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The detailed molecular composition of laboratory generated limoneneozonolysis secondary organic aerosol (SOA) was studied usingultrahigh-resolution Fourier transform ion cyclotron resonance (FT-ICR) massspectrometry. Approximately 1200 molecular formulas were identified in theSOA over the mass range of 140 to 850 Da. Four characteristic groups of highrelative abundance species were observed; they indicate an array ofaccretion products that retain a large fraction of the limonene skeleton.The identified molecular formulas of each of the groups are related to oneanother by CH2, O and CH2O homologous series. The CH2 and Ohomologous series of the low molecular weight (MW) SOA (m/z < 300) are explained witha combination of functionalization and fragmentation of radicalintermediates and reactive uptake of gas-phase carbonyls. They includeisomerization and elimination reactions of Criegee radicals, reactionsbetween alkyl peroxy radicals, and scission of alkoxy radicals resultingfrom the Criegee radicals. The presence of compounds with 10–15 carbon atomsin the first group (e.g. C11H18O6) provides evidence for SOAformation by the reactive uptake of gas-phase carbonyls during limoneneozonolysis. The high MW compounds (m/z > 300) were found to constitute a significantnumber fraction of the identified SOA components. The formation of high MWcompounds was evaluated by molecular formula trends, fragmentation analysisof select high MW compounds and a comprehensive reaction matrix includingthe identified low MW SOA, hydroperoxides and Criegee radicals as buildingblocks. Although the formation of high MW SOA may occur via a variety ofradical and non-radical reaction channels, the combined approach indicates agreater importance of the non-condensation reactions over aldol and estercondensation reaction channels. Among these hemi-acetal reactions appear tobe most dominant followed by hydroperoxide and Criegee reaction channels

High molecular weight SOA formation during limonene ozonolysis: insights from ultrahigh-resolution FT-ICR mass spectrometry characterization