Drivers of Droplet Formation in East Mediterranean Orographic Clouds

Abstract. The purpose of this study is to understand the drivers of cloud droplet formation in orographic clouds. We used a combination of modeling, in-situ and remote sensing measurements at the high-altitude Helmos Hellenic Atmospheric Aerosol and Climate Change station ((HAC)2), which is located at the top of Mt. Helmos (1314 metres above sea level), Greece during the Cloud-AerosoL InteractionS in the Helmos background TropOsphere (CALISTHO) campaign in Fall 2021 (https://calishto.panacea-ri.gr/) to examine the origins of the aerosols (i.e., local aerosol from the Planetary Boundary Layer (PBL), or long-range transported aerosol from the Free Tropospheric Layer (FTL) contributing to the Cloud Condensation Nuclei (CCN), their characteristics (hygroscopicity, size distribution and mixing state), as well as the vertical velocities distributions and resulting supersaturations. We found that the characteristics of the PBL aerosol were considerably different from FTL aerosol and use the aerosol particle number and equivalent mass concentration of the black carbon (eBC) in order to determine when the (HAC)2 was within the FTL or PBL based on timeseries of the height of the PBL. During the (HAC)2 cloud events we sample a mixture of interstitial aerosol and droplet residues, which we characterize using a new approach that utilizes the in-situ droplet measurements to determine time periods where the aerosol sample is purely interstitial. From the dataset we determine the properties (size distribution and hygroscopicity) of the pre-cloud, activated and interstitial aerosol. The hygroscopicity of activated aerosol is found to be higher than that of the interstitial or pre-cloud aerosol. A series of closure studies with the droplet parameterization shows that cloud droplet concentration (Nd) and supersaturation can be predicted to within 25 % of observations when the aerosol size distributions correspond to pre-cloud conditions. Analysis of the characteristic supersaturation of each aerosol population indicates that droplet formation in clouds is aerosol-limited when formed in FTL airmasses – hence droplet formation is driven by aerosol variations, while clouds formed in the PBL tend to be velocity limited and droplet variations are driven by fluctuations in vertical velocity. Given that the cloud dynamics do not vary significantly between airmasses, the variation in aerosol concentration and type is mostly responsible for these shifts in cloud microphysical state and sensitivity to aerosol. With these insights, remote sensing of cloud droplets in such clouds can be used to infer either CCN spectra (when in the FTL) or vertical velocity (when in the PBL). In conclusion, we show that a coordinated measurement of aerosol and cloud properties, together with the novel analysis approaches presented here allow for the determination of the drivers of droplet formation in orographic clouds and their sensitivity to aerosol and vertical velocity variations.