Light absorption enhancement (E-abs) of black carbon (BC) aerosol following atmospheric aging is one of the most challenging issues in the assessment of aerosol radiative forcing. BC E-abs is constrained by complex particle morphologies; however, large uncertainties continue to occur due to certain morphological parameters, including primary particle size. The values of E-abs during BC aging is quantified with diverse primary particle sizes using the superposition T-matrix method (STM). The results show that the uncertainty of absorption enhancement due to the primary particle size of fully aged BC particles ranges from similar to 10% to 20%, while the uncertainties arising from varied BC volume-equivalent size and fractal dimension are similar to 20-30% and similar to 8-12%, respectively. The optical properties of BC particles with volume-equivalent radii ranging from 50 to 70 nm were largely influenced (up to similar to 50%) by inappropriate assumptions regarding primary particle size. The specific assumptions of primary particle size in optical modeling plays an important role in constraining BC E-abs. (C) 2020 Elsevier Ltd. All rights reserved.

Tar balls are frequently found in slightly aged biomass burning plumes. They are spherical in shape, have diameters between similar to 100 and 300 nm, are amorphous and composed mostly of oxygen and carbon. Tar balls are light absorbing and considered to be a component of brown carbon. Tar balls have been typically reported and analyzed as individual spheres: however, in a recent study, we reported the presence of significant fractions of fractal-like aggregates made of several tar balls in fire plumes from different geographical locations. Aggregation affects the optical properties of particles; therefore, we use T-Matrix and Lorenz-Mie simulations to explore the effects of aggregation on the tar balls' optical properties in the 350 - 1150 nm wavelength range. We also evaluate the effects of different refractive indices available from the literature, different monomer numbers, and monomer sizes, as these are key factors determining the aggregates optical properties. Furthermore, we estimate the simple forcing efficiency for low and high surface albedos. Aggregates have a single scattering albedo (SSA) higher than that of individual tar balls (Delta SSA(550) (nm) up to 0.22). The hemispherical upscatter fraction of individual tar balls is more than 100% larger than for tar ball aggregates in many cases. The top of the atmosphere simple forcing efficiency over dark surfaces shows large variabilities with an increase up to similar to 53% for tar ball aggregates compared to individual tar balls. These results demonstrate that aggregation of tar balls can have a significant impact on their optical properties and radiative forcing. (C) 2019 Elsevier Ltd. All rights reserved.

Soot particles positively influence radiative forcing due to their strong absorption. Because of their chain-like structure, aggregated soot particles become more compact with the aging process, and the monomers or particles are always covered by water coatings. The optical parameters of two typical soot-water mixtures (i.e., an aggregate with core-shell monomers and a soot aggregate inside a water droplet) at 550 nm were investigated using the superposition T-matrix method, with a focus on the impact of the morphology and water coating of soot aggregates. For the soot aggregate with core-shell monomers, a relationship among the fractal dimension, relative humidity (RH) and monomer number was established and used to calculate optical parameters. The intensity of forward scattering declined with the increasing RH. The Cext, Csca, Cabs and SSA are much more insensitive to RH under higher RH conditions (RH > 90%) than at a lower RH level. In addition, hygroscopic shrinkage and the thickness of water coating have stronger effects on the optical properties of larger aggregated soot at higher RH than lower RH. For another mixing state, the soot aggregate inside a water droplet, the morphology of the soot core plays an important role in the optical properties when the thickness of the water shell is small. When the diameter ratio of the water droplet to the aggregated soot (D_ratio) changes from 1.2 to 2.8, Cext difference increases from 0.23 mu m(2) to 2.36 mu m(2) for particles with N = 100 and 500, whereas the SSA difference decreases from 0.12 to 0.01. If the agglomerated structure of the soot core is not considered, the Cext, Csca and SSA will be underestimated for a relatively small D_ratio of 1.2. Ignoring the soot core in the water droplet could introduce large errors into the calculation of the optical parameters, and ignoring the structure of the aggregated soot core could enlarge the errors.

The optical properties of light absorbing soot aerosols generally change through interactions with weakly absorbing particles, resulting in complex mixing states, and have been highlighted as a major uncertainty in assessing their radiative forcing and climatic impact. The single scattering properties of soot aggregates partially embedded in the host sulfate particle (semi-embedded soot-containing mixtures) are investigated for two kinds of morphologies with intersecting and non-intersecting surfaces. The surfaces cannot be overlapped in the non-intersecting surface morphology, while the intersecting surface morphology is unconstrained. Based on the modified diffusion limited aggregation (DLA) algorithm, the models with non-intersecting surfaces are simulated and applied for the single scattering calculations of semi-embedded soot-containing mixtures using the superposition T-matrix (STM) method. For comparison, the models with intersecting surfaces are simulated with the same morphological parameters, but some soot monomers are intersected by the host sphere. Due to the limitation of current STM method, the optical properties of these models with intersecting surfaces are calculated using the discrete dipole approximation (DDA) method. The soot volume fractions outside sulfate host (F-s,F-out) are introduced and applied to characterize the mixing states of the soot-containing aerosols. These simulations show that the absorption cross-sections of those internally, deeply, half and slightly embedded mixed soot particles (F-s,F-out = 0.0, 02, 0.5, 0.8) are similar to 105%, similar to 65%, similar to 43% and similar to 14% larger than the semi-external mixtures (F-s,F-out = 1.0), respectively. The results also indicate that the differences of extinction cross-sections, single scattering albedo (SSA) and asymmetry parameter (ASY) between simulations with intersecting and non-intersecting surfaces are small ( < 1%) for semi-embedded soot-containing mixtures with the same morphological parameters. Within the range of visible and near-infrared wavelengths, the relative deviations of absorption cross-sections between these different morphologies are also small ( < similar to 5%). Therefore, based on these simulations, the single scattering properties of semi-embedded soot-containing mixtures are rarely influenced by the morphological differences between the absorbing spheres intersecting and non-intersecting the non-absorbing host, which can nearly be ignored in the single scattering (C) 2015 Elsevier Ltd. All rights reserved.