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Black carbon (BC) aerosols are important for absorbing aerosols, affecting global climate change and regional air quality, and potentially harming human health. From March to May 2023, we investigated black carbon aerosol levels and air pollution in Beijing. Employing methods such as linear regression, Potential Source Contribution Function (PSCF) and Concentration-Weighted Trajectory (CWT), we analyzed the characteristics and sources of black carbon aerosols in the region. Results indicate that the light absorption coefficients of BC and BrC decrease with increasing wavelength, with BrC accounting for less than 40% at 370 nm. Daily variations in BC and PM2.5 concentrations exhibit similar trends, peaking in March, and BC displays a distinct bimodal hourly concentration structure during this period. Aethalometer model results suggest that liquid fuel combustion contributes significantly to black carbon (1.08 ± 0.71 μg·m−3), surpassing the contribution from solid fuel combustion (0.31 ± 0.2 μg·m−3). Furthermore, the significant positive correlation between BC and CO suggests that BC emissions in Beijing predominantly result from liquid fuel combustion. Potential source area analysis indicates that air masses of spring in Beijing mainly originate from the northwest (40.93%), while potential source areas for BC are predominantly distributed in the Beijing–Tianjin–Hebei region, as well as parts of the Shandong, Shanxi and Henan provinces. Moreover, this study reveals that dust processes during spring in Beijing have a limited impact on black carbon concentrations. This study's findings support controlling pollution in Beijing and improving regional air quality. [ABSTRACT FROM AUTHOR]

Black carbon (BC) mass size distribution (BCMSD) is crucial in both the environment and the climate system due to BC's intense size-dependent absorption of solar radiation. BC-containing particles larger than 700 nm (BC >700) could contribute to more than half of bulk BC mass concentration. Unfortunately, previous methods concentrated on BC-containing particles of less than 700 nm because of technical limitations. The contribution of BC to absorption and the radiative effect might be underestimated without consideration of BC >700. In this study, equivalent BCMSD (eBCMSD) from 150 nm up to 1.5 µm was measured at high time resolution of 1 h for the first time by an aerodynamic aerosol classifier in tandem with an aethalometer in two field campaigns over eastern China, namely Changzhou located in the Yangtze River Delta and Beijing located in the North China Plain. The results revealed that the pattern of eBCMSD in Changzhou (Beijing) was mostly bimodal (unimodal) peaking at 240 and 1249 nm (427 nm). The peak diameter of eBCMSD in Changzhou did not shift significantly with increasing pollution (240 to 289 nm). In contrast, the peak diameter of eBCMSD in Beijing shifted towards larger sizes, from 347 to 527 nm, with increasing pollution, indicating that the aging process at the urban site was different from that at the regional background site. eBCMSD in both Changzhou and Beijing had a significant diurnal cycle with a smaller (larger) value of eBCMSD during daytime (nighttime). Equivalent BC >700 (eBC >700) was ubiquitous and varied significantly with different locations and pollution levels. The campaign-averaged contribution of eBC >700 to bulk eBC mass concentration (meBC,bulk), bulk absorption coefficient (σab,bulk) and estimated direct radiative forcing of eBC (DRF eBC) in Changzhou and Beijing were 27.8 % (20.9 %–36.5 %) and 24.1 % (17.5 %–34.2 %), 19.6 % (15.8 %–24.6 %) and 25.9 % (19.6 %–33.7 %) and 20.5 % (18.4 %–22.2 %) and 21.0 % (16.3 %–26.1 %), respectively. meBC,bulk , σab,bulk and DRF eBC of eBC >700 in Changzhou (Beijing) increased by a factor of 3.6 (5.1) from 0.11 (0.07) to 0.40 (0.36) µgm-3 , by a factor of 3.2 (5.5) from 0.54 (0.63) to 1.75 (3.45) Mm -1 and by a factor of 2.4 (4.7) from 0.1 (0.1) to 0.24 (0.47) W m -2 , respectively, with the aggravation of pollution. The contribution of eBC >700 to meBC,bulk and σab,bulk had a significant diurnal cycle with a higher (lower) fraction during daytime (nighttime) in both Changzhou and Beijing. A case study indicated that the contribution of eBC >700 to meBC,bulk , σab,bulk and DRF eBC could reach up to 50 %, 50 % and 40 %, respectively. It was highly recommended to consider the whole size range of BC-containing particles in model estimation of the BC radiative effect. [ABSTRACT FROM AUTHOR]

Black carbon (BC), an important component of atmospheric aerosol, plays a significant role in regional climate, hydrological cycle, variation of monsoon rainfall, and human health. The 40-year detailed atmospheric BC over China from 1981 to 2020 is systematically investigated through the MERRA-2 reanalysis dataset. MERRA-2 BC generally showed a good correlation (R = 0.68) compared with 673 monthly samples from ground-based observation at 35 stations around China. The overall annual average of MERRA-2 BC concentration over China is 1.15 μg/m3, with a fast growth rate during 1981–2007 and a relatively slow decrease after that. The winter season has the highest mean concentration of BC, followed by autumn and spring, whereas summer shows relatively weaker values. The order of annual average BC concentrations during 1981–2020 is Beijing-Tianjin-Hebei region (BTH, 4.02 μg/m3) > Sichuan Basin (SB, 3.94 μg/m3) > Yangtze River Delta (YRD, 2.68 μg/m3) > Pearl River Delta (PRD, 1.47 μg/m3). The monthly mean BC concentrations over the BTH, YRD, PRD and SB are estimated to be smallest 3.18 μg/m3 in May, 1.94 μg/m3 in August, 0.82 μg/m3 in July, 3.04 μg/m3 in June, respectively, whilst largest consistently in December with 5.09 μg/m3, 3.83 μg/m3, 2.12 μg/m3, and 5.41 μg/m3, respectively. Our study indicates the primary potential source areas for BC are concentrated in the research city and its surroundings. Beijing and Chengdu are more BC-polluted areas than Shanghai and Guangzhou. Long-distance, regional transfer from south BTH contributes importantly to BC pollution in Beijing under the influence of prevailing southerly winds. The geographical location of Chengdu causes the transport and accumulation of BC inside the SB. [ABSTRACT FROM AUTHOR]

Observations suggest that the vertical distributions of air pollutants, such as black carbon (BC), present as various types depending on the emission sources and meteorological diffusion conditions. However, the formation process and source appointment of some special BC profiles are not fully understood. In this paper, by using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) with a BC-tagging technique, we investigate the formation mechanism and regional sources of a BC peak in the free troposphere observed by an aircraft flight in Beijing (BJ) on 5 May 2018. The results show that the contribution rate of the Beijing–Tianjin–Hebei (BTH) region to the surface BC of BJ exceeded 80 % in this case. Local sources dominated BC in BJ from the surface to approximately 700 m (78.5 %), while the BC peak in the free troposphere (∼4000 m) was almost entirely imported from external sources (99.8 %). Combining BC tracking and process analysis, we find that horizontal advection (HADV) and vertical advection (VADV) processes played an important role in the convergent and upward movement and the transport of BC. The BC originating from the surface in central provinces, including Shanxi (SX), Henan (HN), and Hebei (HB), had been uplifted through a cyclone system 16 h previously, was transported to a height of approximately 3000 m above BJ, and was then lifted by the VADV process to approximately 4000 m. At the surface, BJ and its surroundings were under the control of a weak pressure gradient, leading to the accumulation of BC within the boundary layer. Our results indicate that cyclone systems can quickly lift air pollutants, such as BC, up to the free troposphere, as well as extend their lifetimes and further affect the regional atmospheric environment and climate. [ABSTRACT FROM AUTHOR]

The light-absorbing organic aerosol (OA), known as brown carbon (BrC), has important radiative impacts; however, its sources and evolution after emission remain to be elucidated. In this study, the light absorption at multiple wavelengths, mass spectra of OA and microphysical properties of black carbon (BC) were characterized at a typical suburban environment in Beijing. The absorption of BC is constrained by its size distribution and mixing state, and the BrC absorption is obtained by subtracting the BC absorption from the total aerosol absorption. Aerosol absorption was further apportioned to BC, primary BrC and secondary BrC by applying the least correlation between secondary BrC and BC. The multilinear regression analysis on the factorized OA mass spectra indicated that the OA from traffic and biomass burning emission contributed to primary BrC. Importantly, the moderately oxygenated OA (O / C = 0.62) was revealed to highly correlate with secondary BrC. These OA had higher nitrogen content, in line with the nitrogen-containing functional groups detected by the Fourier transform infrared spectrometer. The photochemical processes were found to reduce the mass absorption cross section (MAC) of primary OA, reducing its contribution to total absorption by 20 %, at the same time increasing MAC for secondary OA, which showed a 30 % enhancement in contribution to total absorbance, implying the concurrent whitening and darkening of BrC. This provides field evidence that the photochemically produced secondary nitrogen-containing OA can considerably compensate for some bleaching effect on the primary BrC, hereby causing radiative impacts. [ABSTRACT FROM AUTHOR]

The vertical distribution of black carbon (BC), as well as its mixing state, is of great concern due to BC's strong regional climatic and environmental effects. In this study, vertical measurements were conducted through a moveable container based on a meteorological tower in the Beijing urban area during June and July. A total of 112 vertical profiles (0–240 m), including the concentrations of BC, O 3 , NO x and the optical properties of aerosols, were obtained. Based on BC concentration, the vertical profiles could be classified into four categories: uniform, gradual decrease, sharp decrease and sudden increase. The uniform type indicates strong vertical mixing with similar pollutant concentrations along the vertical direction. The gradual and sharp decrease types indicate stable vertical conditions with higher pollutant concentrations on the ground and lower concentrations at higher altitudes. Due to the strong radiation in summer, the vertical profiles exhibited a clear diurnal variation in which ∼ 80 % of profiles were uniform during the daytime and ∼ 40 %–90 % of profiles were of the gradual and sharp decrease types at night. O 3 is an exception, and its concentration generally increases with height, even under strong vertical mixing conditions. The size distribution of the BC core varied slightly along the vertical direction, and the coating thickness, denoted by the diameter ratio between the BC-containing particle and BC core (Dp/Dc), of BC increased with height under stable conditions. Although the coating thickness could increase the absorption ability with an average absorption enhancement of 1.25 at 23:00 LT (local time: UTC + 8), the vertical difference of Dp/Dc (2 %) was much lower than that of BC concentration (∼ 35 %). The vertical variation in absorption ability was mainly caused by the variation in BC concentration. In addition, O 3 and Dp/Dc occasionally increased during 06:00–08:00 but remained stable during 08:00–10:00. Vertical mixing and transportation from upper heights, such as the residual layer, could significantly influence the pollutant properties on the surface during early mornings. This study exhibits a continuous vertical picture of BC and its mixing state in urban areas, which would be helpful for understanding BC's regional environmental effect. [ABSTRACT FROM AUTHOR]

The effective density of black carbon (BC) is a crucial factor that is relevant to its aging degree and adds uncertainty in evaluating its climate effect. Here, we have developed a new method to retrieve the effective density of internally mixed BC in the atmosphere, combining field observations conducted from 15 November to 14 December 2016 in urban Beijing with the Köhler theory. The uncertainty in the retrieval method was evaluated to be within ±30 %, which was primarily caused by assumptions on both the hygroscopic parameter of organics and the proportional distribution of primary organic aerosols in different hygroscopic modes. Using the method, we find that the ambient internally mixed BC, accounting for 80 % ± 20 % of total BC aerosol particles, was retrieved with a campaign mean density of 1.1 ± 0.6 gcm-3 during the observed periods. The retrieved result was comparable with that reported in the literature. By applying a lower (0.14 gcm-3) and upper (2.1 gcm-3) limit of the retrieved BC density in the cloud condensation nuclei (CCN) number concentration (NCCN) estimation, we derived that the neglect of such variations in the BC density would lead to an uncertainty of - 28 %–11 % in predicting NCCN at supersaturations of 0.23 % and 0.40 %. We also find that the NCCN was more sensitive to the variations in BC density when it was <1.0 gcm-3. This illustrates the necessity of accounting for the effect of BC density on CCN activity closer to source regions where the BC particles are mostly freshly emitted. The CCN closure was achieved when introducing the retrieved real-time BC density and mixing state. This study provides a unique way of utilizing field measurements to infer ambient BC density and highlights the importance of applying variable BC density values in models when predicting CCN and assessing its relevant climate effect. [ABSTRACT FROM AUTHOR]

Unprecedented urbanization in China has led to serious urban heat island (UHI) issues, exerting intense heat stress on urban residents. Based on the observed temperature and PM 2.5 concentrations in Beijing over 2016–2020, we find diverse influences of aerosol pollution on urban heat island intensity (UHII) under different circulations. When northerly winds are prevalent in urban Beijing, UHII tends to be much higher in both daytime and nighttime and it is less affected by aerosol concentrations. However, when southerly and westerly winds are dominant in rural Beijing, UHII is significantly reduced by aerosol pollution. Using coupled aerosol-radiation weather simulations, we demonstrate the underlying physical mechanism which is associated with local circulation and resulting spatial distribution of aerosols. Our results also highlight the role of black carbon in aggravating UHI, especially during nighttime. It could thus be targeted for cooperative management of heat islands and aerosol pollution. [ABSTRACT FROM AUTHOR]

The radiative forcing of black carbon (BC) depends strongly on its mixing state in different chemical environments. Here we analyzed the chemical composition and mixing state of BC-containing particles by using a single-particle aerosol mass spectrometer and investigated their impact on light absorption enhancement (Eabs) at an urban (Beijing) and a rural site (Gucheng) in the North China Plain. While the BC was dominantly mixed with organic carbon (OC), nitrate, and sulfate at both the urban and rural sites, the rural site showed a much higher fraction of BC coated with OC and nitrate (36 % vs. 15 %–20 %). Moreover, the BC mixing state evolved significantly as a function of relative humidity (RH), with largely increased coatings of OC–nitrate and nitrate at high RH levels. By linking with an organic aerosol (OA) composition, we found that the OC coated on BC comprised dominantly secondary OA in Beijing, while primary and secondary OA were similarly important in Gucheng. Furthermore, Eabs was highly dependent on secondary inorganic aerosol coated on BC at both sites, while the coated primary OC also resulted in an Eabs of ∼ 1.2 for relatively fresh BC particles at the rural site. A positive matrix factorization analysis was performed to quantify the impact of different mixing states on Eabs. Our results showed a small Eabs (1.06–1.11) for BC particles from fresh primary emissions, while the Eabs increased significantly above 1.3 when BC was aged rapidly with increased coatings of OC–nitrate or nitrate; it can reach above 1.4 as sulfate was involved in BC aging. [ABSTRACT FROM AUTHOR]

Vertical profiles of black carbon (BC) play a critical role in modifying the meteorological conditions such as temperature, planetary boundary layer height (PBLH), and regional circulation, which influence surface layer concentrations of PM 2.5 (particulate matter with a diameter of 2.5 µ m or less; the surface layer covers from 0 to 79.5 m). However, BC vertical profiles in current models usually have large uncertainties. In this study, by using measurements of BC vertical profiles in Beijing collected by King Air 350 aircraft and the Weather Research and Forecasting with Chemistry model (WRF-Chem) coupled with an improved integrated process (IPR) analysis scheme, we investigated the direct radiative effect (DRE) of BC with different vertical profiles on meteorology and PM 2.5 concentrations in Beijing during two severe haze events (11–12 and 16–19 December 2016). Compared with measurements in Beijing, the model overestimated BC concentrations by 87.4 % at the surface and underestimated BC mass by 14.9 % at altitudes of 300–900 m as averaged over the two pollution events. The BC DRE with the default vertical profiles from the model heated the air around 300 m altitude, but the warming would be stronger when BC vertical profiles were modified for each day using the observed data during the two severe haze events. Accordingly, compared to the simulation with the default vertical profiles of BC, PBLH was reduced further by 24.7 m (6.7 %) and 6.4 m (3.8 %) in Beijing in the first and second haze events, respectively, with the modified vertical profiles, and hence the surface layer PM 2.5 concentrations were higher by 9.3 µ g m -3 (4.1 %) and 5.5 µ g m -3 (3.0 %) over central Beijing, owing to increased positive contributions of vertical mixing and chemical processes. Furthermore, we quantified by sensitivity experiments the roles of BC vertical profiles with six exponential decline functions (C(h)=C0×e-h/hs and hs​​​​​​​ = 0.35, 0.48, 0.53, 0.79, 0.82, and 0.96) parameterized on the basis of the observations. A larger hs means less BC at the surface and more BC in the upper atmosphere, resulting in less solar radiation reaching the ground and consequently a stronger cooling at the surface (+ 0.21 with hs of 0.35 vs. - 0.13 ∘ with hs of 0.96). Our results indicate that it is very important to have accurate vertical profiles of BC in simulations of meteorology and PM 2.5 concentrations during haze events. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols play an important role in the radiation balance of the earth–atmosphere system. However, our knowledge of the long-term changes in equivalent black carbon (eBC) and aerosol optical properties in China is very limited. Here we analyze the 9-year measurements of eBC and aerosol optical properties from 2012 to 2020 in Beijing, China. Our results showed large reductions in eBC by 71 % from 6.25 ± 5.73 µ g m -3 in 2012 to 1.80 ± 1.54 µ g m -3 in 2020 and 47 % decreases in the light extinction coefficient (bext , λ = 630 nm) of fine particles due to the Clean Air Action Plan that was implemented in 2013. The seasonal and diurnal variations of eBC illustrated the most significant reductions in the fall and at nighttime, respectively. Δ eBC / Δ CO also showed an annual decrease from ∼ 7 to 4 ng m -3 ppbv -1 and presented strong seasonal variations with high values in spring and fall, indicating that primary emissions in Beijing have changed significantly. As a response to the Clean Air Action Plan, single-scattering albedo (SSA) showed a considerable increase from 0.79 ± 0.11 to 0.88 ± 0.06, and mass extinction efficiency (MEE) increased from 3.2 to 3.8 m 2 g -1. These results highlight the increasing importance of scattering aerosols in radiative forcing and a future challenge in visibility improvement due to enhanced MEE. Brown carbon (BrC) showed similar changes and seasonal variations to eBC during 2018–2020. However, we found a large increase of secondary BrC in the total BrC in most seasons, particularly in summer with the contribution up to 50 %, demonstrating an enhanced role of secondary formation in BrC in recent years. The long-term changes in eBC and BrC have also affected the radiative forcing effect. The direct radiative forcing (ΔFR) of BC decreased by 67 % from + 3.36 W m -2 in 2012 to + 1.09 W m -2 in 2020, and that of BrC decreased from + 0.30 to + 0.17 W m -2 during 2018–2020. Such changes might have important implications for affecting aerosol–boundary layer interactions and the improvement of future air quality. [ABSTRACT FROM AUTHOR]

PM2.5 (fine) and PM2.5–10 (coarse) samples were collected using a Gent stack filter unit sampler in Xinzhen, Beijing. The 220 samples collected from September 2016 to June 2018 were analyzed by neutron activation analysis (NAA) and Black Carbon meter, and 19 elements were determined. Time series analysis, correlation analysis and enrichment factor analysis were performed on the determined component concentrations. The possible sources and temporal variation of some elements were discussed. In addition, the main pollution elements in the three different pollution events were obtained. Furthermore, the element component characteristics of the coarse and fine particles were determined. Finally, the source and backward trajectory of a heavy sandstorm were analyzed by HYSPLIT. Using neutron activation analysis (NAA) and Black Carbon meter, the concentrations of elements and Black Carbon (BC) were determined. Through the correlation analysis and time series analysis, the possible sources and temporal variation of some elements were discussed. Among them, Al, Ca, Ti and Mg in APM are contributed by soil and surface dust. They have strong correlation and similar temporal trend. The concentrations of these elements have obvious seasonal variations. The concentrations of these elements are high in spring and summer, and low in autumn and winter. [ABSTRACT FROM AUTHOR]

Aerosols from surface emission can be transported upwards through convective mixing in the planetary boundary layer (PBL), which subsequently interact with clouds, serving as important sources to nucleate droplets or ice particles. However, the evolution of aerosol composition during this vertical transport has yet to be explicitly understood. In this study, simultaneous measurements of detailed aerosol compositions were conducted at two sites, namely urban Beijing (50 m above sea level – a.s.l.) and Haituo mountain (1344 m a.s.l.) during wintertime, representing the anthropogenically polluted surface environment and the top of the PBL, respectively. The pollutants from surface emissions were observed to reach the mountain site on daily basis through daytime PBL convective mixing. From the surface to the top of PBL, we found efficient transport or formation of lower-volatility species (black carbon, sulfate, and low-volatile organic aerosol, OA); however, a notable reduction in semivolatile substances, such as the fractions of nitrate and semivolatile OA reduced by 74 % and 76 %, respectively, during the upward transport. This implies that the mass loss of these semivolatile species was driven by the evaporation process, which repartitioned the condensed semivolatile substances to the gas phase when aerosols were transported and exposed to a cleaner environment. In combination with the oxidation processes, these led to an enhanced oxidation state of OA at the top of the PBL compared to surface environment, with an increase of oxygen to carbon atomic ratio by 0.2. Such a reduction in aerosol volatility during vertical transport may be important in modifying its viscosity, nucleation activity, and atmospheric lifetime. [ABSTRACT FROM AUTHOR]

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]

Black carbon (BC) forms an important component of particulate matter globally, due to its impact on climate, the environment and human health. Identifying and quantifying its emission sources are critical for effective policymaking and achieving the desired reduction in air pollution. In this study, we present the first direct measurements of urban BC fluxes using eddy covariance. The measurements were made over Beijing within the UK-China Air Pollution and Human Health (APHH) winter 2016 and summer 2017 campaigns. In both seasons, the mean measured BC mass (winter: 5.49 ng m -2 s -1 , summer: 6.10 ng m -2 s -1) and number fluxes (winter: 261.25 particles cm -2 s -1 , summer: 334.37 particles cm -2 s -1) were similar. Traffic was determined to be the dominant source of the BC fluxes measured during both seasons. The total BC emissions within the 2013 Multi-resolution Emission Inventory for China (MEIC) are on average too high compared to measured fluxes by a factor of 58.8 (winter) and 47.2 (summer). Only a comparison with the MEIC transport sector shows that emissions are also larger (factor of 37.5 in winter and 37.7 in summer) than the measured flux. Emission ratios of BC / NO x and BC / CO are comparable to vehicular emission control standards implemented in January 2017 for gasoline (China 5) and diesel (China V) engines, indicating a reduction of BC emissions within central Beijing, and extending this to a larger area would further reduce total BC concentrations. [ABSTRACT FROM AUTHOR]

Black carbon aerosols play an important role in climate change because they directly absorb solar radiation. In this study, the mixing state of refractory black carbon (rBC) at an urban site in Beijing in the early summer of 2018 was studied with a single-particle soot photometer (SP2) as well as a tandem observation system with a centrifugal particle mass analyzer (CPMA) and a differential mobility analyzer (DMA). The results demonstrated that the mass-equivalent size distribution of rBC exhibited an approximately lognormal distribution with a mass median diameter (MMD) of 171 nm. When the site experienced prevailing southerly winds, the MMD of rBC increased notably, by 19 %. During the observational period, the ratio of the diameter of rBC-containing particles (Dp) to the rBC core (Dc) was 1.20 on average for Dc=180 nm, indicating that the majority of rBC particles were thinly coated. The Dp/Dc value exhibited a clear diurnal pattern, with a maximum at 14:00 LST and a Dp growth rate of 2.3 nm h -1 ; higher Ox conditions increased the coating growth rate. The microphysical properties of rBC were also studied. Bare rBC particles were mostly found in fractal structures with a mass fractal dimensions (Dfm) of 2.35, with limited variation during both clean and polluted periods. The morphology of rBC changed with coating thickness increasing. When the mass ratio of nonrefractory matter to rBC (MR) was <1.5, rBC-containing particles were primarily found in external fractal structures, and they changed to a core–shell structure when MR>6 , at which point the measured scattering cross section of rBC-containing particles was consistent with that based on the Mie-scattering simulation. We found that only 28 % of the rBC-containing particles were in core–shell structures with a particle mass of 10 fg in the clean period but that proportion increased considerably, to 45 %, in the polluted period. Due to the morphology change, the absorption enhancement (Eabs) was 12 % lower than that predicted for core–shell structures. [ABSTRACT FROM AUTHOR]

Refractory black carbon (rBC) in the atmosphere is known for its significant impacts on climate. The relationship between the microphysical and optical properties of rBC remains poorly understood and is influenced by its size and mixing state. Mixing state also influences its cloud scavenging potential and thus atmospheric lifetime. This study presents a coupling of a centrifugal particle mass analyser (CPMA) and a single-particle soot photometer (SP2) for the morphology-independent quantification of the mixing state of rBC-containing particles, used in the urban site of Beijing as part of the Air Pollution and Human Health–Beijing (APHH-Beijing) project during winter (10 November–10 December 2016) and summer (18 May–25 June 2017). This represents a highly dynamic polluted environment with a wide variety of conditions that could be considered representative of megacity area sources in Asia. An inversion method (used for the first time on atmospheric aerosols) is applied to the measurements to present two-variable distributions of both rBC mass and total mass of rBC-containing particles and calculate the mass-resolved mixing state of rBC-containing particles, using previously published metrics. The mass ratio between non-rBC material and rBC material (MR) is calculated to determine the thickness of a hypothetical coating if the rBC and other material followed a concentric sphere model (the equivalent coating thickness). The bulk MR (MR bulk) was found to vary between 2 and 12 in winter and between 2 and 3 in summer. This mass-resolved mixing state is used to derive the mass-weighted mixing state index for the rBC-containing particles (χrBC). χrBC quantifies how uniformly the non-rBC material is distributed across the rBC-containing-particle population, with 100 % representing uniform mixing. The χrBC in Beijing varied between 55 % and 70 % in winter depending on the dominant air masses, and χrBC was highly correlated with increased MR bulk and PM 1 mass concentration in winter, whereas χrBC in summer varied significantly (ranging 60 %–75 %) within the narrowly distributed MR bulk and was found to be independent of air mass sources. In some model treatments, it is assumed that more atmospheric ageing causes the BC to tend towards a more homogeneous mixture, but this leads to the conclusion that the MR bulk may only act as a predictor of χrBC in winter. The particle morphology-independent and mass-based information on BC mixing used in this and future studies can be applied to mixing-state-aware models investigating atmospheric rBC ageing. [ABSTRACT FROM AUTHOR]

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 g cm -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 1.4 g cm -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 g cm -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. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is one of the most important climate pollutants due to its strong positive radiative forcing on the climate system. However, long-term observation of BC is inadequate, and its trend remains unknown at both regional and global scales. In this study, using quality-controlled ground-based black carbon observations at 34 stations, the climatology of BC mass concentration during 2006–2017 in China was evaluated for the first time. The national annual average BC concentration was 3534 ng/m3, and the concentration exhibited large spatial variation, from a minimum of 272 ng/m3 to a maximum of 10,228 ng/m3. Significant seasonal variations were also observed. The peak BC concentration (4763 ± 3380 ng/m3) occurred during winter, followed by autumn (3752 ± 2623 ng/m3) and spring (3022 ± 2121 ng/m3). The lowest BC concentration occurred in summer (2583 ± 1780 ng/m3) due to decreased emissions, wet removal by precipitation, and diffusion induced by strong turbulent mixing. Additionally, the diurnal variability at about 80% of the stations in China showed a bimodal pattern. Daily maximum BC concentration during 0000–0600, 0600–1200, 1200–1800, and 1800–2400 local solar time accounted for 0, 41, 12, and 47% of the total, respectively. In particular, the diurnal and monthly variations in BC were explicitly analyzed at seven baseline stations. Surface BC has exhibited a significant declining trend across China, which is partly corroborated by the increase in single scattering albedo during the same period in Beijing. Also, the BC radiative forcing at the top of the atmosphere has declined at the rate of − 0.9 ± 0.1 W/m2/10 years over China, which differs from with the trend in the simulation using the CMIP6 emission. The decreasing BC has led to a larger reduction rate in atmospheric heating (− 3.7 ± 0.4 W/m2/10 years), implying a less stable atmosphere that facilitates the dispersion of air pollutants. The declining BC burden implies for both the air quality in China and regional climate change. [ABSTRACT FROM AUTHOR]

The morphology and effective density of externally mixed black carbon (extBC) aerosols, important factors affecting the radiative forcing of black carbon, were studied using a tandem technique coupling a differential mobility analyzer (DMA) with a single-particle soot photometer (SP2). The study extended the mass–mobility relationship to large extBC particles with a mobility diameter (dmob) larger than 350 nm, a size range seldom included in previous tandem measurements of BC aggregates in the atmosphere. The experiment was conducted at an urban site in Beijing during a 19 d winter period from 23 January to 10 February 2018. Ambient dry particles were selected by the DMA, and the size-resolved extBC particles were distinguished from particles with a thick coating (internally mixed) according to the time delay between the incandescence signal peak and the scattering peak detected by the SP2. The masses of the extBC particles were then quantified. The time differences between the DMA size selection and the SP2 measurement were processed previously. The normalized number size distributions were investigated at the prescribed dmob sizes in the range of 140–750 nm to provide the typical mass of extBC at each dmob. On this basis, the mass–mobility relationship of the ambient extBC was established, inferring a mass–mobility scaling exponent (Dfm) (an important quantity for characterizing the morphology of fractal-like BC aggregates) with a value of 2.34±0.03 in the mobility range investigated in this study. This value is comparable with those of diesel exhaust particles, implying a predominant contribution of vehicle emissions to the ambient extBC in urban Beijing. Compared to the clean period, a higher Dfm value was observed in the polluted episode, indicating a more compact BC aggregate structure than that in the clean period. The effective densities (ρeff) of the extBC in the same dmob range were also derived, with values gradually decreasing from 0.46 g cm -3 at 140 nm mobility to 0.14 g cm -3 at 750 nm mobility. The ρeff values were slightly lower than those measured using the DMA–aerosol particle mass analyzer (APM) system. The difference in ρeff values was likely due to the lower BC masses determined by the SP2 compared to those measured by the APM at the same mobility, since the SP2 measured the refractory BC (rBC) mass instead of the total mass of the BC aggregate, which consists of both rBC and a possible fraction of nonrefractory components measured by the APM. The ρeff values in the 280–350 nm dmob range were much closer to the values for soot aggregates reported in the literature. It might be related to the more compact structure of BC aggregates in this range, resulting from the reconstruction effect by volatile and/or semivolatile components in the atmosphere. The reconstruction effect might also result in a hiatus in the increased dynamic shape factor in the range of 200–350 nm, which presented an overall increase from 2.16 to 2.93 in the 140–750 nm dmob range. [ABSTRACT FROM AUTHOR]

The effect of black carbon (BC) on air quality and the climate is still unclear, which is partly because of the poor understanding regarding the BC aging process in the atmosphere. In this work, we developed a new approach to simulate the BC mixing state (i.e., other species coated on the BC surface) based on an emissions inventory and back-trajectory analysis. The model tracks the evolution of the BC aging degree (characterized by the size ratio of the whole particle and BC core) during atmospheric transport. Using the models, we quantified the mass-averaged aging degree of total BC particles transported to a receptor (e.g., an observation site) from various emission origins (i.e., 0.25∘×0.25∘ grids). The simulations showed good agreement with the field measurements, which validated our model calculation. Modeling the aging process of BC during atmospheric transport showed that it was strongly dependent on emission levels. BC particles from extensive emission origins (i.e., polluted regions) were characterized by a higher aging degree during atmospheric transport due to more co-emitted coating precursors. On the other hand, high-emission regions also controlled the aging process of BC particles that were emitted from cleaner regions and passed through these polluted regions during atmospheric transport. The simulations identified the important roles of extensive emission regions in the BC aging process during atmospheric transport, implying the enhanced contributions of extensive emission regions to BC light absorption. This provides a new perspective on the phenomenon of pollution building up in the North China Plain, further demonstrating that this is mainly driven by regional transport and transformation. The simulation of the BC aging degree during atmospheric transport provided more clues for improving air pollution and climate change. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is known to have major impacts on both human health and climate. The populated megacity represents the most complex anthropogenic BC emissions where the sources and related impacts are very uncertain. This study provides source attribution and characterization of BC in the Beijing urban environment during the joint UK–China APHH (Air Pollution and Human Health) project, in both winter (November–December 2016) and summer (May–June 2017). The size-resolved mixing state of BC-containing particles was characterized by a single-particle soot photometer (SP2) and their mass spectra was measured by a soot particle aerosol mass spectrometer (SP-AMS). The refractory BC (rBC) mass loading was around a factor of 2 higher in winter relative to summer, and more variable coatings were present, likely as a result of additional surface emissions from the residential sector and favourable condensation in the cold season. The characteristics of the BC were relatively independent of air mass direction in summer, whereas in winter air masses from the Northern Plateau were considerably cleaner and contained less-coated and smaller BC, but the BC from the Southern Plateau had the largest core size and coatings. We compare two online source apportionment methods using simultaneous measurements made by the SP2, which measures physical properties of BC, and the chemical approach using the positive matrix factorization (PMF) of mass spectra from the SP-AMS for the first time. A method is proposed to isolate the BC from the transportation sector using a mode of small BC particles (core diameter Dc<0.18 µ m and coating thickness ct < 50 nm). This mode of BC highly correlated with NOx concentration in both seasons (∼14 ng m -3 BC ppb -1 NOx) and corresponded with the morning traffic rush hour, contributing about 30 % and 40 % of the total rBC mass (35 % and 55 % in number) in winter and summer respectively. The BC from coal burning or biomass burning was characterized by moderate coatings (ct = 50–200 nm) contributing ∼20 %–25 % of rBC mass. Large uncoated BC particles (Dc>0.18 µ m and ct < 50 nm) were more likely to be contributed by coal combustion, as these particles were not present in urban London. This mode was present in Beijing in both winter (∼30 %–40 % rBC mass) and summer (∼40 % rBC mass) but may be dominated by the residential and industrial sector respectively. The contribution of BC thickly coated with secondary species (ct > 200 nm) to the total rBC mass increased with pollution level in winter but was minor in summer. These large BC particles importantly enhanced the absorption efficiency at high pollution levels – in winter when PM 1 > 100 µ g m -3 or BC > 2 µ g m -3 , the absorption efficiency of BC increased by 25 %–70 %. The reduction of emissions of these large BC particles and the precursors of the associated secondary coating will be an effective way of mitigating the heating effect of BC in urban environments. [ABSTRACT FROM AUTHOR]

In Beijing, the probability of snowfall is decreasing as a result of global warming. At the same time, Beijing has suffered severe air pollution. In this paper, the concentration and particle size characteristics of BC (Black Carbon) in snow during the winter of 2015 in Beijing were analyzed by the SP2 method. The average concentration of BC in snow meltwater in Beijing is 82 ng/mL, with a minimum value of 62.9 ng/mL and a maximum of 210.6 ng/mL. The BC particle size in snow and ice in the Beijing area is mostly concentrated in the range of 70–400 nm. After log-normal, the BC particle size above 600 nm is still small, which should be closely related to the nature of the local BC emission source. The concentration of BC in snow is highly susceptible to meteorological conditions and local pollution levels. When Beijing is under the control of the east wind or the southeast wind, aerosols in the urban areas can easily accumulate in the northwestern mountains and then settle or participate in the snowfall process, resulting in an increase in BC aerosol accumulation in the snow, thus further changing the optical properties of snow in the Beijing area. [ABSTRACT FROM AUTHOR]