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The complex particle morphology of black carbon (BC) induces considerable uncertainties in constraining its optical properties. In particular, the diversity of how the BC core and coating are combined is yet to be resolved due to the lack of direct ambient quantification. In this study, by concurrent measurements of the electrical mobility diameter (Dm) and optical volume‐equivalent diameter (Dve), the dynamic shape factor (χ = Dm/Dve) of ambient BC‐containing particles at different mixing states was quantified for the first time. BC in urban Beijing showed a widely distributed χ of 1.4 ± 0.43. Particles with larger refractory BC (rBC) cores showed higher non‐sphericity and higher χ. A ten‐fold increase in the volume ratio of the coating over rBC (VR) could decrease the fraction of fractal BC by 36%. This study proposed a χ‐VR space to describe the particle shape, which is able to include all ambient quantified BC morphologies in optical model. Plain Language Summary: Black carbon (BC) is an important short‐lived light‐absorbing aerosol component in the atmosphere. Its optical properties are complicated by the complex particle morphology, such as the non‐BC substances associated with it and the combination of BC and non‐BC substances within particle. The previous quantification of particle morphology could not distinguish the information specifically for ambient BC, nor the single BC particle characterization can represent full diversities for all particles. This study used concurrent measurements of volume‐equivalent and mobility diameter of BC‐containing particles (BCc) to characterize the coating content and particle shape online for all BC particles in the ambient environment. As a result, we can include all the measured particle morphology information in optical models. Particles with larger BC cores showed higher non‐sphericity, with a greater discrepancy between the measured absorbing properties and that calculated by the Mie theory. Key Points: The morphology of ambient black carbon‐containing particles was characterized by volume‐equivalent and mobility diameter measurementsBlack carbon with higher coatings showed more spherical shapesA space using coatings and particle shape was developed to incorporate morphology information for all black carbon‐containing particles [ABSTRACT FROM AUTHOR]

Atmospheric loading of black carbon aerosols influences air quality and visibility, and their mixing state and aerosol chemistry were sensitive to both emission scenarios and regional transport. In this study, the aerodynamic size-resolved mixing state of refractory black carbon aerosols (rBC) was investigated using a novel tandem system consisting of an aerodynamic aerosol classifier (AAC), a single particle soot photometer (SP2), and single-particle-aerosol mass spectrometry (SPA-MS) during the XXIV Olympic Winter Games (OWG) at an urban site in Beijing. Particles with aerodynamic diameter (D ae) of 200 nm and 300 nm were selected by AAC to focus on the effect of relative differences in morphology on the coating thickness, coating compositions, and optical properties of rBC particles. We found that rBC-containing particles with D ae of 300 nm were characterized by a rBC core with a count median diameter (CMD) of 108 ± 4 nm that typically have regular morphology (χ : m e a n ∼ 1) , higher relative coating thickness (RCT: mean ∼1.9), and strong light absorption enhancement (E abs : mean ∼1.5). The rBC-containing particles with D ae = 200 nm normally had irregular shapes (χ : m e a n ∼ 1.4) and weak E abs (E abs : mean ∼1.37). Classification based on air mass clustering and air pollution level revealed that the coating thickness of rBC particles only exhibited unimodal patterns under clean air conditions and distinct bimodal distributions under heavy pollution conditions, implying multiple origins of rBC particles, even during OWG periods. The coating thickness and E abs of rBC particles were greater when influenced by the higher RH air from east. Furthermore, the chemical compositions of the rBC coating quantitatively determined by SPA-MS were used to estimate the possible origins of the D ae = 300 nm, featured by a thicker coating thickness and stronger light absorption enhancement. Our results showed that rBC particles were primarily mixed with organics, nitrate, and sulfate during the XXIV OWG period. The organic components have a limited role in increasing rBC coatings under polluted conditions, while the alkali metal ions (K and Na) associated with traffic emissions and the secondary inorganic species favor the formation of thick coatings. Higher RH makes limited contributions to rBC mixed with sulfate and organics only (BCOC*_S) and pure BC. The relatively fresh BC could directly mix with organics and sulfate at low RH levels while evolving to mix with nitrate at high RH conditions. In addition to high concentrations of locally emitted precursors and high RH that tend to form thick coatings of nitrate-related rBC aerosols, secondary transport from the west and southwest also contributes to rBC aerosols mixed with nitrate with relatively thick coatings. • rBC with an aerodynamic diameter (D ae) of 300 nm typically have regular morphology. • rBC of regular shape(D ae = 300 nm)has thicker coatings and stronger absorption enhancement. • During the OWG, rBC particles were primarily mixed with organics, nitrate and sulfate. • rBC particles had multiple sources, even in the OWG periods. • The organic components have a limited role in increasing rBC coatings under polluted conditions. [ABSTRACT FROM AUTHOR]