Light absorption and scattering by aggregates: Application to black carbon and snow grains

A geometric-optics surface-wave approach has been developed for the computation of light absorption and scattering by nonspherical particles for application to aggregates and snow grains with external and internal mixing structures. Aggregates with closed- (internal mixing) and open-cell configurations are constructed by means of stochastic procedures using homogeneous and core-shell spheres with smooth or rough surfaces as building blocks. The complex aggregate shape and composition can be accounted for by using the hit-and-miss Monte Carlo geometric photon tracing method. We develop an integral expression for diffraction by randomly oriented aggregates based on Babinet's principle and a photon-number weighted geometric cross section. With reference to surface-wave contributions originally developed for spheres, we introduce a nonspherical correction factor using a non-dimensional volume parameter such that it is 1 for spheres and 0 for elongated particles. The extinction efficiency, single-scattering albedo, and asymmetry factor results for randomly oriented columns and plates compare reasonably well with those determined from the finite-difference time domain (FDTD) and the discrete dipole approximation (DDA) computer codes for size parameters up to about 20. The present theoretical approach covers all size ranges and is particularly attractive from the perspective of efficient light absorption and scattering calculations for complex particle shape and inhomogeneous composition.We show that under the condition of equal volume and mass, the closed-cell configuration has larger absorption than its open-cell counterpart for both ballistic and diffusion-limited aggregates. Because of stronger absorption in the closed-cell case, most of the scattered energy is confined to forward directions, leading to a larger asymmetry factor than the open-cell case. Additionally, light absorption for randomly oriented snowflakes is similar to that of their spherical counterparts under the condition of equal geometrical cross section area for both external and internal mixing states; however, nonspherical snowflakes scatter less light in forward directions than spheres, resulting in a substantial reduction of the asymmetry factor. We further demonstrate that small soot particles on the order of 1 μm internally mixed with snow grains could effectively reduce snow albedo by as much as 5-10%. Indeed, the depositions of black carbon would substantially reduce mountain-snow albedo, which would lead to surface warming and snowmelt, critical to regional climatic surface temperature amplification and feedback.

► A light absorption and scattering approach is developed for aggregate aerosols. ► It combines geometric optics and surface waves using spheres as building blocks. ► Internal mixing and closed- and open-cells are accounted for by stochastic means. ► The approach is useful for complex particle shape and inhomogeneous composition. ► A 1 μm soot internally mixed with snow grain is shown to reduce snow albedo by 5-10%.