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. Stabilized Criegee intermediates (SCIs) have the potential tooxidize trace species and to produce secondary organic aerosols (SOAs),making them important factors in tropospheric chemistry. This studyquantitatively investigates the performance of SCIs in SOA formation atdifferent relative humidity (RH) levels, and the first- and second-generationoxidations of endo- and exocyclic double bonds ozonated in limoneneozonolysis are studied separately. Through regulating SCI scavengers, theyields and rate constants of SCIs in a reaction system were derived, and thequantities of SCIs were calculated. The quantity of SOAs decreased by more than20 % under low-humidity conditions (10 % RH–50 % RH), compared to that underdry conditions, due to the reactions of SCIs with water, while the inhibitoryeffect of water on SOA formation was not observed under high-humidityconditions (60 % RH–90 % RH). When using excessive SCI scavengers to excludeSCI reactions, it was found that the effect of water on SOA formation withthe presence of SCIs was different from that without the presence of SCIs,suggesting that SCI reactions were relevant to the non-monotonic impact ofwater. The fractions of the SCI contribution to SOAs were similar between dryand high-humidity conditions, where the SCI reactions accounted for∼ 63 % and ∼ 73 % in SOA formation in thefirst- and second-generation oxidation; however, marked differences in SOAformation mechanisms were observed. SOA formation showed a positivecorrelation with the quantity of SCIs, and the SOA formation potential of SCIsunder high-humidity conditions was more significant than that under dry andlow-humidity conditions. It was estimated that 20 %–30 % of SCIs could beconverted into SOAs under high-humidity conditions, while this value decreasedby nearly half under dry and low-humidity conditions. The typicalcontribution of limonene-derived SCIs to SOA formation is calculated to be(8.21 ± 0.15) × 10−2 µg m−3 h−1 inforest, (4.26 ± 0.46) × 10−2 µg m−3 h−1in urban areas, and (2.52 ± 0.28) × 10−1 µg m−3 h−1 in indoor areas. Water is an uncertainty in the role SCIs playin SOA formation, and the contribution of SCIs to SOA formation needsconsideration even under high RH in the atmosphere.

Quantification of the role of stabilized Criegee intermediates in the formation of aerosols in limonene ozonolysis