Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

J. Kim; L. Ahlm; T. Yli-Juuti; M. Lawler; H. Keskinen; J. Tröstl; S. Schobesberger; J. Duplissy; A. Amorim; F. Bianchi; N. M. Donahue; R. C. Flagan; J. Hakala; M. Heinritzi; T. Jokinen; A. Kürten; A. Laaksonen; K. Lehtipalo; P. Miettinen; T. Petäjä; M. P. Rissanen; L. Rondo; K. Sengupta; M. Simon; A. Tome; C. Williamson; D. Wimmer; P. M. Winkler; S. Ehrhart; P. Ye; J. Kirkby; J. Curtius; U. Baltensperger; M. Kulmala; K. E. J. Lehtinen; J. N. Smith; I. Riipinen; A. Virtanen

doi:10.5194/acp-16-293-2016

Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

J. Kim
, L. Ahlm
, T. Yli-Juuti
, M. Lawler
, H. Keskinen
, J. Tröstl
, S. Schobesberger
, J. Duplissy
, A. Amorim
, F. Bianchi
, N. M. Donahue
, R. C. Flagan
, J. Hakala
, M. Heinritzi
, T. Jokinen
, A. Kürten
, A. Laaksonen
, K. Lehtipalo
, P. Miettinen
, T. Petäjä

M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tome, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, A. Virtanen (Corresponding author)

Aerosol Physics and Environmental Physics

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15gnm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90g% relative humidity at 293gK) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10gnm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15gnm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106gmoleculesgcmg'3 in the gas phase, and the dimethylamine mixing ratio was 11.8gppt, the measured of 15gnm particles was 0.31g±g0.01: close to the value reported for dimethylaminium sulfate (DMAS) (DMAS g1/4 0.28). Furthermore, the difference in between sulfuric acid and sulfuric acid-imethylamine experiments increased with increasing particle size. The values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10gnm sizes.

Original language	English
Pages (from-to)	293-304
Number of pages	12
Journal	Atmospheric Chemistry and Physics
Volume	16
Issue number	1
DOIs	https://doi.org/10.5194/acp-16-293-2016
Publication status	Published - 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, 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. We thank the CSC Centre for Scientific Computing in Espoo, Finland, for computer time. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network CLOUD-ITN no. 215072, MC-ITN CLOUD-TRAIN no. 316662, ERC Starting Grant MOCAPAF no. 57360, ERC Consolidator Grant NANODYNAMITE no. 616075, ERC Advanced Grant ATMNUCLE no. 227463, and ERC Starting Grant "QAPPA" grant no. 335478); the German Federal Ministry of Education and Research (project nos. 01LK0902A and 01LK1222A); the Swiss National Science Foundation (project nos. 200020 135307, 200021 140663, 206021 144947/1, 20FI20 149002/1, and 200021 140663); the Academy of Finland Centre of Excellence program (project no. 1118615); the Academy of Finland (135054, 133872, 251427, 1389515, 139656, 139995, 137749, 141217, 141451, 2720541, 259005, 264989); the Finnish Funding Agency for Technology and Innovation; the Nessling Foundation; the Strategic Funding from University of Eastern Finland; the Austrian Science Fund (FWF; project no. P19546 and L59321); the Portuguese Foundation for Science and Technology (project no. 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 and CHE1012293); a Davidow Grant to Caltech's Global Environmental Science Program; Dreyfus Award EP-11-117; the French National Research Agency (ANR); the Nord-Pas de Calais; the European Funds for Regional Economic Development (FEDER, Labex-Cappa, ANR-11-LABX-0005-01); and the French Civil Aviation Office (MERMOSE).

Austrian Fields of Science 2012

103039 Aerosol physics

Keywords

SECONDARY ORGANIC AEROSOL
DIFFERENTIAL MOBILITY ANALYZER
IONIZATION MASS-SPECTROMETRY
SULFURIC ACID-AMINE
ALPHA-PINENE
PARTICLE FORMATION
ATMOSPHERIC CONDITIONS
CHEMICAL-COMPOSITION
ULTRAFINE PARTICLES
OXIDATION-PRODUCTS

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10.5194/acp-16-293-2016Licence: CC BY 3.0

http://phaidra.univie.ac.at/o:527413Licence: CC BY 3.0

Cite this

Kim, J., Ahlm, L., Yli-Juuti, T., Lawler, M., Keskinen, H., Tröstl, J., Schobesberger, S., Duplissy, J., Amorim, A., Bianchi, F., Donahue, N. M., Flagan, R. C., Hakala, J., Heinritzi, M., Jokinen, T., Kürten, A., Laaksonen, A., Lehtipalo, K., Miettinen, P., ... Virtanen, A. (2016). Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments. Atmospheric Chemistry and Physics, 16(1), 293-304. https://doi.org/10.5194/acp-16-293-2016

@article{44b1a388fd3a4880966592804f198d18,

title = "Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments",

abstract = "Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15gnm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90g\% relative humidity at 293gK) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10gnm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15gnm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106gmoleculesgcmg'3 in the gas phase, and the dimethylamine mixing ratio was 11.8gppt, the measured of 15gnm particles was 0.31g±g0.01: close to the value reported for dimethylaminium sulfate (DMAS) (DMAS g1/4 0.28). Furthermore, the difference in between sulfuric acid and sulfuric acid-imethylamine experiments increased with increasing particle size. The values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10gnm sizes.",

keywords = "SECONDARY ORGANIC AEROSOL, DIFFERENTIAL MOBILITY ANALYZER, IONIZATION MASS-SPECTROMETRY, SULFURIC ACID-AMINE, ALPHA-PINENE, PARTICLE FORMATION, ATMOSPHERIC CONDITIONS, CHEMICAL-COMPOSITION, ULTRAFINE PARTICLES, OXIDATION-PRODUCTS",

author = "J. Kim and L. Ahlm and T. Yli-Juuti and M. Lawler and H. Keskinen and J. Tr{\"o}stl and S. Schobesberger and J. Duplissy and A. Amorim and F. Bianchi and Donahue, \{N. M.\} and Flagan, \{R. C.\} and J. Hakala and M. Heinritzi and T. Jokinen and A. K{\"u}rten and A. Laaksonen and K. Lehtipalo and P. Miettinen and T. Pet{\"a}j{\"a} and Rissanen, \{M. P.\} and L. Rondo and K. Sengupta and M. Simon and A. Tome and C. Williamson and D. Wimmer and Winkler, \{P. M.\} and S. Ehrhart and P. Ye and J. Kirkby and J. Curtius and U. Baltensperger and M. Kulmala and Lehtinen, \{K. E. J.\} and Smith, \{J. N.\} and I. Riipinen and A. Virtanen",

note = "Publisher Copyright: {\textcopyright} Author(s) 2016.",

year = "2016",

doi = "10.5194/acp-16-293-2016",

language = "English",

volume = "16",

pages = "293--304",

journal = "Atmospheric Chemistry and Physics",

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Kim, J, Ahlm, L, Yli-Juuti, T, Lawler, M, Keskinen, H, Tröstl, J, Schobesberger, S, Duplissy, J, Amorim, A, Bianchi, F, Donahue, NM, Flagan, RC, Hakala, J, Heinritzi, M, Jokinen, T, Kürten, A, Laaksonen, A, Lehtipalo, K, Miettinen, P, Petäjä, T, Rissanen, MP, Rondo, L, Sengupta, K, Simon, M, Tome, A, Williamson, C, Wimmer, D, Winkler, PM, Ehrhart, S, Ye, P, Kirkby, J, Curtius, J, Baltensperger, U, Kulmala, M, Lehtinen, KEJ, Smith, JN, Riipinen, I & Virtanen, A 2016, 'Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments', Atmospheric Chemistry and Physics, vol. 16, no. 1, pp. 293-304. https://doi.org/10.5194/acp-16-293-2016

TY - JOUR

T1 - Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

AU - Kim, J.

AU - Ahlm, L.

AU - Yli-Juuti, T.

AU - Lawler, M.

AU - Keskinen, H.

AU - Tröstl, J.

AU - Schobesberger, S.

AU - Duplissy, J.

AU - Amorim, A.

AU - Bianchi, F.

AU - Donahue, N. M.

AU - Flagan, R. C.

AU - Hakala, J.

AU - Heinritzi, M.

AU - Jokinen, T.

AU - Kürten, A.

AU - Laaksonen, A.

AU - Lehtipalo, K.

AU - Miettinen, P.

AU - Petäjä, T.

AU - Rissanen, M. P.

AU - Rondo, L.

AU - Sengupta, K.

AU - Simon, M.

AU - Tome, A.

AU - Williamson, C.

AU - Wimmer, D.

AU - Winkler, P. M.

AU - Ehrhart, S.

AU - Ye, P.

AU - Kirkby, J.

AU - Curtius, J.

AU - Baltensperger, U.

AU - Kulmala, M.

AU - Lehtinen, K. E. J.

AU - Smith, J. N.

AU - Riipinen, I.

AU - Virtanen, A.

PY - 2016

Y1 - 2016

N2 - Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15gnm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90g% relative humidity at 293gK) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10gnm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15gnm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106gmoleculesgcmg'3 in the gas phase, and the dimethylamine mixing ratio was 11.8gppt, the measured of 15gnm particles was 0.31g±g0.01: close to the value reported for dimethylaminium sulfate (DMAS) (DMAS g1/4 0.28). Furthermore, the difference in between sulfuric acid and sulfuric acid-imethylamine experiments increased with increasing particle size. The values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10gnm sizes.

AB - Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15gnm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90g% relative humidity at 293gK) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10gnm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15gnm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106gmoleculesgcmg'3 in the gas phase, and the dimethylamine mixing ratio was 11.8gppt, the measured of 15gnm particles was 0.31g±g0.01: close to the value reported for dimethylaminium sulfate (DMAS) (DMAS g1/4 0.28). Furthermore, the difference in between sulfuric acid and sulfuric acid-imethylamine experiments increased with increasing particle size. The values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10gnm sizes.

KW - SECONDARY ORGANIC AEROSOL

KW - DIFFERENTIAL MOBILITY ANALYZER

KW - IONIZATION MASS-SPECTROMETRY

KW - SULFURIC ACID-AMINE

KW - ALPHA-PINENE

KW - PARTICLE FORMATION

KW - ATMOSPHERIC CONDITIONS

KW - CHEMICAL-COMPOSITION

KW - ULTRAFINE PARTICLES

KW - OXIDATION-PRODUCTS

UR - https://www.scopus.com/pages/publications/84957309648

U2 - 10.5194/acp-16-293-2016

DO - 10.5194/acp-16-293-2016

M3 - Article

SN - 1680-7316

VL - 16

SP - 293

EP - 304

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

IS - 1

ER -

Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

Abstract

Funding

Austrian Fields of Science 2012

Keywords

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NANODYNAMITE: Quantifying Aerosol Nanoparticle Dynamics by High Time Resolution Experiments

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Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

Abstract

Funding

Austrian Fields of Science 2012

Keywords

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Fingerprint

Projects

NANODYNAMITE: Quantifying Aerosol Nanoparticle Dynamics by High Time Resolution Experiments

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