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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]

Severe hailstorms frequently occurred in Beijing between May and August 2021, leading to extensive hail damage. These hailstorms were observed by radar and satellite data, and reported by surface observers. In this study, the spectral and cloud microphysical characteristics of typical Beijing events in 2021 were analyzed using Himawari-8 satellite products and ground-based S-band weather radar data obtained from the Beijing Meteorological Bureau. The relationship between Himawari-8 brightness temperature differences (BTD) and radar reflectivity was also investigated. The results revealed that the significant spectral depression of brightness temperatures (BTs) in hail clouds was observed by a satellite. Furthermore, the stronger the radar reflectivity was, the more rapidly BTD decreased, with a nonlinear relationship between them. The results of cloud physical characteristics show that, for cloud-top heights above 10 km, the cloud effective radius was about 25 μm, with a cloud-top temperature of 225 K during these hail events. By means of Gaussian fitting, the BT threshold value (11.2 μm) was determined by satellite at 230 K, with a BTD focused on 1.9 K when hailstorms occurred. These results will help us better understand the characteristics of hailstorms, while also providing information for future hail suppression in Beijing. [ABSTRACT FROM AUTHOR]

Secondary particulate matter exerts adverse effects on air quality and human health. The production or reaction rate of secondary aerosols in polluted environments remains uncertain and is complicated by diverse emissions and meteorological conditions. By concurrently measuring the mass spectra of compounds in both particulate (using an aerosol mass spectrometer) and gas phases (using proton‐transfer‐reaction mass spectrometry) in suburban Beijing, we linked the secondary organic aerosol (OA) and volatile organic compounds (VOCs) to photochemical age (tage) and obtained their reaction or production rates. Factorization analysis of the mass spectra of OA and the 108 VOC species resolved three oxygenated OAs (OOA) and three secondary VOC factors at different oxidation levels. Primary organic aerosols and VOCs from traffic sources were determined to be important sources for secondary aerosol formation. At high pollution levels under the conditions of weaker solar radiation and higher relative humidity, moderately oxygenated OA (O/C = 0.61) and secondary inorganics were coproduced in combination with rapid consumption of all VOCs. At lower pollution levels, the intense solar radiation caused substantial and rapid production of OOA (O/C = 0.81) and intermediate VOCs (both in a high oxidation state) at a rate of 15.0% h−1 and 14.0% h−1, respectively. These results highlight the feedback effects between radiation and moisture in terms of altering the formation mechanism of secondary aerosols. In particular, highly oxygenated secondary airborne products under strong radiation should be considered in regard to their environmental impact. Plain Language Summary: In this study, the compositions of submicron aerosols and volatile organic compounds (VOCs) in suburban Beijing were concurrently characterized for their detailed mass spectra, and based on these spectra, the primary and secondary sources were apportioned to investigate their evolution and conversion. Our results demonstrate the contrasting phenomena of chemical evolution under the influence of solar radiation and moisture. Photo‐oxidation was observed to rapidly produce organic aerosol (OA) and secondary VOCs in a considerably high oxidation state, while higher relative humidity induced overall moderately oxygenated OA and secondary inorganic aerosols but resulted in more rapid consumption of all VOCs. Key Points: Mass spectra of organic compounds in both aerosols and gases were concurrently characterized in suburban BeijingThe production and consumption rates of organic aerosols (OAs) and gases were obtained under high radiation or moist conditionsHighly oxidized OAs and intermediate volatile gases are rapidly produced through photo oxidation under strong solar radiation [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 water uptake of aerosol influences its optical depth and capacity for cloud formation, depending on the vertical profile of aerosol hygroscopicity because of different solar radiation received and supersaturation (SS) conditions at different atmospheric levels. Such information is lacking over the polluted East Asian region. This study presents aircraft-based in situ measured aerosol size distributions and chemical compositions by a series of flights over the Beijing area in wintertime. Under high relative humidity (hRH) conditions (surface RH > 60 %), a significant enhancement of aerosol hygroscopicity parameter (κ) in the planetary boundary layer (PBL) was observed to increase by 50 % from 0.20 up to 0.34 from the surface to the top of the PBL (vertical gradient of ∼0.13 km -1), along with the dry particle effective diameter (Deff) being increased by 71 % and activation ratio up to 0.23 (0.64) at SS =0.05% (0.1 %). However, a lower vertical gradient of κ (0.05 km -1) and smaller Deff was exhibited under low RH (lRH, surface RH < 60 %). This suggests that the aqueous processes played an important role in promoting the enhancement of particle hygroscopicity in the PBL. The κ in the lower free troposphere (LFT) was relatively stable at 0.24±0.03 with a slight increase during regional transport. The enhancement of aerosol optical depth (AOD) due to water uptake ranged 1.0–1.22 for the PBL under lRH and LFT, but it reached as high as 6.4 in the PBL under hRH. About 80 % and 18 % of the AOD were contributed to by aerosol hygroscopic growth under hRH and lRH, respectively. These results emphasize the important evolution of aerosol water-uptake capacity in the PBL, especially under the high RH condition. [ABSTRACT FROM AUTHOR]

The physical properties of black carbon (BC) including the mass loading, size distribution and mixing state were in-situ characterized by aircraft measurements using a single particle soot photometer (SP2) in the lower troposphere over Beijing area. The flights were conducted in both late spring and winter during the daytime with well-developed planetary boundary layer (PBL). The BC mass in the PBL (BC PBL) in late spring showed no apparent vertical gradient nor correlation with the PBL height (PBLH) due to strong convective mixing; in winter the BC PBL was more concentrated near ground and anti-correlated with the PBLH due to dilution effect of the dominant cleaner northerly air masses at higher altitude. The BC mass loading at height h , C(h) within the PBL can be extended from the surface level (C0) in late spring; for levels above the PBL, C(h) can be parameterized by applying an exponential decline function C(h) = C0*exp(h/hs) , with the scale height (hs) of 0.31 ± 0.16 km and 0.66 ± 0.24 km for late spring and winter respectively. This parameterization excluded the profiles for: turbulent conditions when the BC mass was efficiently vented upwards and diluted, expressed as C(h) = C0 up to the top of the PBL; or in periods of strong southerly advection, when the entire column was significantly influenced by regional transport from the polluted south regions. The BC core mass median diameters (MMD) were commonly populated at 205–220 nm in both seasons, with additional mode of MMD ∼195 nm also frequently observed in late spring. The bulk relative coating thickness of BC (coated diameter divided by uncoated core diameter D p /D c) in the PBL mostly populated at 2.0–2.2 but at ∼1.2–1.6 in the lower free troposphere (FT). The mass absorption cross section of BC at 550 nm (MAC550), constrained by the SP2 measurements, was largely influenced by the coating thickness, was relatively consistent in the PBL at ∼8.6 m2 g−1, but reduced to 7–7.5 m2 g−1 in the FT or turbulent condition due to decreased coatings. The BC was found to exhibit smaller particle size in the FT but larger in the PBL, which may imply larger BC have been scavenged by low-level clouds. The BC particles trapped in the PBL or regionally transported from polluted region represent the most absorbing element in the particulate matter population and should be particularly considered in evaluating the radiative forcing impact of aerosols over this region. • Vertical profiles of black carbon physical properties in the lower troposphere were in-situ characterized over Beijing. • Black carbon at different layers was influenced by seasonal emission and meteorological conditions. • These results will improve modelling on black carbon radiative forcing and constrain remote sensing absorption measurement. [ABSTRACT FROM AUTHOR]

Abstract To investigate the transport and formation mechanism of pollution in Beijing, this study explored the vertical profiles of aerosol properties using aircraft measurement during a regional transport (RT) pollution event from 10th to 12th December 2016. The aerosol chemical composition and size distribution were characterized. Different vertical structures exhibited during three periods (defined as before RT, during RT, and after RT) for this pollution event. Before RT, PM 2.5 and black carbon (BC) mass loading were at low level in the mixing layer (ML) when the clean northerly air mass dominated. During RT, an elevated aerosol layer, in which BC and PM 2.5 mass concentrations were about 1.5 times higher than that at the ground level, was found in the upper ML (at 400–900 m) over Beijing. This elevated aerosol layer was advected by the prevailing southwesterly air mass which transported the pollutants from the intensively polluted southwestern region over Beijing. These aerosols through RT featured with pronounced secondary compositions and large coatings on BC particles. After RT, the pollutants were significantly diluted by the prevailing NW air mass, whereas the aerosol concentration almost maintained in the near surface, leading to notable vertical gradient. The continued surface pollution may result from the low wind speed and secondary aerosol formation in the next day. This study suggests that only the ground observation could not fully explain the pollution event, but the variation of vertical structure of aerosol properties should be considered to elucidate the formation mechanism of pollution over Beijing. Graphical abstract Comparison of vertical BC profiles between Beijing and Baoding show that the BC mass concentration of Baoding was 4 times larger than that of Beijing on December 10, and 1.6 times smaller than that of Beijing on December11. It is very interesting to found an enhanced BC layer from 400 to 900 m in upper mixing layer over Beijing on December11. The meteorological analysis indicated that the enhanced layer was caused by the regional transport from the surface area in the southern part of North China Plain. Through vertical mixing in the mixing layer in Beijing, the ground PM2.5 mass concentration was increased quickly. Our results verified that the rapidly increase of pollution in Beijing was caused by southern transport at high altitude. Image 1 Highlights • Different vertical structures were exhibited during different pollution period. • An elevated layer was found in the upper mixing layer during the regional transport period. • Vertical structure of aerosol properties was needed to elucidate the formation mechanism of pollution over Beijing. [ABSTRACT FROM AUTHOR]

Ice-nucleating particles (INPs) are of great importance for regional weather and climate by altering the microphysical properties of clouds. However, large uncertainties still exist for INP concentrations over the polluted North China Plain (NCP) due to limited INPs observation in this region and the complex physical and chemical properties of aerosols from multiple sources. In this study, the concentrations of INPs active in the immersion freezing mode at temperatures ranging from −5 °C to −30 °C are simultaneously measured for about one month in the Spring season at a mountain site and a suburb site in Beijing representing clean and anthropogenic condition, respectively. Different concentrations and characteristics of INPs are found between the two sites, which reflect the influence of different air masses and INP sources. Consistent with previous studies in this region, dust particles are found to be the most efficient INPs during the Spring season, and the contribution of anthropogenic pollution aerosols was not obvious. Most interestingly, the INP concentration at the mountain site was about one magnitude higher than at the suburban site at temperatures warmer than −10 °C, which is caused by primary biological aerosol originating from the forest in the mountainous area. Our results underline the important role of these biological aerosols, which are also expected to have a strong impact on the glaciation of orographic clouds. • Meteorological conditions were the main influencing factor of INPs over Beijing. • Mineral dusts were found to be the most efficient INPs sources during the Spring season. • Primary biological aerosol particles from the northwest boreal forest area of Beijing might be an important INPs source. [ABSTRACT FROM AUTHOR]