New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals
(2021) In ACS Earth and Space Chemistry 5(4). p.801-811- Abstract
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.... (More)
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.
(Less)
- author
- organization
- publishing date
- 2021
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- atmospheric simulation chamber, dimethyl sulfide, growth rate, methanesulfonic acid, nucleation, photo-oxidation
- in
- ACS Earth and Space Chemistry
- volume
- 5
- issue
- 4
- pages
- 801 - 811
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- pmid:33889792
- scopus:85104909275
- ISSN
- 2472-3452
- DOI
- 10.1021/acsearthspacechem.0c00333
- project
- Continental Biosphere Aerosol Cloud climate feedback loop during the Anthropocene
- Modelling atmospheric new particle formation from first principles – The role of Highly Oxygenated organic Molecules in clean and polluted air
- language
- English
- LU publication?
- yes
- id
- a01bbc89-18fa-4bb1-83e5-10922b9c09a6
- date added to LUP
- 2021-05-18 16:51:56
- date last changed
- 2024-04-20 06:14:56
@article{a01bbc89-18fa-4bb1-83e5-10922b9c09a6,
abstract = {{<p>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. </p>}},
author = {{Rosati, Bernadette and Christiansen, Sigurd and Wollesen De Jonge, Robin and Roldin, Pontus and Jensen, Mads Mørk and Wang, Kai and Moosakutty, Shamjad P. and Thomsen, Ditte and Salomonsen, Camilla and Hyttinen, Noora and Elm, Jonas and Feilberg, Anders and Glasius, Marianne and Bilde, Merete}},
issn = {{2472-3452}},
keywords = {{atmospheric simulation chamber; dimethyl sulfide; growth rate; methanesulfonic acid; nucleation; photo-oxidation}},
language = {{eng}},
number = {{4}},
pages = {{801--811}},
publisher = {{The American Chemical Society (ACS)}},
series = {{ACS Earth and Space Chemistry}},
title = {{New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals}},
url = {{http://dx.doi.org/10.1021/acsearthspacechem.0c00333}},
doi = {{10.1021/acsearthspacechem.0c00333}},
volume = {{5}},
year = {{2021}},
}