Advanced modeling of the absorption enhancement of black carbon particles in chamber experiments by considering the morphology and coating thickness

Highlights

● CS structure overestimates ρ _eff by nearly six times at externally mixed states.

● FA method reproduces the evolution of BCc morphology.

● MSTM can reproduce a more realistic evolution of optical properties.

● A two-stage calibration of E _abs as the function of coating fractions is developed.

Abstract

Measurements studies have shown that the absorption of radiation by black carbon (BC) increases as the particles age. However, there are significant discrepancies between the measured and modeled absorption enhancement (E_abs), largely due to the simplifications used in modeling the mixing states and shape diversities. We took advantage of chamber experiments on BC aging and developed an efficient method to resolve the particle shape based on the relationship between the coating fraction (∆D_ve/D_ve,0) and fractal dimension (D_f), which can also reflect the variations of D_f during the whole BC aging process. BC with externally and partly mixed states (0 ≤ ∆D_ve/D_ve,0 ≤ 0.5) can be considered to be uniformly distributed with the D_f values of 1.8–2.1, whereas the D_f values are constrained in the range 2.2–2.8 for fully mixed states (∆D_ve/D_ve,0 > 0.5). The morphological parameters (i.e., the effective density and the dynamic shape factor) were compared with the measured values to verify the simulated morphology. The simulated mean deviations of morphological parameters were smaller than 8% for the method resolving the particle shape. By applying a realistic shape and refractive index, the mass absorption cross for fully mixed states can be improved by 11% compared with a simplified core–shell model. Based on our understanding of the influence of D_f and ∆D_ve/D_ve,0 on E_abs, we propose a two-stage calibration equation to correct the E_abs values estimated by the core–shell model, which reduces the simulation error in the Mie calculation by 6%–14%.

Graphical abstract

Keywords

Black carbon / Mixing states / Fractal dimension / Dynamic shape factor / Absorption enhancement

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Acknowledgements

This work was supported by the National Key R&D Program of China (2018YFC0213800), the National Natural Science Foundation of China (Grant No. 42021004), and the open fund of the Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control (China) (KHK1908).

Conflict of Interests

The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

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