Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry

Rondo, L.; Ehrhart, S.; Kürten, A.; Adamov, A.; Bianchi, F.; Breitenlechner, M.; Duplissy, J.; Franchin, A.; Dommen, J.; Donahue, N. M.; Dunne, E. M.; Flagan, R. C.; Hakala, J.; Hansel, A.; Keskinen, H.; Kim, J.; Jokinen, T.; Lehtipalo, K.; Leiminger, M.; Praplan, A.; Riccobono, F.; Rissanen, M. P.; Sarnela, N.; Schobesberger, S.; Simon, M.; Sipilä, M.; Smith, J. N.; Tomé, A.; Tröstl, J.; Tsagkogeorgas, G.; Vaattovaara, P.; Winkler, P. M.; Williamson, C.; Wimmer, D.; Baltensperger, U.; Kirkby, J.; Kulmala, M.; Petäjä, T.; Worsnop, D. R.; Curtius, J.

doi:10.1002/2015JD023868

Title: Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry

Journal Article · Thu Mar 24 00:00:00 EDT 2016 · Journal of Geophysical Research: Atmospheres

DOI:https://doi.org/10.1002/2015JD023868· OSTI ID:1244106

Rondo, L. ^[1]; Ehrhart, S. ^[2]; Kürten, A. ^[1]; Adamov, A. ^[3]; Bianchi, F. ^[4]; Breitenlechner, M. ^[5]; Duplissy, J. ^[3]; Franchin, A. ^[3]; Dommen, J. ^[6]; Donahue, N. M. ^[7]; Dunne, E. M. ^[8]; Flagan, R. C. ^[9]; Hakala, J. ^[3]; Hansel, A. ^[5]; Keskinen, H. ^[10]; Kim, J. ^[11]; Jokinen, T. ^[3]; Lehtipalo, K. ^[3]; Leiminger, M. ^[1]; Praplan, A. ^[12] more »

Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt am Main Frankfurt am Main Germany
CERN Geneva Switzerland
Department of Physics University of Helsinki Helsinki Finland
Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland, Institute for Atmospheric and Climate Science ETH Zurich Zurich Switzerland
Institute for Ion Physics and Applied Physics University of Innsbruck Innsbruck Austria
Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland
Center for Atmospheric Particle Studies Carnegie Mellon University Pittsburgh Pennsylvania USA
Kuopio Unit Finnish Meteorological Institute Kuopio Finland, School of Earth and Environment University of Leeds Leeds UK
Division of Chemistry and Chemical Engineering California Institute of Technology Pasadena California USA
Department of Physics University of Helsinki Helsinki Finland, Department of Applied Physics University of Eastern Finland Kuopio Finland
Department of Applied Physics University of Eastern Finland Kuopio Finland
Department of Physics University of Helsinki Helsinki Finland, Kuopio Unit Finnish Meteorological Institute Kuopio 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
CENTRA‐SIM University of Lisbon and University of Beira Interior Lisbon Portugal
Leibniz Institute for Tropospheric Research Leipzig Germany
Department of Applied Physics University of Eastern Finland Kuopio Finland, Department of Environmental Science University of Eastern Finland Kuopio Finland
Faculty of Physics University of Vienna Vienna Austria
Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt am Main Frankfurt am Main Germany, CERN Geneva Switzerland
Department of Physics University of Helsinki Helsinki Finland, Aerodyne Research, Inc. Billerica Massachusetts USA

Abstract Sulfuric acid is widely recognized as a very important substance driving atmospheric aerosol nucleation. Based on quantum chemical calculations it has been suggested that the quantitative detection of gas phase sulfuric acid (H ₂ SO ₄ ) by use of Chemical Ionization Mass Spectrometry (CIMS) could be biased in the presence of gas phase amines such as dimethylamine (DMA). An experiment (CLOUD7 campaign) was set up at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber to investigate the quantitative detection of H ₂ SO ₄ in the presence of dimethylamine by CIMS at atmospherically relevant concentrations. For the first time in the CLOUD experiment, the monomer sulfuric acid concentration was measured by a CIMS and by two CI‐APi‐TOF (Chemical Ionization‐Atmospheric Pressure interface‐Time Of Flight) mass spectrometers. In addition, neutral sulfuric acid clusters were measured with the CI‐APi‐TOFs. The CLOUD7 measurements show that in the presence of dimethylamine (<5 to 70 pptv) the sulfuric acid monomer measured by the CIMS represents only a fraction of the total H ₂ SO ₄ , contained in the monomer and the clusters that is available for particle growth. Although it was found that the addition of dimethylamine dramatically changes the H ₂ SO ₄ cluster distribution compared to binary (H ₂ SO ₄ ‐H ₂ O) conditions, the CIMS detection efficiency does not seem to depend substantially on whether an individual H ₂ SO ₄ monomer is clustered with a DMA molecule. The experimental observations are supported by numerical simulations based on A Self‐contained Atmospheric chemistry coDe coupled with a molecular process model (Sulfuric Acid Water NUCleation) operated in the kinetic limit.

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Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: DE‐SC0014469; SC0014469

OSTI ID:: 1244106

Alternate ID(s):: OSTI ID: 1244107; OSTI ID: 1623443

Journal Information:: Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Vol. 121 Journal Issue: 6; ISSN 2169-897X

Publisher:: American Geophysical Union (AGU)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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Title: Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry

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