New particle formation and growth from dimethyl sulfide oxidation by hydroxyl radicals
|Author:||Rosati, Bernadette1,2; Bilde, Merete1; Christiansen, Sigurd1;|
1Department of Chemistry, Aarhus University, Aarhus C DK-8000, Denmark
2Faculty of Physics,University of Vienna, Vienna AT-1090, Austria
3Division of Nuclear Physics, Lund University, Lund SE-221 00, Sweden
4Clean Combustion Research Center, King Abdullah University of Science and Technology, Thuwal KSA-23955, Saudi Arabia
5Nano and Molecular Systems Research Unit, University of Oulu, Oulu FI-90014, Finland
6Department of Applied Physics, University of Eastern Finland, Kuopio FI-70211, Finland
7Department of Biological and Chemical Engineering, Aarhus University, Aarhus N DK-8200, Denmark
|Online Access:||PDF Full Text (PDF, 7.1 MB)|
|Persistent link:|| http://urn.fi/urn:nbn:fi-fe2021061436791
American Chemical Society,
|Publish Date:|| 2021-06-14
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.
ACS earth and space chemistry
|Pages:||801 - 811|
|Type of Publication:||
A1 Journal article – refereed
|Field of Science:||
114 Physical sciences
116 Chemical sciences
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).
|EU Grant Number:||
(717022) SURFACE - The unexplored world of aerosol surfaces and their impacts.
© 2021 The Authors. Published by American Chemical Society. This article is licensed under the Creative Commons Attribution License 4.0.