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Molecular Understanding of the Enhancement in Organic Aerosol Mass at High Relative Humidity. 2023
Mihnea Surdu, and
Houssni Lamkaddam, and
Dongyu S Wang, and
David M Bell, and
Mao Xiao, and
Chuan Ping Lee, and
Dandan Li, and
Lucía Caudillo, and
Guillaume Marie, and
Wiebke Scholz, and
Mingyi Wang, and
Brandon Lopez, and
Ana A Piedehierro, and
Farnoush Ataei, and
Rima Baalbaki, and
Barbara Bertozzi, and
Pia Bogert, and
Zoé Brasseur, and
Lubna Dada, and
Jonathan Duplissy, and
Henning Finkenzeller, and
Xu-Cheng He, and
Kristina Höhler, and
Kimmo Korhonen, and
Jordan E Krechmer, and
Katrianne Lehtipalo, and
Naser G A Mahfouz, and
Hanna E Manninen, and
Ruby Marten, and
Dario Massabò, and
Roy Mauldin, and
Tuukka Petäjä, and
Joschka Pfeifer, and
Maxim Philippov, and
Birte Rörup, and
Mario Simon, and
Jiali Shen, and
Nsikanabasi Silas Umo, and
Franziska Vogel, and
Stefan K Weber, and
Marcel Zauner-Wieczorek, and
Rainer Volkamer, and
Harald Saathoff, and
Ottmar Möhler, and
Jasper Kirkby, and
Douglas R Worsnop, and
Markku Kulmala, and
Frank Stratmann, and
Armin Hansel, and
Joachim Curtius, and
André Welti, and
Matthieu Riva, and
Neil M Donahue, and
Urs Baltensperger, and
Imad El Haddad
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
The mechanistic pathway by which high relative humidity (RH) affects gas-particle partitioning remains poorly understood, although many studies report increased secondary organic aerosol (SOA) yields at high RH. Here, we use real-time, molecular measurements of both the gas and particle phase to provide a mechanistic understanding of the effect of RH on the partitioning of biogenic oxidized organic molecules (from α-pinene and isoprene) at low temperatures (243 and 263 K) at the CLOUD chamber at CERN. We observe increases in SOA mass of 45 and 85% with increasing RH from 10-20 to 60-80% at 243 and 263 K, respectively, and attribute it to the increased partitioning of semi-volatile compounds. At 263 K, we measure an increase of a factor 2-4 in the concentration of C10H16O2-3, while the particle-phase concentrations of low-volatility species, such as C10H16O6-8, remain almost constant. This results in a substantial shift in the chemical composition and volatility distribution toward less oxygenated and more volatile species at higher RH (e.g., at 263 K, O/C ratio = 0.55 and 0.40, at RH = 10 and 80%, respectively). By modeling particle growth using an aerosol growth model, which accounts for kinetic limitations, we can explain the enhancement in the semi-volatile fraction through the complementary effect of decreased compound activity and increased bulk-phase diffusivity. Our results highlight the importance of particle water content as a diluting agent and a plasticizer for organic aerosol growth.
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Chuan Ping Lee, and
Dandan Li, and
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Wiebke Scholz, and
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Zoé Brasseur, and
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Dario Massabò, and
Roy Mauldin, and
Tuukka Petäjä, and
Joschka Pfeifer, and
Maxim Philippov, and
Birte Rörup, and
Mario Simon, and
Jiali Shen, and
Nsikanabasi Silas Umo, and
Franziska Vogel, and
Stefan K Weber, and
Marcel Zauner-Wieczorek, and
Rainer Volkamer, and
Harald Saathoff, and
Ottmar Möhler, and
Jasper Kirkby, and
Douglas R Worsnop, and
Markku Kulmala, and
Frank Stratmann, and
Armin Hansel, and
Joachim Curtius, and
André Welti, and
Matthieu Riva, and
Neil M Donahue, and
Urs Baltensperger, and
Imad El Haddad
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The journal of physical chemistry. A,
Mihnea Surdu, and
Houssni Lamkaddam, and
Dongyu S Wang, and
David M Bell, and
Mao Xiao, and
Chuan Ping Lee, and
Dandan Li, and
Lucía Caudillo, and
Guillaume Marie, and
Wiebke Scholz, and
Mingyi Wang, and
Brandon Lopez, and
Ana A Piedehierro, and
Farnoush Ataei, and
Rima Baalbaki, and
Barbara Bertozzi, and
Pia Bogert, and
Zoé Brasseur, and
Lubna Dada, and
Jonathan Duplissy, and
Henning Finkenzeller, and
Xu-Cheng He, and
Kristina Höhler, and
Kimmo Korhonen, and
Jordan E Krechmer, and
Katrianne Lehtipalo, and
Naser G A Mahfouz, and
Hanna E Manninen, and
Ruby Marten, and
Dario Massabò, and
Roy Mauldin, and
Tuukka Petäjä, and
Joschka Pfeifer, and
Maxim Philippov, and
Birte Rörup, and
Mario Simon, and
Jiali Shen, and
Nsikanabasi Silas Umo, and
Franziska Vogel, and
Stefan K Weber, and
Marcel Zauner-Wieczorek, and
Rainer Volkamer, and
Harald Saathoff, and
Ottmar Möhler, and
Jasper Kirkby, and
Douglas R Worsnop, and
Markku Kulmala, and
Frank Stratmann, and
Armin Hansel, and
Joachim Curtius, and
André Welti, and
Matthieu Riva, and
Neil M Donahue, and
Urs Baltensperger, and
Imad El Haddad
June 2019,
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