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

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

doi:10.1002/2015JD023868

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

L. Rondo (Corresponding author), 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. PraplanF. 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

Aerosol Physics and Environmental Physics

Publications: Contribution to journal › Article › Peer Reviewed

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 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.

Original language	English
Pages (from-to)	3036-3049
Number of pages	14
Journal	Journal of Geophysical Research: Atmospheres
Volume	121
Issue number	6
DOIs	https://doi.org/10.1002/2015JD023868
Publication status	Published - 24 Mar 2016

Austrian Fields of Science 2012

105904 Environmental research
103039 Aerosol physics

Keywords

CLOUD experiment
nucleation
Chemical Ionization-Atmospheric Pressure interface-Time Of Flight Mass Spectrometer
ATMOSPHERIC AEROSOL NUCLEATION
PARTICLE FORMATION
CLOUD EXPERIMENT
H2SO4 PRODUCTION
BOUNDARY-LAYER
AMMONIA
CLUSTERS
AMINES
RATES
WATER

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10.1002/2015JD023868

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Rondo, L., Ehrhart, S., Kuerten, 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., ... Curtius, J. (2016). Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry. Journal of Geophysical Research: Atmospheres, 121(6), 3036-3049. https://doi.org/10.1002/2015JD023868

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

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 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. ",

keywords = "CLOUD experiment, nucleation, Chemical Ionization-Atmospheric Pressure interface-Time Of Flight Mass Spectrometer, ATMOSPHERIC AEROSOL NUCLEATION, PARTICLE FORMATION, CLOUD EXPERIMENT, H2SO4 PRODUCTION, BOUNDARY-LAYER, AMMONIA, CLUSTERS, AMINES, RATES, WATER",

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

note = "Publisher Copyright: {\textcopyright} 2016. The Authors.",

year = "2016",

month = mar,

day = "24",

doi = "10.1002/2015JD023868",

language = "English",

volume = "121",

pages = "3036--3049",

journal = "Journal of Geophysical Research: Atmospheres",

issn = "2169-897X",

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Rondo, L, Ehrhart, S, Kuerten, A, Adamov, A, Bianchi, F, Breitenlechner, M, Duplissy, J, Franchin, A, Dommen, J, Donahue, NM, Dunne, EM, Flagan, RC, Hakala, J, Hansel, A, Keskinen, H, Kim, J, Jokinen, T, Lehtipalo, K, Leiminger, M, Praplan, A, Riccobono, F, Rissanen, MP, Sarnela, N, Schobesberger, S, Simon, M, Sipila, M, Smith, JN, Tome, A, Trostl, J, Tsagkogeorgas, G, Vaattovaara, P, Winkler, PM, Williamson, C, Wimmer, D, Baltensperger, U, Kirkby, J, Kulmala, M, Petaja, T, Worsnop, DR & Curtius, J 2016, 'Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry', Journal of Geophysical Research: Atmospheres, vol. 121, no. 6, pp. 3036-3049. https://doi.org/10.1002/2015JD023868

TY - JOUR

T1 - Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry

AU - Rondo, L.

AU - Ehrhart, S.

AU - Kuerten, A.

AU - Adamov, A.

AU - Bianchi, F.

AU - Breitenlechner, M.

AU - Duplissy, J.

AU - Franchin, A.

AU - Dommen, J.

AU - Donahue, N. M.

AU - Dunne, E. M.

AU - Flagan, R. C.

AU - Hakala, J.

AU - Hansel, A.

AU - Keskinen, H.

AU - Kim, J.

AU - Jokinen, T.

AU - Lehtipalo, K.

AU - Leiminger, M.

AU - Praplan, A.

AU - Riccobono, F.

AU - Rissanen, M. P.

AU - Sarnela, N.

AU - Schobesberger, S.

AU - Simon, M.

AU - Sipila, M.

AU - Smith, J. N.

AU - Tome, A.

AU - Trostl, J.

AU - Tsagkogeorgas, G.

AU - Vaattovaara, P.

AU - Winkler, P. M.

AU - Williamson, C.

AU - Wimmer, D.

AU - Baltensperger, U.

AU - Kirkby, J.

AU - Kulmala, M.

AU - Petaja, T.

AU - Worsnop, D. R.

AU - Curtius, J.

PY - 2016/3/24

Y1 - 2016/3/24

N2 - 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.

AB - 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.

KW - CLOUD experiment

KW - nucleation

KW - Chemical Ionization-Atmospheric Pressure interface-Time Of Flight Mass Spectrometer

KW - ATMOSPHERIC AEROSOL NUCLEATION

KW - PARTICLE FORMATION

KW - CLOUD EXPERIMENT

KW - H2SO4 PRODUCTION

KW - BOUNDARY-LAYER

KW - AMMONIA

KW - CLUSTERS

KW - AMINES

KW - RATES

KW - WATER

UR - http://www.scopus.com/inward/record.url?scp=84961815174&partnerID=8YFLogxK

U2 - 10.1002/2015JD023868

DO - 10.1002/2015JD023868

M3 - Article

SN - 2169-897X

VL - 121

SP - 3036

EP - 3049

JO - Journal of Geophysical Research: Atmospheres

JF - Journal of Geophysical Research: Atmospheres

IS - 6

ER -

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

Abstract

Austrian Fields of Science 2012

Keywords

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