1School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
2School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
*present address: Department of Civil and Environmental Engineering, Tufts University, Medford, MA, USA
**present address: Physical Research Laboratory, Ahmedabad, India
Abstract. Aerosol composition and mixing state near anthropogenic sources can be highly variable and can challenge predictions of cloud condensation nuclei (CCN). We present in-situ size-resolved CCN measurements to quantify this predictive uncertainty, which were carried out during the 2008 summertime August Mini Intensive Gas and Aerosol Study (AMIGAS) campaign in Atlanta, GA. Aerosol chemical composition was measured by two particle-into-liquid samplers measuring water-soluble inorganic ions and total water-soluble organic carbon. Size-resolved CCN data were collected using the Scanning Mobility CCN Analysis (SMCA) method and were used to obtain characteristic aerosol hygroscopicity distributions, whose breadth reflects the aerosol compositional variability and mixing state. We find that knowledge of aerosol mixing state is important for accurate predictions of CCN concentrations and that the influence of an externally-mixed, non-CCN-active aerosol fraction varies with size from 31% for particle diameters less than 40 nm to 93% for accumulation mode aerosol during the day. This is likely indicative of the interactions between biogenic and anthropogenic emissions which contribute to the formation and transformation of aerosols in this heterogeneous environment. Assuming size-dependent aerosol mixing state and size-invariant chemical composition decreased the average CCN concentration overprediction from greater than 50–200% to less than 20%. CCN activity was parameterized using a single hygroscopicity parameter, κ, which averaged 0.16 ± 0.07 for 80 nm particles and exhibited considerable variability (range: 0.03–0.48) throughout the study period.