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The aerosol liquid water content (ALWC) dictates the hygroscopicity of aerosol particles. To date, measurements of ALWC have been confined primarily to ground-based observations although vertical profiles of ALWC are crucial for understanding its interactions with meteorology. This study proposes a novel method for deriving profiles of ALWC using data acquired by a Light Detection and Ranging (LiDAR), a microwave radiometer, and a suite of aerosol instruments measuring aerosol physical and chemical properties, deployed during a five-month field experiment in Guangzhou, China. The retrieval approach is based on a machine-learning model named the gradient-boosted decision tree model. The inversion accuracy and stability are assessed through comparisons with ALWC data acquired on the ground and at the top of the Guangzhou tower of 532 m above ground. The agreements are encouraging: with the coefficient of determination $({R} ^{2}) = 0.870$ and root-mean-square error (RMSE) = $3.28 ~\mu \text{g} ~\cdot $ m−3 for all data; ${R} ^{2} = 0.776$ and RMSE = $2.18 ~\mu \text{g}~ \cdot $ m−3 for tower data; and ${R} ^{2} = 0.872$ and RMSE = $4.1~ \mu \text{g} ~\cdot $ m−3 for ground data. From the vertical distribution of the retrieved ALWC in Guangzhou, ALWC is higher in the lower boundary layer, especially when air pollution is severe. The proportion of liquid water in aerosol particles is closely related to the relative humidity in the environment, which will affect the morphology of aerosol particles (with about every 10% increase in liquid water, the depolarization ratio decreases by 0.02). The model may be of general use for studying air pollution and secondary aerosol generation. [ABSTRACT FROM AUTHOR]

A comprehensive field experiment measuring aerosol chemical and physical properties at a suburban site in Beijing around the 2019 Spring Festival was carried out to investigate the impact of reduced anthropogenic emissions on aerosol formation. Sharply reduced sulfur dioxide (SO2) and nitrogen dioxide (NO2) concentrations during the festival holiday resulted in an unexpected increase in the surface ozone (O3) concentration caused by the strong O3 -titration phenomenon. Simultaneously, the reduced anthropogenic emissions resulted in massive decreases in particle number concentration at all sizes and the mass concentrations of organics and black carbon. However, the mass concentrations of inorganics (especially sulfate) decreased weakly. Detailed analyses of the sulfur oxidation ratio and the nitrogen oxidation ratio suggest that sulfate formation during the holiday could be promoted by enhanced nocturnal aqueous-phase chemical reactions between SO2 and O3 under moderate relative humidity (RH) conditions (40 % < RH < 80 %). Daytime photochemical reactions in winter in Beijing mainly controlled nitrate formation, which was enhanced a little during the holiday. A regional analysis of air pollution patterns shows that the enhanced formation of secondary aerosols occurred throughout the entire Beijing–Tianjin–Hebei (BTH) region during the holiday, partly offsetting the decrease in particle matter with an aerodynamic diameter less than 2.5 µ m. Our results highlight the necessary control of O3 formation to reduce secondary pollution in winter under current emission conditions. [ABSTRACT FROM AUTHOR]

The aerosol liquid water (ALW) content (ALWC), an important component of atmospheric particles, has a significant effect on atmospheric optical properties, visibility and multiphase chemical reactions. In this study, ALWC is determined from aerosol hygroscopic growth factor (GF) and particle number size distribution (PNSD) measurements and is also simulated by ISORROPIA II, a thermodynamic equilibrium model, with measured aerosol chemical composition data taken at an urban site in Beijing from 8 November to 15 December 2017. Rich measurements made during the experiment concerning virtually all aerosol properties allow us not only to derive the ALWC but also to study the contributions by various species for which little has been done in this region. The simulated ALWC including the contribution of organics and the calculated ALWC are highly correlated (coefficient of determination R2=0.92). The ALWC contributed by organics (ALWC Org) accounts for 30%±22% of the total ALWC during the sampling period. These results suggest a significant contribution of organics to ALWC, which is rather different from previous studies that showed negligible contributions by organics. Our results also show that ALWC correlates well with the mass concentrations of sulfate, nitrate, and secondary organic aerosols (SOAs) (R2=0.66 , 0.56 and 0.60, respectively). We further noted that accumulation mode particles play a key role in determining ALWC, dominating among all the aerosol modes. ALWC is an exponential function of ambient relative humidity (RH), whose strong diurnal variation influence the diurnal variation of ALWC. However, there is a 3 h lag between the extremes of ALWC and RH values, due to the diurnal variations in PNSD and aerosol chemical composition. Finally, a case study reveals that ALWC Org plays an important role in the formation of secondary aerosols through multiphase reactions at the initial stage of a heavy-haze episode. [ABSTRACT FROM AUTHOR]

The effects of aerosols on visibility through scattering and absorption of light and on climate through altering cloud droplet concentration are closely associated with their hygroscopic properties. Here, based on field campaigns in winter and summer in Beijing, we compare the size-resolved hygroscopic parameter (κgf) of ambient fine particles derived by an HTDMA (hygroscopic tandem differential mobility analyzer) to that (denoted as κchem) calculated by an HR-ToF-AMS (high-resolution time-of-flight aerosol mass spectrometer) measurements using a simple rule with the hypothesis of uniform internal mixing of aerosol particles. We mainly focus on contrasting the disparity of κgf and κchem between summer and winter to reveal the impact of atmospheric processes/emission sources on aerosol hygroscopicity and to evaluate the uncertainty in estimating particle hygroscopicity with the hypothesis. We show that, in summer, the κchem for 110, 150, and 200 nm particles was on average ∼10 %–12 % lower than κgf , with the greatest difference between the values observed around noontime when aerosols experience rapid photochemical aging. In winter, no apparent disparity between κchem and κgf is observed for those >100 nm particles around noontime, but the κchem is much higher than κgf in the late afternoon when ambient aerosols are greatly influenced by local traffic and cooking sources. By comparing with the observation from the other two sites (Xingtai, Hebei and Xinzhou, Shanxi) of north China, we verify that atmospheric photochemical aging of aerosols enhances their hygroscopicity and leads to 10 %–20 % underestimation in κchem if using the uniform internal mixing assumption. The effect is found more significant for these >100 nm particles observed in remote or clean regions. The lower κchem likely resulted from multiple impacts of inappropriate application of the density and hygroscopic parameter of organic aerosols in the calculation, as well as influences from chemical interaction between organic and inorganic compounds on the overall hygroscopicity of mixed particles. We also find that local/regional primary emissions, which result in a large number of externally mixed BC (black carbon) and POA (primary organic aerosol) in urban Beijing during traffic rush hour time, cause a 20 %–40 % overestimation of the hygroscopic parameter. This is largely due to an inappropriate use of density of the BC particles that is closely associated with its morphology or the degree of its aging. The results show that the calculation can be improved by applying an effective density of fresh BC (0.25–0.45 g cm -3) in the mixing rule assumption. Our study suggests that it is critical to measure the effective density and morphology of ambient BC, in particular in those regions with influences of rapid secondary conversion/aging processes and local sources, so as to accurately parameterize the effect of BC aging on particle hygroscopicity. [ABSTRACT FROM AUTHOR]

Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (NCCN). In this study, we predict NCCN under five assumed schemes of aerosol chemical composition and mixing state based on field measurements in Beijing during the winter of 2016. Our results show that the best closure is achieved with the assumption of size dependent chemical composition for which sulfate, nitrate, secondary organic aerosols, and aged black carbon are internally mixed with each other but externally mixed with primary organic aerosol and fresh black carbon (external–internal size-resolved, abbreviated as EI–SR scheme). The resulting ratios of predicted-to-measured NCCN (RCCN_p/m) were 0.90 – 0.98 under both clean and polluted conditions. Assumption of an internal mixture and bulk chemical composition (INT–BK scheme) shows good closure with RCCN_p∕m of 1.0 –1.16 under clean conditions, implying that it is adequate for CCN prediction in continental clean regions. On polluted days, assuming the aerosol is internally mixed and has a chemical composition that is size dependent (INT–SR scheme) achieves better closure than the INT–BK scheme due to the heterogeneity and variation in particle composition at different sizes. The improved closure achieved using the EI–SR and INT–SR assumptions highlight the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. NCCN is significantly underestimated (with RCCN_p∕m of 0.66 – 0.75) when using the schemes of external mixtures with bulk (EXT–BK scheme) or size-resolved composition (EXT–SR scheme), implying that primary particles experience rapid aging and physical mixing processes in urban Beijing. However, our results show that the aerosol mixing state plays a minor role in CCN prediction when the κorg exceeds 0.1. [ABSTRACT FROM AUTHOR]

Aerosol growth potentials were investigated based on measurements of aerosol properties from three field campaigns carried out at sites in urban Beijing (BJ) and suburban Xingtai (XT) located in the North China Plain (NCP). BJ and XT were located in a northern megalopolis area and a central-southern industrial area, respectively, in the NCP. Results suggest new particle formation (NPF) events occurred more frequently, and the particle growth potential was greater in the central-southern NCP region than in the northern NCP region in summer. It is found that differences in primary emissions and meteorological conditions can cause regional and seasonal variations in aerosol growth potential in the NCP. Photochemical reactions were more important for particle growth in summer, while nocturnal aqueous chemical reactions were more important in winter. The large nocturnal particle growth rate (7.5 nm h−1) was the reason inducing the severe aerosol pollution in winter BJ. Further analyses of submicron aerosol chemical species indicate more sulfate in submicron aerosols at XT, suggesting that the growth of new particles in the central-southern NCP in summer may be mainly dominated by the secondary formation of inorganics. Diurnal variations in aerosol chemical species during the three field campaigns suggest that the downward vertical mixing of nitrate over the nocturnal boundary layer played an important role in aerosol growth in the morning in summer. Moreover, the enhanced anthropogenic emissions during the late-day rush hours can cause clear increases in nitrate and organics. Our results highlight the distinct aerosol growth potentials in the northern and central-southern areas of NCP, implying that different emission control measures are needed in two regions to further improve air quality in the future. ● Diverse aerosol growth potentials were found in different regions of the North China Plain. ● Different particle growth mechanisms in winter and summer were reported. ● Distinct emission control measures are needed in different regions of the North China Plain to further improve air quality in the future. [ABSTRACT FROM AUTHOR]

This study investigates aerosol hygroscopicity, mixing state, and cloud condensation nucleation as part of the Atmosphere–Aerosol–Boundary Layer–Cloud Interaction Joint Experiment performed in the summer of 2016 at Xingtai (XT), a suburban site located in the center of the North China Plain (NCP). In general, the probability density function (PDF) of the hygroscopicity parameter (κ) for 40–200nm particles had a unimodal distribution, and mean κ-PDF patterns for different sizes were similar, suggesting that the particles were highly aged and internally mixed because of strong photochemical reactions. The κ calculated from the hygroscopic growth factor in the daytime and at night suggests that photochemical reactions largely enhanced the aerosol hygroscopicity. This effect became weaker as the particle size increased. In addition, the aerosol hygroscopicity was much larger at XT than at other sites in the NCP. This is because new particle formation takes place much more frequently in the central NCP, which is heavily polluted from industrial activities, than elsewhere in the region. The evolution of the planetary boundary layer played a dominant role in dictating aerosol mass concentration. Particle size was the most important factor influencing the ability of aerosols to activate, whereas the effect of chemical composition was secondary, especially when supersaturation was high. Using a fixed value of κ = 0.31 to calculate the cloud condensation nuclei number concentration in this region suffices. [ABSTRACT FROM AUTHOR]