Future precipitation changes are controlled by the atmospheric energy budget, with temperature, water vapor, and absorbing aerosols playing dominant roles in driving radiative changes. Atmospheric energy budgets are calculated for different Shared Socioeconomic Pathways (SSPs) using ScenarioMIP projections from phase 6 of the Climate Model Intercomparison Project and are used to quantify the influence of 21st century aerosol cleanup on precipitation. Absorbing aerosol influences on shortwave absorption are isolated from the effects of water vapor. Apparent hydrologic sensitivity is ~40% higher for the “Middle of the Road” (SSP2-4.5) scenario with aerosol cleanup than for the “Regional Rivalry” (SSP3-7.0) scenario that maintains aerosol. Regionally, cleanup-induced changes in the atmospheric energy budget are of a similar magnitude to the precipitation increases themselves and are larger than the influence of changes in atmospheric circulation. Policy choices about future absorbing aerosol emissions will therefore have major impacts on global and regional precipitation changes.

Controls on pristine aerosol over the Southern Ocean (SO) are critical for constraining the strength of global aerosol indirect forcing. Observations of summertime SO clouds and aerosols in synoptically varied conditions during the 2018 SOCRATES aircraft campaign reveal novel mechanisms influencing pristine aerosol-cloud interactions. The SO free troposphere (3-6 km) is characterized by widespread, frequent new particle formation events contributing to much larger concentrations (≥ 1000 mg-1) of condensation nuclei (diameters > 0.01 μm) than in typical sub-tropical regions. Synoptic-scale uplift in warm conveyor belts and sub-polar vortices lifts marine biogenic sulfur-containing gases to free-tropospheric environments favorable for generating Aitken-mode aerosol particles (0.01-0.1 μm). Free-tropospheric Aitken particles subside into the boundary layer, where they grow in size to dominate the sulfur-based cloud condensation nuclei (CCN) driving SO cloud droplet number concentrations (Nd ~ 60-100 cm-3). Evidence is presented for a hypothesized Aitken-buffering mechanism which maintains persistently high summertime SO Nd against precipitation removal through CCN replenishment from activation and growth of boundary layer Aitken particles. Nudged hindcasts from the Community Atmosphere Model (CAM6) are found to underpredict Aitken and accumulation mode aerosols and Nd, impacting summertime cloud brightness and aerosol-cloud interactions and indicating incomplete representations of aerosol mechanisms associated with ocean biology.

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.

A supervised neural network algorithm is used to categorize near-global satellite retrievals into three mesoscale cellular convective (MCC) cloud morphology patterns. At constant cloud amount, morphology patterns differ in brightness associated with the amount of optically-thin cloud features. Environmentally-driven transitions from closed MCC to other morphology patterns, typically accompanied by more optically-thin cloud features, are used as a framework to quantify the morphology contribution to the optical depth component of the shortwave cloud feedback. A marine heat wave is used as an out-of-sample test of closed MCC occurrence predictions. Morphology shifts in optical depth between 65°S - 65°N under projected environmental changes (i.e., from an abrupt quadrupling of CO2) assuming constant cloud cover contributes between 0.04-0.07 W/m2/K (aggregate of 0.06) to the global mean cloud feedback.

Cloud droplet number concentration (Nd) is a key microphysical property that is largely controlled by the balance between sources and sinks of aerosols that serve as cloud condensation nuclei (CCN). Despite being a key sink of CCN, the impact of coalescence scavenging on Southern Ocean (SO) cloud is poorly known. We apply a simple source-and-sink budget model based on parameterizations to austral summer aircraft observations to test model behavior and examine the relative influence of processes that determine Nd in SO stratocumulus clouds. The model predicts Nd with little bias and a correlation coefficient of ~0.7 compared with observations. Coalescence scavenging is found to be an important sink of CCN in both liquid and mixed-phase precipitating stratocumulus and reduces the predicted Nd by as much as 90% depending on the precipitation rate. The free tropospheric aerosol source controls Nd more strongly than the surface aerosol source during austral summer.