<?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-9-5107-2009</article-id>
<title-group>
<article-title>In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>El Haddad</surname>
<given-names>I.</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>Yao Liu</surname>
<given-names></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>Nieto-Gligorovski</surname>
<given-names>L.</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>Michaud</surname>
<given-names>V.</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>Temime-Roussel</surname>
<given-names>B.</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>Quivet</surname>
<given-names>E.</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>Marchand</surname>
<given-names>N.</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>Sellegri</surname>
<given-names>K.</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>Monod</surname>
<given-names>A.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>Universités d&apos;Aix-Marseille I, II et III – CNRS, UMR 6264: Laboratoire Chimie Provence, Equipe: IRA, 3 place Victor Hugo, 13331 Marseilles Cedex 3, France</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Laboratoire de Météorologie Physique (UMR 6016), Observatoire de Physique du Globe de Clermont-Ferrand, Université Blaise Pascal, 24 avenue des Landais, 63177 Aubière, France</addr-line>
</aff>
<pub-date pub-type="epub">
<day>28</day>
<month>07</month>
<year>2009</year>
</pub-date>
<volume>9</volume>
<issue>14</issue>
<fpage>5107</fpage>
<lpage>5117</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/9/5107/2009/acp-9-5107-2009.html">This article is available from http://www.atmos-chem-phys.net/9/5107/2009/acp-9-5107-2009.html</self-uri>
<self-uri xlink:href="http://www.atmos-chem-phys.net/9/5107/2009/acp-9-5107-2009.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys.net/9/5107/2009/acp-9-5107-2009.pdf</self-uri>
<abstract>
<p>The fate of methacrolein in cloud evapo-condensation cycles was
experimentally investigated. To this end, aqueous-phase reactions of
methacrolein with OH radicals were performed (as described in Liu et al.,
2009), and the obtained solutions were then nebulized and dried into a
mixing chamber. ESI-MS and ESI-MS/MS analyses of the aqueous phase
composition denoted the formation of high molecular weight multifunctional
products containing hydroxyl, carbonyl and carboxylic acid moieties. The
time profiles of these products suggest that their formation can imply
radical pathways. These high molecular weight organic products are certainly
responsible for the formation of secondary organic aerosol (SOA) observed
during the nebulization experiments. The size, number and mass concentration
of these particles increased significantly with the reaction time: after 22 h
of reaction, the aerosol mass concentration was about three orders of
magnitude higher than the initial aerosol quantity. The evaluated SOA yield
ranged from 2 to 12%. These yields were confirmed by another estimation
method based on the hygroscopic and volatility properties of the obtained
SOA measured and reported by Michaud et al. (2009). These results
provide, for the first time to our knowledge, strong experimental evidence
that cloud processes can act, through photooxidation reactions, as important
contributors to secondary organic aerosol formation in the troposphere.</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"> % vor jede Referenz Altieri, K. E., Carlton, A. G., Lim, H., Turpin, B. J., and Seitzinger, S. P.: Evidence for Oligomer Formation in Clouds: Reactions of Isoprene Oxidation Products. Environ. Sci. Technol., 40, 4956–4960, 2006. </mixed-citation>
</ref>
<ref id="ref2">
<label>2</label><mixed-citation publication-type="other" xlink:type="simple"> Altieri, K. E., Seitzinger, S. P., Carlton, A. G., Turpin, B. J., Klein, G. C., and Marshall, A. G.: Oligomers formed through in-cloud methylglyoxal reactions: Chemical composition, properties, and mechanisms investigated by ultra-high resolution FT-ICR mass spectrometry, Atmos. Environ., 42, 1476–1490, 2008. </mixed-citation>
</ref>
<ref id="ref3">
<label>3</label><mixed-citation publication-type="other" xlink:type="simple"> Blando, J. D. and Turpin, B. J.: Secondary organic aerosol formation in cloud and fog droplets: a literature evaluation of plausibility, Atmos. Environ., 34, 1623–1632, 2000. </mixed-citation>
</ref>
<ref id="ref4">
<label>4</label><mixed-citation publication-type="other" xlink:type="simple"> Carlton, A. G., Turpin, B. J., Lim, H., Altieri, K. E., and Seitzinger, S.: Link between isoprene and secondary organic aerosol (SOA): pyruvic acid oxidation yields low volatility organic acids in clouds, Geophys. Res. Lett., 33, L06822/1–L06822/4, doi:10.1029/2005GL025374, 2006. </mixed-citation>
</ref>
<ref id="ref5">
<label>5</label><mixed-citation publication-type="other" xlink:type="simple"> Carlton, A. G., Turpin, B. J., Altieri, K. E., Seitzinger, S., Reff, A., Lim, H., and Ervens, B.: Atmospheric oxalic acid and SOA production from glyoxal: Results of aqueous photooxidation experiments, Atmos. Environ., 41, 7588–7602, 2007. </mixed-citation>
</ref>
<ref id="ref6">
<label>6</label><mixed-citation publication-type="other" xlink:type="simple"> Claeys, M., Graham, B., Vas, G., Wang, W., Vermeylen, R., Pashynska, V., Cafmeyer, J., Guyon, P., Andreae, M. O., Artaxo, P., and Maenhaut, W.: Formation of Secondary Organic Aerosols Through Photooxidation of Isoprene, Science (Washington DC, USA), 303, 1173–1176, 2004a </mixed-citation>
</ref>
<ref id="ref7">
<label>7</label><mixed-citation publication-type="other" xlink:type="simple"> Claeys, M., Wang, W., Ion, A. C., Kourtchev, I., Gelencser, A., and Maenhaut, W.: Formation of secondary organic aerosols from isoprene and its gas-phase oxidation products through reaction with hydrogen peroxide, Atmos. Environ., 38, 4093–4098, 2004b. </mixed-citation>
</ref>
<ref id="ref8">
<label>8</label><mixed-citation publication-type="other" xlink:type="simple"> Dommen, J., Metzger, A., Duplissy, J., Kalberer, M., Alfarra, M. R., Gascho, A., Weingartner, E., Prevot, A. S. H., Verheggen, B., and Baltensperger, U.: Laboratory observation of oligomers in the aerosol from isoprene/NO&lt;sub&gt;x&lt;/sub&gt; photooxidation, Geophys. Res. Lett., 33, L13805/1–L13805/5, doi:10.1029/2006GL026523, 2006. </mixed-citation>
</ref>
<ref id="ref9">
<label>9</label><mixed-citation publication-type="other" xlink:type="simple"> Dron, J., Eyglunent, G., Temime-Roussel, B., Marchand, N., and Wortham, H.: Carboxylic acid functional group analysis using constant neutral loss scanning-mass spectrometry, Anal. Chim. Acta, 605, 61–69, 2007. </mixed-citation>
</ref>
<ref id="ref10">
<label>10</label><mixed-citation publication-type="other" xlink:type="simple"> Edney, E. O., Kleindienst, T. E., Jaoui, M., Lewandowski, M., Offenberg, J. H., Wang, W., and Claeys, M.: Formation of 2-methyl tetrols and 2-methylglyceric acid in secondary organic aerosol from laboratory irradiated isoprene/NO&lt;sub&gt;x&lt;/sub&gt;/SO&lt;sub&gt;2&lt;/sub&gt;/air mixtures and their detection in ambient PM$_2.5$ samples collected in the eastern United States, Atmos. Environ., 39, 5281–5289, 2005. </mixed-citation>
</ref>
<ref id="ref11">
<label>11</label><mixed-citation publication-type="other" xlink:type="simple"> Ervens, B., George, C., Williams, J. E., Buxton, G. V., Salmon, G. A., Bydder, M., Wilkinson, F., Dentener, F., Mirabel, P., Wolke, R., and Herrmann, H.: CAPRAM2.4 (MODAC mechanism): An extended and condensed tropospheric aqueous phase mechanism and its application, J. Geophys. Res., 108(D14), 4426, doi:10.1029/2002JD002202, 2003. </mixed-citation>
</ref>
<ref id="ref12">
<label>12</label><mixed-citation publication-type="other" xlink:type="simple"> Ervens, B., Feingold, G., Frost, G. J., and Kreidenweis, S. M.: A modelling study of aqueous production of dicarboxylic acids, Part 1: Chemical pathways and organic mass production, J. Geophys. Res., 109, D15205, doi:10.1029/2003JD004387, 2004a. </mixed-citation>
</ref>
<ref id="ref13">
<label>13</label><mixed-citation publication-type="other" xlink:type="simple"> Ervens, B., Feingold, G., Clegg, S. L., and Kreidenweis, S. M.: A modelling study of aqueous production of dicarboxylic acids, Part 2: Impact on cloud microphysics, J. Geophys. Res., 109, D15206, doi:10.1029/2003JD004575, 2004b. </mixed-citation>
</ref>
<ref id="ref14">
<label>14</label><mixed-citation publication-type="other" xlink:type="simple"> Ervens, B., Carlton, A. G., Turpin, B. J., Altieri, K. E., Kreidensweis, S. M., and Feingold, G.: Secondary organic aerosol yields from cloud-processing of isoprene oxidation products, Geophys. Res. Lett., 35, L02816/1–L02816/5, doi:10.1029/2007GL031828, 2008. </mixed-citation>
</ref>
<ref id="ref15">
<label>15</label><mixed-citation publication-type="other" xlink:type="simple"> Gelencsér, and Varga, Z.: Evaluation of the atmospheric significance of multiphase reactions in atmospheric secondary organic aerosol formation, Atmos. Chem. Phys., 5, 2823–2831, 2005. </mixed-citation>
</ref>
<ref id="ref16">
<label>16</label><mixed-citation publication-type="other" xlink:type="simple"> Guzmán, M. I., Colussi, A. I., and Hoffmann, M. R.: Photoinduced oligomerization of aqueous pyruvic acid, J. Phys. Chem. A, 110, 3619–3626, 2006. </mixed-citation>
</ref>
<ref id="ref17">
<label>17</label><mixed-citation publication-type="other" xlink:type="simple"> Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, 2005. </mixed-citation>
</ref>
<ref id="ref18">
<label>18</label><mixed-citation publication-type="other" xlink:type="simple"> Kawamura, K. and Sakaguchi, F.: Molecular distributions of water soluble dicarboxylic acids in marine aerosols over the Pacific Ocean including tropics. J. Geophys. Res., 104(D3), 3501–3509, 1999. </mixed-citation>
</ref>
<ref id="ref19">
<label>19</label><mixed-citation publication-type="other" xlink:type="simple"> Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C., and Seinfeld, J. H.: Secondary Organic Aerosol Formation from Isoprene Photooxidation, Environ. Sci. Technol., 40, 1869–1877, 2006. </mixed-citation>
</ref>
<ref id="ref20">
<label>20</label><mixed-citation publication-type="other" xlink:type="simple"> Lee, W., Baasandorj, M., Stevens P. S., and Hites, R. A.: Monitoring OH-Initiated Oxidation Kinetics of Isoprene and Its Products Using Online Mass Spectrometry, Environ. Sci. Technol., 39, 1030–1036, 2005. </mixed-citation>
</ref>
<ref id="ref21">
<label>21</label><mixed-citation publication-type="other" xlink:type="simple"> Liao, H., Adams, P. J., Seinfeld, J. H., Mickley, L. J., and Jacob, D. J.: Interactions between tropospheric chemistry and aerosols in a unified GCM simulation, J. Geophys. Res., 108(D1), 4001, doi:10.1029/2001JD001260, 2003. </mixed-citation>
</ref>
<ref id="ref22">
<label>22</label><mixed-citation publication-type="other" xlink:type="simple"> Lim H., Carlton A. G., and Turpin B. J.: Isoprene forms secondary organic aerosol through cloud processing: model simulations. Environ. Sci. Technol., 39, 4441–4446, 2005. </mixed-citation>
</ref>
<ref id="ref23">
<label>23</label><mixed-citation publication-type="other" xlink:type="simple"> Liu, Yao, El Haddad, I., Scarfogliero, M., Nieto-Gligorovski, L., Temime-Roussel, B., Quivet, E., Marchand, N., Picquet-Varrault, B., and Monod, A.: In-cloud processes of methacrolein under simulated conditions – Part 1: Aqueous phase photooxidation, Atmos. Chem. Phys., 9, 5093–5105, 2009. </mixed-citation>
</ref>
<ref id="ref24">
<label>24</label><mixed-citation publication-type="other" xlink:type="simple"> Loeffler, K. W., Koehler, C. A., Paul, N. M., and De Haan, D. O.: Oligomer formation in evaporating aqueous glyoxal and methyl glyoxal solutions, Environ. Sci. Technol., 40, 6318–6323, 2006. </mixed-citation>
</ref>
<ref id="ref25">
<label>25</label><mixed-citation publication-type="other" xlink:type="simple"> Michaud, V., El Haddad, I., Liu, Yao, Sellegri, K., Laj, P., Villani, P., Picard, D., Marchand, N., and Monod, A.: In-cloud processes of methacrolein under simulated conditions – Part 3: Hygroscopic and volatility properties of the formed secondary organic aerosol, Atmos. Chem. Phys., 9, 5119–5130, 2009. </mixed-citation>
</ref>
<ref id="ref26">
<label>26</label><mixed-citation publication-type="other" xlink:type="simple"> Monod, A., Chebbi, A., Durand-Jolibois, R., and Carlier, P.: Oxidation of methanol by hydroxyl radicals in aqueous solution under simulated cloud droplet conditions, Atmos. Environ., 34, 5283–5294, 2000. </mixed-citation>
</ref>
<ref id="ref27">
<label>27</label><mixed-citation publication-type="other" xlink:type="simple"> Müller, J.-F., Stavrakou, T., Wallens, S., De Smedt, I., Van Roozendael, M., Potosnak, M. J., Rinne, J., Munger, B., Goldstein, A., and Guenther, A. B.: Global isoprene emissions estimated using MEGAN, ECMWF analyses and a detailed canopy environment model, Atmos. Chem. Phys., 8, 1329–1341, 2008. </mixed-citation>
</ref>
<ref id="ref28">
<label>28</label><mixed-citation publication-type="other" xlink:type="simple"> Paulsen, D., Weingartner, E., Alfarra, M. R., and Baltensperger, U.: Volatility measurements of photochemically and nebulizer-generated organic aerosol particles, J. Aerosol Sci., 37, 1025–1051, 2006. </mixed-citation>
</ref>
<ref id="ref29">
<label>29</label><mixed-citation publication-type="other" xlink:type="simple"> Poulain, L., Monod, A., and Wortham, H.: Development of a new on-line mass spectrometer to study the reactivity of soluble organic compounds in the aqueous phase under tropospheric conditions: Application to OH-oxidation of N-methylpyrrolidone, J. Photoch. Photobio. A, 187, 10–23, 2007. </mixed-citation>
</ref>
<ref id="ref30">
<label>30</label><mixed-citation publication-type="other" xlink:type="simple"> Sempere, R. and Kawamura, K.: Low molecular weight dicarboxylic acids and related polar compounds in the remote marine rain samples collected from western Pacific, Atmos. Environ., 30, 1609–1619, 1996. </mixed-citation>
</ref>
<ref id="ref31">
<label>31</label><mixed-citation publication-type="other" xlink:type="simple"> Sokal, R. R. and Rohlf, F. J.: Biometry, 2 ed., Freeman, New York, USA, 1981. </mixed-citation>
</ref>
<ref id="ref32">
<label>32</label><mixed-citation publication-type="other" xlink:type="simple"> Surratt, J. D., Murphy, S. M., Kroll, J. H., Ng, N. L., Hildebrandt, L., Sorooshian, A., Szmigielski, R., Vermeylen, R., Maenhaut, W., Claeys, M., Flagan, R. C., and Seinfeld, J. H.: Chemical Composition of Secondary Organic Aerosol Formed from the Photooxidation of Isoprene, J. Phys. Chem. A, 110, 9665–9690, 2006. </mixed-citation>
</ref>
<ref id="ref33">
<label>33</label><mixed-citation publication-type="other" xlink:type="simple"> van Pinxteren, D., Plewka, A., Hofmann, D., Mueller, K.; Kramberger, H., Svrcina, B., Baechmann, K., Jaeschke, W., Mertes, S., Collett, J. L., and Herrmann, H.: Schmuecke hill cap cloud and valley stations aerosol characterisation during FEBUKO (II): Organic compounds, Atmos. Environ., 39, 4305–4320, 2005. </mixed-citation>
</ref>
</ref-list>
</back>
</article>