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Title: Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures

Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10 5 and 1 × 10 9cm -3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximumof ~1400 parts per trillion by volume (pptv).We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm -3 s -1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperaturesmore » between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH 3 levels. In conclusion, we compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [7] ;  [8] ;  [9] ;  [8] ;  [10] ;  [11] ; ORCiD logo [4] ;  [12] ;  [4] ;  [9] ;  [1] ;  [13] ;  [4] ;  [4] more »;  [14] ;  [3] ;  [15] ;  [16] ;  [1] ;  [17] ;  [12] ;  [18] ;  [4] ; ORCiD logo [19] ;  [8] ;  [4] ;  [1] ;  [9] ;  [20] ;  [21] ;  [22] ;  [17] ;  [23] ;  [8] ;  [24] ;  [25] ;  [26] ;  [10] ;  [8] ;  [27] ;  [4] ;  [1] « less
  1. Goethe Univ., Frankfurt (Germany). Inst. for Atmospheric and Environmental Sciences
  2. Paul Scherrer Inst., Villigen (Switzerland). Lab. of Atmospheric Chemistry; Federal Inst. of Technology, Zurich (Switzerland). Inst. of Atmospheric and Climate Science; Univ. of Helsinki (Finland). Dept. of Physics
  3. Goethe Univ., Frankfurt (Germany). Inst. for Atmospheric and Environmental Sciences; European Organization for Nuclear Research (CERN), Geneva (Switzerland). Physics Dept.
  4. Univ. of Helsinki (Finland). Dept. of Physics
  5. Univ. of Leeds (United Kingdom). School of Earth and Environment; Finnish Meteorological Inst., Kuopio (Finland). Atmospheric Research Centre of Eastern Finland
  6. Univ. of Helsinki (Finland). Dept. of Physics; European Organization for Nuclear Research (CERN), Geneva (Switzerland). Physics Dept.
  7. Goethe Univ., Frankfurt (Germany). Inst. for Atmospheric and Environmental Sciences; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences
  8. Paul Scherrer Inst., Villigen (Switzerland). Lab. of Atmospheric Chemistry
  9. Univ. of Innsbruck (Austria). Inst. for Ion and Applied Physics; Ionicon Analytik GmbH, Innsbruck (Austria)
  10. Carnegie Mellon Univ., Pittsburgh, PA (United States). Center for Atmospheric Particle Studies
  11. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering
  12. European Organization for Nuclear Research (CERN), Geneva (Switzerland). Physics Dept.
  13. Goethe Univ., Frankfurt (Germany). Inst. for Atmospheric and Environmental Sciences; Federal Inst. of Technology, Zurich (Switzerland). Inst. of Atmospheric and Climate Science
  14. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  15. Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences; Univ. of Vienna (Austria). Faculty of Physics
  16. Paul Scherrer Inst., Villigen (Switzerland). Lab. of Atmospheric Chemistry; Univ. of Helsinki (Finland). Dept. of Physics
  17. Lebedev Physical Inst., Moscow (Russia). Solar and Cosmic Ray Research Lab.
  18. Univ. of Helsinki (Finland). Dept. of Physics; Onera-The French Aerospace Lab., Palaiseau (France)
  19. Paul Scherrer Inst., Villigen (Switzerland). Lab. of Atmospheric Chemistry; Finnish Meteorological Inst., Helsinki (Finland)
  20. Univ. of Helsinki (Finland). Dept. of Physics; Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences
  21. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics; Univ. of California, Irvine, CA (United States). Dept. of Chemistry
  22. Univ. of Helsinki (Finland). Dept. of Helsinki; Univ. of Innsbruck (Austria). Inst. for Ion and Applied Physics; Univ. of Vienna (Austria). Faculty of Physics
  23. Univ. of Lisbon (Portugal). Scientific and Space Instrumentation and Modeling (SIM); Univ. of Beira Interior, Lisbon (Portugal)
  24. Leibniz Inst. for Tropospheric Research (ITR), Leipzig (Germany)
  25. Univ. of Vienna (Austria). Faculty of Physics
  26. Goethe Univ., Frankfurt (Germany). Inst. for Atmospheric and Environmental Sciences; Univ. of Helsinki (Finland). Dept. of Physics
  27. Univ. of Leeds (United Kingdom). School of Earth and Environment
Publication Date:
Grant/Contract Number:
SC0014469; AGS1447056; AGS1439551; 1133872; 251007
Type:
Published Article
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Volume: 121; Journal Issue: 20; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union
Research Org:
Univ. of California, Irvine, CA (United States)
Sponsoring Org:
USDOE; National Science Foundation (NSF); Swiss National Science Foundation (SNSF); European Union (EU)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES
OSTI Identifier:
1330276
Alternate Identifier(s):
OSTI ID: 1330394; OSTI ID: 1425930

Kürten, Andreas, Bianchi, Federico, Almeida, Joao, Kupiainen-Määttä, Oona, Dunne, Eimear M., Duplissy, Jonathan, Williamson, Christina, Barmet, Peter, Breitenlechner, Martin, Dommen, Josef, Donahue, Neil M., Flagan, Richard C., Franchin, Alessandro, Gordon, Hamish, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Ickes, Luisa, Jokinen, Tuija, Kangasluoma, Juha, Kim, Jaeseok, Kirkby, Jasper, Kupc, Agnieszka, Lehtipalo, Katrianne, Leiminger, Markus, Makhmutov, Vladimir, Onnela, Antti, Ortega, Ismael K., Petäjä, Tuukka, Praplan, Arnaud P., Riccobono, Francesco, Rissanen, Matti P., Rondo, Linda, Schnitzhofer, Ralf, Schobesberger, Siegfried, Smith, James N., Steiner, Gerhard, Stozhkov, Yuri, Tomé, António, Tröstl, Jasmin, Tsagkogeorgas, Georgios, Wagner, Paul E., Wimmer, Daniela, Ye, Penglin, Baltensperger, Urs, Carslaw, Ken, Kulmala, Markku, and Curtius, Joachim. Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures. United States: N. p., Web. doi:10.1002/2015JD023908.
Kürten, Andreas, Bianchi, Federico, Almeida, Joao, Kupiainen-Määttä, Oona, Dunne, Eimear M., Duplissy, Jonathan, Williamson, Christina, Barmet, Peter, Breitenlechner, Martin, Dommen, Josef, Donahue, Neil M., Flagan, Richard C., Franchin, Alessandro, Gordon, Hamish, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Ickes, Luisa, Jokinen, Tuija, Kangasluoma, Juha, Kim, Jaeseok, Kirkby, Jasper, Kupc, Agnieszka, Lehtipalo, Katrianne, Leiminger, Markus, Makhmutov, Vladimir, Onnela, Antti, Ortega, Ismael K., Petäjä, Tuukka, Praplan, Arnaud P., Riccobono, Francesco, Rissanen, Matti P., Rondo, Linda, Schnitzhofer, Ralf, Schobesberger, Siegfried, Smith, James N., Steiner, Gerhard, Stozhkov, Yuri, Tomé, António, Tröstl, Jasmin, Tsagkogeorgas, Georgios, Wagner, Paul E., Wimmer, Daniela, Ye, Penglin, Baltensperger, Urs, Carslaw, Ken, Kulmala, Markku, & Curtius, Joachim. Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures. United States. doi:10.1002/2015JD023908.
Kürten, Andreas, Bianchi, Federico, Almeida, Joao, Kupiainen-Määttä, Oona, Dunne, Eimear M., Duplissy, Jonathan, Williamson, Christina, Barmet, Peter, Breitenlechner, Martin, Dommen, Josef, Donahue, Neil M., Flagan, Richard C., Franchin, Alessandro, Gordon, Hamish, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Ickes, Luisa, Jokinen, Tuija, Kangasluoma, Juha, Kim, Jaeseok, Kirkby, Jasper, Kupc, Agnieszka, Lehtipalo, Katrianne, Leiminger, Markus, Makhmutov, Vladimir, Onnela, Antti, Ortega, Ismael K., Petäjä, Tuukka, Praplan, Arnaud P., Riccobono, Francesco, Rissanen, Matti P., Rondo, Linda, Schnitzhofer, Ralf, Schobesberger, Siegfried, Smith, James N., Steiner, Gerhard, Stozhkov, Yuri, Tomé, António, Tröstl, Jasmin, Tsagkogeorgas, Georgios, Wagner, Paul E., Wimmer, Daniela, Ye, Penglin, Baltensperger, Urs, Carslaw, Ken, Kulmala, Markku, and Curtius, Joachim. 2016. "Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures". United States. doi:10.1002/2015JD023908.
@article{osti_1330276,
title = {Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures},
author = {Kürten, Andreas and Bianchi, Federico and Almeida, Joao and Kupiainen-Määttä, Oona and Dunne, Eimear M. and Duplissy, Jonathan and Williamson, Christina and Barmet, Peter and Breitenlechner, Martin and Dommen, Josef and Donahue, Neil M. and Flagan, Richard C. and Franchin, Alessandro and Gordon, Hamish and Hakala, Jani and Hansel, Armin and Heinritzi, Martin and Ickes, Luisa and Jokinen, Tuija and Kangasluoma, Juha and Kim, Jaeseok and Kirkby, Jasper and Kupc, Agnieszka and Lehtipalo, Katrianne and Leiminger, Markus and Makhmutov, Vladimir and Onnela, Antti and Ortega, Ismael K. and Petäjä, Tuukka and Praplan, Arnaud P. and Riccobono, Francesco and Rissanen, Matti P. and Rondo, Linda and Schnitzhofer, Ralf and Schobesberger, Siegfried and Smith, James N. and Steiner, Gerhard and Stozhkov, Yuri and Tomé, António and Tröstl, Jasmin and Tsagkogeorgas, Georgios and Wagner, Paul E. and Wimmer, Daniela and Ye, Penglin and Baltensperger, Urs and Carslaw, Ken and Kulmala, Markku and Curtius, Joachim},
abstractNote = {Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 105 and 1 × 109cm-3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximumof ~1400 parts per trillion by volume (pptv).We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm-3 s-1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH3 levels. In conclusion, we compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.},
doi = {10.1002/2015JD023908},
journal = {Journal of Geophysical Research: Atmospheres},
number = 20,
volume = 121,
place = {United States},
year = {2016},
month = {10}
}