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 - Funding Information: 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). Publisher Copyright: © 2021 The Authors. Published by American Chemical Society. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.

PY - 2021/4

Y1 - 2021/4

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.

KW - atmospheric simulation chamber

KW - dimethyl sulfide

KW - growth rate

KW - methanesulfonic acid

KW - nucleation

KW - photo-oxidation

UR - http://www.scopus.com/inward/record.url?scp=85104909275&partnerID=8YFLogxK

U2 - 10.1021/acsearthspacechem.0c00333

DO - 10.1021/acsearthspacechem.0c00333

M3 - Journal article

C2 - 33889792

AN - SCOPUS:85104909275

VL - 5

SP - 801

EP - 811

JO - ACS Earth and Space Chemistry

JF - ACS Earth and Space Chemistry

SN - 2472-3452

IS - 4

ER -