03 Mar 2023
 | 03 Mar 2023
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism

Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li

Abstract. Secondary organic aerosol (SOA) formed from the ozonolysis of biogenic monoterpenes is a major source of atmospheric organic aerosol. It has been previously found that relative humidity (RH) can influence the SOA formation from some monoterpenes, yet most studies only observed the increase or decrease in SOA yield without further explanations of molecular-level mechanisms. In this study, we chose two structurally different monoterpenes (limonene with an endocyclic double bond and an exocyclic double bond, Δ3-carene with only an endocyclic double bond) to investigate the effect of RH in a set of oxidation flow reactor experiments. We find contrasting impacts of RH on the SOA formation: limonene SOA yield increases by ~100 % as RH increases, while there is a slight decrease in Δ3-carene SOA yield. By analyzing SOA chemical composition and reaction mechanisms, the enhancement in limonene SOA yield can be attributed to the water-influenced reactions after ozone attack on the exocyclic double bond of limonene, which leads to the increment of lower volatile organic compounds under high RH condition. However, as Δ3-carene only has an endocyclic double bond, it cannot undergo such reactions. This hypothesis is further proved by the SOA yield enhancement of β-caryophyllene, a sesquiterpene that also has an exocyclic double bond. These results greatly improve our understanding of how water vapor influences the ozonolysis of biogenic organic compounds and subsequent SOA formation processes.

Shan Zhang et al.

Status: open (until 26 Apr 2023)

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Shan Zhang et al.


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Short summary
In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene), We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content on aerosol formation, and inform ongoing research on particle environmental effects and applications in models.