TY - JOUR
T1 - New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals
AU - Rosati, Bernadette
AU - Christiansen, Sigurd
AU - Wollesen de Jonge, Robin
AU - Roldin, Pontus
AU - Jensen, Mads Mørk
AU - Wang, Kai
AU - Moosakutty, Shamjad P.
AU - Thomsen, Ditte
AU - Salomonsen, Camilla
AU - Hyttinen, Noora
AU - Elm, Jonas
AU - Feilberg, Anders
AU - Glasius, Marianne
AU - Bilde, Merete
N1 - KAUST Repository Item: Exported on 2021-03-29
Acknowledgements: This research was supported by the Austrian Science Fund (FWF: J 3970-N36), Aarhus University, the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program, Project SURFACE (Grant Agreement No. 717022), the Swedish
Research Council Formas (Project no. 2018-01745-COBACCA), Swedish Research Council VR (project no. 2019-05006), the Faroese Research Foundation (Grant 0454), and the Independent Research Fund Denmark (Grant number 9064-00001B).
PY - 2021/3/25
Y1 - 2021/3/25
N2 - Dimethyl sulfide (DMS) is produced by plankton in oceans and constitutes the largest natural emission of sulfur to the atmosphere. In this work, we examine new particle formation from the primary pathway of oxidation of gas-phase DMS by OH radicals. We particularly focus on particle growth and mass yield as studied experimentally under dry conditions using the atmospheric simulation chamber AURA. Experimentally, we show that aerosol mass yields from oxidation of 50–200 ppb of DMS are low (2–7%) and that particle growth rates (8.2–24.4 nm/h) are comparable with ambient observations. An HR-ToF-AMS was calibrated using methanesulfonic acid (MSA) to account for fragments distributed across both the organic and sulfate fragmentation table. AMS-derived chemical compositions revealed that MSA was always more dominant than sulfate in the secondary aerosols formed. Modeling using the Aerosol Dynamics, gas- and particle-phase chemistry kinetic multilayer model for laboratory CHAMber studies (ADCHAM) indicates that the Master Chemical Mechanism gas-phase chemistry alone underestimates experimentally observed particle formation and that DMS multiphase and autoxidation chemistry is needed to explain observations. Based on quantum chemical calculations, we conclude that particle formation from DMS oxidation in the ambient atmosphere will most likely be driven by mixed sulfuric acid/MSA clusters clustering with both amines and ammonia.
AB - Dimethyl sulfide (DMS) is produced by plankton in oceans and constitutes the largest natural emission of sulfur to the atmosphere. In this work, we examine new particle formation from the primary pathway of oxidation of gas-phase DMS by OH radicals. We particularly focus on particle growth and mass yield as studied experimentally under dry conditions using the atmospheric simulation chamber AURA. Experimentally, we show that aerosol mass yields from oxidation of 50–200 ppb of DMS are low (2–7%) and that particle growth rates (8.2–24.4 nm/h) are comparable with ambient observations. An HR-ToF-AMS was calibrated using methanesulfonic acid (MSA) to account for fragments distributed across both the organic and sulfate fragmentation table. AMS-derived chemical compositions revealed that MSA was always more dominant than sulfate in the secondary aerosols formed. Modeling using the Aerosol Dynamics, gas- and particle-phase chemistry kinetic multilayer model for laboratory CHAMber studies (ADCHAM) indicates that the Master Chemical Mechanism gas-phase chemistry alone underestimates experimentally observed particle formation and that DMS multiphase and autoxidation chemistry is needed to explain observations. Based on quantum chemical calculations, we conclude that particle formation from DMS oxidation in the ambient atmosphere will most likely be driven by mixed sulfuric acid/MSA clusters clustering with both amines and ammonia.
UR - http://hdl.handle.net/10754/668297
UR - https://pubs.acs.org/doi/10.1021/acsearthspacechem.0c00333
U2 - 10.1021/acsearthspacechem.0c00333
DO - 10.1021/acsearthspacechem.0c00333
M3 - Article
C2 - 33889792
SN - 2472-3452
JO - ACS Earth and Space Chemistry
JF - ACS Earth and Space Chemistry
ER -