|
Environ Sci Technol
| Title: | Molecular Understanding of the Enhancement in Organic Aerosol Mass at High Relative Humidity |
|
| Author(s): | Surdu M; Lamkaddam H; Wang DS; Bell DM; Xiao M; Lee CP; Li D; Caudillo L; Marie G; Scholz W; Wang M; Lopez B; Piedehierro AA; Ataei F; Baalbaki R; Bertozzi B; Bogert P; Brasseur Z; Dada L; Duplissy J; Finkenzeller H; He XC; Hohler K; Korhonen K; Krechmer JE; Lehtipalo K; Mahfouz NGA; Manninen HE; Marten R; Massabo D; Mauldin R; Petaja T; Pfeifer J; Philippov M; Rorup B; Simon M; Shen J; Umo NS; Vogel F; Weber SK; Zauner-Wieczorek M; Volkamer R; Saathoff H; Mohler O; Kirkby J; Worsnop DR; Kulmala M; Stratmann F; Hansel A; Curtius J; Welti A; Riva M; Donahue NM; Baltensperger U; El Haddad I; |
|
| Address: | "Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland. Universite de Lyon, Universite Claude Bernard Lyon 1, CNRS, IRCELYON, 69626 Villeurbanne, France. Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany. Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria. Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, 91125 California, United States. Center for Atmospheric Particle Studies, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, 15213 Pennsylvania, United States. Finnish Meteorological Institute, 00560 Helsinki, Finland. Department of Experimental Aerosol and Cloud Microphysics, Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany. Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland. Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76021 Karlsruhe, Germany. Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland. Department of Chemistry & CIRES, University of Colorado Boulder, UCB 215, Boulder, 80309-0215 Colorado, United States. Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, 70211 Kuopio, Finland. Aerodyne Research, Inc., Billerica, 01821 Massachusetts, United States. Atmospheric and Oceanic Sciences, Princeton University, Princeton, 08540 New Jersey, United States. CERN, the European Organization for Nuclear Research, CH-1211 Geneva 23, Switzerland. Department of Physics, University of Genoa & INFN, 16146 Genoa, Italy. Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh, 15213 Pennsylvania, United States. Department of Atmospheric and Oceanic Sciences, University of Colorado, Boulder, UCB 311, Boulder, 80309 Colorado, United States. P. N. Lebedev Physical Institute of the Russian Academy of Sciences, 119991 Moscow, Russia. Tofwerk AG, CH-3600 Thun, Switzerland" |
|
| Journal Title: | Environ Sci Technol |
| Year: | 2023 |
| Volume: | 20230130 |
| Issue: | 6 |
| Page Number: | 2297 - 2309 |
| DOI: | 10.1021/acs.est.2c04587 |
|
| ISSN/ISBN: | 1520-5851 (Electronic) 0013-936X (Print) 0013-936X (Linking) |
|
| Abstract: | "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 alpha-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 C(10)H(16)O(2-3), while the particle-phase concentrations of low-volatility species, such as C(10)H(16)O(6-8), 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" |
|
| Keywords: | *Monoterpenes/chemistry *Air Pollutants Humidity Aerosols molecular composition organic aerosol growth particle diffusivity particle water content relative humidity; |
|
| Notes: | "MedlineSurdu, Mihnea Lamkaddam, Houssni Wang, Dongyu S Bell, David M Xiao, Mao Lee, Chuan Ping Li, Dandan Caudillo, Lucia Marie, Guillaume Scholz, Wiebke Wang, Mingyi Lopez, Brandon Piedehierro, Ana A Ataei, Farnoush Baalbaki, Rima Bertozzi, Barbara Bogert, Pia Brasseur, Zoe Dada, Lubna Duplissy, Jonathan Finkenzeller, Henning He, Xu-Cheng Hohler, Kristina Korhonen, Kimmo Krechmer, Jordan E Lehtipalo, Katrianne Mahfouz, Naser G A Manninen, Hanna E Marten, Ruby Massabo, Dario Mauldin, Roy Petaja, Tuukka Pfeifer, Joschka Philippov, Maxim Rorup, Birte Simon, Mario Shen, Jiali Umo, Nsikanabasi Silas Vogel, Franziska Weber, Stefan K Zauner-Wieczorek, Marcel Volkamer, Rainer Saathoff, Harald Mohler, Ottmar Kirkby, Jasper Worsnop, Douglas R Kulmala, Markku Stratmann, Frank Hansel, Armin Curtius, Joachim Welti, Andre Riva, Matthieu Donahue, Neil M Baltensperger, Urs El Haddad, Imad eng Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S. 2023/01/31 Environ Sci Technol. 2023 Feb 14; 57(6):2297-2309. doi: 10.1021/acs.est.2c04587. Epub 2023 Jan 30" |
|
|
|
|
