Search

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.

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 amplitude 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 amplitude 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 hampered by the Andes. Therefore, over the 21st century, influence from ozone recovery causes a westward shift and a decrease in amplitude. 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 amplitude. 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.

Objective: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.Design:Observational study.Setting:A single ward of a tertiary-care public hospital in Melbourne, Australia.Intervention: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].Results: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.Conclusions: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.

Emission inventories are a fundamental input for atmospheric chemical transport models in order to accurately simulate air pollution and its impacts. In Australia, emission inventories are currently not available for electricity generators at high temporal and spatial resolutions. In this study, a new high spatial and temporal resolution inventory for Australian power plant emissions has been developed. The emissions from coal- and gas-fired power plants have been estimated using 5-min electricity generation time-series data and emission factors. The emissions are estimated from 2010 to 2019 for sulfur dioxide ( $$\hbox {SO}_2$$ ), nitrogen oxide ( $$\hbox {NO}_{2}$$ ), particulate matter (PM) and mercury (Hg). We estimate that, for 2019, the coal-fired power plants in Australia emitted significant amounts of $$\hbox {SO}_2$$ (485.7 kTonne) and $$\hbox {NO}_{2}$$ (452 kTonne), as there are no sulfur dioxide or nitrogen oxide controls in place. In contrast, PM emissions are mitigated by particulate matter control devices and coal-fired power plants emit an estimated 27.48 and 13.46 kTonne of $$\hbox {PM}_{10}$$ and $$\hbox {PM}_{2.5}$$ , respectively. Coal-fired power plants were responsible for an estimated 3.13 tonnes of Hg emissions. Gas-fired plant emissions are significantly lower than coal-fired power emissions for all pollutants. Temporal analysis showed that coal- and gas-fired power plant emissions vary quite markedly during the day and over the week. There is a strong diurnal cycle in the gas-fired emissions, which, if ignored by assuming constant emissions (such as is routinely done), will lead to significant errors in modeled air pollution.

BackgroundHealthcare 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.MethodsWe nebulised 109 plaque forming units (PFU) of bacteriophage PhiX174 virus into a 35.1m3 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.ResultsMedian airborne viral concentration in the room reached 1.41 × 105 PFU.m-3 with the hood inactive. Using the active hood as source containment reduced infectious virus concentration by 374-fold in air samples. 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.ConclusionsThe 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.Lay summaryCOVID-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.

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.

BACKGROUND: The design of cities has been heavily influenced by the needs of private motor vehicles, resulting in significant population and planetary health challenges. Death and injury due to motor vehicle crashes is now the world’s 5(th) leading cause of mortality and morbidity and motor vehicle-related air pollution accounts for 4.2 million deaths per year. This study highlights the global importance of urban design as a factor through which challenges associated with rapid motorisation and road transport injury may be mitigated. METHODS: Urban characteristics were obtained from sample maps for 1692 cities capturing one third of the world’s population. Applying a combined convolutional neural network and graph-based approach, cities were classified into unique types based on selected urban design characteristics represented in sample maps. Associations between identified city types and the burden of road transport injury were estimated using data from the most recent Global Burden of Disease (GBD) study while controlling for the effect of economic activity. FINDINGS: After screening for outliers, nine city types based on 1632 cities were identified that captured the diversity of global urban design configurations and were associated with differences in road transport injury rates. After controlling for economic activity at the city level, burden of road transport injury was an estimated 2x higher (RR=2.00) for the poorest performing city type as compared to the best performing city type. An estimated total loss of 9.6 million DALYs per year to road transport injury were attributed to suboptimal urban design. In general, city types that emphasised combined dense road networks with smaller blocks and more prevalent railed public transport networks demonstrated the lowest rates of road traffic injury per person. INTERPRETATION: With a 2-fold difference observed in the total estimated burden of road transport injury between the best performing city type and the worst performing city types, this study highlights the important role that urban design can play in creating circumstances for the generation of road traffic injury. More upstream investment in promoting urban design that supports transport mode shift that places people within lower risk transport modes such as rail or safe active transport could deliver consequent reductions in road transport injury.

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

International audience; 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.

Summary Background While the range of possible transmission pathways of severe acute respiratory syndrome coronavirus-2 in various settings has been investigated thoroughly, most authorities have recently acknowledged the role of aerosol spread in its transmission, especially in indoor environments where ventilation is poor. Engineering controls are needed to mitigate aerosol transmission in high-risk settings including hospital wards, classrooms and offices. Aim To assess the effectiveness of aerosol filtration by portable air cleaning devices with high-efficiency particulate air filters used in addition to a standard building heating ventilation and air conditioning (HVAC) system. Methods Test rooms, including a single-bed hospital room, were filled with test aerosol to simulate aerosol movement. Aerosol counts were measured over time with various portable air cleaning devices and room ventilation systems to quantify the overall aerosol clearance rate. Findings Portable air cleaning devices were very effective for removal of aerosols. The aerosols were cleared five times faster in a small control room with portable air cleaning devices than in the room with HVAC alone. The single-bed hospital room had an excellent ventilation rate (∼14 air changes per hour) and cleared the aerosols in 20 min. However, with the addition of two air cleaning devices, the clearance time was three times faster. Conclusions Inexpensive portable air cleaning devices should be considered for small and enclosed spaces in healthcare settings, such as inpatient rooms and personal protective equipment donning/doffing stations. Portable air cleaning devices are particularly important where there is limited ability to reduce aerosol transmission with building HVAC ventilation.

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 campaign 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.

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.

ObjectiveTo assess the effectiveness of aerosol filtration by portable air cleaning devices with high efficiency particulate air (HEPA) filters used in addition to standard building heating ventilation and air-conditioning (HVAC).MethodsTest rooms, including a hospital single-patient room, were filled with test aerosol to simulate aerosol movement. Aerosol counts were measured over time with various portable air cleaning devices and room ventilation systems to quantify the aerosol concentration reduction rate and overall clearance rate.ResultsPortable air cleaners were very effective in removing aerosols, especially for the devices with high flow rate. In a small control room, the aerosols were cleared 4 to 5 times faster with portable air cleaners than the room with HVAC alone. A single bed hospital room equipped with an excellent ventilation rate (∼ 14 air changes per hour) can clear the aerosols in 20 minutes. However, with the addition of two air cleaners, the clearance time became 3 times faster (in 6 minutes and 30 seconds).ConclusionsPortable air cleaning devices with HEPA filtration were highly effective at removing aerosols. To clear aerosols (above 90% clearance) in under 10 minutes requires around 25 air changes per hour; readily feasible with air cleaners. Inexpensive portable air cleaning devices should be considered for small and enclosed spaces in health care settings such as inpatient rooms, personal protective equipment donning/doffing stations, and staff tea rooms. Portable air cleaners are particularly important where there is limited ability to reduce aerosol transmission with building HVAC ventilation.

ObjectiveTo 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 COVID-19, and to examine the impact of portable air cleaners on aerosol clearance.DesignObservational studySettingA single ward of a tertiary public hospital in Melbourne AustraliaInterventionGlycerine-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 (also called portable HEPA filters).ResultsAerosols 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 two small domestic air cleaners in a single patient room of a hospital ward, 99% of aerosols could be cleared within 5.5 minutes.ConclusionAir cleaners may be useful in clinical spaces to help reduce the risk of healthcare acquired 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

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.

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 sampling in power generation regions, even after the closure of coal fired power stations, will have important implications to understanding the airborne mercury emissions sources.

International audience; Ozone profile measurements collected at L'Aquila (Italy, 42.4°N) during seventeen years of radio-sounding 30 (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 https://doi.org/10.5194/acp-2020-525 Preprint. Discussion started: 1 July 2020 c Author(s) 2020. CC BY 4.0 License. 2 (+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 35 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 40 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.

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.

To quantify aerosol generation from respiratory interventions and the effectiveness of their removal by a personal ventilation hood.Determination of the aerosol particle generation (in a single, healthy volunteer in a clean room) associated with breathing, speaking, wet coughing, oxygen (OAerosol generation was measured with two particle sizer and counter devices, focusing on aerosols 0.5-5 μm (human-generated aerosols), with and without the hood. An increase from baseline of less than 0.3 particles per mL was considered a low level of generation.Comparisons of aerosol generation between different respiratory interventions. Effectiveness of aerosol reduction by a personal ventilation hood.Results for the 0.5-5 μm aerosol range. Quiet breathing and talking demonstrated very low increase in aerosols (0.1 particles/mL). Aerosol generation was low for wet coughing (0.1 particles/mL), OIn this human volunteer study, the administration of O

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 individual 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.

Two and a half years of multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of nitrogen dioxide (NO

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.

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.

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).

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 samples to a unique time-series of aerosol samples 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&ndash, 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.

30 pags., 11 figs., 5 tabs., We quantify the stratospheric injection of brominated very short-lived substances (VSLS) based on aircraft observations acquired in winter 2014 above the Tropical Western Pacific during the CONvective TRansport of Active Species in the Tropics (CONTRAST) and the Airborne Tropical TRopopause EXperiment (ATTREX) campaigns. The overall contribution of VSLS to stratospheric bromine was determined to be 5.0 ± 2.1 ppt, in agreement with the 5 ± 3 ppt estimate provided in the 2014 World Meteorological Organization (WMO) Ozone Assessment report (WMO 2014), but with lower uncertainty. Measurements of organic bromine compounds, including VSLS, were analyzed using CFC-11 as a reference stratospheric tracer. From this analysis, 2.9 ± 0.6 ppt of bromine enters the stratosphere via organic source gas injection of VSLS. This value is two times the mean bromine content of VSLS measured at the tropical tropopause, for regions outside of the Tropical Western Pacific, summarized in WMO 2014. A photochemical box model, constrained to CONTRAST observations, was used to estimate inorganic bromine from measurements of BrO collected by two instruments. The analysis indicates that 2.1 ± 2.1 ppt of bromine enters the stratosphere via inorganic product gas injection. We also examine the representation of brominated VSLS within 14 global models that participated in the Chemistry-Climate Model Initiative. The representation of stratospheric bromine in these models generally lies within the range of our empirical estimate. Models that include explicit representations of VSLS compare better with bromine observations in the lower stratosphere than models that utilize longer-lived chemicals as a surrogate for VSLS., The CONTRAST field deployment was supported by the U.S. NSF, and the ATTREX field deployment was supported by the National Aeronautics and Space Administration (NASA). P. A. W., R. J. S., T. P. C., J. M. N., and D. C. A. received support from NSF, NASA Atmospheric Composition Modeling and Analysis Program (ACMAP), and the NASA Modeling, Analysis, and Prediction (MAP). D. C. A. also received support from the NASA Upper Atmospheric Research Program. J. M. N. was also supported by the NASA Postdoctoral Program at the NASA Goddard Space Flight Center, administered by Universities Space Research Association under contract with NASA. R. V. acknowledges funding from NSF awards AGS‐1261740 and AGS‐1620530. CONTRAST data are publicly available at “http://data.eol.ucar.edu/master_list/?project= CONTRAST.” ATTREX data are publicly available at “https://espoarchive.nasa.gov/archive/browse/attrex/id4/GHawk.” The National Center for Environmental Prediction (NCEP) meteorological data are available at “https://doi.org/10.5065/D6M043C6.” CCMI outputs from CESM1‐WACCM and CESM1‐CAM4Chem are archived by the National Center for Atmospheric Research (NCAR) at “www.earthsystemgrid.org,” and NCAR is sponsored by NSF. CCMI output from the EMAC‐L90MA‐SD simulation is available at “https://doi.org/10.5281/zenodo.1204495.” All other CCMI simulations are archived by the British Atmospheric Data Centre at “http://badc.nerc.ac.uk/”. Output from CAM‐chem‐SD is available as “NCAR/ACD CAMChem 1 Degree Forecast” at “http://catalog.eol.ucar.edu/contrast/model/CAMChem_NCAR_1deg/.” WACCM and CAM‐Chem are components of the Community Earth System Model (CESM), which is also supported by NSF. Computing resources were provided by NCAR's Climate Simulation Laboratory, sponsored by NSF and other agencies. This research was enabled by the computational and storage resources of NCAR's Computational and Information System Laboratory (CISL). R. S. and K. A. S., with ACCESS‐CCM, acknowledge support from Australian Research Council's Centre of Excellence for Climate System Science (CE110001028), the Australian Government's National Computational Merit Allocation Scheme (q90), and Australian Antarctic science grant program (FoRCES 4012). CCSRNIES research was supported by the Environment Research and Technology Development Fund (2‐1303 and 2‐1709) of the Ministry of the Environment, Japan, and computations were performed on NEC‐SX9/A(ECO) computers at the CGER, NIES. The EMAC simulations have been performed at the German Climate Computing Centre (DKRZ) through support from the Bundesministerium für Bildung und Forschung (BMBF). DKRZ and its scientific steering committee are gratefully acknowledged for providing the HPC and data archiving resources for the consortial project ESCiMo (Earth System Chemistry integrated Modelling). The TOMCAT modeling was supported by NERC NCAS and the SISLAC project (NE/R001782/1), and the simulations were performed on the Archer and Leeds HPC Systems.

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.

The rapid environmental changes in Australia prompt a more thorough investigation of the influence of transportation, local emissions, and optical–chemical properties on aerosol production across the region. A month-long intensive measurement campaign was conducted during spring 2016 at Mission Beach, a remote coastal site west of the Great Barrier Reef (GBR) on the north-east coast of Australia. One aerosol pollution episode was investigated in early October. This event was governed by meteorological conditions and characterized by the increase in black carbon (BC) mass concentration (averaged value of 0.35 ± 0.20 μg m−3). Under the influence of the continental transportation, a new layer of nucleation-mode aerosols with an initial size diameter of 20 nm was observed and aerosol number concentrations reached the peak of 6733 cm−3 at a diameter of 29 nm. The averaged aerosol extinction coefficient at the height of 2 km was 150 Mm−1, with a small depolarized ratio (3.5–5%). Simultaneously, the boundary layer height presented a fall–rise trend in the presence of these enhanced aerosol concentrations and became stable in a later stage of the episode. We did not observe clear boundary layer height diurnal variations from the LiDAR observations or from the Weather Research and Forecasting (WRF) model outputs, except in an earlier stage of the aerosol episode for the former. Although the sea breeze may have been responsible for these particles, on the balance of available data, we suggest that the aerosol properties at the GBR surface during this period are more likely influenced by regional transportation of continental sources, including biomass-burning aerosols.

Poor air quality is an emerging problem in Australia primarily due to ozone pollution events and lengthening and more severe wildfire seasons. A significant deterioration in air quality was experienced in Australia's most populous cities, Melbourne and Sydney, as a result of fires during the so-called Black Summer which ran from November 2019 through to February 2020. Following this period, social, mobility and economic restrictions to curb the spread of the COVID-19 pandemic were implemented in Australia. We quantify the air quality impact of these contrasting periods in the south-eastern states of Victoria and New South Wales (NSW) using a meteorological normalisation approach. A Random Forest (RF) machine learning algorithm was used to compute baseline time series' of nitrogen dioxide (NO2), ozone (O3), carbon monoxide CO and particulate matter with diameter < 2.5 μm (PM2.5), based on a 19 year, detrended training dataset. Across Victorian sites, large increases in CO (188%), PM2.5 (322%) and ozone (22%) were observed over the RF prediction in January 2020. In NSW, smaller pollutant increases above the RF prediction were seen (CO 58%, PM2.5 80%, ozone 19%). This can be partly explained by the RF predictions being high compared to the mean of previous months, due to high temperatures and strong wind speeds, highlighting the importance of meteorological normalisation in attributing pollution changes to specific events. From the daily observation-RF prediction differences we estimated 249.8 (95% CI: 156.6-343.) excess deaths and 3490.0 (95% CI 1325.9-5653.5) additional hospitalisations were likely as a result of PM2.5 and O3 exposure in Victoria and NSW. During April 2019, when COVID-19 restrictions were in place, on average NO2 decreased by 21.5 and 8% in Victoria and NSW respectively. O3 and PM2.5 remained effectively unchanged in Victoria on average but increased by 20 and 24% in NSW respectively, supporting the suggestion that community mobility reduced more in Victoria than NSW. Overall the air quality change during the COVID-19 lockdown had a negligible impact on the calculated health outcomes.

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.

Ozone depletion events in the polar troposphere have been linked to extremely high concentrations of bromine, known as bromine explosion events (BEE). However, the optimum meteorological conditions for the occurrence of these events remain uncertain. On 4–5 April 2011, a combination of both blowing snow and a stable shallow boundary layer was observed during a BEE at Eureka, Canada (86.4°W, 80.1°N). Measurements made by a Multi-Axis Differential Optical Absorption Spectroscopy spectrometer were used to retrieve BrO profiles and partial columns. During this event, the near-surface BrO volume mixing ratio increased to ~20 parts per trillion by volume, while ozone was depleted to ~1 ppbv from the surface to 700 m. Back trajectories and Global Ozone Monitoring Experiment-2 satellite tropospheric BrO columns confirmed that this event originated from a bromine explosion over the Beaufort Sea. From 30 to 31 March, meteorological data showed high wind speeds (24 m/s) and elevated boundary layer heights (~800 m) over the Beaufort Sea. Long-distance transportation (~1800 km over 5 days) to Eureka indicated strong recycling of BrO within the bromine plume. This event was generally captured by a global chemistry-climate model when a sea-salt bromine source from blowing snow was included. A model sensitivity study indicated that the surface BrO at Eureka was controlled by both local photochemistry and boundary layer dynamics. Comparison of the model results with both ground-based and satellite measurements confirmed that the BEE observed at Eureka was triggered by transport of enhanced BrO from the Beaufort Sea followed by local production/recycling under stable atmospheric shallow boundary layer conditions.

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.

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 individual 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.

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 individuals. 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.

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.

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.