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	<journal>
		<journal_title>Atmospheric Chemistry and Physics</journal_title>
		<journal_url>www.atmos-chem-phys.net</journal_url>
		<issn>1680-7316</issn>
		<eissn>1680-7324</eissn>
		<volume_number>9</volume_number>
		<issue_number>9</issue_number>
		<publication_year>2009</publication_year>
	</journal>
	<doi>10.5194/acp-9-2933-2009</doi>
	<article_url>http://www.atmos-chem-phys.net/9/2933/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/9/2933/2009/acp-9-2933-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/9/2933/2009/acp-9-2933-2009.pdf</fulltext_pdf>
	<start_page>2933</start_page>
	<end_page>2947</end_page>
	<publication_date>2009-05-06</publication_date>
	<article_title content_type="html">Aerosol dynamics simulations on the connection of sulphuric acid and new particle formation</article_title>
	<authors>
		<author numeration="1" affiliations="1">
			<name>S.-L. Sihto</name>
			<email>sanna-liisa.sihto@helsinki.fi</email>
		</author>
		<author numeration="2" affiliations="1">
			<name>H. Vuollekoski</name>
		</author>
		<author numeration="3" affiliations="2">
			<name>J. Leppä</name>
		</author>
		<author numeration="4" affiliations="1">
			<name>I. Riipinen</name>
		</author>
		<author numeration="5" affiliations="2">
			<name>V.-M. Kerminen</name>
		</author>
		<author numeration="6" affiliations="3">
			<name>H. Korhonen</name>
		</author>
		<author numeration="7" affiliations="3,4">
			<name>K. E. J. Lehtinen</name>
		</author>
		<author numeration="8" affiliations="1">
			<name>M. Boy</name>
		</author>
		<author numeration="9" affiliations="1">
			<name>M. Kulmala</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">University of Helsinki, Department of Physics, P.O. Box 64, 00014 University of Helsinki, Finland</affiliation>
		<affiliation numeration="2" content_type="html">Finnish Meteorological Institute, Climate and Global Change, P.O. Box 503, 00101 Helsinki, Finland</affiliation>
		<affiliation numeration="3" content_type="html">University of Kuopio, Department of Physics, P.O. Box 1627, 70211 Kuopio, Finland</affiliation>
		<affiliation numeration="4" content_type="html">Finnish Meteorological Institute, Kuopio Unit, P.O. Box 1627, 70211 Kuopio, Finland</affiliation>
	</affiliations>
	<abstract content_type="html">We have performed a series of simulations with an aerosol dynamics box model to
study the connection between new particle formation and sulphuric acid
concentration. For nucleation either activation mechanism with a linear
dependence on the sulphuric acid concentration, kinetic mechanism with a squared
dependence on the sulphuric acid concentration or ternary
H&lt;sub&gt;2&lt;/sub&gt;O-H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-NH&lt;sub&gt;3&lt;/sub&gt; nucleation was assumed. The aim was to study
the factors that affect the sulphuric acid dependence during the early
stages of particle growth, and specifically to find conditions which would yield
the linear dependence between the particle number concentration at 3–6 nm
and sulphuric acid, as observed in field experiments. The simulations showed
that the correlation with sulphuric acid may change during the growth from
nucleation size to 3–6 nm size range, the main reason being the size
dependent growth rate between 1 and 3 nm. In addition, the assumed size for
the nucleated clusters had a crucial impact on the sulphuric acid dependence
at 3 nm. A linear dependence between the particle
number concentration at 3 nm and sulphuric acid was achieved, when activation
nucleation mechanism was used with a low saturation vapour pressure for the
condensable organic vapour, or with nucleation taking place at ~2 nm
instead of ~1 nm. Simulations with activation, kinetic and ternary nucleation showed that ternary
nucleation reproduces too steep dependence on sulphuric acid as compared to
the linear or square dependence observed in field measurements.</abstract>
	<references>
		<reference numeration="1" content_type="text">Anttila, T., Kerminen, V.-M., Kulmala, M., Laaksonen, A., and O&apos;Dowd, C.: Modelling the formation of organic particles in the atmosphere, Atmos. Chem. Phys., 4, 1071–1083, 2004. </reference>
		<reference numeration="2" content_type="text">Baker, M. B. and Peter, T.: Small-scale cloud processes and climate, Nature, 451, 299–300, 2008. </reference>
		<reference numeration="3" content_type="text">Boy, M., Kulmala, M., Ruuskanen, T. M., Pihlatie, M., Reissell, A., Aalto, P. P., Keronen, P., Dal Maso, M., Hellen, H., Hakola, H., Jansson, R., Hanke, M., and Arnold, F.: Sulphuric acid closure and contribution to nucleation mode particle growth, Atmos. Chem. Phys., 5, 863–878, 2005. </reference>
		<reference numeration="4" content_type="text">Boy, M., Hellmuth, O., Korhonen, H., Nilsson, E. D., ReVelle, D., Turnipseed, A., Arnold, F., and Kulmala, M.: MALTE – model to predict new aerosol formation in the lower troposphere, Atmos. Chem. Phys., 6, 4499–4517, 2006. </reference>
		<reference numeration="5" content_type="text">Fuchs, N. A. and Sutugin, A. G., High dispersed aerosols, in: Topics in Current Aerosol Research (Part 2), edited by: Hidy, G. M. and Brock, J. R., Pergamon, New York, USA, 1–200, 1971. </reference>
		<reference numeration="6" content_type="text">Gaydos, T. M., Stanier, C. O., and Pandis, S. P.: Modeling of in situ ultrafine atmospheric particle formation in the eastern United States, J. Geophys. Res., 110, D07S12, doi:10.1029/2004JD004683, 2005. </reference>
		<reference numeration="7" content_type="text">Hari, P. and Kulmala, M.: Station for Measuring Ecosystem Atmosphere Relations (SMEAR II), Boreal Env. Res., 10, 315–322, 2005. </reference>
		<reference numeration="8" content_type="text">Heaton, K. J., Dreyffus, M. A., Wang, S., and Johnston, M. V.: Oligomers in the early stage of biogenic secondary organic aerosol formation and growth, Environ. Sci. Technol., 41, 6129–6136, 2007. </reference>
		<reference numeration="9" content_type="text">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 Env. Res., 10, 357–369, 2005. </reference>
		<reference numeration="10" content_type="text">IPCC (Intergovernmental Panel on Climate Change) Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the IPCC, http://www.ipcc.ch/ipccreports/ar4-wg1.htm, 2007. </reference>
		<reference numeration="11" content_type="text">Jung, J. G., Pandis, S. N., and Adams, P. J.: Evaluation of Nucleation Theories in a Sulfur-Rich Environment, Aerosol Sci. Tech., 42, 495–504, doi:10.1080/02786820802187085, 2008. </reference>
		<reference numeration="12" content_type="text">Kerminen, V.-M., Lehtinen, K. E. J., Anttila, T., and Kulmala, M.: Dynamics of atmospheric nucleation mode particles: a time scale analysis, Tellus, 56B, 135–146, 2004. </reference>
		<reference numeration="13" content_type="text">Kerminen, V.-M., Lihavainen, H., Komppula, M., Viisanen, Y., and Kulmala, M.: Direct observational evidence linking atmospheric aerosol formation and cloud droplet activation, Geophys. Res. Lett., 32, L14803, doi:10.1029/2005GL023130, 2005. </reference>
		<reference numeration="14" content_type="text">Komppula, M., Sihto, S.-L., Korhonen, H., Lihavainen, H., Kerminen, V.-M., Kulmala, M., and Viisanen, Y.: New particle formation in air mass transported between two measurement sites in Northern Finland, Atmos. Chem. Phys., 6, 2811–2824, 2006. </reference>
		<reference numeration="15" content_type="text">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. </reference>
		<reference numeration="16" content_type="text">Korhonen, H., Kerminen, V.-M., Lehtinen, K. E. J., and Kulmala, M.: CCN activation and cloud processing in sectional aerosol models with low size resolution, Atmos. Chem. Phys., 5, 2561–2570, 2005. </reference>
		<reference numeration="17" content_type="text">Kuang, C., McMurry, P. H., McCormick, A. V., and Eisele, F.: Dependence of nucleation rates on sulfuric acid vapor concentration in diverse atmospheric locations, J. Geophys. Res., 113, D10209, doi:10.1029/2007JD009253, 2008. </reference>
		<reference numeration="18" content_type="text">Kulmala, M., Kerminen, V.-M., and Laaksonen, A.: Simulations on the effect of sulphuric acid formation on atmospheric aerosol concentrations, Atmos. Environ., 29, 377–382, 1995. </reference>
		<reference numeration="19" content_type="text">Kulmala, M., Toivonen, A., Mäkelä, J., and Laaksonen, A.: Analysis of the growth of nucleation mode particles observed in Boreal forest, Tellus, 50B, 449–462, 1998. </reference>
		<reference numeration="20" content_type="text">Kulmala, M., Vehkamäki, H., Petäjä, T., Dal Maso, M., Lauri, A., Kerminen, V.-M., Birmili, W., and McMurry, P. H.: Formation and growth rates of ultrafine atmospheric particles: A review of observations, J. Aerosol Sci., 35, 143–176, 2004a. </reference>
		<reference numeration="21" content_type="text">Kulmala, M., Suni, T., Lehtinen, K. E. J., Dal Maso, M., Boy, M., Reissell, A., Rannik, Ü., Aalto, P., Keronen, P., Hakola, H., Bäck, J., Hoffmann, T., Vesala, T., and Hari, P.: A new feedback mechanism linking forests, aerosols, and climate, Atmos. Chem. Phys., 4, 557–562, 2004b. </reference>
		<reference numeration="22" content_type="text">Kulmala, M., Kerminen, V.-M., Anttila, T., Laaksonen, A., and O&apos;Dowd, C. D.: Organic aerosol formation via sulphate cluster activation, J. Geophys. Res., 109, D04205, doi:10.1029/2003JD003961, 2004c. </reference>
		<reference numeration="23" content_type="text">Kulmala, M., Lehtinen, K. E. J., and Laaksonen, A.: Cluster activation theory as an explanation of the linear dependence of the formation rate of 3 nm particles and sulphuric acid concentrations, Atmos. Chem. Phys., 6, 787–793, 2006. </reference>
		<reference numeration="24" content_type="text">Kulmala, M., Riipinen, I., Sipilä, M., Manninen, H. E., Petäjä, T., Junninen, H., Dal Maso, M., Mordas, G., Mirme, A., Vana, M., Hirsikko, A., Laakso, L., Harrison, R. M., Hanson, I., Leung, C., Lehtinen, K. E. J., and Kerminen, V.-M.: Toward Direct Measurement of Atmospheric Nucleation, Science, 318, 89–92, 2007. </reference>
		<reference numeration="25" content_type="text">Kulmala, M. and Kerminen, V.-M.: On the formation and growth of atmospheric nanoparticles, Atmos. Res., 90, 132–150, 2008. </reference>
		<reference numeration="26" content_type="text">Laakso, L., Anttila, T., Lehtinen, K. E. J., Aalto, P. P., Kulmala, M., Hõrrak, U., Paatero, J., Hanke, M., and Arnold, F.: Kinetic nucleation and ions in boreal forest particle formation events, Atmos. Chem. Phys., 4, 2353–2366, 2004. </reference>
		<reference numeration="27" content_type="text">Laaksonen, A., Hamed, A., Joutsensaari, J., Hiltunen, L, Cavalli, F., Junkermann, W., Asmi, A., Fuzzi, S., and Facchini, M. C.: Cloud condensation nucleus production from nucleation events at a highly polluted region, Geophys. Res. Lett., 32, L06812, doi:10.1029/2004GL022092, 2005. </reference>
		<reference numeration="28" content_type="text">Lehtinen, K. E. J. and Kulmala, M.: A model for particle formation and growth in the atmosphere with molecular resolution in size, Atmos. Chem. Phys., 3, 251–257, 2003. </reference>
		<reference numeration="29" content_type="text">Limbeck, A., Kulmala, M., and Puxbaum, H.: Secondary organic aerosol formation in the atmosphere via heterogenous reaction of gaseous isoprene on acidic particles, Geophys. Res. Lett., 30, 1996, doi:10.1029/2003GL017738, 2003. </reference>
		<reference numeration="30" content_type="text">McMurry, P. and Friedlander, S. K.: New particle formation in the presence of an aerosol, Atmos. Environ., 13, 1635–1651, 1979. </reference>
		<reference numeration="31" content_type="text">McMurry, P. H.: New partcle formation in the presence of an aerosol: Rates, time scales and sub-0.01 um size distributions, J. Colloid Interface Sci., 95, 72–80, 1983. </reference>
		<reference numeration="32" content_type="text">McMurry, P. H., Fink, M. A., Sakurai, H., Stolzenburg, M. R., Mauldin, L., Moore, K., Smith, J. N., Eisele, F. L., Sjostedt, S., Tanner, D., Huey, L. G., Nowak, J. B., Edgerton, E., and Voisin, D.: A criterion for new particle formation in the sulfur-rich Atlanta atmosphere, J. Geophys. Res., 110, D22S02, doi:10.1029/2005JD005901, 2005. </reference>
		<reference numeration="33" content_type="text">Napari, I., Noppel, M., Vehkamäki, H., and Kulmala, M.: An improved model for ternary nucleation of sulfuric acid-ammonia-water, J. Chem. Phys. 116, 4221, 2002a. </reference>
		<reference numeration="34" content_type="text">Napari, I., Noppel, M., Vehkamäki, H., and Kulmala, M.: Parametrization of ternary nucleation rates for H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;–NH&lt;sub&gt;3&lt;/sub&gt;–H&lt;sub&gt;2&lt;/sub&gt;O vapors, J. Geophys. Res., 107(D19), 4381, doi:10.1029/2002JD002132, 2002b. </reference>
		<reference numeration="35" content_type="text">Napari, I., Makkonen, R., Kulmala, M., and Vehkamäki, H.: Parameterization of ammonia and water content of atmospheric droplets with fixed number of sulfuric acid molecules, Atmos. Res., 82, 514–522, 2006. </reference>
		<reference numeration="36" content_type="text">Penner, J. E., Quaas, J., Storelvmo, T., Takemura, T., Boucher, O., Guo, H., Kirkev&amp;aring;g, A., Kristjansson, J. E., and Seland, Ø: Model intercomparison of indirect aerosol effects, Atmos. Chem. Phys., 6, 3391–3405, 2006. </reference>
		<reference numeration="37" content_type="text">Rannik, Ü., Aalto, P., Keronen, P., Vesala, T., and Kulmala, M.: Interpretation of aerosol particle fluxes over a pine forest: Dry deposition and random errors, J. Geophys. Res., 108(D17), 4544, doi:10.1029/2003JD003542, 2003. </reference>
		<reference numeration="38" content_type="text">Riipinen, I., Sihto, S.-L., Kulmala, M., Arnold, F., Dal Maso, M., Birmili, W., Saarnio, K., Teinilä, K., Kerminen, V. M., Laaksonen, A., and Lehtinen, K. E. J.: Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä, Atmos. Chem. Phys., 7, 1899–1914, 2007. </reference>
		<reference numeration="39" content_type="text">Rosenfeld, D.: Aerosol, clouds, and climate, Science, 312, 1323–1324, 2006. </reference>
		<reference numeration="40" content_type="text">Sihto, S.-L., Kulmala, M., Kerminen, V.-M., Dal Maso, M., Petäjä, T., Riipinen, I., Korhonen, H., Arnold, F., Janson, R., Boy, M., Laaksonen, A., and Lehtinen, K. E. J.: Atmospheric sulphuric acid and aerosol formation: Implications from atmospheric measurements for nucleation and early growth mechanisms, Atmos. Chem. Phys., 6, 4079–4091, 2006. </reference>
		<reference numeration="41" content_type="text">Spracklen, D. V., Carslaw, K. S., Kulmala, M., Kerminen, V.-M., Mann, G. W., and Sihto, S.-L.: The contribution of boundary layer nucleation events to total particle concentrations on regional and global scales, Atmos. Chem. Phys., 6, 5631–5648, 2006. </reference>
		<reference numeration="42" content_type="text">Spracklen, D. V., Carslaw, K. S., Kulmala, M., Kerminen, V.-M., Sihto, S.-L., Riipinen, I., Merikanto, J., Mann, G. W., Chipperfield, M. P., Wiedensohler, A., Birmili, W., and Lihavainen, H.: Contribution of particle formation to global cloud condensation nuclei concentrations, Geophys. Res. Lett., 35, L06808, doi:10.1029/2007GL033038, 2008. </reference>
		<reference numeration="43" content_type="text">Tunved, P., Hansson, H.-C., Kerminen, V.-M., Ström, J., Dal Maso, M., Lihavainen, H., Viisanen, Y., Aalto, P. P., Komppula, M., and Kulmala, M.: High natural aerosol loading over boreal forests, Science, 312, 261–263, 2006. </reference>
		<reference numeration="44" content_type="text">Vehkamäki, H., Kulmala, M., Napari, I., Lehtinen, K. E. J., Timmreck, C., Noppel, M., and Laaksonen, A.: An improved parameterization for sulfuric acid-water nucleation rates for tropospheric and stratospheric conditions, J. Geophys. Res., 107, 4622, 2002. </reference>
		<reference numeration="45" content_type="text">Weber, R. J., Marti, J. J., McMurry, P. H., Eisele, F. L., Tanner, D. J., and Jefferson, A.: Measured atmospheric new particle formation rates: implications for nucleation mechanisms, Chem. Eng. Comm., 151, 53–64, 1996. </reference>
		<reference numeration="46" content_type="text">Weber, R. J., Marti, J. J., McMurry, P. H., Eisele, F. L., Tanner, D. J., and Jefferson A.: Measurements of new particle formation and ultrafine particle growth rates at a clean continental site, J. Geophys. Res., 102, 4375–4385, 1997. </reference>
		<reference numeration="47" content_type="text">Wehner, B., Petäjä, T., Boy, M., Engler, C., Birmili, W., Tuch, T., Wiedensohler, A., and Kulmala, M.: The contribution of sulfuric acid and non-volatile compounds on the growth of freshly formed atmospheric aerosols, Geophys. Res. Lett., 32, L17810, doi:10.1029/2005GL023827, 2005. </reference>
		<reference numeration="48" content_type="text">Yu, F.: From molecular clusters to nanoparticles: Second-generation ion-mediated nucleation model, Atmos. Chem. Phys., 6, 5193–5211, 2006. </reference>
		<reference numeration="49" content_type="text">Zhang, K. M. and Wexler, A. S: A hypothesis for growth of fresh atmospheric nuclei, J. Geophys. Res., 107(D21), 4577, doi:10.1029/2002JD002180, 2002. </reference>
	</references>
</article>

