Optical-chemical relationships for carbonaceous aerosols observed at Jeju Island, Korea with a 3-laser photoacoustic spectrometer

Abstract

Abstract. Transport of aerosols in pollution plumes from the mainland Asian continent was observed in situ at Jeju, South Korea during the Cheju Asian Brown Cloud Plume-Asian Monsoon Experiment (CAPMEX) field campaign throughout August and September 2008 using a 3-laser photoacoustic spectrometer. Transport of mixed sulfate, carbonaceous, and nitrate aerosols from various Asian pollution plumes to Jeju accounted for 76% of the deployment days, showing large variations in their measured chemical and optical properties. Our analysis of eight distinct episodes, spanning a wide range of chemical composition, optical properties, and source regions, reveals that at episodes with higher OC/SO2−4 and NO−3/SO2−4 composition ratios exhibit lower single scatter albedo at shorter wavelengths (ω405); significantly lower [ω405meas = 0.79±0.06, ω405calc = 0.86±0.01] than predicted by an optical model that assumes constant complex index of refraction with wavelength (an optical model of soot). We attribute this discrepancy to enhanced absorption by organic material. Organic carbon absorption accounts for up to 50% of the measured aerosol absorption at 405 nm for the high OC/SO2−4 episode. Coatings of elemental carbon aerosol cores are hypothesized to increase absorption by factors up to 6 at visible wavelengths. Carbonaceous aerosol absorption can alter global radiative forcing estimates substantially, underscoring the need to understand and predict chemical composition effects on optical properties.