Supercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below -20 °C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model inferences that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. An updated parameterization for marine INPs is proposed, which reduces bias relative to existing methods by including wind speed as an additional variable. Direct and indirect inference of marine INP size suggests MBL INPs, at least those in the sub-2.5 μm range, are dominated by particles with diameters smaller than 500 nm.

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.

Modeling the shortwave radiation balance over the Southern Ocean region remains a challenge for Earth system models. To investigate whether this is related to the representation of aerosol-cloud interactions, we compared measurements of the total number concentration of sea spray generated particles within the Southern Ocean region to model predictions thereof. Measurements were conducted from a container laboratory aboard the R/V Tangaroa throughout an austral summer voyage to the Ross Sea. We used source-receptor modeling to calculate the sensitivity of our measurements to upwind surface fluxes. From this approach, we could constrain empirical parameterizations of sea spray surface flux based on surface wind speed and sea surface temperature. A newly tuned parameterization for the flux of sea spray particles based on the near-surface wind speed is presented. Comparisons to existing model parameterizations revealed that present model parameterizations led to over-estimations of sea spray concentrations. In contrast to previous studies, we found that including sea surface temperature as an explanatory variable did not substantially improve model-measurement agreement. To test whether or not the parameterization may be applicable globally, we conducted a similar regression analysis using a database of in situ whitecap measurements. We found that the key fitting parameter within this regression agreed well the parameterization of sea spray flux. Finally, we compared calculations from the best model of surface flux to boundary layer measurements collected onboard an aircraft throughout the Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES), finding good agreement overall.

Small cumulus clouds over the western United States were measured via airborne instruments during the wildfire season in summer of 2018. Statistics of the sampled clouds are presented and compared to smoke aerosol properties. Cloud droplet concentrations were enhanced in regions impacted by biomass burning smoke, at times exceeding 3,000 cm-3. Images and elemental composition of individual smoke particles and cloud droplet residuals are presented and show that most are dominantly organic, internally mixed with some inorganic elements. Despite their high organic content and relatively low hygroscopicity, on average about half of smoke aerosol particles >80 nm diameter formed cloud droplets. This reduced cloud droplet size in small, smoke-impacted clouds. A number of complex and competing climatic impacts may result from wide-spread reductions in cloud droplet size due to wildfires prevalent across the region during summer months.