Analysis of CCN activity of Arctic aerosol and Canadian biomass burning during summer 2008

The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARC-TAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50-85 degrees N and 40-130 degrees W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66-94% by volume), with a water-soluble mass fraction of more than 50 %. The aerosol hygroscopicity parameter, kappa, ranged between kappa = 0.08-0.32 for all air mass types. Industrial pollution had the lowest kappa of 0.08 +/- 0.01, while the Arctic background had the highest and most variable kappa of 0.32 +/- 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar kappa (0.18 +/- 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (kappa(org)) was parameterized by the volume fraction of water-soluble organic matter (epsilon(WSOM)), with a kappa = 0.12, such that kappa(org) = 0.12 " WSOM. Assuming bulk (size-independent) composition and including the kappa(org) parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine the true degree of external mixing and therefore may not always be representative of the environments sampled. No correlation was observed between kappa(org) and O: C. A novel correction of the CCN instrument supersaturation for water vapor depletion, resulting from high concentrations of CCN, was also employed. This correction was especially important for fresh biomass burning plumes where concentrations exceeded 1.5x10(4) cm(-3) and introduced supersaturation depletions of >= 25 %. Not accounting for supersaturation depletion in these high concentration environments would therefore bias CCN closure up to 25% and inferred kappa by up to 50 %.