A likely important feature of the poorly understood aerosol‐cloud interactions over the Southern Ocean (SO) is the dominant role of sea spray aerosol, versus terrestrial aerosol. Ice nucleating particles (INPs), or particles required for heterogeneous ice nucleation, present over the SO have not been studied in several decades. In this study, boundary layer aerosol properties and immersion freezing INP number concentrations (nINPs) were measured during a ship campaign that occurred south of Australia (down to 53°S) in March–April 2016. Ocean surface chlorophyll a concentrations ranged from 0.11 to 1.77 mg/m3, and nINPs were a factor of 100 lower than historical surveys, ranging from 0.38 to 4.6 m−3 at −20 °C. The INP population included organic heat‐stable material, with contributions from heat‐labile material. Lower INP source potentials of SO seawater samples compared to Arctic seawater were consistent with lower ice nucleating site densities in this study compared to north Atlantic air masses.

Abstract. Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north–south transects between Hobart, Tasmania, and 62∘ S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5 d HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO in the region south of Australia. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5 d of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A coarse-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution, which accounted for <20 % of CCN (at 0.3 % supersaturation) and cloud droplet number concentrations. Vertical profiles of CN and large particle concentrations (Dp>0.07 µm) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols, Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean (CAPRICORN-2) campaign were also conducted during the same period as the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south, CCN sources from the midlatitudes, and enhanced precipitation sink in the cyclonic circulation between the Ferrel and polar cells (around 60∘ S) create opposing latitudinal gradients in the CCN concentration with an observed minimum in the SO between 55 and 60∘ S. The SOCRATES airborne measurements are not influenced by Australian continental emissions but still show evidence of elevated CCN concentrations to the south of 60∘ S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition, south of the Australian and Tasmanian coasts, is apparent in aerosol hygroscopicity derived from CCN spectra and aerosol particle size distribution. The particles are more hygroscopic to the north, consistent with a greater fraction of sea salt from PMA, and less hygroscopic to the south as there is more sulfate and organic particles originating from biogenic sources in coastal Antarctica.

Stratocumulus clouds over the Southern Ocean have fewer droplets and are more likely to exist in the predominately supercooled phase than clouds at similar temperatures over northern oceans. One likely reason is that this region has few continental and anthropogenic sources of cloud-nucleating particles that can form droplets and ice. In this work, we present an overview of aerosol particle types over the Southern Ocean, including new measurements made below, in and above clouds in this region. These measurements and others indicate that biogenic sulfur-based particles >0.1 μm diameter contribute the majority of cloud condensation nuclei number concentrations in summer. Ice nucleating particles tend to have more organic components, likely from sea-spray. Both types of cloud nucleating particles may increase in a warming climate likely to have less sea ice, more phytoplankton activity, and stronger winds over the Southern Ocean near Antarctica. Taken together, clouds over the Southern Ocean may become more reflective and partially counter the region's expected albedo decrease due to diminishing sea ice. However, detailed modeling studies are needed to test this hypothesis due to the complexity of oceancloud-climate feedbacks in the region. Plain Language Summary Clouds over the Southern Ocean tend to have less droplets and ice crystals than similar clouds over northern oceans due to fewer sources of cloud-nucleating aerosol particles in the region. In this work, we present an overview of aerosol particle types over the Southern Ocean, including new measurements made below, in and above clouds. These measurements indicate that while sea-spray-derived salts do provide cloud nuclei, the majority of aerosol particles that influence summertime clouds in this region are biogenic-that is, derived from ocean microorganisms, with the ocean region near Antarctica being a large summertime source. These cloud-nucleating particles may increase in a warming climate likely to have less sea ice and more phytoplankton activity near Antarctica. These additional particles could make low clouds reflect more light and offset a portion of the warming expected due to diminishing sea ice in a future climate. TWOHY ET AL.

Abstract. The Southern Ocean region is one of the most pristine in the world and serves as an important proxy for the pre-industrial atmosphere. Improving our understanding of the natural processes in this region is likely to result in the largest reductions in the uncertainty of climate and earth system models. While remoteness from anthropogenic and continental sources is responsible for its clean atmosphere, this also results in the dearth of atmospheric observations in the region. Here we present a statistical summary of the latitudinal gradient of aerosol (condensation nuclei larger than 10 nm, CN10) and cloud condensation nuclei (CCN at various supersaturations) concentrations obtained from five voyages spanning the Southern Ocean between Australia and Antarctica from late spring to early autumn (October to March) of the 2017/18 austral seasons. Three main regions of influence were identified: the northern sector (40–45∘ S), where continental and anthropogenic sources coexisted with background marine aerosol populations; the mid-latitude sector (45–65∘ S), where the aerosol populations reflected a mixture of biogenic and sea-salt aerosol; and the southern sector (65–70∘ S), south of the atmospheric polar front, where sea-salt aerosol concentrations were greatly reduced and aerosol populations were primarily biologically derived sulfur species with a significant history in the Antarctic free troposphere. The northern sector showed the highest number concentrations with median (25th to 75th percentiles) CN10 and CCN0.5 concentrations of 681 (388–839) cm−3 and 322 (105–443) cm−3, respectively. Concentrations in the mid-latitudes were typically around 350 cm−3 and 160 cm−3 for CN10 and CCN0.5, respectively. In the southern sector, concentrations rose markedly, reaching 447 (298–446) cm−3 and 232 (186–271) cm−3 for CN10 and CCN0.5, respectively. The aerosol composition in this sector was marked by a distinct drop in sea salt and increase in both sulfate fraction and absolute concentrations, resulting in a substantially higher CCN0.5/CN10 activation ratio of 0.8 compared to around 0.4 for mid-latitudes. Long-term measurements at land-based research stations surrounding the Southern Ocean were found to be good representations at their respective latitudes; however this study highlighted the need for more long-term measurements in the region. CCN observations at Cape Grim (40∘39′ S) corresponded with CCN measurements from northern and mid-latitude sectors, while CN10 observations only corresponded with observations from the northern sector. Measurements from a simultaneous 2-year campaign at Macquarie Island (54∘30′ S) were found to represent all aerosol species well. The southernmost latitudes differed significantly from both of these stations, and previous work suggests that Antarctic stations on the East Antarctic coastline do not represent the East Antarctic sea-ice latitudes well. Further measurements are needed to capture the long-term, seasonal and longitudinal variability in aerosol processes across the Southern Ocean.

While the region is known for deep midlatitude cyclones, it is the accompanying fields of marine boundary layer (MBL) clouds that seem to be critical to understanding the radiative energy balance of this region (Bodas-Salcedo et al., 2012, 2014, 2016, 2019). Inspired by Trenberth and Fasullo (2010), who showed a high bias in surface-absorbed solar energy by models, studies have increasingly focused on the ubiquity of supercooled liquid water in SO clouds. Simulations of these clouds too aggressively reduce cloud cover through ice phase precipitation processes (Frey & Kay, 2017; Vergara-Temprado et al., 2018). Recent modeling studies have mitigated this bias through various means and have shown the climate system's sensitivity to these SO MBL clouds (Kay et al., 2016; Tan et al., 2016). How the properties of liquid phase clouds-especially supercooled liquid phase clouds-vary across the SO remains an important topic. While the meteorology of the SO is predictable, variations in factors that control the local and regional aerosol properties differ considerably from regions north of the Antarctic Circumpolar Current (ACC) to the marginal seas along the Antarctic (Armour et al., 2016; Fossum et al., 2018). While seasonally varying sea surface temperatures and sea ice contribute to the cloud variability (Huang et al., 2016), the Antarctic Circumpolar Current essentially divides the SO into lower latitude temperate and high latitude oceans. Especially in the high latitude SO, seasonal biological productivity results in