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

Autor(en)

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

Abstrakt

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

₂SO

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

₂SO

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

₂SO

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

₂SO

₄ cluster distribution compared to binary (H

₂SO

₄-H

₂O) conditions, the CIMS detection efficiency does not seem to depend substantially on whether an individual H

₂SO

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.

Organisation(en)

Aerosolphysik und Umweltphysik

Externe Organisation(en)

Johann Wolfgang Goethe-Universität Frankfurt am Main, European Organization for Nuclear Research (CERN), University of Helsinki, Paul Scherrer Institute, Eidgenössische Technische Hochschule Zürich, Leopold-Franzens-Universität Innsbruck, Carnegie Mellon University, Finnish Meteorological Institute, University of Leeds, California Institute of Technology (Caltech), University of Eastern Finland, University of Washington, University of California, Irvine, Universidade de Lisboa, Universidade da Beira Interior, Leibniz-Institut für Troposphärenforschung, Aerodyne Res Inc

Journal

Journal of Geophysical Research: Atmospheres

Band

121

Seiten

3036-3049

Anzahl der Seiten

14

ISSN

2169-897X

DOI

https://doi.org/10.1002/2015JD023868

Publikationsdatum

03-2016

Peer-reviewed

Ja

ÖFOS 2012

105904 Umweltforschung, 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/466141f6-ce1a-45a2-a785-f2765194b6ee