Browsing by Subject "AEROSOL-SIZE DISTRIBUTION"

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  • Hoyle, C. R.; Fuchs, C.; Jaervinen, E.; Saathoff, H.; Dias, A.; El Haddad, I.; Gysel, M.; Coburn, S. C.; Troestl, J.; Bernhammer, A. -K.; Bianchi, F.; Breitenlechner, M.; Corbin, J. C.; Craven, J.; Donahue, N. M.; Duplissy, J.; Ehrhart, S.; Frege, C.; Gordon, H.; Hoeppel, N.; Heinritzi, M.; Kristensen, T. B.; Molteni, U.; Nichman, L.; Pinterich, T.; Prevot, A. S. H.; Simon, M.; Slowik, J. G.; Steiner, G.; Tome, A.; Vogel, A. L.; Volkamer, R.; Wagner, A. C.; Wagner, R.; Wexler, A. S.; Williamson, C.; Winkler, P. M.; Yan, C.; Amorim, A.; Dommen, J.; Curtius, J.; Gallagher, M. W.; Flagan, R. C.; Hansel, A.; Kirkby, J.; Kulmala, M.; Moehler, O.; Stratmann, F.; Worsnop, D. R.; Baltensperger, U. (2016)
    The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and -10 degrees C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion-pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and -10 degrees C, indicating that, in contrast to some previous studies, the oxidation rates of SO2 in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, supercooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 degrees C is correct.
  • Zaidan, Martha A.; Haapasilta, Ville; Relan, Rishi; Paasonen, Pauli; Kerminen, Veli-Matti; Junninen, Heikki; Kulmala, Markku; Foster, Adam S. (2018)
    Atmospheric new-particle formation (NPF) is a very non-linear process that includes atmospheric chemistry of precursors and clustering physics as well as subsequent growth before NPF can be observed. Thanks to ongoing efforts, now there exists a tremendous amount of atmospheric data, obtained through continuous measurements directly from the atmosphere. This fact makes the analysis by human brains difficult but, on the other hand, enables the usage of modern data science techniques. Here, we calculate and explore the mutual information (MI) between observed NPF events (measured at Hyytiala, Finland) and a wide variety of simultaneously monitored ambient variables: trace gas and aerosol particle concentrations, meteorology, radiation and a few derived quantities. The purpose of the investigations is to identify key factors contributing to the NPF. The applied mutual information method finds that the formation events are strongly linked to sulfuric acid concentration and water content, ultraviolet radiation, condensation sink (CS) and temperature. Previously, these quantities have been well-established to be important players in the phenomenon via dedicated field, laboratory and theoretical research. The novelty of this work is to demonstrate that the same results are now obtained by a data analysis method which operates without supervision and without the need of understanding the physics deeply. This suggests that the method is suitable to be implemented widely in the atmospheric field to discover other interesting phenomena and their relevant variables.
  • Nieminen, Tuomo; Kerminen, Veli-Matti; Petäjä, Tuukka; Aalto, Pasi P.; Arshinov, Mikhail; Asmi, Eija; Baltensperger, Urs; Beddows, David C. S.; Beukes, Johan Paul; Collins, Don; Ding, Aijun; Harrison, Roy M.; Henzing, Bas; Hooda, Rakesh; Hu, Min; Horrak, Urmas; Kivekäs, Niku; Komsaare, Kaupo; Krejci, Radovan; Kristensson, Adam; Laakso, Lauri; Laaksonen, Ari; Leaitch, W. Richard; Lihavainen, Heikki; Mihalopoulos, Nikolaos; Nemeth, Zoltan; Nie, Wei; O'Dowd, Colin; Salma, Imre; Sellegri, Karine; Svenningsson, Birgitta; Swietlicki, Erik; Tunved, Peter; Ulevicius, Vidmantas; Vakkari, Ville; Vana, Marko; Wiedensohler, Alfred; Wu, Zhijun; Virtanen, Annele; Kulmala, Markku (2018)
    Atmospheric new particle formation (NPF) is an important phenomenon in terms of global particle number concentrations. Here we investigated the frequency of NPF, formation rates of 10 nm particles, and growth rates in the size range of 10-25 nm using at least 1 year of aerosol number size-distribution observations at 36 different locations around the world. The majority of these measurement sites are in the Northern Hemisphere. We found that the NPF frequency has a strong seasonal variability. At the measurement sites analyzed in this study, NPF occurs most frequently in March-May (on about 30 % of the days) and least frequently in December-February (about 10 % of the days). The median formation rate of 10 nm particles varies by about 3 orders of magnitude (0.01-10 cm(-3) s(-1)) and the growth rate by about an order of magnitude (1-10 nm h(-1)). The smallest values of both formation and growth rates were observed at polar sites and the largest ones in urban environments or anthropogenically influenced rural sites. The correlation between the NPF event frequency and the particle formation and growth rate was at best moderate among the different measurement sites, as well as among the sites belonging to a certain environmental regime. For a better understanding of atmospheric NPF and its regional importance, we would need more observational data from different urban areas in practically all parts of the world, from additional remote and rural locations in North America, Asia, and most of the Southern Hemisphere (especially Australia), from polar areas, and from at least a few locations over the oceans.
  • Qi, Ximeng; Ding, Aijun; Roldin, Pontus; Xu, Zhengning; Zhou, Putian; Sarnela, Nina; Nie, Wei; Huang, Xin; Rusanen, Anton; Ehn, Mikael; Rissanen, Matti P.; Petäjä, Tuukka; Kulmala, Markku; Boy, Michael (2018)
    Highly oxygenated multifunctional compounds (HOMs) play a key role in new particle formation (NPF), but their quantitative roles in different environments of the globe have not been well studied yet. Frequent NPF events were observed at two "flagship" stations under different environmental conditions, i.e. a remote boreal forest site (SMEAR II) in Finland and a suburban site (SORPES) in polluted eastern China. The averaged formation rate of 6 nm particles and the growth rate of 6-30 nm particles were 0.3 cm(-3) s(-1) and 4.5 nm h(-1) at SMEAR II compared to 2.3 cm(-3) s(-1) and 8.7 nm h(-1) at SORPES, respectively. To explore the differences of NPF at the two stations, the HOM concentrations and NPF events at two sites were simulated with the MALTE-BOX model, and their roles in NPF and particle growth in the two distinctly different environments are discussed. The model provides an acceptable agreement between the simulated and measured concentrations of sulfuric acid and HOMs at SMEAR II. The sulfuric acid and HOM organonitrate concentrations are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower at SORPES compared to SMEAR II. The model simulates the NPF events at SMEAR II with a good agreement but underestimates the growth of new particles at SORPES, indicating a dominant role of anthropogenic processes in the polluted environment. HOMs from monoter-pene oxidation dominate the growth of ultrafine particles at SMEAR II while sulfuric acid and HOMs from aromatics oxidation play a more important role in particle growth. This study highlights the distinct roles of sulfuric acid and HOMs in NPF and particle growth in different environmental conditions and suggests the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas like eastern China.
  • Xiao, S.; Wang, M. Y.; Yao, L.; Kulmala, M.; Zhou, B.; Yang, X.; Chen, J. M.; Wang, D. F.; Fu, Q. Y.; Worsnop, D. R.; Wang, L. (2015)