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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]

Black carbon (BC) exerts important radiative effects over regions with intensive emissions. This study presents in-situ aircraft measurements of BC vertical profiles including mass loading, size distribution and mixing state, spanning a range of pollution levels in both warm and cold seasons over Beijing. The development of planetary boundary layer (PBL) influenced the properties of pollutants at low levels, and regional transport from the southwest elevated the pollution at higher altitudes. Thicker coatings of BC were associated with higher pollution in the PBL, where interactions between BC and other substances intensively took place. Considering the mixing state of BC, the absorption efficiency could be potentially increased by up to 86% and 60% in the PBL and lower free troposphere, respectively. Including a column-integrated absorption enhancement, the in-situ constrained absorption aerosol optical depth at wavelength 870 nm (AAOD 870) improved the agreement with AERONET by 28%, but the in-situ measurement remained 19% lower. A radiative transfer model finds a BC heating rate of 0.1–0.3 K/d and 0.5–3.1 K/d for less and more polluted environments respectively, and the BC coating effect could positively introduce a +0.1–4.2 Wm-2 radiative forcing. The presence of aerosol layer enhanced the positive vertical gradient of heating rate by redistributing the actinic flux. In particular, this gradient was further enhanced by introducing thickly-coated BC at higher level during the regional transport events, which may promote the temperature inversion and further depress the PBL development on polluted days. • BC mass loading for less polluted Beijing was consistent with urban EU/NA. • BC heating rate in the PBL increased to 0.5-3.1K/d on polluted days and had positive vertical gradient. • BC coatings enhanced the columnar absorption up to 80% with positive radiative forcing +0.1–4.2 Wm-2. [ABSTRACT FROM AUTHOR]

The accurate derivation of the proportion and absorption enhancement of black carbon (BC)-containing aerosols in the atmosphere is critical to assess their effect on air quality and climate. Here, using the field measured size-resolved volatility shrink factor, BC bulk mass concentration and the BC mass fraction in BC-containing particles in winter Beijing, we retrieved and quantified both the number and mass concentration of (1) non-BC, (2) internally mixed BC and (3) externally mixed BC of ambient fine aerosol particles. The reliability of the retrieval method has been evaluated by comparing with the simultaneously measured data. The number fraction of BC-containing particles accounts for 60–78% of ambient fine particles, with internally (both BC core and coating materials) and externally mixed BC of 51–64% and 9–23%, respectively. Only for nucleated particles on clean days, when nucleation is a major source of aerosol particles, did the non-BC component dominate (54%). A large amount of aerosols are BC-containing particles, with mass fraction of 32–52%, suggesting the dominant role of BC in elevating mass concentration of particulate matter (PM) in a polluted urban area. We also show that the BC particles are thickly coated with coating thickness (characterized by D p /D c , ratio of the BC diameter before and after heating at 300 °C) of 1.6–2.2, implying efficient aging of BC particles in polluted urban area. Our results imply a large proportion of BC-containing particles in the atmosphere, which could help towards understanding the role of BC on regional haze formation and climate forcing. Image 1 • Mixing state of BC was retrieved using a new method. • BC-containing particles account for large proportions of ambient fine aerosols. • The BC-containing particles are thickly coated. Main findings of this work: 1. BC-containing particles account for large proportion. 2. The BC-containing particles are thickly coated. [ABSTRACT FROM AUTHOR]