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© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 17 Feb 2020

Submitted as: research article | 17 Feb 2020

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This preprint is currently under review for the journal ACP.

Molecular understanding of the suppression of new-particle formation by isoprene

Martin Heinritzi1, Lubna Dada2, Mario Simon1, Dominik Stolzenburg3, Andrea C. Wagner1,4, Lukas Fischer5, Lauri R. Ahonen2, Stavros Amanatidis6, Rima Baalbaki2, Andrea Baccarini7, Paulus S. Bauer3, Bernhard Baumgartner3, Federico Bianchi2,8, Sophia Brilke3, Dexian Chen9, Randall Chiu4, Antonio Dias10,11, Josef Dommen7, Jonathan Duplissy2, Henning Finkenzeller4, Carla Frege7, Claudia Fuchs7, Olga Garmash2, Hamish Gordon11,12, Manuel Granzin1, Imad El Haddad7, Xucheng He2, Johanna Helm1, Victoria Hofbauer9, Christopher R. Hoyle13, Juha Kangasluoma2,8, Timo Keber1, Changhyuk Kim6,14, Andreas Kürten1, Houssni Lamkaddam7, Janne Lampilahti2, Tiia M. Laurila2, Chuan Ping Lee7, Katrianne Lehtipalo2, Markus Leiminger5, Huajun Mai6, Vladimir Makhmutov15, Hanna Elina Manninen11, Ruby Marten7, Serge Mathot11, Roy Lee Mauldin2,16,17, Bernhard Mentler5, Ugo Molteni7, Tatjana Müller1, Wei Nie18, Tuomo Nieminen19, Antti Onnela11, Eva Partoll5, Monica Passananti2, Tuukka Petäjä2, Joschka Pfeifer1,11, Veronika Pospisilova7, Lauriane Quéléver2, Matti P. Rissanen2, Clémence Rose2,20, Siegfried Schobesberger19, Wiebke Scholz5, Kay Scholze3, Mikko Sipilä2, Gerhard Steiner5, Yuri Stozhkov15, Christian Tauber3, Yee Jun Tham2, Miguel Vazquez-Pufleau3, Annele Virtanen19, Alexander L. Vogel1,11, Rainer Volkamer4, Robert Wagner2, Mingyi Wang9, Lena Weitz1, Daniela Wimmer2, Mao Xiao7, Chao Yan2, Penglin Ye9,21, Qiaozhi Zha2, Xueqin Zhou1,7, Antonio Amorim10, Urs Baltensperger7, Armin Hansel5, Markku Kulmala2,8,22, António Tomé23, Paul M. Winkler3, Douglas R. Worsnop2,21, Neil M. Donahue9, Jasper Kirkby1,11, and Joachim Curtius1 Martin Heinritzi et al.
  • 1Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
  • 2Institute for Atmospheric and Earth System Research (INAR) / Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
  • 3Faculty of Physics, University of Vienna, 1090 Vienna, Austria
  • 4Department of Chemistry & CIRES, University of Colorado at Boulder, Boulder, CO, 80309-0215, USA
  • 5Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
  • 6California Institute of Technology, Pasadena, CA 91125, USA
  • 7Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
  • 8Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P.R. China
  • 9Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
  • 10CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
  • 11CERN, 1211 Geneva, Switzerland
  • 12University of Leeds, Leeds LS2 9JT, UK
  • 13Institute for Atmospheric and Climate Science, ETH Zurich, Switzerland
  • 14Department of Environmental Engineering, Pusan National University, Busan 46241, Republic of Korea
  • 15Lebedev Physical Institute, Russian Academy of Sciences, 119991, Moscow, Russia
  • 16Department of Atmospheric and Oceanic Sciences, University of Colorado at Boulder, Boulder, CO 80309, USA
  • 17Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213, USA
  • 18Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, 210023, China
  • 19Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, 70211 Kuopio, Finland
  • 20Laboratory for physical meteorology, UMR6016, University Clermont Auvergne-CNRS, 63178, Aubière, France
  • 21Aerodyne Research, Inc., Billerica, MA 01821, USA
  • 22Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland
  • 23IDL-University of Beira Interior, Covilhã, Portugal

Abstract. Nucleation of atmospheric vapors 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 vapors. 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 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.

Martin Heinritzi et al.

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Martin Heinritzi et al.

Martin Heinritzi et al.


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Publications Copernicus
Short summary
With experiments performed at CLOUD we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of Highly Oxygenated organic Molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene rich environments.
With experiments performed at CLOUD we show how isoprene interferes in monoterpene oxidation via...