The dynamic surface tension of atmospheric aerosol surfactants reveals new aspects of cloud activation
Identifieur interne : 000106 ( Pmc/Curation ); précédent : 000105; suivant : 000107The dynamic surface tension of atmospheric aerosol surfactants reveals new aspects of cloud activation
Auteurs : Barbara Nozière [Suède, France] ; Christine Baduel [Suède, Australie] ; Jean-Luc Jaffrezo [France]Source :
- Nature Communications [ 2041-1723 ] ; 2014.
Abstract
The activation of aerosol particles into cloud droplets in the Earth’s atmosphere is both a key process for the climate budget and a main source of uncertainty. Its investigation is facing major experimental challenges, as no technique can measure the main driving parameters, the Raoult’s term and surface tension,
Url:
DOI: 10.1038/ncomms4335
PubMed: 24566451
PubMed Central: 3948073
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<front><div type="abstract" xml:lang="en"><p>The activation of aerosol particles into cloud droplets in the Earth’s atmosphere is both a key process for the climate budget and a main source of uncertainty. Its investigation is facing major experimental challenges, as no technique can measure the main driving parameters, the Raoult’s term and surface tension, <italic>σ</italic>
, for sub-micron atmospheric particles. In addition, the surfactant fraction of atmospheric aerosols could not be isolated until recently. Here we present the first dynamic investigation of the total surfactant fraction of atmospheric aerosols, evidencing adsorption barriers that limit their gradient (partitioning) in particles and should enhance their cloud-forming efficiency compared with current models. The results also show that the equilibration time of surfactants in sub-micron atmospheric particles should be beyond the detection of most on-line instruments. Such instrumental and theoretical shortcomings would be consistent with atmospheric and laboratory observations and could have limited the understanding of cloud activation until now.</p>
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<front><journal-meta><journal-id journal-id-type="nlm-ta">Nat Commun</journal-id>
<journal-id journal-id-type="iso-abbrev">Nat Commun</journal-id>
<journal-title-group><journal-title>Nature Communications</journal-title>
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<issn pub-type="epub">2041-1723</issn>
<publisher><publisher-name>Nature Pub. Group</publisher-name>
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<article-meta><article-id pub-id-type="pmid">24566451</article-id>
<article-id pub-id-type="pmc">3948073</article-id>
<article-id pub-id-type="pii">ncomms4335</article-id>
<article-id pub-id-type="doi">10.1038/ncomms4335</article-id>
<article-categories><subj-group subj-group-type="heading"><subject>Article</subject>
</subj-group>
</article-categories>
<title-group><article-title>The dynamic surface tension of atmospheric aerosol surfactants reveals new aspects of cloud activation</article-title>
</title-group>
<contrib-group><contrib contrib-type="author"><name><surname>Nozière</surname>
<given-names>Barbara</given-names>
</name>
<xref ref-type="corresp" rid="c1">a</xref>
<xref ref-type="aff" rid="a1">1</xref>
<xref ref-type="aff" rid="a3">3</xref>
</contrib>
<contrib contrib-type="author"><name><surname>Baduel</surname>
<given-names>Christine</given-names>
</name>
<xref ref-type="aff" rid="a1">1</xref>
<xref ref-type="aff" rid="a4">4</xref>
</contrib>
<contrib contrib-type="author"><name><surname>Jaffrezo</surname>
<given-names>Jean-Luc</given-names>
</name>
<xref ref-type="aff" rid="a2">2</xref>
</contrib>
<aff id="a1"><label>1</label>
<institution>Stockholm University, Department of Applied Environmental Science (ITM)</institution>
, Svante Arrhenius väg 8, Stockholm 106 91,<country>Sweden</country>
</aff>
<aff id="a2"><label>2</label>
<institution>Université Joseph Fourier-Grenoble 1/CNRS, Laboratoire de Glaciologie et Géophysique de l’Environnement UMR 5183</institution>
, Grenoble F-38041,<country>France</country>
</aff>
<aff id="a3"><label>3</label>
Present address: Institut de Recherches sur la Catalyse et l’Environnement de Lyon, UMR5256, CNRS and Université Claude Bernard Lyon 1, Villeurbanne 69626, France</aff>
<aff id="a4"><label>4</label>
Present address: The National Research Center for Environmental Toxicology, The University of Queensland, Brisbane, Queensland, Australia</aff>
</contrib-group>
<author-notes><corresp id="c1"><label>a</label>
<email>barbara.noziere@ircelyon.univ-lyon1.fr</email>
</corresp>
</author-notes>
<pub-date pub-type="epub"><day>25</day>
<month>02</month>
<year>2014</year>
</pub-date>
<volume>5</volume>
<elocation-id>3335</elocation-id>
<history><date date-type="received"><day>02</day>
<month>08</month>
<year>2013</year>
</date>
<date date-type="accepted"><day>28</day>
<month>01</month>
<year>2014</year>
</date>
</history>
<permissions><copyright-statement>Copyright © 2014, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.</copyright-statement>
<copyright-year>2014</copyright-year>
<copyright-holder>Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.</copyright-holder>
<license license-type="open-access" xlink:href="http://creativecommons.org/licenses/by-nc-nd/3.0/"><pmc-comment>author-paid</pmc-comment>
<license-p>This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivs 3.0 Unported License. To view a copy of this license, visit http://creativecommons.org/licenses/by-nc-nd/3.0/</license-p>
</license>
</permissions>
<abstract><p>The activation of aerosol particles into cloud droplets in the Earth’s atmosphere is both a key process for the climate budget and a main source of uncertainty. Its investigation is facing major experimental challenges, as no technique can measure the main driving parameters, the Raoult’s term and surface tension, <italic>σ</italic>
, for sub-micron atmospheric particles. In addition, the surfactant fraction of atmospheric aerosols could not be isolated until recently. Here we present the first dynamic investigation of the total surfactant fraction of atmospheric aerosols, evidencing adsorption barriers that limit their gradient (partitioning) in particles and should enhance their cloud-forming efficiency compared with current models. The results also show that the equilibration time of surfactants in sub-micron atmospheric particles should be beyond the detection of most on-line instruments. Such instrumental and theoretical shortcomings would be consistent with atmospheric and laboratory observations and could have limited the understanding of cloud activation until now.</p>
</abstract>
<abstract abstract-type="web-summary"><p><inline-graphic id="i1" xlink:href="ncomms4335-i1.jpg"></inline-graphic>
The formation of cloud droplets from aerosol particles in the atmosphere is difficult to comprehend experimentally and theoretically. Here, the authors measure the dynamic surface tension of atmospheric aerosols and evidence previously overlooked processes, likely to improve this understanding.</p>
</abstract>
</article-meta>
</front>
<floats-group><fig id="f1"><label>Figure 1</label>
<caption><title>Dynamic surface tension curves for the aerosol samples and reference compounds.</title>
<p>(<bold>a</bold>
) Curves obtained for surfactin (green), rhamnolipids (red) and SDS (blue), and the aerosol samples (black symbols): 4 June 2009 (diamonds), 7 July 2007 (circles), 16 July 2009 (pluses), 10 November 2009 (crosses), 20 November 2009 (squares) and 3 January 2010 (triangles) in water. (<bold>b</bold>
) Curves obtained by adding increasing amounts of NaCl to SDS solutions, 3.4 mM: no salt (white symbols), +4.2 mM NaCl (pale grey), +8.4 mM NaCl (darl grey) and +12.6 mM NaCl (black).</p>
</caption>
<graphic xlink:href="ncomms4335-f1"></graphic>
</fig>
<fig id="f2"><label>Figure 2</label>
<caption><title>Effect of surfactant concentration on the dynamic curves.</title>
<p>Dynamic curves obtained by progressively diluting the aerosol surfactant extract of 04 June 2009 and fit to <xref ref-type="disp-formula" rid="eq1">equation (1)</xref>
(lines) to determine <italic>t</italic>
<sub>m</sub>
for each concentration. From bottom: pure extract (filled red symbols), and dilutions by 0.67 (open red symbols), 0.44 (orange), 0.33 (yellow), 0.24 (filled green), 0.15 (open green), 0.095 (filled cyan), 0.065 (open cyan), 0.044 (filled blue), 0.028 (open blue), 0.017 (filled purple) and 0.009 (open purple).</p>
</caption>
<graphic xlink:href="ncomms4335-f2"></graphic>
</fig>
<fig id="f3"><label>Figure 3</label>
<caption><title>Variations of the meso-equilibrium with surfactant concentration.</title>
<p>Variations of the characteristic time of the meso-equilibrium, <italic>t</italic>
<sub>m</sub>
, with the relative concentration of surfactant for the different aerosol samples, and best fits (lines): 04 June 2009 black diamonds (<italic>n</italic>
=1.15), 07 July 2009 red diamonds (<italic>n</italic>
=1.26), 17 July 2009 white circles (<italic>n</italic>
=1.20), 10 November 2009 black squares (<italic>n</italic>
=2.38), 20 November 2009 blue triangles (<italic>n</italic>
=0.86) and 03 January 2010 green squares (<italic>n</italic>
=0.87). Comparison with data for C15 surfactin from the study by Razafindralambo <italic>et al</italic>
.<xref ref-type="bibr" rid="b17">17</xref>
(black circles, <italic>n</italic>
=1.7).</p>
</caption>
<graphic xlink:href="ncomms4335-f3"></graphic>
</fig>
<fig id="f4"><label>Figure 4</label>
<caption><title>Time-dependent Köhler curves.</title>
<p>Köhler curves illustrating the effects of the dynamic surface tension on droplet activation for the sample of 04 June 2009: <italic>t</italic>
=0.03 s (just after the rapid fall, red) 10 s (orange), 30 s (green), 100 s (blue) and <italic>t</italic>
<sub>eq</sub>
(black).</p>
</caption>
<graphic xlink:href="ncomms4335-f4"></graphic>
</fig>
<table-wrap position="float" id="t1"><label>Table 1</label>
<caption><title>List of the samples studied and results of this work.</title>
</caption>
<table frame="hsides" rules="groups" border="1"><colgroup><col align="left"></col>
<col align="center"></col>
<col align="center"></col>
<col align="center"></col>
<col align="center"></col>
<col align="center"></col>
<col align="center"></col>
<col align="center"></col>
</colgroup>
<thead valign="bottom"><tr><th align="left" valign="top" charoff="50"><bold>Surfactant/sample</bold>
</th>
<th align="center" valign="top" charoff="50"><italic><bold>C</bold>
</italic>
,<xref ref-type="fn" rid="t1-fn2">*</xref>
<bold>mol m</bold>
<sup><bold>−3</bold>
</sup>
</th>
<th align="center" valign="top" charoff="50"><bold>[NaCl],</bold>
<xref ref-type="fn" rid="t1-fn3">†</xref>
<bold>M</bold>
</th>
<th align="center" valign="top" charoff="50"><italic><bold>t</bold>
</italic>
<sub><bold>m</bold>
</sub>
,<xref ref-type="fn" rid="t1-fn3">‡</xref>
<bold>s=</bold>
<italic><bold>t</bold>
</italic>
<sub><bold>lab</bold>
</sub>
</th>
<th align="center" valign="top" charoff="50">Γ,<xref ref-type="fn" rid="t1-fn4">§</xref>
<bold>mol m</bold>
<sup><bold>−2</bold>
</sup>
</th>
<th align="center" valign="top" charoff="50"><bold>Slope,</bold>
<xref ref-type="fn" rid="t1-fn5">||</xref>
<bold>N m</bold>
<sup><bold>−1</bold>
</sup>
<bold>s</bold>
<sup><bold>1/2</bold>
</sup>
</th>
<th align="center" valign="top" charoff="50"><italic><bold>D</bold>
</italic>
<sub><bold>a</bold>
</sub>
,<xref ref-type="fn" rid="t1-fn6">¶</xref>
<bold>cm</bold>
<sup><bold>2</bold>
</sup>
<bold>s</bold>
<sup><bold>−1</bold>
</sup>
</th>
<th align="center" valign="top" charoff="50"><italic><bold>t</bold>
</italic>
<sub><bold>eq</bold>
</sub>
,<xref ref-type="fn" rid="t1-fn7">#</xref>
<bold>s</bold>
</th>
</tr>
</thead>
<tbody valign="top"><tr><td align="left" valign="top" charoff="50">4 June 2009</td>
<td align="center" valign="top" charoff="50">Unknown</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">8</td>
<td align="center" valign="top" charoff="50">2 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">7.0 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.6 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">36</td>
</tr>
<tr><td align="left" valign="top" charoff="50">7 July 2009</td>
<td align="center" valign="top" charoff="50">Unknown</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">30</td>
<td align="center" valign="top" charoff="50">2 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">24.8 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.2 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50">135</td>
</tr>
<tr><td align="left" valign="top" charoff="50">17 July 2009</td>
<td align="center" valign="top" charoff="50">Unknown</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">20</td>
<td align="center" valign="top" charoff="50">2 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">16.6 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">2.8 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50">90</td>
</tr>
<tr><td align="left" valign="top" charoff="50">10 November 2009</td>
<td align="center" valign="top" charoff="50">Unknown</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">20</td>
<td align="center" valign="top" charoff="50">2 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">13.4 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">4.3 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50">90</td>
</tr>
<tr><td align="left" valign="top" charoff="50">20 November 2009</td>
<td align="center" valign="top" charoff="50">Unknown</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">80</td>
<td align="center" valign="top" charoff="50">2 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">25.5 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.2 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50">360</td>
</tr>
<tr><td align="left" valign="top" charoff="50">03 January 2010</td>
<td align="center" valign="top" charoff="50">Unknown</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">110</td>
<td align="center" valign="top" charoff="50">2 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">56.6 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">2.4 × 10<sup>−8</sup>
</td>
<td align="center" valign="top" charoff="50">495</td>
</tr>
<tr><td align="left" valign="top" charoff="50">SDS</td>
<td align="char" valign="top" char="." charoff="50">3.4</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">3,000</td>
<td align="center" valign="top" charoff="50">5.5 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">1,413 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">4.3 × 10<sup>−12</sup>
</td>
<td align="center" valign="top" charoff="50">0.1</td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="char" valign="top" char="." charoff="50">3.4</td>
<td align="center" valign="top" charoff="50">4.2 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">200</td>
<td align="center" valign="top" charoff="50">5.5 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">73.5 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.6 × 10<sup>−9</sup>
</td>
<td align="center" valign="top" charoff="50"> </td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="char" valign="top" char="." charoff="50">3.4</td>
<td align="center" valign="top" charoff="50">8.4 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">50</td>
<td align="center" valign="top" charoff="50">5.5 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">15.0 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">3.8 × 10<sup>−8</sup>
</td>
<td align="center" valign="top" charoff="50"> </td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="char" valign="top" char="." charoff="50">3.4</td>
<td align="center" valign="top" charoff="50">12.6 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">25</td>
<td align="center" valign="top" charoff="50">5.5 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">5.4 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">2.9 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50"> </td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="char" valign="top" char="." charoff="50">7</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">43</td>
<td align="center" valign="top" charoff="50">2.7 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">32.9 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.1 × 10<sup>−10</sup>
</td>
<td align="center" valign="top" charoff="50">0.1</td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="char" valign="top" char="." charoff="50">7</td>
<td align="center" valign="top" charoff="50">34.5 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">ND</td>
<td align="center" valign="top" charoff="50">5.4 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">1.5 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">8.4 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50"> </td>
</tr>
<tr><td align="left" valign="top" charoff="50">Rhamnolipids</td>
<td align="center" valign="top" charoff="50">48.6 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">6</td>
<td align="center" valign="top" charoff="50">1.3 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">16.4 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">6.0 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50">450</td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="center" valign="top" charoff="50">48.6 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">42.4 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">10</td>
<td align="center" valign="top" charoff="50">2.0 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">9.5 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">8.2 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50"> </td>
</tr>
<tr><td align="left" valign="top" charoff="50">Surfactin</td>
<td align="center" valign="top" charoff="50">58 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">/</td>
<td align="center" valign="top" charoff="50">7</td>
<td align="center" valign="top" charoff="50">3.5 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">104.6 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">8.3 × 10<sup>−7</sup>
</td>
<td align="center" valign="top" charoff="50">9</td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="center" valign="top" charoff="50">58 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.0 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">5</td>
<td align="center" valign="top" charoff="50">3.5 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">92.3 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.1 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50"> </td>
</tr>
<tr><td align="left" valign="top" charoff="50"> </td>
<td align="center" valign="top" charoff="50">58 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">0.1</td>
<td align="center" valign="top" charoff="50">20</td>
<td align="center" valign="top" charoff="50">3.5 × 10<sup>−6</sup>
</td>
<td align="center" valign="top" charoff="50">16.9 × 10<sup>−3</sup>
</td>
<td align="center" valign="top" charoff="50">1.7 × 10<sup>−5</sup>
</td>
<td align="center" valign="top" charoff="50"> </td>
</tr>
</tbody>
</table>
<table-wrap-foot><fn id="t1-fn1"><p>ND, not detected.</p>
</fn>
<fn id="t1-fn2"><p><sup>*</sup>
Concentration of surfactant.</p>
</fn>
<fn id="t1-fn3"><p><sup>†</sup>
Concentration of NaCl.</p>
</fn>
<fn id="t1-fn4"><p><sup>‡</sup>
Meso-equilibration time.</p>
</fn>
<fn id="t1-fn5"><p><sup>§</sup>
Excess surface concentration.</p>
</fn>
<fn id="t1-fn6"><p><sup>||</sup>
Slope of d<italic>σ</italic>
/d<italic>t</italic>
<sup>−1/2.</sup>
</p>
</fn>
<fn id="t1-fn7"><p><sup>¶</sup>
Apparent diffusion coefficient.</p>
</fn>
<fn id="t1-fn8"><p><sup>#</sup>
Equilibration time in an activated atmospheric particle.</p>
</fn>
</table-wrap-foot>
</table-wrap>
</floats-group>
</pmc>
</record>
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