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Proc Natl Acad Sci U S A. 2018 Sep 11;115(37):9122-9127. doi: 10.1073/pnas.1807604115. Epub 2018 Aug 28.

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

Author information

1
Faculty of Physics, University of Vienna, 1090 Vienna, Austria.
2
Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
3
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
4
CERN, the European Organization for Nuclear Research, 1211 Geneva, Switzerland.
5
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
6
Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213.
7
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
8
Centro Multidisciplinar de Astrofísica, University of Lisbon, 1749-016 Lisbon, Portugal.
9
Faculdade de Ciências da Universidade de Lisboa, University of Lisbon, 1749-016 Lisbon, Portugal.
10
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138.
11
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138.
12
Department of Chemistry, University of California, Irvine, CA 92697.
13
Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO 80309.
14
School of Earth and Environment, University of Leeds, LS2 9JT Leeds, United Kingdom.
15
Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich, Switzerland.
16
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125.
17
Department of Environmental Engineering, Pusan National University, 46241 Busan, Republic of Korea.
18
Joint International Research Laboratory of Atmospheric and Earth System Sciences, Nanjing University, 210023 Nanjing, China.
19
Department of Applied Physics, University of Eastern Finland, 70211 Kuopio, Finland.
20
Aerodyne Research Inc., Billerica, MA 01821.
21
Finnish Meteorological Institute, 00101 Helsinki, Finland.
22
Institute Infante Dom Luíz, University of Beira Interior, 6200 Covilhã, Portugal.
23
Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China.
24
Ionicon Analytik GmbH, 6020 Innsbruck, Austria.
25
Faculty of Physics, University of Vienna, 1090 Vienna, Austria; paul.winkler@univie.ac.at.

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. 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.

KEYWORDS:

CLOUD experiment; aerosol formation; aerosols; nanoparticle growth; volatile organic compounds

PMID:
30154167
DOI:
10.1073/pnas.1807604115
Free PMC Article

Conflict of interest statement

The authors declare no conflict of interest.

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