New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals

Autor(en)

Bernadette Rosati, Sigurd Christiansen, Robin Wollesen de Jonge, Pontus Roldin, Mads Mørk Jensen, Kai Wang, Shamjad P. Moosakutty, Ditte Thomsen, Camilla Salomonsen, Noora Hyttinen, Jonas Elm, Anders Feilberg, Marianne Glasius, Merete Bilde

Abstrakt

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.

Organisation(en)

Aerosolphysik und Umweltphysik

Externe Organisation(en)

Aarhus University, Lund University, King Abdullah University for Science and Technology, University of Oulu, University of Eastern Finland

Journal

ACS Earth and Space Chemistry

Band

5

Seiten

801-811

Anzahl der Seiten

11

ISSN

2472-3452

DOI

https://doi.org/10.1021/acsearthspacechem.0c00333

Publikationsdatum

03-2021

Peer-reviewed

Ja

ÖFOS 2012

103039 Aerosolphysik, 105208 Atmosphärenchemie

Schlagwörter

ASJC Scopus Sachgebiete

Geochemistry and Petrology, Space and Planetary Science, Atmospheric Science

Link zum Portal

https://ucrisportal.univie.ac.at/de/publications/2d129d3f-5116-434b-b8ce-8fda11073aa1