Effective densities of soot particles and their relationships with the mixing state at an urban site in the Beijing megacity in the winter of 2018

摘要

The effective density (ρeff) of refractory black carbon (rBC) is a key parameter relevant to its mixing state that imposes great uncertainty in evaluating the direct radiation forcing effect. In this study, a tandem differential mobility analyzer–centrifugal particle analyzer–single-particle soot photometer (DMA–CPMA–SP2) system was used to investigate the relationship between the effective density (ρeff) and the mixing state of rBC particles during the winter of 2018 in the Beijing megacity. During the experiment, aerosols with a known mobility diameter (Dmob) and known ρeff values (0.8, 1.0, 1.2, 1.4, 1.6, and 1.8 gcm?3) were precisely selected and measured by the SP2 to obtain their corresponding mixing states. The results showed that the ρeff well represented the morphological variation in rBC-containing particles. The rBC-containing particles changed from an irregular structure to a compact spherical structure with the increase in ρeff. A ρeff value of 1.4gcm?3 was the morphological transition point. The morphology and ρeff value of the rBC-containing particles were intrinsically related to the mass ratio of non-refractory matter to rBC (MR). As the ρeff values of the rBC-containing particles increased from 0.8 to 1.8 gcm?3, the MR of the rBC-containing particles significantly increased from 2 up to 6–8, indicating that atmospheric aging processes were likely to lead to the reconstruction of more compact and regular particle shapes. During the observation period, the ρeff of the majority of rBC-containing particles was smaller than the morphology transition point independent of the pollution conditions. This suggested that the major rBC-containing particles did not have a spherical structure. Simulation based on an aggregate model considering the morphological information of the particles demonstrated that absorption enhancement of rBC-containing particles could be overestimated by ～17% by using a core–shell model. This study highlights the strong dependence of the morphology of ambient rBC-containing particles on ρeff and will be helpful for elucidating the microphysical characteristics of rBC and reducing uncertainty in the evaluation of rBC climate effects and health risks.