Atmospheric Chemistry and Physics (Oct 2020)
Molecular understanding of the suppression of new-particle formation by isoprene
- M. Heinritzi,
- L. Dada,
- M. Simon,
- D. Stolzenburg,
- A. C. Wagner,
- A. C. Wagner,
- L. Fischer,
- L. R. Ahonen,
- S. Amanatidis,
- R. Baalbaki,
- A. Baccarini,
- P. S. Bauer,
- B. Baumgartner,
- F. Bianchi,
- F. Bianchi,
- S. Brilke,
- D. Chen,
- R. Chiu,
- A. Dias,
- A. Dias,
- J. Dommen,
- J. Duplissy,
- H. Finkenzeller,
- C. Frege,
- C. Fuchs,
- O. Garmash,
- H. Gordon,
- H. Gordon,
- M. Granzin,
- I. El Haddad,
- X. He,
- J. Helm,
- V. Hofbauer,
- C. R. Hoyle,
- J. Kangasluoma,
- J. Kangasluoma,
- T. Keber,
- C. Kim,
- C. Kim,
- A. Kürten,
- H. Lamkaddam,
- T. M. Laurila,
- J. Lampilahti,
- C. P. Lee,
- K. Lehtipalo,
- M. Leiminger,
- H. Mai,
- V. Makhmutov,
- H. E. Manninen,
- R. Marten,
- S. Mathot,
- R. L. Mauldin,
- R. L. Mauldin,
- R. L. Mauldin,
- B. Mentler,
- U. Molteni,
- T. Müller,
- W. Nie,
- T. Nieminen,
- A. Onnela,
- E. Partoll,
- M. Passananti,
- T. Petäjä,
- J. Pfeifer,
- J. Pfeifer,
- V. Pospisilova,
- L. L. J. Quéléver,
- M. P. Rissanen,
- C. Rose,
- C. Rose,
- S. Schobesberger,
- W. Scholz,
- K. Scholze,
- M. Sipilä,
- G. Steiner,
- Y. Stozhkov,
- C. Tauber,
- Y. J. Tham,
- M. Vazquez-Pufleau,
- A. Virtanen,
- A. L. Vogel,
- A. L. Vogel,
- R. Volkamer,
- R. Wagner,
- M. Wang,
- L. Weitz,
- D. Wimmer,
- M. Xiao,
- C. Yan,
- P. Ye,
- P. Ye,
- Q. Zha,
- X. Zhou,
- X. Zhou,
- A. Amorim,
- U. Baltensperger,
- A. Hansel,
- M. Kulmala,
- M. Kulmala,
- M. Kulmala,
- A. Tomé,
- P. M. Winkler,
- D. R. Worsnop,
- D. R. Worsnop,
- N. M. Donahue,
- J. Kirkby,
- J. Kirkby,
- J. Curtius
Affiliations
- M. Heinritzi
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- L. Dada
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- M. Simon
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- D. Stolzenburg
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- A. C. Wagner
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- A. C. Wagner
- Department of Chemistry & CIRES, University of Colorado at Boulder, Boulder, CO 80309-0215, USA
- L. Fischer
- Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- L. R. Ahonen
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- S. Amanatidis
- California Institute of Technology, Pasadena, CA 91125, USA
- R. Baalbaki
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- A. Baccarini
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- P. S. Bauer
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- B. Baumgartner
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- F. Bianchi
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- F. Bianchi
- Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China
- S. Brilke
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- D. Chen
- Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
- R. Chiu
- Department of Chemistry & CIRES, University of Colorado at Boulder, Boulder, CO 80309-0215, USA
- A. Dias
- CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
- A. Dias
- CERN, 1211 Geneva, Switzerland
- J. Dommen
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- J. Duplissy
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- H. Finkenzeller
- Department of Chemistry & CIRES, University of Colorado at Boulder, Boulder, CO 80309-0215, USA
- C. Frege
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- C. Fuchs
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- O. Garmash
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- H. Gordon
- CERN, 1211 Geneva, Switzerland
- H. Gordon
- School of Earth and Environment, University of Leeds, Leeds, LS 9JT, UK
- M. Granzin
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- I. El Haddad
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- X. He
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- J. Helm
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- V. Hofbauer
- Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
- C. R. Hoyle
- Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
- J. Kangasluoma
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- J. Kangasluoma
- Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China
- T. Keber
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- C. Kim
- California Institute of Technology, Pasadena, CA 91125, USA
- C. Kim
- Department of Environmental Engineering, Pusan National University, Busan 46241, Republic of Korea
- A. Kürten
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- H. Lamkaddam
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- T. M. Laurila
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- J. Lampilahti
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- C. P. Lee
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- K. Lehtipalo
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- M. Leiminger
- Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- H. Mai
- California Institute of Technology, Pasadena, CA 91125, USA
- V. Makhmutov
- Lebedev Physical Institute, Russian Academy of Sciences, 119991, Moscow, Russia
- H. E. Manninen
- CERN, 1211 Geneva, Switzerland
- R. Marten
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- S. Mathot
- CERN, 1211 Geneva, Switzerland
- R. L. Mauldin
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- R. L. Mauldin
- Department of Atmospheric and Oceanic Sciences, University of Colorado at Boulder, Boulder, CO 80309, USA
- R. L. Mauldin
- Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213, USA
- B. Mentler
- Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- U. Molteni
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- T. Müller
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- W. Nie
- Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, 210023, China
- T. Nieminen
- Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, 70211 Kuopio, Finland
- A. Onnela
- CERN, 1211 Geneva, Switzerland
- E. Partoll
- Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- M. Passananti
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- T. Petäjä
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- J. Pfeifer
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- J. Pfeifer
- CERN, 1211 Geneva, Switzerland
- V. Pospisilova
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- L. L. J. Quéléver
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- M. P. Rissanen
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- C. Rose
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- C. Rose
- Laboratory for physical meteorology, UMR6016, University Clermont Auvergne-CNRS, 63178, Aubière, France
- S. Schobesberger
- Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, 70211 Kuopio, Finland
- W. Scholz
- Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- K. Scholze
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- M. Sipilä
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- G. Steiner
- Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- Y. Stozhkov
- Lebedev Physical Institute, Russian Academy of Sciences, 119991, Moscow, Russia
- C. Tauber
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- Y. J. Tham
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- M. Vazquez-Pufleau
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- A. Virtanen
- Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, 70211 Kuopio, Finland
- A. L. Vogel
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- A. L. Vogel
- CERN, 1211 Geneva, Switzerland
- R. Volkamer
- Department of Chemistry & CIRES, University of Colorado at Boulder, Boulder, CO 80309-0215, USA
- R. Wagner
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- M. Wang
- Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
- L. Weitz
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- D. Wimmer
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- M. Xiao
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- C. Yan
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- P. Ye
- Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
- P. Ye
- Aerodyne Research, Inc., Billerica, MA 01821, USA
- Q. Zha
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- X. Zhou
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- X. Zhou
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- A. Amorim
- CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
- U. Baltensperger
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- A. Hansel
- Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- M. Kulmala
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- M. Kulmala
- Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China
- M. Kulmala
- Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland
- A. Tomé
- IDL-University of Beira Interior, Covilhã, Portugal
- P. M. Winkler
- Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- D. R. Worsnop
- Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- D. R. Worsnop
- Aerodyne Research, Inc., Billerica, MA 01821, USA
- N. M. Donahue
- Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
- J. Kirkby
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- J. Kirkby
- CERN, 1211 Geneva, Switzerland
- J. Curtius
- Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- DOI
- https://doi.org/10.5194/acp-20-11809-2020
- Journal volume & issue
-
Vol. 20
pp. 11809 – 11821
Abstract
Nucleation of atmospheric vapours produces more than half of global cloud condensation nuclei and so has an important influence on climate. Recent studies show that monoterpene (C10H16) oxidation yields highly oxygenated products that can nucleate with or without sulfuric acid. Monoterpenes are emitted mainly by trees, frequently together with isoprene (C5H8), which has the highest global emission of all organic vapours. Previous studies have shown that isoprene suppresses new-particle formation from monoterpenes, but the cause of this suppression is under debate. Here, in experiments performed under atmospheric conditions in the CERN CLOUD chamber, we show that isoprene reduces the yield of highly oxygenated dimers with 19 or 20 carbon atoms – which drive particle nucleation and early growth – while increasing the production of dimers with 14 or 15 carbon atoms. The dimers (termed C20 and C15, respectively) are produced by termination reactions between pairs of peroxy radicals (RO2⚫) arising from monoterpenes or isoprene. Compared with pure monoterpene conditions, isoprene reduces nucleation rates at 1.7 nm (depending on the isoprene ∕ monoterpene ratio) and approximately halves particle growth rates between 1.3 and 3.2 nm. However, above 3.2 nm, C15 dimers contribute to secondary organic aerosol, and the growth rates are unaffected by isoprene. We further show that increased hydroxyl radical (OH⚫) reduces particle formation in our chemical system rather than enhances it as previously proposed, since it increases isoprene-derived RO2⚫ radicals that reduce C20 formation. RO2⚫ termination emerges as the critical step that determines the highly oxygenated organic molecule (HOM) distribution and the corresponding nucleation capability. Species that reduce the C20 yield, such as NO, HO2 and as we show isoprene, can thus effectively reduce biogenic nucleation and early growth. Therefore the formation rate of organic aerosol in a particular region of the atmosphere under study will vary according to the precise ambient conditions.
