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Abstract. 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.

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Clouds over the Southern Ocean can contain super-cooled liquid water, which means the water remains liquid below 0°C. This is because the water in these clouds has had little contact with pollution or dust, which can help water freeze. Super-cooled liquid water clouds reflect more sunlight back into space than ice clouds, which can affect the temperature of the ocean. The Southern Ocean is a unique environment with fewer ice nucleating particles, making it difficult to study. Scientists are conducting research expeditions to gather more data and improve climate models. [Extracted from the article]

The evaluation and quantification of Southern Ocean cloud-radiation interactions simulated by climate models is 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 and are unable to quantitatively define the impact of cloud properties on the radiative bias whilst considering the system as a whole. 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 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 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 liquid water path is 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. [ABSTRACT FROM AUTHOR]

The evaluation and quantification of Southern Ocean cloud-radiation interactions simulated by climate models is 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 and are unable to quantitatively define the impact of cloud properties on the radiative bias whilst considering the system as a whole. 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 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 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 liquid water path is 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. [ABSTRACT FROM AUTHOR]

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 are therefore the region is under-represented in existing parameterisations. The Surface Ocean Aerosol Production (SOAP) voyage was a 23 day 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 87 % of the particle volume in the Aitken mode. The composition of the organic fraction was consistent throughout the voyage and was largely comprised 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 models. OCEANFILMS improved on the representation of the organic fraction predicted using chlorophyll-a, in particular when the co-adsoprtion of polysaccharides was included, however the model still under predicted the proportion of polysaccharides by an average of 33 %. Nascent sea spray aerosol hygroscopic growth factors 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 was attributed to the surface partitioning of the organic components which leads to a decrease in particle surface tension and an increase in hygroscopicity. The compressed film model was used to estimate the influence of surface partitioning and the error in the modelled hygroscopicity was low only when the entire organic fraction was available to partition to the particle surface. The modelled sea spray aerosol hygroscopicity at high organic fractions was underestimated when only a portion of the organic component was available to be partitioned to the surface. 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. [ABSTRACT FROM AUTHOR]

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 the Special Observation Period 1a (SOP-1a) from 11 June until 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 sulphate. On average, ammonium sulphate contributed 63 % to the non-refractory PM1 mass, followed by organics (33 %). The organic aerosol was generally very highly oxidised (f44 values were typically between 0.25 and 0.26). The contribution of ammonium sulphate 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 factorisation) model revealed four factors; a hydrocarbon-like organic aerosol (HOA), a methanesulfonic acid related oxygenated organic aerosol (MSA-OOA), a more oxidised oxygenated organic aerosol (MO-OOA) and a less oxidised oxygenated organic aerosol we label (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 oxidised, 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 in 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 northwesterly winds. From a climatology analysis from 1999 until 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. [ABSTRACT FROM AUTHOR]

The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29th of May, 2014 until the 30th June, 2014 at the Australian Tropical Atmospheric Research Station (ATARS) in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, mercury cycle, and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various emitted species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS. Biomass burning emissions dominated the gas and aerosol concentrations in this region. Nine major biomass burning events were identified and associated with intense or close individual smoke plumes. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. The outcomes of this campaign will be numerous. This region is an environment with little human impact and provides a unique look into the characteristics of biomass burning aerosol without the influence of other significant emission sources. Relationships between the aerosol physical and chemical properties, gas concentrations and meteorological data for the entire month will provide fundamental knowledge required to understand the influence of early dry season burning in this tropical region on the atmosphere. In this paper we present characteristics of the biomass burning observed at the sampling site and provide an overview of the more specific outcomes of the SAFIRED campaign. [ABSTRACT FROM AUTHOR]

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 and aging of aerosols monitored during the one month long SAFIRED (Savannah Fires in the Early Dry Season) field study, with an emphasis on 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 80% of submicron carbonaceous mass and 90% of submicron non-refractory mass was composed of organic material. Ozone enhancement in biomass burning plumes indicated increased air mass photochemistry and increased organic aerosol and particle diameter with the aging parameter (f44) suggested secondary organic aerosol formation. Diversity of biomass burning emissions was illustrated through variability in chemical signature (e.g. wide range in f44, from 0.06 to 0.13) 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 sampled aerosol fraction, illustrating the importance of aerosol aging in the Northern Territory. Biogenic IEPOX-SOA (isoprene epoxydiols-related secondary organic aerosol) was the third significant fraction of the background aerosol (28%). [ABSTRACT FROM AUTHOR]