<?xml version="1.0" encoding="UTF-8"?>
<!DOCTYPE article PUBLIC "-//NLM//DTD Journal Publishing DTD v3.0 20080202//EN" "http://dtd.nlm.nih.gov/publishing/3.0/journalpublishing3.dtd">
<article xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink" article-type="research-article" dtd-version="3.0" xml:lang="en">
<front>
<journal-meta>
<journal-id journal-id-type="publisher">ACP</journal-id>
<journal-title-group>
<journal-title>Atmospheric Chemistry and Physics</journal-title>
<abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1680-7324</issn>
<publisher><publisher-name>Copernicus GmbH</publisher-name>
<publisher-loc>Göttingen, Germany</publisher-loc>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="doi">10.5194/acp-9-3999-2009</article-id>
<title-group>
<article-title>Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol – Part 2: Theoretical approaches</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Petters</surname>
<given-names>M. D.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Wex</surname>
<given-names>H.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Carrico</surname>
<given-names>C. M.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Hallbauer</surname>
<given-names>E.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Massling</surname>
<given-names>A.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<xref ref-type="aff" rid="aff3">
<sup>3</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>McMeeking</surname>
<given-names>G. R.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Poulain</surname>
<given-names>L.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Wu</surname>
<given-names>Z.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Kreidenweis</surname>
<given-names>S. M.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Stratmann</surname>
<given-names>F.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Institute for Tropospheric Research, Leipzig, Germany</addr-line>
</aff>
<aff id="aff3">
<label>3</label>
<addr-line>now at: National Environmental Research Institute, Aarhus University, Roskilde, Denmark</addr-line>
</aff>
<aff id="aff4">
<label>4</label>
<addr-line>now at: Centre for Atmospheric Science, University of Manchester, Manchester, UK</addr-line>
</aff>
<pub-date pub-type="epub">
<day>18</day>
<month>06</month>
<year>2009</year>
</pub-date>
<volume>9</volume>
<issue>12</issue>
<fpage>3999</fpage>
<lpage>4009</lpage>
<permissions>
<license xlink:type="simple">
<license-p>This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.</license-p>
</license>
</permissions>
<self-uri xlink:href="http://www.atmos-chem-phys.net/9/3999/2009/acp-9-3999-2009.html">This article is available from http://www.atmos-chem-phys.net/9/3999/2009/acp-9-3999-2009.html</self-uri>
<self-uri xlink:href="http://www.atmos-chem-phys.net/9/3999/2009/acp-9-3999-2009.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys.net/9/3999/2009/acp-9-3999-2009.pdf</self-uri>
<abstract>
<p>We examine the hygroscopic properties of secondary organic aerosol particles
generated through the reaction of α-pinene and ozone using a
continuous flow reaction chamber. The water activity versus composition
relationship is calculated from measurements of growth factors at relative
humidities up to 99.6% and from measurements of cloud condensation nuclei
activity. The observed relationships are complex, suggesting highly
non-ideal behavior for aerosol water contents at relative humidities less
than 98%. We present two models that may explain the observed water
activity-composition relationship equally well. The first model assumes that
the aerosol is a pseudo binary mixture of infinitely water soluble compounds
and sparingly soluble compounds that gradually enter the solution as
dilution increases. The second model is used to compute the Gibbs free
energy of the aerosol-water mixture and shows that the aerosol behaves
similarly to what can be expected for single compounds that contain a
certain fraction of oxygenated and non-polar functional groups.</p>
</abstract>
<counts><page-count count="11"/></counts>
</article-meta>
</front>
<body/>
<back>
<ref-list>
<title>References</title>
<ref id="ref1">
<label>1</label><mixed-citation publication-type="other" xlink:type="simple"> Amundson, N. R., Caboussat, A., He, J. W., Martynenko, A. V., Landry, C., Tong, C., and Seinfeld, J. H.: A new atmospheric aerosol phase equilibrium model (UHAERO): organic systems, Atmos. Chem. Phys., 7(17), 4675–4698, 2007. </mixed-citation>
</ref>
<ref id="ref2">
<label>2</label><mixed-citation publication-type="other" xlink:type="simple"> Asa-Awuku, A., Nenes, A., Gao, S., Flagan, R. C., and Seinfeld, J. H.: Alkene ozonolysis SOA: inferences of composition and droplet growth kinetics from Köhler theory analysis, Atmos. Chem. Phys. Discuss., 7, 8983–9011, 2007. </mixed-citation>
</ref>
<ref id="ref3">
<label>3</label><mixed-citation publication-type="other" xlink:type="simple"> Bahreini, R., Keywood, M. D., Ng, N. L., Varutbangkul, V., Gao, S., Flagan, R. C., Seinfeld, J. H., Worsnop, D. R., and Jimenez, J. L.: Measurements of secondary organic aerosol from oxidation of cycloalkenes, terpenes, and m-xylene using an Aerodyne aerosol mass spectrometer, Environ. Sci. Technol., 39(15), 5674–5688, 2005. </mixed-citation>
</ref>
<ref id="ref4">
<label>4</label><mixed-citation publication-type="other" xlink:type="simple"> Baltensperger, U., Kalberer, M., Dommen, J., Paulsen, D., Alfarra, M. R., Coe, H., Fisseha, R., Gascho, A., Gysel, M., Nyeki, S., Sax, M., Steinbacher, M., Prevot, A. S. H., Sjoren, S., Weingartner, E., and Zenobi, R.: Secondary organic aerosols from anthropogenic and biogenic precursors, Faraday Discuss., 130, 265–278, 2005. </mixed-citation>
</ref>
<ref id="ref5">
<label>5</label><mixed-citation publication-type="other" xlink:type="simple"> Carrico, C. M., Petters, M. D., Kreidenweis, S. M., Collett, J. L., Engling, G., and Malm, W. C.: Aerosol hygroscopicity and cloud droplet activation of extracts of filters from biomass burning experiments, J. Geophys. Res., 113(D8), 08206, 2008. </mixed-citation>
</ref>
<ref id="ref6">
<label>6</label><mixed-citation publication-type="other" xlink:type="simple"> Chan, M. N., Kreidenweis, S. M., and Chan, C. K.: Measurements of the Hygroscopic and Deliquescence Properties of Organic Compounds of Different Solubilities in Water and Their Relationship with Cloud Condensation Nuclei Activities, Environ. Sci. Technol., 42, 3602–3608, 2008. </mixed-citation>
</ref>
<ref id="ref7">
<label>7</label><mixed-citation publication-type="other" xlink:type="simple"> Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: Thermodynamic model of the system H$^+$-NH$_4^+$-Na$^+$-SO$_4^2-$-NO$_3^-$-Cl$^-$-H&lt;sub&gt;2&lt;/sub&gt;O at 298.15 K, J. Phys. Chem., 102(11), 2155–2171, 1998. </mixed-citation>
</ref>
<ref id="ref8">
<label>8</label><mixed-citation publication-type="other" xlink:type="simple"> Duplissy, J., M. Gysel, M. R. Alfarra, J. Dommen, A. Metzger, A. S. H. Prevot, E. Weingartner, A. Laaksonen, T. Raatikainen, N. Good, S. F. Turner, G. McFiggans and U. Baltensperger: Cloud forming potential of secondary organic aerosol under near atmospheric conditions, Geophys. Res. Lett., 35(3), L03818, doi:03810.01029/02007GL031075, 2008. </mixed-citation>
</ref>
<ref id="ref9">
<label>9</label><mixed-citation publication-type="other" xlink:type="simple"> 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. </mixed-citation>
</ref>
<ref id="ref10">
<label>10</label><mixed-citation publication-type="other" xlink:type="simple"> Facchini, M. C., Mircea, M., Fuzzi, S., and Charlson, R. J.: Cloud albedo enhancement by surface-active organic solutes in growing droplets, Nature, 401(6750), 257–259, 1999. </mixed-citation>
</ref>
<ref id="ref11">
<label>11</label><mixed-citation publication-type="other" xlink:type="simple"> Frank, H. S. and Evans, M. W.: Free Volume and Entropy in Condensed Systems .3. Entropy in Binary Liquid Mixtures – Partial Molal Entropy in Dilute Solutions - Structure and Thermodynamics in Aqueous Electrolytes, J. Chem. Phys., 13(11), 507–532, 1945. </mixed-citation>
</ref>
<ref id="ref12">
<label>12</label><mixed-citation publication-type="other" xlink:type="simple"> 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(3), 155–166, 2001. </mixed-citation>
</ref>
<ref id="ref13">
<label>13</label><mixed-citation publication-type="other" xlink:type="simple"> Huff Hartz, K. E. H., Rosenorn, 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(D14), D14208, doi:14210.11029/12004JD005754, 2005. </mixed-citation>
</ref>
<ref id="ref14">
<label>14</label><mixed-citation publication-type="other" xlink:type="simple"> Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of polymers as major components of atmospheric organic aerosols, Science, 303(5664), 1659–1662, 2004. </mixed-citation>
</ref>
<ref id="ref15">
<label>15</label><mixed-citation publication-type="other" xlink:type="simple"> King, S. M., T. Rosenoern, J. E. Shilling, Q. Chen and S. T. Martin: Cloud condensation nucleus activity of secondary organic aerosol particles mixed with sulfate, Geophys. Res. Lett., 34(24), L24806, doi:24810.21029/22007GL030390., 2007. </mixed-citation>
</ref>
<ref id="ref16">
<label>16</label><mixed-citation publication-type="other" xlink:type="simple"> Lance, S., Medina, J., Smith, J. N., and Nenes, A.: Mapping the operation of the DMT Continuous Flow CCN counter, Aerosol Sci. Tech., 40(4), 242–254, 2006. </mixed-citation>
</ref>
<ref id="ref17">
<label>17</label><mixed-citation publication-type="other" xlink:type="simple"> Ming, Y. and Russell, L. M.: Thermodynamic equilibrium of organic-electrolyte mixtures in aerosol particles, Aiche J., 48(6), 1331–1348, 2002. </mixed-citation>
</ref>
<ref id="ref18">
<label>18</label><mixed-citation publication-type="other" xlink:type="simple"> Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of aerosol hygroscopicity and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, 2007. </mixed-citation>
</ref>
<ref id="ref19">
<label>19</label><mixed-citation publication-type="other" xlink:type="simple"> Petters, M. D. and S. M. Kreidenweis: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 2: Including solubility, Atmos. Chem. Phys., 8, 6273–6279, 2008. </mixed-citation>
</ref>
<ref id="ref20">
<label>20</label><mixed-citation publication-type="other" xlink:type="simple"> 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(10), 907–913, 2007. </mixed-citation>
</ref>
<ref id="ref21">
<label>21</label><mixed-citation publication-type="other" xlink:type="simple"> Pöschl, U.: Atmospheric aerosols: Composition, transformation, climate and health effects, Angewandte Chemie-International Edition, 44(46), 7520–7540, 2005. </mixed-citation>
</ref>
<ref id="ref22">
<label>22</label><mixed-citation publication-type="other" xlink:type="simple"> Prausnitz, J. M., Lichtenthaler, R. N., and Azevedo, E. G.: Molecular thermodynamics of fluid-phase equilibria, Upper Saddle River, NJ, USA, Prentice Hall PTR, 1999. </mixed-citation>
</ref>
<ref id="ref23">
<label>23</label><mixed-citation publication-type="other" xlink:type="simple"> Prenni, A. J., Petters, M. D., DeMott, P. J., Kreidenweis, S. M., Ziemann, P. J., Matsunaga, A., and Lim, Y. B.: Cloud drop activation of secondary organic aerosol, J. Geophys. Res., 112, D10223, doi:10210.11029/12006JD007963, 2007. </mixed-citation>
</ref>
<ref id="ref24">
<label>24</label><mixed-citation publication-type="other" xlink:type="simple"> Raymond, T. M. and Pandis, S. N.: Cloud activation of single-component organic aerosol particles, J Geophys Res, 107(D24), 4787, doi:4710.1029/2002JD002159, 2002. </mixed-citation>
</ref>
<ref id="ref25">
<label>25</label><mixed-citation publication-type="other" xlink:type="simple"> Rissler, J., Vestin, A., Swietlicki, E., Fisch, G., Zhou, J., Artaxo, P., and Andreae, M. O.: Size distribution and hygroscopic properties of aerosol particles from dry-season biomass burning in Amazonia, Atmos. Chem. Phys., 6, 471–491, 2006. </mixed-citation>
</ref>
<ref id="ref26">
<label>26</label><mixed-citation publication-type="other" xlink:type="simple"> Roberts, G. C. and Nenes, A.: A continuous-flow streamwise thermal-gradient CCN chamber for atmospheric measurements, Aerosol Sci Tech, 39(3), 206–221, 2005. </mixed-citation>
</ref>
<ref id="ref27">
<label>27</label><mixed-citation publication-type="other" xlink:type="simple"> Rose, D., Gunthe, S. S., Mikhailov, E., Frank, G. P., Dusek, U., Andrea, M. O., and Pöschl, U.: Calibration and measurement uncertainties of a continuous-flow cloud condensation nuclei counter (DMT-CCNC): CCN activation of ammonium sulfate and sodium chloride aerosol particles in theory and experiment, Atmos. Chem. Phys., 8, 1153–1179, 2008. </mixed-citation>
</ref>
<ref id="ref28">
<label>28</label><mixed-citation publication-type="other" xlink:type="simple"> Saathoff, H., Naumann, K. H., Schnaiter, M., Schock, W., Mohler, O., Schurath, U., Weingartner, E., Gysel, M., and Baltensperger, U.: Coating of soot and (NH&lt;sub&gt;4&lt;/sub&gt;)(2)SO&lt;sub&gt;4&lt;/sub&gt; particles by ozonolysis products of alpha-pinene, J. Aerosol. Sci., 34(10), 1297–1321, 2003. </mixed-citation>
</ref>
<ref id="ref29">
<label>29</label><mixed-citation publication-type="other" xlink:type="simple"> Stratmann, F., Kiselev, A., Wurzler, S., Wendisch, M., Heintzenberg, J., Charlson, R. J., Diehl, K., Wex, H., and Schmidt, S.: Laboratory studies and numerical simulations of cloud droplet formation under realistic supersaturation conditions, J. Atmos. Ocean. Technol., 21(6), 876–887, 2004. </mixed-citation>
</ref>
<ref id="ref30">
<label>30</label><mixed-citation publication-type="other" xlink:type="simple"> Svenningsson, B., H. C. Hansson, A. Wiedensohler, K. Noone, J. Ogren, A. Hallberg and R. Colvile: Hygroscopic Growth of Aerosol-Particles and Its Influence on Nucleation Scavenging in-Cloud - Experimental Results from Kleiner-Feldberg, J. Atmos. Chem., 19(1–2), 129–152, 1994. </mixed-citation>
</ref>
<ref id="ref31">
<label>31</label><mixed-citation publication-type="other" xlink:type="simple"> Topping, D. O., McFiggans. G. B.. and Coe. H.: A curved multi-component aerosol hygroscopicity model framework: Part 2 – Including organic compounds, Atmos. Chem. Phys., 5, 1223–1242, 2005. </mixed-citation>
</ref>
<ref id="ref32">
<label>32</label><mixed-citation publication-type="other" xlink:type="simple"> Tuckermann, R. and Cammenga, H. K.: The surface tension of aqueous solutions of some atmospheric water-soluble organic compounds, Atmos. Environ., 38(36), 6135–6138, 2004. </mixed-citation>
</ref>
<ref id="ref33">
<label>33</label><mixed-citation publication-type="other" xlink:type="simple"> VanReken, T. M., Ng, N. L., Flagan, R. C., and Seinfeld, J. H.: Cloud condensation nucleus activation properties of biogenic secondary organic aerosol, J. Geophy. Res., 110(D7), D07206, doi:07210.01029/02004JD005465, 2005. </mixed-citation>
</ref>
<ref id="ref34">
<label>34</label><mixed-citation publication-type="other" xlink:type="simple"> Varutbangkul, V., Brechtel, F. J., Bahreini, R., Ng, N. L., Keywood, M. D., Kroll, J. H., Flagan, R. C., Seinfeld, J. H., Lee, J. H., and Goldstein, A. H.: Hygroscopicity of secondary organic aerosols formed by oxidation of cycloalkenes, monoterpenes, sesquiterpenes, and related compounds, Atmos. Chem. Phys., 6, 2367–2388, 2006. </mixed-citation>
</ref>
<ref id="ref35">
<label>35</label><mixed-citation publication-type="other" xlink:type="simple"> Virkkula, A., Van Dingenen, R., Raes, F., and Hjorth, J.: Hygroscopic properties of aerosol formed by oxidation of limonene, alpha-pinene, and beta-pinene, J. Geophys. Res., 104(D3), 3569–3579, 1999. </mixed-citation>
</ref>
<ref id="ref36">
<label>36</label><mixed-citation publication-type="other" xlink:type="simple"> Wex, H., Hennig, T., Salma, I., Ocskay, R., Kiselev, A., Henning, S., Massling, A., Wiedensohler, A., and Stratmann, F.: Hygroscopic growth and measured and modeled critical super-saturations of an atmospheric HULIS sample, Geophys Res Lett, 34(2), L02818, doi:02810.01029/02006GL028260, 2007. </mixed-citation>
</ref>
<ref id="ref37">
<label>37</label><mixed-citation publication-type="other" xlink:type="simple"> Wex, H., Petters, M. D., Carrico, C. M., Hallbauer, E., Massling, A., McMeeking, G. R., Poulain, L., Wu, Z., Kreidenweis, S. M., and Stratmann, F.: Towards Closing the Gap between Hygroscopic Growth and Activation for Secondary Organic Aerosol: Part I – Evidence from Measurements, Atmos. Chem. Phys. Discuss., 9, 955–989, 2009. </mixed-citation>
</ref>
<ref id="ref38">
<label>38</label><mixed-citation publication-type="other" xlink:type="simple"> Wex, H., F. Stratmann, D. Topping and G. McFiggans: The Kelvin versus the Raoult term in the Köhler equation, J. Atmos. Sci., in press, 2008b. </mixed-citation>
</ref>
<ref id="ref39">
<label>39</label><mixed-citation publication-type="other" xlink:type="simple"> Ziese, M., Wex, H., Nilsson, E. D., Salma, I., Ocskay, R., Hennig, T., Massling, A., and Stratmann, F.: Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles, Atmos. Chem. Phys., 8, 1855–1866, 2008. </mixed-citation>
</ref>
</ref-list>
</back>
</article>