ORCID Profile
0000-0002-4230-717X
Current Organisation
University of Melbourne
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Research Topics
In Research Link Australia (RLA), "Research Topics" refer to ANZSRC FOR and SEO codes. These topics are either sourced from ANZSRC FOR and SEO codes listed in researchers' related grants or generated by a large language model (LLM) based on their publications.
Top 5 Research Topics
ANZSRC Field of Research (FoR)
Atmospheric Sciences | Atmospheric Aerosols | Physical Oceanography | Climate Change Processes | Environmental Chemistry (incl. Atmospheric Chemistry) | Atmospheric Sciences not elsewhere classified | Systems engineering | Engineering practice and education | Transport Planning | Environmentally sustainable engineering | Building science technologies and systems | Atmospheric sciences | Atmospheric Dynamics | Glaciology | Urban Analysis and Development | Urban Design | Cloud Physics | Other Chemical Sciences | Air pollution processes and air quality measurement | Atmospheric aerosols | Urban and Regional Planning | Atmospheric composition chemistry and processes | Maritime Engineering | Ocean Engineering |
ANZSRC Socio-Economic Objective (SEO)
Atmospheric Composition (incl. Greenhouse Gas Inventory) | Atmospheric Processes and Dynamics | Climate Change Models | Effects of Climate Change and Variability on Antarctic and Sub-Antarctic Environments (excl. Social Impacts) | Ecosystem Adaptation to Climate Change | Urban and Industrial Air Quality | Antarctic and Sub-Antarctic Air Quality | Antarctic and Sub-Antarctic Oceanography | Expanding Knowledge in Built Environment and Design | Air Quality not elsewhere classified | Expanding Knowledge in the Environmental Sciences | Expanding Knowledge in the Information and Computing Sciences | Road Infrastructure and Networks | Environmentally Sustainable Transport not elsewhere classified
Related Links
Publications
Characterization of aerosols over the Great Barrier Reef: The influence of transported continental sources
Publisher: Elsevier BV
Date: 11-2019
DOI: 10.1016/J.SCITOTENV.2019.07.007
Abstract: 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 c aign 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
Intercomparison exercise between different radiative transfer models used for the interpretation of ground-based zenith-sky and multi-axis DOAS observations
Publisher: Copernicus GmbH
Date: 20-01-2006
Abstract: Abstract. We present the results of an intercomparison exercise between six different radiative transfer (RT) models carried out in the framework of QUILT, an EU funded project based on the exploitation of the Network for the Detection of Stratospheric Change (NDSC). RT modelling is an important step in the interpretation of Differential Optical Absorption Spectroscopy (DOAS) observations. It allows the conversion of slant column densities (SCDs) into vertical column densities (VCDs) using calculated air mass factors (AMFs). The originality of our study resides in comparing SCD simulations in multi-axis (MAX) geometry (trace gases: NO2 and HCHO) and in taking into account photochemical enhancement for calculating SCDs of rapidly photolysing species (BrO, NO2, and OClO) in zenith-sky geometry. Concerning the zenith-sky simulations, the different models agree generally well, especially below 90° SZA. At higher SZA, larger discrepancies are obtained with relative differences ranging between 2% and 14% in some cases. In MAX geometry, good agreement is found between the models with the calculated NO2 and HCHO SCDs differing by no more than 5% in the elevation and solar zenith angle (SZA) ranges investigated (5°–20° and 35°–85°, respectively). The impacts of aerosol scattering, ground albedo, and relative azimuth on MAX simulations have also been tested. Significant discrepancies appear for the aerosol effect, suggesting differences between models in the treatment of aerosol scattering. A better agreement is found in case of the ground albedo and relative azimuth effects. The complete set of initialization data and results have been made publicly available through the QUILT project web site (nadir.nilu.no/quilt/), enabling the testing of other RT codes designed for the calculation of SCDs/AMFs.
Measurement Report: Real-Time Remote Sensing of the Coastal Boundary Layer and its Interaction with Meteorology at Cape Grim, Australia
Publisher: Copernicus GmbH
Date: 09-03-2022
DOI: 10.5194/ACP-2022-104
Abstract: Abstract. Despite considerable efforts during the last decade, real-time characterization of the marine boundary layer and aerosol optical properties over the Southern Ocean remains scarce. We conducted simultaneous measurements of the marine boundary layer utilizing a synergy of remote sensing technology at the Baseline Air Pollution Station at Cape Grim in northwestern Tasmania, Australia, from 14 May to 16 July 2019. Aerosol optical properties were monitored by lidar (miniMPL) and a ceilometer to identify the boundary layer height, and sodar provided wind profiles to investigate their influences on the layer evolution. Boundary layer heights simulated using the Weather Research and Forecasting (WRF) model were also employed for comparison purposes. Through complementary analyses of three cases representing different source influences (marine, sea breeze and continental), this paper evaluates two algorithms (Image Edge Detection Algorithm (IEDA) and gradient method) for boundary layer height detection and examines the vertical aerosol distribution within the boundary layer at Cape Grim with an emphasis on the contributions of regional and local meteorology. We found IEDA generally performed better than the gradient method, especially during the marine-flow-influenced period with a convective layer structure. Different features of boundary layer structures in three episodes, including differential boundary layer growth and interaction with wind evolutionary processes were investigated. One was characterized by a diurnal variation with a boundary layer height of approximately 0.2–0.5 km, associated with the veering of the wind vector within the marine boundary layer during the development of a sea breeze. The other showed a thermally stable layer below 0.3 km with an enhanced extinction coefficient and linear depolarization ratio under the influence of continental sources, which was also validated by the observation from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite. The increasing extinction coefficient and depolarization ratio with wind speeds may be attributed to the increased wet sea salt production and regional transportation from mainland Australia.
Coral reef-derived dimethyl sulfide and the climatic impact of the loss of coral reefs
Publisher: Copernicus GmbH
Date: 27-10-2020
Abstract: Abstract. Dimethyl sulfide (DMS) is a naturally occurring aerosol precursor gas which plays an important role in the global sulfur budget, aerosol formation and climate. While DMS is produced predominantly by phytoplankton, recent observational literature has suggested that corals and their symbionts produce a comparable amount of DMS, which is unaccounted for in models. It has further been hypothesised that the coral reef source of DMS may modulate regional climate. This hypothesis presents a particular concern given the current threat to coral reefs under anthropogenic climate change. In this paper, a global climate model with online chemistry and aerosol is used to explore the influence of coral reef-derived DMS on atmospheric composition and climate. A simple representation of coral reef-derived DMS is developed and added to a common DMS surface water climatology, resulting in an additional DMS flux of 0.3 Tg year−1 S, or 1.7 % of the global flux. By comparing the differences between both nudged and free running ensemble simulations with and without coral reef-derived DMS, the influence of coral reef-derived DMS on regional climate is quantified. In the Maritime Continent-Australian region, where the highest density of coral reefs exist, a small decrease in nucleation and Aitken mode aerosol number concentration and mass is found when coral reef DMS emissions are removed from the system. However, these small responses are found to have no robust effect on regional climate via direct and indirect aerosol effects. This work emphasises the complexities of the aerosol-climate system and the limitations of current modelling capabilities are highlighted, in particular surrounding convective responses to changes in aerosol. In conclusion we find no robust evidence that coral reef-derived DMS influences global and regional climate.
Measurement report: Understanding the seasonal cycle of Southern Ocean aerosols
Publisher: Copernicus GmbH
Date: 29-03-2023
Abstract: Abstract. 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.
Large-scale transport into the Arctic: the roles of the midlatitude jet and the Hadley Cell
Publisher: Copernicus GmbH
Date: 26-04-2019
Abstract: Abstract. Transport from the Northern Hemisphere (NH) midlatitudes to the Arctic plays a crucial role in determining the abundance of trace gases and aerosols that are important to Arctic climate via impacts on radiation and chemistry. Here we examine this transport using an idealized tracer with a fixed lifetime and predominantly midlatitude land-based sources in models participating in the Chemistry Climate Model Initiative (CCMI). We show that there is a 25 %–45 % difference in the Arctic concentrations of this tracer among the models. This spread is correlated with the spread in the location of the Pacific jet, as well as the spread in the location of the Hadley Cell (HC) edge, which varies consistently with jet latitude. Our results suggest that it is likely that the HC-related zonal-mean meridional transport rather than the jet-related eddy mixing is the major contributor to the inter-model spread in the transport of land-based tracers into the Arctic. Specifically, in models with a more northern jet, the HC generally extends further north and the tracer source region is mostly covered by surface southward flow associated with the lower branch of the HC, resulting in less efficient transport poleward to the Arctic. During boreal summer, there are poleward biases in jet location in free-running models, and these models likely underestimate the rate of transport into the Arctic. Models using specified dynamics do not have biases in the jet location, but do have biases in the surface meridional flow, which may result in differences in transport into the Arctic. In addition to the land-based tracer, the midlatitude-to-Arctic transport is further examined by another idealized tracer with zonally uniform sources. With equal sources from both land and ocean, the inter-model spread of this zonally uniform tracer is more related to variations in parameterized convection over oceans rather than variations in HC extent, particularly during boreal winter. This suggests that transport of land-based and oceanic tracers or aerosols towards the Arctic differs in pathways and therefore their corresponding inter-model variabilities result from different physical processes.
Sulfur dioxide emission flux measurements from point sources using airborne near ultraviolet spectroscopy during the New England Air Quality Study 2004
Publisher: American Geophysical Union (AGU)
Date: 23-01-2008
DOI: 10.1029/2007JD008923
Atmospheric goals for sustainable development.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 20-01-2023
Daytime HONO, NO<sub>2</sub> and aerosol distributions from MAX-DOAS observations in Melbourne
Publisher: Copernicus GmbH
Date: 02-10-2018
DOI: 10.5194/ACP-18-13969-2018
Abstract: Abstract. Toxic nitrogen oxides produced by high temperature combustion are prevalent in urban environments, contributing to a significant health burden. Nitrogen oxides such as NO2 and HONO in pollution are important for hydroxyl radical (OH) production and overall oxidative capacity in urban environments however, current mechanisms cannot explain high daytime levels of HONO observed in many urban and rural locations around the world. Here we present HONO, NO2 and aerosol extinction vertical distributions retrieved from multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements in suburban Melbourne, which are the first MAX-DOAS results from the Australian continent. Using the optimal estimation algorithm HEIPRO we show that vertical profiles for NO2 and HONO can be calculated with a low dependence on the retrieval forward model and a priori parameters, despite a lack of independent co-located aerosol or trace gas measurements. Between December 2016 and April 2017 average peak NO2 values of 8±2 ppb indicated moderate traffic pollution levels, and high daytime peak values of HONO were frequently detected, averaging 220±30 ppt in the middle of the day. HONO levels measured in Melbourne were typically lower than those recorded in the morning in other places around the world, indicating minimal overnight accumulation, but peaked in the middle of the day to be commensurate with midday concentrations in locations with much higher NO2 pollution. Regular midday peaks in the diurnal cycle of HONO surface concentrations have only previously been reported in rural locations. The HONO measured implies a daytime source term 1 ppb h−1 above the predicted photostationary state (PSS) concentration and represents an OH radical source up to 4 times stronger than from ozone photolysis alone in the lowest 500 m of the troposphere. The dependence of the high midday HONO levels on soil moisture, combined with the observed diurnal and vertical profiles, provides evidence for a strong photoactivated and ground-based daytime HONO source.
Review of the global models used within phase 1 of the Chemistry–Climate Model Initiative (CCMI)
Publisher: Copernicus GmbH
Date: 13-02-2017
Abstract: Abstract. We present an overview of state-of-the-art chemistry–climate and chemistry transport models that are used within phase 1 of the Chemistry–Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.
Hourly emission inventories for air toxic emissions for eastern Australian electricity generators derived from energy distribution data
Publisher: Springer Science and Business Media LLC
Date: 21-06-2021
Atmospheric mercury in the Latrobe Valley, Australia: Case study June 2013
Publisher: University of California Press
Date: 2021
DOI: 10.1525/ELEMENTA.2021.00072
Abstract: Gaseous elemental mercury observations were conducted at Churchill, Victoria, in Australia from April to July, 2013, using a Tekran 2537 analyzer. A strong diurnal variation with daytime average values of 1.2–1.3 ng m–3 and nighttime average values of 1.6–1.8 ng m–3 was observed. These values are significantly higher than the Southern Hemisphere average of 0.85–1.05 ng m–3. Churchill is in the Latrobe Valley, approximately 150 km East of Melbourne, where approximately 80% of Victoria’s electricity is generated from low-rank brown coal from four major power stations: Loy Yang A, Loy Yang B, Hazelwood, and Yallourn. These aging generators do not have any sulfur, nitrogen oxide, or mercury air pollution controls. Mercury emitted in the 2015–2016 year in the Latrobe Valley is estimated to have had an externalized health cost of $AUD88 million. Air pollution mercury simulations were conducted using the Weather Research and Forecast model with Chemistry at 3 × 3 km resolution. Electrical power generation emissions were added using mercury emissions created from the National Energy Market’s 5-min energy distribution data. The strong diurnal cycle in the observed mercury was well simulated (R2 = .49 and P value = 0.00) when soil mercury emissions arising from several years of wet and dry deposition in a radius around the power generators was included in the model, as has been observed around aging lignite coal power generators elsewhere. These results indicate that long-term air and soil s ling in power generation regions, even after the closure of coal fired power stations, will have important implications to understanding the airborne mercury emissions sources.
Supplementary material to "Seventeen years of ozone sounding at L'Aquila, Italy: evidence of mid-latitude stratospheric ozone recovery and tropospheric profile changes"
Publisher: Copernicus GmbH
Date: 07-2020
Daytime HONO, NO<sub>2</sub> and aerosol distributions from MAX-DOAS observations in Melbourne
Publisher: Copernicus GmbH
Date: 18-05-2018
DOI: 10.5194/ACP-2018-409
Abstract: Abstract. Nitrogen oxides produced by high temperature combustion are prevalent in urban environments and toxic, contributing to a significant health burden. The chemistry of nitrogen oxides such as NO2 and HONO in pollution are important for hydroxyl radical production and overall oxidative capacity in urban environments, however current mechanisms cannot explain high daytime levels of HONO observed in many urban and rural locations around the world. Here we present HONO, NO2 and aerosol extinction vertical distributions retrieved from MAX-DOAS measurements in suburban Melbourne, which are the first MAX-DOAS results from Australia. Using the optimal estimation algorithm HEIPRO we show that vertical profiles for NO2 and HONO can be calculated with low dependence on the retrieval forward model and a priori parameters, despite a lack of independent co-located aerosol or trace gas measurements. Between December 2016 and April 2017 average peak NO2 values of 8 ± 2 ppb indicated moderate traffic pollution levels, and high daytime peak values of HONO were frequently detected, averaging 220 ± 30 ppt in the middle of the day. HONO levels measured in Melbourne were typically lower than those recorded in the morning in other places around the world, indicating minimal overnight accumulation, but peaked in the middle of the day to be commensurate with midday concentrations in locations with much higher NO2 pollution. Regular midday peaks in the diurnal cycle of HONO surface concentrations have only previously been reported in rural locations. The HONO measured represents an OH radical source in the middle of the day in Melbourne up to ten times stronger than from ozone photolysis. The dependence of the high HONO levels on time since rainfall, combined with the observed diurnal and vertical profiles, provide evidence for a strong photo-activated and ground-based daytime HONO source.
Retrievals of chlorine chemistry kinetic parameters from Antarctic ClO microwave radiometer measurements
Publisher: Copernicus GmbH
Date: 06-2011
Abstract: Abstract. Key kinetic parameters governing the partitioning of chlorine species in the Antarctic polar stratosphere were retrieved from 28 days of chlorine monoxide (ClO) microwave radiometer measurements made during the late winter/early spring of 2005 at Scott Base (77.85° S, 166.75° E). During day-time the loss of the ClO dimer chlorine peroxide (ClOOCl) occurs mainly by photolysis. Some time after sunrise, a photochemical equilibrium is established and the ClO/ClOOCl partitioning is determined by the ratio of the photolysis frequency, J, and the dimer formation rate, kf. The values of J and kf from laboratory studies remain uncertain to a considerable extent, and as a complement to these ongoing studies, the goal of this work is to provide a constraint on that uncertainty based on observations of ClO profiles in the Antarctic. First an optimal estimation technique was used to derive J/kf ratios for a range of Keq values. The optimal estimation forward model was a photochemical box model that takes J, kf, and Keq as inputs, together with a priori profiles of activated chlorine (ClOx = ClO+2×ClOOCl), profiles of ozone, temperature, and pressure. JPL06 kinetics are used as a priori in the optimal estimation and for all other chemistry in the forward model. Using the more recent JPL09 kinetics results in insignificant differences in the retrieved value of J/kf. A complementary approach was used to derive the optimal kinetic parameters the full parameter space of J, kf, Keq and ClOx was s led to find the minimum in differences between measured and modelled ClO profiles. Furthermore, values of Keq up to 2.0 times larger than recommended by JPL06 were explored to test the sensitivity of the J/kf ratio to changes in Keq. The results show that the retrieved J/kf ratios bracket the range of 1.23 to 1.97 times the J/kf value recommended by JPL06 over the range of Keq values considered. The retrieved J/kf ratios lie in the lower half of the large uncertainty range of J/kf recommended by JPL06 and towards the upper portion of the smaller uncertainty range recommended by JPL09.
Use of portable air cleaners to reduce aerosol transmission on a hospital coronavirus disease 2019 (COVID-19) ward
Publisher: Cambridge University Press (CUP)
Date: 24-06-2021
DOI: 10.1017/ICE.2021.284
Abstract: To study the airflow, transmission, and clearance of aerosols in the clinical spaces of a hospital ward that had been used to care for patients with coronavirus disease 2019 (COVID-19) and to examine the impact of portable air cleaners on aerosol clearance. Observational study. A single ward of a tertiary-care public hospital in Melbourne, Australia. Glycerin-based aerosol was used as a surrogate for respiratory aerosols. The transmission of aerosols from a single patient room into corridors and a nurses’ station in the ward was measured. The rate of clearance of aerosols was measured over time from the patient room, nurses’ station and ward corridors with and without air cleaners [ie, portable high-efficiency particulate air (HEPA) filters]. Aerosols rapidly travelled from the patient room into other parts of the ward. Air cleaners were effective in increasing the clearance of aerosols from the air in clinical spaces and reducing their spread to other areas. With 2 small domestic air cleaners in a single patient room of a hospital ward, 99% of aerosols could be cleared within 5.5 minutes. Air cleaners may be useful in clinical spaces to help reduce the risk of acquisition of respiratory viruses that are transmitted via aerosols. They are easy to deploy and are likely to be cost-effective in a variety of healthcare settings.
Ozone sensitivity to varying greenhouse gases and ozone-depleting substances in CCMI-1 simulations
Publisher: Copernicus GmbH
Date: 29-01-2018
Abstract: Abstract. Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in in idual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these in idual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.
First quasi-Lagrangian in situ measurements of Antarctic Polar springtime ozone: observed ozone loss rates from the Concordiasi long-duration balloon campaign
Publisher: Copernicus GmbH
Date: 05-03-2015
Abstract: Abstract. We present ozone measurements made using state-of-the-art ultraviolet photometers onboard three long-duration stratospheric balloons launched as part of the Concordiasi c aign in austral spring 2010. Ozone loss rates calculated by matching air parcels s led at different times and places during the polar spring are in agreement with rates previously derived from ozonesonde measurements, for the vortex average, ranging between 2 and 7 ppbv per sunlit hour or between 25 and 110 ppbv per day. However, the geographical coverage of these long-duration stratospheric balloon platforms provides new insights into the temporal and spatial patterns of ozone loss over Antarctica. Very large ozone loss rates of up to 230 ppbv per day (16 ppbv per sunlit hour) are observed for air masses that are downwind of the Antarctic Peninsula and/or over the East Antarctic region. The ozone loss rate maximum downstream of the Antarctic Peninsula region is consistent with high PSC occurrence from CALIPSO and large ClO abundances from MLS satellite observations for 12–22 September 2010, and with a chemical box model simulation using JPL 2011 kinetics with full chlorine activation.
Quantifying the effect of mixing on the mean age of air in CCMVal-2 and CCMI-1 models
Publisher: Copernicus GmbH
Date: 14-05-2018
Abstract: Abstract. The stratospheric age of air (AoA) is a useful measure of the overall capabilities of a general circulation model (GCM) to simulate stratospheric transport. Previous studies have reported a large spread in the simulation of AoA by GCMs and coupled chemistry–climate models (CCMs). Compared to observational estimates, simulated AoA is mostly too low. Here we attempt to untangle the processes that lead to the AoA differences between the models and between models and observations. AoA is influenced by both mean transport by the residual circulation and two-way mixing we quantify the effects of these processes using data from the CCM inter-comparison projects CCMVal-2 (Chemistry–Climate Model Validation Activity 2) and CCMI-1 (Chemistry–Climate Model Initiative, phase 1). Transport along the residual circulation is measured by the residual circulation transit time (RCTT). We interpret the difference between AoA and RCTT as additional aging by mixing. Aging by mixing thus includes mixing on both the resolved and subgrid scale. We find that the spread in AoA between the models is primarily caused by differences in the effects of mixing and only to some extent by differences in residual circulation strength. These effects are quantified by the mixing efficiency, a measure of the relative increase in AoA by mixing. The mixing efficiency varies strongly between the models from 0.24 to 1.02. We show that the mixing efficiency is not only controlled by horizontal mixing, but by vertical mixing and vertical diffusion as well. Possible causes for the differences in the models' mixing efficiencies are discussed. Differences in subgrid-scale mixing (including differences in advection schemes and model resolutions) likely contribute to the differences in mixing efficiency. However, differences in the relative contribution of resolved versus parameterized wave forcing do not appear to be related to differences in mixing efficiency or AoA.
Large-scale transport into the Arctic: the roles of the midlatitude jet and the Hadley Cell
Publisher: Copernicus GmbH
Date: 30-08-2018
DOI: 10.5194/ACP-2018-841
Abstract: Abstract. Transport from the Northern Hemisphere (NH) midlatitudes to the Arctic plays a crucial role in determining the abundance of trace gases and aerosols that are important to Arctic climate via impacts on radiation and chemistry. Here we examine this transport using an idealized tracer with fixed lifetime and predominantly midlatitude land-based sources in models participating in the Chemistry Climate Model Initiative (CCMI). We show that there is a 20 %–40 % difference in the Arctic concentrations of this tracer among the models. This spread is found to be generally related to the spread in location of the Pacific jet, with lower Arctic tracer concentrations occurring in models with a more northern jet, during both winter and summer. However, the underlying mechanism for this relationship does not involve the jet directly, but instead involves differences in the surface meridional flow over the tracer source region, that vary with jet latitude. Specifically, in models with a more northern jet, the Hadley Cell (HC) generally extends further north and the tracer source region is mostly covered by surface southward flow associated with the lower branch of the HC, resulting in less efficient transport poleward to the Arctic. During boreal summer, there are poleward biases in jet location in free-running models, and these models likely underestimate the rate of transport into the Arctic. Models using specified dynamics do not have biases in the jet location, but do have biases in the surface meridional flow, which results in differences in the transport into the Arctic. In addition to the land-based tracer, the midlatitude-to-Arctic transport is further examined by another idealized tracer with zonally uniform sources. With equal sources from lands and oceans, the intermodel spread of this zonally uniform tracer is more related to variations of parameterized convection over oceans than variations of HC extent particularly during boreal summer. This suggests that transport of land-based and oceanic tracers or aerosols towards the Arctic differ in pathways and therefore their corresponding intermodel variabilities result from different physical processes.
Effects of ozone cooling in the tropical lower stratosphere and upper troposphere
Publisher: American Geophysical Union (AGU)
Date: 13-12-2007
DOI: 10.1029/2007GL031994
WHY ARE PEOPLE STILL NOT WALKING? THE NEED FOR A MICRO-SCALED MULTI-CRITERIA SPATIO-TEMPORAL DESIGN APPROACH TO IMPROVE WALK-QUALITY
Publisher: Copernicus GmbH
Date: 14-10-2022
DOI: 10.5194/ISPRS-ANNALS-X-4-W3-2022-269-2022
Abstract: Abstract. Walking is essential for the health and well-being of communities as well as meeting environmental challenges of the 21st Century. There have been significant research contributions in recent decades to understanding factors that can influence the likelihood of citizens choosing active travel modes, with great advances in understanding the built environment, particularly macro-scaled urban factors such as land-use mix, population density, and street patterns. So why are people still not walking? And is there anything we can do to try to change this? To answer these questions, this paper explores walking environment assessment approaches using a trans-disciplinary narrative approach, touching on multiple critical disciplinary knowledge areas. We find that while much of the research into the built environment’s influence on walking has made positive contributions in helping identify areas of cities that discourage active travel, the capacity to improve these areas has been limited. While macro-scaled factors commonly considered in ‘walkability’ analysis are highly influential to mode choice, unless working on green-field development, these factors may require re-zoning private land, substantial demolition and renewal, and may be financially or politically infeasible and thus extremely difficult to change. There is a need to augment macro-scaled analysis with micro-scaled tools, and to establish multi-criterion spatio-temporal design decision support approaches drawing from emerging technologies to make informed, integrated and effective urban design changes. These methods applied at precinct and streetscape levels have the potential to make feasible improvements to the ‘walk-quality’ of the built environment and contribute to facilitating active travel.
A global analysis of urban design types and road transport injury: an image processing study.
Publisher: Elsevier BV
Date: 2020
On the variability of the Ring effect in the near ultraviolet: understanding the role of aerosols and multiple scattering
Publisher: Copernicus GmbH
Date: 31-01-2007
Abstract: Abstract. The "filling-in" (FI) of Fraunhofer lines, often referred to as the Ring effect, was examined using measurements of near ultraviolet sunlight scattered from the zenith sky above Boulder, Colorado during July and August 2005. The FI of the 344.1 nm Fe I line was directly determined by comparing direct sun and cloud-free zenith sky spectra recorded on the same day. The results, obtained over solar zenith angles (SZA) from 20° to 70°, are compared to the predictions of a simple rotational Raman Scattering (RRS) spectral model. The measured FI was found to be up to 70% greater than that predicted by first-order molecular scattering with a much stronger SZA dependence. Simultaneously measured aerosol optical depths and Monte Carlo calculations show that the combination of aerosol scattering and second-order molecular scattering can account for these differences, and potentially explain the contradictory SZA dependences in previously published measurements of FI. These two scattering processes also introduce a wavelength dependence to FI that complicates the fitting of diffuse sunlight observations in differential optical absorption spectroscopy (DOAS). A simple correction to improve DOAS retrievals by removing this wavelength dependence is described.
Past and future simulations of NO2 from a coupled chemistry-climate model in comparison with observations
Publisher: Copernicus GmbH
Date: 22-11-2004
Abstract: Abstract. Trends in derived from a 45 year integration of a chemistry-climate model (CCM) run have been compared with ground-based measurements at Lauder (45° S) and Arrival Heights (78° S). Observed trends in at both sites exceed the modelled trends in N2O, the primary source gas for stratospheric NO2. This suggests that the processes driving the trend are not solely dictated by changes in but are coupled to global atmospheric change, either chemically or dynamically or both. If CCMs are to accurately estimate future changes in ozone, it is important that they comprehensively include all processes affecting NOx (NO+NO2) because NOx concentrations are an important factor affecting ozone concentrations. Comparison of measured and modelled NO2 trends is a sensitive test of the degree to which these processes are incorporated in the CCM used here. At Lauder the 1980-2000 CCM NO2 trends (4.2% per decade at sunrise, 3.8% per decade at sunset) are lower than the observed trends (6.5% per decade at sunrise, 6.0% per decade at sunset) but not significantly different at the 2σ level. Large variability in both the model and measurement data from Arrival Heights makes trend analysis of the data difficult. CCM predictions (2001-2019) of NO2 at Lauder and Arrival Heights show significant reductions in the rate of increase of NO2 compared with the previous 20 years (1980-2000). The model results indicate that the partitioning of oxides of nitrogen changes with time and is influenced by both chemical forcing and circulation changes.
Tropospheric and stratospheric BrO columns over Arrival Heights, Antarctica, 2002
Publisher: American Geophysical Union (AGU)
Date: 27-11-2006
DOI: 10.1029/2005JD007022
Estimates of Ozone Return Dates from Chemistry-Climate Model Initiative Simulations
Publisher: Copernicus GmbH
Date: 06-02-2018
DOI: 10.5194/ACP-2018-87
Abstract: Abstract. We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2047 (with a 1-σ uncertainty of 2042–2052). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2046 (2042–2050), and at Northern Hemisphere mid-latitudes in 2034 (2024–2044). In the polar regions, the return dates are 2062 (2055–2066) in the Antarctic in October and 2035 (2025–2040) in the Arctic in March. The earlier return dates in the NH reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–15 years, depending on the region. In the tropics only around half the models predict a return to 1980 values, at around 2040, while the other half do not reach this value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine, which is the main driver of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, the effect in the simulations analysed here is small and at the limit of detectability from the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ~ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also changes ozone return by ~ 15 years, again mainly through its impact in the tropics. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that is more important to have multi-member (at least 3) ensembles for each scenario from each established participating model, rather than a large number of in idual models.
Sensitivity of stratospheric Br<sub>y</sub> to uncertainties in very short lived substance emissions and atmospheric transport
Publisher: Copernicus GmbH
Date: 16-02-2011
Abstract: Abstract. We evaluate the sensitivity of Bry entering the stratosphere with a simplified model that allows calculations over a wide parameter range for parameters that are currently poorly quantified. The model examines the transport process uncertainties in the source concentrations and lifetimes, in the convective parameterization and in the inorganic bromine washout process due to dehydration. Source concentrations at the surface and lifetimes were found to have a slight effect on the resultant Bry (1 ppt), however this was highly dependent upon, with increasing significance, the BL component of convectively delivered air. Efficiency of convective delivery of boundary layer (BL) air to the tropical tropopause layer (TTL) along with washout at the CPT were found to substantially affect Bry at 400 K – altering the delivered Bry by 3.3 ppt and 2.9 ppt, respectively. We find that the results critically depend on free tropospheric bromine source gas concentrations due to dilution of convective updrafts, and the processes that control free tropospheric bromine source gas concentrations require further attention.
The retrieval of profile and chemical information from ground-based UV-visible spectroscopic measurements
Publisher: Elsevier BV
Date: 06-2004
Supplementary material to "Large-scale transport into the Arctic: the roles of the midlatitude jet and the Hadley Cell"
Publisher: Copernicus GmbH
Date: 30-08-2018
Review of the global models used within the Chemistry-Climate Model Initiative (CCMI)
Publisher: Copernicus GmbH
Date: 14-09-2016
DOI: 10.5194/GMD-2016-199
Abstract: Abstract. We present an overview of state-of-the-art chemistry-climate and -transport models that are used within the Chemistry-Climate Model Initiative (CCMI). CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI recommendations for simulations have been followed is necessary to understand model response to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI simulations with the aim to inform CCMI data users.
Cloud, precipitation and radiation responses to large perturbations in global dimethyl sulfide
Publisher: Copernicus GmbH
Date: 17-07-2018
DOI: 10.5194/ACP-18-10177-2018
Abstract: Abstract. 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 −1.4 W 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/-5 W 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 ex le of the aerosol lifetime effect. Globally, we find a sensitivity of temperature to annual DMS flux of 0.027 and 0.019 K 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.
Boundary layer new particle formation over East Antarctic sea ice – possible Hg driven nucleation?
Publisher: Copernicus GmbH
Date: 16-07-2015
DOI: 10.5194/ACPD-15-19477-2015
Abstract: Abstract. Aerosol observations above the Southern Ocean and Antarctic sea ice are scarce. Measurements of aerosols and atmospheric composition were made in East Antarctic pack ice on-board the Australian icebreaker Aurora Australis during the spring of 2012. One particle formation event was observed during the 32 days of observations. This event occurred on the only day to exhibit extended periods of global irradiance in excess of 600 W m−2. Within the single air-mass influencing the measurements, number concentrations of particles larger than 3 nm (CN3) reached almost 7700 cm−3 within a few hours of clouds clearing, and grew at rates of 5.6 nm h−1. Formation rates of 3 nm particles were in the range of those measured at other Antarctic locations at 0.2–1.1 ± 0.1 cm−3 s−1. Our investigations into the nucleation chemistry found that there were insufficient precursor concentrations for known halogen or organic chemistry to explain the nucleation event. Modelling studies utilising known sulfuric acid nucleation schemes could not simultaneously reproduce both particle formation or growth rates. Surprising correlations with Total Gaseous Mercury (TGM) were found that, together with other data, suggest a mercury driven photochemical nucleation mechanism may be responsible for aerosol nucleation. Given the very low vapour pressures of the mercury species involved, this nucleation chemistry is likely only possible where pre-existing aerosol concentrations are low and both TGM concentrations and solar radiation levels are relatively high (~ 1.5 ng m−3 and & geq 600 W m−2, respectively), such as those observed in the Antarctic sea ice boundary layer in this study or in the global free-troposphere, particularly in the Northern Hemisphere.
Microbial mercury methylation in Antarctic sea ice
Publisher: Springer Science and Business Media LLC
Date: 08-2016
DOI: 10.1038/NMICROBIOL.2016.127
Abstract: Atmospheric deposition of mercury onto sea ice and circumpolar sea water provides mercury for microbial methylation, and contributes to the bioaccumulation of the potent neurotoxin methylmercury in the marine food web. Little is known about the abiotic and biotic controls on microbial mercury methylation in polar marine systems. However, mercury methylation is known to occur alongside photochemical and microbial mercury reduction and subsequent volatilization. Here, we combine mercury speciation measurements of total and methylated mercury with metagenomic analysis of whole-community microbial DNA from Antarctic snow, brine, sea ice and sea water to elucidate potential microbially mediated mercury methylation and volatilization pathways in polar marine environments. Our results identify the marine microaerophilic bacterium Nitrospina as a potential mercury methylator within sea ice. Anaerobic bacteria known to methylate mercury were notably absent from sea-ice metagenomes. We propose that Antarctic sea ice can harbour a microbial source of methylmercury in the Southern Ocean.
A new Dobson Umkehr ozone profile retrieval method optimising information content and resolution
Publisher: Copernicus GmbH
Date: 19-08-2014
Abstract: Abstract. The standard Dobson Umkehr methodology to retrieve coarse resolution ozone profiles used by the National Oceanographic and Atmospheric Administration uses designated solar zenith angles (SZA). 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 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 raw 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 km and 45–80 km). Investigating a case from 13 April 1970 where the measurements extend beyond the 90° SZA range gives an even further amount of 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 km and 25–30 km) for both C and A + C + D-pairs. Retrievals in layers 5 and 6 (25–30 km and 30–35 km) consistently show lower ozone partial column compared to ozonesondes. This is likely due to and stray light effects that are not accounted for in the forward model, and under represented stratospheric aerosol.
Supplementary material to "Large-Scale Tropospheric Transport in the Chemistry Climate Model Initiative (CCMI) Simulations"
Publisher: Copernicus GmbH
Date: 30-11-2017
Large-Scale Tropospheric Transport in the Chemistry Climate Model Initiative (CCMI) Simulations
Publisher: Copernicus GmbH
Date: 30-11-2017
Abstract: Abstract. Understanding and modeling the large-scale transport of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. Here we show that there are large differences in the global-scale atmospheric transport properties among models participating in the IGAC SPARC Chemistry-Climate Model Initiative (CCMI). Specifically, we find up to 40 % differences in the transport timescales connecting the Northern Hemisphere (NH) midlatitude surface to the Arctic and to Southern Hemisphere high latitudes, where the mean age ranges between 1.7 years and 2.6 years. We show that these differences are related to large differences in vertical transport among the simulations and, in particular, to differences in parameterized convection over the oceans. While stronger convection over NH midlatitudes is associated with slower transport to the Arctic, stronger convection in the tropics and subtropics is associated with faster interhemispheric transport. We also show that the differences among simulations constrained with fields derived from the same reanalysis products are as large as (and, in some cases, larger than) the differences among free-running simulations, due to larger differences in parameterized convection. Our results indicate that care must be taken when using simulations constrained with analyzed winds to interpret the influence of meteorology on tropospheric composition.
The contribution of coral reef-derived dimethyl sulfide to aerosol burden over the Great Barrier Reef: a modelling study
Publisher: Copernicus GmbH
Date: 29-07-2021
DOI: 10.5194/ACP-2021-507
Abstract: Abstract. 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 time scales 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 – chemistry model (WRF-Chem) has been used in this work to study the role of coral reef-derived DMS at sub-daily time scales for the first time. WRF-Chem was run to coincide with an October 2016 field c aign over the Great Barrier Reef, Queensland, Australia, against which the model was evaluated. After updating 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.
High-resolution modeling of gaseous air pollutants over Tehran and validation with surface and satellite data
Publisher: Elsevier BV
Date: 02-2022
Air quality and health impact of 2019–20 Black Summer megafires and COVID-19 lockdown in Melbourne and Sydney, Australia
Publisher: Elsevier BV
Date: 04-2021
Comparison of formaldehyde tropospheric columns in Australia and New Zealand using MAX-DOAS, FTIR and TROPOMI
Publisher: Copernicus GmbH
Date: 04-12-2020
Abstract: Abstract. South-eastern Australia has been identified by modelling studies as a hotspot of biogenic volatile organic compound (VOC) emissions however, long-term observational VOC studies are lacking in this region. Here, 2.5 years of multi-axis differential optical absorption spectroscopy (MAX-DOAS) formaldehyde (HCHO) measurements in Australasia are presented, from Broadmeadows, in northern Melbourne, Australia, and from Lauder, a rural site in the South Island of New Zealand. Across the measurement period from December 2016 to November 2019, the mean formaldehyde columns measured by the MAX-DOAS were 2.50±0.61×1015 molec. cm−2 at Lauder and 5.40±1.59×1015 molec. cm−2 at Broadmeadows. In both locations, the seasonal cycle showed a pronounced peak in Austral summer (December–January–February) consistent with temperature-dependent formaldehyde production from biogenic precursor gases. The litude of the seasonal cycle was 0.7×1015 molec. cm−2 at Lauder, and it was 2.0×1015 molec. cm−2 at Broadmeadows. The Lauder MAX-DOAS HCHO measurements are compared with 27 months of co-located Fourier transform infrared (FTIR) observations. The seasonal variation of Lauder MAX-DOAS HCHO, smoothed by the FTIR averaging kernels, showed good agreement with the FTIR measurements, with a linear regression slope of 1.03 and an R2 of 0.66 for monthly averaged formaldehyde partial columns (0–4 km). In addition to ground-based observations, a clear way to address the VOC measurement gap in areas such as Australasia is with satellite measurements. Here, we demonstrate that the TROPOspheric Monitoring Instrument (TROPOMI) can be used to distinguish formaldehyde hotspots in forested and agricultural regions of south-eastern Australia. The MAX-DOAS measurements are also compared to TROPOMI HCHO vertical columns at Lauder and Melbourne very strong monthly average agreement is found for Melbourne (regression slope of 0.61 and R2 of 0.95) and a strong agreement is found at Lauder (regression slope of 0.73 and R2 of 0.61) for MAX-DOAS vs. TROPOMI between May 2018 and November 2019. This study, the first long-term satellite comparison study using MAX-DOAS in the Southern Hemisphere, highlights the improvement offered by TROPOMI's high resolution over previous satellite products and provides the groundwork for future studies using ground-based and satellite DOAS for studying VOCs in Australasia.
Estimates of ozone return dates from Chemistry-Climate Model Initiative simulations
Publisher: Copernicus GmbH
Date: 15-06-2018
Abstract: Abstract. We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼ 15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of in idual models.
A Theoretical Investigation of the Effects of Electronegative Substitution on the Strength of C−H···N Hydrogen Bonds
Publisher: American Chemical Society (ACS)
Date: 29-08-2001
DOI: 10.1021/JP011087T
The NIMO Monte Carlo model for box-air-mass factor and radiance calculations
Publisher: Elsevier BV
Date: 06-2012
Tropospheric ozone in CCMI models and Gaussian emulation to understand biases in the SOCOLv3 chemistry-climate model
Publisher: Copernicus GmbH
Date: 26-06-2018
DOI: 10.5194/ACP-2018-615
Abstract: Abstract. Previous multi-model intercomparisons have shown that chemistry-climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC/IGAC (Stratosphere-troposphere Processes and their Role in Climate/International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40–50 % in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ~ 30 % in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33 % larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, SOCOLv3.1, which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx, carbon monoxide, methane and other volatile organic compounds) are responsible for more than 90 % of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20 % more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry-climate models.
Time dependent profile retrieval of UV/vis absorbing radicals from balloon-borne limb measurements – a case study on NO<sub>2</sub> and O<sub>3</sub&am
Publisher: Copernicus GmbH
Date: 16-07-2010
Abstract: Abstract. A new "Bayesian" minimization algorithm for the retrieval of the diurnal variation of UV/vis absorbing radicals (O3, NO2, BrO, OClO and HONO) from balloon-borne limb scattered skylight observations is discussed. The method evaluates spectroscopic measurements in combination with radiative transfer calculations to drive a mathematical inversion on a discrete time and height grid. Here, the proposed method is applied to data obtained during two deployments of the mini-DOAS instrument on different balloon payloads in northern Brazil in June 2005. The retrieval is tested by comparing the inferred profiles to in-situ ozone sounding data and to measurements of the ENVISAT/SCIAMACHY satellite instrument performed during a collocated overpass. The comparison demonstrates the strength and validity of our approach. In particular for time-varying radical concentrations, photochemical corrections due to temporal mismatch of the corresponding observations are rendered dispensable. Thus, limb scanning UV/vis spectrometry from balloon platforms offers a more direct and concise approach for satellite validation of radical measurements than solar occultation measurements. Furthermore, monitoring of the diurnal variation of stratospheric radicals allows us to constrain photochemical parameters which are critical for stratospheric ozone chemistry, such as the photolysis frequency of N2O5 by observations of the diurnal variation of NO2.
Polar stratospheric chlorine kinetics from a self‐match flight during SOLVE‐II/EUPLEX
Publisher: American Geophysical Union (AGU)
Date: 2008
DOI: 10.1029/2007GL031740
Use of portable air cleaners to reduce aerosol transmission on a hospital COVID-19 ward
Publisher: Elsevier BV
Date: 11-2021
Atmospheric Trace Metal Deposition from Natural and Anthropogenic Sources in Western Australia
Publisher: MDPI AG
Date: 07-05-2020
Abstract: Aerosols from Western Australia supply micronutrient trace elements including Fe into the western shelf of Australia and further afield into the Southern and Indian Oceans. However, regional observations of atmospheric trace metal deposition are limited. Here, we applied a series of leaching experiments followed by total analysis of bulk aerosol s les to a unique time-series of aerosol s les collected in Western Australia to determine atmospheric concentrations and solubilities of Fe and V, Mn, Co, Zn, and Pb. Positive matrix factorisation analysis indicated that mineral dust, biomass burning particulates, sea salt, and industrial emissions were the major types of aerosols. Overall, natural sources dominated Fe deposition. Higher atmospheric concentrations of mineral dust (sixfold) and biomass burning emissions were observed in warmer compared to cooler months. The fraction of labile Fe (0.6–6.0%) was lower than that reported for other regions of Australia. Bushfire emissions are a temporary source of labile Fe and may cause a peak in the delivery of its more easily available forms to the ocean. Increased labile Fe deposition may result in higher ocean productivity in regions where Fe is limiting, and the effect of aerosol deposition on ocean productivity in this region requires further study.
Supplementary material to "The influence of mixing on stratospheric circulation changes in the 21st century"
Publisher: Copernicus GmbH
Date: 25-10-2018
Evaluation of the ACCESS - Chemistry-climate model for the Southern Hemisphere
Publisher: Copernicus GmbH
Date: 29-02-2016
Abstract: Abstract. 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 50 hPa 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.
Stratospheric Injection of Brominated Very Short‐Lived Substances: Aircraft Observations in the Western Pacific and Representation in Global Models
Publisher: American Geophysical Union (AGU)
Date: 27-05-2018
DOI: 10.1029/2017JD027978
A new Dobson Umkehr ozone profile retrieval method optimising information content and resolution
Publisher: Copernicus GmbH
Date: 04-03-2015
Abstract: Abstract. 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.
Cloud property estimates from zenith spectral measurements of scattered sunlight between 0.9 and 1.7 μm
Publisher: American Geophysical Union (AGU)
Date: 27-08-2006
DOI: 10.1029/2005JD006641
Atmospheric Trace Metal Deposition near the Great Barrier Reef, Australia
Publisher: MDPI AG
Date: 15-04-2020
Abstract: 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 s les 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 Antarctic ozone hole during 2014
Publisher: CSIRO Publishing
Date: 2019
DOI: 10.1071/ES19023
Abstract: We review the 2014 Antarctic ozone hole, making use of a variety of ground-based and space-based measurements of ozone and ultra-violet radiation, supplemented by meteorological reanalyses. Although the polar vortex was relatively stable in 2014 and persisted some weeks longer into November than was the case in 2012 or 2013, the vortex temperature was close to the long-term mean in September and October with modest warming events occurring in both months, preventing severe depletion from taking place. Of the seven metrics reported here, all were close to their respective median values of the 1979–2014 record, being ranked between 16th and 21st of the 35 years for which adequate satellite observations exist.
World climate research programme special workshop on climatic effects of ozone depletion in the southern hemisphere
Publisher: American Meteorological Society
Date: 06-2014
Observations of Clouds, Aerosols, Precipitation, and Surface Radiation over the Southern Ocean: An Overview of CAPRICORN, MARCUS, MICRE, and SOCRATES
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.
The Antarctic ozone hole during 2015 and 2016
Publisher: CSIRO Publishing
Date: 2019
DOI: 10.1071/ES19021
Abstract: We reviewed the 2015 and 2016 Antarctic ozone holes, making use of a variety of ground-based and spacebased measurements of ozone and ultraviolet radiation, supplemented by meteorological reanalyses. The ozone hole of 2015 was one of the most severe on record with respect to maximum area and integrated deficit and was notably longlasting, with many values above previous extremes in October, November and December. In contrast, all assessed metrics for the 2016 ozone hole were at or below their median values for the 37 ozone holes since 1979 for which adequate satellite observations exist. The 2015 ozone hole was influenced both by very cold conditions and enhanced ozone depletion caused by stratospheric aerosol resulting from the April 2015 volcanic eruption of Calbuco (Chile).
First quasi-Lagrangian in-situ measurements of Antarctic Polar springtime ozone: observed ozone loss rates from the Concordiasi long-duration balloon campaign
Publisher: Copernicus GmbH
Date: 09-2014
DOI: 10.5194/ACPD-14-22245-2014
Abstract: Abstract. We present ozone measurements made using state-of-the-art ultraviolet photometers onboard three long-duration stratospheric balloons launched as part of the Concordiasi c aign in austral spring 2010. Ozone loss rates calculated by matching air-parcels s led at different times and places during the polar spring are in agreement with rates previously derived from ozonesonde measurements, for the vortex-average, ranging between 2–7 ppbv (sunlit h)−1 or 25–110 ppbv per day. However, the geographical coverage of these long-duration stratospheric balloon platforms provides new insights into the temporal and spatial patterns of ozone loss over Antarctica. Very large ozone loss rates of up to 200 ppbv day−1 (16 ppbv (sunlit h)−1) are observed for airmasses that are down-wind of the Antarctic Peninsula and/or over the East Antarctic region. The ozone loss rate maximum downstream of the Antarctic Peninsula region is consistent with high PSC occurrence from Calipso and large ClO abundances from MLS satellite observations for 12–22 September 2010.
The Antarctic ozone hole during 2012
Publisher: Bureau of Meteorology, Australia
Date: 12-2014
DOI: 10.22499/2.6404.007
Surface ozone exceedances in Melbourne, Australia are shown to be under NOx control, as demonstrated using formaldehyde:NO2 and glyoxal:formaldehyde ratios
Publisher: Elsevier BV
Date: 12-2020
Key challenges for tropospheric chemistry in the Southern Hemisphere
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.
Quantifying the effect of mixing on the mean Age of Air in CCMVal-2 and CCMI-1 models
Publisher: Copernicus GmbH
Date: 20-12-2017
Abstract: Abstract. Stratospheric age of air (AoA) is a useful measure of the overall capabilities of a general circulation model (GCM) to simulate stratospheric transport. Previous studies have reported a large spread in the simulation of AoA by GCMs and coupled chemistry-climate models (CCMs). Compared to observational estimates simulated AoA is mostly too low. Here we attempt to untangle the processes that lead to the AoA differences between the models and between models and observations. AoA is influenced by both, mean transport along the residual circulation and two-way mixing we quantify the effects of these processes using data from the CCM inter-comparison projects CCMVal-2 and CCMI-1. Transport along the residual circulation is measured by the residual circulation transit time (RCTT). We interpret the difference between AoA and RCTT as additional aging by mixing. Aging by mixing thus includes mixing on both the resolved and subgrid scale. We find that the spread in AoA between the models is primarily caused by differences in the effects of mixing, and only to some extent by differences in residual circulation strength. These effects are quantified by the mixing efficiency, a measure of the relative increase of AoA by mixing. The mixing efficiency varies strongly between the models from 0.21 to 0.99. We show that the mixing efficiency is not only controlled by horizontal mixing, but by vertical mixing and vertical diffusion as well. Possible causes for the differences in the models' mixing efficiencies are discussed. Differences in subgrid scale mixing (including differences in advection schemes and model resolutions) likely contribute to the differences in mixing efficiency. However, differences in the relative contribution of resolved versus parametrized wave forcing do not appear to be related to differences in mixing efficiency or AoA.
Supplementary material to "Estimates of Ozone Return Dates from Chemistry-Climate Model Initiative Simulations"
Publisher: Copernicus GmbH
Date: 06-02-2018
A case study of a transported bromine explosion event in the Canadian high arctic
Publisher: American Geophysical Union (AGU)
Date: 05-01-2016
DOI: 10.1002/2015JD023711
The influence of mixing on the stratospheric age of air changes in the 21st century
Publisher: Copernicus GmbH
Date: 24-01-2019
Abstract: Abstract. Climate models consistently predict an acceleration of the Brewer–Dobson circulation (BDC) due to climate change in the 21st century. However, the strength of this acceleration varies considerably among in idual models, which constitutes a notable source of uncertainty for future climate projections. To shed more light upon the magnitude of this uncertainty and on its causes, we analyse the stratospheric mean age of air (AoA) of 10 climate projection simulations from the Chemistry-Climate Model Initiative phase 1 (CCMI-I), covering the period between 1960 and 2100. In agreement with previous multi-model studies, we find a large model spread in the magnitude of the AoA trend over the simulation period. Differences between future and past AoA are found to be predominantly due to differences in mixing (reduced aging by mixing and recirculation) rather than differences in residual mean transport. We furthermore analyse the mixing efficiency, a measure of the relative strength of mixing for given residual mean transport, which was previously hypothesised to be a model constant. Here, the mixing efficiency is found to vary not only across models, but also over time in all models. Changes in mixing efficiency are shown to be closely related to changes in AoA and quantified to roughly contribute 10 % to the long-term AoA decrease over the 21st century. Additionally, mixing efficiency variations are shown to considerably enhance model spread in AoA changes. To understand these mixing efficiency variations, we also present a consistent dynamical framework based on diffusive closure, which highlights the role of basic state potential vorticity gradients in controlling mixing efficiency and therefore aging by mixing.
The impact of overshooting deep convection on local transport and mixing in the tropical upper troposphere/lower stratosphere (UTLS)
Publisher: Copernicus GmbH
Date: 14-01-2015
DOI: 10.5194/ACPD-15-1041-2015
Abstract: Abstract. In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 c aign in connection to a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward transport from the boundary layer into the cloud anvils and overshooting tops. For ex le, a passive ozone tracer (i.e. a tracer not undergoing chemical processing) shows an enhancement in the upper troposphere of up to about 30 ppbv locally in the cloud, while the in situ measurements show an increase of 50 ppbv. However, the passive carbon monoxide tracer exhibits an increase, while the observations show a decrease of about 10 ppbv, indicative of an erroneous model representation of the transport processes in the tropical tropopause layer. Furthermore, it could point to insufficient entrainment and detrainment in the model. The simulation shows a general moistening of air in the lower stratosphere but it also exhibits local dehydration features. Here we use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.
Retrieved tropospheric and stratospheric BrO columns over Lauder, New Zealand
Publisher: American Geophysical Union (AGU)
Date: 27-07-2004
DOI: 10.1029/2003JD004463
Measurement Report: Understanding the seasonal cycle of Southern Ocean aerosols
Publisher: Copernicus GmbH
Date: 07-09-2022
DOI: 10.5194/ACP-2022-568
Abstract: Abstract. 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 mid-latitudes 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 two 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 cm-3, 426 cm-3 and 468 cm-3 at KCG, MQI and SYO, respectively). In wintertime, seasonal minima at KCG and MQI were similar (142 cm-3 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 cm-3 and 145 cm-3, respectively), whereas KCG showed ∼40 % lower concentrations than MQI in winter (medians of 57 cm-3 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, highlight the heterogeneity of this pristine region, and the need for further long-term observations that capture the seasonal cycles.
Coral-reef-derived dimethyl sulfide and the climatic impact of the loss of coral reefs
Publisher: Copernicus GmbH
Date: 20-04-2021
Abstract: Abstract. Dimethyl sulfide (DMS) is a naturally occurring aerosol precursor gas which plays an important role in the global sulfur budget, aerosol formation and climate. While DMS is produced predominantly by phytoplankton, recent observational literature has suggested that corals and their symbionts produce a comparable amount of DMS, which is unaccounted for in models. It has further been hypothesised that the coral reef source of DMS may modulate regional climate. This hypothesis presents a particular concern given the current threat to coral reefs under anthropogenic climate change. In this paper, a global climate model with online chemistry and aerosol is used to explore the influence of coral-reef-derived DMS on atmospheric composition and climate. A simple representation of coral-reef-derived DMS is developed and added to a common DMS surface water climatology, resulting in an additional flux of 0.3 Tg yr−1 S, or 1.7 % of the global sulfur flux from DMS. By comparing the differences between both nudged and free-running ensemble simulations with and without coral-reef-derived DMS, the influence of coral-reef-derived DMS on regional climate is quantified. In the Maritime Continent–Australian region, where the highest density of coral reefs exists, a small decrease in nucleation- and Aitken-mode aerosol number concentration and mass is found when coral reef DMS emissions are removed from the system. However, these small responses are found to have no robust effect on regional climate via direct and indirect aerosol effects. This work emphasises the complexities of the aerosol–climate system, and the limitations of current modelling capabilities are highlighted, in particular surrounding convective responses to changes in aerosol. In conclusion, we find no robust evidence that coral-reef-derived DMS influences global and regional climate.
The contribution of coral-reef-derived dimethyl sulfide to aerosol burden over the Great Barrier Reef
Publisher: Copernicus GmbH
Date: 22-02-2022
Abstract: Abstract. 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 c aign 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.
Retrieval of effective radius and liquid water path from ground‐based instruments: A case study at Barrow, Alaska
Publisher: American Geophysical Union (AGU)
Date: 06-11-2007
DOI: 10.1029/2007JD008737
Efficacy of a patient isolation hood in reducing exposure to airborne infectious virus in a simulated healthcare setting
Publisher: Cold Spring Harbor Laboratory
Date: 29-07-2022
DOI: 10.1101/2022.07.24.22277784
Abstract: Healthcare workers treating patients with SARS-CoV-2 are at risk of infection from patient-emitted virus-laden aerosols. We quantified the reduction of airborne infectious virus in a simulated hospital room when a ventilated patient isolation (McMonty) hood was in use. We nebulised 10 9 plaque forming units (PFU) of bacteriophage PhiX174 virus into a 35.1m 3 room with a hood active or inactive. The airborne concentration of infectious virus was measured by BioSpot-VIVAS and settle plates using plaque assay quantification on the bacterial host Escherichia coli C . The particle number concentration (PNC) was monitored continuously using an optical particle sizer. Median airborne viral concentration in the room reached 1.41 × 10 5 PFU.m -3 with the hood inactive. Using the active hood as source containment reduced infectious virus concentration by 374-fold in air s les. This was associated with a 109-fold reduction in total airborne particle number escape rate. The deposition of infectious virus on the surface of settle plates was reduced by 87-fold. The isolation hood significantly reduced airborne infectious virus exposure in a simulated hospital room. Our findings support the use of the hood to limit exposure of healthcare workers to airborne virus in clinical environments. COVID-19 patients exhale aerosol particles which can potentially carry infectious viruses into the hospital environment, putting healthcare workers at risk of infection. This risk can be reduced by proper use of personal protective equipment (PPE) to protect workers from virus exposure. More effective strategies, however, aim to provide source control, reducing the amount of virus-contaminated air that is exhaled into the hospital room. The McMonty isolation hood has been developed to trap and decontaminate the air around an infected patient. We tested the efficacy of the hood using a live virus model to mimic a COVID-19 patient in a hospital room. Using the McMonty hood reduced the amount of exhaled air particles in the room by over 109-times. In our tests, people working in the room were exposed to 374-times less infectious virus in the air, and room surfaces were 87-times less contaminated. Our study supports using devices like the McMonty hood in combination with PPE to keep healthcare workers safe from virus exposure at work.
Large-scale tropospheric transport in the Chemistry–Climate Model Initiative (CCMI) simulations
Publisher: Copernicus GmbH
Date: 25-05-2018
Abstract: Abstract. Understanding and modeling the large-scale transport of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. Here we show that there are large differences in the global-scale atmospheric transport properties among the models participating in the IGAC SPARC Chemistry–Climate Model Initiative (CCMI). Specifically, we find up to 40 % differences in the transport timescales connecting the Northern Hemisphere (NH) midlatitude surface to the Arctic and to Southern Hemisphere high latitudes, where the mean age ranges between 1.7 and 2.6 years. We show that these differences are related to large differences in vertical transport among the simulations, in particular to differences in parameterized convection over the oceans. While stronger convection over NH midlatitudes is associated with slower transport to the Arctic, stronger convection in the tropics and subtropics is associated with faster interhemispheric transport. We also show that the differences among simulations constrained with fields derived from the same reanalysis products are as large as (and in some cases larger than) the differences among free-running simulations, most likely due to larger differences in parameterized convection. Our results indicate that care must be taken when using simulations constrained with analyzed winds to interpret the influence of meteorology on tropospheric composition.
Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice
Publisher: Copernicus GmbH
Date: 25-02-2016
Abstract: Abstract. 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.
Comparison of formaldehyde tropospheric columns in Australia and New Zealand using MAX-DOAS, FTIR and TROPOMI
Publisher: Copernicus GmbH
Date: 03-07-2020
DOI: 10.5194/AMT-2020-232
Abstract: Abstract. South-eastern Australia has been identified by modelling studies as a hotspot of biogenic volatile organic compound (VOC) emissions, however long term observational VOC studies are lacking in this region. Here, two and a half years of MAX-DOAS formaldehyde (HCHO) measurements in Australasia are presented, from Broadmeadows in northern Melbourne, Australia and from Lauder, a rural site in the South Island of New Zealand. Across the measurement period from December 2016 to November 2019, the mean formaldehyde column measured by the MAX-DOAS at Lauder was 2.50 ± 0.61 × 1014 molec cm−2 and at Broadmeadows was 5.40 ± 1.59 × 1015 molec cm−2. In both locations the seasonal cycle showed a pronounced peak in Austral summer (DJF) consistent with temperature-dependent formaldehyde production from biogenic precursor gases. The litude of the seasonal cycle at Lauder was 0.7 × 1015 molec cm−2 while it was 2.0 × 1015 molec cm−2 at Broadmeadows. The Lauder MAX-DOAS HCHO measurements are compared with 27 months of co-located fourier-transform infrared (FTIR) observations. The seasonal variation of Lauder MAX-DOAS HCHO, smoothed by the FTIR averaging kernels, correlated strongly with the FTIR measurements, with linear regression slope of 0.91 and R2 of 0.81 for monthly averaged formaldehyde partial columns. In addition to ground-based observations, a clear way to address the VOC measurement gap in areas such as Australasia is with satellite measurements. Here we demonstrate that the Tropospheric Monitoring Instrument (TROPOMI) can be used to distinguish formaldehyde hotspots in forested and agricultural regions of south-eastern Australia. The MAX-DOAS measurements are also compared to TROPOMI HCHO vertical columns at Lauder and Melbourne very strong monthly average agreement is found for Melbourne (regression slope of 0.61, R2 of 0.95) and a strong agreement is found at Lauder (regression slope of 0.73, R2 of 0.61) for MAX-DOAS vs. TROPOMI between May 2018 and November 2019. This study, the first long term satellite comparison study using MAX-DOAS in the southern hemisphere, highlights the improvement offered by TROPOMI's high resolution over previous satellite products and provides the groundwork for future studies using ground based and satellite DOAS for studying VOCs in Australasia.
Evaluation of the Australian Community Climate and Earth-System Simulator Chemistry-Climate Model
Publisher: Copernicus GmbH
Date: 13-07-2015
DOI: 10.5194/ACPD-15-19161-2015
Abstract: Abstract. Chemistry climate models are important tools for addressing interactions of composition and climate in the Earth System. In particular, they are used for assessing 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, 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 show a similar amount of depletion compared to observations. A significant innovation is 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 (up to 26.4 % at Davis during winter) and stratospheric cold biases (up to 10.1 K at the South Pole) 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: centered around 100 hPa in ozonesonde data compared to above 50 hPa 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 models inability to explicitly simulated supercooled ternary solution may also explain the lack of depletion at lower altitudes. The simulated Southern Annular Mode (SAM) index compares well with ERA-Interim data. 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 shows 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.
The Antarctic ozone hole during 2013
Publisher: Bureau of Meteorology, Australia
Date: 07-2015
DOI: 10.22499/2.6502.005
The Antarctic ozone hole during 2017
Publisher: CSIRO Publishing
Date: 2019
DOI: 10.1071/ES19019
Abstract: We review the 2017 Antarctic ozone hole, making use of various meteorological reanalyses, and in-situ, satellite and ground-based measurements of ozone and related trace gases, and ground-based measurements of ultraviolet radiation. The 2017 ozone hole was associated with relatively high-ozone concentrations over the Antarctic region compared to other years, and our analysis ranked it in the smallest 25% of observed ozone holes in terms of size. The severity of stratospheric ozone loss was comparable with that which occurred in 2002 (when the stratospheric vortex exhibited an unprecedented major warming) and most years prior to 1989 (which were early in the development of the ozone hole). Disturbances to the polar vortex in August and September that were associated with intervals of anomalous planetary wave activity resulted in significant erosion of the polar vortex and the mitigation of the overall level of ozone depletion. The enhanced wave activity was favoured by below-average westerly winds at high southern latitudes during winter, and the prevailing easterly phase of the quasi-biennial oscillation (QBO). Using proxy information on the chemical make-up of the polar vortex based on the analysis of nitrous oxide and the likely influence of the QBO, we suggest that the concentration of inorganic chlorine, which plays a key role in ozone loss, was likely similar to that in 2014 and 2016, when the ozone hole was larger than that in 2017. Finally, we found that the overall severity of Antarctic ozone loss in 2017 was largely dictated by the timing of the disturbances to the polar vortex rather than interannual variability in the level of inorganic chlorine.
Evaluating the relationship between interannual variations in the Antarctic ozone hole and Southern Hemisphere surface climate in Chemistry-Climate Models
Publisher: American Meteorological Society
Date: 06-2019
Abstract: Studies have recently reported statistically significant relationships between observed year-to-year spring Antarctic ozone variability and the Southern Hemisphere annular mode and surface temperatures in spring–summer. This study investigates whether current chemistry–climate models (CCMs) can capture these relationships, in particular, the connection between November total column ozone (TCO) and Australian summer surface temperatures, where years with anomalously high TCO over the Antarctic polar cap tend to be followed by warmer summers. The interannual ozone–temperature teleconnection is examined over the historical period in the observations and simulations from the Whole Atmosphere Community Climate Model (WACCM) and nine other models participating in the Chemistry–Climate Model Initiative (CCMI). There is a systematic difference between the WACCM experiments forced with prescribed observed sea surface temperatures (SSTs) and those with an interactive ocean. Strong correlations between TCO and Australian temperatures are only obtained for the uncoupled experiment, suggesting that the SSTs could be important for driving both variations in Australian temperatures and the ozone hole, with no causal link between the two. Other CCMI models also tend to capture this relationship with more fidelity when driven by observed SSTs, although additional research and targeted modeling experiments are required to determine causality and further explore the role of model biases and observational uncertainty. The results indicate that CCMs can reproduce the relationship between spring ozone and summer Australian climate reported in observational studies, suggesting that incorporating ozone variability could improve seasonal predictions however, more work is required to understand the difference between the coupled and uncoupled simulations.
Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea-ice
Publisher: Copernicus GmbH
Date: 27-10-2015
DOI: 10.5194/ACPD-15-29125-2015
Abstract: Abstract. The effect of aerosols on clouds and their radiative properties is one of the largest uncertainties in our understanding of radiative forcing. A recent study has concluded that better characterisation of pristine, natural aerosol processes leads to the largest reduction in these uncertainties. Antarctica, being far from anthropogenic activities, is an ideal location for the study of natural aerosol processes. Aerosol measurements in Antarctica are often limited to boundary layer air-masses at spatially sparse coastal and continental research stations, with only a handful of studies in the 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 ice-breaker 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 equator-ward into the low albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei where, 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.
The impact of overshooting deep convection on local transport and mixing in the tropical upper troposphere/lower stratosphere (UTLS)
Publisher: Copernicus GmbH
Date: 12-06-2015
Abstract: Abstract. In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 c aign in connection with a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward transport from the boundary layer into the cloud anvils and overshooting tops. For ex le, a passive ozone tracer (i.e. a tracer not undergoing chemical processing) shows an enhancement in the upper troposphere of up to about 30 ppbv locally in the cloud, while the in situ measurements show an increase of 50 ppbv. However, the passive carbon monoxide tracer exhibits an increase, while the observations show a decrease of about 10 ppbv, indicative of an erroneous model representation of the transport processes in the tropical tropopause layer. Furthermore, it could point to insufficient entrainment and detrainment in the model. The simulation shows a general moistening of air in the lower stratosphere, but it also exhibits local dehydration features. Here we use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.
Cloud, precipitation and radiation responses to large perturbations in global dimethyl sulfide
Publisher: Copernicus GmbH
Date: 22-12-2017
Abstract: Abstract. Natural aerosol emission represents one of the largest uncertainties in our understanding of the climate system. 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. In this study we quantify the role of DMS in the chemistry-climate system and determine the climate's response to large DMS perturbations. By removing all marine DMS in the Australian Community Climate and Earth System Simulator (ACCESS) – United Kingdom Chemistry and Aerosol (UKCA), we find a top of atmosphere radiative effect of 1.7 W m−2. The largest responses to removing marine DMS are in stratiform cloud decks in the Southern Hemisphere's eastern ocean basins. These regions show significant differences in low-cloud (−9 %), radiation (+7 W m−2 in short wave incoming surface radiation) and large-scale rainfall (+15 %) when all DMS is removed. We demonstrate a precipitation suppression effect of DMS-derived aerosol in stratiform cloud deck regions, coupled with an increase in low cloud fraction. The increase in low cloud fraction is an ex le of the aerosol lifetime effect. 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. Our study highlights the need for further modelling and field studies of natural aerosols and their impact on cloud and precipitation, in particular in Southern Hemisphere stratiform cloud regions.
Supplementary material to "Review of the global models used within the Chemistry-Climate Model Initiative (CCMI)"
Publisher: Copernicus GmbH
Date: 14-09-2016
Effectiveness of portable air filtration on reducing indoor aerosol transmission: preclinical observational trials
Publisher: Elsevier BV
Date: 2022
Stratospheric ozone intrusion events and their impacts on tropospheric ozone in the Southern Hemisphere
Publisher: Copernicus GmbH
Date: 09-2017
DOI: 10.5194/ACP-17-10269-2017
Abstract: Abstract. Stratosphere-to-troposphere transport (STT) provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the Southern Hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality of STT events and quantify the ozone transported across the tropopause over Davis (69° S, 2006–2013), Macquarie Island (54° S, 2004–2013), and Melbourne (38° S, 2004–2013). STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile and an analysis of the Brunt–Väisälä frequency. Using a bandpass filter on 7–9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter for all three sites. The majority of tropospheric ozone enhancements owing to STT events occur within 2.5 and 3 km of the tropopause at Davis and Macquarie Island respectively. Events are more spread out at Melbourne, occurring frequently up to 6 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is ∼ 1. 0–3. 5 % at each site however, during in idual events, over 10 % of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low-pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, which are apparent during austral winter and spring and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely resolved to distinguish STT events but is able to accurately simulate the seasonal cycle of tropospheric ozone columns over the three southern hemispheric sites. Combining the ozonesonde-derived STT event characteristics with the simulated tropospheric ozone columns from GEOS-Chem, we estimate STT ozone flux near the three sites and see austral summer dominated yearly amounts of between 5. 7 and 8. 7 × 1017 molecules cm−2 a−1.
Supplementary material to "Tropospheric ozone in CCMI models and Gaussian emulation to understand biases in the SOCOLv3 chemistry-climate model"
Publisher: Copernicus GmbH
Date: 26-06-2018
Boundary layer new particle formation over East Antarctic sea ice – possible Hg-driven nucleation?
Publisher: Copernicus GmbH
Date: 02-12-2015
DOI: 10.5194/ACP-15-13339-2015
Abstract: Abstract. Aerosol observations above the Southern Ocean and Antarctic sea ice are scarce. Measurements of aerosols and atmospheric composition were made in East Antarctic pack ice on board the Australian icebreaker Aurora Australis during the spring of 2012. One particle formation event was observed during the 32 days of observations. This event occurred on the only day to exhibit extended periods of global irradiance in excess of 600 W m−2. Within the single air mass influencing the measurements, number concentrations of particles larger than 3 nm (CN3) reached almost 7700 cm−3 within a few hours of clouds clearing, and grew at rates of 5.6 nm h−1. Formation rates of 3 nm particles were in the range of those measured at other Antarctic locations at 0.2–1.1 ± 0.1 cm−3 s−1. Our investigations into the nucleation chemistry found that there were insufficient precursor concentrations for known halogen or organic chemistry to explain the nucleation event. Modelling studies utilising known sulfuric acid nucleation schemes could not simultaneously reproduce both particle formation or growth rates. Surprising correlations with total gaseous mercury (TGM) were found that, together with other data, suggest a mercury-driven photochemical nucleation mechanism may be responsible for aerosol nucleation. Given the very low vapour pressures of the mercury species involved, this nucleation chemistry is likely only possible where pre-existing aerosol concentrations are low and both TGM concentrations and solar radiation levels are relatively high (∼ 1.5 ng m−3 and & geq 600 W m−2, respectively), such as those observed in the Antarctic sea ice boundary layer in this study or in the global free troposphere, particularly in the Northern Hemisphere.
Observations of the Boundary Layer in the Cape Grim Coastal Region: Interaction with Wind and the Influences of Continental Sources
Publisher: MDPI AG
Date: 12-01-2023
DOI: 10.3390/RS15020461
Abstract: A comparative study and evaluation of boundary layer height (BLH) estimation was conducted during an experimental c aign conducted at the Cape Grim Air Pollution station, Australia, from 1 June to 13 July 2019. The temporal and spatial distributions of BLH were studied using data from a ceilometer, sodar, in situ meteorological measurements, and back-trajectory analyses. Generally, the BLH under continental sources is lower than that under marine sources. The BLH is featured with a shallow depth of 515 ± 340 m under the Melbourne/East Victoria continental source. Especially the mixed continental sources (Melbourne/East Victoria and Tasmania direction) lead to a rise in radon concentration and lower BLH. In comparison, the boundary layer reaches a higher averaged BLH value of 730 ± 305 m when marine air is prevalent. The BLH derived from ERA5 is positively biased compared to the ceilometer observations, except when the boundary layer is stable. The height at which wind profiles experience rapid changes corresponds to the BLH value. The wind flow within the boundary layer increased up to ∼200 m, where it then meandered up to ∼300 m. Furthermore, the statistic shows that BLH is positively associated with near-surface wind speed. This study firstly provides information on boundary layer structure in Cape Grim and the interaction with wind, which may aid in further evaluating their associated impacts on the climate and ecosystem.
Future changes in stratospheric quasi-stationary wave-1 in the extratropical southern hemisphere spring and summer as simulated by ACCESS-CCM
Publisher: CSIRO Publishing
Date: 26-08-2021
DOI: 10.1071/ES21002
Abstract: Seasonally dependent quasi-stationary planetary wave activity in the southern hemisphere influences the distribution of ozone within and near the equatorward edge of the stratospheric polar vortex. Accurate representation of this zonal asymmetry in ozone is important in the characterisation of stratospheric circulation and climate and their associated effects at the surface. In this study, we used the Australian Community and Climate Earth System Simulator-Chemistry Climate Model to investigate the influence of greenhouse gases (GHGs) and ozone depleting substances (ODSs) on the zonal asymmetry of total column ozone (TCO) and 10 hPa zonal wind between 50 and 70°S. Sensitivity simulations were used from 1960 to 2100 with fixed ODSs and GHGs at 1960 levels and a regression model that uses equivalent effective stratospheric chlorine and carbon dioxide equivalent radiative forcing as the regressors. The model simulates the spring and summer zonal wave-1 reasonably well, albeit with a slight bias in the phase and litude compared to observations. An eastward shift in the TCO and 10 hPa zonal wave-1 is associated with both decreasing ozone and increasing GHGs. Amplitude increases are associated with ozone decline and litude decreases with GHG increases. The influence of ODSs typically outweigh those by GHGs, partly due to the GHG influence on TCO phase at 50°S likely being h ered by the Andes. Therefore, over the 21st century, influence from ozone recovery causes a westward shift and a decrease in litude. An exception is at 70°S during spring, where the GHG influence is larger than that of ozone recovery, causing a continued eastward trend throughout the 21st century. Also, GHGs have the largest influence on the 10 hPa zonal wave-1 phase, but still only induce a small change in the wave-1 litude. Different local longitudes also experience different rates of ozone recovery due to the changes in phase of the zonal wave-1. The results from this study have important implications for understanding future ozone layer distribution in the Southern Hemisphere under changing GHG and ODS concentrations. Important future work would involve conducting a similar study using a large ensemble of models to gain more statistically significant results.
The influence of mixing on stratospheric circulation changes in the 21st century
Publisher: Copernicus GmbH
Date: 25-10-2018
Abstract: Abstract. Climate models consistently predict an acceleration of the Brewer-Dobson circulation (BDC) due to climate change in the 21st century. However, the strength of this acceleration varies considerably among in idual models, which constitutes a notable source of uncertainty for future climate projections. To shed more light upon the magnitude of this uncertainty and on its causes, we analyze the stratospheric mean age of air (AoA) of 10 climate projection simulations from the Chemistry Climate Model Initiative phase 1 (CCMI-I), covering the period between 1960 and 2100. In agreement with previous multi-model studies, we find a large model spread in the magnitude of the AoA trend over the simulation period. Differences between future and past AoA are found to be predominantly due to differences in mixing (reduced aging by mixing and recirculation) rather than differences in residual mean transport. We furthermore analyze the mixing efficiency, a measure of the relative strength of mixing for given residual mean transport, which was previously hypothesized to be a model constant. Here, the mixing efficiency is found to vary not only across models, but also over time in all models. Changes in mixing efficiency are shown to be closely related to changes in AoA and quantified to roughly contribute 10 % to the long-term AoA decrease over the 21st century. Additionally, mixing efficiency variations are shown to considerably enhance model spread in AoA changes. To understand these mixing efficiency variations, we also present a consistent dynamical framework based on diffusive closure, which highlights the role of basic state potential vorticity gradients in controlling mixing efficiency and therefore aging by mixing.
Seventeen years of ozone sounding at L'Aquila, Italy: evidence of mid-latitude stratospheric ozone recovery and tropospheric profile changes
Publisher: Copernicus GmbH
Date: 07-2020
DOI: 10.5194/ACP-2020-525
Abstract: Abstract. Ozone profile measurements collected at L'Aquila (Italy, 42.4° N) during seventeen years of radio-sounding (2000–2016) are presented here, with an analysis of derived trends. Model results from the SPARC-CCMI exercise are used in parallel to highlight the physical and chemical mechanisms regulating mid-latitude ozone trends. The statistically significant trends highlighted in time series at L'Aquila are those in the mid-upper stratosphere (+5.9 ± 4.2), mid troposphere (+5.9 ± 2.4) and upper troposphere (+2.5 ± 0.9), all in percent/decade. The upper stratospheric positive trend was already well documented in recent WMO assessments and attributed to the starting decline of stratospheric Cly and Bry and to the stratospheric cooling induced by increasing well mixed greenhouse gases, thus slowing down gas-phase reactions that destroy ozone in the upper stratosphere. The ozone increase in the mid-upper troposphere is largely regulated by the increasing strength of the Brewer-Dobson circulation, which moves more ozone from the tropics to the extratropics and enhances the tropospheric influx from the lowermost stratosphere. This climate feedback mechanism on tropospheric ozone is only partially compensated by the increasing chemical ozone loss associated to higher H2O values in response to the tropospheric warming. We also note that ozone trends obtained in the lower stratosphere are negative (−2.2 percent/decade), but do not result to be statistically significant in our analyses.
Stratospheric ozone intrusion events and their impacts on tropospheric ozone
Publisher: Copernicus GmbH
Date: 05-01-2017
Abstract: Abstract. Stratosphere-to-troposphere transport (STT) provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the southern hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality and quantify the ozone transported across the tropopause over Davis (69° S), Macquarie Island (54° S), and Melbourne (38° S). STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile, and an analysis of the Brunt-Viäsälä frequency. Using a bandpass filter on 7–9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter above all three sites. The majority of tropospheric ozone enhancements from STT events occur within 2.5 km, 3 km of the tropopause at Davis, and Macquarie Island. Events are more spread out at Melbourne, occurring frequently up to 7.5 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is 2–4 % at each site however, during in idual events over 10 % of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, these are apparent during austral winter and spring, and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely resolved to distinguish STT events but is able to accurately simulate the seasonal cycle of tropospheric ozone columns over the three southern hemisphere sites. Combining the ozonesonde-derived STT event characteristics with the simulated tropospheric ozone columns from GEOS-Chem, we conservatively estimate that the annual tropospheric ozone flux over the Southern Ocean due to STT events is ~ 3.2 ×1016 molecules cm−2 yr−1. This value is significantly lower than expected from previous global estimates due to the conservative nature of several components of our calculation, in particular the contribution of STT to total tropospheric ozone during an event (STT impact). Using an assumed STT impact of 35 % based on prior modelling studies rather than our observational estimate of 2–4 % increases the estimated Southern Ocean flux by an order of magnitude. Despite lingering uncertainties in scaling ozonesonde measurements to regional values, ozonesonde datasets provide a useful tool for STT detection, and the analysis methods described in this paper could be applied to many existing long-term records.
A Clean Air Plan for Sydney: An Overview of the Special Issue on Air Quality in New South Wales
Publisher: MDPI AG
Date: 04-12-2019
Abstract: This paper presents a summary of the key findings of the special issue of Atmosphere on Air Quality in New South Wales and discusses the implications of the work for policy makers and in iduals. This special edition presents new air quality research in Australia undertaken by (or in association with) the Clean Air and Urban Landscapes hub, which is funded by the National Environmental Science Program on behalf of the Australian Government’s Department of the Environment and Energy. Air pollution in Australian cities is generally low, with typical concentrations of key pollutants at much lower levels than experienced in comparable cities in many other parts of the world. Australian cities do experience occasional exceedances in ozone and PM2.5 (above air pollution guidelines), as well as extreme pollution events, often as a result of bushfires, dust storms, or heatwaves. Even in the absence of extreme events, natural emissions play a significant role in influencing the Australian urban environment, due to the remoteness from large regional anthropogenic emission sources. By studying air quality in Australia, we can gain a greater understanding of the underlying atmospheric chemistry and health risks in less polluted atmospheric environments, and the health benefits of continued reduction in air pollution. These conditions may be representative of future air quality scenarios for parts of the Northern Hemisphere, as legislation and cleaner technologies reduce anthropogenic air pollution in European, American, and Asian cities. However, in many instances, current legislation regarding emissions in Australia is significantly more lax than in other developed countries, making Australia vulnerable to worsening air pollution in association with future population growth. The need to avoid complacency is highlighted by recent epidemiological research, reporting associations between air pollution and adverse health outcomes even at air pollutant concentrations that are lower than Australia’s national air quality standards. Improving air quality is expected to improve health outcomes at any pollution level, with specific benefits projected for reductions in long-term exposure to average PM2.5 concentrations.
Tropospheric ozone in CCMI models and Gaussian process emulation to understand biases in the SOCOLv3 chemistry–climate model
Publisher: Copernicus GmbH
Date: 13-11-2018
DOI: 10.5194/ACP-18-16155-2018
Abstract: Abstract. Previous multi-model intercomparisons have shown that chemistry–climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC–IGAC (Stratosphere–troposphere Processes And their Role in Climate–International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40 %–50 % in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ∼30 % in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33 % larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, “SOCOLv3.1”, which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx), carbon monoxide, methane and other volatile organic compounds, VOCs) are responsible for more than 90 % of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20 % more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry–climate models.
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