Size-resolved observations of refractory black carbon particles in cloud droplets at a marine boundary layer site

Abstract

Abstract. Size resolved observations of aerosol particles (including black carbon particles) and cloud residuals were studied at a marine boundary layer site (251 m a.m.s.l.) in La Jolla, CA during 2012. A counterflow virtual impactor was used to sample cloud residuals while a total inlet was used to sample both cloud residuals and interstitial particles. Two cloud events totaling ten hours of in-cloud sampling were analyzed. Since the CVI only sampled cloud droplets larger than ≈11 μm, less than 100% of the cloud droplets were sampled during the two cloud events (≈38% of the cloud droplets for the first cloud event and ≈24% of the cloud droplets for the second cloud were sampled). Back trajectories showed that air masses for both cloud events spent at least 96 h over the Pacific Ocean and traveled near, or over populated regions just before sampling. Based on bulk aerosol particle concentrations measured from the total inlet the two air masses sampled were classified as polluted marine air, a classification that was consistent with back trajectory analysis and the mass concentrations of refractory black carbon (rBC) measured from the total inlet. The activated fraction of rBC, estimated from the measurements, ranged from 0.01 to 0.1 for core diameters ranging from 70 to 220 nm. Since the fraction of cloud droplets sampled by the CVI was less than 100%, the measured activated fractions of rBC should be considered as lower limits to the total fraction of rBC activated during the two cloud events. Size distributions of rBC sampled from the residual inlet show that sub-100 nm rBC cores were incorporated into the droplets in both clouds. The coating analysis shows that the rBC cores had average coating thicknesses of 75 nm for core diameters of 70 nm and 29 nm for core diameters of 220 nm. The presence of sub-100 nm rBC cores in the cloud residuals is consistent with kappa-Köhler theory and the measured coating thicknesses of the rBC cores.