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

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
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  1. Univ. of Vienna (Austria); None
  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. of Vienna (Austria)
  10. Univ. Innsbruck (Austria); Harvard Univ., Cambridge, MA (United States)
  11. European Organization for Nuclear Research (CERN), Geneva (Switzerland); Univ. of Lisbon (Portugal)
  12. Univ. of California, Irvine, CA (United States)
  13. Univ. of Colorado, Boulder, CO (United States)
  14. European Organization for Nuclear Research (CERN), Geneva (Switzerland); Univ. of Leeds (United Kingdom)
  15. ETH Zurich (Switzerland)
  16. California Inst. of Technology (CalTech), Pasadena, CA (United States); Pusan National Univ., Busan (Korea)
  17. Goethe Univ., Frankfurt (Germany); European Organization for Nuclear Research (CERN), Geneva (Switzerland)
  18. California Inst. of Technology (CalTech), Pasadena, CA (United States)
  19. European Organization for Nuclear Research (CERN), Geneva (Switzerland)
  20. Nanjing Univ. (China)
  21. Univ. of Eastern Finland, Kuopio (Finland)
  22. Aerodyne Research Inc., Billerica, MA (United States)
  23. Univ. of Helsinki (Finland); Finnish Meteorological Inst., Helsinki (Finland)
  24. Univ. of Beira Interior (Portugal)
  25. Univ. of Helsinki (Finland); Beijing Univ. of Chemical Technology (China)
  26. Univ. of Helsinki (Finland); Aerodyne Research Inc., Billerica, MA (United States)
  27. Univ. Innsbruck (Austria); Ionicon Analytik GmbH, Innsbruck (Austria)
+ Show Author Affiliations

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.

Research Organization:
Univ. of California, Irvine, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); German Federal Ministry of Education and Research; Swiss National Science Foundation; Austrian Research Funding Association
Grant/Contract Number:
SC0014469
OSTI ID:
1547344
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 37 Vol. 115; ISSN 0027-8424
Publisher:
National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

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Cloud droplet number enhanced by co-condensation of organic vapours journal May 2013
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Cited By (20)

Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol journal January 2019
Impact of a hydrophobic ion on the early stage of atmospheric aerosol formation journal October 2019
Photochemistry of the Cloud Aqueous Phase: A Review journal January 2020
Secondary organic aerosol formation from smoldering and flaming combustion of biomass: a box model parametrization based on volatility basis set journal January 2019
Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysis journal January 2019
Molecular understanding of the suppression of new-particle formation by isoprene journal January 2020
Peroxy radical chemistry and the volatility basis set journal January 2020
Seasonal characteristics of organic aerosol chemical composition and volatility in Stuttgart, Germany text January 2019
Widespread Pollution From Secondary Sources of Organic Aerosols During Winter in the Northeastern United States journal March 2019
New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate journal July 2019
Molecular identification of organic vapors driving atmospheric nanoparticle growth journal September 2019
Understanding interactions of organic nitrates with the surface and bulk of organic films: implications for particle growth in the atmosphere journal January 2018
Impact of a hydrophobic ion on the early stage of atmospheric aerosol formation journal October 2019
Photochemistry of the Cloud Aqueous Phase: A Review journal January 2020
Secondary organic aerosol formation from smoldering and flaming combustion of biomass: a box model parametrization based on volatility basis set journal January 2019
Seasonal characteristics of organic aerosol chemical composition and volatility in Stuttgart, Germany journal January 2019
Observations of highly oxidized molecules and particle nucleation in the atmosphere of Beijing journal January 2019
Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysis journal January 2019
Temperature effects on sulfuric acid aerosol nucleation and growth: initial results from the TANGENT study journal January 2019
Peroxy radical chemistry and the volatility basis set journal January 2020

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Related Subjects

54 ENVIRONMENTAL SCIENCES
CLOUD experiment
aerosol formation
aerosols
nanoparticle growth
volatile organic compounds