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Hygroscopicity and CCN potential of DMS-derived aerosol particles

Rosati, Bernadette ; Isokääntä, Sini ; Christiansen, Sigurd ; Jensen, Mads Mørk ; Moosakutty, Shamjad P. ; De Jonge, Robin Wollesen LU ; Massling, Andreas ; Glasius, Marianne ; Elm, Jonas and Virtanen, Annele , et al. (2022) In Atmospheric Chemistry and Physics 22(20). p.13449-13466
Abstract

Dimethyl sulfide (DMS) is emitted by phytoplankton species in the oceans and constitutes the largest source of naturally emitted sulfur to the atmosphere. The climate impact of secondary particles, formed through the oxidation of DMS by hydroxyl radicals, is still elusive. This study investigates the hygroscopicity and cloud condensation nuclei activity of such particles and discusses the results in relation to their chemical composition. We show that mean hygroscopicity parameters, κ, during an experiment for particles of 80 nm in diameter range from 0.46 to 0.52 or higher, as measured at both sub- and supersaturated water vapour conditions. Ageing of the particles leads to an increase in κ from, for example, 0.50 to 0.58 over the... (More)

Dimethyl sulfide (DMS) is emitted by phytoplankton species in the oceans and constitutes the largest source of naturally emitted sulfur to the atmosphere. The climate impact of secondary particles, formed through the oxidation of DMS by hydroxyl radicals, is still elusive. This study investigates the hygroscopicity and cloud condensation nuclei activity of such particles and discusses the results in relation to their chemical composition. We show that mean hygroscopicity parameters, κ, during an experiment for particles of 80 nm in diameter range from 0.46 to 0.52 or higher, as measured at both sub- and supersaturated water vapour conditions. Ageing of the particles leads to an increase in κ from, for example, 0.50 to 0.58 over the course of 3 h (Exp. 7). Aerosol mass spectrometer measurements from this study indicate that this change most probably stems from a change in chemical composition leading to slightly higher fractions of ammonium sulfate compared to methanesulfonic acid (MSA) within the particles with ageing time. Lowering the temperature to 258 K increases κ slightly, particularly for small particles. These κ values are well comparable to previously reported model values for MSA or mixtures between MSA and ammonium sulfate. Particle nucleation and growth rates suggest a clear temperature dependence, with slower rates at cold temperatures. Quantum chemical calculations show that gas-phase MSA clusters are predominantly not hydrated, even at high humidity conditions, indicating that their gas-phase chemistry should be independent of relative humidity.

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Contribution to journal
publication status
published
subject
in
Atmospheric Chemistry and Physics
volume
22
issue
20
pages
18 pages
publisher
Copernicus GmbH
external identifiers
  • scopus:85141950847
ISSN
1680-7316
DOI
10.5194/acp-22-13449-2022
language
English
LU publication?
yes
id
7504f1b9-016c-425e-a589-dbfa101dafff
date added to LUP
2023-01-03 15:45:29
date last changed
2023-10-05 11:44:44
@article{7504f1b9-016c-425e-a589-dbfa101dafff,
  abstract     = {{<p>Dimethyl sulfide (DMS) is emitted by phytoplankton species in the oceans and constitutes the largest source of naturally emitted sulfur to the atmosphere. The climate impact of secondary particles, formed through the oxidation of DMS by hydroxyl radicals, is still elusive. This study investigates the hygroscopicity and cloud condensation nuclei activity of such particles and discusses the results in relation to their chemical composition. We show that mean hygroscopicity parameters, κ, during an experiment for particles of 80 nm in diameter range from 0.46 to 0.52 or higher, as measured at both sub- and supersaturated water vapour conditions. Ageing of the particles leads to an increase in κ from, for example, 0.50 to 0.58 over the course of 3 h (Exp. 7). Aerosol mass spectrometer measurements from this study indicate that this change most probably stems from a change in chemical composition leading to slightly higher fractions of ammonium sulfate compared to methanesulfonic acid (MSA) within the particles with ageing time. Lowering the temperature to 258 K increases κ slightly, particularly for small particles. These κ values are well comparable to previously reported model values for MSA or mixtures between MSA and ammonium sulfate. Particle nucleation and growth rates suggest a clear temperature dependence, with slower rates at cold temperatures. Quantum chemical calculations show that gas-phase MSA clusters are predominantly not hydrated, even at high humidity conditions, indicating that their gas-phase chemistry should be independent of relative humidity.</p>}},
  author       = {{Rosati, Bernadette and Isokääntä, Sini and Christiansen, Sigurd and Jensen, Mads Mørk and Moosakutty, Shamjad P. and De Jonge, Robin Wollesen and Massling, Andreas and Glasius, Marianne and Elm, Jonas and Virtanen, Annele and Bilde, Merete}},
  issn         = {{1680-7316}},
  language     = {{eng}},
  number       = {{20}},
  pages        = {{13449--13466}},
  publisher    = {{Copernicus GmbH}},
  series       = {{Atmospheric Chemistry and Physics}},
  title        = {{Hygroscopicity and CCN potential of DMS-derived aerosol particles}},
  url          = {{http://dx.doi.org/10.5194/acp-22-13449-2022}},
  doi          = {{10.5194/acp-22-13449-2022}},
  volume       = {{22}},
  year         = {{2022}},
}