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Using chemical ionization mass spectrometry to detect particle-phase acids (acid-CIMS) and aerosol mass spectrometry (AMS) measurements from Colorado, USA, and two studies in Hyytiala, Finland, we quantify the fraction of organic aerosol (OA) mass that is composed of molecules with acid functional groups (facid). Molecules containing one or more carboxylic acid functionality contributed approximately 29% (45-51%) of the OA mass in Colorado (Finland). Organic acid mass concentration correlates well with AMS m/z 44 (primarily CO2+), a commonly used marker for highly oxidized aerosol. Using the average empirical relationship between AMS m/z 44 and organic acids in these three studies, together with m/z 44 data from 29 continental northern hemispheric (NH) AMS datasets, we estimate that molecules containing carboxylic acid functionality constitute on average 28% (range 10-50%) of NH continental OA mass with typically higher values at rural/remote sites and during summer and lower values at urban sites and during winter.

[1] Laboratory experiments investigated the relationship between oxidation level and hygroscopic properties of secondary organic aerosol (SOA) particles generated via OH radical oxidation in an aerosol flow reactor. The hygroscopic growth factor at 90% RH (HGF90%), the CCN activity (ORG,CCN) and the level of oxidation (atomic O:C ratio) of the SOA particles were measured. Both HGF90% and ORG,CCN increased with O:C; the HGF90% varied linearly with O:C, while ORG,CCN mostly followed a nonlinear trend. An average HGF90% of 1.25 and ORG,CCN of 0.19 were measured for O:C of 0.65, in agreement with results reported for ambient data. The ORG values estimated from the HGF90% (ORG,HGF )w ere 20 to 50% lower than paired ORG,CCN values for all SOA particles except 1,3,5‐trimethylbenzene (TMB), the least hygroscopic of the SOA systems. Within the limitations of instrumental capabilities, we show that differences in hygroscopic behavior among the investigated SOA systems may correspond to differences in elemental composition. Citation: Massoli, P., et al. (2010), Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles, Geophys. Res. Lett., 37, L24801, doi:10.1029/2010GL045258.

Secondary organic aerosols (SOA) forms a major fraction of organic aerosols in the atmosphere. Knowledge of SOA properties that affect their dynamics in the atmosphere is needed for improving climate models. By combining experimental and modeling techniques, we investigated the factors controlling SOA evaporation under different humidity conditions. Our experiments support the conclusion of particle phase diffusivity limiting the evaporation under dry conditions. Viscosity of particles at dry conditions was estimated to increase several orders of magnitude during evaporation, up to 109 Pa s. However, at atmospherically relevant relative humidity and time scales, our results show that diffusion limitations may have a minor effect on evaporation of the studied α-pinene SOA particles. Based on previous studies and our model simulations, we suggest that, in warm environments dominated by biogenic emissions, the major uncertainty in models describing the SOA particle evaporation is related to the volatility of SOA constituents., published version, peerReviewed