ORCID Profile
0000-0003-2749-8833
Current Organisation
University of Tasmania
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Air pollution processes and air quality measurement | Atmospheric aerosols | Atmospheric composition chemistry and processes | Maritime Engineering | Ocean Engineering | Atmospheric sciences | Physical Oceanography | Glaciology
Effects of Climate Change and Variability on Antarctic and Sub-Antarctic Environments (excl. Social Impacts) | Climate Change Models | Antarctic and Sub-Antarctic Oceanography |
Publisher: Copernicus GmbH
Date: 23-03-2017
Abstract: Abstract. 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 c aign 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 ersity 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 s led 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 %).
Publisher: Copernicus GmbH
Date: 15-12-2021
DOI: 10.5194/AMT-2021-403
Abstract: Abstract. Optical particle counters (OPC) are widely used to measure the aerosol particle number size distribution at atmospheric ambient conditions and over a large size range. Their measurement principle is based on the dependence of light scattering on particle size. However, this dependence is not monotonic at all sizes and light scattering also depends on the particle composition (i.e., the complex refractive index, CRI) and morphology. Therefore, the conversion of the measured scattered intensity to the desired particle size depends on the microphysical properties of the s led aerosol population and might not be unique at all sizes. While these complexities have been addressed before, corrections are typically applied ad-hoc and are not standardised. This paper addresses this issue by providing a consistent and extended database of pre−computed correction factors for a wide range of complex refractive index values representing the composition variability of atmospheric aerosols. These correction factors are calculated for five different commercial OPCs (USHAS, PCASP, FSSP, GRIMM and its airborne version Sky− GRIMM, CDP) by assuming Mie theory for homogeneous spherical particles, and by varying the real part of the CRI between 1.33 and 1.75 in steps of 0.01 and the imaginary part between 0.0 and 0.4 in steps of 0.001. Correction factors for mineral dust are provided at the CRI of 1.53 – 0.003i and account for the asphericity of these particles. The datasets described in this paper are distributed at open-access repository: 0.25326/234 (license CC BY, Formenti et al., 2021) maintained by the French national center for Atmospheric data and services AERIS to data users/geophysicists who number size distribution measurements from OPC for their research on atmospheric aerosols. Application and caveats of the CRI-corrections factors are presented and discussed. The dataset presented in this paper is not only useful for correcting the size distribution from an OPC when the particle refractive index is known, but even when only assumptions can be made. Furthermore, this dataset can be useful in calculating uncertainties or sensitivities of aerosol volume/mass/extinction from OPCs given no or limited knowledge of refractive index.
Publisher: Copernicus GmbH
Date: 17-11-2017
DOI: 10.5194/ACP-17-13681-2017
Abstract: Abstract. The SAFIRED (Savannah Fires in the Early Dry Season) c aign 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 c aign 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 c aign, 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 s ling site and provide an overview of the more specific outcomes of the SAFIRED c aign.
Publisher: American Meteorological Society
Date: 04-2023
Abstract: Earth system models struggle to simulate clouds and their radiative effects over the Southern Ocean, partly due to a lack of measurements and targeted cloud microphysics knowledge. We have evaluated biases of downwelling shortwave radiation in the ERA5 climate reanalysis using 25 years (1995–2019) of summertime surface measurements, collected on the Research and Supply Vessel (RSV) Aurora Australis , the Research Vessel (R/V) Investigator , and at Macquarie Island. During October–March daylight hours, the ERA5 simulation of SW down exhibited large errors (mean bias = 54 W m −2 , mean absolute error = 82 W m −2 , root-mean-square error = 132 W m −2 , and R 2 = 0.71). To determine whether we could improve these statistics, we bypassed ERA5’s radiative transfer model for SW down with machine learning–based models using a number of ERA5’s gridscale meteorological variables as predictors. These models were trained and tested with the surface measurements of SW down using a 10-fold shuffle split. An extreme gradient boosting (XGBoost) and a random forest–based model setup had the best performance relative to ERA5, both with a near complete reduction of the mean bias error, a decrease in the mean absolute error and root-mean-square error by 25% ± 3%, and an increase in the R 2 value of 5% ± 1% over the 10 splits. Large improvements occurred at higher latitudes and cyclone cold sectors, where ERA5 performed most poorly. We further interpret our methods using Shapley additive explanations. Our results indicate that data-driven techniques could have an important role in simulating surface radiation fluxes and in improving reanalysis products. Simulating the amount of sunlight reaching Earth’s surface is difficult because it relies on a good understanding of how much clouds absorb and scatter sunlight. Relative to summertime surface observations, the ERA5 reanalysis still overestimates the amount of sunlight entering the Southern Ocean. We taught some models how to predict the amount of sunlight entering the Southern Ocean using 25 years of surface observations and a small set of meteorological variables from ERA5. By bypassing the ERA5’s internal simulation of the absorption and scattering of sunlight, we can drastically reduce biases in the predicted surface shortwave radiation. Large improvements in cold sectors of cyclones and closer to Antarctica were observed in regions where many numerical models struggle to simulate the amount of incoming sunlight correctly.
Publisher: American Meteorological Society
Date: 04-2021
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 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 R/V 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 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, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals 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.
Publisher: Copernicus GmbH
Date: 25-07-2023
DOI: 10.5194/EGUSPHERE-2023-531
Abstract: Abstract. 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 in idual 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.
Publisher: University of California Press
Date: 2022
DOI: 10.1525/ELEMENTA.2021.00050
Abstract: This commentary paper from the recently formed International Global Atmospheric Chemistry (IGAC) Southern Hemisphere Working Group outlines key issues in atmospheric composition research that particularly impact the Southern Hemisphere. In this article, we present a broad overview of many of the challenges for understanding atmospheric chemistry in the Southern Hemisphere, before focusing in on the most significant factors that differentiate it from the Northern Hemisphere. We present sections on the importance of biogenic emissions and fires in the Southern Hemisphere, showing that these emissions often dominate over anthropogenic emissions in many regions. We then describe how these and other factors influence air quality in different parts of the Southern Hemisphere. Finally, we describe the key role of the Southern Ocean in influencing atmospheric chemistry and conclude with a description of the aims and scope of the newly formed IGAC Southern Hemisphere Working Group.
Publisher: Elsevier BV
Date: 2021
Publisher: Copernicus GmbH
Date: 15-12-2021
Publisher: Elsevier BV
Date: 08-2016
DOI: 10.1016/J.SCITOTENV.2016.04.036
Abstract: Prescribed burnings are conducted in Queensland each year from August until November aiming to decrease the impact of bushfire hazards and maintain the health of vegetation. This study reports chemical characteristics of the ambient aerosol, with a focus on source apportionment of the organic aerosol (OA) fraction, during the prescribed biomass burning (BB) season in Brisbane 2013. All measurements were conducted within the International Laboratory for Air Quality and Health (ILAQH) located in Brisbane's Central Business District. Chemical composition, degree of ageing and the influence of BB emission on the air quality of central Brisbane were characterized using a compact Time of Flight Aerosol Mass Spectrometer (cToF-AMS). AMS loadings were dominated by OA (64%), followed by, sulfate (17%), ammonium (14%) and nitrates (5%). Source apportionment was applied on the AMS OA mass spectra via the multilinear engine solver (ME-2) implementation within the recently developed Source Finder (SoFi) interface. Six factors were extracted including hydrocarbon-like OA (HOA), cooking-related OA (COA), biomass burning OA (BBOA), low-volatility oxygenated OA (LV-OOA), semivolatile oxygenated OA (SV-OOA), and nitrogen-enriched OA (NOA). The aerosol fraction that was attributed to BB factor was 9%, on average over the s ling period. The high proportion of oxygenated OA (72%), typically representing aged emissions, could possess a fraction of oxygenated species transfored from BB components on their way to the s ling site.
Publisher: American Geophysical Union (AGU)
Date: 22-06-2016
DOI: 10.1002/2016JD024966
Publisher: Copernicus GmbH
Date: 14-10-2016
DOI: 10.5194/ACP-16-12829-2016
Abstract: Abstract. 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) c aign 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.
Publisher: Copernicus GmbH
Date: 10-03-2023
DOI: 10.5194/EGUSPHERE-2023-349
Abstract: Abstract. 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 utilise 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 underestimation of cloud fraction. The associated biases in cloud occurrence are less clear and we suggest that modelled 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.
Publisher: AIP
Date: 2013
DOI: 10.1063/1.4803329
Publisher: Copernicus GmbH
Date: 19-04-2022
DOI: 10.5194/ACP-2022-259
Abstract: Abstract. 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 frequency and phase. In this work, we use k-means cloud clustering, combined with nudged simulations of the latest generation ACCESS atmosphere model, to evaluate cloud and radiation biases when cloud types are correctly and incorrectly simulated. We find that even if the ACCESS model correctly simulates the cloud type, biases of equivalent, or in some cases greater, magnitude then when they are incorrectly simulated remain in the cloud and radiation fields examined. 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.
Publisher: Copernicus GmbH
Date: 03-09-2019
DOI: 10.5194/ACP-19-11123-2019
Abstract: Abstract. Measurements of aerosol composition and size distributions were taken during the summer of 2013 at the remote island of L edusa 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 c aign (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 c aign. Even though L edusa 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 c aign 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.
Publisher: Copernicus GmbH
Date: 14-03-2017
Abstract: Abstract. 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 c aign 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.
Publisher: American Meteorological Society
Date: 07-2019
Abstract: The Aerosol, Radiation and Clouds in southern Africa (AEROCLO-sA) project investigates the role of aerosols on the regional climate of southern Africa. This is a unique environment where natural and anthropogenic aerosols and a semipermanent and widespread stratocumulus (Sc) cloud deck are found. The project aims to understand the dynamical, chemical, and radiative processes involved in aerosol–cloud–radiation interactions over land and ocean and under various meteorological conditions. The AEROCLO-sA field c aign was conducted in August and September of 2017 over Namibia. An aircraft equipped with active and passive remote sensors and aerosol in situ probes performed a total of 30 research flight hours. In parallel, a ground-based mobile station with state-of-the-art in situ aerosol probes and remote sensing instrumentation was implemented over coastal Namibia, and complemented by ground-based and balloonborne observations of the dynamical, thermodynamical, and physical properties of the lower troposphere. The focus laid on mineral dust emitted from salty pans and ephemeral riverbeds in northern Namibia, the advection of biomass-burning aerosol plumes from Angola subsequently transported over the Atlantic Ocean, and aerosols in the marine boundary layer at the ocean–atmosphere interface. This article presents an overview of the AEROCLO-sA field c aign with results from the airborne and surface measurements. These observations provide new knowledge of the interactions of aerosols and radiation in cloudy and clear skies in connection with the atmospheric dynamics over southern Africa. They will foster new advanced climate simulations and enhance the capability of spaceborne sensors, ultimately allowing a better prediction of future climate and weather in southern Africa.
Publisher: University of California Press
Date: 2023
DOI: 10.1525/ELEMENTA.2022.00130
Abstract: Polar environments are among the fastest changing regions on the planet. It is a crucial time to make significant improvements in our understanding of how ocean and ice biogeochemical processes are linked with the atmosphere. This is especially true over Antarctica and the Southern Ocean where observations are severely limited and the environment is far from anthropogenic influences. In this commentary, we outline major gaps in our knowledge, emerging research priorities, and upcoming opportunities and needs. We then give an overview of the large-scale measurement c aigns planned across Antarctica and the Southern Ocean in the next 5 years that will address the key issues. Until we do this, climate models will likely continue to exhibit biases in the simulated energy balance over this delicate region. Addressing these issues will require an international and interdisciplinary approach which we hope to foster and facilitate with ongoing community activities and collaborations.
Publisher: American Geophysical Union (AGU)
Date: 03-06-2202
DOI: 10.1029/2021GL097538
Abstract: Large ash plumes emitted by the 2019–2020 Australian wildfires were associated with a widespread phytoplankton bloom in the iron‐limited Pacific sector of the Southern Ocean. In this study, we used satellite observations and aerosol reanalysis products to study the regional phytoplankton community response to wildfire emissions. The bloom was stimulated by pyrogenic iron fertilization and coincided with elevated cellular pigment concentrations, increased photochemical efficiency, and apparent community structural shifts. Physiological anomalies were consistent with previously observed phytoplankton responses to iron stress relief and persisted for up to 9 months. Supported by a regional iron budget, we conclude that the bloom was sustained by iron recycling and episodic inputs of pyrogenic and dust‐borne mineral iron. The continuous regeneration of iron was likely facilitated by the bloom's large size, mitigating edge dilution effects, as well as enhanced bioavailability of pyrogenic and mineral iron due to atmospheric and chemical processing during long‐range transport.
Publisher: Queensland University of Technology
Publisher: Springer Science and Business Media LLC
Date: 02-03-2020
Publisher: Copernicus GmbH
Date: 17-11-2022
DOI: 10.5194/ACP-22-14603-2022
Abstract: Abstract. 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.
Publisher: American Geophysical Union (AGU)
Date: 10-06-2017
DOI: 10.1002/2016JD025925
Publisher: Copernicus GmbH
Date: 09-07-2020
Abstract: 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 s led 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 s les 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.
Publisher: American Chemical Society (ACS)
Date: 18-01-2016
Abstract: The emission factors (EFs) for a broad range of semivolatile organic chemicals (SVOCs) from subtropical eucalypt forest and tropical savannah fires were determined for the first time from in situ investigations. Significantly higher (t test, P < 0.01) EFs (μg kg
Publisher: Copernicus GmbH
Date: 24-07-2018
Abstract: Abstract. Internally and externally mixed aerosols present significant challenges in assessing the hygroscopicity of each aerosol component. This study presents a new s ling 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 erse 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.
Publisher: American Geophysical Union (AGU)
Date: 20-05-2022
DOI: 10.1029/2022GL098770
Abstract: Marine ecosystems are important drivers of the global climate system. They emit volatile species into the atmosphere, involved in complex reaction cycles that influence the lifetime of greenhouse gases. Sea spray and marine biogenic aerosols affect Earth's climate by scattering solar radiation and controlling cloud microphysical properties. Here we show larger than expected marine biogenic emissions of butenes, three orders of magnitude higher than dimethyl sulfide, produced by the coastal part of the Benguela upwelling system, one of the most productive marine ecosystems in the world. We show that these emissions may contribute to new particle formation in the atmosphere within the marine boundary layer through production of Criegee intermediates that oxidize SO 2 to H 2 SO 4 . Butene emissions from the marine biota may affect air quality and climate through ozone, secondary organic aerosol, and cloud condensation nuclei formation even in pristine regions of the world. Our results indicate a potentially important role of butene emissions in marine particle formation that requires investigation in other regions.
Start Date: 07-2022
End Date: 12-2023
Amount: $328,389.00
Funder: Australian Research Council
View Funded ActivityStart Date: 2023
End Date: 12-2023
Amount: $831,200.00
Funder: Australian Research Council
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