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Background: Glyoxal has been implicated as a significant contributor to the formation of secondary organic aerosols, which play a key role in our ability to estimate the impact of aerosols on climate. Elevated concentrations of glyoxal over remote ocean waters suggests that there is an additional source, distinct from urban and forest environments, which has yet to be identified. Herein, we demonstrate that the ocean can serve as an appreciable source of glyoxal in the atmosphere due to microbiological activity. Methods and Results: Based on mass spectrometric analyses of nascent sea spray aerosols and the sea surface microlayer (SSML) of naturally occurring algal blooms, we provide evidence that during the algae death phase phospholipids become enriched in the SSML and undergo autoxidation thereby generating glyoxal as a degradation product. Conclusions: We propose that the death phase of an algal bloom could serve as an important and currently missing source of glyoxal in the atmosphere. 

Abstract. Sea spray aerosols (SSAs) represent one of the most abundant aerosol types on a global scale and have been observed at all altitudes including the upper troposphere. SSA has been explored in recent years as a source of ice-nucleating particles (INPs) in cirrus clouds due to the ubiquity of cirrus clouds and the uncertainties in their radiative forcing. This study expands upon previous works on low-temperature ice nucleation of SSA by investigating the effects of atmospheric aging of SSA and the ice-nucleating activity of newly formed secondary marine aerosols (SMAs) using an oxidation flow reactor. Polydisperse aerosol distributions were generated from a marine aerosol reference tank (MART) filled with 120 L of real or artificial seawater and were dried to very low relative humidity to crystallize the salt constituents of SSA prior to their subsequent freezing, which was measured using a continuous flow diffusion chamber (CFDC). Results show that for primary SSA (pSSA), as well as aged SSA and SMA (aSSA+SMA) at temperatures >220 K, homogeneous conditions (92 %–97 % relative humidity with respect to water – RHw) were required to freeze 1 % of the particles. However, below 220 K, heterogeneous nucleation occurs for both pSSA and aSSA+SMA at much lower RHw, where up to 1 % of the aerosol population freezes between 75 % and 80 % RHw. Similarities between freezing behaviors of the pSSA and aSSA+SMA at all temperatures suggest that the contributions of condensed organics onto the pSSA or alteration of functional groups in pSSA via atmospheric aging did not hinder the major heterogeneous ice nucleation process at these cirrus temperatures, which have previously been shown to be dominated by the crystalline salts. Occurrence of a 1 % frozen fraction of SMA, generated in the absence of primary SSA, was observed at or near water saturation below 220 K, suggesting it is not an effective INP at cirrus temperatures, similar to findings in the literature on other organic aerosols. Thus, any SMA coatings on the pSSA would only decrease the ice nucleation behavior of pSSA if the organic components were able to significantly delay water uptake of the inorganic salts, and apparently this was not the case. Results from this study demonstrate the ability of lofted primary sea spray particles to remain an effective ice nucleator at cirrus temperatures, even after atmospheric aging has occurred over a period of days in the marine boundary layer prior to lofting. We were not able to address aging processes under upper-tropospheric conditions. 

Abstract 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 simulations 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. Including wind speed in addition to activation temperature in a marine INP parameterization reduces bias but does not explain the large range of observed INP concentrations. Direct and indirect inference of marine INP size suggests MBL INPs, at least during Austral summer, are dominated by particles with diameters smaller than 500 nm. 

The 540s, 1450s, and 1600s represent three of the five coldest decades in the Common Era (CE). In each of these cases, the cause of these cold pulses has been attributed to large volcanic eruptions. However, the provenance of the eruption and magnitude of the volcanic forcing remains uncertain. Here, we use high-resolution sulfur isotopes in Greenland and Antarctic ice cores measured across these events to provide a means of improving sulfur loading estimates for these eruptions. In each case, the largest reconstructed tree-ring cooling is associated with an extratropical eruption, and the high-altitude stratospheric sulfate loading of these events is substantially smaller than previous estimates (by up to a factor of two). These results suggest an increased sensitivity of the reconstructed Northern Hemisphere summer temperature response to extratropical eruptions. This highlights the importance of climate feedbacks and processes that amplify and prolong the cooling signal from high latitudes, such as changes in sea ice extent and ocean heat content. 

Ice nucleating particles (INPs) in sea spray aerosol (SSA) are important for ice formation in clouds over oceans. We found that SSA INP concentrations during a phytoplankton bloom were degraded with exposure to 3 to 8 days of atmospheric oxidation. 

Oceans emit ice-nucleating particles (INPs) which freeze supercooled cloud droplets, modifying clouds. We added dead biomass of three phytoplankton to seawater. Each time, this stimulated INP production in the water and INP emissions in sea spray. 

Abstract The secondary ice process (SIP) is a major microphysical process, which can result in rapid enhancement of ice particle concentration in the presence of preexisting ice. SPICULE was conducted to further investigate the effect of collision–coalescence on the rate of the fragmentation of freezing drop (FFD) SIP mechanism in cumulus congestus clouds. Measurements were conducted over the Great Plains and central United States from two coordinated aircraft, the NSF Gulfstream V (GV) and SPEC Learjet 35A, both equipped with state-of-the-art microphysical instrumentation and vertically pointing W- and Ka-band radars, respectively. The GV primarily targeted measurements of subcloud aerosols with subsequent sampling in warm cloud. Simultaneously, the Learjet performed multiple penetrations of the ascending cumulus congestus (CuCg) cloud top. First primary ice was typically detected at temperatures colder than −10°C, consistent with measured ice nucleating particles. Subsequent production of ice via FFD SIP was strongly related to the concentration of supercooled large drops (SLDs), with diameters from about 0.2 to a few millimeters. The concentration of SLDs is directly linked to the rate of collision–coalescence, which depends primarily on the subcloud aerosol size distribution and cloud-base temperature. SPICULE supports previous observational results showing that FFD SIP efficiency could be deduced from the product of cloud-base temperature and maximum diameter of drops measured ∼300 m above cloud base. However, new measurements with higher concentrations of aerosol and total cloud-base drop concentrations show an attenuating effect on the rate of coalescence. The SPICULE dataset provides rich material for validation of numerical schemes of collision–coalescence and SIP to improve weather prediction simulations 

Microorganisms are ubiquitous and highly diverse in the atmosphere. Despite the potential impacts of airborne bacteria found in the lower atmosphere over the Southern Ocean (SO) on the ecology of Antarctica and on marine cloud phase, no previous region-wide assessment of bioaerosols over the SO has been reported. We conducted bacterial profiling of boundary layer shipboard aerosol samples obtained during an Austral summer research voyage, spanning 42.8 to 66.5°S. Contrary to findings over global subtropical regions and the Northern Hemisphere, where transport of microorganisms from continents often controls airborne communities, the great majority of the bacteria detected in our samples were marine, based on taxonomy, back trajectories, and source tracking analysis. Further, the beta diversity of airborne bacterial communities varied with latitude and temperature, but not with other meteorological variables. Limited meridional airborne transport restricts southward community dispersal, isolating Antarctica and inhibiting microorganism and nutrient deposition from lower latitudes to these same regions. A consequence and implication for this region’s marine boundary layer and the clouds that overtop it is that it is truly pristine, free from continental and anthropogenic influences, with the ocean as the dominant source controlling low-level concentrations of cloud condensation nuclei and ice nucleating particles. 

Abstract Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation and radiative processes, and their interactions. Projects between 2016 and 2018 used in-situ probes, radar, lidar and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN) and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase cloudsnucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF/NCAR G-V aircraft flying north-south gradients south of Tasmania, at Macquarie Island, and on the RV Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show a largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multi-layered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of confirmed low clouds were responsible for radiation biases. The combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.