Optical Properties and Radiative Forcing of Aged BC due to Hygroscopic Growth: Effects of the Aggregate Structure

Abstract

Black carbon (BC) particles become hydrophilic after mixing with soluble matter in the atmosphere, and their optical and radiative properties can be significantly modified accordingly. This study investigates the impact of aggregate structure on optical and radiative properties of aged BC, that is, BC coated by sulfate or organic aerosols, especially during hygroscopic growth. A more realistic BC morphology based on fractal aggregates is considered, and inhomogeneous mixtures of BC aggregates are treated more realistically (with respect to particle geometries) in the multiple sphere T‐matrix method for optical property simulations. As relative humidity increases, BC extinction is significantly enhanced due to an increase in scattering, and the enhancement depends on the amount and hydrophilicity of the coating. The absorption exhibits less variation during hygroscopic growth because the coating of aerosols already leads to BC absorption close to the maximum. Furthermore, hygroscopic growth not only results in negative radiative forcing (RF) at the top of the atmosphere but also slightly weakens the absorption in the atmosphere (inducing a negative RF in the atmosphere). Compared to the more realistic model with BC as aggregates, the currently popular core‐shell model reasonably approximates the top of the atmosphere RF but underestimates the atmospheric RF due to hygroscopic growth by up to 40%. Furthermore, for the RF caused by internal mixing, the core‐shell model overestimates the RFs at the surface and in the atmosphere by ~10%.