Isoprene chemistry under upper-tropospheric conditions

Isoprene (C<sub>5</sub>H<sub>8</sub>) is the non-methane hydrocarbon with the highest emissions to the atmosphere. It is mainly produced by vegetation, especially broad-leaved trees, and efficiently transported to the upper troposphere in deep convective clouds, where it is mixed with lightning NO<sub>x</sub>. Isoprene oxidation products drive rapid formation and growth of new particles in the tropical upper troposphere. However, isoprene oxidation pathways at low temperatures are not well understood. Here, in experiments at the CERN CLOUD chamber at 223 K and 243 K, we find that isoprene oxygenated organic molecules (IP-OOM) all involve two successive <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup><mml:mrow><mml:mi>OH</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> </mml:math> oxidations. However, depending on the ambient concentrations of the termination radicals ( <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mrow> <mml:msub><mml:mrow><mml:mi>HO</mml:mi></mml:mrow> <mml:mrow><mml:mn>2</mml:mn></mml:mrow> </mml:msub> </mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> <mml:mo>,</mml:mo> <mml:mspace></mml:mspace> <mml:msup><mml:mrow><mml:mi>NO</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> </mml:math> , and <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msubsup><mml:mrow><mml:mi>NO</mml:mi></mml:mrow> <mml:mrow><mml:mn>2</mml:mn></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> </mml:math> ), vastly-different IP-OOM emerge, comprising compounds with zero, one or two nitrogen atoms. Our findings indicate high IP-OOM production rates for the tropical upper troposphere, mainly resulting in nitrate IP-OOM but with an increasing non-nitrate fraction around midday, in close agreement with aircraft observations.

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Journal
Nature Communications
Published
2025-09-29
DOI
https://doi.org/10.1038/s41467-025-64229-w
Citations
1
Primary Topic
Atmospheric chemistry and aerosols
Type
article
Field-Weighted Citation Impact
1.30

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article

Isoprene chemistry under upper-tropospheric conditions

Markku Kulmala, Paap Koemets, J. Kirkby, Richard C. Flagan et al.
1 citations
Nature Communications
Atmospheric chemistry and aerosols
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article

Isoprene chemistry under upper-tropospheric conditions

Markku Kulmala, Paap Koemets, J. Kirkby, Richard C. Flagan, Jens Top, M. Busato, Nirvan Bhattacharyya, Marcel Zauner-Wieczorek, Rainer Volkamer, Katrianne Lehtipalo, António Tomé, Philip Holzbeck, Hartwig Harder, Wenjuan Yu, Yandong Tong, Douglas R. Worsnop, Jos Lelieveld, Joachim Curtius, Siegfried Schobesberger, Neil M. Donahue, Ryan X. Ward, Paul M. Winkler, Nsikanabasi Silas Umo, Xu‐Cheng He, Mónica Martínez, Jiali Shen, Lubna Dada, Rómulo Cruz-Simbrón, A. Amorim, Manjula R. Canagaratna, Eva Sommer, T. Christoudias, Tuukka Petäjä, Wiebke Scholz, Heikki Junninen, Matthias Kohl, Imad El Haddad, Andrea Pozzer, Zhensen Zheng, Mario Simon, Antti Onnela, Armin Hansel, Ottmar Möhler, Bernhard Mentler, Gabriela R. Unfer, Jenna DeVivo, Lucía Caudillo-Plath, Imad Zgheib, Mago Reza, Lu Liu, Boxing Yang, João Almeida, Jiangyi Zhang, Christos Xenofontos, Felix Kunkler, Samuel Ruhl, Thinus F. Kruger, H. Beckmann, Douglas M. Russell, Milin Kaniyodical Sebastian, Emelda Ahongshangbam, Hannah Klebach, Anouck Chassaing, Aleksandra Morawiec, Pedro Rato, Jakob Weissbacher, Bernhard Judmaier
article en
1 citations

Abstract

Isoprene (C<sub>5</sub>H<sub>8</sub>) is the non-methane hydrocarbon with the highest emissions to the atmosphere. It is mainly produced by vegetation, especially broad-leaved trees, and efficiently transported to the upper troposphere in deep convective clouds, where it is mixed with lightning NO<sub>x</sub>. Isoprene oxidation products drive rapid formation and growth of new particles in the tropical upper troposphere. However, isoprene oxidation pathways at low temperatures are not well understood. Here, in experiments at the CERN CLOUD chamber at 223 K and 243 K, we find that isoprene oxygenated organic molecules (IP-OOM) all involve two successive <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup><mml:mrow><mml:mi>OH</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> </mml:math> oxidations. However, depending on the ambient concentrations of the termination radicals ( <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msup> <mml:mrow> <mml:msub><mml:mrow><mml:mi>HO</mml:mi></mml:mrow> <mml:mrow><mml:mn>2</mml:mn></mml:mrow> </mml:msub> </mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> <mml:mo>,</mml:mo> <mml:mspace></mml:mspace> <mml:msup><mml:mrow><mml:mi>NO</mml:mi></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msup> </mml:math> , and <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msubsup><mml:mrow><mml:mi>NO</mml:mi></mml:mrow> <mml:mrow><mml:mn>2</mml:mn></mml:mrow> <mml:mrow><mml:mo>∙</mml:mo></mml:mrow> </mml:msubsup> </mml:math> ), vastly-different IP-OOM emerge, comprising compounds with zero, one or two nitrogen atoms. Our findings indicate high IP-OOM production rates for the tropical upper troposphere, mainly resulting in nitrate IP-OOM but with an increasing non-nitrate fraction around midday, in close agreement with aircraft observations.

Nature CommunicationsVol. 16(1)
Karlsruhe Institute of Technology (DE), Goethe University Frankfurt (DE), California Institute of Technology (US), Finnish Meteorological Institute (FI), University of Vienna (AT), University of Helsinki (FI), University of Lisbon (PT), Cyprus Institute (CY), University of North Carolina Wilmington (US), University of Beira Interior (PT), Stockholm University (SE), Cooperative Institute for Research in Environmental Sciences (US), University of Eastern Finland (FI), University of Colorado Boulder (US), Universität Innsbruck (AT), University of Cambridge (GB), LIP - Laboratory of Instrumentation and Experimental Particle Physics (PT), Helsinki Institute of Physics (FI), Frankfurt Institute for Advanced Studies (DE), Paul Scherrer Institute (CH), Ionicon Analytik (Austria) (AT), Tofwerk (Switzerland) (CH), Aerodyne Research (US), Max Planck Institute for Chemistry (DE), Leibniz Institute for Tropospheric Research (DE), University of Tartu (EE), European Organization for Nuclear Research (CH), Carnegie Mellon University (US), Beijing University of Chemical Technology (CN), Nanjing University (CN)
National Science Foundation, CERN, European Commission, Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, Eesti Teadusagentuur, Bundesministerium für Bildung und Forschung, Division of Chemistry
Openalex Percentile: Top 18%
Atmospheric chemistry and aerosols
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