North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei

Abstract

Measurements of aerosol and cloud properties in the Eastern Pacific Ocean were taken during an airborne experiment on the University of Wyoming's King Air during April 2004 as part of the Cloud Indirect Forcing Experiment (CIFEX). We observed a wide variety of aerosols, including those of long‐range transport from Asia, clean marine boundary layer, and North American emissions. These aerosols, classified by their size distribution and history, were found in stratified layers between 500 to 7500 m above sea level and thicknesses from 100 to 3000 m. A comparison of the aerosol size distributions to measurements of cloud condensation nuclei (CCN) provides insight to the CCN activity of the different aerosol types. The overall ratio of measured to predicted CCN concentration (NCCN) is 0.56 ± 0.41 with a relationship of NCCN,measured = NCCN,predicted0.846±0.002 for 23 research flights and 1884 comparisons. Such a relationship does not accurately describe a CCN closure; however, it is consistent with our measurements that high CCN concentrations are more influenced by anthropogenic sources, which are less CCN active. While other CCN closures have obtained results closer to the expected 1:1 relationship, the different aerosol types (and presumably differences in aerosol chemistry) are responsible for the discrepancy. The measured NCCN at 0.3% supersaturation (Sc) ranged from 20 cm−3 (pristine) to 350 cm−3 (anthropogenic) with an average of 106 ± 54 cm−3 over the experiment. The inferred supersaturation in the clouds sampled during this experiment is ∼0.3%. CCN concentrations of cloud‐processed aerosol were well predicted using an ammonium sulfate approximation for Sc ≤ 0.4%. Predicted NCCN for other aerosol types (i.e., Asian and North American aerosols) were high compared to measured values indicating a less CCN active aerosol. This study highlights the importance of chemical effects on CCN measurements and introduces a CCN activation index as a method of classifying the efficiency of an aerosol to serve as CCN relative to an ammonium sulfate particle. This index ranged from close to unity for cloud processed aerosols to as low as 0.31 for aged aerosols transported from Asia. We also compare the performance of two CCN instruments (static thermal diffusion chamber and streamwise continuous flow chamber) on a 45 minute level leg where we observe an aged layer and a nucleation event. More than 50% of the aged aerosol served as CCN at 0.2% Sc, primarily owing to their large size, while CCN concentrations during the nucleation event were close to 0 cm−3. CCN concentrations from both instruments agreed within instrument errors; however, the continuous flow chamber effectively captured the rapid transition in aerosol properties.