New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals
Wollesen de Jonge, Robin
Jensen, Mads Mørk
Moosakutty, Shamjad P.
KAUST DepartmentClean Combustion Research Center
Clean Combustion Research Center, King Abdullah University of Science and Technology, Thuwal KSA-23955, Saudi Arabia
Embargo End Date2022-03-25
Permanent link to this recordhttp://hdl.handle.net/10754/668297
MetadataShow full item record
AbstractDimethyl 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.
CitationRosati, B., Christiansen, S., Wollesen de Jonge, R., Roldin, P., Jensen, M. M., Wang, K., … Bilde, M. (2021). New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals. ACS Earth and Space Chemistry. doi:10.1021/acsearthspacechem.0c00333
SponsorsThis 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).
PublisherAmerican Chemical Society (ACS)
JournalACS Earth and Space Chemistry
Except where otherwise noted, this item's license is described as This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Earth and Space Chemistry, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acsearthspacechem.0c00333.