PittsburghV1, France, Analysis, bibRecord, 000097

Effect of ions on sulfuric acid-water binary particle formation I: Theory for kinetic and nucleation-type particle formation and atmospheric implications

Identifieur interne : 000097 ( France/Analysis ); précédent : 000096; suivant : 000098

Effect of ions on sulfuric acid-water binary particle formation I: Theory for kinetic and nucleation-type particle formation and atmospheric implications

Auteurs : Joonas Merikanto [Finlande] ; Jonathan Duplissy [Finlande] ; Anni M Tt Nen [France] ; Henning Henschel [Finlande] ; Neil M. Donahue [États-Unis] ; David Brus [Finlande] ; Siegfried Schobesberger [États-Unis] ; Markku Kulmala [Finlande] ; Hanna Vehkam Ki [Finlande]

Source :

Journal of Geophysical Research: Atmospheres [ 2169-897X ] ; 2016.

RBID : Hal:insu-01240821

English descriptors

mix :
- classical nucleation theory, ion-induced nucleation, sulfuric acid, binary particle formation.

Abstract

We derive a version of Classical Nucleation Theory normalized by quantum chemical results on sulfuric acid-water hydration to describe neutral and ion-induced particle formation in the binary sulfuric acid-water system. The theory is extended to treat the kinetic regime where the nucleation free energy barrier vanishes at high sulfuric acid concentrations or low temperatures. In the kinetic regime particle formation rates become proportional to sulfuric acid concentration to second power in the neutral system or first power in the ion-induced system. We derive simple general expressions for the prefactors in kinetic-type and activation-type particle formation calculations applicable also to more complex systems stabilized by other species. The theory predicts that the binary water-sulfuric acid system can produce strong new particle formation in the free troposphere both through barrier crossing and through kinetic pathways. At cold stratospheric and upper free tropospheric temperatures neutral formation dominates the binary particle formation rates. At midtropospheric temperatures the ion-induced pathway becomes the dominant mechanism. However, even the ion-induced binary mechanism does not produce significant particle formation in warm boundary layer conditions, as it requires temperatures below 0°C to take place at atmospheric concentrations. The theory successfully reproduces the characteristics of measured charged and neutral binary particle formation in CERN CLOUD3 and CLOUD5 experiments, as discussed in a companion paper.

Url:

https://hal-insu.archives-ouvertes.fr/insu-01240821

DOI: 10.1002/2015JD023538

Affiliations:

Links toward previous steps (curation, corpus...)

to stream Hal, to step Corpus: 000222
to stream Hal, to step Curation: 000222
to stream Hal, to step Checkpoint: 000120
to stream Main, to step Merge: 000109
to stream Main, to step Curation: 000109
to stream Main, to step Exploration: 000109
to stream France, to step Extraction: 000097

Links to Exploration step

Hal:insu-01240821

Le document en format XML

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          <orgName type="acronym">FMI</orgName>
          <desc>            <address>              <addrLine>P.O. box 503,, FI-00101 Helsinki, Finlande</addrLine>
              <country key="FI"></country>
            </address>
            <ref type="url">http://en.ilmatieteenlaitos.fi</ref>
          </desc>
        </hal:affiliation>
<country>Finlande</country>
</affiliation>
</author>
<author><name sortKey="Schobesberger, Siegfried" sort="Schobesberger, Siegfried" uniqKey="Schobesberger S" first="Siegfried" last="Schobesberger">Siegfried Schobesberger</name>
<affiliation wicri:level="1"><hal:affiliation type="department" xml:id="struct-91318" status="VALID">          <orgName>Department of Atmospheric Sciences [Seattle]</orgName>
          <desc>            <address>              <addrLine>Seattle, Washington</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.atmos.washington.edu/</ref>
          </desc>
          <listRelation>            <relation active="#struct-300433" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-300433" type="direct"><org type="institution" xml:id="struct-300433" status="VALID">          <orgName>University of Washington [Seattle]</orgName>
          <desc>            <address>              <addrLine>Seattle, Washington 98105</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.washington.edu/</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
<author><name sortKey="Kulmala, Markku" sort="Kulmala, Markku" uniqKey="Kulmala M" first="Markku" last="Kulmala">Markku Kulmala</name>
<affiliation wicri:level="1"><hal:affiliation type="laboratory" xml:id="struct-61421" status="INCOMING">          <orgName>Department of Physics</orgName>
          <desc>            <address>              <country key="FI"></country>
            </address>
          </desc>
        </hal:affiliation>
<country>Finlande</country>
</affiliation>
</author>
<author><name sortKey="Vehkam Ki, Hanna" sort="Vehkam Ki, Hanna" uniqKey="Vehkam Ki H" first="Hanna" last="Vehkam Ki">Hanna Vehkam Ki</name>
<affiliation wicri:level="1"><hal:affiliation type="laboratory" xml:id="struct-61421" status="INCOMING">          <orgName>Department of Physics</orgName>
          <desc>            <address>              <country key="FI"></country>
            </address>
          </desc>
        </hal:affiliation>
<country>Finlande</country>
</affiliation>
</author>
</analytic>
<idno type="DOI">10.1002/2015JD023538</idno>
<series><title level="j">Journal of Geophysical Research: Atmospheres</title>
<idno type="ISSN">2169-897X</idno>
<imprint><date type="datePub">2016</date>
</imprint>
</series>
</biblStruct>
</sourceDesc>
</fileDesc>
<profileDesc><textClass><keywords scheme="mix" xml:lang="en"><term> classical nucleation theory</term>
<term> ion-induced nucleation</term>
<term> sulfuric acid</term>
<term>binary particle formation</term>
</keywords>
</textClass>
</profileDesc>
</teiHeader>
<front><div type="abstract" xml:lang="en">We derive a version of Classical Nucleation Theory normalized by quantum chemical results on sulfuric acid-water hydration to describe neutral and ion-induced particle formation in the binary sulfuric acid-water system. The theory is extended to treat the kinetic regime where the nucleation free energy barrier vanishes at high sulfuric acid concentrations or low temperatures. In the kinetic regime particle formation rates become proportional to sulfuric acid concentration to second power in the neutral system or first power in the ion-induced system. We derive simple general expressions for the prefactors in kinetic-type and activation-type particle formation calculations applicable also to more complex systems stabilized by other species. The theory predicts that the binary water-sulfuric acid system can produce strong new particle formation in the free troposphere both through barrier crossing and through kinetic pathways. At cold stratospheric and upper free tropospheric temperatures neutral formation dominates the binary particle formation rates. At midtropospheric temperatures the ion-induced pathway becomes the dominant mechanism. However, even the ion-induced binary mechanism does not produce significant particle formation in warm boundary layer conditions, as it requires temperatures below 0°C to take place at atmospheric concentrations. The theory successfully reproduces the characteristics of measured charged and neutral binary particle formation in CERN CLOUD3 and CLOUD5 experiments, as discussed in a companion paper.</div>
</front>
</TEI>
<affiliations><list><country><li>Finlande</li>
<li>France</li>
<li>États-Unis</li>
</country>
<region><li>Île-de-France</li>
</region>
<settlement><li>Versailles</li>
</settlement>
<orgName><li>Université de Versailles-Saint-Quentin-en-Yvelines</li>
</orgName>
</list>
<tree><country name="Finlande"><noRegion><name sortKey="Merikanto, Joonas" sort="Merikanto, Joonas" uniqKey="Merikanto J" first="Joonas" last="Merikanto">Joonas Merikanto</name>
</noRegion>
<name sortKey="Brus, David" sort="Brus, David" uniqKey="Brus D" first="David" last="Brus">David Brus</name>
<name sortKey="Duplissy, Jonathan" sort="Duplissy, Jonathan" uniqKey="Duplissy J" first="Jonathan" last="Duplissy">Jonathan Duplissy</name>
<name sortKey="Henschel, Henning" sort="Henschel, Henning" uniqKey="Henschel H" first="Henning" last="Henschel">Henning Henschel</name>
<name sortKey="Kulmala, Markku" sort="Kulmala, Markku" uniqKey="Kulmala M" first="Markku" last="Kulmala">Markku Kulmala</name>
<name sortKey="Vehkam Ki, Hanna" sort="Vehkam Ki, Hanna" uniqKey="Vehkam Ki H" first="Hanna" last="Vehkam Ki">Hanna Vehkam Ki</name>
</country>
<country name="France"><region name="Île-de-France"><name sortKey="M Tt Nen, Anni" sort="M Tt Nen, Anni" uniqKey="M Tt Nen A" first="Anni" last="M Tt Nen">Anni M Tt Nen</name>
</region>
</country>
<country name="États-Unis"><noRegion><name sortKey="Donahue, Neil M" sort="Donahue, Neil M" uniqKey="Donahue N" first="Neil M." last="Donahue">Neil M. Donahue</name>
</noRegion>
<name sortKey="Schobesberger, Siegfried" sort="Schobesberger, Siegfried" uniqKey="Schobesberger S" first="Siegfried" last="Schobesberger">Siegfried Schobesberger</name>
</country>
</tree>
</affiliations>
</record>

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Effect of ions on sulfuric acid-water binary particle formation I: Theory for kinetic and nucleation-type particle formation and atmospheric implications

Effect of ions on sulfuric acid-water binary particle formation I: Theory for kinetic and nucleation-type particle formation and atmospheric implications

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