Preprints
https://doi.org/10.5194/egusphere-2024-1386
https://doi.org/10.5194/egusphere-2024-1386
15 May 2024
 | 15 May 2024
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Formation and temperature dependence of Highly Oxygenated Organic Molecules (HOM) from Δ3-carene ozonolysis

Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn

Abstract.3-carene is a prominent monoterpene in the atmosphere, contributing significantly to secondary organic aerosol (SOA) formation. However, knowledge about ∆3-carene oxidation pathways, particularly regarding its ability to form highly oxygenated organic molecules (HOM), is still limited. In this study, we present HOM measurements during ∆3-carene ozonolysis under various conditions in two simulation chambers. We identified numerous HOM (monomers: C7-10H10-18O6-14, dimers: C17-20H24-34O6-18) using a chemical ionization mass spectrometer (CIMS). ∆3-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, 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 6 or 7 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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Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn

Status: open (until 26 Jun 2024)

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Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn
Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn

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Short summary
3-carene is abundantly emitted from vegetation, but its atmospheric oxidation chemistry has received limited attention. We explored highly oxygenated organic molecules (HOM) formation from ∆3-carene ozonolysis in chambers and investigated the impact of temperature and relative humidity on HOM formation. Our findings provide new insights into ∆3-carene oxidation pathways and its potential to impact atmospheric aerosol.