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The scattering of light by aerosol particles dictates atmospheric visibility, which is a straightforward indicator of air quality. It is affected by numerous factors, such as particle number size distribution, particle mass concentration (PM2.5), ambient relative humidity (RH), and chemical composition. The latter two factors jointly influence the aerosol liquid water content (ALWC). Here, the particle backscattering coefficient (βp) under ambient RH conditions is investigated to differentiate and quantify the contributions of aerosol properties and meteorology using comprehensive observational datasets acquired at three megacities in China, that is, Beijing (BJ), Nanjing (NJ), and Guangzhou (GZ). Overall, the temporal variations in βp under ambient RH conditions are consistent with those in ALWC at the three sites. The PM2.5 in BJ is systematically higher than in NJ and GZ, while ambient RH and aerosol hygroscopicity in NJ are much higher than in BJ and GZ. Notable differences in the variations of βp with related factors at the three sites are demonstrated. βp is more sensitive to particle hygroscopicity and mass in NJ and ambient RH in BJ. The relative contributions of these factors to βp at the three sites under different pollution conditions are differentiated and quantified. The factor with the largest impact on the variability in βp shifts from particle mass to ambient RH as air quality deteriorated to heavy pollution in BJ. The opposite is true in NJ. In GZ, the contributions of these factors to changes in βp under different pollution conditions are similar, both dominated by PM2.5. Plain Language Summary: Scattering of light by aerosol is a straightforward measure of air quality because of its close link to visibility. It is dictated primarily by aerosol mass loading, size distribution, chemical composition, and humidity. We used comprehensive observational datasets acquired at three sites in China to differentiate and quantify the contributions to the scattering of light by aerosol loading measured by aerosol particulate mass and aerosol properties, as well as humidity. The findings differ among the three cities due to differences in aerosol properties and meteorology. Scattering of light by aerosol is more sensitive to particle hygroscopicity and mass concentration in Nanjing and more sensitive to ambient humidity in Beijing. Local emission control measures can effectively reduce aerosol mass concentrations in Nanjing and Guangzhou. Weather conditions are more influential in Beijing due to the dominant influence of humidity. Key Points: This study differentially quantifies the impacts of aerosol loading and properties and meteorology on scattering at three sites in ChinaScattering of light by aerosol is most sensitive to particle hygroscopicity and mass in Nanjing and humidity in BeijingHumidity substantially affects scattering during heavy haze in Beijing, whereas particle mass is more impactful in Nanjing and Guangzhou [ABSTRACT FROM AUTHOR]

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]