Significant contribution of fractal morphology to aerosol light absorption in polluted environments dominated by black carbon (BC)

Abstract

In recent years, researchers have emphasized the use of fractal aggregate morphology instead of the core-shell morphology in global climate models for estimating black carbon (BC) forcing. This study confirms that fractal morphology plays an important role in reducing the overestimation of aerosol light absorption calculations in the case of an urban polluted environment. During periods of high anthropogenic BC emissions at Delhi, the particle light absorption is overestimated by 50 to 200% by assumptions of both external mixing and internal core-shell mixing. While incorporating the aggregate morphology model into light absorption simulations is beneficial in such cases, it comes with a high computational burden. To address this, we propose a metric known as morphology index (MI). This index distributes the weightage between the two extreme cases of core-shell and fractal aggregate to obtain accurate particle light absorption. Long-range transported aerosols were estimated to have an MI of 0.78, and fresh local emissions had an MI of 0.48. A BC-based aerosol classification approach was developed to determine the most relevant particle size mode for light absorption. The method is based on patterns found between the correlations of the BC mass concentrations and aerosol number concentrations at the different particles sizes (BC-size correlation spectra). BC-size correlation spectra are introduced as a concept that may be used (i) independently to understand the size-dependent heterogeneous distribution of aerosol light absorption and (ii) in conjunction with MI to accurately model the optical properties of aerosols in different BC regimes.