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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 %).

Aerosols deposited into the Great Barrier Reef (GBR) contain iron (Fe) and other trace metals, which may act as micronutrients or as toxins to this sensitive marine ecosystem. In this paper, we quantified the atmospheric deposition of Fe and investigated aerosol sources in Mission Beach (Queensland) next to the GBR. Leaching experiments were applied to distinguish pools of Fe with regard to its solubility. The labile Fe concentration in aerosols was 2.3–10.6 ng m−3, which is equivalent to 4.9%–11.4% of total Fe and was linked to combustion and biomass burning processes, while total Fe was dominated by crustal sources. A one-day precipitation event provided more soluble iron than the average dry deposition flux, 0.165 and 0.143 μmol m−2 day−1, respectively. Scanning Electron Microscopy indicated that alumina-silicates were the main carriers of total Fe and samples affected by combustion emissions were accompanied by regular round-shaped carbonaceous particulates. Collected aerosols contained significant amounts of Cd, Co, Cu, Mo, Mn, Pb, V, and Zn, which were mostly (47.5%–96.7%) in the labile form. In this study, we provide the first field data on the atmospheric delivery of Fe and other trace metals to the GBR and propose that this is an important delivery mechanism to this region.

The frequency of coral bleaching events increased during the past decade in the Great Barrier Reef (GBR) due to climate change, and rising ocean temperatures. Recent work has demonstrated that enhancing local-scale cloud albedo can reduce the sea surface temperatures (SSTs) in this region. However, little research has been done on variations in the aerosol properties, as well as aerosol–radiation and aerosol–cloud interactions over different regions of the GBR, which is critical for predicting the potential for marine cloud brightening (MCB) climate forcing on a local or regional scale. Here, we examined trends in the aerosol population in terms of their physical and cloud condensation nuclei (CCN) properties during a research cruise in the Central and Northern GBR. Overall higher particle number concentrations, CCN number concentrations, and CCN activation ratios were observed during periods where the air masses passed over the continent prior to reaching the research vessel, despite lower hygroscopicity parameters. We suggest that organics contribute considerably to CCN number concentrations in this region of the GBR, which highlight the important role of additional emissions from inland Queensland. As well as the total aerosol number concentration, precipitation history along the back trajectory affected CCN number concentrations. These results represent a first step towards building a climatological understanding of aerosol and CCN properties over the GBR during summertime, a region and season where no observations have been previously reported.

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.

Cloud–radiation interactions over the Southern Ocean are not well constrained in climate models, in part due to uncertainties in the sources, concentrations, and cloud-forming potential of aerosol in this region. To date, most studies in this region have reported measurements from fixed terrestrial stations or a limited set of instrumentation and often present findings as broad seasonal or latitudinal trends. Here, we present an extensive set of aerosol and meteorological observations obtained during an austral summer cruise across the full width of the Southern Ocean south of Australia. Three episodes of continental-influenced air masses were identified, including an apparent transition between the Ferrel atmospheric cell and the polar cell at approximately 64∘ S, and accompanied by the highest median cloud condensation nuclei (CCN) concentrations, at 252 cm−3. During the other two episodes, synoptic-scale weather patterns diverted air masses across distances greater than 1000 km from the Australian and Antarctic coastlines, respectively, indicating that a large proportion of the Southern Ocean may be periodically influenced by continental air masses. In all three cases, a highly cloud-active accumulation mode dominated the size distribution, with up to 93 % of the total number concentration activating as CCN. Frequent cyclonic weather conditions were observed at high latitudes and the associated strong wind speeds led to predictions of high concentrations of sea spray aerosol. However, these modelled concentrations were not achieved due to increased aerosol scavenging rates from precipitation and convective transport into the free troposphere, which decoupled the air mass from the sea spray flux at the ocean surface. CCN concentrations were more strongly impacted by high concentrations of large-diameter Aitken mode aerosol in air masses which passed over regions of elevated marine biological productivity, potentially contributing up to 56 % of the cloud condensation nuclei concentration. Weather systems were vital for aerosol growth in biologically influenced air masses and in their absence ultrafine aerosol diameters were less than 30 nm. These results demonstrate that air mass meteorological history must be considered when modelling sea spray concentrations and highlight the potential importance of sub-grid-scale variability when modelling atmospheric conditions in the remote Southern Ocean.

The remoteness and extreme conditions of the Southern Ocean and Antarctic region have meant that observations in this region are rare, and typically restricted to summertime during research or resupply voyages. Observations of aerosols outside of the summer season are typically limited to long-term stations, such as Kennaook / Cape Grim (KCG; 40.7∘ S, 144.7∘ E), which is situated in the northern latitudes of the Southern Ocean, and Antarctic research stations, such as the Japanese operated Syowa (SYO; 69.0∘ S, 39.6∘ E). Measurements in the midlatitudes of the Southern Ocean are important, particularly in light of recent observations that highlighted the latitudinal gradient that exists across the region in summertime. Here we present 2 years (March 2016–March 2018) of observations from Macquarie Island (MQI; 54.5∘ S, 159.0∘ E) of aerosol (condensation nuclei larger than 10 nm, CN10) and cloud condensation nuclei (CCN at various supersaturations) concentrations. This important multi-year data set is characterised, and its features are compared with the long-term data sets from KCG and SYO together with those from recent, regionally relevant voyages. CN10 concentrations were the highest at KCG by a factor of ∼50 % across all non-winter seasons compared to the other two stations, which were similar (summer medians of 530, 426 and 468 cm−3 at KCG, MQI and SYO, respectively). In wintertime, seasonal minima at KCG and MQI were similar (142 and 152 cm−3, respectively), with SYO being distinctly lower (87 cm−3), likely the result of the reduction in sea spray aerosol generation due to the sea ice ocean cover around the site. CN10 seasonal maxima were observed at the stations at different times of year, with KCG and MQI exhibiting January maxima and SYO having a distinct February high. Comparison of CCN0.5 data between KCG and MQI showed similar overall trends with summertime maxima and wintertime minima; however, KCG exhibited slightly (∼10 %) higher concentrations in summer (medians of 158 and 145 cm−3, respectively), whereas KCG showed ∼40 % lower concentrations than MQI in winter (medians of 57 and 92 cm−3, respectively). Spatial and temporal trends in the data were analysed further by contrasting data to coincident observations that occurred aboard several voyages of the RSV Aurora Australis and the RV Investigator. Results from this study are important for validating and improving our models and highlight the heterogeneity of this pristine region and the need for further long-term observations that capture the seasonal cycles.

Coral reefs have been found to produce the sulfur compound dimethyl sulfide (DMS), a climatically relevant aerosol precursor predominantly associated with phytoplankton. Until recently, the role of coral-reef-derived DMS within the climate system had not been quantified. A study preceding the present work found that DMS produced by corals had negligible long-term climatic forcing at the global–regional scale. However, at sub-daily timescales more typically associated with aerosol and cloud formation, the influence of coral-reef-derived DMS on local aerosol radiative effects remains unquantified. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) has been used in this work to study the role of coral-reef-derived DMS at sub-daily timescales for the first time. WRF-Chem was run to coincide with an October 2016 field campaign over the Great Barrier Reef, Queensland, Australia, against which the model was evaluated. After updating and scaling the DMS surface water climatology, the model reproduced DMS and sulfur concentrations well. The inclusion of coral-reef-derived DMS resulted in no significant change in sulfate aerosol mass or total aerosol number. Subsequently, no direct or indirect aerosol effects were detected. The results suggest that the co-location of the Great Barrier Reef with significant anthropogenic aerosol sources along the Queensland coast prevents coral-reef-derived aerosol from having a modulating influence on local aerosol burdens in the current climate.

The vast majority of Australia's fires occur in the tropical north of the continent during the dry season. These fires are a significant source of aerosol and cloud condensation nuclei (CCN) in the region, providing a unique opportunity to investigate the biomass burning aerosol (BBA) in the absence of other sources. CCN concentrations at 0.5 % supersaturation and aerosol size and chemical properties were measured at the Australian Tropical Atmospheric Research Station (ATARS) during June 2014. CCN concentrations reached over 104 cm−3 when frequent and close fires were burning – up to 45 times higher than periods with no fires. Both the size distribution and composition of BBA appeared to significantly influence CCN concentrations. A distinct diurnal trend in the proportion of BBA activating to cloud droplets was observed, with an activation ratio of 40 ± 20 % during the night and 60 ± 20 % during the day. BBA was, on average, less hygroscopic during the night (κ = 0. 04 ± 0.03) than during the day (κ =  0.07 ± 0.05), with a maximum typically observed just before midday. Size-resolved composition of BBA showed that organics comprised a constant 90 % of the aerosol volume for aerodynamic diameters between 100 and 200 nm. While this suggests that the photochemical oxidation of organics led to an increase in the hygroscopic growth and an increase in daytime activation ratios, it does not explain the decrease in hygroscopicity after midday. Modelled CCN concentrations assuming typical continental hygroscopicities produced very large overestimations of up to 200 %. Smaller, but still significant, overpredictions up to  ∼  100 % were observed using aerosol mass spectrometer (AMS)- and hygroscopicity tandem differential mobility analyser (H-TDMA)-derived hygroscopicities as well as campaign night and day averages. The largest estimations in every case occurred during the night, when the small variations in very weakly hygroscopic species corresponded to large variations in the activation diameters. Trade winds carry the smoke generated from these fires over the Timor Sea, where aerosol–cloud interactions are likely to be sensitive to changes in CCN concentrations, perturbing cloud albedo and lifetime. Dry season fires in northern Australia are therefore potentially very important in cloud processes in this region.

The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29 May until 30 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, speciated atmospheric mercury and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various 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. 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. Here 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.

Internally and externally mixed aerosols present significant challenges in assessing the hygroscopicity of each aerosol component. This study presents a new sampling technique which uses differences in volatility to separate mixtures and directly examine their respective composition and hygroscopic contribution. A shared thermodenuder and unheated bypass line are continuously cycled between an aerosol mass spectrometer and a volatility and hygroscopicity tandem differential mobility analyser, allowing real-time comparative analysis of heated and unheated aerosol properties. Measurements have been taken of both chamber-generated secondary organic aerosol and coastal marine aerosol at Cape Grim, Australia, to investigate system performance under diverse conditions. Despite rapidly changing aerosol properties and the need to restrict analysis to a narrow size range, the former experiment separated the hygroscopic influences of ammonium sulfate and two distinct organic components with similar oxygen to carbon ratios but different volatilities. Analysis of the marine aerosol revealed an external mixture of non-sea-salt sulfates and sea spray aerosol, which likely shared similar volatile fractions composed of sulfuric acid and a non-hygroscopic organic component.