Abstract.The relationship between cloud condensation nuclei (CCN) number and the physical and chemical properties of the atmospheric aerosol distribution is explored for a polluted urban data set from the Study of Organic Aerosols at Riverside I (SOAR-1) campaign conducted at Riverside, California, USA during summer 2005. The mixing state and, to a lesser degree, the average chemical composition are shown to be important parameters in determining the activation properties of those particles around the critical activation diameters for atmospherically-realistic supersaturation values. Closure between predictions and measurements of CCN number at several supersaturations is attempted by modeling a number of aerosol chemical composition and mixing state cases of increasing complexity. It is shown that a realistic treatment of the state of mixing of the urban aerosol distribution is critical in order to eliminate model bias. Fresh emissions such as elemental carbon and small organic particles must be treated as non-activating and explicitly accounted for in the model. The relative number concentration of these particles compared to inorganics and oxygenated organic compounds of limited hygroscopicity plays an important role in determining the CCN number. Furthermore, expanding the different composition/mixing state cases to predictions of cloud droplet number concentration in a cloud parcel model highlights the dependence of cloud optical properties on the state of mixing and hygroscopic properties of the different Correspondence to: J. L. Jimenez (jose.jimenez@colorado.edu) aerosol modes, but shows that the relative differences between the different cases are reduced compared to those from the CCN model.

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Simultaneous measurements of the effective density and chemical composition of individual ambient particles were made in Riverside, California by coupling a differential mobility analyzer (DMA) with an ultrafine aerosol time-of-flight mass spectrometer (UF-ATOFMS). In the summer, chemically diverse particle types (i.e., aged-OC, vanadium-OC-sulfate-nitrate, biomass) all had similar effective densities when measured during the same time period. This result suggests that during the summer study the majority of particle mass for the different particle types was dominated by secondary species (OC, sulfates, nitrates) of the same density, while only a small fraction of the total particle mass is accounted for by the primary particle cores. Also shown herein, the effective density is a dynamic characteristic of the Riverside, CA ambient aerosol, changing by as much as 40% within 16 h. During the summer measurement period, changes in the ambient atmospheric water content correlated with changes in the measured effective densities which ranged from approximately 1.0 to 1.5 g x cm(-3). This correlation is potentially due to evaporation of water from particles in the aerodynamic lens. In contrast, in the fall during a Santa Ana meteorological event, ambient particles with a mobility diameter of 450 nm showed three distinct effective densities, each related to a chemically unique particle class. Particles with effective densities of approximately 0.27 g x cm(-3), 0.87 g x cm(-3), and 0.93 g x cm(-3) were composed mostly of elemental carbon, lubricating oil, and aged organic carbon, respectively. It is interesting to contrast the seasonal differences where in the summer, particle density and mass were determined by high amounts of secondary species, whereas in the fall, relatively clean and dry Santa Ana conditions resulted in freshly emitted particles which retained their distinct source chemistries and densities.

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Abstract. The relationship between cloud condensation nuclei (CCN) number and the physical and chemical properties of the atmospheric aerosol distribution is explored for a polluted urban data set from the Study of Organic Aerosols at Riverside I (SOAR-1) campaign conducted at Riverside, California, USA during summer 2005. The mixing state and, to a lesser degree, the average chemical composition are shown to be important parameters in determining the activation properties of those particles around the critical activation diameters for atmospherically-realistic supersaturation values. Closure between predictions and measurements of CCN number at several supersaturations is attempted by modeling a number of aerosol chemical composition and mixing state schemes of increasing complexity. It is shown that a realistic treatment of the state of mixing of the urban aerosol distribution is critical in order to eliminate model bias. Fresh emissions such as elemental carbon and small organic particles must be treated as non-activating and explicitly accounted for in the model scheme. The relative number concentration of these particles compared to inorganics and oxygenated organic compounds of limited hygroscopicity plays an important role in determining the CCN number. Furthermore, expanding the different composition/mixing state schemes to predictions of cloud droplet number concentration in a cloud parcel model highlights the dependence of cloud optical properties on the state of mixing and hygroscopic properties of the different aerosol modes, but shows that the relative differences between the different schemes are reduced compared to those from the CCN model.