<?xml version="1.0" encoding="utf-8" standalone="no"?>
<!DOCTYPE article SYSTEM "http://www.atmos-chem-phys.net/inc/acp/copernicus.dtd">
<article language="en">
	<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-9-2959-2009</doi>
	<article_url>http://www.atmos-chem-phys.net/9/2959/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/9/2959/2009/acp-9-2959-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/9/2959/2009/acp-9-2959-2009.pdf</fulltext_pdf>
	<start_page>2959</start_page>
	<end_page>2971</end_page>
	<publication_date>2009-05-06</publication_date>
	<article_title content_type="html">Increased cloud activation potential of secondary organic aerosol for  atmospheric mass loadings</article_title>
	<authors>
		<author numeration="1" affiliations="1,3">
			<name>S. M. King</name>
		</author>
		<author numeration="2" affiliations="1,3">
			<name>T. Rosenoern</name>
		</author>
		<author numeration="3" affiliations="1,4">
			<name>J. E. Shilling</name>
		</author>
		<author numeration="4" affiliations="1">
			<name>Q. Chen</name>
		</author>
		<author numeration="5" affiliations="1,2">
			<name>S. T. Martin</name>
			<email>scot_martin@harvard.edu</email>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">School of Engineering and Applied Sciences,  Harvard University, Cambridge, MA 02138, USA</affiliation>
		<affiliation numeration="2" content_type="html">Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138, USA</affiliation>
		<affiliation numeration="3" content_type="html">now at: Institut de Recherches sur la Catalyse et l&apos;Environnement de Lyon,  UMR5256, Université de Lyon 1, CNRS, Villeurbanne, France</affiliation>
		<affiliation numeration="4" content_type="html">now at: Pacific Northwest National Laboratory, Atmospheric Sciences and  Global Change Division,  Richland, WA 99352, USA</affiliation>
	</affiliations>
	<abstract content_type="html">The effect of organic particle mass loading from 1 to
&amp;ge;100 &amp;mu;g m&lt;sup&gt;&amp;minus;3&lt;/sup&gt; on the cloud condensation nuclei (CCN)
properties of mixed organic-sulfate particles was investigated in the
Harvard Environmental Chamber. Mixed particles were produced by the
condensation of organic molecules onto ammonium sulfate particles
during the dark ozonolysis of α-pinene.  A continuous-flow
mode of the chamber provided stable conditions over long time periods,
allowing for signal integration and hence increased measurement
precision at low organic mass loadings representative of atmospheric
conditions. CCN activity was measured at eight mass loadings for 80-
and 100-nm particles grown on 50-nm sulfate seeds. A two-component
(organic/sulfate) Köhler model, which included the particle
heterogeneity arising from DMA size selection and from organic volume
fraction for the selected 80- and 100-nm particles, was used to
predict CCN activity. For organic mass loadings of 2.9 &amp;mu;g m&lt;sup&gt;&amp;minus;3&lt;/sup&gt;
and greater, the observed activation curves were well
predicted using a single set of physicochemical parameters for the
organic component. For mass loadings of 1.74 &amp;mu;g m&lt;sup&gt;&amp;minus;3&lt;/sup&gt; and
less, the observed CCN activity increased beyond predicted values
using the same parameters, implying changed physicochemical properties
of the organic component. A sensitivity analysis suggests that a drop in surface
tension must be invoked to explain quantitatively the CCN observations at low
SOA particle mass loadings. Other factors, such as decreased molecular weight,
increased density, or increased van&apos;t Hoff factor, can contribute to the
explanation but are quantitatively insufficient as the full explanation.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Alofs,~D J. and Balakumar,~P.: Inversion to obtain aerosol size distributions from measurements with a differential mobility analyzer, J Aerosol Sci., 13, 513–527, 1982. </reference>
		<reference numeration="2" content_type="text"> Capouet,~M. and Müller,~J F.: A group contribution method for estimating the vapour pressures of $\alpha $-pinene oxidation products, Atmos. Chem. Phys., 6, 1455–1467, 2006. </reference>
		<reference numeration="3" content_type="text"> Cocker,~D R., Clegg,~S L., Flagan,~R C., and Seinfeld,~J H.: The effect of water on gas-particle partitioning of secondary organic aerosol. Part I: α-pinene/ozone system, Atmos. Environ., 35, 6049–6072, 2001a. </reference>
		<reference numeration="4" content_type="text"> Cocker,~D R., Flagan,~R C., and Seinfeld,~J H.: State-of-the-art chamber facility for studying atmospheric aerosol chemistry, Environ. Sci. Technol., 35, 2594–2601, 2001b. </reference>
		<reference numeration="5" content_type="text"> Collins,~D R., Flagan,~R C., and Seinfeld,~J H.: Improved inversion of scanning DMA data, Aerosol Sci. Technol., 36, 1–9, 2002. </reference>
		<reference numeration="6" content_type="text"> DeCarlo,~P F., Slowik,~J G., Worsnop,~D R., Davidovits,~P., and Jimenez,~J L.: Particle morphology and density characterization by combined mobility and aerodynamic diameter measurements. Part 1: Theory, Aerosol Sci. Technol., 38, 1185–1205, 2004. </reference>
		<reference numeration="7" content_type="text"> DeCarlo,~P F., Kimmel,~J R., Trimborn,~A., Northway,~M J., Jayne,~J T., Aiken,~A C., Gonin,~M., Fuhrer,~K., Horvath,~T., Docherty,~K S., Worsnop,~D R., and Jimenez,~J L.: Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer, Anal. Chem., 78, 8281–8289, 2006. </reference>
		<reference numeration="8" content_type="text"> Donahue,~N M., Robinson,~A L., Stanier,~C O., and Pandis,~S N.: Coupled partitioning, dilution, and chemical aging of semivolatile organics, Environ. Sci. Technol., 40, 2635–2643, 2006. </reference>
		<reference numeration="9" content_type="text"> Duplissy,~J., Gysel,~M., Alfarra,~M R., Dommen,~J., Metzger,~A., Prevot,~A S H., Weingartner,~E., Laaksonen,~A., Raatikainen,~T., Good,~N., Turner,~S F., McFiggans,~G., and Baltensperger,~U.: Cloud forming potential of secondary organic aerosol under near atmospheric conditions, Geophys. Res. Lett., 35, L03818, doi:03810.01029/02007GL031075, 2008. </reference>
		<reference numeration="10" content_type="text"> Engelhart,~G J., Asa-Awuku,~A., Nenes,~A., and Pandis,~S N.: CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol, Atmos. Chem. Phys., 8, 3937–3949, 2008. </reference>
		<reference numeration="11" content_type="text"> Ervens,~B., Feingold,~G., and Kreidenweis,~S M.: Influence of water-soluble organic carbon on cloud drop number concentration, J Geophys. Res., 110, D18211, doi:18210.11029/12004JD005634, 2005. </reference>
		<reference numeration="12" content_type="text"> Facchini,~M C., Mircea,~M., Fuzzi,~S., and Charlson,~R J.: Cloud albedo enhancement by surface-active organic solutes in growing droplets, Nature, 401, 257–259, 1999. </reference>
		<reference numeration="13" content_type="text"> Grieshop,~A P., Donahue,~N M., and Robinson,~A L.: Is the gas-particle partitioning in alpha-pinene secondary organic aerosol reversible?, Geophys. Res. Lett., 34, L14810, doi:14810.11029/12007GL029987, 2007. </reference>
		<reference numeration="14" content_type="text"> Hartz,~K E H., Rosenoern,~T., Ferchak,~S R., Raymond,~T M., Bilde,~M., Donahue,~N M., and Pandis,~S N.: Cloud condensation nuclei activation of monoterpene and sesquiterpene secondary organic aerosol, J Geophys. Res., 110, D14208, doi:14210.11029/12004JD005754, 2005. </reference>
		<reference numeration="15" content_type="text"> Hegg,~D A., Gao,~S., Hoppel,~W., Frick,~G., Caffrey,~P., Leaitch,~W R., Shantz,~N., Ambrusko,~J., and Albrechcinski,~T.: Laboratory studies of the efficiency of selected organic aerosols as CCN, Atmos. Res., 58, 155–166, 2001. </reference>
		<reference numeration="16" content_type="text"> Hyvärinen,~A.-P., Lihavainen,~H., Gaman,~A., Vairila,~L., Ojala,~H., Kulmala,~M., and Viisanen, Y.: Surface tensions and densities of oxalic, malonic, succinic, maleic, malic, and cis-pinonic acids, J Chem. Eng. Data, 51, 255-260, 2006. </reference>
		<reference numeration="17" content_type="text"> IPCC (Intergovernmental Panel on Climate Change): Climate Change 2007: The Physical Science Basis, Cambridge University Press, 2007. </reference>
		<reference numeration="18" content_type="text"> Katrib,~Y., Martin,~S T., Rudich,~Y., Davidovits,~P., Jayne,~J T., and Worsnop,~D R.: Density changes of aerosol particles as a result of chemical reaction, Atmos. Chem. Phys., 5, 275–291, 2005. </reference>
		<reference numeration="19" content_type="text"> King,~S M., Rosenoern,~T., Shilling,~J E., Chen,~Q., and Martin,~S T.: Cloud condensation nucleus activity of secondary organic aerosol particles mixed with sulfate, Geophys. Res. Lett., 34, L24803, doi:24810.21029/22007GL030390, 2007. </reference>
		<reference numeration="20" content_type="text"> Kleindienst,~T E., Smith,~D F., Li,~W., Edney,~E O., Driscoll,~D J., Speer,~R E., and Weathers,~W S.: Secondary organic aerosol formation from the oxidation of aromatic hydrocarbons in the presence of dry submicron ammonium sulfate aerosol, Atmos. Environ., 33, 3669–3681, 1999. </reference>
		<reference numeration="21" content_type="text"> Knutson,~E O. and Whitby,~T B.: Aerosol classification by electric mobility: Apparatus, theory, and applications, J Aerosol Sci., 6, 443–451, 1975. </reference>
		<reference numeration="22" content_type="text"> Kostenidou,~E., Pathak,~R K., and Pandis,~S N.: An algorithm for the calculation of secondary organic aerosol density combining AMS and SMPS data, Aerosol Sci. Technol., 41, 1002–1010, 2007. </reference>
		<reference numeration="23" content_type="text"> Lance,~S., Medina,~J., Smith,~J N., and Nenes,~A.: Mapping the operation of the DMT Continuous Flow CCN counter, Aerosol Sci. Technol., 40, 242–254, 2006. </reference>
		<reference numeration="24" content_type="text"> Lohmann,~U. and Feichter,~J.: Global indirect aerosol effects: a review, Atmos. Chem. Phys., 5, 715–737, 2005. </reference>
		<reference numeration="25" content_type="text"> McFiggans,~G., Artaxo,~P., Baltensperger,~U., Coe,~H., Facchini,~M C., Feingold,~G., Fuzzi,~S., Gysel,~M., Laaksonen,~A., Lohmann,~U., Mentel,~T F., Murphy,~D M., O&apos;Dowd,~C D., Snider,~J R., and Weingartner,~E.: The effect of physical and chemical aerosol properties on warm cloud droplet activation, Atmos. Chem. Phys., 6, 2593–2649, 2006. </reference>
		<reference numeration="26" content_type="text"> Paulsen,~D., Dommen,~J., Kalberer,~M., Prevot,~A S H., Richter,~R., Sax,~M., Steinbacher,~M., Weingartner,~E., and Baltensperger,~U.: Secondary organic aerosol formation by irradiation of 1,3,5-trimethylbenzene-\chemNO_x-\chemH_2O in a new reaction chamber for atmospheric chemistry and physics, Environ. Sci. Technol., 39, 2668–2678, 2005. </reference>
		<reference numeration="27" content_type="text"> Petters,~M D. and Kreidenweis,~S M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, 2007. </reference>
		<reference numeration="28" content_type="text"> Petters,~M D., Prenni,~A J., Kreidenweis,~S M., and DeMott,~P J.: On measuring the critical diameter of cloud condensation nuclei using mobility selected aerosol, Aerosol Sci. Technol., 41, 907–913, 2007. </reference>
		<reference numeration="29" content_type="text"> Prenni,~A J., Petters,~M D., Kreidenweis,~S M., and DeMott,~P J.: Cloud droplet activation of secondary organic aerosol, J Geophys. Res., 112, D10223, doi:10210.11029/12006JD007963, 2007. </reference>
		<reference numeration="30" content_type="text"> Prisle,~N L., Raatikainen,~T., Sorjamaa,~R., Svenningsson,~B., Laaksonen,~A., Bilde,~M.: Surfactant partitioning in cloud droplet activation: a study of C8, C10, C12 and C14 normal fatty acid sodium salts, Tellus, 60B, 416–431, 2008. </reference>
		<reference numeration="31" content_type="text"> Roberts,~G C. and Nenes,~A.: A continuous-flow streamwise thermal-gradient CCN chamber for atmospheric measurements, Aerosol Sci. Technol., 39, 206–221, 2005. </reference>
		<reference numeration="32" content_type="text"> Rose,~D., Frank,~G P., Dusek,~U., Gunthe,~S S., Andreae,~M O., and Pöschl,~U.: Calibration and measurement uncertainties of a continuous-flow cloud condensation nucleus counter (DMT-CCNC): CCN activation of ammonium sulfate and sodium chloride aerosol particles in theory and experiment, Atmos. Chem. Phys., 8, 1153–1179, 2008. </reference>
		<reference numeration="33" content_type="text"> Seinfeld,~J H., Kleindienst,~T E., Edney,~E O., and Cohen,~J B.: Aerosol growth in a steady-state, continuous flow chamber: Application to studies of secondary aerosol formation, Aerosol Sci. Technol., 37, 728–734, 2003. </reference>
		<reference numeration="34" content_type="text"> Seinfeld,~J H. and Pankow,~J F.: Organic Atmospheric Particulate Material, Annu. Rev. Phys. Chem., 54, 121–140, 2003. </reference>
		<reference numeration="35" content_type="text"> Shilling,~J E., King,~S M., Mochida,~M., Worsnop,~D R., and Martin,~S T.: Mass spectral evidence that small changes in composition caused by oxidative aging processes alter aerosol CCN properties, J Phys. Chem. A, 111, 3358–3368, 2007.  </reference>
		<reference numeration="36" content_type="text"> Shilling,~J E., Chen,~Q., King,~S M., Rosenoern,~T., Kroll,~J H., Worsnop,~D R., McKinney,~K A., and Martin,~S T.: Particle mass yield in secondary organic aerosol formed by the dark ozonolysis of α-pinene, Atmos. Chem. Phys., 8, 2073–2088, 2008. </reference>
		<reference numeration="37" content_type="text"> Shilling,~J E., Chen,~Q., King,~S M., Rosenoern,~T., Kroll,~J H., Worsnop,~D R., DeCarlo,~P F., Aiken,~A C., Sueper,~D., Jimenez,~J L., and Martin,~S T.: Loading-dependent elemental composition of $\alpha $-pinene SOA particles, Atmos. Chem. Phys. 9, 771–782,, 2009. </reference>
		<reference numeration="38" content_type="text"> Shulman,~M L., Jacobson,~M C., Carlson,~R J., Synovec,~R E., and Young,~T E.: Dissolution behavior and surface tension effects of organic compounds in nucleating cloud droplets, Geophys. Res. Lett., 23, 277–280, 1996. </reference>
		<reference numeration="39" content_type="text"> Sorjamaa,~R., Svenningsson,~B., Raatikainen,~T., Henning,~S., Bilde,~M., Laaksonen,~A.: The role of surfactants in Köhler theory reconsidered, Atmos. Chem. Phys., 4, 2107–2117, 2004. </reference>
		<reference numeration="40" content_type="text"> Stanier,~C O., Pathak,~R K., and Pandis,~S N.: Measurements of the volatility of aerosols from α-pinene ozonolysis, Environ. Sci. Technol., 41, 2756–2763, 2007. </reference>
		<reference numeration="41" content_type="text"> Svenningsson,~B., Rissler,~J., Swietlicki,~E., Mircea,~M., Bilde,~M., Facchini,~M C., Decesari,~S., Fuzzi,~S., Zhou,~J., Mønster,~J., and Rosenoern,~T.: Hygroscopic growth and critical supersaturations for mixed aerosol particles of inorganic and organic compounds of atmospheric relevance, Atmos. Chem. Phys., 6, 1937–1952, 2006. </reference>
		<reference numeration="42" content_type="text"> Topping,~D O., McFiggans,~G B., Kiss,~G., Varga,~Z., Facchini,~M C., Decesari,~S., and Mircea,~M.: Surface tensions of multi-component mixed inorganic/organic aqueous systems of atmospheric significance: measurements, model predictions and importance for cloud activation predictions, Atmos. Chem. Phys., 7, 2371-2398, 2007. </reference>
		<reference numeration="43" content_type="text"> Tuckermann,~R.: Surface tensions of aqueous solutions of water-soluble organic and inorganic compounds, Atmos. Env., 41, 6265–6275, 2007. </reference>
		<reference numeration="44" content_type="text"> VanReken,~T M., Ng,~N L., Flagan,~R C., and Seinfeld,~J H.: Cloud condensation nucleus activation properties of biogenic secondary organic aerosol, J Geophys. Res., 110, D07206, doi:07210.01029/02004JD005465, 2005. </reference>
		<reference numeration="45" content_type="text"> Wiedensohler,~A.: An approximation of the bipolar charge distribution for particles in the submicron size range, J Aerosol Sci., 19, 387–389, 1988. </reference>
	</references>
</article>

