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<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-3-1509-2003</article-id>
<title-group>
<article-title>Contribution of gaseous and particulate species to droplet solute composition at the Puy de Dôme, France</article-title>
</title-group>
<contrib-group><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="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Laj</surname>
<given-names>P.</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>Marinoni</surname>
<given-names>A.</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>Dupuy</surname>
<given-names>R.</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>Legrand</surname>
<given-names>M.</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>Preunkert</surname>
<given-names>S.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>Laboratoire de Meteorologie Physique, CNRS, Université Blaise Pascal, 24, av; des landais 63 177 Aubiere cedex, France</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Laboratoire de Glaciologie et Géophysique de l’Environnement, 54, rue Molière, 38402 St Martin d’Hères cedex, France</addr-line>
</aff>
<pub-date pub-type="epub">
<day>26</day>
<month>09</month>
<year>2003</year>
</pub-date>
<volume>3</volume>
<issue>5</issue>
<fpage>1509</fpage>
<lpage>1522</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/3/1509/2003/acp-3-1509-2003.html">This article is available from http://www.atmos-chem-phys.net/3/1509/2003/acp-3-1509-2003.html</self-uri>
<self-uri xlink:href="http://www.atmos-chem-phys.net/3/1509/2003/acp-3-1509-2003.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys.net/3/1509/2003/acp-3-1509-2003.pdf</self-uri>
<abstract>
<p>Chemical reactions of dissolved gases in the liquid phase play a key role in atmospheric
      processes both in the formation of secondary atmospheric compounds and their wet removal
      rate but also in the regulation of the oxidizing capacity of the troposphere. The behavior of
      gaseous species and their chemical transformation in clouds are difficult to observe
      experimentally given the complex nature of clouds.&lt;br&gt;
      &lt;br&gt;
      During a winter field campaign at the summit of the Puy de Dôme (central France,
      1465 m a.s.l), we have deployed an experimental set-up to provide a quantification of phase
      partitioning of both organic (CH&lt;sub&gt;3&lt;/sub&gt;COOH, HCOOH, H&lt;sub&gt;2&lt;/sub&gt;C&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;4&lt;/sub&gt;) and inorganic
      (NH&lt;sub&gt;3&lt;/sub&gt;, HNO&lt;sub&gt;3&lt;/sub&gt;, SO&lt;sub&gt;2&lt;/sub&gt;, HCl) species in clouds.&lt;br&gt;
      &lt;br&gt;
      We found that nitric and hydrochloric acids can be considered close to Henry&apos;s law
      equilibrium, within analytical uncertainty and instrumental errors. On another hand, for
      NH&lt;sub&gt;3&lt;/sub&gt; and carboxylic acids, dissolution of material from the gas phase is kinetically limited and
      never reaches the equilibrium predicted by thermodynamics, resulting in significant
      sub-saturation of the liquid phase. On the contrary, S&lt;sup&gt;IV&lt;/sup&gt; is supersaturated in the liquid phase, in
      addition to the presence of significant aerosol-derived S&lt;sup&gt;VI &lt;/sup&gt; transferred through nucleation
      scavenging.&lt;br&gt;
      &lt;br&gt;
      Upon droplet evaporation, a significant part of most species, including S&lt;sup&gt;IV&lt;/sup&gt;, tends to
      efficiently return back into the gas phase. Overall, gas contribution to the droplet solute
      concentration ranges from at least 48.5 to 98% depending on the chemical species. This is
      particularly important considering that aerosol scavenging efficiencies are often calculated
      assuming a negligible gas-phase contribution to the solute concentration. Our study
      emphasizes the need to account for the in-cloud interaction between particles and gases to
      provide an adequate modeling of multiphase chemistry systems and its impact on the
      atmospheric aerosol and gas phases.</p>
</abstract>
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