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The aerosol-driven radiative effects on marine low-level cloud represent a large uncertainty in climate simulations, in particular over the Southern Ocean, which is also an important region for sea spray aerosol production. Observations of sea spray aerosol organic enrichment and the resulting impact on water uptake over the remote Southern Hemisphere are scarce, and therefore the region is under-represented in existing parameterisations. The Surface Ocean Aerosol Production (SOAP) voyage was a 23 d voyage which sampled three phytoplankton blooms in the highly productive water of the Chatham Rise, east of New Zealand. In this study we examined the enrichment of organics to nascent sea spray aerosol and the modifications to sea spray aerosol water uptake using in situ chamber measurements of seawater samples taken during the SOAP voyage. Primary marine organics contributed up to 23 % of the sea spray mass for particles with diameter less than approximately 1 µm and up to 79 % of the particle volume for 50 nm diameter sea spray. The composition of the submicron organic fraction was consistent throughout the voyage and was largely composed of a polysaccharide-like component, characterised by very low alkane-to-hydroxyl-concentration ratios of approximately 0.1–0.2. The enrichment of organics was compared to the output from the chlorophyll-a-based sea spray aerosol parameterisation suggested by Gantt et al. (2011) and the OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) models. OCEANFILMS improved on the representation of the organic fraction predicted using chlorophyll a, in particular when the co-adsorption of polysaccharides was included; however, the model still under-predicted the proportion of polysaccharides by an average of 33 %. Nascent 50 nm diameter sea spray aerosol hygroscopic growth factors measured at 90 % relative humidity averaged 1.93±0.08 and did not decrease with increasing sea spray aerosol organic fractions. The observed hygroscopicity was greater than expected from the assumption of full solubility, particularly during the most productive phytoplankton bloom (B1), during which organic fractions were greater than approximately 0.4. The water uptake behaviour observed in this study is consistent with that observed for other measurements of phytoplankton blooms and can be partially attributed to the presence of sea salt hydrates, which lowers the sea spray aerosol hygroscopicity when the organic enrichment is low. The inclusion of surface tension effects only marginally improved the modelled hygroscopicity, and a significant discrepancy between the observed and modelled hygroscopicity at high organic volume fractions remained. The findings from the SOAP voyage highlight the influence of biologically sourced organics on sea spray aerosol composition; these data improve the capacity to parameterise sea spray aerosol organic enrichment and water uptake.

Marine nitrogen fixation is co-limited by the supply of iron (Fe) and phosphorus in large regions of the global ocean. The deposition of soluble aerosol Fe can initiate nitrogen fixation and trigger toxic algal blooms in nitrate-poor tropical waters. We present dry season soluble Fe data from the Savannah Fires in the Early Dry Season (SAFIRED) campaign in northern Australia that reflects coincident dust and biomass burning sources of soluble aerosol Fe. The mean soluble and total aerosol Fe concentrations were 40 and 500 ng m−3 respectively. Our results show that while biomass burning species may not be a direct source of soluble Fe, biomass burning may substantially enhance the solubility of mineral dust. We observed fractional Fe solubility up to 12 % in mixed aerosols. Thus, Fe in dust may be more soluble in the tropics compared to higher latitudes due to higher concentrations of biomass-burning-derived reactive organic species in the atmosphere. In addition, biomass-burning-derived particles can act as a surface for aerosol Fe to bind during atmospheric transport and subsequently be released to the ocean upon deposition. As the aerosol loading is dominated by biomass burning emissions over the tropical waters in the dry season, additions of biomass-burning-derived soluble Fe could have harmful consequences for initiating nitrogen-fixing toxic algal blooms. Future research is required to quantify biomass-burning-derived particle sources of soluble Fe over tropical waters.

There is a lack of knowledge of how biomass burning aerosols in the tropics age, including those in the fire-prone Northern Territory in Australia. This paper reports chemical characterization of fresh and aged aerosols monitored during the 1-month-long SAFIRED (Savannah Fires in the Early Dry Season) field study, with an emphasis on the chemical signature and aging of organic aerosols. The campaign took place in June 2014 during the early dry season when the surface measurement site, the Australian Tropical Atmospheric Research Station (ATARS), located in the Northern Territory, was heavily influenced by thousands of wild and prescribed bushfires. ATARS was equipped with a wide suite of instrumentation for gaseous and aerosol characterization. A compact time-of-flight aerosol mass spectrometer was deployed to monitor aerosol chemical composition. Approximately 90 % of submicron non-refractory mass was composed of organic material. Ozone enhancement in biomass burning plumes indicated increased air mass photochemistry. The diversity in biomass burning emissions was illustrated through variability in chemical signature (e.g. wide range in f44, from 0.06 to 0.18) for five intense fire events. The background particulate loading was characterized using positive matrix factorization (PMF). A PMF-resolved BBOA (biomass burning organic aerosol) factor comprised 24 % of the submicron non-refractory organic aerosol mass, confirming the significance of fire sources. A dominant PMF factor, OOA (oxygenated organic aerosol), made up 47 % of the sampled aerosol, illustrating the importance of aerosol aging in the Northern Territory. Biogenic isoprene-derived organic aerosol factor was the third significant fraction of the background aerosol (28 %).

The Southern Ocean radiative bias continues to impact climate and weather models, including the Australian Community Climate and Earth System Simulator (ACCESS). The radiative bias, characterised by too much shortwave radiation reaching the surface, is attributed to the incorrect simulation of cloud properties, including frequency and phase. To identify cloud regimes important to the Southern Ocean, we use k-means cloud histogram clustering, applied to a satellite product and then fitted to nudged simulations of the latest-generation ACCESS atmosphere model. We identify instances when the model correctly or incorrectly simulates the same cloud type as the satellite product for any point in time or space. We then evaluate the cloud and radiation biases in these instances. We find that when the ACCESS model correctly simulates the cloud type, cloud property and radiation biases of equivalent, or in some cases greater, magnitude remain compared to when cloud types are incorrectly simulated. Furthermore, we find that even when radiative biases appear small on average, cloud property biases, such as liquid or ice water paths or cloud fractions, remain large. Our results suggest that simply getting the right cloud type (or the cloud macrophysics) is not enough to reduce the Southern Ocean radiative bias. Furthermore, in instances where the radiative bias is small, it may be so for the wrong reasons. Considerable effort is still required to improve cloud microphysics, with a particular focus on cloud phase.

Dimethyl sulfide (DMS) and methanethiol (MeSH) are biologically co‐produced marine volatile sulfur compounds, which play a critical role in climate‐cooling aerosol formation. The spatio‐temporal distributions of MeSH are poorly constrained, especially over the Southern Ocean. DMS and MeSH atmospheric concentrations and relative contributions to volatile methylated sulfur (VMS) were measured across the Southern Ocean, spanning all seasons and latitudes from 37°S to 67°S. Highest absolute mixing ratios of MeSH occurred in summer (up to 250 ppt), over biologically productive waters at 45°S to 52°S and close to the Antarctic coast (>${ >} $ 62°S). Highest MeSH/VMS occurred in spring and winter (up to 35%), and at the Subtropical Front and Antarctic coast. These results constrain MeSH contributions to VMS over the Southern Ocean, explore mechanisms driving these dynamics, and support recently modeled MeSH importance to the atmospheric sulfur burden, with significant implications for modeling climate‐cooling aerosols.

The interaction of natural marine aerosol with clouds and radiation is a significant source of climate model uncertainty. The Southern Ocean represents a key area to understand these interactions, and a region where significant model biases exist. Here we provide an evaluation of the Australian Community Climate and Earth System Simulator atmosphere model which includes a double-moment aerosol scheme. We evaluate against measurements of condensation nuclei (N10) and cloud condensation nuclei (CCN) number from seven ship campaigns and three terrestrial locations, spanning the years 2015–2019. We find that N10 is heavily underestimated in the model across all regions and seasons by more than 50 % and in some cases by over 80 % at higher latitudes. CCN is also strongly underestimated over marine and Antarctic regions, often by more than 50 %. We then perform seven sensitivity tests to explore different aerosol configurations. We find that updating the dimethyl sulfide climatology and turning on the primary marine organic aerosol flux marginally improves marine CCN by between 4 %–9 %. N10 was reduced by between 3 %–9 %. The Southern Ocean radiative bias is also reduced by this combination of changes, with limited adverse effects. We also test altering the sea spray flux to use wind gust instead of mean wind speed. This significantly improved CCN in the marine regions, but resulted in detrimental impacts on the region's radiation budget, indicating that drastically improving the Southern Ocean's CCN budget may lead to poorer simulations of the global climate.

As a long-standing problem in climate models, large positive shortwave radiation biases exist at the surface over the Southern Ocean, impacting the accurate simulation of sea surface temperature, atmospheric circulation, and precipitation. Underestimations of low-level cloud fraction and liquid water content are suggested to predominantly contribute to these radiation biases. Most model evaluations for radiation focus on summer and rely on satellite products, which have their own limitations. In this work, we use surface-based observations at Macquarie Island to provide the first long-term, seasonal evaluation of both downwelling surface shortwave and longwave radiation in the Australian Community Climate and Earth System Simulator Atmosphere-only Model version 2 (ACCESS-AM2) over the Southern Ocean. The capacity of the Clouds and the Earth’s Radiant Energy System (CERES) product to simulate radiation is also investigated. We utilize the novel lidar simulator, the Automatic Lidar and Ceilometer Framework (ALCF), and all-sky cloud camera observations of cloud fraction to investigate how radiation biases are influenced by cloud properties. Overall, we find an overestimation of +9.5±33.5 W m−2 for downwelling surface shortwave radiation fluxes and an underestimation of -2.3±13.5 W m−2 for downwelling surface longwave radiation in ACCESS-AM2 in all-sky conditions, with more pronounced shortwave biases of +25.0±48.0 W m−2 occurring in summer. CERES presents an overestimation of +8.0±18.0 W m−2 for the shortwave and an underestimation of -12.1±12.2 W m−2 for the longwave in all-sky conditions. For the cloud radiative effect (CRE) biases, there is an overestimation of +4.8±28.0 W m−2 in ACCESS-AM2 and an underestimation of -7.9±20.9 W m−2 in CERES. An overestimation of downwelling surface shortwave radiation is associated with an underestimated cloud fraction and low-level cloud occurrence. We suggest that modeled cloud phase is also having an impact on the radiation biases. Our results show that the ACCESS-AM2 model and CERES product require further development to reduce these radiation biases not just in shortwave and in all-sky conditions, but also in longwave and in clear-sky conditions.

Measurements of aerosol composition and size distributions were taken during the summer of 2013 at the remote island of Lampedusa in the southern central Mediterranean Sea. These measurements were part of the ChArMEx/ADRIMED (Chemistry and Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate) framework and took place during Special Observation Period 1a (SOP-1a) from 11 June to 5 July 2013. From compact time-of-flight aerosol mass spectrometer (cToF-AMS) measurements in the size range below 1 µm in aerodynamic diameter (PM1), particles were predominately comprised of ammonium and sulfate. On average, ammonium sulfate contributed 63 % to the non-refractory PM1 mass, followed by organics (33 %). The organic aerosol was generally very highly oxidized (f44 values were typically between 0.25 and 0.26). The contribution of ammonium sulfate was generally higher than organic aerosol in comparison to measurements taken in the western Mediterranean but is consistent with studies undertaken in the eastern basin. Source apportionment of organics using a statistical (positive matrix factorization) model revealed four factors: a hydrocarbon-like organic aerosol (HOA), a methanesulfonic-acid-related oxygenated organic aerosol (MSA-OOA), a more oxidized oxygenated organic aerosol (MO-OOA) and a less oxidized oxygenated organic aerosol (LO-OOA). The MO-OOA was the dominant factor for most of the campaign (53 % of the PM1 OA mass). It was well correlated with SO42-, highly oxidized and generally more dominant during easterly air masses originating from the eastern Mediterranean and central Europe. The LO-OOA factor had a very similar composition to the MO-OOA factor but was more prevalent during westerly winds, with air masses originating from the Atlantic Ocean, the western Mediterranean and at high altitudes over France and Spain from mistral winds. The MSA-OOA factor contributed an average 12 % to the PM1 OA and was more dominant during the mistral winds. The HOA, representing observed primary organic aerosol, only contributed 8 % of the average PM1 OA during the campaign. Even though Lampedusa is one of the most remote sites in the Mediterranean, PM1 concentrations (10 ± 5 µg m−3) were comparable to those observed in coastal cities and sites closer to continental Europe. Cleaner conditions corresponded to higher wind speeds. Nucleation and growth of new aerosol particles was observed during periods of north-westerly winds. From a climatology analysis from 1999 to 2012, these periods were much more prevalent during the measurement campaign than during the preceding 13 years. These results support previous findings that highlight the importance of different large-scale synoptic conditions in determining the regional and local aerosol composition and oxidation and also suggest that a non-polluted surface atmosphere over the Mediterranean is rare.

The evaluation and quantification of Southern Ocean cloud–radiation interactions simulated by climate models are essential in understanding the sources and magnitude of the radiative bias that persists in climate models for this region. To date, most evaluation methods focus on specific synoptic or cloud-type conditions that do not consider the entirety of the Southern Ocean's cloud regimes at once. Furthermore, it is difficult to directly quantify the complex and non-linear role that different cloud properties have on modulating cloud radiative effect. In this study, we present a new method of model evaluation, using machine learning that can at once identify complexities within a system and individual contributions.To do this, we use an XGBoost (eXtreme Gradient Boosting) model to predict the radiative bias within a nudged version of the Australian Community Climate and Earth System Simulator – Atmosphere-only model, using cloud property biases as predictive features. We find that the XGBoost model can explain up to 55 % of the radiative bias from these cloud properties alone. We then apply SHAP (SHapley Additive exPlanations) feature importance analysis to quantify the role each cloud property bias plays in predicting the radiative bias. We find that biases in the liquid water path are the largest contributor to the cloud radiative bias over the Southern Ocean, though important regional and cloud-type dependencies exist. We then test the usefulness of this method in evaluating model perturbations and find that it can clearly identify complex responses, including cloud property and cloud-type compensating errors.