Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures
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- Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt Frankfurt am Main Germany
- Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland, Institute of Atmospheric and Climate Science ETH Zurich Zurich Switzerland, Department of Physics University of Helsinki Helsinki Finland
- Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt Frankfurt am Main Germany, Physics Department CERN Geneva Switzerland
- Department of Physics University of Helsinki Helsinki Finland
- School of Earth and Environment University of Leeds Leeds UK, Atmospheric Research Centre of Eastern Finland Finnish Meteorological Institute Kuopio Finland
- Department of Physics University of Helsinki Helsinki Finland, Physics Department CERN Geneva Switzerland
- Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt Frankfurt am Main Germany, Cooperative Institute for Research in Environmental Sciences University of Colorado Boulder Boulder Colorado USA
- Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland
- Institute for Ion and Applied Physics University of Innsbruck Innsbruck Austria, Ionicon Analytik GmbH Innsbruck Austria
- Center for Atmospheric Particle Studies Carnegie Mellon University Pittsburgh Pennsylvania USA
- Division of Chemistry and Chemical Engineering California Institute of Technology Pasadena California USA
- Physics Department CERN Geneva Switzerland
- Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt Frankfurt am Main Germany, Institute of Atmospheric and Climate Science ETH Zurich Zurich Switzerland
- Department of Applied Physics University of Eastern Finland Kuopio Finland
- Cooperative Institute for Research in Environmental Sciences University of Colorado Boulder Boulder Colorado USA, Faculty of Physics University of Vienna Vienna Austria
- Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland, Department of Physics University of Helsinki Helsinki Finland
- Solar and Cosmic Ray Research Laboratory Lebedev Physical Institute Moscow Russia
- Department of Physics University of Helsinki Helsinki Finland, Onera‐The French Aerospace Lab Palaiseau France
- Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland, Finnish Meteorological Institute Helsinki Finland
- Department of Physics University of Helsinki Helsinki Finland, Department of Atmospheric Sciences University of Washington Seattle Washington USA
- Department of Applied Physics University of Eastern Finland Kuopio Finland, Department of Chemistry University of California Irvine California USA
- Department of Physics University of Helsinki Helsinki Finland, Institute for Ion and Applied Physics University of Innsbruck Innsbruck Austria, Faculty of Physics University of Vienna Vienna Austria
- SIM University of Lisbon and University of Beira Interior Lisbon Portugal
- Leibniz Institute for Tropospheric Research Leipzig Germany
- Faculty of Physics University of Vienna Vienna Austria
- Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt Frankfurt am Main Germany, Department of Physics University of Helsinki Helsinki Finland
- School of Earth and Environment University of Leeds Leeds UK
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 NH 3 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.
- Research Organization:
- Univ. of California, Irvine, CA (United States)
- Sponsoring Organization:
- USDOE; National Science Foundation (NSF); Swiss National Science Foundation (SNSF); European Union (EU)
- Grant/Contract Number:
- DE‐SC0014469; SC0014469; AGS1447056; AGS1439551; 1133872; 251007
- OSTI ID:
- 1330276
- Alternate ID(s):
- OSTI ID: 1330394; OSTI ID: 1425930
- Journal Information:
- Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Vol. 121 Journal Issue: 20; ISSN 2169-897X
- Publisher:
- American Geophysical Union (AGU)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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