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Formation and temperature dependence of highly oxygenated organic molecules (HOMs) from δ3-carene ozonolysis

Luo, Yuanyuan ; Thomsen, Ditte ; Iversen, Emil Mark ; Roldin, Pontus LU ; Skønager, Jane Tygesen ; Li, Linjie ; Priestley, Michael ; Pedersen, Henrik B. ; Hallquist, Mattias and Bilde, Merete , et al. (2024) In Atmospheric Chemistry and Physics 24(16). p.9459-9473
Abstract

δ3-carene is a prominent monoterpene in the atmosphere, contributing significantly to secondary organic aerosol (SOA) formation. However, knowledge about δ3-carene oxidation pathways, particularly regarding their ability to form highly oxygenated organic molecules (HOMs), is still limited. In this study, we present HOM measurements during δ3-carene ozonolysis under various conditions in two simulation chambers. We identified numerous HOMs (monomers: C7-10H10-18O6-14; dimers: C17-20H24-34O6-18) using a chemical ionization mass spectrometer (CIMS). δ3-carene ozonolysis yielded higher HOM concentrations than α-pinene, with a distinct distribution, indicating differences in formation pathways. All HOM signals decreased considerably at lower... (More)

δ3-carene is a prominent monoterpene in the atmosphere, contributing significantly to secondary organic aerosol (SOA) formation. However, knowledge about δ3-carene oxidation pathways, particularly regarding their ability to form highly oxygenated organic molecules (HOMs), is still limited. In this study, we present HOM measurements during δ3-carene ozonolysis under various conditions in two simulation chambers. We identified numerous HOMs (monomers: C7-10H10-18O6-14; dimers: C17-20H24-34O6-18) using a chemical ionization mass spectrometer (CIMS). δ3-carene ozonolysis yielded higher HOM concentrations than α-pinene, with a distinct distribution, indicating differences in formation pathways. All HOM signals decreased considerably at lower temperatures, reducing the estimated molar HOM yield from ∼ 3 % at 20 °C to ∼ 0.5 % at 0 °C. Interestingly, the temperature change altered the HOM distribution, increasing the observed dimer-to-monomer ratios from roughly 0.8 at 20 °C to 1.5 at 0 °C. HOM monomers with six or seven O atoms condensed more efficiently onto particles at colder temperatures, while monomers with nine or more O atoms and all dimers condensed irreversibly even at 20 °C. Using the gas- and particle-phase chemistry kinetic multilayer model ADCHAM, we were also able to reproduce the experimentally observed HOM composition, yields, and temperature dependence.

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type
Contribution to journal
publication status
published
subject
in
Atmospheric Chemistry and Physics
volume
24
issue
16
pages
15 pages
publisher
Copernicus GmbH
external identifiers
  • scopus:85202807571
ISSN
1680-7316
DOI
10.5194/acp-24-9459-2024
language
English
LU publication?
yes
id
9f589f5a-d4c3-449c-8259-c6be2999d217
date added to LUP
2024-11-25 14:17:06
date last changed
2025-04-04 15:00:15
@article{9f589f5a-d4c3-449c-8259-c6be2999d217,
  abstract     = {{<p>δ3-carene is a prominent monoterpene in the atmosphere, contributing significantly to secondary organic aerosol (SOA) formation. However, knowledge about δ3-carene oxidation pathways, particularly regarding their ability to form highly oxygenated organic molecules (HOMs), is still limited. In this study, we present HOM measurements during δ3-carene ozonolysis under various conditions in two simulation chambers. We identified numerous HOMs (monomers: C7-10H10-18O6-14; dimers: C17-20H24-34O6-18) using a chemical ionization mass spectrometer (CIMS). δ3-carene ozonolysis yielded higher HOM concentrations than α-pinene, with a distinct distribution, indicating differences in formation pathways. All HOM signals decreased considerably at lower temperatures, reducing the estimated molar HOM yield from ∼ 3 % at 20 °C to ∼ 0.5 % at 0 °C. Interestingly, the temperature change altered the HOM distribution, increasing the observed dimer-to-monomer ratios from roughly 0.8 at 20 °C to 1.5 at 0 °C. HOM monomers with six or seven O atoms condensed more efficiently onto particles at colder temperatures, while monomers with nine or more O atoms and all dimers condensed irreversibly even at 20 °C. Using the gas- and particle-phase chemistry kinetic multilayer model ADCHAM, we were also able to reproduce the experimentally observed HOM composition, yields, and temperature dependence.</p>}},
  author       = {{Luo, Yuanyuan and Thomsen, Ditte and Iversen, Emil Mark and Roldin, Pontus and Skønager, Jane Tygesen and Li, Linjie and Priestley, Michael and Pedersen, Henrik B. and Hallquist, Mattias and Bilde, Merete and Glasius, Marianne and Ehn, Mikael}},
  issn         = {{1680-7316}},
  language     = {{eng}},
  number       = {{16}},
  pages        = {{9459--9473}},
  publisher    = {{Copernicus GmbH}},
  series       = {{Atmospheric Chemistry and Physics}},
  title        = {{Formation and temperature dependence of highly oxygenated organic molecules (HOMs) from δ3-carene ozonolysis}},
  url          = {{http://dx.doi.org/10.5194/acp-24-9459-2024}},
  doi          = {{10.5194/acp-24-9459-2024}},
  volume       = {{24}},
  year         = {{2024}},
}