On the drivers of droplet variability in alpine mixed-phase clouds

Droplet formation provides a direct microphysical link between aerosols and clouds (liquid or mixed-phase), and its adequate description poses a major challenge for any atmospheric model. Observations are critical for evaluating and constraining the process. To this end, aerosol size distributions, cloud condensation nuclei (CCN), hygroscopicity, and lidar-derived vertical velocities were observed in alpine mixed-phase clouds during the Role of Aerosols and Clouds Enhanced by Topography on Snow (RACLETS) field campaign in the Davos, Switzerland, region during February and March 2019. Data from the mountain-top site of Weissfluhjoch (WFJ) and the valley site of Davos Wolfgang are studied. These observations are coupled with a state-of-the-art droplet activation parameterization to investigate the aerosol-cloud droplet link in mixed-phase clouds. The mean CCN-derived hygroscopicity parameter, kappa, at WFJ ranges between 0.2-0.3, consistent with expectations for continental aerosols. kappa tends to decrease with size, possibly from an enrichment in organic material associated with the vertical transport of fresh ultrafine particle emissions (likely from biomass burning) from the valley floor in Davos. The parameterization provides a droplet number that agrees with observations to within similar to 25 %. We also find that the susceptibility of droplet formation to aerosol concentration and vertical velocity variations can be appropriately described as a function of the standard deviation of the distribution of updraft velocities, sigma(w), as the droplet number never exceeds a characteristic limit, termed the "limiting droplet number", of similar to 150-550 cm(-3), which depends solely on sigma(w). We also show that high aerosol levels in the valley, most likely from anthropogenic activities, increase the cloud droplet number, reduce cloud supersaturation (< 0.1 %), and shift the clouds to a state that is less susceptible to changes in aerosol concentrations and very sensitive to vertical velocity variations. The transition from an aerosol to velocity-limited regime depends on the ratio of cloud droplet number to the limiting droplet number, as droplet formation becomes velocity limited when this ratio exceeds 0.65. Under such conditions, droplet size tends to be minimal, reducing the likelihood that large drops are present that would otherwise promote glaciation through rime splintering and droplet shattering. Identifying regimes where droplet number variability is dominated by dynamical - rather than aerosol - changes is key for interpreting and constraining when and which types of aerosol effects on clouds are active.