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<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">ACPD</journal-id>
<journal-title-group>
<journal-title>Atmospheric Chemistry and Physics Discussions</journal-title>
<abbrev-journal-title abbrev-type="publisher">ACPD</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1680-7375</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/acpd-6-701-2006</article-id>
<title-group>
<article-title>20th Century trends and budget implications of trihalomethanes and dihalomethanes inferred from North GRIP firn air</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Worton</surname>
<given-names>D. 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>Sturges</surname>
<given-names>W. T.</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>Schwander</surname>
<given-names>J.</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>Mulvaney</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>Barnola</surname>
<given-names>J.-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>Chappellaz</surname>
<given-names>J.</given-names>
</name>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Physics Institute, University of Berne, Berne, Switzerland</addr-line>
</aff>
<aff id="aff3">
<label>3</label>
<addr-line>British Antarctic Survey, Natural Environment Research Council, Cambridge, UK</addr-line>
</aff>
<aff id="aff4">
<label>4</label>
<addr-line>CNRS Laboratoire de Glaciologie et Geophysique de l’Environnement, Saint Martin d’Heres, France</addr-line>
</aff>
<pub-date pub-type="epub">
<day>24</day>
<month>01</month>
<year>2006</year>
</pub-date>
<volume>6</volume>
<issue>1</issue>
<fpage>701</fpage>
<lpage>754</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-discuss.net/6/701/2006/acpd-6-701-2006.html">This article is available from http://www.atmos-chem-phys-discuss.net/6/701/2006/acpd-6-701-2006.html</self-uri>
<self-uri xlink:href="http://www.atmos-chem-phys-discuss.net/6/701/2006/acpd-6-701-2006.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/6/701/2006/acpd-6-701-2006.pdf</self-uri>
<abstract>
<p>Four trihalomethane (THM; CHCl&lt;sub&gt;3&lt;/sub&gt;, CHBrCl&lt;sub&gt;2&lt;/sub&gt;, CHBr&lt;sub&gt;2&lt;/sub&gt;Cl and
CHBr&lt;sub&gt;3&lt;/sub&gt;) and two dihalomethane (DHM; CH&lt;sub&gt;2&lt;/sub&gt;BrCl and CH&lt;sub&gt;2&lt;/sub&gt;Br&lt;sub&gt;2&lt;/sub&gt;)
trace gases have been measured in air extracted from polar firn collected at
the North Greenland Icecore Project (NGRIP) site. CHCl&lt;sub&gt;3&lt;/sub&gt; was also
measured in firn air from Devon Island (DI), Canada, Dronning Maud Land
(DML), Antarctica and Dome Concordia (Dome C), Antarctica. All of these
species are believed to be almost entirely of natural origin except for
CHCl&lt;sub&gt;3&lt;/sub&gt; where anthropogenic sources have been reported to contribute
~10% to the global burden. A 2-D atmospheric model was run for
CHCl&lt;sub&gt;3&lt;/sub&gt; using reported emission estimates to produce historical
atmospheric trends at the three firn sites, which were then input into a
firn diffusion model to produce concentration depth profiles that were
compared against the measurements. The anthropogenic emissions were modified
in order to give the best model fit to the firn data at NGRIP, Dome C and
DML. As a result, the contribution of CHCl&lt;sub&gt;3&lt;/sub&gt; from anthropogenic sources,
mainly from pulp and paper manufacture, to the total chloroform budget
appears to have been considerably underestimated and was likely to have been
close to ~40% at the maximum in atmospheric CHCl&lt;sub&gt;3&lt;/sub&gt;
concentrations around 1990, declining to ~19% at the beginning of
the 21st Century. We also show that the atmospheric burden of the
brominated THM&apos;s in the northern hemisphere have increased over the
20th Century while CH&lt;sub&gt;2&lt;/sub&gt;Br&lt;sub&gt;2&lt;/sub&gt; has remained constant over time
implying that it is entirely of natural origin.</p>
</abstract>
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