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Title: New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

Here, a recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up toca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (~100)relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlledmore » (a.k.a.kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 10 6 and 3 × 10 7 cm -3, and dimethylamine mixing ratio of ~ 40 pptv, i.e., 1 × 10 9 cm -3).« less
Authors:
 [1] ;  [2] ; ORCiD logo [3] ; ORCiD logo [1] ;  [4] ; ORCiD logo [5] ;  [3] ; ORCiD logo [6] ;  [3] ; ORCiD logo [3] ; ORCiD logo [7] ; ORCiD logo [3] ; ORCiD logo [8] ; ORCiD logo [9] ;  [10] ;  [11] ; ORCiD logo [3] ;  [1] ;  [3] ;  [10] more »;  [12] ; ORCiD logo [13] ;  [2] « less
  1. Goethe Univ. Frankfurt, Frankfurt am Main (Germany)
  2. Univ. of Minnesota, Minneapolis, MN (United States)
  3. Univ. of Helsinki, Helsinki (Finland)
  4. Univ. of Lisbon, Lisbon (Portugal)
  5. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  6. California Institute of Technology, Pasadena, CA (United States)
  7. Goethe Univ. Frankfurt, Frankfurt am Main (Germany); European Organization for Nuclear Research (CERN), Geneva (Switzerland)
  8. Finnish Meteorological Inst., Helsinki (Finland)
  9. Univ. of Helsinki, Helsinki (Finland); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  10. Lebedev Physical Inst., Moscow (Russia)
  11. European Organization for Nuclear Research (CERN), Geneva (Switzerland)
  12. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  13. Carnegie Mellon Univ., Pittsburgh, PA (United States); Aerodyne Research Inc., Billerica, MA (United States)
Publication Date:
Grant/Contract Number:
SC0011780
Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 18; Journal Issue: 2; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Research Org:
Colorado State Univ., Fort Collins, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1502082

Kürten, Andreas, Li, Chenxi, Bianchi, Federico, Curtius, Joachim, Dias, António, Donahue, Neil M., Duplissy, Jonathan, Flagan, Richard C., Hakala, Jani, Jokinen, Tuija, Kirkby, Jasper, Kulmala, Markku, Laaksonen, Ari, Lehtipalo, Katrianne, Makhmutov, Vladimir, Onnela, Antti, Rissanen, Matti P., Simon, Mario, Sipilä, Mikko, Stozhkov, Yuri, Tröstl, Jasmin, Ye, Penglin, and McMurry, Peter H.. New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model. United States: N. p., Web. doi:10.5194/acp-18-845-2018.
Kürten, Andreas, Li, Chenxi, Bianchi, Federico, Curtius, Joachim, Dias, António, Donahue, Neil M., Duplissy, Jonathan, Flagan, Richard C., Hakala, Jani, Jokinen, Tuija, Kirkby, Jasper, Kulmala, Markku, Laaksonen, Ari, Lehtipalo, Katrianne, Makhmutov, Vladimir, Onnela, Antti, Rissanen, Matti P., Simon, Mario, Sipilä, Mikko, Stozhkov, Yuri, Tröstl, Jasmin, Ye, Penglin, & McMurry, Peter H.. New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model. United States. doi:10.5194/acp-18-845-2018.
Kürten, Andreas, Li, Chenxi, Bianchi, Federico, Curtius, Joachim, Dias, António, Donahue, Neil M., Duplissy, Jonathan, Flagan, Richard C., Hakala, Jani, Jokinen, Tuija, Kirkby, Jasper, Kulmala, Markku, Laaksonen, Ari, Lehtipalo, Katrianne, Makhmutov, Vladimir, Onnela, Antti, Rissanen, Matti P., Simon, Mario, Sipilä, Mikko, Stozhkov, Yuri, Tröstl, Jasmin, Ye, Penglin, and McMurry, Peter H.. 2018. "New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model". United States. doi:10.5194/acp-18-845-2018. https://www.osti.gov/servlets/purl/1502082.
@article{osti_1502082,
title = {New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model},
author = {Kürten, Andreas and Li, Chenxi and Bianchi, Federico and Curtius, Joachim and Dias, António and Donahue, Neil M. and Duplissy, Jonathan and Flagan, Richard C. and Hakala, Jani and Jokinen, Tuija and Kirkby, Jasper and Kulmala, Markku and Laaksonen, Ari and Lehtipalo, Katrianne and Makhmutov, Vladimir and Onnela, Antti and Rissanen, Matti P. and Simon, Mario and Sipilä, Mikko and Stozhkov, Yuri and Tröstl, Jasmin and Ye, Penglin and McMurry, Peter H.},
abstractNote = {Here, a recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up toca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (~100)relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a.kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 106 and 3 × 107 cm-3, and dimethylamine mixing ratio of ~ 40 pptv, i.e., 1 × 109 cm-3).},
doi = {10.5194/acp-18-845-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 2,
volume = 18,
place = {United States},
year = {2018},
month = {1}
}