent 2008-2009(München : European Geopyhsical Union, 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.
- ItemGeneral overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales(München : European Geopyhsical Union, 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.
- ItemNumber size distributions and seasonality of submicron particles in Europe 2008–2009(München : European Geopyhsical Union, 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.
- ItemPrimary versus secondary contributions to particle number concentrations in the European boundary layer(München : European Geopyhsical Union, 2011) Reddington, C.L.; Carslaw, K.S.; Spracklen, D.V.; Frontoso, M.G.; Collins, L.; Merikanto, J.; Minikin, A.; Hamburger, T.; Coe, H.; Kulmala, M.; Aalto, P.; Flentje, H.; Plass-Dülmer, C.; Birmili, W.; Wiedensohler, A.; Wehner, B.; Tuch, T.; Sonntag, A.; O'Dowd, C.D.; Jennings, S.G.; Dupuy, R.; Baltensperger, U.; Weingartner, E.; Hansson, H.-C.; Tunved, P.; Laj, P.; Sellegri, K.; Boulon, J.; Putaud, J.-P.; Gruening, C.; Swietlicki, E.; Roldin, P.; Henzing, J.S.; Moerman, M.; Mihalopoulos, N.; Kouvarakis, G.; Ždímal, V.; Zíková, N.; Marinoni, A.; Bonasoni, P.; Duchi, R.It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
- ItemHygroscopic properties of submicrometer atmospheric aerosol particles measured with H-TDMA instruments in various environments - A review(Milton Park : Taylor & Francis, 2017) Swietlicki, E.; Hansson, H.-C.; Hämeri, K.; Svenningsson, B.; Massling, A.; Mcfiggans, G.; Mcmurry, P.H.; Petäjä, T.; Tunved, P.; Gysel, M.; Topping, D.; Weingartner, E.; Baltensperger, U.; Rissler, J.; Wiedensohler, A.; Kulmala, M.The hygroscopic properties play a vital role for the direct and indirect effects of aerosols on climate, as well as the health effects of particulate matter (PM) by modifying the deposition pattern of inhaled particles in the humid human respiratory tract. Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) instruments have been used in field campaigns in various environments globally over the last 25 yr to determine the water uptake on submicrometre particles at subsaturated conditions. These investigations have yielded valuable and comprehensive information regarding the particle hygroscopic properties of the atmospheric aerosol, including state of mixing. These properties determine the equilibrium particle size at ambient relative humidities and have successfully been used to calculate the activation of particles at water vapour supersaturation. This paper summarizes the existing published H-TDMA results on the sizeresolved submicrometre aerosol particle hygroscopic properties obtained from ground-based measurements at multiple marine, rural, urban and free tropospheric measurement sites. The data is classified into groups of hygroscopic growth indicating the external mixture, and providing clues to the sources and processes controlling the aerosol. An evaluation is given on how different chemical and physical properties affect the hygroscopic growth.