Optical closure for an aerosol column: Method, accuracy, and inferable properties applied to a biomass-burning aerosol and its radiative forcing

[1] During the Lindenberg Aerosol Characterization Experiment (LACE 98), airborne measurements of aerosol size distribution, fine-particle concentration, particle absorption coefficient, backscatter coefficient, depolarization, and chemical composition as well as ground-based measurements of spectral particle optical depth and of spectral backscatter and extinction coefficients were performed in the aerosol column above Lindenberg, Germany. We compare the measured optical parameters with calculations from the size distributions, which assume the aerosol to consist of sulfuric acid near the tropopause and mixtures of ammonium sulfate and soot in the remaining column. We obtain closure to within 25% for the optical depth of a column, which includes a biomass-burning aerosol of North American origin, and infer a soot volume fraction of 35% for this aerosol. Assuming spheroidal particles of prolate shape and the average aspect ratio of the particles to be 1.3 in the biomass-burning aerosol layer, the calculated depolarization agrees with the lidar measurement, whereas comparing the spectral backscatter coefficient shows the soot to be externally mixed with the nonabsorbing particles. With the two-stream approximation, we estimate the local, instantaneous, cloud-free radiative forcing of the biomass-burning aerosol at the tropopause to -5.8 W/m(2) with a corresponding optical depth of 0.09 at 710 nm wavelength and solar zenith angle of 56degrees. The radiative forcing for the biomass-burning aerosol is as sensitive to a change in state of mixture, either external or internal, as to a change in surface albedo, ocean to coniferous forest.