Aerosol-cloud-precipitation interactions are a leading source of uncertainty in estimating climate sensitivity. Remote marine boundary layers where accumulation mode (~100-400 nm diameter) aerosol concentrations are relatively low are very susceptible to aerosol changes. These regions also experience heightened Aitken mode aerosol (~10-100 nm) concentrations associated with ocean biology. Aitken aerosols may significantly influence cloud properties and evolution by replenishing cloud condensation nuclei and droplet number lost through precipitation (i.e., Aitken buffering). We use a large-eddy simulation with an Aitken-mode enabled microphysics scheme to examine the role of Aitken buffering in a mid-latitude decoupled boundary layer cloud regime observed on July 15, 2017 during the ACE-ENA flight campaign: cumulus rising into stratocumulus under elevated Aitken concentrations (~100-200 mg-1). In situ measurements are used to constrain and evaluate this case study. Our simulation accurately captures observed aerosol-cloud-precipitation interactions and reveals time-evolving processes driving regime development and evolution. Aitken activation into the accumulation mode occurs primarily in the cumulus layer, providing a reservoir for turbulence and convection to carry accumulation aerosols into the drizzling stratocumulus layer above. Thus, the cloud regime is buffered against precipitation removal, reducing cloud break-up and associated increases in heterogeneity. We examine cloud evolution sensitivity to initial aerosol conditions. With halved accumulation number, Aitken aerosols restore accumulation concentrations, maintain droplet number similar to original values, and prevent cloud break-up. Without Aitken aerosols, precipitation-driven cloud break-up occurs rapidly. In this regime, mesoscale and synoptic-scale uplift enhance cloud condensate and brightness, but Aitken buffering sustains brighter, more homogeneous clouds for longer.

Observed stratocumulus to cumulus transitions (SCT) and their sensitivity to aerosols are studied using a Large-Eddy Simulation (LES) model that simulates the aerosol lifecycle, including aerosol sources and sinks. To initialize, force, and evaluate the LES, we used a combination of reanalysis, satellite, and aircraft data from the 2015 Cloud System Evolution in the Trades field campaign over the Northeast Pacific. The simulations follow two Lagrangian trajectories from initially overcast stratocumulus to the tropical shallow cumulus region near Hawaii. The first trajectory is characterized by an initially clean, well-mixed stratocumulus-topped marine boundary layer (MBL), then continuous MBL deepening and precipitation onset followed by a clear SCT and a consistent reduction of aerosols that ultimately leads to an ultra-clean layer in the upper MBL. The second trajectory is characterized by an initially polluted and decoupled MBL, weak precipitation, and a late SCT. Overall, the LES simulates the observed general MBL features. Sensitivity studies with different aerosol initial and boundary conditions reveal aerosol-induced changes in the transition, and albedo changes are decomposed into the Twomey effect and adjustments of cloud liquid water path and cloud fraction. Impacts on precipitation play a key role in the sensitivity to aerosols: for the first case, runs with enhanced aerosols exhibit distinct changes in microphysics and macrophysics such as enhanced cloud droplet number concentration, reduced precipitation, and delayed SCT. Cloud adjustments are dominant in this case. For the second case, enhancing aerosols does not affect cloud macrophysical properties significantly, and the Twomey effect dominates.

A new Aitken mode aerosol scheme is developed for a large eddy simulation (LES) model in order to better investigate cloud-aerosol interactions in the marine boundary layer and to study the Aitken buffering hypothesis of McCoy et al. (2021). This scheme extends the single-mode two-moment prognostic aerosol scheme of Berner et al. (2013). Nine prognostic variables represent accumulation and Aitken log-normal aerosol modes in air and droplets as well as 3 gas species. Scavenging of interstitial aerosol by cloud and rain drops and coagulation of dry aerosol are treated using the scheme described in B13. The scheme includes a simple chemistry model with gas phase H2SO4, SO2, and DMS as prognostic variables to capture basic influences of sulfur chemistry on the model aerosols. Primary nucleation of H2SO4 aerosol particles from gas-phase H2SO4 is neglected. A deep, precipitating stratocumulus case (VOCALS RF06) is used to test the new scheme. The presence of the Aitken mode aerosol increases the cloud droplet concentration through activation of the larger Aitken particles and delays the creation of an ultraclean, strongly precipitating cumulus state. Scavenging of dry accumulation and Aitken particles by cloud and precipitation droplets accelerates the collapse. Increasing either the above-inversion Aitken concentration or the surface Aitken flux increases the Aitken population in the boundary layer and prevents the transition to an ultraclean state.