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The response in cloud water content to changes in cloud condensation nuclei remains one of the major uncertainties in determining how aerosols can perturb cloud properties. In this study, we used an ensemble of large eddy simulations of marine stratocumulus clouds to investigate the correlation between cloud liquid water path (LWP) and the amount of cloud condensation nuclei. We compare this correlation directly from the model to the correlation derived using equations which are used to retrieve liquid water path from satellite observations. Our comparison shows that spatial variability in cloud properties and instrumental noise in satellite retrievals of cloud optical depth and cloud effective radii results in bias in the satellite-derived liquid water path. In-depth investigation of high-resolution model data shows that in large part of a cloud, the assumption of adiabaticity does not hold, which results in a similar bias in the LWP–CDNC (cloud droplet number concentration) relationship as seen in satellite data. In addition, our analysis shows a significant positive bias of between 18 % and 40 % in satellite-derived cloud droplet number concentration. However, for the individual ensemble members, the correlation between the cloud condensation nuclei and the mean of the liquid water path was very similar between the methods. This suggests that if cloud cases are carefully chosen for similar meteorological conditions and it is ensured that cloud condensation nuclei concentrations are well-defined, changes in liquid water can be confidently determined using satellite data. [ABSTRACT FROM AUTHOR]

Surfactants have been a focus of investigation in atmospheric sciences for decades due to their ability to modify the water uptake and cloud formation potential of aerosols. Surfactants adsorb at the surface and can decrease the surface tension of aqueous solutions. In microscopic aqueous droplets with finite amounts of solute, surface adsorption may simultaneously deplete the droplet bulk of the surfactant. While this mechanism is now broadly accepted, the representation in atmospheric and cloud droplet models is still not well constrained. We compare the predictions of five bulk–surface partitioning models documented in the literature to represent aerosol surface activity in Köhler calculations of cloud droplet activation. The models are applied to common aerosol systems, consisting of strong atmospheric surfactants (sodium myristate or myristic acid) and sodium chloride in a wide range of relative mixing ratios. For the same particles, the partitioning models predict similar critical droplet properties at small surfactant mass fractions, but differences between the model predictions increase significantly with the surfactant mass fraction in the particles. Furthermore, significantly different surface tensions are predicted for growing droplets at given ambient conditions along the Köhler curves. The inter-model variation for these strong surfactant particles is different than previously observed for moderately surface active atmospheric aerosol components. Our results highlight the importance of establishing bulk–surface partitioning effects in Köhler calculations for a wide range of conditions and aerosol types relevant to the atmosphere. In particular, conclusions made for a single type of surface active aerosol and surface activity model may not be immediately generalized. [ABSTRACT FROM AUTHOR]

Surface active compounds (surfactants) found in atmospheric aerosols can decrease droplet surface tension as they adsorb to the droplet surfaces simultaneously depleting the droplet bulk. These processes may influence the activation properties of aerosols into cloud droplets and investigation of their role in cloud microphysics has been ongoing for decades. In this study, we have used six different approaches documented in the literature to represent surface activity in Köhler calculations predicting cloud droplet activation properties for particles consisting of one of three different moderately surface active organics mixed with ammonium sulphate in different ratios. We find that the different models predict comparable activation properties at small organic mass fractions in the dry particles for all three moderately surface active organics tested, even with large differences in the predicted degree of bulk-to-surface partitioning of the surface active component. However, differences between the models regarding both the predicted critical diameter and supersaturation for the same dry particle size increase with the organic fraction in the particles. Comparison with available experimental data shows that assuming complete bulk-to-surface partitioning of the organic component (total depletion of the bulk) along the full droplet growth curve does not adequately represent the activation properties of particles with high moderate surfactant mass fractions. Accounting for the surface tension depression mitigates some of the effect. Models that include the possibility for partial bulk-to-surface partitioning yield comparable results to the experimental data, even at high organic mass fractions in the particles. The study highlights the need for using thermodynamically consistent model frameworks to treat surface activity of atmospheric aerosols and for firm experimental validation of model predictions across a wide range of states relevant to the atmosphere. [ABSTRACT FROM AUTHOR]