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Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates and temperatures

Identifieur interne : 000058 ( Main/Exploration ); précédent : 000057; suivant : 000059

Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates and temperatures

Auteurs : Andreas Kürten [Allemagne] ; Federico Bianchi [Suisse] ; Joao Almeida [Allemagne] ; Oona Kupiainen-Maata [Finlande] ; Eimear Dunne [Royaume-Uni] ; Jonathan Duplissy [Finlande] ; Christina Williamson [Allemagne] ; Peter Barmet [Suisse] ; Martin Breitenlechner [Autriche] ; Josef Dommen [Suisse] ; Neil M. Donahue [États-Unis] ; Rchard C. Flagan [États-Unis] ; Alessandro Franchin [Finlande] ; Hamish Gordon [Suisse] ; Jani Hakala [Finlande] ; Armin Hansel [Autriche] ; Martin Heinritzi [Allemagne] ; Luisa Ickes [Allemagne] ; Tuija Jokinen [Finlande] ; Juha Kangasluoma [Finlande] ; Jaeseok Kim [Finlande] ; Jasper Kirkby [Allemagne] ; Agnieszka Kupc [États-Unis] ; Katrianne Lehtipalo [Suisse] ; Markus Leiminger [Allemagne] ; Vladimir Makhmutov [Russie] ; Antti Onnela [Autriche] ; Ismael K. Ortega Colomer [France] ; Tuukka Pet J [Finlande] ; Arnaud P. Praplan [Suisse] ; Francesco Riccobono [Suisse] ; Matti P. Rissanen [Finlande] ; Linda Rondo [Allemagne] ; Ralf Schnitzhofer [Autriche] ; Siegfried Schobesberger [Finlande] ; James N. Smith [Finlande] ; Gérard Steiner [Finlande] ; Yuri Stozhkov [Russie] ; Antonio Tomé [Portugal] ; Jasmin Tröstl [Suisse] ; Georgios Tsagkogeorgas [Allemagne] ; Paul E. Wagner [Autriche] ; Daniela Wimmer [Allemagne] ; Penglin Ye [États-Unis] ; Urs Baltensperger [Suisse] ; Ken Carslaw [Royaume-Uni] ; Markku Kulmala [Finlande] ; Joachim Curtius [Allemagne]

Source :

RBID : Hal:hal-01443859

English descriptors

Abstract

Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10^5 and 1 × 10^9 cm^-3 , and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximum of ~1400 parts per trillion by volume (pptv). We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm 3 s 1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH3 levels. We compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.

Url:
DOI: 10.1002/2015JD023908


Affiliations:


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<address>
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<orgName>University of Leeds</orgName>
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<name sortKey="Kulmala, Markku" sort="Kulmala, Markku" uniqKey="Kulmala M" first="Markku" last="Kulmala">Markku Kulmala</name>
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<orgName>University of Helsinki [Helsinki]</orgName>
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<author>
<name sortKey="Curtius, Joachim" sort="Curtius, Joachim" uniqKey="Curtius J" first="Joachim" last="Curtius">Joachim Curtius</name>
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<orgName>Institute for Atmospheric and Environmental Sciences [Frankfurt/Main]</orgName>
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<idno type="DOI">10.1002/2015JD023908</idno>
<series>
<title level="j">Journal of Geophysical Research: Atmospheres</title>
<idno type="ISSN">2169-897X</idno>
<imprint>
<date type="datePub">2016-10-27</date>
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<keywords scheme="mix" xml:lang="en">
<term>AMMONIA</term>
<term>NUCLEATION</term>
<term>SULFURIC ACID</term>
</keywords>
</textClass>
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<front>
<div type="abstract" xml:lang="en">Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10^5 and 1 × 10^9 cm^-3 , and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximum of ~1400 parts per trillion by volume (pptv). We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm 3 s 1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH3 levels. We compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry. </div>
</front>
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