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

  • Stolzenburg D Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
  • Fischer L Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
  • Vogel AL Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Heinritzi M Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Schervish M Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
  • Simon M Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Wagner AC Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Dada L Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Ahonen LR Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Amorim A Centro Multidisciplinar de Astrofísica, University of Lisbon, 1749-016 Lisbon, Portugal.
  • Baccarini A Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Bauer PS Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
  • Baumgartner B Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
  • Bergen A Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Bianchi F Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Breitenlechner M Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
  • Brilke S Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
  • Buenrostro Mazon S Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Chen D Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
  • Dias A CERN, the European Organization for Nuclear Research, 1211 Geneva, Switzerland.
  • Draper DC Department of Chemistry, University of California, Irvine, CA 92697.
  • Duplissy J Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • El Haddad I Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Finkenzeller H Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO 80309.
  • Frege C Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Fuchs C Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Garmash O Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Gordon H CERN, the European Organization for Nuclear Research, 1211 Geneva, Switzerland.
  • He X Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Helm J Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Hofbauer V Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
  • Hoyle CR Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich, Switzerland.
  • Kim C Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125.
  • Kirkby J Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Kontkanen J Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Kürten A Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Lampilahti J Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Lawler M Department of Chemistry, University of California, Irvine, CA 92697.
  • Lehtipalo K Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Leiminger M Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
  • Mai H Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125.
  • Mathot S CERN, the European Organization for Nuclear Research, 1211 Geneva, Switzerland.
  • Mentler B Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
  • Molteni U Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Nie W Joint International Research Laboratory of Atmospheric and Earth System Sciences, Nanjing University, 210023 Nanjing, China.
  • Nieminen T Department of Applied Physics, University of Eastern Finland, 70211 Kuopio, Finland.
  • Nowak JB Aerodyne Research Inc., Billerica, MA 01821.
  • Ojdanic A Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
  • Onnela A CERN, the European Organization for Nuclear Research, 1211 Geneva, Switzerland.
  • Passananti M Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Petäjä T Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Quéléver LLJ Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Rissanen MP Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Sarnela N Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Schallhart S Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Tauber C Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
  • Tomé A Institute Infante Dom Luíz, University of Beira Interior, 6200 Covilhã, Portugal.
  • Wagner R Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Wang M Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
  • Weitz L Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Wimmer D Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Xiao M Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Yan C Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
  • Ye P Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
  • Zha Q Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Baltensperger U Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Curtius J Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
  • Dommen J Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
  • Flagan RC Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125.
  • Kulmala M Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Smith JN Department of Chemistry, University of California, Irvine, CA 92697.
  • Worsnop DR Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
  • Hansel A Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
  • Donahue NM Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
  • Winkler PM Faculty of Physics, University of Vienna, 1090 Vienna, Austria; paul.winkler@univie.ac.at.
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  • 2018-08-30
Published in:
  • Proceedings of the National Academy of Sciences of the United States of America. - 2018
CLOUD experiment
aerosol formation
aerosols
nanoparticle growth
volatile organic compounds
English 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. Recent 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 [Formula: see text]C to [Formula: see text]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 show 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.
Language
  • English
Open access status
hybrid
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https://sonar.ch/global/documents/175366
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