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The core diameter and shell thickness of black carbon (BC)-containing ambient aerosols directly determine their corresponding optical properties and aging processing, influencing significantly on the environment and climate change. The information of ambient particle core-shell structure is usually obtained using the single particle soot photometer (SP2) measurements. In this study, we found that the particle sizes measured by SP2 were limited within the core diameter larger than 84 nm and particle scattering diameter larger than 178 nm. There were about 34.9% of the ambient BC-containing aerosols that are mistaken for pure BC aerosols without coating. The lower limits of SP2 measurement lead to overestimation of the pure BC aerosol number concentrations and missing information of the shell thickness of BC-containing aerosol. Thus the statistical shell thickness of ambient BC-containing particles was underestimated and the aging process of ambient BC-containing aerosols derived from the SP2 measurements is misleading. [ABSTRACT FROM AUTHOR]

Abstract The light scattering enhancement factor f (RH), defined as the ratio of the light scattering coefficient (σ S P ) observed under an elevated relative humidity (RH) conditions to that under dry conditions, is a crucial parameter for estimating aerosol direct radiative effects and atmospheric visibility. In this paper, a new f (RH) parameterization scheme considering both the influence of aerosol chemical compositions and that of particle number size distribution (PNSD) is proposed based on in situ measurements in the North China Plain. The development of this parameterization scheme includes three steps. First, aerosol hygroscopicity parameter κ is parameterized with aerosol chemical compositions. Then, the ratio between f (RH) fitted parameter κ s c a (f (R H) = 1 + κ s c a R H 100 − R H ) and κ is introduced to correlate f (RH) with κ. The ratio, influenced mostly by PNSD, is described as a function of scattering Ångström exponent (SAE) because the SAE can represent the predominant size of aerosol particles to some extent. Finally, f (RH) cycle is parameterized with κ s c a . Validation results show that a good consistency between the parameterized and measured f (RH = 80%) is achieved and the correlation coefficient is 0.80. This parameterization scheme between aerosol chemistry and f (RH) can be used in chemical transport models for reducing uncertainties in estimations of direct aerosol radiative forcing and air quality assessments. Highlights • A relationship between the f (RH) fitted parameter (κ sca) and the aerosol hygroscopicity parameter (κ f(RH)) is found. • The ratio of κ sca and κ f(RH) increases linearly with the increase of the scattering Ångström exponent. • A new parameterization of f (RH) considering the aerosol chemical compositions is developed. [ABSTRACT FROM AUTHOR]

Due to the limited spatial coverage of surface PM 2.5 monitoring sites, satellite AOD (aerosol optical depth) products have been widely used to estimate surface PM 2.5 in different parts of the world. A major difficulty as well as source of uncertainty in converting AOD to PM 2.5 is the determination of aerosol vertical distribution, usually represented by the boundary layer height (BLH). In this study, we evaluate the performance of different approaches of estimating aerosol vertical distributions in the AOD-PM 2.5 conversion process, using long-term and multi-source data acquired at a super station, Yuen Long, Hong Kong. The monthly climatology of aerosol vertical distribution and BLH products derived from lidar, radiosonde, and MERRA reanalysis data are respectively applied for converting AOD to surface aerosol extinction coefficients. Seasonal empirical hygroscopic growth functions are constructed to convert aerosol extinction to dry PM 2.5 mass concentration. Results indicate that different vertical distribution estimation approaches can have highly varying effect on the converted PM 2.5 concentration. Using lidar-derived BLHs shows the best agreement, with a correlation coefficient of 0.73 and a relative bias of 30.6% between retrievals and observations. Since continuous lidar measurements are not available for most regions, the climatology pattern of aerosol structure and radiosonde-derived BLHs are found to be suitable alternatives with a correlation coefficient of ∼0.6, and considerably outperform the results using BLHs derived from reanalysis data. Elevated aerosol layers appear to be the major source of uncertainty and result in an overestimate of satellite results, especially during the spring and summer seasons. [ABSTRACT FROM AUTHOR]

Aerosol surface area concentration ( S A ) is crucial for studying atmospheric chemical reactions happened in aerosol water or on aerosol surface. However, there is no commercial instrument that can provide direct measurements of ambient S A . In this paper, we propose a method to calculate ambient S A based only on measurements of a three-wavelength humidified nephelometer system, which measures aerosol optical properties at three wavelengths under dry state and different relative humidity (RH) conditions. Two critical steps are required in this method: (1) Calculating surface area concentration of ambient aerosols in dry state, S A (dry) , using a trained random forest machine learning model based only on optical properties measured by the "dry" nephelometer. The proposed machine learning method is evaluated with particle number size distributions (PNSD) datasets from eight field campaigns conducted on the North China Plain during different seasons. The square of correlation coefficients between predicted and calculated S A (dry) for PNSD is about 0.99, the average ratio between predicted and calculated S A (dry) is 1.01 and 70% of data points has a relative difference less than 10%. (2) Calculating the surface area growth factor f S (RH) of ambient aerosol particles due to water uptake using the proposed f S (RH) parameterization scheme f S (RH) = (1 + κ S R H 100 − R H) 2 3 , and the hygroscopicity parameter κ S can be calculated using measured aerosol light scattering enhancement factor and Å ngstr o ¨ m exponent. The ambient S A values during two field campaigns which are conducted on the North China Plain (Wangdu campaign and Gucheng campaign, in summer and winter respectively) are calculated using the proposed method. The ambient S A ranges from 42 to 1871 μ m 2 / c m 3 with an average of 319 μ m 2 / c m 3 during Wangdu campaign, and ranges from 19 to 4156 μ m 2 / c m 3 with an average of 788 μ m 2 / c m 3 during Gucheng campaign. Drastic daily variations of ambient S A are observed during these two campaigns. The results demonstrate that aerosol hygroscopic growth impacts significantly on variations in ambient S A especially under high RH conditions. The f S (RH) ranges from near 1 to 4 with an average of 1.4 during Wangdu campaign, and ranges from near 1 to 2.7 with an average of 1.3 during Gucheng campaign. The results indicate that the larger RH, the more sensitive f S (RH) becomes to variations in κ S which highlights that real-time measurements of aerosol hygroscopicity are required for accurate calculations of ambient S A . The advantage of the proposed method is that the ambient S A can be obtained solely based on measurements of a three-wavelength humidified nephelometer system, facilitating real-time measurements of ambient S A and promoting studies in aerosol heterogeneous reactions. • Humidified nephelometer system performs great in predicting aerosol surface area. • Proposed method can be used in different regions. • Aerosol hygroscopic growth impacts significantly on aerosol surface area. [ABSTRACT FROM AUTHOR]