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The interaction between atmospheric aerosols and moisture is crucial for aerosol properties and their climate effects. In this study, thanks to the rich measurements of aerosol properties during the 2016 and 2018 ORACLES campaigns, we investigate the aerosol liquid water content (ALWC) over the south-eastern Atlantic Ocean during the biomass burning (BB) season, as well as the seldom-reported ALWC associated with organic aerosols (OA) (ALWCOA) (OA). ALWCOA is determined using the OA hygroscopicity parameter κ OA, derived from in-situ hygroscopicity measurements, particle number size distribution, and chemical composition. The ALWC can be determined either with the overall hygroscopic parameter κ f(RH) or from the sum of ALWCOA and the ALWC simulated from ISORROPIA-II, a thermodynamic equilibrium model for inorganic aerosol. The ALWC from both methods is highly correlated at all RHs with an R2 of 0.99. The ALWC increases with aerosol loading and ambient relative humidity (RH). Due to the lower RH and higher aerosol loading in the 2016 campaign, the ALWC for both campaigns are generally consistent. ALWCOA accounts for 38±16 % of the total ALWC during both campaigns. Notably, the contribution of ALWCOA is greater than commonly reported in the literature, highlighting the significance of OA in ALWC and therefore the aerosol direct radiative forcing in this climatically significant region. The strong correlation between κ OA and ALWCOA/ALWC, as indicated by an R2 value of 0.72, underscores the importance of a good estimation of κ OA in the ALWC estimation. Additionally, the significant difference between ALWCOA values calculated using real-time κ OA and those calculated with the campaign mean κ OA, highlights the limitation of using a constant κ OA value, a practice commonly adopted in climate models. [ABSTRACT FROM AUTHOR]

Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f (RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f (80 %) from ORACLES 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the South-East Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f (80 %) of 1.40±0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f (80 %) of 1.51±0.22, consistent with higher values of BB hygroscopicity found in the literature. The hygroscopicity parameter of OA (κOA) is retrieved from the Mie model with a mean value of 0.11±0.08, which is in the middle to upper range compared to literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced BBA hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulphate fraction, and greater κOA at lower altitudes. We propose a parameterization that quantifies f (RH) with chemical composition and κOA based on Mie simulation of internally mixed OA-(NH4)2SO4-BC mixture. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA-(NH4)2SO4-BC internal mixture with respect to the f (RH) prediction. The sensitivity of f (RH) to κOA indicates that applying a constant κOA is only suitable when the OA fraction is low and κOA shows limited variation. However, in situations deviating these two criteria, κOA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κOA variability is recommended. [ABSTRACT FROM AUTHOR]

Study on the upper ocean is of great significance to the global climate change and carbon cycle. Lidar can be used to effectively detect depth-resolved optical properties of the ocean. However, both theory and experiment of oceanic lidar are limited by complex multiple scattering. Several progresses by Zhejiang University will be illustrated in this paper: 1) a polarized lidar system was developed, and a Monte Carlo model and a radiative transfer model were established (Zhou, et al. remote sensing, 2019; Zhou, et al. Journal of remote sensing, 2019; Xu, et al. and Liu, et al. Journal of remote sensing, 2019); 2) Cross validations are demonstrated to verify the availability of the lidar system and models (Liu, et al. IEEE TGRS, 2019); 3) phase function effects on backscatter and attenuation are studied considering multiple scattering, respectively (Liu, et al. Optics Express, 2019). Oceanic lidar is proven to have great potential in marine studies.

From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are westward transported over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. A 17-month in-situ campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e., SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ~0.85 in October and the lowest ~0.78 in August. The absorption enhancement Eabs derived from the MACBC shows similar trends with SSA, with the average during the whole BB seasons at ~ 1.96 and ~ 2.07 in 2016 and 2017. As the Eabs is higher than the ~1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (BC/∆CO) is well correlated with SSA and MACBC, providing a simple way to estimate those aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/∆CO, and can better capture the growth of SSA as the decrease of BC/∆CO, especially when BC/∆CO is small. BC/∆CO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB burning, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of BB plume, we conclude that the increase in BC/∆CO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the changing of the burning conditions during these periods. The decrease in BC/∆CO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC. [ABSTRACT FROM AUTHOR]

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 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. These results suggest that atmospheric processing such as photolysis and cloud processing, rather than BB fuel type, has a major role in the elemental composition and morphology of aged BBA. [ABSTRACT FROM AUTHOR]

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 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). The July-August means are used to characterise aerosols, clouds and the radiation balance during the fire season. Results show around 68% of CCN at 0.2% supersaturation in the SEA domain can be attributed to biomass burning. The absorption effect of biomass burning aerosols is the most significant in affecting clouds and radiation. Near the continent it increases the maximum supersaturation diagnosed by the activation scheme, while further from the continent it reduces the altitude of the maximum supersaturation. As a result, the cloud droplet number concentration shows a similar pattern. The microphysical effect of biomass burning aerosols decreases the maximum supersaturation and increases the cloud droplets concentration over the ocean; however, 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 on clouds in this region. Among the effects of biomass burning aerosols on radiation balance, the semi-direct radiative effects (rapid adjustments induced by biomass burning aerosols radiative effects) have a dominant cooling impact over the SEA, which offset the warming direct radiative effect (radiative forcing from biomass burning aerosol"radiation interactions). However, the magnitude and the sign of the semi-direct effects are dependent on the relative location of biomass burning aerosols and clouds. The net biomass burning aerosols radiative effect shows a negative cooling effect in the SEA, indicating the significant role of biomass burning aerosols in affecting the regional radiation balance and climate. [ABSTRACT FROM AUTHOR]