Aerosol - stratocumulus interactions: towards a better process understanding using closures between observations and large eddy simulations

We carried out a closure study of aerosol-cloud interactions during stratocumulus formation using a large eddy simulation model UCLALES-SALSA and observations from the 2020 cloud sampling campaign at the Puijo SMEAR IV station in Kuopio, Finland. The unique observational setup combining in situ and cloud remote sensing measurements allowed a closer look into the aerosol size-composition dependence of droplet activation and droplet growth in turbulent boundary layer driven by surface forcing and radiative cooling. UCLALES-SALSA uses spectral bin microphysics for aerosols and hydrometeors and incorporates a full description of their interactions into the turbulent-convective radiation-dynamical model of stratocumulus. Based on our results, the model successfully described the probability distribution of updraft velocities and consequently the size dependency of aerosol activation into cloud droplets, and further recreated the size distributions for both interstitial aerosol and cloud droplets. This is the first time such a detailed closure is achieved not only accounting for activation of cloud droplets in different updrafts, but also accounting for processes evaporating droplets and drizzle production through coagulation-coalescence. We studied two cases of cloud formation, one diurnal (24 September 2020) and one nocturnal (31 October 2020), with high and low aerosol loadings, respectively. Aerosol number concentrations differ more than 1 order of magnitude between cases and therefore, lead to cloud droplet number concentration (CDNC) values which range from less than 100cm-3 up to 1000cm-3. Different aerosol loadings affected supersaturation at the cloud base, and thus the size of aerosol particles activating to cloud droplets. Due to higher CDNC, the mean size of cloud droplets in the diurnal-high aerosol case was lower. Thus, droplet evaporation in downdrafts affected more the observed CDNC at Puijo altitude compared to the low aerosol case. In addition, in the low aerosol case, the presence of large aerosol particles in the accumulation mode played a significant role in the droplet spectrum evolution as it promoted the drizzle formation through collision and coalescence processes. Also, during the event, the formation of ice particles was observed due to subzero temperature at the cloud top. Although the modeled number concentration of ice hydrometeors was too low to be directly measured, the retrieval of hydrometeor sedimentation velocities with cloud radar allowed us to assess the realism of modeled ice particles. The studied cases are presented in detail and can be further used by the cloud modellers to test and validate their models in a well-characterized modelling setup. We also provide recommendations on how increasing amount of information on aerosol properties could improve the understanding of processes affecting cloud droplet number and liquid water content in stratiform clouds.