Sensitivity of warm clouds to large particles in measured marine aerosol size distributions – a theoretical study

Abstract. Aerosol size distribution has major effects on warm cloud processes. Here, we use newly acquired marine aerosol size distributions (MSDs), measured in situ over the open ocean during the Tara Pacific expedition (2016–2018), to examine how the total aerosol concentration (Ntot) and the shape of the MSDs change warm clouds' properties. For this, we used a toy model with detailed bin microphysics initialized using three different atmospheric profiles, supporting the formation of shallow to intermediate and deeper warm clouds. The changes in the MSDs affected the clouds' total mass and surface precipitation. In general, the clouds showed higher sensitivity to changes in Ntot than to changes in the MSD's shape, except for the case where the MSD contained giant and ultragiant cloud condensation nuclei (GCCN, UGCCN). For increased Ntot (for the deep and intermediate profiles), most of the MSDs drove an expected non-monotonic trend of mass and precipitation (the shallow clouds showed only the decreasing part of the curves with mass and precipitation monotonically decreasing). The addition of GCCN and UGCCN drastically changed the non-monotonic trend, such that surface rain saturated and the mass monotonically increased with Ntot. GCCN and UGCCN changed the interplay between the microphysical processes by triggering an early initiation of collision–coalescence. The early fallout of drizzle in those cases enhanced the evaporation below the cloud base. Testing the sensitivity of rain yield to GCCN and UGCCN revealed an enhancement of surface rain upon the addition of larger particles to the MSD, up to a certain particle size, when the addition of larger particles resulted in rain suppression. This finding suggests a physical lower bound can be defined for the size ranges of GCCN and UGCCN.