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Volatility of secondary organic aerosol from β-caryophyllene ozonolysis over a wide tropospheric temperature range

We investigated secondary organic aerosol (SOA) from β-caryophyllene oxidation generated over a wide tropospheric temperature range (213-313 K) from ozonolysis. Positive matrix factorization (PMF) was used to deconvolute the desorption data (thermograms) of SOA products detected by a chemical ioniza...

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Main Authors: Gao, Linyu (Author) , Buchholz, Angela (Author) , Li, Zijun (Author) , Song, Junwei (Author) , Vallon, Magdalena (Author) , Jiang, Feng (Author) , Möhler, Ottmar (Author) , Leisner, Thomas (Author) , Saathoff, Harald (Author)
Format: Article (Journal)
Language:English
Published: June 20, 2023
In: Environmental science & technology
Year: 2023, Volume: 57, Issue: 24, Pages: 8965-8974
ISSN:1520-5851
DOI:10.1021/acs.est.3c01151
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.est.3c01151
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Author Notes:Linyu Gao, Angela Buchholz, Zijun Li, Junwei Song, Magdalena Vallon, Feng Jiang, Ottmar Möhler, Thomas Leisner, and Harald Saathoff
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Summary:We investigated secondary organic aerosol (SOA) from β-caryophyllene oxidation generated over a wide tropospheric temperature range (213-313 K) from ozonolysis. Positive matrix factorization (PMF) was used to deconvolute the desorption data (thermograms) of SOA products detected by a chemical ionization mass spectrometer (FIGAERO-CIMS). A nonmonotonic dependence of particle volatility (saturation concentration at 298 K, C298K*) on formation temperature (213-313 K) was observed, primarily due to temperature-dependent formation pathways of β-caryophyllene oxidation products. The PMF analysis grouped detected ions into 11 compound groups (factors) with characteristic volatility. These compound groups act as indicators for the underlying SOA formation mechanisms. Their different temperature responses revealed that the relevant chemical pathways (e.g., autoxidation, oligomer formation, and isomer formation) had distinct optimal temperatures between 213 and 313 K, significantly beyond the effect of temperature-dependent partitioning. Furthermore, PMF-resolved volatility groups were compared with volatility basis set (VBS) distributions based on different vapor pressure estimation methods. The variation of the volatilities predicted by different methods is affected by highly oxygenated molecules, isomers, and thermal decomposition of oligomers with long carbon chains. This work distinguishes multiple isomers and identifies compound groups of varying volatilities, providing new insights into the temperature-dependent formation mechanisms of β-caryophyllene-derived SOA particles.
Item Description:Veröffentlicht: 07. Juni 2023
Gesehen am 09.08.2023
Physical Description:Online Resource
ISSN:1520-5851
DOI:10.1021/acs.est.3c01151

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