Large differences in aerosol optical properties over the north-west Atlantic Ocean during the TCAP field campaign

Abstract:

Aerosol radiative forcing is an important parameter in the Earth’s radiation budget and can be an important driver of atmospheric circulation and the hydrological cycle. Accurate estimation of aerosol radiative forcing requires measurement of both the extensive and intensive optical properties of aerosols. While the intensive optical properties are independent of aerosol mass or number, they are critical inputs when calculating radiative forcing with applications to climate research, satellite remote sensing and model validations. The key aerosol intensive properties that need to be evaluated include single scattering albedo (SSA), the angstrom exponent, the asymmetry parameter, the radiative forcing efficiency, and the hygroscopic scattering factor. We report here on values of these variables over the Cape Cod and nearby northwest Atlantic Ocean during the Two Column Aerosol Project (TCAP). The average SSA shows a distinct profile having higher SSA values below the top of well-mixed residual layer (RL) and lower SSA above it. Aerosol in the free troposphere (FT) were found to have less spectral dependence in their optical properties, lower back scatter fraction and higher hygroscopic growth relative to aerosols found in the RL. Analysis of individual particle composition suggests that that ratio of aged to fresh aerosol numbers in the FT is 70% higher compared to aerosols measured in the RL, and that smoke from biomass burning contributed ~10% to this number. Single particle analysis also reveals that the fraction and variability of coated black carbon (BC) aerosol is higher in the FT relative to that measured in the residual layer. The daily radiative forcing efficiency of these aerosols in the FT is factor 2 higher than below RL. Seven years (2007-2013) of CALIPSO satellite observations show that the mean altitude of the top of smoke layers (~3.3 km) consistent with these in situ observations from TCAP. Overall, the long term CALIPSO observations characterizes 13% of aerosol layers as smoke over TCAP region and indicate that these smoke layers have been present over this area every year. The aircraft and satellite observations both suggest that while smoke contributes around 10% of total aerosol, it must be taken into account, as the radiative forcing estimates are sensitive to the amount of absorbing aerosol.