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.

Here we present a multi-season study of ice nucleating particles (INPs) active via the immersion freezing mechanism, which took place in north central Argentina, a worldwide hotspot for mesoscale convective storms. INPs were measured untreated, after heating to 95 °C, and after hydrogen peroxide digestion. No seasonal cycle of INP concentrations was observed. Biological INPs (denatured by heat) dominated the population active at -5 to -20 °C, while non-heat-labile organic INPs (decomposed by peroxide) dominated at lower temperatures, from -20 to -28 °C. Inorganic INPs (remaining after peroxide digestion), were minor contributors to the overall INP activity. Biological INP concentration active around -12 °C peaked during rain events and under high relative humidity, reflecting emission mechanisms independent of the background aerosol concentration. The ratio of non-heat-labile organic and inorganic INPs was generally constant, suggesting they originated from the same source, presumably from regional arable topsoil based on air mass histories. Single particle mass spectrometry showed that soil particles aerosolized from a regionally-common agricultural topsoil contained known mineral INP sources (K-feldspar and illite) as well as a significant organic component. The INP activity observed in this study correlates well with agricultural soil INP activities from this and other regions of the world, suggesting that the observed INP spectra might be typical of many arable landscapes. These results demonstrate the strong influence of regional continental landscapes, emitting INPs of types that are not yet well represented in global models.

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.

Climate models exhibit major radiative biases over the Southern Ocean owing to a poor representation of mixed-phase clouds. This study uses the remote-sensing dataset from the Measurements of Aerosols, Radiation and Clouds over the Southern Ocean (MARCUS) campaign to assess the ability of the Weather Research and Forecasting (WRF) model to reproduce frontal clouds off Antarctica. It focuses on the modeling of thin mid-level supercooled liquid water layers which precipitate ice. The standard version of WRF produces almost fully glaciated clouds and cannot reproduce cloud top turbulence. Our work demonstrates the importance of adapting the ice nucleation parameterization to the pristine austral atmosphere to reproduce the supercooled liquid layers. Once simulated, droplets significantly impact the cloud radiative effect by increasing downwelling longwave fluxes and decreasing downwelling shortwave fluxes at the surface. The net radiative effect is a warming of snow and ice covered surfaces and a cooling of the ocean. Despite improvements in our simulations, the local circulation related to cloud-top radiative cooling is not properly reproduced, advocating for the need to develop a parameterization for top-down convection to capture the turbulence-microphysics interplay at cloud top.

This study focuses on methods to estimate dry marine aerosol surface area (SA) from bulk optical measurements. Aerosol SA is used in many models’ ice nucleating particle (INP) parameterizations, as well as influencing particle light scattering, hygroscopic growth, and reactivity, but direct observations are scarce in the Southern Ocean (SO). Two campaigns jointly conducted in austral summer 2018 provided co-located measurements of aerosol surface area from particle size distributions and lidar to evaluate SA estimation methods in this region. Mie theory calculations based on measured size distributions were used to test a proposed approximation for dry aerosol SA, which relies on estimating effective scattering efficiency (Q) as a function of Ångström exponent (å). For distributions with dry å<1, Q=2 was found to be a good approximation within ±50%, but for distributions with dry å>1, an assumption of Q=3 as in some prior studies underestimates dry aerosol surface area by a factor of 2 or more. We propose a new relationship between dry å and Q, which can be used for -0.2