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DOI10.5194/acp-20-11809-2020
Molecular understanding of the suppression of new-particle formation by isoprene
Heinritzi M.; Dada L.; Simon M.; Stolzenburg D.; Wagner A.C.; Fischer L.; Ahonen L.R.; Amanatidis S.; Baalbaki R.; Baccarini A.; Bauer P.S.; Baumgartner B.; Bianchi F.; Brilke S.; Chen D.; Chiu R.; Dias A.; Dommen J.; Duplissy J.; Finkenzeller H.; Frege C.; Fuchs C.; Garmash O.; Gordon H.; Granzin M.; Haddad I.E.; He X.; Helm J.; Hofbauer V.; Hoyle C.R.; Kangasluoma J.; Keber T.; Kim C.; Kürten A.; Lamkaddam H.; Laurila T.M.; Lampilahti J.; Lee C.P.; Lehtipalo K.; Leiminger M.; Mai H.; Makhmutov V.; Manninen H.E.; Marten R.; Mathot S.; Mauldin R.L.; Mentler B.; Molteni U.; Müller T.; Nie W.; Nieminen T.; Onnela A.; Partoll E.; Passananti M.; Petäje T.; Pfeifer J.; Pospisilova V.; Quéléver L.L.J.; Rissanen M.P.; Rose C.; Schobesberger S.; Scholz W.; Scholze K.; Sipile M.; Steiner G.; Stozhkov Y.; Tauber C.; Tham Y.J.; Vazquez-Pufleau M.; Virtanen A.; Vogel A.L.; Volkamer R.; Wagner R.; Mingyi W.; Lena W.; Daniela W.; Xiao M.; Yan C.; Ye P.; Zha Q.; Zhou X.; Amorim A.; Baltensperger U.; Hansel A.; Kulmala M.; Tome A.; Winkler P.M.; Worsnop D.R.; Donahue N.M.; Kirkby J.; Curtius J.
发表日期2020
ISSN16807316
起始页码11809
结束页码11821
卷号20期号:20
英文摘要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 q) 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 q) reduces particle formation in our chemical system rather than enhances it as previously proposed, since it increases isoprene-derived RO2 q radicals that reduce C20 formation. RO2 q 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. © Author(s) 2020. This work is distributed under.
语种英语
scopus关键词aerosol formation; cloud condensation nucleus; isoprene; molecular analysis; monoterpene; nucleation; water vapor
来源期刊Atmospheric Chemistry and Physics
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/143897
作者单位Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, 60438, Germany; Institute for Atmospheric and Earth System Research (INAR)/Physics, University of Helsinki, Helsinki, 00014, Finland; University of Vienna, Vienna, 1090, Austria; Department of Chemistry and Cires, University of Colorado at Boulder, Boulder, CO 80309-0215, United States; Institute for Ion and Applied Physics, University of Innsbruck, Innsbruck, 6020, Austria; California Institute of Technology, Pasadena, CA 91125, United States; Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, 5232, Switzerland; Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China; Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, United States; University of Lisbon, Centra, Fcul, Lisbon, 1749-016, Portugal; Cern, Geneva, 1211, Switzerland; ...
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Heinritzi M.,Dada L.,Simon M.,et al. Molecular understanding of the suppression of new-particle formation by isoprene[J],2020,20(20).
APA Heinritzi M..,Dada L..,Simon M..,Stolzenburg D..,Wagner A.C..,...&Curtius J..(2020).Molecular understanding of the suppression of new-particle formation by isoprene.Atmospheric Chemistry and Physics,20(20).
MLA Heinritzi M.,et al."Molecular understanding of the suppression of new-particle formation by isoprene".Atmospheric Chemistry and Physics 20.20(2020).
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