School of Earth Sciences - Research Publications

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    Characterization of aerosols over the Great Barrier Reef: The influence of transported continental sources
    Chen, Z ; Schofield, R ; Rayner, P ; Zhang, T ; Liu, C ; Vincent, C ; Fiddes, S ; Ryan, RG ; Alroe, J ; Ristovski, ZD ; Humphries, RS ; Keywood, MD ; Ward, J ; Paton-Walsh, C ; Naylor, T ; Shu, X (ELSEVIER, 2019-11-10)
    The rapid environmental changes in Australia prompt a more thorough investigation of the influence of transportation, local emissions, and optical-chemical properties on aerosol production across the region. A month-long intensive measurement campaign was conducted during spring 2016 at Mission Beach, a remote coastal site west of the Great Barrier Reef (GBR) on the north-east coast of Australia. One aerosol pollution episode was investigated in early October. This event was governed by meteorological conditions and characterized by the increase in black carbon (BC) mass concentration (averaged value of 0.35 ± 0.20 μg m-3). Under the influence of the continental transportation, a new layer of nucleation-mode aerosols with an initial size diameter of 20 nm was observed and aerosol number concentrations reached the peak of 6733 cm-3 at a diameter of 29 nm. The averaged aerosol extinction coefficient at the height of 2 km was 150 Mm-1, with a small depolarized ratio (3.5-5%). Simultaneously, the boundary layer height presented a fall-rise trend in the presence of these enhanced aerosol concentrations and became stable in a later stage of the episode. We did not observe clear boundary layer height diurnal variations from the LiDAR observations or from the Weather Research and Forecasting (WRF) model outputs, except in an earlier stage of the aerosol episode for the former. Although the sea breeze may have been responsible for these particles, on the balance of available data, we suggest that the aerosol properties at the GBR surface during this period are more likely influenced by regional transportation of continental sources, including biomass-burning aerosols.
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    The Antarctic ozone hole during 2013
    Klekociuk, AR ; Krummel, PB ; Tully, MB ; Gies, HP ; Alexander, SP ; Fraser, PJ ; Henderson, SI ; Javorniczky, J ; Shanklin, JD ; Schofield, R ; Stone, KA (Australian Bureau of Meteorology, 2015-01-01)
    We review the 2013 Antarctic ozone hole, making use of various ground-based, in-situ and remotely-sensed ozone measurements, ground-based measurements of ultraviolet radiation and meteorological reanalyses. Based on analysis of 34 years of satellite records spanning 1979-2013 (which excludes 1995), we find that in terms of maximum area, minimum ozone level and total ozone deficit, the ozone hole in 2013 was typical of other years of moderate ozone loss. The estimated integrated ozone mass effectively depleted within the ozone hole of 2013 was approximately 1037 Mt, which was the 17th largest deficit on record and 41% of the peak deficit observed in 2006. Anomalously cold winter temper-atures in the lower stratosphere over Antarctica and concurrent strong and stable vortex conditions favoured the potential for strong ozone depletion in 2013. However, anomalous warming of the polar vortex that occurred from late Au-gust limited the overall severity of ozone depletion during spring, and resulted in the relatively early breakup of the ozone hole in mid-November.
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    A new Dobson Umkehr ozone profile retrieval method optimising information content and resolution
    Stone, K ; Tully, MB ; Rhodes, SK ; Schofield, R (European Geosciences Union, 2015-03-04)
    The standard Dobson Umkehr methodology to retrieve coarse-resolution ozone profiles used by the National Oceanographic and Atmospheric Administration uses designated solar zenith angles (SZAs). However, some information may be lost if measurements lie outside the designated SZA range (between 60° and 90°), or do not conform to the fitting technique. Also, while Umkehr measurements can be taken using multiple wavelength pairs (A, C and D), past retrieval methods have focused on a single pair (C). Here we present an Umkehr inversion method that uses measurements at all SZAs (termed operational) and all wavelength pairs. (Although, we caution direct comparison to other algorithms.) Information content for a Melbourne, Australia (38° S, 145° E) Umkehr measurement case study from 28 January 1994, with SZA range similar to that designated in previous algorithms is shown. When comparing the typical single wavelength pair with designated SZAs to the operational measurements, the total degrees of freedom (independent pieces of information) increases from 3.1 to 3.4, with the majority of the information gain originating from Umkehr layers 2 + 3 and 4 (10-20 km and 25-30 km respectively). In addition to this, using all available wavelength pairs increases the total degrees of freedom to 5.2, with the most significant increases in Umkehr layers 2 + 3 to 7 and 9+ (10-40 and 45-80 km). Investigating a case from 13 April 1970 where the measurements extend beyond the 90° SZA range gives further information gain, with total degrees of freedom extending to 6.5. Similar increases are seen in the information content. Comparing the retrieved Melbourne Umkehr time series with ozonesondes shows excellent agreement in layers 2 + 3 and 4 (10-20 and 25-30 km) for both C and A + C + D-pairs. Retrievals in layers 5 and 6 (25-30 and 30-35 km) consistently show lower ozone partial column compared to ozonesondes. This is likely due to stray light effects that are not accounted for in the forward model, and under represented stratospheric aerosol.
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    Cloud, precipitation and radiation responses to large perturbations in global dimethyl sulfide
    Fiddes, SL ; Woodhouse, MT ; Nicholls, Z ; Lane, TP ; Schofield, R (Copernicus Publications, 2018)
    Natural aerosol emission represents one of the largest uncertainties in our understanding of the radiation budget. Sulfur emitted by marine organisms, as dimethyl sulfide (DMS), constitutes one-fifth of the global sulfur budget and yet the distribution, fluxes and fate of DMS remain poorly constrained. This study evaluates the Australian Community Climate and Earth System Simulator (ACCESS) United Kingdom Chemistry and Aerosol (UKCA) model in terms of cloud fraction, radiation and precipitation, and then quantifies the role of DMS in the chemistry–climate system. We find that ACCESS-UKCA has similar cloud and radiation biases to other global climate models. By removing all DMS, or alternatively significantly enhancing marine DMS, we find a top of the atmosphere radiative effect of 1.7 and −1.4W m−2 respectively. The largest responses to these DMS perturbations (removal/enhancement) are in stratiform cloud decks in the Southern Hemisphere's eastern ocean basins. These regions show significant differences in low cloud (−9∕ + 6%), surface incoming shortwave radiation (+7∕ − 5W m−2) and large-scale rainfall (+15∕ − 10%). We demonstrate a precipitation suppression effect of DMS-derived aerosol in stratiform cloud deck regions due to DMS, coupled with an increase in low cloud fraction. The difference in low cloud fraction is an example of the aerosol lifetime effect. Globally, we find a sensitivity of temperature to annual DMS flux of 0.027 and 0.019K per Tg yr−1 of sulfur, respectively. Other areas of low cloud formation, such as the Southern Ocean and stratiform cloud decks in the Northern Hemisphere, have a relatively weak response to DMS perturbations. We highlight the need for greater understanding of the DMS–climate cycle within the context of uncertainties and biases of climate models as well as those of DMS–climate observations.
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    Evaluation of the ACCESS - chemistry-climate model for the Southern Hemisphere
    Stone, KA ; Morgenstern, O ; Karoly, DJ ; Klekociuk, AR ; French, WJ ; Abraham, NL ; Schofield, R (Copernicus Publications, 2016-01-01)
    Chemistry–climate models are important tools for addressing interactions of composition and climate in the Earth system. In particular, they are used to assess the combined roles of greenhouse gases and ozone in Southern Hemisphere climate and weather. Here we present an evaluation of the Australian Community Climate and Earth System Simulator – chemistry–climate model (ACCESS-CCM), focusing on the Southern Hemisphere and the Australian region. This model is used for the Australian contribution to the international Chemistry–Climate Model Initiative, which is soliciting hindcast, future projection and sensitivity simulations. The model simulates global total column ozone (TCO) distributions accurately, with a slight delay in the onset and recovery of springtime Antarctic ozone depletion, and consistently higher ozone values. However, October-averaged Antarctic TCO from 1960 to 2010 shows a similar amount of depletion compared to observations. Comparison with model precursors shows large improvements in the representation of the Southern Hemisphere stratosphere, especially in TCO concentrations. A significant innovation is seen in the evaluation of simulated vertical profiles of ozone and temperature with ozonesonde data from Australia, New Zealand and Antarctica from 38 to 90° S. Excess ozone concentrations (greater than 26 % at Davis and the South Pole during winter) and stratospheric cold biases (up to 10 K at the South Pole during summer and autumn) outside the period of perturbed springtime ozone depletion are seen during all seasons compared to ozonesondes. A disparity in the vertical location of ozone depletion is seen: centred around 100 hPa in ozonesonde data compared to above 50hPa in the model. Analysis of vertical chlorine monoxide profiles indicates that colder Antarctic stratospheric temperatures (possibly due to reduced mid-latitude heat flux) are artificially enhancing polar stratospheric cloud formation at high altitudes. The model's inability to explicitly simulate a supercooled ternary solution may also explain the lack of depletion at lower altitudes. Analysis of the simulated Southern Annular Mode (SAM) index compares well with ERA-Interim data, an important metric for correct representation of Australian climate. Accompanying these modulations of the SAM, 50 hPa zonal wind differences between 2001–2010 and 1979–1998 show increasing zonal wind strength southward of 60° S during December for both the model simulations and ERA-Interim data. These model diagnostics show that the model reasonably captures the stratospheric ozone-driven chemistry–climate interactions important for Australian climate and weather while highlighting areas for future model development.
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    A case study of a transported bromine explosion event in the Canadian High Arctic
    Zhao, X ; Strong, K ; Adams, C ; Schofield, R ; Yang, X ; Richter, A ; Friess, U ; Blechschmidt, AM ; Koo, JH (American Geophysical Union, 2016-01-16)
    Ozone depletion events in the polar troposphere have been linked to extremely high concentrations of bromine, known as bromine explosion events (BEE). However, the optimum meteorological conditions for the occurrence of these events remain uncertain. On 4–5 April 2011, a combination of both blowing snow and a stable shallow boundary layer was observed during a BEE at Eureka, Canada (86.4°W, 80.1°N). Measurements made by a Multi-Axis Differential Optical Absorption Spectroscopy spectrometer were used to retrieve BrO profiles and partial columns. During this event, the near-surface BrO volume mixing ratio increased to ~20 parts per trillion by volume, while ozone was depleted to ~1 ppbv from the surface to 700 m. Back trajectories and Global Ozone Monitoring Experiment-2 satellite tropospheric BrO columns confirmed that this event originated from a bromine explosion over the Beaufort Sea. From 30 to 31 March, meteorological data showed high wind speeds (24 m/s) and elevated boundary layer heights (~800 m) over the Beaufort Sea. Long-distance transportation (~1800 km over 5 days) to Eureka indicated strong recycling of BrO within the bromine plume. This event was generally captured by a global chemistry-climate model when a sea-salt bromine source from blowing snow was included. A model sensitivity study indicated that the surface BrO at Eureka was controlled by both local photochemistry and boundary layer dynamics. Comparison of the model results with both ground-based and satellite measurements confirmed that the BEE observed at Eureka was triggered by transport of enhanced BrO from the Beaufort Sea followed by local production/recycling under stable atmospheric shallow boundary layer conditions.
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    The Antarctic ozone hole during 2012
    Klekociuk, AR ; Tully, MB ; Krummel, PB ; Gies, HP ; Alexander, SP ; Fraser, PJ ; Henderson, SI ; Javorniczky, J ; Petelina, SV ; Shanklin, JD ; Schofield, R ; Stone, KA (AUSTRALIAN BUREAU METEOROLOGY, 2014-01-01)
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    Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice
    Humphries, RS ; Klekociuk, AR ; Schofield, R ; Keywood, M ; Ward, J ; Wilson, SR (Copernicus GmBH, 2016-02-25)
    Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm-3-higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of cloud and aerosol over the Southern Ocean.
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    Update on Polar Ozone: Past, Present, and Future
    Dameris, M ; Godin-Beekmann, S ; Alexander, S ; Braesicke, P ; Chipperfield, M ; de Laat, ATJ ; Orsolini, Y ; Rex, M ; Santee, ML ; van der A, R ; Cionni, I ; Dhomse, S ; Diaz, S ; Engel, I ; von der Gathen, P ; Grooß, J-U ; Hassler, B ; Horowitz, L ; Kreher, K ; Kunze, M ; Langematz, U ; Manney, GL ; Müller, R ; Pitari, G ; Pitts, M ; Poole, L ; SCHOFIELD, R ; Tilmes, S ; Weber, M ; Bekki, S ; Perlwitz, J (World Meteorological Organization, 2014)
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    Scenarios, information, and options for policymakers
    Harris, NPR ; Wuebbles, DJ ; Daniel, JS ; Hu, J ; Kuijpers, LJM ; Law, KS ; Prather, MJ ; SCHOFIELD, R ; Fleming, EL ; Hossaini, R ; Jackman, CH ; Phoenix, D ; McFarland, M ; Velders, GJM (World Meteorological Organization, 2014)