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<article language="en">
	<journal>
		<journal_title>Atmospheric Chemistry and Physics Discussions</journal_title>
		<journal_url>www.atmos-chem-phys-discuss.net</journal_url>
		<issn>1680-7367</issn>
		<eissn>1680-7375</eissn>
		<volume_number>9</volume_number>
		<issue_number>4</issue_number>
		<publication_year>2009</publication_year>
	</journal>
	<doi>10.5194/acpd-9-15083-2009</doi>
	<article_url>http://www.atmos-chem-phys-discuss.net/9/15083/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys-discuss.net/9/15083/2009/acpd-9-15083-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys-discuss.net/9/15083/2009/acpd-9-15083-2009.pdf</fulltext_pdf>
	<start_page>15083</start_page>
	<end_page>15123</end_page>
	<publication_date>2009-07-13</publication_date>
	<article_title content_type="html">Changes in the production rate of secondary aerosol particles in  central Europe in view of decreasing SO&lt;sub&gt;2&lt;/sub&gt; emissions between  1996 and 2006</article_title>
	<authors>
		<author numeration="1" affiliations="1">
			<name>A. Hamed</name>
		</author>
		<author numeration="2" affiliations="2">
			<name>W. Birmili</name>
		</author>
		<author numeration="3" affiliations="1">
			<name>J. Joutsensaari</name>
		</author>
		<author numeration="4" affiliations="1">
			<name>S. Mikkonen</name>
		</author>
		<author numeration="5" affiliations="3">
			<name>A. Asmi</name>
		</author>
		<author numeration="6" affiliations="2">
			<name>B. Wehner</name>
		</author>
		<author numeration="7" affiliations="2">
			<name>G. Spindler</name>
		</author>
		<author numeration="8" affiliations="1">
			<name>A. Jaatinen</name>
		</author>
		<author numeration="9" affiliations="4">
			<name>K. Uhse</name>
		</author>
		<author numeration="10" affiliations="2">
			<name>A. Wiedensohler</name>
		</author>
		<author numeration="11" affiliations="1,5">
			<name>K. E. J. Lehtinen</name>
		</author>
		<author numeration="12" affiliations="1,6">
			<name>A. Laaksonen</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">Department of Physics, University of Kuopio, P.O. Box 1627, 70211 Kuopio, Finland</affiliation>
		<affiliation numeration="2" content_type="html">Leibniz Institute for Tropospheric Research, Permoserstrasse 15, 04318 Leipzig, Germany</affiliation>
		<affiliation numeration="3" content_type="html">Division of Atmospheric Sciences, Department of Physical Sciences, P.O. Box 64, 00014, University of Helsinki, Finland</affiliation>
		<affiliation numeration="4" content_type="html">Federal Environment Agency of Germany (UBA), Paul-Ehrlich-Strasse 29, 63225 Langen Germany</affiliation>
		<affiliation numeration="5" content_type="html">Finnish Meteorological Institute, Kuopio Unit, P.O. Box 1627, 70210 Kuopio, Finland</affiliation>
		<affiliation numeration="6" content_type="html">Finnish Meteorological Institute, P.O. Box 503, 00101 Helsinki, Finland</affiliation>
	</affiliations>
	<abstract content_type="html">In anthropogenically influenced atmospheres, sulphur dioxide
      (SO&lt;sub&gt;2&lt;/sub&gt;) is the main precursor of gaseous sulphuric acid
      (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;), which in turn forms new aerosol particles
      (diameter &amp;lt;10 nm) through nucleation. As a result of
      socio-economic changes, East Germany has seen a dramatic
      decrease in anthropogenic SO&lt;sub&gt;2&lt;/sub&gt; emissions between 1989 and
      present, as documented by routine air quality measurements in
      many locations. Using two different data sets of experimental
      particle number size distributions (3–750 nm) from the
      research station Melpitz (1996–1997 and 2003–2006) we have
      attempted to evaluate the possible influence of changing
      SO&lt;sub&gt;2&lt;/sub&gt; concentrations on the frequency and intensity of new
      particle formation (NPF). Between the two periods SO&lt;sub&gt;2&lt;/sub&gt;
      concentrations decreased on average by 65%, while the
      frequency of NPF events dropped by 45%. In addition, the
      average formation rate of 3 nm particles decreased by
      68%. The trends were statistically significant, therefore
      suggesting a connection between the availability of
      anthropogenic SO&lt;sub&gt;2&lt;/sub&gt; and the production of new particle
      number. A contrasting finding was the 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 H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;, the SO&lt;sub&gt;2&lt;/sub&gt; concentration, and global
      radiation intensity, we could define the characteristic range
      of atmospheric conditions under which particle formation
      events at the Melpitz site take place or not. While the
      connection between anthropogenic SO&lt;sub&gt;2&lt;/sub&gt;, H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; and
      NPF appears very plausible, our analysis yielded no
      significant evidence whether decreasing SO&lt;sub&gt;2&lt;/sub&gt;
      concentrations did affect the production of cloud condensation
      nuclei (CCN).</abstract>
	<references>
		<reference numeration="1" content_type="text"> Alves, C., Pio, C., Carvalho, A., and Santos, C.: Atmospheric carbonaceous aerosols over grasslands of central Europe and a Boreal forest, Chemosphere, 63, 153–164, 2006. </reference>
		<reference numeration="2" content_type="text"> Balkanski, Y. J.: Atmospheric residence times of continental aerosols. Ph.D. thesis, Harvard Univ., Cambridge, MA, USA, 1991. </reference>
		<reference numeration="3" content_type="text"> Beilke, S. and Uhse, K.: Trend in concentration and deposition of sulfuric and nitrogenic compounds in Germany between 1982 and 1998 (translated from German), in: Jahresbericht 1998 aus dem Messnetz des Umweltbundesamtes. UBA-Texte, 66/99, Federal Environment Agency (UBA), Berlin, ISSN 0722-186X, 1999. </reference>
		<reference numeration="4" content_type="text"> Birmili, W., Berresheim, H., Plass-Dülmer, C., Elste, T., Gilge, S., Wiedensohler, A., and Uhrner, U.: The Hohenpeissenberg aerosol formation experiment (HAFEX): a long-term study including size resolved aerosol, H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;, OH, and monoterpenes measurements, Atmos. Chem. Phys., 3, 361–376, 2003. </reference>
		<reference numeration="5" content_type="text"> Birmili, W., Stratmann, F., and Wiedensohler, A.: Design of a DMA-based size spectrometer for a large particle size range and stable operation, J. Aerosol Sci., 30, 549–553, 1999. </reference>
		<reference numeration="6" content_type="text"> Birmili, W. and Wiedensohler, A.: New particle formation in the continental boundary layer: Meteorological and gas phase parameter influence, Geophys. Res. Lett., 27, 3325–3328, 2000. </reference>
		<reference numeration="7" content_type="text"> Ehrlich, C., Noll, G., Kalkoff, W. D., Baumback, G., and Dreiseidler, A.: PM$_10$, PM$_2.5$ and PM$_1.0$ emissions from industrial plants – Results from measurement programmes in Germany, Atmos. Environ., 41, 6236–6254, 2007. </reference>
		<reference numeration="8" content_type="text"> Eisele, F. L. and McMurry, P. H.: Recent progress in understanding particle nucleation and growth, Phil. Trans. R. Soc. Lond. B., 352, 191–201, 1997. </reference>
		<reference numeration="9" content_type="text"> Engler, C., Rose, D., Wehner, B., Wiedensohler, A., Brüggemann, E., Gnauk, T., Spindler, G., Tuch, T., and Birmili, W.: Size distributions of non-volatile particle residuals (Dp$&lt;$800 nm) at a rural site in Germany and relation to air mass origin, Atmos. Chem. Phys., 7, 5785–5802, 2007. </reference>
		<reference numeration="10" content_type="text"> Fagerli, H., Spranger, T., and Posch, M.: Chapter 3: Acidification and eutrophication – progress towards the Gothenburg protocol target year (2010), in: EMEP Report 1/2006, Transboundary acidification, eutrophication and ground level ozone in Europe from 1990 to 2004 in support for the review of the Gothenburg Protocol, ISSN 1504–610, 2006. </reference>
		<reference numeration="11" content_type="text"> Gaydos, T. M., Stanier, C. O., and Pandis, S. N.: 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="12" content_type="text"> Hamed, A., Joutsensaari, J., Mikkonen, S., Sogacheva, L., Dal Maso, M., Kulmala, M., Cavalli, F., Fuzzi, S., Facchini, M. C., Decesari, S., Mircea, M., Lehtinen, K. E. J., and Laaksonen, A.: Nucleation and growth of new particles in Po Valley, Italy, Atmos. Chem. Phys., 7, 355–376, 2007. </reference>
		<reference numeration="13" content_type="text"> Haywood, J. M. and Boucher, O.: Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review, Rev. Geophys., 38, 513–543, 2000. </reference>
		<reference numeration="14" content_type="text"> Heald, C. L., Henze, D. K., Horowitz, L. W., Feddema, J., Lamarque, J.-F. , Guenther, A., Hess, P. G., Vitt, F., Goldstein, A. H., Fung, I., and Seinfeld, J. H.: Predicted change in global secondary organic aerosol concentrations in response to future climate, emissions, and land-use change, J. Geophys. Res., 113, D05211, doi:10.1029/2007JD009092, 2008. </reference>
		<reference numeration="15" content_type="text"> Jeong, C. H., Hopke, P. K., Chalupa, D., and Utell, M.: Characteristics of nucleation and growth events of ultrafine particles measured in Rochester, NY, Environ. Sci. Technol., 38, 1933–1940, 2004. </reference>
		<reference numeration="16" content_type="text"> Kerminen, V.-M., Anttila, T., Lehtinen, K. E. J., and Kulmala, M.: Parameterization for atmospheric new-particle formation: application to a system involving sulfuric acid and condensable water-soluble organic vapors, Aerosol. Sci. Technol., 38, 1001–1008, 2004. </reference>
		<reference numeration="17" content_type="text"> Krüger, O., Marks, R., and Graßl, H.: Influence of pollution on cloud reflectance, J. Geophys. Res., 109, D24210, doi:10.1029/2004JD004625, 2004. </reference>
		<reference numeration="18" content_type="text"> Kuang, C., McMurry, P. H., McCormick, A. V., and Eisele, F.: Dependence of nucleation rates on sulfuric acid vapor concentrations in diverse atmospheric locations, J. Geophys. Res., 13, D10209, doi:10.1029/2007JD009253, 2008. </reference>
		<reference numeration="19" content_type="text"> Kulmala, M.: How particles nucleate and grow, Science, 302, 1000–1001, 2003. </reference>
		<reference numeration="20" content_type="text"> Kulmala, M., Hämeri, K., Aalto, P. P., Mäkelä, J. M., Pirjola, L., Nilsson, E. D., Buzorius, G., Rannik, U., Dal Maso, M., Seidl, W., Hoffmann, T., Jansson, R., Hansson, H.-C., Viisanen, Y., Laaksonen, A., and O&apos;Dowd, C. D.: Overview of the international project on biogenic aerosol formation in the boreal forest (BIOFOR), Tellus, 53B, 324–343, 2001. </reference>
		<reference numeration="21" content_type="text"> Kulmala, M., Laakso, L., Lehtinen, K. E. J., Riipinen, I., Dal Maso, M., Anttila, T., Kerminen, V.-M., Hörrak, U, Vana, M., and Tammet, H.: Initial steps of aerosol growth, Atmos. Chem. Phys., 4, 2553–2560, 2004a. </reference>
		<reference numeration="22" content_type="text"> Kulmala, M., Lehtinen, K. E. J., and Laaksonen, A.: Cluster activation theory as an explanation of the linear dependence between formation rate of 3 nm particles and sulphuric acid concentration, Atmos. Chem. Phys., 6, 787–793, 2006. </reference>
		<reference numeration="23" content_type="text"> Kulmala, M., Petäjä, T., Mönkkönen, P., Koponen, I., Dal Maso, M., Aalto, P., Lehtinen, K. E. J., and Kerminen, V.-M.: On the growth of nucleation mode particles: source rates of condensable vapor in polluted and clean environments, Atmos. Chem. Phys., 5, 409–416, 2005. </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, 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., 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, 2004b. </reference>
		<reference numeration="26" 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, 1–4, 2005. </reference>
		<reference numeration="27" content_type="text"> Laaksonen,~A., Kulmala,~M., O&apos;Dowd,~C D., Joutsensaari,~J., Vaattovaara,~P., Mikkonen,~S., Lehtinen,~K E J., Sogacheva,~L., Dal~Maso,~M., Aalto,~P., Petäjä,~T., Sogachev,~A., Yoon,~Y J., Lihavainen,~H., Nilsson,~D., Facchini,~M C., Cavalli,~F., Fuzzi,~S., Hoffmann,~T., Arnold,~F., Hanke,~M., Sellegri,~K., Umann,~B., Junkermann,~W., Coe,~H., Allan,~J D., Alfarra,~M R., Worsnop,~D R., Riekkola,~M -L., Hyötyläinen,~T., and Viisanen,~Y.: The role of VOC oxidation products in continental new particle formation, Atmos. Chem. Phys., 8, 2657–2665, 2008. </reference>
		<reference numeration="28" content_type="text"> Lintz, G. and Schmude, K.: Germany: Tackling the East-West divide. In Bernhard Müller, Maroš Finka and Gerd Lintz, Rise and Decline of Industry in Central and Eastern Europe: A Comparative Study of Cities and Regions in Eleven Countries. Series of Central and Eastern European Development Studies, Springer, Berlin, 81–110, 2005. </reference>
		<reference numeration="29" content_type="text"> Lohmann, U., and Feichter, J.: Global indirect aerosol effects: a review, Atmos. Chem. Phys., 5, 715–737, 2005. </reference>
		<reference numeration="30" content_type="text"> Lövblad, G., Tarrasön, L., Tørseth, K., and Dutchak, S.: EMEP Assessment Report Part I, European Perspective. ISBN 82-7144-032-2, available from http://www.emep.int, Oslo, 2004. </reference>
		<reference numeration="31" content_type="text"> Manktelow, P. T., Mann, G. W., Carslaw, K. S., Spracklen, D. V., and Chipperfield, M. P.: Regional and global trends in sulfate aerosol since the 1980s, Geophys. Res. Lett., 34, L14803, doi:10.1029/2006GL028668, 2007. </reference>
		<reference numeration="32" content_type="text"> Marquardt, W., Brüggemann, E., Auel, R., Herrmann, H., and Möller, D.: Trends of pollution in rain over East Germany caused by changing emissions, Tellus, 53, 529–545, 2001. </reference>
		<reference numeration="33" content_type="text"> Morawska, L., Bofinger, N. D., and Kocis, L.: Submicrometer and supermicrometer particles from diesel vehicle emissions, Environ. Sci. Technol., 32, 2033–2042, 1998. </reference>
		<reference numeration="34" content_type="text"> Müller, K., Pelzing, M., Gnauk, T., Kappe, A., Teichmann, U., Spindler, G., Haferkorn, S., Jahn, Y., and Herrmann, H.: Monoterpene emissions and carbonyl compound air concentrations during the blooming period of rape (Brassica napus), Chemosphere, 49, 1247–1256, 2002. </reference>
		<reference numeration="35" content_type="text"> Myhre, G., Stordal, F., Berglen, T. F., Sundet, J., and Isaksen, I. S. A.: Uncertainties in the radiative forcing due to sulfate aerosols, J. Atmos. Sci., 61, 485–498, 2004. </reference>
		<reference numeration="36" content_type="text"> Ohlström, M. O., Lehtinen, K .E. J., Moisio, M., and Jokiniemi, J. K.: Fine-particle emissions of energy production in Finland, Atmos. Environ., 34, 3701–3711, 2000. </reference>
		<reference numeration="37" content_type="text"> Pirjola, L., Laaksonen, A., Aalto, P., and Kulmala, M.: Sulfate aerosol formation in the Arctic boundary layer, J. Geophys. Res., 103, 8309–8322, 1998. </reference>
		<reference numeration="38" content_type="text"> R Development Core Team R.: A language and environment for statistical computing. R Foundation for Statistical Computing, Vienna, Austria. ISBN:3-900051-07-0, available online: http://www.R-project.org, 2008. </reference>
		<reference numeration="39" content_type="text"> Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld. D.: Aerosols, climate, and the hydrological cycle, Science, 294, 2119–2124, 2001. </reference>
		<reference numeration="40" content_type="text"> Ravishankara, A. R.: Heterogeneous and multiphase chemistry in the troposphere, Science, 276, 1058–1065, 1997. </reference>
		<reference numeration="41" content_type="text"> Riipinen, I., Sihto, S.-L., Kulmala, M., Arnold, F., Dal Maso, M., Birlmili, 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 Hyytiälä and Heidelberg, Atmos. Chem. Phys., 7, 1899–1914, 2007. </reference>
		<reference numeration="42" content_type="text"> Rohrer, F., and Berresheim, H.: Strong correlation between levels of tropospheric hydroxyl radical and solar ultraviolet radiation, Nature, 442, 184–187, 2006. </reference>
		<reference numeration="43" content_type="text"> Sekiguchi, M., Nakajima, T., Suzuki, K., Kawamoto, K., Higurashi, A., Rosenfeld, D., Sano, I., and Mukai, S.: A study of the direct and indirect effects of aerosols using global satellite data sets of aerosol and cloud parameters, J. Geophys. Res., 108(D22), 4699, doi:10.1029/2002JD003359, 2003. </reference>
		<reference numeration="44" 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="45" content_type="text"> Spindler, G., Müller, K. , Brüggemann, E., Gnauk, T., and Herrmann, H.: Long-term size-segregated characterization of PM$_10$, PM$_2.5$, and PM$_1$ at the IfT research station Melpitz downwind of Leipzig (Germany) using high and low-volume filter samplers, Atmos. Environ., 38, 5333–5347, 2004. </reference>
		<reference numeration="46" content_type="text"> Stanier, C. O., Khlystov, A. Y., and Pandis, S. N.: Nucleation events during the Pittsburgh Air Quality Study: Description and relation to key meteorological, gas phase, and aerosol parameters, Aerosol Sci. Tech., 38, 253–264, 2004. </reference>
		<reference numeration="47" 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="48" content_type="text"> Vestreng, V., Myhre, G., Fagerli, H., Reis, S., and Tarrasön, L.: Twenty-five years of continuous sulphur dioxide emission reduction in Europe, Atmos. Chem. Phys., 7, 3663–3681, 2007. </reference>
		<reference numeration="49" content_type="text"> Vestreng, V., Rigler, E., Adams, M., Kindbom, K., Pacyna, J. M., Denier van der Gon, H., Reis, S., and Travnikov, O.: Inventory review 2006, Emission data reported to LRTAP and NEC Directive, Stage 1, 2 and 3 review and Evaluation of inventories of HM and POPs. EMEP/MSC-W Technical Report 1/2006 ISSN:1504-6179, available from http://www.emep.int, 2006. </reference>
		<reference numeration="50" 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., D102, 4375–4385, 1997. </reference>
		<reference numeration="51" content_type="text"> Weber, R. J., McMurry, P. H., Mauldin, R. L., Tanner, D. J., Eisele, F. L., Clarke, A. D., and Kapustin, V. N.: New particle formation in the remote troposphere: A comparison of observations at various sites, Geophys. Res. Lett., 26, 307–310, 1999. </reference>
		<reference numeration="52" content_type="text"> Weber, R. J., McMurry, P. H., Mauldlin, R. L., Tanner, D. J., Eisele, F. L., Clarke, A. D., and Kapustin, V. N.: New particle formation in the remort troposphere: A comparison of observations at various sites, Geophys. Res. Lett., 26, 307–310, 1999. </reference>
		<reference numeration="53" content_type="text"> Wehner, B. and Wiedensohler, A.: Long term measurements of submicrometer urban aerosols: Statistical analysis for correlations with meteorological conditions and trace gases, Atmos. Chem. Phys., 3, 867–879, 2003. </reference>
		<reference numeration="54" 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="55" content_type="text"> Zhang, Q., Stanier, C. O., Canagaratna, M., Jayne, J., Worsnop, D. R., Pandis, S., and Jimenez, J.: Insights into the chemistry of new particle formation and growth events in Pittsburgh based on aerosol mass spectrometry, Environ. Sci. Technol., 38, 4797–4809, 2004. </reference>
	</references>
</article>

