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<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-5-3437-2005</article-id>
<title-group>
<article-title>A global off-line model of size-resolved aerosol microphysics: II. Identification of key uncertainties</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Spracklen</surname>
<given-names>D. V.</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>Pringle</surname>
<given-names>K. J.</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>Carslaw</surname>
<given-names>K. S.</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>Chipperfield</surname>
<given-names>M. 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>Mann</surname>
<given-names>G. W.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>Institute of Atmospheric Science, School of Earth and Environment, University of Leeds, UK</addr-line>
</aff>
<pub-date pub-type="epub">
<day>30</day>
<month>05</month>
<year>2005</year>
</pub-date>
<volume>5</volume>
<issue>3</issue>
<fpage>3437</fpage>
<lpage>3489</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>
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<self-uri xlink:href="http://www.atmos-chem-phys-discuss.net/5/3437/2005/acpd-5-3437-2005.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/5/3437/2005/acpd-5-3437-2005.pdf</self-uri>
<abstract>
<p>We use the new GLOMAP model of global aerosol microphysics to investigate the sensitivity of modelled sulfate and
sea salt aerosol properties to uncertainties in the driving microphysical processes and compare these
uncertainties with those associated with aerosol and precursor gas emissions. Overall, we conclude that
uncertainties in microphysical processes have a larger effect on global condensation nuclei (CN) and cloud
condensation nuclei (CCN) concentrations than uncertainties in present-day sulfur emissions. Our simulations
suggest that uncertainties in predicted sulfate and sea salt CCN abundances due to poorly constrained
microphysical processes are likely to be of a similar magnitude to long-term changes in CCN due to changes in
anthropogenic emissions. A microphysical treatment of the global sulfate aerosol allows the uncertainty in
climate-relevant aerosol properties to be attributed to specific processes in a way that has not been possible
with simpler aerosol schemes. In particular we conclude that: (1) changes in the binary H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-H&lt;sub&gt;2&lt;/sub&gt;O
nucleation rate and condensation rate of gaseous H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; cause a shift in the vertical location of the
upper tropospheric CN layer by as much as 3 km, while changes in absolute concentration are relatively small; (2)
uncertainties in the binary H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-H&lt;sub&gt;2&lt;/sub&gt;O nucleation rate have a relatively insignificant effect on boundary
layer aerosol properties; (3) production of sulfate particles in power plant plumes below the scale of the model
grid (which is of the order of 300 km) has the potential to change the global mean sulfate-derived CN
concentration by a factor 2 or more at the surface, and changes of up to a factor 20 can occur in polluted
regions; (4) predicted global mean sulfate and sea salt CCN concentrations change by 10 to 40% at the surface
when several microphysical processes are changed within reasonable uncertainty ranges; (5) CCN concentrations are
particularly sensitive to primary sulfate particle emissions, with global mean CCN changing by up to 40% and
local concentrations changing by more than 100% when the percentage of anthropogenic SO&lt;sub&gt;2&lt;/sub&gt; emitted as
particulates in plumes is changed from 0 to 5%; (6) uncertainties in CCN due to the mode of sulfate emission
(i.e., the fraction of sulfur emitted as primary particles) are larger than those (~15%) caused by a
&amp;plusmn;25% change in total sulfur emissions; (7) large changes in sea spray flux have insignificant effects on global
sulfate aerosol except when the mass accommodation coefficient of sulfuric acid on the salt particles is set
unrealistically low.</p>
</abstract>
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