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Connections Between Atmospheric Sulphuric Acid and New Particle Formation During Quest Iii–iv Campaigns in Heidelberg and Hyytiälä : Volume 7, Issue 8 (17/04/2007)

By Riipinen, I.

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Book Id: WPLBN0003994753
Format Type: PDF Article :
File Size: Pages 16
Reproduction Date: 2015

Title: Connections Between Atmospheric Sulphuric Acid and New Particle Formation During Quest Iii–iv Campaigns in Heidelberg and Hyytiälä : Volume 7, Issue 8 (17/04/2007)  
Author: Riipinen, I.
Volume: Vol. 7, Issue 8
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection, Copernicus GmbH
Historic
Publication Date:
2007
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: Copernicus Publications

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Arnold, F., Kulmala, M., Birmili, W., J. Lehtine, K. E., Riipinen, I., Saarnio, K.,...Teinilä, K. (2007). Connections Between Atmospheric Sulphuric Acid and New Particle Formation During Quest Iii–iv Campaigns in Heidelberg and Hyytiälä : Volume 7, Issue 8 (17/04/2007). Retrieved from http://www.ebooklibrary.org/


Description
Description: University of Helsinki, Department of Physical Sciences, P.O. Box 64, 00014 University of Helsinki, Finland. This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H2SO4]), and particle concentrations (N3–6) or formation rates at 1 nm and 3 nm (J1 and J3); 2) the time delays between [H2SO4] and N3–6 or J3, and the growth rates for 1–3 nm particles; 3) the empirical nucleation coefficients A and K in relations J1=A[H2SO4] and J1=K[H2SO4]2, respectively; 4) theoretical predictions for J1 and J3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N3–6 or J3 and [H2SO4] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The nucleation coefficients were about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between J3 and [H2SO4] were consistently lower than the corresponding delays between N3–6 and [H2SO4]. The exponents in the J3∝[H2SO4 ]nJ3-connection were consistently higher than or equal to the exponents in the relation N3–6∝[H2SO4 ]nN36. In the J1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J3 values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by

Summary
Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä

Excerpt
Anttila, T., Vehkam�ki, H., Napari, I., and Kulmala, M.: Effect of ammonium bisulphate formation on atmospheric water-sulphuric acid-ammonia nucleation, Bor. Env. Res., 10, 511–523, 2005.; Berndt, T., Böge, O., Stratmann, F., Heintzenberg, J., and Kulmala, M.: Rapid formation of new sulfuric acid particles at near-atmospheric conditions, Science, 307(5710), 698–700, 2005.; Cabada, J. C., Khlystov, A., Wittig, A. E., Pilinis, C., and Pandis, S. N.: Light scattering by fine particles during the Pittsburgh Air Quality Study: Measurements and modelling, J. Geophys. Res., 109, D16S03, doi:10.1029/2003JD004155, 2004.; Dal Maso, M., Kulmala, M., Riipinen, I., Wagner, R., Hussein, T., Aalto, P. P., and Lehtinen, K. E. J.: Formation and growth of fresh atmospheric aerosols: Eight years of aerosol size distribution data from SMEAR II, Hyytiälä, Finland, Boreal Environ. Res., 10, 323–336, 2005.; Donaldson, K., Xy, Li, and MacNee, W.: Ultra-fine (nanometer) particle-mediated lung injury, J. Aerosol. Sci., 29, 553–560, 1998.; Fiedler, V., Dal Maso, M., Boy, M., Aufmhoff, H., Hoffmann, J., Schuch, T., Birmili, W., Hanke, M., Uecker, J., Arnold, F., and Kulmala, M.: The contribution of sulphuric acid to atmospheric particle formation and growth: a comparison between boundary layers in Northern and Central Europe, Atmos. Chem. Phys., 5, 1773–1785, 2005.; Hari, P. and Kulmala, M.: Station for measuring ecosystem-atmosphere relations (SMEAR II), Boreal Environ. Res., 10, 315–322, 2005.; Hanke, M., Uecker, J., Reiner, T., and Arnold, F.: Atmospheric peroxy radicals: ROXMAS, a new mass-spectrometric methodology for speciated measurements of HO2 and Sigma RO2 and first results, Int. J. Mass Spectr., 213(2–3), 91–99, 2002.; Hirsikko, A., Laakso, L., Hõrrak, U., Aalto, P. P., Kerminen, V.-M., and Kulmala, M.: Annual and size dependent variation of growth rates and ion concentrations in boreal forest, Boreal Environ. Res., 10, 357–369, 2005.; Kerminen, V.-M. and Kulmala, M.: Analytical formulae connecting the real and the apparent nucleation rate and the nuclei number concentration for atmospheric nucleation events, J. Aerosol Sci., 33, 609–622, 2002.; Korhonen, H., Lehtinen, K. E. J., and Kulmala, M.: Multicomponent aerosol dynamics model UHMA: model development and validation, Atmos. Chem. Phys., 4, 757–771, 2004.; Korhonen, P., Kulmala, M., Laaksonen, A., Viisanen, Y., McGraw, R., and Seinfeld, J. H.: Ternary nucleation of H2SO4, NH3 and H2O in the atmosphere, J. Geophys. Res., 104, 26 349–26 353, 1999.; Kulmala, M., Pirjola, L., and Mäkelä, J.: Stable sulphate clusters as a source of new atmospheric particles, Nature, 404, 66–69, 2000.; Kulmala, M., Hämeri, K., Aalto, P. P., Mäkelä, J. M., Pirjola, L., Nilsson, E. D., Buzorius, G., Rannik, Ü, Dal Maso, M., Seidl, W., Hoffmann, T., Janson, R., Hansson, H.-C., Viisanen, Y., Laaksonen, A., and O'Dowd, C. D.: Overview of the international project on Biogenic aerosol formation in the boreal forest (BIOFOR), Tellus, 53B, 324–343, 2001a.; Kulmala, M., Dal Maso, M., Mäkelä, J. M., Pirjola, L., Väkevä, M., Aalto, P. P., Miikkulainen, P., Hämeri, K., and O'Dowd, C. D.: On the formation, growth and composition of nucleation mode particles, Tellus, 53B, 479–490, 2001b.; Kulmala, M.: How Particles Nucleate and Grow, Science, 302, 1000–1001, 2003.; Kulmala, M., Vehkamäki, H., Petäjä, T., Dal Maso, M., Lauri, A., Kerminen, V.-M., Birmili, W., McMurry, P. H.: Formation and growth rates of ultrafine atmospheric particles: A review of observations, J. Aerosol Sci., 35, 143–176, 2004a.; Kulmala, M., Laakso, L., Lehtinen, K. E. J., Riipinen, I., Dal Maso, M., Anttila, T., Kerminen, V.-M., Horrak, U., Vana, M., an

 

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