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Title: The effect of acid–base clustering and ions on the growth of atmospheric nano-particles

Abstract

The growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. Furthermore, we bring these observations into a coherent framework and discuss their significance in the atmosphere.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [2];  [4];  [3];  [5];  [6];  [5];  [7]; ORCiD logo [8];  [3];  [9];  [10];  [11]; ORCiD logo [12];  [13] more »;  [6];  [14];  [15];  [14];  [11];  [3];  [16];  [13];  [3];  [3];  [17];  [18]; ORCiD logo [2];  [19];  [3];  [20];  [21];  [2];  [22];  [3];  [3];  [22];  [3];  [1];  [3];  [3];  [11];  [3];  [13];  [2];  [21];  [6];  [23];  [11];  [18];  [3];  [19];  [19];  [2];  [24];  [19];  [18]; ORCiD logo [25];  [26];  [6];  [9];  [2];  [27];  [5] « less
  1. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Paul Scherrer Inst., Villigen (Switzerland). Laboratory of Atmospheric Chemistry
  2. Goethe-Univ. of Frankfurt, Frankfurt am Main (Germany). Inst. for Atmospheric and Environmental Sciences
  3. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics
  4. Goethe-Univ. of Frankfurt, Frankfurt am Main (Germany). Inst. for Atmospheric and Environmental Sciences; CERN, Geneva (Switzerland)
  5. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics, Inst. of Physics
  6. Paul Scherrer Inst., Villigen (Switzerland). Laboratory of Atmospheric Chemistry
  7. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  8. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics, Inst. of Physics; CERN, Geneva (Switzerland)
  9. Stockholm Univ., Stockholm (Sweden). Dept. of Environmental Science and Analytical Chemistry (ACES) & Bolin Centre for Climate Research
  10. CERN, Geneva (Switzerland); Univ. of Lisbon and Univ. of Beira Interior, Lisbon (Portugal). SIM
  11. Univ. of Lisbon and Univ. of Beira Interior, Lisbon (Portugal). SIM
  12. Paul Scherrer Inst., Villigen (Switzerland). Laboratory of Atmospheric Chemistry; ETH Zurich, Zurich (Switzerland). Inst. for Atmospheric and Climate Science
  13. TechnikerstraBe 25, Innsbruck (Austria). Inst. for Ion Physics and Applied Physics
  14. California Inst. of Technology, Pasadena, CA (United States). Div. of Chemistry and Chemical Engineering
  15. Univ. of Leeds, Leeds (United Kingdom). School of Earth and Environment;Atmospheric Research Centre of Eastern Finland, Kuopio (Finland). Finnish Meteorological Inst.
  16. TechnikerstraBe 25, Innsbruck (Austria). Inst. for Ion Physics and Applied Physics; Ionicon Analytik GmbH, Innsbruck (Austria)
  17. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics;Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  18. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  19. Univ. of Vienna, Vienna (Austria). Faculty of Physics
  20. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics; Finnish Meteorological Inst., Helsinki (Finland)
  21. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics; Univ. of California, Irvine, CA (United States). Dept. of Chemistry
  22. CERN, Geneva (Switzerland)
  23. Leibniz Inst. for Tropospheric Research, Leipzig (Germany)
  24. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Goethe-Univ. of Frankfurt, Frankfurt am Main (Germany). Inst. for Atmospheric and Environmental Sciences
  25. Carnegie Mellon Univ., Pittsburgh, PA (United States). Center for Atmospheric Particle Studies
  26. Univ. of Leeds, Leeds (United Kingdom). School of Earth and Environment
  27. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics; Atmospheric Research Centre of Eastern Finland, Kuopio (Finland). Finnish Meteorological Inst.; Aerodyne Research Inc., Billerica, MA (United States)
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE; CERN; European Union (EU); German Federal Ministry of Education and Research (BMBF); Swiss National Science Foundation (SNSF); Academy of Finland, Center of Excellence program; Austrian Science Fund (FWF); Portuguese Foundation for Science and Technology; Swedish Research Council (SRC); Russian Foundation for Basic Research; National Science Foundation (NSF); Vaisala foundation; EC Seventh Framework Programme (Marie Curie Initial Training Network 'CLOUD-ITN'); EC Seventh Framework Programme (Marie Curie Initial Training Network 'CLOUD-TRAIN'); EC Seventh Framework Programme (ERC grant 'ATMOGAIN'); EC Seventh Framework Programme (ERC grant 'MOCAPAF'; EC Seventh Framework Programme (ERC grant 'NANODYNAMITE'); EC Seventh Framework Programme (ERC grant 'ATMNUCLE')
OSTI Identifier:
1270918
Grant/Contract Number:  
SC0014469
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ionization mass-spectrometry; phase sulfuric-acid; neutral cluster; boreal forest; cloud chamber; size range; nucleation; rates; ammonia; aerosol

Citation Formats

Lehtipalo, Katrianne, Rondo, Linda, Kontkanen, Jenni, Schobesberger, Siegfried, Jokinen, Tuija, Sarnela, Nina, Kürten, Andreas, Ehrhart, Sebastian, Franchin, Alessandro, Nieminen, Tuomo, Riccobono, Francesco, Sipilä, Mikko, Yli-Juuti, Taina, Duplissy, Jonathan, Adamov, Alexey, Ahlm, Lars, Almeida, Joao, Amorim, Antonio, Bianchi, Federico, Breitenlechner, Martin, Dommen, Josef, Downard, Andrew J., Dunne, Eimear M., Flagan, Richard C., Guida, Roberto, Hakala, Jani, Hansel, Armin, Jud, Werner, Kangasluoma, Juha, Kerminen, Veli-Matti, Keskinen, Helmi, Kim, Jaeseok, Kirkby, Jasper, Kupc, Agnieszka, Kupiainen-Maatta, Oona, Laaksonen, Ari, Lawler, Michael J., Leiminger, Markus, Mathot, Serge, Olenius, Tinja, Ortega, Ismael K., Onnela, Antti, Petaja, Tuukka, Praplan, Arnaud, Rissanen, Matti P., Ruuskanen, Taina, Santos, Filipe D., Schallhart, Simon, Schnitzhofer, Ralf, Simon, Mario, Smith, James N., Trostl, Jasmin, Tsagkogeorgas, Georgios, Tomé, António, Vaattovaara, Petri, Vehkamaki, Hanna, Vrtala, Aron E., Wagner, Paul E., Williamson, Christina, Wimmer, Daniela, Winkler, Paul M., Virtanen, Annele, Donahue, Neil M., Carslaw, Kenneth S., Baltensperger, Urs, Riipinen, Ilona, Curtius, Joachim, Worsnop, Douglas R., and Kulmala, Markku. The effect of acid–base clustering and ions on the growth of atmospheric nano-particles. United States: N. p., 2016. Web. doi:10.1038/ncomms11594.
Lehtipalo, Katrianne, Rondo, Linda, Kontkanen, Jenni, Schobesberger, Siegfried, Jokinen, Tuija, Sarnela, Nina, Kürten, Andreas, Ehrhart, Sebastian, Franchin, Alessandro, Nieminen, Tuomo, Riccobono, Francesco, Sipilä, Mikko, Yli-Juuti, Taina, Duplissy, Jonathan, Adamov, Alexey, Ahlm, Lars, Almeida, Joao, Amorim, Antonio, Bianchi, Federico, Breitenlechner, Martin, Dommen, Josef, Downard, Andrew J., Dunne, Eimear M., Flagan, Richard C., Guida, Roberto, Hakala, Jani, Hansel, Armin, Jud, Werner, Kangasluoma, Juha, Kerminen, Veli-Matti, Keskinen, Helmi, Kim, Jaeseok, Kirkby, Jasper, Kupc, Agnieszka, Kupiainen-Maatta, Oona, Laaksonen, Ari, Lawler, Michael J., Leiminger, Markus, Mathot, Serge, Olenius, Tinja, Ortega, Ismael K., Onnela, Antti, Petaja, Tuukka, Praplan, Arnaud, Rissanen, Matti P., Ruuskanen, Taina, Santos, Filipe D., Schallhart, Simon, Schnitzhofer, Ralf, Simon, Mario, Smith, James N., Trostl, Jasmin, Tsagkogeorgas, Georgios, Tomé, António, Vaattovaara, Petri, Vehkamaki, Hanna, Vrtala, Aron E., Wagner, Paul E., Williamson, Christina, Wimmer, Daniela, Winkler, Paul M., Virtanen, Annele, Donahue, Neil M., Carslaw, Kenneth S., Baltensperger, Urs, Riipinen, Ilona, Curtius, Joachim, Worsnop, Douglas R., & Kulmala, Markku. The effect of acid–base clustering and ions on the growth of atmospheric nano-particles. United States. doi:10.1038/ncomms11594.
Lehtipalo, Katrianne, Rondo, Linda, Kontkanen, Jenni, Schobesberger, Siegfried, Jokinen, Tuija, Sarnela, Nina, Kürten, Andreas, Ehrhart, Sebastian, Franchin, Alessandro, Nieminen, Tuomo, Riccobono, Francesco, Sipilä, Mikko, Yli-Juuti, Taina, Duplissy, Jonathan, Adamov, Alexey, Ahlm, Lars, Almeida, Joao, Amorim, Antonio, Bianchi, Federico, Breitenlechner, Martin, Dommen, Josef, Downard, Andrew J., Dunne, Eimear M., Flagan, Richard C., Guida, Roberto, Hakala, Jani, Hansel, Armin, Jud, Werner, Kangasluoma, Juha, Kerminen, Veli-Matti, Keskinen, Helmi, Kim, Jaeseok, Kirkby, Jasper, Kupc, Agnieszka, Kupiainen-Maatta, Oona, Laaksonen, Ari, Lawler, Michael J., Leiminger, Markus, Mathot, Serge, Olenius, Tinja, Ortega, Ismael K., Onnela, Antti, Petaja, Tuukka, Praplan, Arnaud, Rissanen, Matti P., Ruuskanen, Taina, Santos, Filipe D., Schallhart, Simon, Schnitzhofer, Ralf, Simon, Mario, Smith, James N., Trostl, Jasmin, Tsagkogeorgas, Georgios, Tomé, António, Vaattovaara, Petri, Vehkamaki, Hanna, Vrtala, Aron E., Wagner, Paul E., Williamson, Christina, Wimmer, Daniela, Winkler, Paul M., Virtanen, Annele, Donahue, Neil M., Carslaw, Kenneth S., Baltensperger, Urs, Riipinen, Ilona, Curtius, Joachim, Worsnop, Douglas R., and Kulmala, Markku. Fri . "The effect of acid–base clustering and ions on the growth of atmospheric nano-particles". United States. doi:10.1038/ncomms11594. https://www.osti.gov/servlets/purl/1270918.
@article{osti_1270918,
title = {The effect of acid–base clustering and ions on the growth of atmospheric nano-particles},
author = {Lehtipalo, Katrianne and Rondo, Linda and Kontkanen, Jenni and Schobesberger, Siegfried and Jokinen, Tuija and Sarnela, Nina and Kürten, Andreas and Ehrhart, Sebastian and Franchin, Alessandro and Nieminen, Tuomo and Riccobono, Francesco and Sipilä, Mikko and Yli-Juuti, Taina and Duplissy, Jonathan and Adamov, Alexey and Ahlm, Lars and Almeida, Joao and Amorim, Antonio and Bianchi, Federico and Breitenlechner, Martin and Dommen, Josef and Downard, Andrew J. and Dunne, Eimear M. and Flagan, Richard C. and Guida, Roberto and Hakala, Jani and Hansel, Armin and Jud, Werner and Kangasluoma, Juha and Kerminen, Veli-Matti and Keskinen, Helmi and Kim, Jaeseok and Kirkby, Jasper and Kupc, Agnieszka and Kupiainen-Maatta, Oona and Laaksonen, Ari and Lawler, Michael J. and Leiminger, Markus and Mathot, Serge and Olenius, Tinja and Ortega, Ismael K. and Onnela, Antti and Petaja, Tuukka and Praplan, Arnaud and Rissanen, Matti P. and Ruuskanen, Taina and Santos, Filipe D. and Schallhart, Simon and Schnitzhofer, Ralf and Simon, Mario and Smith, James N. and Trostl, Jasmin and Tsagkogeorgas, Georgios and Tomé, António and Vaattovaara, Petri and Vehkamaki, Hanna and Vrtala, Aron E. and Wagner, Paul E. and Williamson, Christina and Wimmer, Daniela and Winkler, Paul M. and Virtanen, Annele and Donahue, Neil M. and Carslaw, Kenneth S. and Baltensperger, Urs and Riipinen, Ilona and Curtius, Joachim and Worsnop, Douglas R. and Kulmala, Markku},
abstractNote = {The growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. Furthermore, we bring these observations into a coherent framework and discuss their significance in the atmosphere.},
doi = {10.1038/ncomms11594},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {5}
}

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    • Journal of Geophysical Research: Atmospheres, Vol. 124, Issue 13
    • DOI: 10.1029/2018jd029356

    Chemical accuracy in modeling halide ion hydration from many-body representations
    journal, January 2019


    Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD
    journal, January 2016

    • Lawler, Michael J.; Winkler, Paul M.; Kim, Jaeseok
    • Atmospheric Chemistry and Physics, Vol. 16, Issue 21
    • DOI: 10.5194/acp-16-13601-2016

    Measurements of sub-3 nm particles using a particle size magnifier in different environments: from clean mountain top to polluted megacities
    journal, January 2017

    • Kontkanen, Jenni; Lehtipalo, Katrianne; Ahonen, Lauri
    • Atmospheric Chemistry and Physics, Vol. 17, Issue 3
    • DOI: 10.5194/acp-17-2163-2017

    Temperature effects on sulfuric acid aerosol nucleation and growth: initial results from the TANGENT study
    journal, January 2019

    • Tiszenkel, Lee; Stangl, Chris; Krasnomowitz, Justin
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 13
    • DOI: 10.5194/acp-19-8915-2019