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Title: The role of low-volatility organic compounds in initial particle growth in the atmosphere

Abstract

About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absencemore » of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10-4.5 micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10-4.5 to 10-0.5 micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [1];  [6];  [1];  [7];  [5];  [4];  [8];  [9];  [10];  [5];  [5];  [3];  [11];  [11];  [4] more »;  [3];  [3];  [10];  [5];  [1];  [3];  [1];  [11];  [12];  [5];  [5];  [5];  [13];  [14];  [1];  [4];  [15];  [16];  [4];  [3];  [17];  [5];  [3];  [5];  [4];  [14];  [5];  [4];  [5];  [5];  [18];  [5];  [19];  [20];  [21];  [14];  [4];  [1];  [22];  [23];  [2];  [18];  [4];  [1];  [24];  [5];  [6];  [25];  [26];  [1] « less
+ Show Author Affiliations
  1. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  2. Carnegie Mellon University, Pittsburgh, PA (United States)
  3. European Organization for Nuclear Research (CERN), Geneva (Switzerland)
  4. Goethe University, Frankfurt (Germany)
  5. University of Helsinki (Finland)
  6. Stockholm University (Sweden)
  7. Paul Scherrer Inst. (PSI), Villigen (Switzerland); University of Helsinki (Finland); Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
  8. Paul Scherrer Inst. (PSI), Villigen (Switzerland); University of Helsinki (Finland)
  9. Goethe University, Frankfurt (Germany); National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States)
  10. California Institute of Technology (CalTech), Pasadena, CA (United States)
  11. University Innsbruck (Austria); Ionicon Analytik GmbH, Innsbruck (Austria)
  12. Paul Scherrer Inst. (PSI), Villigen (Switzerland); WSL Institute for Snow and Avalanche Research, Davos (Switzerland)
  13. University of Helsinki (Finland); University of Eastern Finland, Kuopio (Finland)
  14. University of Eastern Finland, Kuopio (Finland)
  15. University of Eastern Finland, Kuopio (Finland); Finnish Meteorological Institute, Helsinki (Finland)
  16. University of Eastern Finland, Kuopio (Finland); National Center for Atmospheric Research (NCAR), Boulder, CO (United States)
  17. Karlsruhe Institute of Technology (KIT) (Germany)
  18. University of Leeds (United Kingdom)
  19. University of Eastern Finland, Kuopio (Finland); University of California, Irvine, CA (United States)
  20. University of Helsinki (Finland); University Innsbruck (Austria); University of Vienna (Austria)
  21. University of Lisbon (Portugal); University of Beira Interior, Lisbon (Portugal)
  22. Goethe University, Frankfurt (Germany); University of Helsinki (Finland)
  23. University of Vienna (Austria)
  24. European Organization for Nuclear Research (CERN), Geneva (Switzerland); Goethe University, Frankfurt (Germany)
  25. University of Helsinki (Finland); Aerodyne Research, Inc., Billerica, MA (United States)
  26. Carnegie Mellon University, Pittsburgh, PA (United States); University of Helsinki (Finland)
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); Swiss National Science Foundation (SNSF); Academy of Finland; Horizon 2020; Swedish Research Council (SRC); Vetenskapsrådet; Portuguese Foundation for Science and Technology; Russian Academy of Sciences; Russian Foundation for Basic Research
OSTI Identifier:
1904770
Grant/Contract Number:  
SC0014469; AGS1136479; AGS1447056; AGS1439551; CHE1012293; 2011-5120; 08-02-91006-CERN; 12-02-91522-CERN
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 533; Journal Issue: 7604; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Tröstl, Jasmin, Chuang, Wayne K., Gordon, Hamish, Heinritzi, Martin, Yan, Chao, Molteni, Ugo, Ahlm, Lars, Frege, Carla, Bianchi, Federico, Wagner, Robert, Simon, Mario, Lehtipalo, Katrianne, Williamson, Christina, Craven, Jill S., Duplissy, Jonathan, Adamov, Alexey, Almeida, Joao, Bernhammer, Anne-Kathrin, Breitenlechner, Martin, Brilke, Sophia, Dias, Antònio, Ehrhart, Sebastian, Flagan, Richard C., Franchin, Alessandro, Fuchs, Claudia, Guida, Roberto, Gysel, Martin, Hansel, Armin, Hoyle, Christopher R., Jokinen, Tuija, Junninen, Heikki, Kangasluoma, Juha, Keskinen, Helmi, Kim, Jaeseok, Krapf, Manuel, Kürten, Andreas, Laaksonen, Ari, Lawler, Michael, Leiminger, Markus, Mathot, Serge, Möhler, Ottmar, Nieminen, Tuomo, Onnela, Antti, Petäjä, Tuukka, Piel, Felix M., Miettinen, Pasi, Rissanen, Matti P., Rondo, Linda, Sarnela, Nina, Schobesberger, Siegfried, Sengupta, Kamalika, Sipilä, Mikko, Smith, James N., Steiner, Gerhard, Tomè, Antònio, Virtanen, Annele, Wagner, Andrea C., Weingartner, Ernest, Wimmer, Daniela, Winkler, Paul M., Ye, Penglin, Carslaw, Kenneth S., Curtius, Joachim, Dommen, Josef, Kirkby, Jasper, Kulmala, Markku, Riipinen, Ilona, Worsnop, Douglas R., Donahue, Neil M., and Baltensperger, Urs. The role of low-volatility organic compounds in initial particle growth in the atmosphere. United States: N. p., 2016. Web. doi:10.1038/nature18271.
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Tröstl, Jasmin, Chuang, Wayne K., Gordon, Hamish, Heinritzi, Martin, Yan, Chao, Molteni, Ugo, Ahlm, Lars, Frege, Carla, Bianchi, Federico, Wagner, Robert, Simon, Mario, Lehtipalo, Katrianne, Williamson, Christina, Craven, Jill S., Duplissy, Jonathan, Adamov, Alexey, Almeida, Joao, Bernhammer, Anne-Kathrin, Breitenlechner, Martin, Brilke, Sophia, Dias, Antònio, Ehrhart, Sebastian, Flagan, Richard C., Franchin, Alessandro, Fuchs, Claudia, Guida, Roberto, Gysel, Martin, Hansel, Armin, Hoyle, Christopher R., Jokinen, Tuija, Junninen, Heikki, Kangasluoma, Juha, Keskinen, Helmi, Kim, Jaeseok, Krapf, Manuel, Kürten, Andreas, Laaksonen, Ari, Lawler, Michael, Leiminger, Markus, Mathot, Serge, Möhler, Ottmar, Nieminen, Tuomo, Onnela, Antti, Petäjä, Tuukka, Piel, Felix M., Miettinen, Pasi, Rissanen, Matti P., Rondo, Linda, Sarnela, Nina, Schobesberger, Siegfried, Sengupta, Kamalika, Sipilä, Mikko, Smith, James N., Steiner, Gerhard, Tomè, Antònio, Virtanen, Annele, Wagner, Andrea C., Weingartner, Ernest, Wimmer, Daniela, Winkler, Paul M., Ye, Penglin, Carslaw, Kenneth S., Curtius, Joachim, Dommen, Josef, Kirkby, Jasper, Kulmala, Markku, Riipinen, Ilona, Worsnop, Douglas R., Donahue, Neil M., & Baltensperger, Urs. The role of low-volatility organic compounds in initial particle growth in the atmosphere. United States. https://doi.org/10.1038/nature18271
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Tröstl, Jasmin, Chuang, Wayne K., Gordon, Hamish, Heinritzi, Martin, Yan, Chao, Molteni, Ugo, Ahlm, Lars, Frege, Carla, Bianchi, Federico, Wagner, Robert, Simon, Mario, Lehtipalo, Katrianne, Williamson, Christina, Craven, Jill S., Duplissy, Jonathan, Adamov, Alexey, Almeida, Joao, Bernhammer, Anne-Kathrin, Breitenlechner, Martin, Brilke, Sophia, Dias, Antònio, Ehrhart, Sebastian, Flagan, Richard C., Franchin, Alessandro, Fuchs, Claudia, Guida, Roberto, Gysel, Martin, Hansel, Armin, Hoyle, Christopher R., Jokinen, Tuija, Junninen, Heikki, Kangasluoma, Juha, Keskinen, Helmi, Kim, Jaeseok, Krapf, Manuel, Kürten, Andreas, Laaksonen, Ari, Lawler, Michael, Leiminger, Markus, Mathot, Serge, Möhler, Ottmar, Nieminen, Tuomo, Onnela, Antti, Petäjä, Tuukka, Piel, Felix M., Miettinen, Pasi, Rissanen, Matti P., Rondo, Linda, Sarnela, Nina, Schobesberger, Siegfried, Sengupta, Kamalika, Sipilä, Mikko, Smith, James N., Steiner, Gerhard, Tomè, Antònio, Virtanen, Annele, Wagner, Andrea C., Weingartner, Ernest, Wimmer, Daniela, Winkler, Paul M., Ye, Penglin, Carslaw, Kenneth S., Curtius, Joachim, Dommen, Josef, Kirkby, Jasper, Kulmala, Markku, Riipinen, Ilona, Worsnop, Douglas R., Donahue, Neil M., and Baltensperger, Urs. Wed . "The role of low-volatility organic compounds in initial particle growth in the atmosphere". United States. https://doi.org/10.1038/nature18271. https://www.osti.gov/servlets/purl/1904770.
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@article{osti_1904770,
title = {The role of low-volatility organic compounds in initial particle growth in the atmosphere},
author = {Tröstl, Jasmin and Chuang, Wayne K. and Gordon, Hamish and Heinritzi, Martin and Yan, Chao and Molteni, Ugo and Ahlm, Lars and Frege, Carla and Bianchi, Federico and Wagner, Robert and Simon, Mario and Lehtipalo, Katrianne and Williamson, Christina and Craven, Jill S. and Duplissy, Jonathan and Adamov, Alexey and Almeida, Joao and Bernhammer, Anne-Kathrin and Breitenlechner, Martin and Brilke, Sophia and Dias, Antònio and Ehrhart, Sebastian and Flagan, Richard C. and Franchin, Alessandro and Fuchs, Claudia and Guida, Roberto and Gysel, Martin and Hansel, Armin and Hoyle, Christopher R. and Jokinen, Tuija and Junninen, Heikki and Kangasluoma, Juha and Keskinen, Helmi and Kim, Jaeseok and Krapf, Manuel and Kürten, Andreas and Laaksonen, Ari and Lawler, Michael and Leiminger, Markus and Mathot, Serge and Möhler, Ottmar and Nieminen, Tuomo and Onnela, Antti and Petäjä, Tuukka and Piel, Felix M. and Miettinen, Pasi and Rissanen, Matti P. and Rondo, Linda and Sarnela, Nina and Schobesberger, Siegfried and Sengupta, Kamalika and Sipilä, Mikko and Smith, James N. and Steiner, Gerhard and Tomè, Antònio and Virtanen, Annele and Wagner, Andrea C. and Weingartner, Ernest and Wimmer, Daniela and Winkler, Paul M. and Ye, Penglin and Carslaw, Kenneth S. and Curtius, Joachim and Dommen, Josef and Kirkby, Jasper and Kulmala, Markku and Riipinen, Ilona and Worsnop, Douglas R. and Donahue, Neil M. and Baltensperger, Urs},
abstractNote = {About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10-4.5 micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10-4.5 to 10-0.5 micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.},
doi = {10.1038/nature18271},
journal = {Nature (London)},
number = 7604,
volume = 533,
place = {United States},
year = {Wed May 25 00:00:00 EDT 2016},
month = {Wed May 25 00:00:00 EDT 2016}
}
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