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

Autor(en)

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 Kangasluoma, Jaeseok 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, Antonio Tome, Jasmin Tröstl, Georgios Tsagkogeorgas, Paul E. Wagner, Daniela Wimmer, Penglin Ye, Urs Baltensperger, Ken Carslaw, Markku Kulmala, Joachim Curtius

Abstrakt

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

⁹cm

^-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.

Organisation(en)

Aerosolphysik und Umweltphysik

Externe Organisation(en)

Johann Wolfgang Goethe-Universität Frankfurt am Main, Paul Scherrer Institute, Eidgenössische Technische Hochschule Zürich, University of Helsinki, European Organization for Nuclear Research (CERN), University of Leeds, Finnish Meteorological Institute, University of Colorado, Boulder, Leopold-Franzens-Universität Innsbruck, IONICON Analytik GmbH, Carnegie Mellon University, California Institute of Technology (Caltech), University of Eastern Finland, Russian Academy of Sciences, ONERA-The French Aerospac Lab., University of Washington, University of California, Irvine, Universidade de Lisboa, Universidade da Beira Interior, Leibniz-Institut für Troposphärenforschung

Journal

Journal of Geophysical Research: Atmospheres

Band

121

Seiten

12,377-12,400

Anzahl der Seiten

24

ISSN

2169-897X

DOI

https://doi.org/10.1002/2015JD023908

Publikationsdatum

10-2016

Peer-reviewed

Ja

ÖFOS 2012

103037 Umweltphysik, 103039 Aerosolphysik

Schlagwörter

ASJC Scopus Sachgebiete

Condensed Matter Physics, Materials Chemistry, Polymers and Plastics, Physical and Theoretical Chemistry

Link zum Portal

https://ucrisportal.univie.ac.at/de/publications/4e30455b-84f2-4d94-bced-9885bf37d9ef