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- ItemAerosol particle formation events and analysis of high growth rates observed above a subarctic wetland-forest mosaic(Milton Park : Taylor & Francis, 2017) Svenningsson, Birgitta; Arneth, Almut; Hayward, Sean; Holst, Thomas; Massling, Andreas; Swietlicki, Erik; Hirsikko, Anne; Junninen, Heikki; Riipinen, Ilona; Vana, Marko; Dal Maso, Miikka; Hussein, Tareq; Kulmala, MarkkuAn analysis of particle formation (PF) events over a subarctic mire in northern Swedenwas performed, based on number– size distributions of atmospheric aerosol particles (10–500 nm in diameter) and ions (0.4–40 nm in Tammet diameter). We present classification statistics for PF events from measurements covering the period July 2005–September 2006, with a break over the winter period. The PF event frequency peaked during the summer months, in contrast to other Scandinavian sites where the frequency is highest during spring and autumn. Our analysis includes calculated growth rates and estimates of concentrations and production rates of condensing vapour, deduced from the growth rates and condensational sink calculations, using AIS and SMPS data. Particle formation events with high growth rates (up to 50 nm h-1) occurred repeatedly. In these cases, the newly formed nucleation mode particles were often only present for periods of a few hours. On several occasions, repeated particle formation events were observed within 1 d, with differences in onset time of a few hours. These high growth rates were only observed when the condensation sink was higher than 0.001 s-1.
- 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.
- ItemNew particle formation in the Svalbard region 2006-2015(Katlenburg-Lindau : EGU, 2017) Heintzenberg, Jost; Tunved, Peter; GalÃ, MartÃ; Leck, CarolineEvents of new particle formation (NPF) were analyzed in a 10-year data set of hourly particle size distributions recorded on Mt. Zeppelin, Spitsbergen, Svalbard. Three different types of NPF events were identified through objective search algorithms. The first and simplest algorithm utilizes short-term increases in particle concentrations below 25 nm (PCT (percentiles) events). The second one builds on the growth of the sub-50 nm diameter median (DGR (diameter growth) events) and is most closely related to the classical "banana type" of event. The third and most complex, multiple-size approach to identifying NPF events builds on a hypothesis suggesting the concurrent production of polymer gel particles at several sizes below ca. 60 nm (MEV (multisize growth) events). As a first and general conclusion, we can state that NPF events are a summer phenomenon and not related to Arctic haze, which is a late winter to early spring feature. The occurrence of NPF events appears to be somewhat sensitive to the available data on precipitation. The seasonal distribution of solar flux suggests some photochemical control that may affect marine biological processes generating particle precursors and/or atmospheric photochemical processes that generate condensable vapors from precursor gases. Notably, the seasonal distribution of the biogenic methanesulfonate (MSA) follows that of the solar flux although it peaks before the maxima in NPF occurrence. A host of ancillary data and findings point to varying and rather complex marine biological source processes. The potential source regions for all types of new particle formation appear to be restricted to the marginal-ice and open-water areas between northeastern Greenland and eastern Svalbard. Depending on conditions, yet to be clarified new particle formation may become visible as short bursts of particles around 20 nm (PCT events), longer events involving condensation growth (DGR events), or extended events with elevated concentrations of particles at several sizes below 100 nm (MEV events). The seasonal distribution of NPF events peaks later than that of MSA and DGR, and in particular than that of MEV events, which reach into late summer and early fall with open, warm, and biologically active waters around Svalbard. Consequently, a simple model to describe the seasonal distribution of the total number of NPF events can be based on solar flux and sea surface temperature, representing environmental conditions for marine biological activity and condensation sink, controlling the balance between new particle nucleation and their condensational growth. Based on the sparse knowledge about the seasonal cycle of gel-forming marine microorganisms and their controlling factors, we hypothesize that the seasonal distribution of DGR and, more so, MEV events reflect the seasonal cycle of the gel-forming phytoplankton.
- ItemOn the abundance and source contributions of dicarboxylic acids in size-resolved aerosol particles at continental sites in central Europe(München : European Geopyhsical Union, 2014) van Pinxteren, D.; Neusüß, C.; Herrmann, H.Dicarboxylic acids (DCAs) are among the most abundant organic compounds observed in atmospheric aerosol particles and have been extensively studied at many places around the world. The importance of the various primary sources and secondary formation pathways discussed in the literature is often difficult to assess from field studies, though. In the present study, a large data set of size-resolved DCA concentrations from several inland sites in Germany is combined with results from a recently developed approach of statistical back-trajectory analysis and additional data. Principal component analysis is then used to reveal the most important factors governing the abundance of DCAs in different particle size ranges. The two most important sources revealed are (i) photochemical formation during intense radiation days in polluted air masses, likely occurring in the gas phase on short timescales (gasSOA), and (ii) secondary reactions in anthropogenically influenced air masses, likely occurring in the aqueous phase on longer timescales (aqSOA). While the first source strongly impacts DCA concentrations mainly in small and large particles, the second one enhances accumulation mode DCAs and is responsible for the bulk of the observed concentrations. Primary sources were found to be minor (sea salt, soil resuspension) or non-existent (biomass burning, traffic). The results can be regarded as representative for typical central European continental conditions.
- ItemVariability of air ion concentrations in urban Paris(München : European Geopyhsical Union, 2015) Dos Santos, V.N.; Herrmann, E.; Manninen, H.E.; Hussein, T.; Hakala, J.; Nieminen, T.; Aalto, P.P.; Merkel, M.; Wiedensohler, A.; Kulmala, M.; Petäjä, T.; Hämeri, K.Air ion concentrations influence new particle formation and consequently the global aerosol as potential cloud condensation nuclei. We aimed to evaluate air ion concentrations and characteristics of new particle formation events (NPF) in the megacity of Paris, France, within the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric Pollution and climate effects, and Integrated tools for assessment and mitigation) project. We measured air ion number size distributions (0.8–42 nm) with an air ion spectrometer and fine particle number concentrations (> 6 nm) with a twin differential mobility particle sizer in an urban site of Paris between 26 June 2009 and 4 October 2010. Air ions were size classified as small (0.8–2 nm), intermediate (2–7 nm), and large (7–20 nm). The median concentrations of small and large ions were 670 and 680 cm−3, respectively, (sum of positive and negative polarities), whereas the median concentration of intermediate ions was only 20 cm−3, as these ions were mostly present during new particle formation bursts, i.e. when gas-to-particle conversion produced fresh aerosol particles from gas phase precursors. During peaks in traffic-related particle number, the concentrations of small and intermediate ions decreased, whereas the concentrations of large ions increased. Seasonal variations affected the ion population differently, with respect to their size and polarity. NPF was observed in 13 % of the days, being most frequent in spring and late summer (April, May, July, and August). The results also suggest that NPF was favoured on the weekends in comparison to workdays, likely due to the lower levels of condensation sinks in the mornings of weekends (CS weekdays 09:00: 18 × 10−3 s−1; CS weekend 09:00: 8 × 10−3 s−1). The median growth rates (GR) of ions during the NPF events varied between 3 and 7 nm h−1, increasing with the ion size and being higher on workdays than on weekends for intermediate and large ions. The median GR of small ions on the other hand were rather similar on workdays and weekends. In general, NPF bursts changed the diurnal cycle of particle number as well as intermediate and large ions by causing an extra peak between 09:00 and 14:00. On average, during the NPF bursts the concentrations of intermediate ions were 8.5–10 times higher than on NPF non-event days, depending on the polarity, and the concentrations of large ions and particles were 1.5–1.8 and 1.2 times higher, respectively. Because the median concentrations of intermediate ions were considerably higher on NPF event days in comparison to NPF non-event days, the results indicate that intermediate ion concentrations could be used as an indication for NPF in Paris. The results suggest that NPF was a source of ions and aerosol particles in Paris and therefore contributed to both air quality degradation and climatic effects, especially in the spring and summer.
- ItemA European aerosol phenomenology - 6: Scattering properties of atmospheric aerosol particles from 28 ACTRIS sites(Katlenburg-Lindau : EGU, 2018) Pandolfi, Marco; Alados-Arboledas, Lucas; Alastuey, Andrés; Andrade, Marcos; Angelov, Christo; Artiñano, Begoña; Backman, John; Baltensperger, Urs; Bonasoni, Paolo; Bukowiecki, Nicolas; Collaud Coen, Martine; Conil, Sébastien; Coz, Esther; Crenn, Vincent; Dudoitis, Vadimas; Ealo, Marina; Eleftheriadis, Kostas; Favez, Olivier; Fetfatzis, Prodromos; Fiebig, Markus; Flentje, Harald; Ginot, Patrick; Gysel, Martin; Henzing, Bas; Hoffer, Andras; Holubova Smejkalova, Adela; Kalapov, Ivo; Kalivitis, Nikos; Kouvarakis, Giorgos; Kristensson, Adam; Kulmala, Markku; Lihavainen, Heikki; Lunder, Chris; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mihalopoulos, Nikos; Moerman, Marcel; Nicolas, José; O'Dowd, Colin; Petäjä, Tuukka; Petit, Jean-Eudes; Pichon, Jean Marc; Prokopciuk, Nina; Putaud, Jean-Philippe; RodrÃguez, Sergio; Sciare, Jean; Sellegri, Karine; Swietlicki, Erik; Titos, Gloria; Tuch, Thomas; Tunved, Peter; Ulevicius, Vidmantas; Vaishya, Aditya; Vana, Milan; Virkkula, Aki; Vratolis, Stergios; Weingartner, Ernest; Wiedensohler, Alfred; Laj, PaoloThis paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (σsp) and hemispheric backscattering (σbsp) coefficients, scattering Ã…ngström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of σsp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, σsp also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intraannual variability. At mountain sites, higher σsp and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher σsp values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low σsp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high σsp values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of σsp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of σsp are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.
- ItemSimulating ultrafine particle formation in Europe using a regional CTM: Contribution of primary emissions versus secondary formation to aerosol number concentrations(München : European Geopyhsical Union, 2012) Fountoukis, C.; Riipinen, I.; Denier van der Gon, H.A.C.; Charalampidis, P.E.; Pilinis, C.; Wiedensohler, A.; O'Dowd, C.; Putaud, J.P.; Moerman, M.; Pandis, S.N.A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.
- ItemChanges in the production rate of secondary aerosol particles in Central Europe in view of decreasing SO2 emissions between 1996 and 2006(München : European Geopyhsical Union, 2010) Hamed, A.; Birmili, W.; Joutsensaari, J.; Mikkonen, S.; Asmi, A.; Wehner, B.; Spindler, G.; Jaatinen, A.; Wiedensohler, A.; Korhonen, H.; Lehtinen, K.E.J.; Laaksonen, A.In anthropogenically influenced atmospheres, sulphur dioxide (SO2) is the main precursor of gaseous sulphuric acid (H2SO4), which in turn is a main precursor for atmospheric particle nucleation. As a result of socio-economic changes, East Germany has seen a dramatic decrease in anthropogenic SO2 emissions between 1989 and present, as documented by routine air quality measurements in many locations. We have attempted to evaluate the influence of changing SO2 concentrations on the frequency and intensity of new particle formation (NPF) using two different data sets (1996–1997; 2003–2006) of experimental particle number size distributions (diameter range 3–750 nm) from the atmospheric research station Melpitz near Leipzig, Germany. Between the two periods SO2 concentrations decreased by 65% on average, while the frequency of NPF events dropped by 45%. Meanwhile, the average formation rate of 3 nm particles decreased by 68% on average. The trends were statistically significant and therefore suggest a connection between the availability of anthropogenic SO2 and freshly formed new particles. In contrast to the decrease in new particle formation, we found an increase in the mean growth rate of freshly nucleated particles (+22%), suggesting that particle nucleation and subsequent growth into larger sizes are delineated with respect to their precursor species. Using three basic parameters, the condensation sink for H2SO4, the SO2 concentration, and the global radiation intensity, we were able to define the characteristic range of atmospheric conditions under which particle formation events take place at the Melpitz site. While the decrease in the concentrations and formation rates of the new particles was rather evident, no similar decrease was found with respect to the generation of cloud condensation nuclei (CCN; particle diameter >100 nm) as a result of atmospheric nucleation events. On the contrary, the production of CCN following nucleation events appears to have increased by tens of percents. Our aerosol dynamics model simulations suggest that such an increase can be caused by the increased particle growth rate.
- ItemResults from the CERN pilot CLOUD experiment(München : European Geopyhsical Union, 2010) Duplissy, J.; Enghoff, M.B.; Aplin, K.L.; Arnold, F.; Aufmhoff, H.; Avngaard, M.; Baltensperger, U.; Bondo, T.; Bingham, R.; Carslaw, K.; Curtius, J.; David, A.; Fastrup, B.; Gagné, S.; Hahn, F.; Harrison, R.G.; Kellett, B.; Kirkby, J.; Kulmala, M.; Laakso, L.; Laaksonen, A.; Lillestol, E.; Lockwood, M.; Mäkelä, J.; Makhmutov, V.; Marsh, N.D.; Nieminen, T.; Onnela, A.; Pedersen, E.; Pedersen, J.O.P.; Polny, J.; Reichl, U.; Seinfeld, J.H.; Sipilä, M.; Stozhkov, Y.; Stratmann, F.; Svensmark, H.; Svensmark, J.; Veenhof, R.; Verheggen, B.; Viisanen, Y.; Wagner, P.E.; Wehrle, G.; Weingartner, E.; Wex, H.; Wilhelmsson, M.; Winkler, P.M.During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally-measured formation rates and \htwosofour concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C
- ItemStatus and future of numerical atmospheric aerosol prediction with a focus on data requirements(Katlenburg-Lindau : EGU, 2018) Benedetti, Angela; Reid, Jeffrey S.; Knippertz, Peter; Marsham, John H.; Di Giuseppe, Francesca; Rémy, Samuel; Basart, Sara; Boucher, Olivier; Brooks, Ian M.; Menut, Laurent; Mona, Lucia; Laj, Paolo; Pappalardo, Gelsomina; Wiedensohler, Alfred; Baklanov, Alexander; Brooks, Malcolm; Colarco, Peter R.; Cuevas, Emilio; da Silva, Arlindo; Escribano, Jeronimo; Flemming, Johannes; Huneeus, Nicolas; Jorba, Oriol; Kazadzis, Stelios; Kinne, Stefan; Popp, Thomas; Quinn, Patricia K.; Sekiyama, Thomas T.; Tanaka, Taichu; Terradellas, EnricNumerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation and military authorities, solar energy plant managers, climate services providers, and health professionals. Owing to the complexity of atmospheric aerosol processes and their sensitivity to the underlying meteorological conditions, the prediction of aerosol particle concentrations and properties in the numerical weather prediction (NWP) framework faces a number of challenges. The modeling of numerous aerosol-related parameters increases computational expense. Errors in aerosol prediction concern all processes involved in the aerosol life cycle including (a) errors on the source terms (for both anthropogenic and natural emissions), (b) errors directly dependent on the meteorology (e.g., mixing, transport, scavenging by precipitation), and (c) errors related to aerosol chemistry (e.g., nucleation, gas-aerosol partitioning, chemical transformation and growth, hygroscopicity). Finally, there are fundamental uncertainties and significant processing overhead in the diverse observations used for verification and assimilation within these systems. Indeed, a significant component of aerosol forecast development consists in streamlining aerosol-related observations and reducing the most important errors through model development and data assimilation. Aerosol particle observations from satellite- and ground-based platforms have been crucial to guide model development of the recent years and have been made more readily available for model evaluation and assimilation. However, for the sustainability of the aerosol particle prediction activities around the globe, it is crucial that quality aerosol observations continue to be made available from different platforms (space, near surface, and aircraft) and freely shared. This paper reviews current requirements for aerosol observations in the context of the operational activities carried out at various global and regional centers. While some of the requirements are equally applicable to aerosol-climate, the focus here is on global operational prediction of aerosol properties such as mass concentrations and optical parameters. It is also recognized that the term "requirements" is loosely used here given the diversity in global aerosol observing systems and that utilized data are typically not from operational sources. Most operational models are based on bulk schemes that do not predict the size distribution of the aerosol particles. Others are based on a mix of "bin" and bulk schemes with limited capability of simulating the size information. However the next generation of aerosol operational models will output both mass and number density concentration to provide a more complete description of the aerosol population. A brief overview of the state of the art is provided with an introduction on the importance of aerosol prediction activities. The criteria on which the requirements for aerosol observations are based are also outlined. Assimilation and evaluation aspects are discussed from the perspective of the user requirements.