In January 2013, February 2014, December 2015 and December 2016 to 10 January 2017, 12 persistent heavy aerosol pollution episodes (HPEs) occurred in Beijing, which received special attention from the public. During the HPEs, the precise cause of PM_2.5 explosive growth (mass concentration at least doubled in several hours to 10 h) is uncertain. Here, we analyzed and estimated relative contributions of boundary-layer meteorological factors to such growth, using ground and vertical meteorological data. Beijing HPEs are generally characterized by the transport stage (TS), whose aerosol pollution formation is primarily caused by pollutants transported from the south of Beijing, and the cumulative stage (CS), in which the cumulative explosive growth of PM_2.5 mass is dominated by stable atmospheric stratification characteristics of southerly slight or calm winds, near-ground anomalous inversion, and moisture accumulation. During the CSs, observed southerly weak winds facilitate local pollutant accumulation by minimizing horizontal pollutant diffusion. Established by TSs, elevated PM_2.5 levels scatter more solar radiation back to space to reduce near-ground temperature, which very likely causes anomalous inversion. This surface cooling by PM_2.5 decreases near-ground saturation vapor pressure and increases relative humidity significantly; the inversion subsequently reduces vertical turbulent diffusion and boundary-layer height to trap pollutants and accumulate water vapor. Appreciable near-ground moisture accumulation (relative humidity > 80 %) would further enhance aerosol hygroscopic growth and accelerate liquid-phase and heterogeneous reactions, in which incompletely quantified chemical mechanisms need more investigation. The positive meteorological feedback noted on PM_2.5 mass explains over 70 % of cumulative explosive growth.

The representations of clouds, aerosols, and cloud–aerosol–radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct past climate and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing an optimum region for studying the full range of aerosol–radiation and aerosol–cloud interactions and their perturbations of the Earth's radiation budget. While satellite measurements have provided some useful insights into aerosol–radiation and aerosol–cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process-level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of five principal UK universities with project partners from the UK Met Office and European- and USA-based universities and research centres involved in the complementary ORACLES, LASIC, and AEROCLO-sA projects. The aims of CLARIFY-2017 were fourfold: (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct, and indirect radiative effect of absorbing biomass burning aerosols; (2) to improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) to challenge, validate, and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) to improve the impacts of aerosols in weather and climate numerical models. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarizes the flight objectives and flight patterns, and highlights some key results from our initial analyses.

Scattering of solar radiation by aerosol particles is highly dependent on relative humidity (RH) as hygroscopic particles take up water with increasing RH. To achieve a better understanding of the effect of aerosol hygroscopic growth on light scattering properties and radiative forcing, the aerosol scattering coefficients at RH in the range of 40 to ~ 90 % were measured using a humidified nephelometer system in the Yangtze River Delta of China in March 2013. In addition, the aerosol size distribution and chemical composition were measured. During the observation period, the mean and standard deviation (SD) of enhancement factors at RH = 85 % for the scattering coefficient (f(85 %)), backscattering coefficient (f_b(85 %)), and hemispheric backscatter fraction (f_β(85 %)) were 1.58 ± 0.12, 1.25 ± 0.07, and 0.79 ± 0.04, respectively, i.e., aerosol scattering coefficient and backscattering coefficient increased by 58 and 25 % as the RH increased from 40 to 85 %. Concurrently, the aerosol hemispheric backscatter fraction decreased by 21 %. The relative amount of organic matter (OM) or inorganics in PM₁ was found to be a main factor determining the magnitude of f(RH). The highest values of f(RH) corresponded to the aerosols with a small fraction of OM, and vice versa. The relative amount of NO₃⁻ in fine particles was strongly correlated with f(85 %), which suggests that NO₃⁻ played a vital role in aerosol hygroscopic growth during this study. The mass fraction of nitrate also had a close relationship to the curvature of the humidograms; higher mass fractions of nitrate were associated with humidograms that had the least curvature. Aerosol hygroscopic growth caused a 47 % increase in the calculated aerosol direct radiative forcing at 85 % RH, compared to the forcing at 40 % RH.

Southern Africa produces a third of global biomass burning emissions, which have a long atmospheric lifetime and influence regional radiation balance and climate. Here, we use airmass trajectories to link different aircraft observations to investigate the evolution of biomass-burning aerosols during their westward transport from Southern Africa over the south-eastern Atlantic, where a semi-permanent stratocumulus cloud deck is located. Our results show secondary organic aerosol formation during the initial 3 days of transport, followed by decreases in organic aerosol via photolysis before reaching equilibrium. Aerosol absorption wavelength dependency decreases with ageing, due to an increase in particle size and photochemical bleaching of brown carbon. Cloud processing, including aqueous-phase reaction and scavenging, contributes to the oxidation of organic aerosols, while it strongly reduces large diameter particles and single-scattering albedo of biomass burning aerosols. Together, these processes resulted in a marine boundary layer with fewer yet more oxidized and absorbing aerosols.

This study characterizes single-particle aerosol composition from filters collected during the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) and CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) campaigns. In particular the study describes aged biomass burning aerosol (BBA), its interaction with the marine boundary layer and the influence of biomass burning (BB) air on marine aerosol. The study finds evidence of BBA influenced by marine boundary layer processing as well as sea salt influenced by BB air. Secondary chloride aerosols were observed in clean marine air as well as in BB-influenced air in the free troposphere. Higher-volatility organic aerosol appears to be associated with increased age of biomass burning plumes, and photolysis or oxidation may be a mechanism for the apparent increased volatility. Aqueous processing and interaction with the marine boundary layer air may be a mechanism for the presence of sodium on many aged potassium salts. By number, biomass burning potassium salts and modified sea salts are the most observed particles on filter samples. The most commonly observed BC coatings are inorganic salts. These results suggest that atmospheric processes such as photolysis, oxidation and cloud processing are key drivers in the elemental composition and morphology of aged BBA. Fresh BBA inorganic salt content, as it has an important role in the particles' ability to uptake water, may be a key driver in how aqueous processing and atmospheric aging proceed.

The south-eastern Atlantic Ocean (SEA) is semi-permanently covered by one of the most extensive stratocumulus cloud decks on the planet and experiences about one-third of the global biomass burning emissions from the southern Africa savannah region during the fire season. To get a better understanding of the impact of these biomass burning aerosols on clouds and the radiation balance over the SEA, the latest generation of the UK Earth System Model (UKESM1) is employed. Measurements from the CLARIFY and ORACLES flight campaigns are used to evaluate the model, demonstrating that the model has good skill in reproducing the biomass burning plume. To investigate the underlying mechanisms in detail, the effects of biomass burning aerosols on the clouds are decomposed into radiative effects (via absorption and scattering) and microphysical effects (via perturbation of cloud condensation nuclei – CCN – and cloud microphysical processes). July–August means are used to characterize aerosols, clouds, and the radiation balance during the fire season. Results show that around 65 % of CCN at 0.2 % supersaturation in the SEA can be attributed to biomass burning. The absorption effect of biomass burning aerosols is the most significant on clouds and radiation. Near the continent, it increases the supersaturation diagnosed by the activation scheme, while further from the continent it reduces the altitude of the supersaturation. As a result, the cloud droplet number concentration responds with a similar pattern to the absorption effect of biomass burning aerosols. The microphysical effect, however, decreases the supersaturation and increases the cloud droplet concentration over the ocean, although this change is relatively small. The liquid water path is also significantly increased over the SEA (mainly caused by the absorption effect of biomass burning aerosols) when biomass burning aerosols are above the stratocumulus cloud deck. The microphysical pathways lead to a slight increase in the liquid water path over the ocean. These changes in cloud properties indicate the significant role of biomass burning aerosols for clouds in this region. Among the effects of biomass burning aerosols on the radiation balance, the semi-direct radiative effects (rapid adjustments induced by the radiative effects of biomass burning aerosols) have a dominant cooling impact over the SEA, which offset the warming direct radiative effect (radiative forcing from biomass burning aerosol–radiation interactions) and lead to an overall net cooling radiative effect in the SEA. However, the magnitude and the sign of the semi-direct effects are sensitive to the relative location of biomass burning aerosols and clouds, reflecting the critical task of the accurate modelling of the biomass burning plume and clouds in this region.