Abstract
We show the effect of composition heterogeneity and shape on the optical properties of urban dust particles based on the three-dimensional spatial and optical modeling of individual particles. Using scanning electron microscopy/energy-dispersive X-ray spectroscopy (SEM/EDX) and focused ion beam (FIB) tomography, spatial models of particles collected in Los Angeles and Seattle accounted for surface features, inclusions, and voids, as well as overall composition and shape. Using voxel data from the spatial models and the discrete dipole approximation method, we report extinction efficiency, asymmetry parameter, and single-scattering albedo (SSA). Test models of the particles involved (1) the particle's actual morphology as a single homogeneous phase and (2) simple geometric shapes (spheres, cubes, and tetrahedra) depicting composition homogeneity or heterogeneity (with multiple spheres). Test models were compared with a reference model, which included the particle's actual morphology and heterogeneity based on SEM/EDX and FIB tomography. Results show particle shape to be a more important factor for determining extinction efficiency than accounting for individual phases in a particle, regardless of whether absorption or scattering dominated. In addition to homogeneous models with the particles' actual morphology, tetrahedral geometric models provided better extinction accuracy than spherical or cubic models. For iron-containing heterogeneous particles, the asymmetry parameter and SSA varied with the composition of the iron-containing phase, even if the phase was <10% of the particle volume. For particles containing loosely held phases with widely varying refractive indexes (i.e., exhibiting "severe" heterogeneity), only models that account for heterogeneity may sufficiently determine SSA.