Aerosols have significant and complex impacts on regional climate in East Asia. Cloud‐aerosol‐precipitation interactions (CAPI) remain most challenging in climate studies. The quantitative understanding of CAPI requires good knowledge of aerosols, ranging from their formation, composition, transport, and their radiative, hygroscopic, and microphysical properties. A comprehensive review is presented here centered on the CAPI based chiefly, but not limited to, publications in the special section named EAST‐AIRcpc concerning (1) observations of aerosol loading and properties, (2) relationships between aerosols and meteorological variables affecting CAPI, (3) mechanisms behind CAPI, and (4) quantification of CAPI and their impact on climate. Heavy aerosol loading in East Asia has significant radiative effects by reducing surface radiation, increasing the air temperature, and lowering the boundary layer height. A key factor is aerosol absorption, which is particularly strong in central China. This absorption can have a wide range of impacts such as creating an imbalance of aerosol radiative forcing at the top and bottom of the atmosphere, leading to inconsistent retrievals of cloud variables from space‐borne and ground‐based instruments. Aerosol radiative forcing can delay or suppress the initiation and development of convective clouds whose microphysics can be further altered by the microphysical effect of aerosols. For the same cloud thickness, the likelihood of precipitation is influenced by aerosols: suppressing light rain and enhancing heavy rain, delaying but intensifying thunderstorms, and reducing the onset of isolated showers in most parts of China. Rainfall has become more inhomogeneous and more extreme in the heavily polluted urban regions.
Four extreme haze episodes occurred in October 2014 in the North China Plain (NCP). To clarify the formation mechanism of hazes in autumn, strengthened observations were conducted in Beijing from 5 October to 2 November. The meteorological parameters, satellite data, chemical compositions and optical properties of aerosols were obtained. The hazes originated from the NCP, developing in the southwest and northeast directions, with the highest concentration of PM2.5 of 469 μg m−3 in Beijing. The NCP was dominated by a weak high pressure system during the haze episode, which resulted in low surface wind speed and relatively stagnant weather. Moreover, the wind slowed down around Beijing city. The secondary aerosols NO3− was always higher than that of SO42−, which indicated the motor vehicles played a more important part in the hazes in October 2014, even though the oxidation rate from SO2 to SO42− was faster than that of NOx to NO3−. Sudden increases of the concentrations of organic matter, Cl− and BC (black carbon) before each haze episode implied that regional transport of pollutants by biomass burning was important for haze formation during autumn. A satellite map of fire points and the backward trajectories of the air masses also indicated this pollution source. The distinct decrease in the PBL (planetary boundary layer) height during four haze episodes restrained the vertical dispersion of the air pollutants. Water vapor also played a vital role in the formation of hazes by accelerating the chemical transformation of secondary pollutants, leading to hygroscopic growth of aerosols and altering the thermal balance of the atmosphere.
Atmospheric measurements showed rapid sulfate formation during severe haze episodes in China, with fine particulate matter (PM) consisting of a multi-component mixture that is dominated by organic species. Several recent studies using the thermodynamic model estimated the particle acidity and sulfate production rate, by treating the PM exclusively as a mixture of inorganic salts dominated by ammonium sulfate and neglecting the effects of organic compounds. Noticeably, the estimated pH and sulfate formation rate during pollution periods in China were highly conflicting among the previous studies. Here we show that a particle mixture of inorganic salts adopted by the previous studies does not represent a suitable model system and that the acidity and sulfate formation cannot be reliably inferred without accounting for the effects of multi-aerosol compositions during severe haze events in China. Our laboratory experiments show that SO2 oxidation by NO2 with NH3 neutralization on fine aerosols is dependent on the particle hygroscopicity, phase-state, and acidity. Ammonium sulfate and oxalic acid seed particles exposed to vapors of SO2, NO2, and NH3 at high relative humidity (RH) exhibit distinct size growth and sulfate formation. Aqueous ammonium sulfate particles exhibit little sulfate production, in contrast to aqueous oxalic acid particles with significant sulfate production. Our field measurements demonstrate significant contribution of water-soluble organic matter to fine PM in China and indicate that the use of oxalic acid in laboratory experiments is representative of ambient organic dominant aerosols. While the particle acidity cannot be accurately determined from field measurements or calculated using the thermodynamic model, our results reveal that the pH value of ambient organics-dominated aerosols is sufficiently high to promote efficient SO2 oxidation by NO2 with NH3 neutralization under polluted conditions in China.
17 August 2018 in Atmospheric Chemistry and Physics
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 40–200 nm 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.
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.
4 November 2017 in Journal of Geophysical Research: Atmospheres