Black carbon fractal morphology and short-wave radiative impact: a modelling study

Abstract

Abstract. We investigate the impact of the morphological properties of freshly emitted black carbon aerosols on optical properties and on radiative forcing. To this end, we model the optical properties of fractal black carbon aggregates by use of numerically exact solutions to Maxwell's equations within a spectral range from the UVC to the mid-IR. The results are coupled to radiative transfer computations, in which we consider six realistic case studies representing different atmospheric pollution conditions and surface albedos. The spectrally integrated radiative impacts of black carbon are compared for two different fractal morphologies, which brace the range of recently reported experimental observations of black carbon fractal structures. We also gauge our results by performing corresponding calculations based on the homogeneous sphere approximation, which is commonly employed in climate models. We find that at top of atmosphere the aggregate models yield radiative impacts that can be as much as 2 times higher than those based on the homogeneous sphere approximation. An aggregate model with a low fractal dimension can predict a radiative impact that is higher than that obtained with a high fractal dimension by a factor ranging between 1.1–1.6. Although the lower end of this scale seems like a rather small effect, a closer analysis reveals that the single scattering optical properties of more compact and more lacy aggregates differ considerably. In radiative flux computations there can be a partial cancellation due to the opposing effects of different error sources. However, this cancellation effect can strongly depend on atmospheric conditions and is therefore quite unpredictable. We conclude that the fractal morphology of black carbon aerosols and their fractal parameters can have a profound impact on their radiative forcing effect, and that the use of the homogeneous sphere model introduces unacceptably high biases in radiative impact studies. We emphasise that there are other potentially important morphological features that have not been addressed in the present study, such as sintering and coating of freshly emitted black carbon by films of organic material. Finally, we found that the spectral variation of the absorption cross section of black carbon significantly deviates from a simple 1/λ scaling law. We therefore discourage the use of single-wavelength absorption measurements in conjunction with a 1/λ scaling relation in broadband radiative forcing simulations of black carbon.