Isoprene Aerosol Growth in the Upper Troposphere: Application of the Diagonal Volatility Basis Set to CLOUD Chamber Measurements

Isoprene oxygenated organic molecules (IP-OOM) can nucleate new particles in the upper troposphere. These particles may grow into cloud condensation nuclei and influence the clouds and climate. However, little is known about the individual species driving growth and whether they undergo condensed-phase reactions. We conducted isoprene oxidation experiments at 223 and 243 K in the CLOUD chamber at CERN. Gas-phase concentrations were measured with chemical ionization mass spectrometers (NO<sub>3</sub> <sup>-</sup>-CIMS, Br<sup>-</sup>-MION2-CIMS, and NH<sub>4</sub> <sup>+</sup>-CIMS). Growth rates from 8 to 20 nm were measured by a Neutral Cluster and Air Ion Spectrometer. Particle-phase composition was measured by a filter sampling chemical ionization mass spectrometer. We use the diagonal volatility basis set (dVBS) analysis framework to compare gas- and particle-phase measurements and assess species and processes influencing growth. We find that kinetically limited condensation of a few species dominates particle composition and growth. Particle-phase processes, including oligomerization and organonitrate hydrolysis, do not influence the early growth. dVBS growth rate predictions can explain 90% of the measured growth, dominated by kinetic condensation of low-volatility species. Our findings indicate that initial growth of IP-OOM particles under cold, low-acid conditions may be controlled and modeled by the kinetically limited condensation of low-volatility compounds.

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Journal
ACS ES&T Air
Published
2025-09-15
DOI
https://doi.org/10.1021/acsestair.5c00106
Primary Topic
Atmospheric chemistry and aerosols
Type
article
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article

Isoprene Aerosol Growth in the Upper Troposphere: Application of the Diagonal Volatility Basis Set to CLOUD Chamber Measurements

Markku Kulmala, P. Rato Mendes, J. Kirkby, Richard C. Flagan et al.
ACS ES&T Air
Atmospheric chemistry and aerosols
article

Isoprene Aerosol Growth in the Upper Troposphere: Application of the Diagonal Volatility Basis Set to CLOUD Chamber Measurements

Markku Kulmala, P. Rato Mendes, J. Kirkby, Richard C. Flagan, Jens Top, M. Busato, Nirvan Bhattacharyya, Marcel Zauner-Wieczorek, Rainer Volkamer, Brandon Lopez, Katrianne Lehtipalo, António Tomé, Birte Rörup, Hartwig Harder, Wenjuan Yu, Yandong Tong, Douglas R. Worsnop, Joachim Curtius, Siegfried Schobesberger, Neil M. Donahue, Nsikanabasi Silas Umo, Xu‐Cheng He, Jiali Shen, Lubna Dada, A. Amorim, Manjula R. Canagaratna, Eva Sommer, Dominik Stolzenburg, João Paulo A. Almeida, T. Christoudias, Tuukka Petäjä, Wiebke Scholz, Lucía Caudillo, Imad El Haddad, Zhensen Zheng, Mario Simon, Bernhard Mentler, Jenna DeVivo, Imad Zgheib, Lu Liu, Boxing Yang, Ottmar Möhler, Jiangyi Zhang, Christos Xenofontos, Felix Kunkler, Samuel Ruhl, H. Beckmann, Douglas M. Russell, Milin Kaniyodical Sebastian, Hannah Klebach, Anouck Chassaing, Aleksandra Morawiec, Jakob Weissbacher, Bernhard Judmaier
article en

Abstract

Isoprene oxygenated organic molecules (IP-OOM) can nucleate new particles in the upper troposphere. These particles may grow into cloud condensation nuclei and influence the clouds and climate. However, little is known about the individual species driving growth and whether they undergo condensed-phase reactions. We conducted isoprene oxidation experiments at 223 and 243 K in the CLOUD chamber at CERN. Gas-phase concentrations were measured with chemical ionization mass spectrometers (NO<sub>3</sub> <sup>-</sup>-CIMS, Br<sup>-</sup>-MION2-CIMS, and NH<sub>4</sub> <sup>+</sup>-CIMS). Growth rates from 8 to 20 nm were measured by a Neutral Cluster and Air Ion Spectrometer. Particle-phase composition was measured by a filter sampling chemical ionization mass spectrometer. We use the diagonal volatility basis set (dVBS) analysis framework to compare gas- and particle-phase measurements and assess species and processes influencing growth. We find that kinetically limited condensation of a few species dominates particle composition and growth. Particle-phase processes, including oligomerization and organonitrate hydrolysis, do not influence the early growth. dVBS growth rate predictions can explain 90% of the measured growth, dominated by kinetic condensation of low-volatility species. Our findings indicate that initial growth of IP-OOM particles under cold, low-acid conditions may be controlled and modeled by the kinetically limited condensation of low-volatility compounds.

ACS ES&T AirVol. 2(10)
Karlsruhe Institute of Technology (DE), Goethe University Frankfurt (DE), California Institute of Technology (US), University of Vienna (AT), Department of Natural and Environmental Resources (PR), University of Helsinki (FI), University of Lisbon (PT), TU Wien (AT), Cyprus Institute (CY), 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), Helsinki Institute of Physics (FI), Paul Scherrer Institute (CH), University of Colorado System (US), Finnish Geospatial Research Institute (FI), Ionicon Analytik (Austria) (AT), Tofwerk (Switzerland) (CH), Finland University (FI), Division of Chemistry (US), Aerodyne Research (US), Max Planck Institute for Chemistry (DE), Climate Centre (NL), Institute for Physics (US), Universitas Islam Syekh Yusuf (ID), National Institute of Meteorology (TN), Instituto Dom Luiz, University of Tartu (EE), European Organization for Nuclear Research (CH), Carnegie Mellon University (US), Universidade Nova de Lisboa (PT)
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Atmospheric chemistry and aerosols
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