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

Abstract

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 4more » 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.« less

Authors:
 [1];  [2];  [1];  [3];  [4];  [5];  [3];  [3];  [6];  [7];  [8];  [9];  [3];  [5];  [10];  [11];  [3];  [3];  [1];  [12] more »;  [6];  [3];  [3];  [13];  [1];  [3];  [14];  [15];  [6];  [16];  [17];  [18];  [1];  [3];  [6];  [19];  [3];  [3];  [20];  [1] « less
+ Show Author Affiliations
  1. Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt am Main Frankfurt am Main Germany
  2. CERN Geneva Switzerland
  3. Department of Physics University of Helsinki Helsinki Finland
  4. Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland, Institute for Atmospheric and Climate Science ETH Zurich Zurich Switzerland
  5. Institute for Ion Physics and Applied Physics University of Innsbruck Innsbruck Austria
  6. Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland
  7. Center for Atmospheric Particle Studies Carnegie Mellon University Pittsburgh Pennsylvania USA
  8. Kuopio Unit Finnish Meteorological Institute Kuopio Finland, School of Earth and Environment University of Leeds Leeds UK
  9. Division of Chemistry and Chemical Engineering California Institute of Technology Pasadena California USA
  10. Department of Physics University of Helsinki Helsinki Finland, Department of Applied Physics University of Eastern Finland Kuopio Finland
  11. Department of Applied Physics University of Eastern Finland Kuopio Finland
  12. Department of Physics University of Helsinki Helsinki Finland, Kuopio Unit Finnish Meteorological Institute Kuopio Finland
  13. Department of Physics University of Helsinki Helsinki Finland, Department of Atmospheric Sciences University of Washington Seattle Washington USA
  14. Department of Applied Physics University of Eastern Finland Kuopio Finland, Department of Chemistry University of California Irvine California USA
  15. CENTRA‐SIM University of Lisbon and University of Beira Interior Lisbon Portugal
  16. Leibniz Institute for Tropospheric Research Leipzig Germany
  17. Department of Applied Physics University of Eastern Finland Kuopio Finland, Department of Environmental Science University of Eastern Finland Kuopio Finland
  18. Faculty of Physics University of Vienna Vienna Austria
  19. Institute for Atmospheric and Environmental Sciences Goethe University Frankfurt am Main Frankfurt am Main Germany, CERN Geneva Switzerland
  20. Department of Physics University of Helsinki Helsinki Finland, Aerodyne Research, Inc. Billerica Massachusetts USA
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1244106
Alternate Identifier(s):
OSTI ID: 1244107; OSTI ID: 1623443
Grant/Contract Number:  
DE‐SC0014469; SC0014469
Resource Type:
Published Article
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Name: Journal of Geophysical Research: Atmospheres Journal Volume: 121 Journal Issue: 6; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union (AGU)
Country of Publication:
United States
Language:
English
Subject:
Meteorology & Atmospheric Sciences; CLOUD experiment; nucleation; Chemical Ionization‐Atmospheric Pressure interface‐Time Of Flight

Citation Formats

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., and Curtius, J. Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry. United States: N. p., 2016. Web. doi:10.1002/2015JD023868.
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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. Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry. United States. https://doi.org/10.1002/2015JD023868
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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., and Curtius, J. Thu . "Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry". United States. https://doi.org/10.1002/2015JD023868.
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@article{osti_1244106,
title = {Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry},
author = {Rondo, L. and Ehrhart, S. and Kürten, A. and Adamov, A. and Bianchi, F. and Breitenlechner, M. and Duplissy, J. and Franchin, A. and Dommen, J. and Donahue, N. M. and Dunne, E. M. and Flagan, R. C. and Hakala, J. and Hansel, A. and Keskinen, H. and Kim, J. and Jokinen, T. and Lehtipalo, K. and Leiminger, M. and Praplan, A. and Riccobono, F. and Rissanen, M. P. and Sarnela, N. and Schobesberger, S. and Simon, M. and Sipilä, M. and Smith, J. N. and Tomé, A. and Tröstl, J. and Tsagkogeorgas, G. and Vaattovaara, P. and Winkler, P. M. and Williamson, C. and Wimmer, D. and Baltensperger, U. and Kirkby, J. and Kulmala, M. and Petäjä, T. and Worsnop, D. R. and Curtius, J.},
abstractNote = {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.},
doi = {10.1002/2015JD023868},
journal = {Journal of Geophysical Research: Atmospheres},
number = 6,
volume = 121,
place = {United States},
year = {Thu Mar 24 00:00:00 EDT 2016},
month = {Thu Mar 24 00:00:00 EDT 2016}
}
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https://doi.org/10.1002/2015JD023868
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Figures / Tables:

Figure 1 Figure 1: (a) Example of a measurement of the sulfuric acid concentration (displayed with red color for both 5 s raw data and 1min averaged data) a variation of the UV light (10% to 100%UV light aperture) for the pure H2SO4-H2O binary system. (b) Comparison of the expected H2SO4 (ASADmore » model and UV light dependency) and the average measured H2SO4 concentration for different UV light intensities applied in the chamber after equilibration of the H2SO4 concentration to the new settings. The displayed CIMS sulfuric acid concentrations include 1σ total errors, while the systematic scale uncertainty is a factor of 2. The averaged measured concentrations are taken after H2SO4 equilibrium is established within 650 ± 33 s, which is given from the sulfuric acid lifetime fit as shown in Figure 1a.« less
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