Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory

J. Duplissy; J. Merikanto; A. Franchin; G. Tsagkogeorgas; J. Kangasluoma; Daniela Wimmer; H. Vuollekoski; S. Schobesberger; K. Lehtipalo; R. C. Flagan; D. Brus; N. M. Donahue; H. Vehkamaki; J. Almeida; A. Amorim; P. Barmet; F. Bianchi; M. Breitenlechner; E. M. Dunne; R. Guida; H. Henschel; H. Junninen; J. Kirkby; A. Kuerten; A. Kupc; Anni Määttänen; V. Makhmutov; S. Mathot; T. Nieminen; A. Onnela; A. P. Praplan; F. Riccobono; L. Rondo; Gerhard Steiner; A. Tome; H. Walther; U. Baltensperger; K. S. Carslaw; J. Dommen; A. Hansel; T. Petaja; M. Sipila; F. Stratmann; A. Vrtala; P. E. Wagner; D. R. Worsnop; J. Curtius; M. Kulmala

doi:10.1002/2015JD023539

Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory

J. Duplissy
, J. Merikanto
, A. Franchin
, G. Tsagkogeorgas
, J. Kangasluoma
, Daniela Wimmer
, H. Vuollekoski
, S. Schobesberger
, K. Lehtipalo
, R. C. Flagan
, D. Brus
, N. M. Donahue
, H. Vehkamaki
, J. Almeida
, A. Amorim
, P. Barmet
, F. Bianchi
, M. Breitenlechner
, E. M. Dunne
, R. Guida

H. Henschel, H. Junninen, J. Kirkby, A. Kuerten, A. Kupc, Anni Määttänen, V. Makhmutov, S. Mathot, T. Nieminen, A. Onnela, A. P. Praplan, F. Riccobono, L. Rondo, Gerhard Steiner, A. Tome, H. Walther, U. Baltensperger, K. S. Carslaw, J. Dommen, A. Hansel, T. Petaja, M. Sipila, F. Stratmann, A. Vrtala, P. E. Wagner, D. R. Worsnop, J. Curtius, M. Kulmala

Aerosol Physics and Environmental Physics

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (10(5) to 10(9)molcm(-3)), relative humidity (11% to 58%), temperature (207K to 299K), and total ion concentration (0 to 6800ionscm(-3)). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3nm to 3.2nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.

Original language	English
Pages (from-to)	1752-1775
Number of pages	24
Journal	Journal of Geophysical Research: Atmospheres
Volume	121
Issue number	4
DOIs	https://doi.org/10.1002/2015JD023539
Publication status	Published - 16 Feb 2016

Funding

We would like to thank CERN for supporting CLOUD with important technical and financial resources, and for providing a particle beam from the CERN Proton Synchrotron. We also thank P. Carrie, L.-P. De Menezes, J. Dumollard, K. Ivanova, F. Josa, I. Krasin, R. Kristic, A. Laassiri, O.S. Maksumov, B. Marichy, H. Martinati, S.V. Mizin, R. Sitals, A. Wasem, and M. Wilhelmsson for their important contributions to the experiment. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network "CLOUD-ITN" 215072, MC-ITN "CLOUD-TRAIN" 316662, ERC-Starting "MOCAPAF" grant 57360 and ERC-Advanced "ATMNUCLE" grant 227463), the German Federal Ministry of Education and Research (projects 01LK0902A and 01LK1222A), the Swiss National Science Foundation (projects 200020 135307 and 206620 141278), the Academy of Finland (Center of Excellence project 1118615), the Academy of Finland (135054, 133872, 251427, 1133872, 139656, 139995, 137749, 141217, and 141451), the Finnish Funding Agency for Technology and Innovation, the Vaisala Foundation, the Kone foundation, the Nessling Foundation, the Austrian Science Fund (FWF; project J3198-N21), the Portuguese Foundation for Science and Technology (project CERN/FP/116387/2010), the Swedish Research Council, Vetenskapsradet (grant 2011-5120), the Presidium of the Russian Academy of Sciences and Russian Foundation for Basic Research (grants 08-02-91006-CERN and 12-02-91522-CERN), the U.S. National Science Foundation (grants AGS1136479, CHE1012293, and AGS1447056), PEGASOS project (funded by the European Commission under the Framework Program 7 (FP7-ENV-2010-265148)), and the Davidow Foundation. We thank the tofTools team for providing tools for mass spectrometry analysis. In keeping with AGU's Data Policy, all process experimental data used in this paper are summarized in Table 2, and raw data used to produce the results of the paper are available from the author upon request ([email protected]).

Austrian Fields of Science 2012

105904 Environmental research
103039 Aerosol physics
210006 Nanotechnology
103008 Experimental physics

Keywords

binary particle formation
ion-induced nucleation
sulfuric acid
classical nucleation theory
ATMOSPHERIC AEROSOL NUCLEATION
IONIZATION MASS-SPECTROMETER
HOMOGENEOUS NUCLEATION
HYDRATE FORMATION
VAPOR-PRESSURE
BOREAL FOREST
CLOUD CHAMBER
CHEMICAL-COMPOSITION
OXIDATION-PRODUCTS
EXPERIMENTAL SETUP

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10.1002/2015JD023539

Cite this

Duplissy, J., Merikanto, J., Franchin, A., Tsagkogeorgas, G., Kangasluoma, J., Wimmer, D., Vuollekoski, H., Schobesberger, S., Lehtipalo, K., Flagan, R. C., Brus, D., Donahue, N. M., Vehkamaki, H., Almeida, J., Amorim, A., Barmet, P., Bianchi, F., Breitenlechner, M., Dunne, E. M., ... Kulmala, M. (2016). Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory. Journal of Geophysical Research: Atmospheres, 121(4), 1752-1775. https://doi.org/10.1002/2015JD023539

@article{e543ee2dc8304b4eafa4b8b94c8a0d6b,

title = "Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory",

abstract = "We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (10(5) to 10(9)molcm(-3)), relative humidity (11\% to 58\%), temperature (207K to 299K), and total ion concentration (0 to 6800ionscm(-3)). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3nm to 3.2nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.",

keywords = "binary particle formation, ion-induced nucleation, sulfuric acid, classical nucleation theory, ATMOSPHERIC AEROSOL NUCLEATION, IONIZATION MASS-SPECTROMETER, HOMOGENEOUS NUCLEATION, HYDRATE FORMATION, VAPOR-PRESSURE, BOREAL FOREST, CLOUD CHAMBER, CHEMICAL-COMPOSITION, OXIDATION-PRODUCTS, EXPERIMENTAL SETUP",

author = "J. Duplissy and J. Merikanto and A. Franchin and G. Tsagkogeorgas and J. Kangasluoma and Daniela Wimmer and H. Vuollekoski and S. Schobesberger and K. Lehtipalo and Flagan, \{R. C.\} and D. Brus and Donahue, \{N. M.\} and H. Vehkamaki and J. Almeida and A. Amorim and P. Barmet and F. Bianchi and M. Breitenlechner and Dunne, \{E. M.\} and R. Guida and H. Henschel and H. Junninen and J. Kirkby and A. Kuerten and A. Kupc and Anni M{\"a}{\"a}tt{\"a}nen and V. Makhmutov and S. Mathot and T. Nieminen and A. Onnela and Praplan, \{A. P.\} and F. Riccobono and L. Rondo and Gerhard Steiner and A. Tome and H. Walther and U. Baltensperger and Carslaw, \{K. S.\} and J. Dommen and A. Hansel and T. Petaja and M. Sipila and F. Stratmann and A. Vrtala and Wagner, \{P. E.\} and Worsnop, \{D. R.\} and J. Curtius and M. Kulmala",

year = "2016",

month = feb,

day = "16",

doi = "10.1002/2015JD023539",

language = "English",

volume = "121",

pages = "1752--1775",

journal = "Journal of Geophysical Research: Atmospheres",

issn = "2169-897X",

publisher = "AMER GEOPHYSICAL UNION",

number = "4",

}

Duplissy, J, Merikanto, J, Franchin, A, Tsagkogeorgas, G, Kangasluoma, J, Wimmer, D, Vuollekoski, H, Schobesberger, S, Lehtipalo, K, Flagan, RC, Brus, D, Donahue, NM, Vehkamaki, H, Almeida, J, Amorim, A, Barmet, P, Bianchi, F, Breitenlechner, M, Dunne, EM, Guida, R, Henschel, H, Junninen, H, Kirkby, J, Kuerten, A, Kupc, A, Määttänen, A, Makhmutov, V, Mathot, S, Nieminen, T, Onnela, A, Praplan, AP, Riccobono, F, Rondo, L, Steiner, G, Tome, A, Walther, H, Baltensperger, U, Carslaw, KS, Dommen, J, Hansel, A, Petaja, T, Sipila, M, Stratmann, F, Vrtala, A, Wagner, PE, Worsnop, DR, Curtius, J & Kulmala, M 2016, 'Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory', Journal of Geophysical Research: Atmospheres, vol. 121, no. 4, pp. 1752-1775. https://doi.org/10.1002/2015JD023539

TY - JOUR

T1 - Effect of ions on sulfuric acid-water binary particle formation

T2 - 2. Experimental data and comparison with QC-normalized classical nucleation theory

AU - Duplissy, J.

AU - Merikanto, J.

AU - Franchin, A.

AU - Tsagkogeorgas, G.

AU - Kangasluoma, J.

AU - Wimmer, Daniela

AU - Vuollekoski, H.

AU - Schobesberger, S.

AU - Lehtipalo, K.

AU - Flagan, R. C.

AU - Brus, D.

AU - Donahue, N. M.

AU - Vehkamaki, H.

AU - Almeida, J.

AU - Amorim, A.

AU - Barmet, P.

AU - Bianchi, F.

AU - Breitenlechner, M.

AU - Dunne, E. M.

AU - Guida, R.

AU - Henschel, H.

AU - Junninen, H.

AU - Kirkby, J.

AU - Kuerten, A.

AU - Kupc, A.

AU - Määttänen, Anni

AU - Makhmutov, V.

AU - Mathot, S.

AU - Nieminen, T.

AU - Onnela, A.

AU - Praplan, A. P.

AU - Riccobono, F.

AU - Rondo, L.

AU - Steiner, Gerhard

AU - Tome, A.

AU - Walther, H.

AU - Baltensperger, U.

AU - Carslaw, K. S.

AU - Dommen, J.

AU - Hansel, A.

AU - Petaja, T.

AU - Sipila, M.

AU - Stratmann, F.

AU - Vrtala, A.

AU - Wagner, P. E.

AU - Worsnop, D. R.

AU - Curtius, J.

AU - Kulmala, M.

PY - 2016/2/16

Y1 - 2016/2/16

N2 - We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (10(5) to 10(9)molcm(-3)), relative humidity (11% to 58%), temperature (207K to 299K), and total ion concentration (0 to 6800ionscm(-3)). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3nm to 3.2nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.

AB - We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (10(5) to 10(9)molcm(-3)), relative humidity (11% to 58%), temperature (207K to 299K), and total ion concentration (0 to 6800ionscm(-3)). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3nm to 3.2nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.

KW - binary particle formation

KW - ion-induced nucleation

KW - sulfuric acid

KW - classical nucleation theory

KW - ATMOSPHERIC AEROSOL NUCLEATION

KW - IONIZATION MASS-SPECTROMETER

KW - HOMOGENEOUS NUCLEATION

KW - HYDRATE FORMATION

KW - VAPOR-PRESSURE

KW - BOREAL FOREST

KW - CLOUD CHAMBER

KW - CHEMICAL-COMPOSITION

KW - OXIDATION-PRODUCTS

KW - EXPERIMENTAL SETUP

UR - https://www.scopus.com/pages/publications/84957309741

U2 - 10.1002/2015JD023539

DO - 10.1002/2015JD023539

M3 - Article

SN - 2169-897X

VL - 121

SP - 1752

EP - 1775

JO - Journal of Geophysical Research: Atmospheres

JF - Journal of Geophysical Research: Atmospheres

IS - 4

ER -

Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory

Abstract

Funding

Austrian Fields of Science 2012

Keywords

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