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1. Cloud Processes and the Transport of Biological Emissions Regulate Southern Ocean Particle and Cloud Condensation Nuclei Concentrations

   Sanchez, K. J.; Roberts, G. C.; Saliba, G.; Russell, L. M.; Twohy, C.; Reeves, M.; Humphries, R. S.; Keywood, M. D.; Ward, J. P.; McRobert, I. M. (January 2021, Atmospheric chemistry and physics)

   null (Ed.)

   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-day 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-days 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 > 0.07µm) 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. 

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2. Evidence for Secondary Ice Production in Southern Ocean Maritime Boundary Layer Clouds

   https://doi.org/10.1029/2021JD036411  

   Järvinen, Emma; McCluskey, Christina S.; Waitz, Fritz; Schnaiter, Martin; Bansemer, Aaron; Bardeen, Charles G.; Gettelman, Andrew; Heymsfield, Andrew; Stith, Jeffrey L.; Wu, Wei; et al (August 2022, Journal of Geophysical Research: Atmospheres)

   Abstract Maritime boundary‐layer clouds over the Southern Ocean (SO) have a large shortwave radiative effect. Yet, climate models have difficulties in representing these clouds and, especially, their phase in this observationally sparse region. This study aims to increase the knowledge of SO cloud phase by presenting in‐situ cloud microphysical observations from the Southern Ocean Clouds, Radiation, Aerosol, Transport Experimental Study (SOCRATES). We investigate the occurrence of ice in summertime marine stratocumulus and cumulus clouds in the temperature range between 6 and −25°C. Our observations show that in ice‐containing clouds, maximum ice number concentrations of up to several hundreds per liter were found. The observed ice crystal concentrations were on average one to two orders of magnitude higher than the simultaneously measured ice nucleating particle (INP) concentrations in the temperature range below −10°C and up to five orders of magnitude higher than estimated INP concentrations in the temperature range above −10°C. These results highlight the importance of secondary ice production (SIP) in SO summertime marine boundary‐layer clouds. Evidence for rime splintering was found in the Hallett‐Mossop (HM) temperature range but the exact SIP mechanism active at lower temperatures remains unclear. Finally, instrument simulators were used to assess simulated co‐located cloud ice concentrations and the role of modeled HM rime‐splintering. We found that CAM6 is deficient in simulating number concentrations across the HM temperature range with little sensitivity to the model HM process, which is inconsistent with the aforementioned observational evidence of highly active SIP processes in SO low‐level clouds. 

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3. Ejection of Dust From the Ocean as a Potential Source of Marine Ice Nucleating Particles

   https://doi.org/10.1029/2020JD033073  

   Cornwell, Gavin C.; Sultana, Camille M.; Prank, Marje; Cochran, Richard E.; Hill, Thomas C. J.; Schill, Gregory P.; DeMott, Paul J.; Mahowald, Natalie; Prather, Kimberly A. (December 2020, Journal of Geophysical Research: Atmospheres)

   Abstract Oceans are, generally, relatively weak sources of ice nucleating particles (INPs). Thus, dust transported from terrestrial regions can dominate atmospheric INP concentrations even in remote marine regions. Studies of ocean‐emitted INPs have focused upon sea spray aerosols containing biogenic species. Even though large concentrations of dust are transported over marine regions, resuspended dust has never been explicitly considered as another possible source of ocean‐emitted INPs. Current models assume that deposited dust is not re‐emitted from surface waters. Our laboratory studies of aerosol particles produced from coastal seawater and synthetic seawater doped with dust show that dust can indeed be ejected from water during bubble bursting. INP concentration measurements show these ejected dust particles retain ice nucleating activity. Doping synthetic seawater to simulate a strong dust deposition event produced INPs active at temperatures colder than −13°C and INP concentrations 1 to 2 orders of magnitude greater than either lab sea spray or marine boundary layer measurements. The relevance of these laboratory findings is highlighted by single‐particle composition measurements along the Californian coast where at least 9% of dust particles were mixed with sea salt. Additionally, global modeling studies show that resuspension of dust from the ocean could exert the most impact over the Southern Ocean, where ocean‐emitted INPs are thought to dominate atmospheric INP populations. More work characterizing the factors governing the resuspension of dust particles is required to understand the potential impact upon clouds. 

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4. A numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particles

   https://doi.org/10.5194/acp-22-847-2022  

   Steinke, Isabelle; DeMott, Paul J.; Deane, Grant B.; Hill, Thomas C.; Maltrud, Mathew; Raman, Aishwarya; Burrows, Susannah M. (January 2022, Atmospheric Chemistry and Physics)

   Abstract. We present a framework for estimating concentrations of episodicallyelevated high-temperature marine ice nucleating particles (INPs) in the seasurface microlayer and their subsequent emission into the atmosphericboundary layer. These episodic INPs have been observed in multipleship-based and coastal field campaigns, but the processes controlling theirocean concentrations and transfer to the atmosphere are not yet fullyunderstood. We use a combination of empirical constraints and simulationoutputs from an Earth system model to explore different hypotheses forexplaining the variability of INP concentrations, and the occurrence ofepisodic INPs, in the marine atmosphere. In our calculations, we examine the following two proposed oceanic sources of high-temperature INPs: heterotrophic bacteria and marine biopolymer aggregates (MBPAs). Furthermore, we assume that the emission of these INPs is determined by the production of supermicron sea spray aerosol formed from jet drops, with an entrainment probability that is described by Poisson statistics. The concentration of jet drops is derived from the number concentration of supermicron sea spray aerosol calculated from model runs. We then derive the resulting number concentrations of marine high-temperature INPs (at 253 K) in the atmospheric boundary layer and compare their variability to atmospheric observations of INP variability. Specifically, we compare against concentrations of episodically occurring high-temperature INPs observed during field campaigns in the Southern Ocean, the Equatorial Pacific, and the North Atlantic. In this case study, we evaluate our framework at 253 K because reliable observational data at this temperature are available across three different ocean regions, but suitable data are sparse at higher temperatures. We find that heterotrophic bacteria and MBPAs acting as INPs provide only apartial explanation for the observed high INP concentrations. We note,however, that there are still substantial knowledge gaps, particularlyconcerning the identity of the oceanic INPs contributing most frequently toepisodic high-temperature INPs, their specific ice nucleation activity, andthe enrichment of their concentrations during the sea–air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs and drivers for their emissions are needed, ideally incombination with modeling studies focused on the potential cloud impacts ofthese high-temperature INPs. 

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5. Measurement report: Cloud processes and the transport of biological emissions affect southern ocean particle and cloud condensation nuclei concentrations

   https://doi.org/10.5194/acp-21-3427-2021  

   Sanchez, Kevin J.; Roberts, Gregory C.; Saliba, Georges; Russell, Lynn M.; Twohy, Cynthia; Reeves, Michael J.; Humphries, Ruhi S.; Keywood, Melita D.; Ward, Jason P.; McRobert, Ian M. (January 2021, Atmospheric Chemistry and Physics)

   null (Ed.)

   Abstract. Long-range transport of biogenic emissions from the coastof Antarctica, precipitation scavenging, and cloud processing are the mainprocesses that influence the observed variability in Southern Ocean (SO)marine boundary layer (MBL) condensation nuclei (CN) and cloud condensationnuclei (CCN) concentrations during the austral summer. Airborne particlemeasurements on the HIAPER GV from north–south transects between Hobart,Tasmania, and 62∘ S during the Southern Ocean Clouds, RadiationAerosol Transport Experimental Study (SOCRATES) were separated into fourregimes comprising combinations of high and low concentrations of CCN andCN. In 5 d HYSPLIT back trajectories, air parcels with elevated CCNconcentrations were almost always shown to have crossed the Antarctic coast,a location with elevated phytoplankton emissions relative to the rest of theSO in the region south of Australia. The presence of high CCN concentrationswas also consistent with high cloud fractions over their trajectory,suggesting there was substantial growth of biogenically formed particlesthrough cloud processing. Cases with low cloud fraction, due to the presenceof cumulus clouds, had high CN concentrations, consistent with previouslyreported new particle formation in cumulus outflow regions. Measurementsassociated with elevated precipitation during the previous 1.5 d of theirtrajectory had low CCN concentrations indicating CCN were effectivelyscavenged by precipitation. A coarse-mode fitting algorithm was used todetermine the primary marine aerosol (PMA) contribution, which accounted for<20 % of CCN (at 0.3 % supersaturation) and cloud dropletnumber concentrations. Vertical profiles of CN and large particleconcentrations (Dp>0.07 µm) indicated that particleformation occurs more frequently above the MBL; however, the growth ofrecently formed particles typically occurs in the MBL, consistent with cloudprocessing 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 theSOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia,likely due to continental and coastal biogenic emissions. The Antarcticcoastal source of CCN from the south, CCN sources from the midlatitudes, andenhanced precipitation sink in the cyclonic circulation between the Ferreland polar cells (around 60∘ S) create opposing latitudinalgradients in the CCN concentration with an observed minimum in the SObetween 55 and 60∘ S. The SOCRATES airbornemeasurements are not influenced by Australian continental emissions butstill show evidence of elevated CCN concentrations to the south of60∘ S, consistent with biogenic coastal emissions. In addition, alatitudinal gradient in the particle composition, south of the Australianand Tasmanian coasts, is apparent in aerosol hygroscopicity derived from CCNspectra and aerosol particle size distribution. The particles are morehygroscopic to the north, consistent with a greater fraction of sea saltfrom PMA, and less hygroscopic to the south as there is more sulfate andorganic particles originating from biogenic sources in coastal Antarctica. 

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