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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-5-863-2005</article-id>
<title-group>
<article-title>Sulphuric acid closure and contribution to nucleation mode particle growth</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Boy</surname>
<given-names>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>Kulmala</surname>
<given-names>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>Ruuskanen</surname>
<given-names>T. 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>Pihlatie</surname>
<given-names>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>Reissell</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>Aalto</surname>
<given-names>P. 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>Keronen</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>Dal Maso</surname>
<given-names>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>Hellen</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>Hakola</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>Jansson</surname>
<given-names>R.</given-names>
</name>
<xref ref-type="aff" rid="aff3">
<sup>3</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Hanke</surname>
<given-names>M.</given-names>
</name>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Arnold</surname>
<given-names>F.</given-names>
</name>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>University of Helsinki, Dept. Physical Sciences, P.O. Box 64, FIN-00014 Univ. of Helsinki, Finland</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Finnish Meteorological Institute, Air Quality Research, Sahaajankatu 20 E, FIN-00880 Helsinki, Finland</addr-line>
</aff>
<aff id="aff3">
<label>3</label>
<addr-line>Stockholm University (ITML), Air Pollution Laboratory, Institute for Applied Environmental Research, Stockholm University, S-10691 Stockholm, Sweden</addr-line>
</aff>
<aff id="aff4">
<label>4</label>
<addr-line>Atmospheric Physics Division, Max-Planck Institute for Nuclear Physics, (MPIK), P.O. Box 103980, D-69029 Heidelberg, Germany</addr-line>
</aff>
<pub-date pub-type="epub">
<day>16</day>
<month>03</month>
<year>2005</year>
</pub-date>
<volume>5</volume>
<issue>4</issue>
<fpage>863</fpage>
<lpage>878</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/5/863/2005/acp-5-863-2005.html">This article is available from http://www.atmos-chem-phys.net/5/863/2005/acp-5-863-2005.html</self-uri>
<self-uri xlink:href="http://www.atmos-chem-phys.net/5/863/2005/acp-5-863-2005.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys.net/5/863/2005/acp-5-863-2005.pdf</self-uri>
<abstract>
<p>Sulphuric acid concentrations were measured and calculated based on pseudo
steady state model with corresponding measurements of CO, NO&lt;sub&gt;x&lt;/sub&gt;, O&lt;sub&gt;3&lt;/sub&gt;,
SO&lt;sub&gt;2&lt;/sub&gt;, methane and non-methane hydrocarbon (NMHC) concentrations as well
as solar spectral irradiance and particle number concentrations with size
distributions. The measurements were performed as a part of the EU project
QUEST (Quantification of Aerosol Nucleation in the European Boundary layer)
during an intensive field campaign, which was conducted in Hyyti&amp;#228;l&amp;#228;,
Finland in March&amp;ndash;April 2003. In this paper, the closure between measured and
calculated H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; concentrations is investigated. Besides that,
also the contribution of sulphuric acid to nucleation mode particle growth
rates is studied. Hydroxyl and hydroperoxy radical concentrations were
determined using a pseudo steady state box model including photo stationary
states. The maximum midday OH concentrations ranged between 4.1&amp;times;10&lt;sup&gt;5&lt;/sup&gt; to
1.8&amp;times;10&lt;sup&gt;6&lt;/sup&gt; molecules&amp;nbsp;cm&lt;sup&gt;-3&lt;/sup&gt; and the corresponding values for HO&lt;sub&gt;2&lt;/sub&gt;
were 1.0&amp;times;10&lt;sup&gt;7&lt;/sup&gt; to 1.5&amp;times;10&lt;sup&gt;8&lt;/sup&gt; molecules&amp;nbsp;cm&lt;sup&gt;-3&lt;/sup&gt;.
The dominant source
term for hydroxyl radicals is the reaction of NO with HO&lt;sub&gt;2&lt;/sub&gt; (56%) and
the reaction of CO with OH covers around 41% of the sinks. The sulphuric
acid source term is the reaction SO&lt;sub&gt;2&lt;/sub&gt; with OH and the sink term is
condensation of sulphuric acid. The closure between measured and calculated
sulphuric acid concentrations is achieved with a high agreement to the
measured values. In sensitivity studies, we used different values for the
non-methane hydrocarbons, the peroxy radicals and nitrogen dioxide. The best
fits between calculated and measured values were found by decreasing the
NO&lt;sub&gt;2&lt;/sub&gt; concentration when it exceeded values of 1.5 ppb and doubling the
non-methane hydrocarbon concentrations. The ratio, standard deviation and
correlation coefficient between measured and calculated sulphuric acid
concentrations are 0.99, 0.412 and 0.645, respectively. The maximum midday
sulphuric acid concentrations varied between 3&amp;times;10&lt;sup&gt;5&lt;/sup&gt; to
1.9&amp;times;10&lt;sup&gt;7&lt;/sup&gt; molecules&amp;nbsp;cm&lt;sup&gt;-3&lt;/sup&gt; for the measurements and
3&amp;times;10&lt;sup&gt;5&lt;/sup&gt; to 1.4&amp;times;10&lt;sup&gt;7&lt;/sup&gt; molecules&amp;nbsp;cm&lt;sup&gt;-3&lt;/sup&gt;
for the calculations, respectively. An average
participation of sulphuric acid to the nucleation mode particle growth rates
is 8.8%. Classifying the days into two groups &amp;ndash; &apos;&apos;polluted&apos;&apos; days with
air masses originated over Central Europe or UK, and &apos;&apos;cleaner&apos;&apos; days with
air masses originated over the Northern Atlantic or the Polar regions &amp;ndash;
reflects an equal sulphuric acid contribution to the aerosol growth in both
air mass classes.</p>
</abstract>
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