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

Andreas Kürten, Federico Bianchi, Joao Almeida, Oona Kupiainen-Määttä, Eimear M. Dunne, Jonathan Duplissy, Christina Williamson, Peter Barmet, Martin Breitenlechner, Josef Dommen, Neil M. Donahue, Richard C. Flagan, Alessandro Franchin, Hamish Gordon, Jani Hakala, Armin Hansel, Martin Heinritzi, Luisa Ickes, Tuija Jokinen, Juha KangasluomaJaeseok Kim, Jasper Kirkby, Agnieszka Kupc, Katrianne Lehtipalo, Markus Leiminger, Vladimir Makhmutov, Antti Onnela, Ismael K. Ortega, Tuukka Petäjä, Arnaud P. Praplan, Francesco Riccobono, Matti P. Rissanen, Linda Rondo, Ralf Schnitzhofer, Siegfried Schobesberger, James N. Smith, Gerhard Steiner, Yuri Stozhkov, António Tomé, Jasmin Tröstl, Georgios Tsagkogeorgas, Paul E. Wagner, Daniela Wimmer, Penglin Ye, Urs Baltensperger, Ken Carslaw, Markku Kulmala, Joachim Curtius

Research output: Contribution to journalArticleScientificpeer-review

74 Citations (Scopus)

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 × 105 and 1 × 109cm-3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximumof ~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.

Original languageEnglish
Pages (from-to)12,377-12,400
JournalJournal of Geophysical Research
Volume121
Issue number20
DOIs
Publication statusPublished - 27 Oct 2016
MoE publication typeA1 Journal article-refereed

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