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Title: Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range

Abstract

Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Currnet results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from 25 ° C to 25 ° C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We report that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.

Authors:
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  1. Univ. of Vienna (Austria)
  2. Univ. Innsbruck (Austria)
  3. Goethe Univ., Frankfurt (Germany); European Organization for Nuclear Research (CERN), Geneva (Switzerland); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  4. Goethe Univ., Frankfurt (Germany)
  5. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  6. Univ. of Helsinki (Finland)
  7. Univ. of Lisbon (Portugal)
  8. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  9. Univ. Innsbruck (Austria); Harvard Univ., Cambridge, MA (United States)
  10. European Organization for Nuclear Research (CERN), Geneva (Switzerland); Univ. of Lisbon (Portugal)
  11. Univ. of California, Irvine, CA (United States)
  12. Univ. of Colorado, Boulder, CO (United States)
  13. European Organization for Nuclear Research (CERN), Geneva (Switzerland); Univ. of Leeds (United Kingdom)
  14. ETH Zurich (Switzerland)
  15. California Inst. of Technology (CalTech), Pasadena, CA (United States); Pusan National Univ., Busan (Korea)
  16. Goethe Univ., Frankfurt (Germany); European Organization for Nuclear Research (CERN), Geneva (Switzerland)
  17. California Inst. of Technology (CalTech), Pasadena, CA (United States)
  18. European Organization for Nuclear Research (CERN), Geneva (Switzerland)
  19. Nanjing Univ. (China)
  20. Univ. of Eastern Finland, Kuopio (Finland)
  21. Aerodyne Research Inc., Billerica, MA (United States)
  22. Univ. of Helsinki (Finland); Finnish Meteorological Inst., Helsinki (Finland)
  23. Univ. of Beira Interior (Portugal)
  24. Univ. of Helsinki (Finland); Beijing Univ. of Chemical Technology (China)
  25. Univ. of Helsinki (Finland); Aerodyne Research Inc., Billerica, MA (United States)
  26. Univ. Innsbruck (Austria); Ionicon Analytik GmbH, Innsbruck (Austria)
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); German Federal Ministry of Education and Research (BMBF); Swiss National Science Foundation (SNSF); Austrian Research Funding Association
OSTI Identifier:
1547344
Grant/Contract Number:  
[SC0014469]
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
[ Journal Volume: 115; Journal Issue: 37]; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; aerosols; nanoparticle growth; aerosol formation; CLOUD experiment; volatile organic compounds

Citation Formats

Stolzenburg, Dominik, Fischer, Lukas, Vogel, Alexander L., Heinritzi, Martin, Schervish, Meredith, Simon, Mario, Wagner, Andrea C., Dada, Lubna, Ahonen, Lauri R., Amorim, Antonio, Baccarini, Andrea, Bauer, Paulus S., Baumgartner, Bernhard, Bergen, Anton, Bianchi, Federico, Breitenlechner, Martin, Brilke, Sophia, Buenrostro Mazon, Stephany, Chen, Dexian, Dias, António, Draper, Danielle C., Duplissy, Jonathan, El Haddad, Imad, Finkenzeller, Henning, Frege, Carla, Fuchs, Claudia, Garmash, Olga, Gordon, Hamish, He, Xucheng, Helm, Johanna, Hofbauer, Victoria, Hoyle, Christopher R., Kim, Changhyuk, Kirkby, Jasper, Kontkanen, Jenni, Kürten, Andreas, Lampilahti, Janne, Lawler, Michael, Lehtipalo, Katrianne, Leiminger, Markus, Mai, Huajun, Mathot, Serge, Mentler, Bernhard, Molteni, Ugo, Nie, Wei, Nieminen, Tuomo, Nowak, John B., Ojdanic, Andrea, Onnela, Antti, Passananti, Monica, Petäjä, Tuukka, Quéléver, Lauriane L. J., Rissanen, Matti P., Sarnela, Nina, Schallhart, Simon, Tauber, Christian, Tomé, António, Wagner, Robert, Wang, Mingyi, Weitz, Lena, Wimmer, Daniela, Xiao, Mao, Yan, Chao, Ye, Penglin, Zha, Qiaozhi, Baltensperger, Urs, Curtius, Joachim, Dommen, Josef, Flagan, Richard C., Kulmala, Markku, Smith, James N., Worsnop, Douglas R., Hansel, Armin, Donahue, Neil M., and Winkler, Paul M. Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range. United States: N. p., 2018. Web. doi:10.1073/pnas.1807604115.
Stolzenburg, Dominik, Fischer, Lukas, Vogel, Alexander L., Heinritzi, Martin, Schervish, Meredith, Simon, Mario, Wagner, Andrea C., Dada, Lubna, Ahonen, Lauri R., Amorim, Antonio, Baccarini, Andrea, Bauer, Paulus S., Baumgartner, Bernhard, Bergen, Anton, Bianchi, Federico, Breitenlechner, Martin, Brilke, Sophia, Buenrostro Mazon, Stephany, Chen, Dexian, Dias, António, Draper, Danielle C., Duplissy, Jonathan, El Haddad, Imad, Finkenzeller, Henning, Frege, Carla, Fuchs, Claudia, Garmash, Olga, Gordon, Hamish, He, Xucheng, Helm, Johanna, Hofbauer, Victoria, Hoyle, Christopher R., Kim, Changhyuk, Kirkby, Jasper, Kontkanen, Jenni, Kürten, Andreas, Lampilahti, Janne, Lawler, Michael, Lehtipalo, Katrianne, Leiminger, Markus, Mai, Huajun, Mathot, Serge, Mentler, Bernhard, Molteni, Ugo, Nie, Wei, Nieminen, Tuomo, Nowak, John B., Ojdanic, Andrea, Onnela, Antti, Passananti, Monica, Petäjä, Tuukka, Quéléver, Lauriane L. J., Rissanen, Matti P., Sarnela, Nina, Schallhart, Simon, Tauber, Christian, Tomé, António, Wagner, Robert, Wang, Mingyi, Weitz, Lena, Wimmer, Daniela, Xiao, Mao, Yan, Chao, Ye, Penglin, Zha, Qiaozhi, Baltensperger, Urs, Curtius, Joachim, Dommen, Josef, Flagan, Richard C., Kulmala, Markku, Smith, James N., Worsnop, Douglas R., Hansel, Armin, Donahue, Neil M., & Winkler, Paul M. Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range. United States. doi:10.1073/pnas.1807604115.
Stolzenburg, Dominik, Fischer, Lukas, Vogel, Alexander L., Heinritzi, Martin, Schervish, Meredith, Simon, Mario, Wagner, Andrea C., Dada, Lubna, Ahonen, Lauri R., Amorim, Antonio, Baccarini, Andrea, Bauer, Paulus S., Baumgartner, Bernhard, Bergen, Anton, Bianchi, Federico, Breitenlechner, Martin, Brilke, Sophia, Buenrostro Mazon, Stephany, Chen, Dexian, Dias, António, Draper, Danielle C., Duplissy, Jonathan, El Haddad, Imad, Finkenzeller, Henning, Frege, Carla, Fuchs, Claudia, Garmash, Olga, Gordon, Hamish, He, Xucheng, Helm, Johanna, Hofbauer, Victoria, Hoyle, Christopher R., Kim, Changhyuk, Kirkby, Jasper, Kontkanen, Jenni, Kürten, Andreas, Lampilahti, Janne, Lawler, Michael, Lehtipalo, Katrianne, Leiminger, Markus, Mai, Huajun, Mathot, Serge, Mentler, Bernhard, Molteni, Ugo, Nie, Wei, Nieminen, Tuomo, Nowak, John B., Ojdanic, Andrea, Onnela, Antti, Passananti, Monica, Petäjä, Tuukka, Quéléver, Lauriane L. J., Rissanen, Matti P., Sarnela, Nina, Schallhart, Simon, Tauber, Christian, Tomé, António, Wagner, Robert, Wang, Mingyi, Weitz, Lena, Wimmer, Daniela, Xiao, Mao, Yan, Chao, Ye, Penglin, Zha, Qiaozhi, Baltensperger, Urs, Curtius, Joachim, Dommen, Josef, Flagan, Richard C., Kulmala, Markku, Smith, James N., Worsnop, Douglas R., Hansel, Armin, Donahue, Neil M., and Winkler, Paul M. Tue . "Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range". United States. doi:10.1073/pnas.1807604115. https://www.osti.gov/servlets/purl/1547344.
@article{osti_1547344,
title = {Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range},
author = {Stolzenburg, Dominik and Fischer, Lukas and Vogel, Alexander L. and Heinritzi, Martin and Schervish, Meredith and Simon, Mario and Wagner, Andrea C. and Dada, Lubna and Ahonen, Lauri R. and Amorim, Antonio and Baccarini, Andrea and Bauer, Paulus S. and Baumgartner, Bernhard and Bergen, Anton and Bianchi, Federico and Breitenlechner, Martin and Brilke, Sophia and Buenrostro Mazon, Stephany and Chen, Dexian and Dias, António and Draper, Danielle C. and Duplissy, Jonathan and El Haddad, Imad and Finkenzeller, Henning and Frege, Carla and Fuchs, Claudia and Garmash, Olga and Gordon, Hamish and He, Xucheng and Helm, Johanna and Hofbauer, Victoria and Hoyle, Christopher R. and Kim, Changhyuk and Kirkby, Jasper and Kontkanen, Jenni and Kürten, Andreas and Lampilahti, Janne and Lawler, Michael and Lehtipalo, Katrianne and Leiminger, Markus and Mai, Huajun and Mathot, Serge and Mentler, Bernhard and Molteni, Ugo and Nie, Wei and Nieminen, Tuomo and Nowak, John B. and Ojdanic, Andrea and Onnela, Antti and Passananti, Monica and Petäjä, Tuukka and Quéléver, Lauriane L. J. and Rissanen, Matti P. and Sarnela, Nina and Schallhart, Simon and Tauber, Christian and Tomé, António and Wagner, Robert and Wang, Mingyi and Weitz, Lena and Wimmer, Daniela and Xiao, Mao and Yan, Chao and Ye, Penglin and Zha, Qiaozhi and Baltensperger, Urs and Curtius, Joachim and Dommen, Josef and Flagan, Richard C. and Kulmala, Markku and Smith, James N. and Worsnop, Douglas R. and Hansel, Armin and Donahue, Neil M. and Winkler, Paul M.},
abstractNote = {Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Currnet results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from–25°C to25°C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We report that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.},
doi = {10.1073/pnas.1807604115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = [37],
volume = [115],
place = {United States},
year = {2018},
month = {8}
}

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