Under environment with various water contents, the variations in the mixing state and particle size of coated black carbon (BC) aerosols cause changes in optical and radiative effects. In this study, fractal models for thinly, partially, and thickly coated BC under six relative humidities (RHs 1/4 0-95%) are constructed and optically simulated at 1064 and 532 nm. Differential scattering cross-sections are selected to retrieve the mixing state (Dp/Dc) of BC to investigate the possible retrieval errors caused by the nonspherical morphology when using the single-particle soot photometer (SP2). Furthermore, the radiative forcing of BC aerosols at different RHs are analyzed. Results showed that the retrieval errors (REs) of Dp/Dc are negative for coated particles with BC volume fraction smaller than 0.10, indicating that the mixing states of coated fractal BC are underestimated during the hygroscopic growth. The partiallycoated BC has the best retrieval accuracy of the mixing state, followed by the closed-cell and coatedaggregate model, judging from averaged REs. Radiative forcing enhancements for partially-coated aerosols with different BC volume fractions exponentially increase to opposite values, resulting in a warming or cooling effect. This study helps understand the uncertainties in Dp/Dcof BC aerosols retrieved by SP2 and their radiative forcing at different RHs. (c) 2025 Chinese Society of Particuology and Institute of Process Engineering, Chinese Academy of Sciences. Published by Elsevier B.V. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Reducing the uncertainty in aerosol radiative forcing requires a comprehensive understanding of the factors affecting black carbon (BC) light absorption. In this study, the characteristics and influencing factors of light absorption enhancement (Eabs) of refractory BC (rBC) were investigated by conducting intensive measurements at an urban site in northwest China during the early summer of 2018. On average, the absorption of rBC was enhanced by 34% as a result of the internal mixing of rBC with other aerosol components. Secondary inorganic aerosols (SIAs) were found to have considerable effects on the Eabs of rBC. The Eabs showed a robust linear relationship with the bulk nitrate/rBC mass ratio in fine particles, with an increase of 3% per nitrate/rBC ratio unit. A notable increase in Eabs from dusk to the next morning was observed, in accordance with the diurnal variations in nitrate and sulfate, indicating the excellent contribution of non-photochemical formation of SIAs to Eabs. This fact was further supported by the positive correlation of the nitrate/rBC and sulfate/rBC ratios with relative humidity (RH) rather than photochemical indicators. This study indicates that the aqueous and/or heterogeneous formation of SIAs is likely the dominant aging pathway leading to the high Eabs of rBC.

Aerosol mixtures, which are still unclear in current knowledge, may cause large uncertainties in aerosol climate effect assessments. To better understand this research gap, a well-developed online coupled regional climate-chemistry model is employed here to investigate the influences of different aerosol mixing states on the direct interactions between aerosols and the East Asian summer monsoon (EASM). The results show that anthropogenic aerosols have high-level loadings with heterogeneous spatial distributions in East Asia. Black carbon aerosol loading accounts for more than 13% of the totals in this region in summer. Thus, different aerosol mixing states cause very different aerosol single scattering albedos, with a variation of 0.27 in East Asia in summer. Consequently, the sign of the aerosol instantaneous direct radiative forcing at the top of the atmosphere is changed, varying from - 0.95 to + 1.50 W/m(2) with increasing internal mixing aerosols. The influence of aerosol mixtures on regional climate responses seems to be weaker. The EASM circulation can be enhanced due to the warming effect of anthropogenic aerosols in the lower atmosphere, which further induces considerable aerosol accumulation associated with dynamic field anomaly, decrease in rainfall and so on, despite aerosol mixtures. However, this interaction between aerosols and the EASM will become more obvious if the aerosols are more mixed internally. Additionally, the differences in aerosol-induced EASM anomalies during the strongest and weakest monsoon index years are highly determined by the aerosol mixing states. The results here may further help us better address the environmental and climate change issues in East Asia.

The addition of coating to the black carbon (BC) enhances its absorption as more light is focused by the coating lens. The absorption enhancement factor (E-abs) of BC is difficult to quantify due to an inadequate representation of its mixing structure and the interaction with radiation. Here, by tracking the evolution of the fresh BC particles in the ambient, we found a transitional stage of the particle E-abs with the non-BC-to-BC mass ratio (R-BC) at similar to 2, below which there were insufficient coating materials to encapsulate the BC core and the absorption enhancement was not significant (similar to 14%). When the R-BC >similar to 2, obvious absorption enhancement occurred as the BC cores were fully covered. Secondary inorganic species played the most critical role in the coating materials to enhance the lensing effect. We suppose the particle-resolved core-shell Mie model can be applied in the E-abs prediction for most cases.

To establish the direct climatic and environmental effect of anthropogenic aerosols in East Asia in winter under external, internal, and partial internal mixing (EM, IM and PIM) states, a well-developed regional climate-chemical model RegCCMS is used by carrying out sensitive numerical simulations. Different aerosol mixing states yield different aerosol optical and radiative properties. The regional averaged EM aerosol single scattering albedo is approximately 1.4 times that of IM. The average aerosol effective radiative forcing in the atmosphere ranges from -0.35 to +1.40 W/m(2) with increasing internal mixed aerosols. Due to the absorption of black carbon aerosol, lower air temperatures are increased, which likely weakens the EAWM circulations and makes the atmospheric boundary more stable. Consequently, substantial accumulations of aerosols further appear in most regions of China. This type of interaction will be intensified when more aerosols are internally mixed. Overall, the aerosol mixing states may be important for regional air pollution and climate change assessments. The different aerosol mixing states in East Asia in winter will result in a variation from 0.04 to 0.11 K for the averaged lower air temperature anomaly and from approximately 0.45 to 2.98 mu g/m(3) for the aerosol loading anomaly, respectively, due to the different mixing aerosols.

Atmospheric black carbon (BC) has a large yet highly uncertain contribution to global warming. When mixed with non-BC/coating material during atmospheric aging, the BC light absorption can be enhanced through the lensing effect. Laboratory and modeling studies have consistently found strong BC absorption enhancement, while the results in ambient measurements are conflicting, with some reporting weak absorption enhancement even for particles with large bulk coating amounts. Here, from our direct field observations, we report both large and minor absorption enhancement factors for different BC-containing particle populations with large bulk non-BC-to-BC mass ratios. By gaining insights into the measured coating material distribution across each particle population, we find that the level of absorption enhancement is strongly dependent on the particle-resolved mixing state. Our study shows that the greater mixing-state heterogeneity results in the larger difference between observed and predicted absorption enhancement. We demonstrate that by considering the variability in coating material thickness in the optical model, the previously observed model measurement discrepancy of absorption enhancement can be reconciled. The observations and improved optical models reported here highlight the importance of mixing-state heterogeneity on BC's radiative forcing, which should be better resolved in large-scale models to increase confidence when estimating the aerosol radiation effect.

Mixing state of black carbon (BC) with secondary species has been highlighted as a major uncertainty in assessing its radiative forcing. While recent laboratory simulation has demonstrated that BC could serve as a catalyst to enhance the formation of sulfate, its role in the formation and evolution of secondary aerosols in the real atmosphere remains poorly understood. In the present study, the mixing of BC with sulfate/nitrate in the atmosphere of Guangzhou (China) was directly investigated with a single particle aerosol mass spectrometer (SPAMS). The peak area ratios of sulfate to nitrate (SNRs) for the BC-containing particles are constantly higher than those of the BC-free particles (defined as particles with negligible BC signals). Furthermore, the seasonal SNR peak is observed in summer and autumn, and the diurnal peak is found in the afternoon, consistent with the trends of radiation-related parameters (i.e., solar radiation and temperature), pointing to the BC-induced photochemical production of sulfate. Such hypothesis is further supported by the multilinear regression and random forest analysis, showing that the variation of SNRs associated with the BC-containing particles could be well explained (R-2 = similar to 0.7-0.8) by the radiation-related parameters (>30% of the variance) and the relative BC content (similar to 20%) in individual particles, but with limited influence of precursors (SO2/NOx: <5%). Differently, the radiation-related factors only explain <10% of the SNR variation for the BC-free particles. These results provide ambient observational evidence pointing to a unique role of BC on the photochemical formation and evolution of sulfate, which merits further quantitative evaluations.

Black carbon (BC) aerosols strongly absorb the solar radiation, affecting the regional and global climate through direct and indirect radiative forcing. The optical properties of BC are critical factors to estimate their radiative forcing. However, the optical absorption of BC is still under controversy partially due to the weakness in quantifying their complex morphology and mixing structures. Although a Discrete Dipole Approximation (DDA) can calculate optical properties of fine particles with arbitrary shapes, an appropriate definition of realistic BC shape models for optical simulation is essentially required. Here we present a novel Electron-Microscope-to-BC-Simulation (EMBS) tool to construct realistic BC shape models with various morphology and mixing structures for optical calculation using DDA. The optical properties of BC particles with different particle morphology, coating thickness, and embedded fraction (F) are estimated based on electron microscope. We find that absorption enhancement (E-abs) of the realistic irregular model is larger than that of the present commonly used spherical model (i.e., BC aggregate with spherical coating). The BC core morphology greatly influences E-abs of the embedded BC particles with irregular coating when the volume-equivalent-diameter ratio of particle to core (D-p/D-c) is larger than 1.8. The F significantly influences E-abs of BC particles, suggesting that the mixing structure between coating and core is an important factor to determine the optical absorption of aged BC particles. The study highlights that the BC core morphology, coating shape, coating thickness, and mixing structures influence their optical properties and should be considered as important variables in climate models.

Interactions between clouds and black carbon (BC) represent a significant uncertainty in aerosol radiative forcing. To investigate the influence of cloud processing on the scavenging of BC, concurrent measurement of individual cloud droplet residue particles (cloud RES) and interstitial particles (cloud INT) throughout a cloud event was deployed at Mt. Tianjing (1690 m a.s.l.) in southern China. An aethalometer (AE-33), a single particle aerosol mass spectrometer (SPAMS) and a scanning mobility particle sizer (SMPS) were used to investigate the mass concentration of equivalent BC (EBC), size-resolved number of BC-containing particles, and size-resolved number concentration of submicron particles in real-time, respectively. The number-based SEs of the submicron particles varied between 2.7 and 31.1%. Mass scavenging efficiency (MSE) ranged from 4.7% to 52.6% for EBC, consistent with the number-based SE (from 11.3% to 59.6%) of the BC-containing particles throughout the cloud event. Several factors that may influence the SEs of the BC-containing particles are considered and examined. SEs are most likely determined by a single factor, i.e., liquid water content (LWC), with R-2 > 0.8 in a power function throughout the cloud event. Stage-resolved investigation of SEs further reveals that particle size matters more than other factors in the cloud formation stage, whereas there is an increasing role of the mixing state in the development and stability stage. We also observed lower SEs for the BC-containing particles internally mixed organics, consistent with previous literature.

The refractive index of ambient aerosols is one of the most important parameters indicating the scattering and absorption properties of aerosols. We proposed a new method for retrieving the refractive index (RI) of ambient particles. The main advantage of our method is that it assimilates the single particle mixing states measured by a single-particle soot photometer, when compared to the traditional optical method of retrieving the ambient aerosol RI. This method was validated by good consistency between the determined RI with this method and retrieved RI with the method of Zhao et al. (2019c) using datasets from field measurements conducted in East China in June of 2018. The results show that the real part of the refractive index of the black carbon (BC)-free particles ranged between 1.37 and 1.51 and this value changed little across different tested wavelengths. The mean complex refractive index for the refractory BC was 1.67 +/- 0.67i at 525 nm. The mean imaginary parts of the other non-BC components were 0.019 and 0.023 at 450 nm and 370 nm respectively. Brown carbon contributed to 5%, 13% and 29% of the ambient aerosol light absorption at 525 nm, 450 nm and 370 nm respectively in East China. This study provides the ability to determine the ambient aerosol complex refractive index and these data can be used in models to reduce the uncertainties in estimating aerosol radiative forcing.