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Quantitative understanding of the sources and sinks of greenhouse gases is essential for predicting greenhouse-gas-climate feedback processes and their impacts on climate variability and change. Australia plays a significant role in driving variability in global carbon cycling, but the budgets of carbon gases in Australia remain highly uncertain. Here, shipborne Fourier transform infrared spectrometer measurements collected around Australia are used together with a global chemical transport model (GEOS-Chem) to analyse the variability of three direct and indirect carbon greenhouse gases: carbon dioxide (CO2), methane (CH4) and carbon monoxide (CO). Using these measurements, we provide an updated distribution of these gases. From the model, we quantify their sources and sinks, and we exploit the benefits of multi-species analysis to explore co-variations to constrain relevant processes. We find that for all three gases, the eastern Australian coast is largely influenced by local anthropogenic sources, while the southern, western and northern coasts are characterised by a mixture of anthropogenic and natural sources. Comparing coincident and co-located enhancements in the three carbon gases highlighted several common sources from the Australian continent. We found evidence for 17 events with similar enhancement patterns indicative of co-emission and calculated enhancement ratios and modelled source contributions for each event. We found that anthropogenic co-enhancement events are common along the eastern coast, while co-enhancement events in the tropics primarily derive from biomass burning sources. While the GEOS-Chem model generally reproduced the timing of co-enhancement events, it was less able to reproduce the magnitude of enhancements. We used these differences to identify underestimated, overestimated and missing processes in the model. We found model overestimates of CH4 from coal burning and underestimates of all three gases from biomass burning. We identifi

A field aerosol measurement campaign as part of the Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign was conducted between 16 January 2013 and 15 February 2013 in the coastal city of Wollongong, Australia. The objectives of this research were to study the occurrence frequency, characteristics and factors that influence new particle formation processes. Particle formation and growth events were observed from particle number size distribution data in the range of 14 nm-660 nm measured using a scanning particle mobility sizer (SMPS). Four weak Class I particle formation and growth event days were observed, which is equivalent to 13% of the total observation days. The events occurred during the day, starting after 8:30 Australian Eastern Standard time with an average duration of five hours. The events also appeared to be positively linked to the prevailing easterly to north easterly sea breezes that carry pollutants from sources in and around Sydney. This suggests that photochemical reactions and a combination of oceanic and anthropogenic air masses are among the factors that influenced these events.

Urbanisation largely consists of removing native vegetation. Plants that remain interact with air quality in complex ways. Pollutants can be detrimental to plant growth; plants sometimes reduce air quality, yet some species also improve it through phytoremediation. A common pollutant of concern to human health in urban areas is particulate matter (PM), small particles of solid or liquid. Our study compared roadside moss turfs with leaves of a common Australian tree species, Pittosporum undulatum, in their ability to capture PM along an urban gradient. We sampled nine sites, three in each of three levels of urbanisation: low, medium, and high according to road type (freeway, suburban road, quiet peri-urban road). In addition, we deployed a PM monitor over a two-week period in one site of each urban level to provide concentrations of PM2.5. We used chlorophyll fluorescence (Fv/Fm; maximum quantum yield of photosystem II) as a measure of plant stress. We extracted PM in three size fractions using a filtration and washing technique with water and chloroform. Site averages for moss turfs were between 5.60 and 33.00 mg per g dry weight for total PM compared to between 2.15 and 10.24 mg per g dry weight for the tree leaves. We found that moss was more sensitive to increasing urbanisation, both in terms of trapping proportionately more PM than the leaves, and also in terms of photosynthetic stress, with moss Fv/Fm declining by a site average of 40% from low to high urban "class" (0.76 to 0.45). Our study highlights the stressors potentially limiting moss persistence in cities. It also demonstrates its ability to trap PM, a trait that could be useful in urban applications relating to urban greening or air quality.

Plants in urban areas interact with air quality in numerous ways. Firstly, pollutants from industry, vehicular and residential sources can be detrimental to plant growth. Secondly, plants sometimes contribute to poor air quality, for instance by emitting allergens such as pollen, or by trapping pollutants in street canyons and thirdly, with appropriate placement some species improve air quality through phytoremediation. A common urban pollutant is particulate matter (PM - small particles of solid or liquid). While this is of concern to human health, less well known is its effect on vegetation and while moss is commonly studied as a biomonitor, there is little research on how it is affected by urbanisation. Our objective was to measure PM entrapment by roadside moss turfs and compare it to leaves of a common Australian tree species, Pittosporum undulatum on an urban gradient.

2019 by the authors. 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 concent

Motivated by public interest, the Clean Air and Urban Landscapes (CAUL) hub deployed instrumentation to measure air quality at a roadside location in Sydney. The main aim was to compare concentrations of fine particulate matter (PM2.5) measured along a busy road section with ambient regional urban background levels, as measured at nearby regulatory air quality stations. The study also explored spatial and temporal variations in the observed PM2.5 concentrations. The chosen area was Randwick in Sydney, because it was also the subject area for an agent-based traffic model. Over a four-day campaign in February 2017, continuous measurements of PM2.5 were made along and around the main road. In addition, a traffic counting application was used to gather data for evaluation of the agent-based traffic model. The average hourly PM2.5 concentration was 13 µg/m3, which is approximately twice the concentrations at the nearby regulatory air quality network sites measured over the same period. Roadside concentrations of PM2.5 were about 50% higher in the morning rush-hour than the afternoon rush hour, and slightly lower (reductions of <30%) 50 m away from the main road, on cross-roads. The traffic model under-estimated vehicle numbers by about 4 fold, and failed to replicate the temporal variations in traffic flow, which we assume was due to an influx of traffic from outside the study region dominating traffic patterns. Our findings suggest that those working for long hours outdoors at busy roadside locations are at greater risk of suffering detrimental health effects associated with higher levels of exposure to PM2.5. Furthermore, the worse air quality in the morning rush hour means that, where possible, joggers and cyclists should avoid busy roads around these times.

Airborne particulate matter (PM) is a major health risk in urban settings. Ammonia (NH3) from vehicle exhaust is an under-recognised ingredient in the formation of inorganic PM and there remains a shortage of data to properly quantify the role of NH3 from vehicles in PM formation. An Open-path Fourier transform infra-red (OP-FTIR) spectrometer measured atmospheric NH3, carbon monoxide (CO) and carbon dioxide (CO2) at high temporal resolution (5 min) in Western Sydney over 11 months. The oxides of nitrogen (NO2 and NO; NOx) and sulphur dioxide (SO2) were measured at an adjacent air quality monitoring station. NH3 levels were maxima in the morning and evening coincident with peak traffic. During peak traffic NH3:CO ratio ranged from 0.018 to 0.022 ppbv:ppbv. Results were compared with the Greater Metropolitan Region 2008 (GMR2008) emissions inventory. Measured NH3:CO was higher during peak traffic times than the GMR2008 emissions estimates, indicating an underestimation of vehicle NH3 emissions in the inventory. Measurements also indicated the urban atmosphere was NH3 rich for the formation of ammonium sulphate ((NH4)2SO4) particulate was SO2 limited while the formation of ammonium nitrate (NH4NO3) was NH3 limited. Any reduction in NOx emissions with improved catalytic converter efficiency will be accompanied by an increase in NH3 production and potentially with an increase in NH4NO3 particulate.

In this study, we present ground-based measurements of column-averaged dry-air mole fractions (DMFs) of CO2 (or XCO2) taken in a semiarid region of Australia with an EM27/SUN portable spectrometer equipped with an automated clamshell cover. We compared these measurements to space-based XCO2 retrievals from the Greenhouse Gases Observing Satellite (GOSAT). Side-by-side measurements of EM27/SUN with the Total Carbon Column Observing Network (TCCON) instrument at the University of Wollongong were conducted in 2015-2016 to derive an XCO2 scaling factor of 0.9954 relative to TCCON. Although we found a slight drift of 0.13 % over 3 months in the calibration curve of the EM27/SUN vs. TCCON XCO2, the alignment of the EM27/SUN proved stable enough for a 2-week campaign, keeping the retrieved Xair values, another measure of stability, to within 0.5 % and the modulation efficiency to within 2 %. From the measurements in Alice Springs, we confirm a small bias of around 2 ppm in the GOSAT M-gain to H-gain XCO2 retrievals, as reported by the NIES GOSAT validation team. Based on the reported random errors from GOSAT, we estimate the required duration of a future campaign in order to better understand the estimated bias between the EM27/SUN and GOSAT. The dataset from the Alice Springs measurements is accessible at https://doi.org/10.4225/48/5b21f16ce69bc (Velazco et al., 2018).

The response of atmospheric composition to ongoing environmental change remains poorly constrained across much of the Southern Hemisphere. We use a 20-year record of ground-based total column measurements from Wollongong, southeast Australia to identify a statistically significant decreasing trend in formaldehyde of −1.9 [−2.2, −1.7]%/year. The trend is consistently negative across all months except November. Satellite data indicate that the trend at Wollongong is distinctly local and is superimposed on a regional-scale increase likely driven by changes in methane. In austral summer, coincident changes in hydrogen cyanide suggest that decreases in local biomass burning can only partly explain the observed trend. In the absence of other explanations, we infer that the observed formaldehyde trend is likely driven by decreasing industrial emissions. In November, an observed increasing temperature trend is consistent with an earlier onset of biogenic emissions in the region, driving increased biogenic formaldehyde that counteracts the overall decrease.

A field aerosol measurement campaign as part of the Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign was conducted between 16 January 2013 and 15 February 2013 in the coastal city of Wollongong, Australia. The objectives of this research were to study the occurrence frequency, characteristics and factors that influence new particle formation processes. Particle formation and growth events were observed from particle number size distribution data in the range of 14 nm-660 nm measured using a scanning particle mobility sizer (SMPS). Four weak Class I particle formation and growth event days were observed, which is equivalent to 13% of the total observation days. The events occurred during the day, starting after 8:30 Australian Eastern Standard time with an average duration of five hours. The events also appeared to be positively linked to the prevailing easterly to north easterly sea breezes that carry pollutants from sources in and around Sydney. This suggests that photochemical reactions and a combination of oceanic and anthropogenic air masses are among the factors that influenced these events.

Quantitative understanding of the sources and sinks of greenhouse gases is essential for predicting greenhouse-gas-climate feedback processes and their impacts on climate variability and change. Australia plays a significant role in driving variability in global carbon cycling, but the budgets of carbon gases in Australia remain highly uncertain. Here, shipborne Fourier transform infrared spectrometer measurements collected around Australia are used together with a global chemical transport model (GEOS-Chem) to analyse the variability of three direct and indirect carbon greenhouse gases: carbon dioxide (CO2), methane (CH4) and carbon monoxide (CO). Using these measurements, we provide an updated distribution of these gases. From the model, we quantify their sources and sinks, and we exploit the benefits of multi-species analysis to explore co-variations to constrain relevant processes. We find that for all three gases, the eastern Australian coast is largely influenced by local anthropogenic sources, while the southern, western and northern coasts are characterised by a mixture of anthropogenic and natural sources. Comparing coincident and co-located enhancements in the three carbon gases highlighted several common sources from the Australian continent. We found evidence for 17 events with similar enhancement patterns indicative of co-emission and calculated enhancement ratios and modelled source contributions for each event. We found that anthropogenic co-enhancement events are common along the eastern coast, while co-enhancement events in the tropics primarily derive from biomass burning sources. While the GEOS-Chem model generally reproduced the timing of co-enhancement events, it was less able to reproduce the magnitude of enhancements. We used these differences to identify underestimated, overestimated and missing processes in the model. We found model overestimates of CH4 from coal burning and underestimates of all three gases from biomass burning. We identifi

Volatile organic compounds (VOCs) are important precursors to the formation of ozone and fine particulate matter, the two pollutants of most concern in Sydney, Australia. Despite this importance, there are very few published measurements of ambient VOC concentrations in Australia. In this paper, we present mole fractions of several important VOCs measured during the campaign known as MUMBA (Measurements of Urban, Marine and Biogenic Air) in the Australian city of Wollongong (34°S). We particularly focus on measurements made during periods when clean marine air impacted the measurement site and on VOCs of biogenic origin. Typical unpolluted marine air mole fractions during austral summer 2012-2013 at latitude 34°S were established for CO2 (391.0 ± 0.6 ppm), CH4 (1760.1 ± 0.4 ppb), N2O (325.04 ± 0.08 ppb), CO (52.4 ± 1.7 ppb), O3 (20.5 ± 1.1 ppb), acetaldehyde (190 ± 40 ppt), acetone (260 ± 30 ppt), dimethyl sulphide (50 ± 10 ppt), benzene (20 ± 10 ppt), toluene (30 ± 20 ppt), C8H10 aromatics (23 ± 6 ppt) and C9H12 aromatics (36 ± 7 ppt). The MUMBA site was frequently influenced by VOCs of biogenic origin from a nearby strip of forested parkland to the east due to the dominant north-easterly afternoon sea breeze. VOCs from the more distant densely forested escarpment to the west also impacted the site, especially during two days of extreme heat and strong westerly winds. The relative amounts of different biogenic VOCs observed for these two biomes differed, with much larger increases of isoprene than of monoterpenes or methanol during the hot westerly winds from the escarpment than with cooler winds from the east. However, whether this was due to different vegetation types or was solely the result of the extreme temperatures is not entirely clear. We conclude that the clean marine air and biogenic signatures measured during the MUMBA campaign provide useful information about the typical abundance of several key VOCs and can be used to constrain chemical transport mode

The ability of meteorological models to accurately characterise regional meteorology plays a crucial role in the performance of photochemical simulations of air pollution. As part of the research funded by the Australian government's Department of the Environment Clean Air and Urban Landscape hub, this study set out to complete an intercomparison of air quality models over the Sydney region. This intercomparison would test existing modelling capabilities, identify any problems and provide the necessary validation of models in the region. The first component of the intercomparison study was to assess the ability of the models to reproduce meteorological observations, since it is a significant driver of air quality. To evaluate the meteorological component of these air quality modelling systems, seven different simulations based on varying configurations of inputs, integrations and physical parameterizations of two meteorological models (the Weather Research and Forecasting (WRF) and Conformal Cubic Atmospheric Model (CCAM)) were examined. The modelling was conducted for three periods coinciding with comprehensive air quality measurement campaigns (the Sydney Particle Studies (SPS) 1 and 2 and the Measurement of Urban, Marine and Biogenic Air (MUMBA)). The analysis focuses on meteorological variables (temperature, mixing ratio of water, wind (via wind speed and zonal wind components), precipitation and planetary boundary layer height), that are relevant to air quality. The surface meteorology simulations were evaluated against observations from seven Bureau of Meteorology (BoM) Automatic Weather Stations through composite diurnal plots, Taylor plots and paired mean bias plots. Simulated vertical profiles of temperature, mixing ratio of water and wind (via wind speed and zonal wind components) were assessed through comparison with radiosonde data from the Sydney Airport BoM site. The statistical comparisons with observations identified systematic overestimations of win

The response of atmospheric composition to ongoing environmental change remains poorly constrained across much of the Southern Hemisphere. We use a 20-year record of ground-based total column measurements from Wollongong, southeast Australia to identify a statistically significant decreasing trend in formaldehyde of −1.9 [−2.2, −1.7]%/year. The trend is consistently negative across all months except November. Satellite data indicate that the trend at Wollongong is distinctly local and is superimposed on a regional-scale increase likely driven by changes in methane. In austral summer, coincident changes in hydrogen cyanide suggest that decreases in local biomass burning can only partly explain the observed trend. In the absence of other explanations, we infer that the observed formaldehyde trend is likely driven by decreasing industrial emissions. In November, an observed increasing temperature trend is consistent with an earlier onset of biogenic emissions in the region, driving increased biogenic formaldehyde that counteracts the overall decrease.

In this study, we present ground-based measurements of column-averaged dry-air mole fractions (DMFs) of CO2 (or XCO2) taken in a semiarid region of Australia with an EM27/SUN portable spectrometer equipped with an automated clamshell cover. We compared these measurements to space-based XCO2 retrievals from the Greenhouse Gases Observing Satellite (GOSAT). Side-by-side measurements of EM27/SUN with the Total Carbon Column Observing Network (TCCON) instrument at the University of Wollongong were conducted in 2015-2016 to derive an XCO2 scaling factor of 0.9954 relative to TCCON. Although we found a slight drift of 0.13 % over 3 months in the calibration curve of the EM27/SUN vs. TCCON XCO2, the alignment of the EM27/SUN proved stable enough for a 2-week campaign, keeping the retrieved Xair values, another measure of stability, to within 0.5 % and the modulation efficiency to within 2 %. From the measurements in Alice Springs, we confirm a small bias of around 2 ppm in the GOSAT M-gain to H-gain XCO2 retrievals, as reported by the NIES GOSAT validation team. Based on the reported random errors from GOSAT, we estimate the required duration of a future campaign in order to better understand the estimated bias between the EM27/SUN and GOSAT. The dataset from the Alice Springs measurements is accessible at https://doi.org/10.4225/48/5b21f16ce69bc (Velazco et al., 2018).

Volatile organic compounds (VOCs) are important precursors to the formation of ozone and fine particulate matter, the two pollutants of most concern in Sydney, Australia. Despite this importance, there are very few published measurements of ambient VOC concentrations in Australia. In this paper, we present mole fractions of several important VOCs measured during the campaign known as MUMBA (Measurements of Urban, Marine and Biogenic Air) in the Australian city of Wollongong (34°S). We particularly focus on measurements made during periods when clean marine air impacted the measurement site and on VOCs of biogenic origin. Typical unpolluted marine air mole fractions during austral summer 2012-2013 at latitude 34°S were established for CO2 (391.0 ± 0.6 ppm), CH4 (1760.1 ± 0.4 ppb), N2O (325.04 ± 0.08 ppb), CO (52.4 ± 1.7 ppb), O3 (20.5 ± 1.1 ppb), acetaldehyde (190 ± 40 ppt), acetone (260 ± 30 ppt), dimethyl sulphide (50 ± 10 ppt), benzene (20 ± 10 ppt), toluene (30 ± 20 ppt), C8H10 aromatics (23 ± 6 ppt) and C9H12 aromatics (36 ± 7 ppt). The MUMBA site was frequently influenced by VOCs of biogenic origin from a nearby strip of forested parkland to the east due to the dominant north-easterly afternoon sea breeze. VOCs from the more distant densely forested escarpment to the west also impacted the site, especially during two days of extreme heat and strong westerly winds. The relative amounts of different biogenic VOCs observed for these two biomes differed, with much larger increases of isoprene than of monoterpenes or methanol during the hot westerly winds from the escarpment than with cooler winds from the east. However, whether this was due to different vegetation types or was solely the result of the extreme temperatures is not entirely clear. We conclude that the clean marine air and biogenic signatures measured during the MUMBA campaign provide useful information about the typical abundance of several key VOCs and can be used to constrain chemical transport mode

Air pollution and associated human exposure are important research areas in Greater Sydney, Australia. Several field campaigns were conducted to characterize the pollution sources and their impacts on ambient air quality including the Sydney Particle Study Stages 1 and 2 (SPS1 and SPS2), and the Measurements of Urban, Marine, and Biogenic Air (MUMBA). In this work, the Weather Research and Forecasting model with chemistry (WRF/Chem) and the coupled WRF/Chem with the Regional Ocean Model System (ROMS) (WRF/Chem-ROMS) are applied during these field campaigns to assess the models' capability in reproducing atmospheric observations. The model simulations are performed over quadruple-nested domains at grid resolutions of 81-, 27-, 9-, and 3-km over Australia, an area in southeastern Australia, an area in New South Wales, and the Greater Sydney area, respectively. A comprehensive model evaluation is conducted using surface observations from these field campaigns, satellite retrievals, and other data. This paper evaluates the performance of WRF/Chem-ROMS and its sensitivity to spatial grid resolutions. The model generally performs well at 3-, 9-, and 27-km resolutions for sea-surface temperature and boundary layer meteorology in terms of performance statistics, seasonality, and daily variation. Moderate biases occur for temperature at 2-m and wind speed at 10-m in the mornings and evenings due to the inaccurate representation of the nocturnal boundary layer and surface heat fluxes. Larger underpredictions occur for total precipitation due to the limitations of the cloud microphysics scheme or cumulus parameterization. The model performs well at 3-, 9-, and 27-km resolutions for surface O 3 in terms of statistics, spatial distributions, and diurnal and daily variations. The model underpredicts PM 2.5 and PM 10 during SPS1 and MUMBA but overpredicts PM 2.5 and underpredicts PM 10 during SPS2. These biases are attributed to inaccurate meteorology, precursor emissions, insuffi

2018 by the authors. Poor air quality is often associated with hot weather, but the quantitative attribution of high temperatures on air quality remains unclear. In this study, the effect of elevated temperatures on air quality is investigated in Greater Sydney using January 2013, a period of extreme heat during which temperatures at times exceeded 40 °C, as a case study. Using observations from 17 measurement sites and the Weather Research and Forecasting Chemistry (WRF-Chem) model, we analyse the effect of elevated temperatures on ozone in Sydney by running a number of sensitivity studies in which: (1) the model is run with biogenic emissions generated by MEGAN and separately run with monthly average Model of Emissions of Gases and Aerosols from Nature ( MEGAN) biogenic emissions (for January 2013); (2) the model results from the standard run are compared with those in which average temperatures (for January 2013) are only applied to the chemistry; (3) the model is run using both averaged biogenic emissions and temperatures; and (4 and 5) the model is run with half and zero biogenic emissions. The results show that the impact on simulated ozone through the effect of temperature on reaction rates is similar to the impact via the effect of temperature on biogenic emissions and the relative impacts are largely additive when compared to the run in which both are averaged. When averaged across 17 sites in Greater Sydney, the differences between ozone simulated under standard and averaged model conditions are as high as 16 ppbv. Removing biogenic emissions in the model has the effect of removing all simulated ozone episodes during extreme heat periods, highlighting the important role of biogenic emissions in Australia, where Eucalypts are a key biogenic source.

We present findings from the Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign, which took place in the coastal city of Wollongong in New SouthWales, Australia. We focus on a few key air quality indicators, along with a comparison to regional scale chemical transport model predictions at a spatial resolution of 1 km by 1 km. We find that the CSIRO chemical transport model provides accurate simulations of ozone concentrations at most times, but underestimates the ozone enhancements that occur during extreme temperature events. Themodel alsomeets previously published performance standards for fine particulate matter less than 2.5 microns in diameter (PM2.5), and the larger aerosol fraction (PM10). We explore the observed composition of the atmosphere within this urban air-shed during the MUMBA campaign and discuss the different influences on air quality in the city. Our findings suggest that further improvements to our ability to simulate air quality in this coastal city can be made through more accurate anthropogenic and biogenic emissions inventories and better understanding of the impact of extreme temperatures on air quality. The challenges in modelling air quality within the urban air-shed ofWollongong, including difficulties in accurate simulation of the local meteorology, are likely to be replicated in many other coastal cities in the Southern Hemisphere.

Among the more than 20 ground-based FTIR (Fourier transform infrared) stations currently operating around the globe, only a few have provided formaldehyde (HCHO) total column time series until now. Although several independent studies have shown that the FTIR measurements can provide formaldehyde total columns with good precision, the spatial coverage has not been optimal for providing good diagnostics for satellite or model validation. Furthermore, these past studies used different retrieval settings, and biases as large as 50% can be observed in the HCHO total columns depending on these retrieval choices, which is also a weakness for validation studies combining data from different ground-based stations. For the present work, the HCHO retrieval settings have been optimized based on experience gained from past studies and have been applied consistently at the 21 participating stations. Most of them are either part of the Network for the Detection of Atmospheric Composition Change (NDACC) or under consideration for membership. We provide the harmonized settings and a characterization of the HCHO FTIR products. Depending on the station, the total systematic and random uncertainties of an individual HCHO total column measurement lie between 12% and 27% and between 1 and 11x1014 moleccm-2, respectively. The median values among all stations are 13% and 2.9x1014 moleccm-2 for the total systematic and random uncertainties. This unprecedented harmonized formaldehyde data set from 21 ground-based FTIR stations is presented and its comparison with a global chemistry transport model shows consistency in absolute values as well as in seasonal cycles. The network covers very different concentration levels of formaldehyde, from very clean levels at the limit of detection (few 1013moleccm-2) to highly polluted levels (7x1016moleccm-2). Because the measurements can be made at any time during daylight, the diurnal cycle can be observed and is found to be significant at many station

Particle number size distributions are among the most important parameters in trying to understand the characteristics of particle population. Atmospheric particles were measured in an interaction of mixed environments in the Southeastern coastal city of Wollongong, Australia, during a comprehensive field campaign known as Measurements of Urban, Marine and Biogenic Air (MUMBA). MUMBA ran in summer season between 21 st December 2012 and 15 th February 2013. Particle number concentrations measured during this campaign were indicative of the interplay between marine environments and urban air which met the objective of this campaign. Particle number size distributions ranging from 14 nm to 660 nm in diameter, as measured by Scanning Mobility Particle Sizer (SMPS) in this study, were grouped using Principal Component Analysis. Based on strong component loadings (value ≥ 0.75), three different factors were identified (i) Small Factor (N S ): 15 nm < Dp < 50 nm, (ii) Medium Factor (N M ): 60 nm < Dp < 150 nm and (iii) Large Factor (N L ): 210 nm < Dp < 450 nm. The three factors describe 89% of the dataset cumulative variance. Particles in this region are dependent upon the interaction between the sources, and cannot be viewed as a simple mixture of biogenic and anthropogenic sources associated with various mechanical processes. The particles observed in the morning were found to be influenced by combustion emissions, presumably primarily from traffic, which is most obvious in N L . The particle population during the day was found to be influenced by a mixture of marine sources and secondary aerosols production initiated by photochemical oxidation. The local steel works and the urban environment were the major contributors of particles at night. Secondary organic aerosols were identified in this study by the mass ratio of organic carbon to elemental carbon (OC/EC). Biogenic sources influenced secondary organic aerosols formation as a moderate correlation (R 2 = 0.6) was ob

We characterised trace gas emissions from Australian temperate forest fires through a mixture of open-path Fourier transform infrared (OP-FTIR) measurements and selective ion flow tube mass spectrometry (SIFT-MS) and White cell FTIR analysis of grab samples. We report emission factors for a total of 25 trace gas species measured in smoke from nine prescribed fires. We find significant dependence on modified combustion efficiency (MCE) for some species, although regional differences indicate that the use of MCE as a proxy may be limited. We also find that the fire-integrated MCE values derived from our in situ on-the-ground open-path measurements are not significantly different from those reported for airborne measurements of smoke from fires in the same ecosystem. We then compare our average emission factors to those measured for temperate forest fires elsewhere (North America) and for fires in another dominant Australian ecosystem (savanna) and find significant differences in both cases. Indeed, we find that although the emission factors of some species agree within 20%, including those of hydrogen cyanide, ethene, methanol, formaldehyde and 1,3-butadiene, others, such as acetic acid, ethanol, monoterpenes, ammonia, acetonitrile and pyrrole, differ by a factor of 2 or more. This indicates that the use of ecosystem-specific emission factors is warranted for applications involving emissions from Australian forest fires.

Southeast Asia experiences frequent fires in fuel-rich tropical peatlands, leading to extreme episodes of regional haze with high concentrations of fine particulate matter (PM 2.5 ) impacting human health. In a study published recently, the first field measurements of PM 2.5 emission factors for tropical peat fires showed larger emissions than from other fuel types. Here we report even higher PM 2.5 emission factors, measured at newly ignited peat fires in Malaysia, suggesting that current estimates of fine particulate emissions from peat fires may be underestimated by a factor of 3 or more. In addition, we use both field and laboratory measurements of burning peat to provide the first mechanistic explanation for the high variability in PM 2.5 emission factors, demonstrating that buildup of a surface ash layer causes the emissions of PM 2.5 to decrease as the peat fire progresses. This finding implies that peat fires are more hazardous (in terms of aerosol emissions) when first ignited than when still burning many days later. Varying emission factors for PM 2.5 also have implications for our ability to correctly model the climate and air quality impacts downwind of the peat fires. For modelers able to implement a time-varying emission factor, we recommend an emission factor for PM 2.5 from newly ignited tropical peat fires of 58 g of PM 2.5 per kilogram of dry fuel consumed (g/kg), reducing exponentially at a rate of 9%/day. If the age of the fire is unknown or only a single value may be used, we recommend an average value of 24 g/kg.

We present findings from the Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign, which took place in the coastal city of Wollongong in New SouthWales, Australia. We focus on a few key air quality indicators, along with a comparison to regional scale chemical transport model predictions at a spatial resolution of 1 km by 1 km. We find that the CSIRO chemical transport model provides accurate simulations of ozone concentrations at most times, but underestimates the ozone enhancements that occur during extreme temperature events. Themodel alsomeets previously published performance standards for fine particulate matter less than 2.5 microns in diameter (PM2.5), and the larger aerosol fraction (PM10). We explore the observed composition of the atmosphere within this urban air-shed during the MUMBA campaign and discuss the different influences on air quality in the city. Our findings suggest that further improvements to our ability to simulate air quality in this coastal city can be made through more accurate anthropogenic and biogenic emissions inventories and better understanding of the impact of extreme temperatures on air quality. The challenges in modelling air quality within the urban air-shed ofWollongong, including difficulties in accurate simulation of the local meteorology, are likely to be replicated in many other coastal cities in the Southern Hemisphere.

We characterised trace gas emissions from Australian temperate forest fires through a mixture of open-path Fourier transform infrared (OP-FTIR) measurements and selective ion flow tube mass spectrometry (SIFT-MS) and White cell FTIR analysis of grab samples. We report emission factors for a total of 25 trace gas species measured in smoke from nine prescribed fires. We find significant dependence on modified combustion efficiency (MCE) for some species, although regional differences indicate that the use of MCE as a proxy may be limited. We also find that the fire-integrated MCE values derived from our in situ on-the-ground open-path measurements are not significantly different from those reported for airborne measurements of smoke from fires in the same ecosystem. We then compare our average emission factors to those measured for temperate forest fires elsewhere (North America) and for fires in another dominant Australian ecosystem (savanna) and find significant differences in both cases. Indeed, we find that although the emission factors of some species agree within 20%, including those of hydrogen cyanide, ethene, methanol, formaldehyde and 1,3-butadiene, others, such as acetic acid, ethanol, monoterpenes, ammonia, acetonitrile and pyrrole, differ by a factor of 2 or more. This indicates that the use of ecosystem-specific emission factors is warranted for applications involving emissions from Australian forest fires.

Southeast Asia experiences frequent fires in fuel-rich tropical peatlands, leading to extreme episodes of regional haze with high concentrations of fine particulate matter (PM 2.5 ) impacting human health. In a study published recently, the first field measurements of PM 2.5 emission factors for tropical peat fires showed larger emissions than from other fuel types. Here we report even higher PM 2.5 emission factors, measured at newly ignited peat fires in Malaysia, suggesting that current estimates of fine particulate emissions from peat fires may be underestimated by a factor of 3 or more. In addition, we use both field and laboratory measurements of burning peat to provide the first mechanistic explanation for the high variability in PM 2.5 emission factors, demonstrating that buildup of a surface ash layer causes the emissions of PM 2.5 to decrease as the peat fire progresses. This finding implies that peat fires are more hazardous (in terms of aerosol emissions) when first ignited than when still burning many days later. Varying emission factors for PM 2.5 also have implications for our ability to correctly model the climate and air quality impacts downwind of the peat fires. For modelers able to implement a time-varying emission factor, we recommend an emission factor for PM 2.5 from newly ignited tropical peat fires of 58 g of PM 2.5 per kilogram of dry fuel consumed (g/kg), reducing exponentially at a rate of 9%/day. If the age of the fire is unknown or only a single value may be used, we recommend an average value of 24 g/kg.

Particle number size distributions are among the most important parameters in trying to understand the characteristics of particle population. Atmospheric particles were measured in an interaction of mixed environments in the Southeastern coastal city of Wollongong, Australia, during a comprehensive field campaign known as Measurements of Urban, Marine and Biogenic Air (MUMBA). MUMBA ran in summer season between 21 st December 2012 and 15 th February 2013. Particle number concentrations measured during this campaign were indicative of the interplay between marine environments and urban air which met the objective of this campaign. Particle number size distributions ranging from 14 nm to 660 nm in diameter, as measured by Scanning Mobility Particle Sizer (SMPS) in this study, were grouped using Principal Component Analysis. Based on strong component loadings (value ≥ 0.75), three different factors were identified (i) Small Factor (N S ): 15 nm < Dp < 50 nm, (ii) Medium Factor (N M ): 60 nm < Dp < 150 nm and (iii) Large Factor (N L ): 210 nm < Dp < 450 nm. The three factors describe 89% of the dataset cumulative variance. Particles in this region are dependent upon the interaction between the sources, and cannot be viewed as a simple mixture of biogenic and anthropogenic sources associated with various mechanical processes. The particles observed in the morning were found to be influenced by combustion emissions, presumably primarily from traffic, which is most obvious in N L . The particle population during the day was found to be influenced by a mixture of marine sources and secondary aerosols production initiated by photochemical oxidation. The local steel works and the urban environment were the major contributors of particles at night. Secondary organic aerosols were identified in this study by the mass ratio of organic carbon to elemental carbon (OC/EC). Biogenic sources influenced secondary organic aerosols formation as a moderate correlation (R 2 = 0.6) was ob

We characterised trace gas emissions from Australian temperate forest fires through a mixture of open-path Fourier transform infrared (OP-FTIR) measurements and selective ion flow tube mass spectrometry (SIFT-MS) and White cell FTIR analysis of grab samples. We report emission factors for a total of 25 trace gas species measured in smoke from nine prescribed fires. We find significant dependence on modified combustion efficiency (MCE) for some species, although regional differences indicate that the use of MCE as a proxy may be limited. We also find that the fire-integrated MCE values derived from our in situ on-the-ground open-path measurements are not significantly different from those reported for airborne measurements of smoke from fires in the same ecosystem. We then compare our average emission factors to those measured for temperate forest fires elsewhere (North America) and for fires in another dominant Australian ecosystem (savanna) and find significant differences in both cases. Indeed, we find that although the emission factors of some species agree within 20%, including those of hydrogen cyanide, ethene, methanol, formaldehyde and 1,3-butadiene, others, such as acetic acid, ethanol, monoterpenes, ammonia, acetonitrile and pyrrole, differ by a factor of 2 or more. This indicates that the use of ecosystem-specific emission factors is warranted for applications involving emissions from Australian forest fires.

The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29th of May, 2014 until the 30th June, 2014 at the Australian Tropical Atmospheric Research Station (ATARS) in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, mercury cycle, and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various emitted species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS. Biomass burning emissions dominated the gas and aerosol concentrations in this region. Nine major biomass burning events were identified and associated with intense or close individual smoke plumes. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. The outcomes of this campaign will be numerous. This region is an environment with little human impact and provides a unique look into the characteristics of biomass burning aerosol without the influence of other significant emission sources. Relationships between the aerosol physical and chemical properties, gas concentrations and meteorological data for the entire month will provide fundamental knowledge required t

The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument provides the longest continuous dataset of carbon monoxide (CO) from space. We perform the first validation of MOPITT version 6 retrievals using total column CO measurements from ground-based remote-sensing Fourier transform infrared spectrometers (FTSs). Validation uses data recorded at 14 stations, that span a wide range of latitudes (80° N to 78° S), in the Network for the Detection of Atmospheric Composition Change (NDACC). MOPITT measurements are spatially co-located with each station, and different vertical sensitivities between instruments are accounted for by using MOPITT averaging kernels (AKs). All three MOPITT retrieval types are analyzed: thermal infrared (TIR-only), joint thermal and near infrared (TIR-NIR), and near infrared (NIR-only). Generally, MOPITT measurements overestimate CO relative to FTS measurements, but the bias is typically less than 10 %. Mean bias is 2.4 % for TIR-only, 5.1 % for TIR-NIR, and 6.5 % for NIR-only. The TIR-NIR and NIR-only products consistently produce a larger bias and lower correlation than the TIR-only. Validation performance of MOPITT for TIR-only and TIR-NIR retrievals over land or water scenes is equivalent. The four MOPITT detector element pixels are validated separately to account for their different uncertainty characteristics. Pixel 1 produces the highest standard deviation and lowest correlation for all three MOPITT products. However, for TIR-only and TIR-NIR, the error-weighted average that includes all four pixels often provides the best correlation, indicating compensating pixel biases and well-captured error characteristics. We find that MOPITT bias does not depend on latitude but rather is influenced by the proximity to rapidly changing atmospheric CO. MOPITT bias drift has been bound geographically to within ±0.5 % yr−1 or lower at almost all locations.

The Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign took place in Wollongong, New South Wales (a small coastal city approximately 80 km south of Sydney, Australia) from 21 December 2012 to 15 February 2013. Like many Australian cities, Wollongong is surrounded by dense eucalyptus forest, so the urban airshed is heavily influenced by biogenic emissions. Instruments were deployed during MUMBA to measure the gaseous and aerosol composition of the atmosphere with the aim of providing a detailed characterisation of the complex environment of the ocean-forest-urban interface that could be used to test the skill of atmospheric models. The gases measured included ozone, oxides of nitrogen, carbon monoxide, carbon dioxide, methane and many of the most abundant volatile organic compounds. The aerosol characterisation included total particle counts above 3 nm, total cloud condensation nuclei counts, mass concentration, number concentration size distribution, aerosol chemical analyses and elemental analysis. The campaign captured varied meteorological conditions, including two extreme heat events, providing a potentially valuable test for models of future air quality in a warmer climate. There was also an episode when the site sampled clean marine air for many hours, providing a useful additional measure of the background concentrations of these trace gases within this poorly sampled region of the globe. In this paper we describe the campaign, the meteorology and the resulting observations of atmospheric composition in general terms in order to equip the reader with a sufficient understanding of the Wollongong regional influences to use the MUMBA datasets as a case study for testing a chemical transport model. The data are available from PANGAEA (http: //doi.pangaea.de/10.1594/PANGAEA.871982).

There is a lack of knowledge of how biomass burning aerosols in the tropics age, including those in the fire-prone Northern Territory in Australia. This paper reports chemical characterization of fresh and aged aerosols monitored during the 1-month-long SAFIRED (Savannah Fires in the Early Dry Season) field study, with an emphasis on the chemical signature and aging of organic aerosols. The campaign took place in June 2014 during the early dry season when the surface measurement site, the Australian Tropical Atmospheric Research Station (ATARS), located in the Northern Territory, was heavily influenced by thousands of wild and prescribed bushfires. ATARS was equipped with a wide suite of instrumentation for gaseous and aerosol characterization. A compact time-of-flight aerosol mass spectrometer was deployed to monitor aerosol chemical composition. Approximately 90% of submicron non-refractory mass was composed of organic material. Ozone enhancement in biomass burning plumes indicated increased air mass photochemistry. The diversity in biomass burning emissions was illustrated through variability in chemical signature (e.g. wide range in f44, from 0.06 to 0.18) for five intense fire events. The background particulate loading was characterized using positive matrix factorization (PMF). A PMF-resolved BBOA (biomass burning organic aerosol) factor comprised 24% of the submicron non-refractory organic aerosol mass, confirming the significance of fire sources. A dominant PMF factor, OOA (oxygenated organic aerosol), made up 47% of the sampled aerosol, illustrating the importance of aerosol aging in the Northern Territory. Biogenic isoprene-derived organic aerosol factor was the third significant fraction of the background aerosol (28%).

The Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign took place in Wollongong, New South Wales (a small coastal city approximately 80 km south of Sydney, Australia) from 21 December 2012 to 15 February 2013. Like many Australian cities, Wollongong is surrounded by dense eucalyptus forest, so the urban airshed is heavily influenced by biogenic emissions. Instruments were deployed during MUMBA to measure the gaseous and aerosol composition of the atmosphere with the aim of providing a detailed characterisation of the complex environment of the ocean-forest-urban interface that could be used to test the skill of atmospheric models. The gases measured included ozone, oxides of nitrogen, carbon monoxide, carbon dioxide, methane and many of the most abundant volatile organic compounds. The aerosol characterisation included total particle counts above 3 nm, total cloud condensation nuclei counts, mass concentration, number concentration size distribution, aerosol chemical analyses and elemental analysis. The campaign captured varied meteorological conditions, including two extreme heat events, providing a potentially valuable test for models of future air quality in a warmer climate. There was also an episode when the site sampled clean marine air for many hours, providing a useful additional measure of the background concentrations of these trace gases within this poorly sampled region of the globe. In this paper we describe the campaign, the meteorology and the resulting observations of atmospheric composition in general terms in order to equip the reader with a sufficient understanding of the Wollongong regional influences to use the MUMBA datasets as a case study for testing a chemical transport model. The data are available from PANGAEA (http: //doi.pangaea.de/10.1594/PANGAEA.871982).

The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument provides the longest continuous dataset of carbon monoxide (CO) from space. We perform the first validation of MOPITT version 6 retrievals using total column CO measurements from ground-based remote-sensing Fourier transform infrared spectrometers (FTSs). Validation uses data recorded at 14 stations, that span a wide range of latitudes (80° N to 78° S), in the Network for the Detection of Atmospheric Composition Change (NDACC). MOPITT measurements are spatially co-located with each station, and different vertical sensitivities between instruments are accounted for by using MOPITT averaging kernels (AKs). All three MOPITT retrieval types are analyzed: thermal infrared (TIR-only), joint thermal and near infrared (TIR-NIR), and near infrared (NIR-only). Generally, MOPITT measurements overestimate CO relative to FTS measurements, but the bias is typically less than 10 %. Mean bias is 2.4 % for TIR-only, 5.1 % for TIR-NIR, and 6.5 % for NIR-only. The TIR-NIR and NIR-only products consistently produce a larger bias and lower correlation than the TIR-only. Validation performance of MOPITT for TIR-only and TIR-NIR retrievals over land or water scenes is equivalent. The four MOPITT detector element pixels are validated separately to account for their different uncertainty characteristics. Pixel 1 produces the highest standard deviation and lowest correlation for all three MOPITT products. However, for TIR-only and TIR-NIR, the error-weighted average that includes all four pixels often provides the best correlation, indicating compensating pixel biases and well-captured error characteristics. We find that MOPITT bias does not depend on latitude but rather is influenced by the proximity to rapidly changing atmospheric CO. MOPITT bias drift has been bound geographically to within ±0.5 % yr−1 or lower at almost all locations.

There is a lack of knowledge of how biomass burning aerosols in the tropics age, including those in the fire-prone Northern Territory in Australia. This paper reports chemical characterization of fresh and aged aerosols monitored during the 1-month-long SAFIRED (Savannah Fires in the Early Dry Season) field study, with an emphasis on the chemical signature and aging of organic aerosols. The campaign took place in June 2014 during the early dry season when the surface measurement site, the Australian Tropical Atmospheric Research Station (ATARS), located in the Northern Territory, was heavily influenced by thousands of wild and prescribed bushfires. ATARS was equipped with a wide suite of instrumentation for gaseous and aerosol characterization. A compact time-of-flight aerosol mass spectrometer was deployed to monitor aerosol chemical composition. Approximately 90% of submicron non-refractory mass was composed of organic material. Ozone enhancement in biomass burning plumes indicated increased air mass photochemistry. The diversity in biomass burning emissions was illustrated through variability in chemical signature (e.g. wide range in f44, from 0.06 to 0.18) for five intense fire events. The background particulate loading was characterized using positive matrix factorization (PMF). A PMF-resolved BBOA (biomass burning organic aerosol) factor comprised 24% of the submicron non-refractory organic aerosol mass, confirming the significance of fire sources. A dominant PMF factor, OOA (oxygenated organic aerosol), made up 47% of the sampled aerosol, illustrating the importance of aerosol aging in the Northern Territory. Biogenic isoprene-derived organic aerosol factor was the third significant fraction of the background aerosol (28%).

The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29th of May, 2014 until the 30th June, 2014 at the Australian Tropical Atmospheric Research Station (ATARS) in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, mercury cycle, and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various emitted species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS. Biomass burning emissions dominated the gas and aerosol concentrations in this region. Nine major biomass burning events were identified and associated with intense or close individual smoke plumes. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. The outcomes of this campaign will be numerous. This region is an environment with little human impact and provides a unique look into the characteristics of biomass burning aerosol without the influence of other significant emission sources. Relationships between the aerosol physical and chemical properties, gas concentrations and meteorological data for the entire month will provide fundamental knowledge required t

The Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign took place in Wollongong, New South Wales (a small coastal city approximately 80 km south of Sydney, Australia) from 21 December 2012 to 15 February 2013. Like many Australian cities, Wollongong is surrounded by dense eucalyptus forest, so the urban airshed is heavily influenced by biogenic emissions. Instruments were deployed during MUMBA to measure the gaseous and aerosol composition of the atmosphere with the aim of providing a detailed characterisation of the complex environment of the ocean-forest-urban interface that could be used to test the skill of atmospheric models. The gases measured included ozone, oxides of nitrogen, carbon monoxide, carbon dioxide, methane and many of the most abundant volatile organic compounds. The aerosol characterisation included total particle counts above 3 nm, total cloud condensation nuclei counts, mass concentration, number concentration size distribution, aerosol chemical analyses and elemental analysis. The campaign captured varied meteorological conditions, including two extreme heat events, providing a potentially valuable test for models of future air quality in a warmer climate. There was also an episode when the site sampled clean marine air for many hours, providing a useful additional measure of the background concentrations of these trace gases within this poorly sampled region of the globe. In this paper we describe the campaign, the meteorology and the resulting observations of atmospheric composition in general terms in order to equip the reader with a sufficient understanding of the Wollongong regional influences to use the MUMBA datasets as a case study for testing a chemical transport model. The data are available from PANGAEA (http: //doi.pangaea.de/10.1594/PANGAEA.871982).

The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument provides the longest continuous dataset of carbon monoxide (CO) from space. We perform the first validation of MOPITT version 6 retrievals using total column CO measurements from ground-based remote-sensing Fourier transform infrared spectrometers (FTSs). Validation uses data recorded at 14 stations, that span a wide range of latitudes (80° N to 78° S), in the Network for the Detection of Atmospheric Composition Change (NDACC). MOPITT measurements are spatially co-located with each station, and different vertical sensitivities between instruments are accounted for by using MOPITT averaging kernels (AKs). All three MOPITT retrieval types are analyzed: thermal infrared (TIR-only), joint thermal and near infrared (TIR-NIR), and near infrared (NIR-only). Generally, MOPITT measurements overestimate CO relative to FTS measurements, but the bias is typically less than 10 %. Mean bias is 2.4 % for TIR-only, 5.1 % for TIR-NIR, and 6.5 % for NIR-only. The TIR-NIR and NIR-only products consistently produce a larger bias and lower correlation than the TIR-only. Validation performance of MOPITT for TIR-only and TIR-NIR retrievals over land or water scenes is equivalent. The four MOPITT detector element pixels are validated separately to account for their different uncertainty characteristics. Pixel 1 produces the highest standard deviation and lowest correlation for all three MOPITT products. However, for TIR-only and TIR-NIR, the error-weighted average that includes all four pixels often provides the best correlation, indicating compensating pixel biases and well-captured error characteristics. We find that MOPITT bias does not depend on latitude but rather is influenced by the proximity to rapidly changing atmospheric CO. MOPITT bias drift has been bound geographically to within ±0.5 % yr−1 or lower at almost all locations.

This paper studies the seasonal variation of surface and column CO at three different sites (Paris, Jungfraujoch and Wollongong), with an emphasis on establishing a link between the CO vertical distribution and the nature of CO emission sources. We find the first evidence of a time lag between surface and free tropospheric CO seasonal variations in the Northern Hemisphere. The CO seasonal variability obtained from the total columns and free tropospheric partial columns shows a maximum around March-April and a minimum around September-October in the Northern Hemisphere (Paris and Jungfraujoch). In the Southern Hemisphere (Wollongong) this seasonal variability is shifted by about 6 months. Satellite observations by the IASI-MetOp (Infrared Atmospheric Sounding Interferometer) and MOPITT (Measurements Of Pollution In The Troposphere) instruments confirm this seasonality. Ground-based FTIR (Fourier transform infrared) measurements provide useful complementary information due to good sensitivity in the boundary layer. In situ surface measurements of CO volume mixing ratios at the Paris and Jungfraujoch sites reveal a time lag of the near-surface seasonal variability of about 2 months with respect to the total column variability at the same sites. The chemical transport model GEOS-Chem (Goddard Earth Observing System chemical transport model) is employed to interpret our observations. GEOS-Chem sensitivity runs identify the emission sources influencing the seasonal variation of CO. At both Paris and Jungfraujoch, the surface seasonality is mainly driven by anthropogenic emissions, while the total column seasonality is also controlled by air masses transported from distant sources. At Wollongong, where the CO seasonality is mainly affected by biomass burning, no time shift is observed between surface measurements and total column data.

This paper studies the seasonal variation of surface and column CO at three different sites (Paris, Jungfraujoch and Wollongong), with an emphasis on establishing a link between the CO vertical distribution and the nature of CO emission sources. We find the first evidence of a time lag between surface and free tropospheric CO seasonal variations in the Northern Hemisphere. The CO seasonal variability obtained from the total columns and free tropospheric partial columns shows a maximum around March-April and a minimum around September-October in the Northern Hemisphere (Paris and Jungfraujoch). In the Southern Hemisphere (Wollongong) this seasonal variability is shifted by about 6 months. Satellite observations by the IASI-MetOp (Infrared Atmospheric Sounding Interferometer) and MOPITT (Measurements Of Pollution In The Troposphere) instruments confirm this seasonality. Ground-based FTIR (Fourier transform infrared) measurements provide useful complementary information due to good sensitivity in the boundary layer. In situ surface measurements of CO volume mixing ratios at the Paris and Jungfraujoch sites reveal a time lag of the near-surface seasonal variability of about 2 months with respect to the total column variability at the same sites. The chemical transport model GEOS-Chem (Goddard Earth Observing System chemical transport model) is employed to interpret our observations. GEOS-Chem sensitivity runs identify the emission sources influencing the seasonal variation of CO. At both Paris and Jungfraujoch, the surface seasonality is mainly driven by anthropogenic emissions, while the total column seasonality is also controlled by air masses transported from distant sources. At Wollongong, where the CO seasonality is mainly affected by biomass burning, no time shift is observed between surface measurements and total column data.

This paper studies the seasonal variation of surface and column CO at three different sites (Paris, Jungfraujoch and Wollongong), with an emphasis on establishing a link between the CO vertical distribution and the nature of CO emission sources. We find the first evidence of a time lag between surface and free tropospheric CO seasonal variations in the Northern Hemisphere. The CO seasonal variability obtained from the total columns and free tropospheric partial columns shows a maximum around March-April and a minimum around September-October in the Northern Hemisphere (Paris and Jungfraujoch). In the Southern Hemisphere (Wollongong) this seasonal variability is shifted by about 6 months. Satellite observations by the IASI-MetOp (Infrared Atmospheric Sounding Interferometer) and MOPITT (Measurements Of Pollution In The Troposphere) instruments confirm this seasonality. Ground-based FTIR (Fourier transform infrared) measurements provide useful complementary information due to good sensitivity in the boundary layer. In situ surface measurements of CO volume mixing ratios at the Paris and Jungfraujoch sites reveal a time lag of the near-surface seasonal variability of about 2 months with respect to the total column variability at the same sites. The chemical transport model GEOS-Chem (Goddard Earth Observing System chemical transport model) is employed to interpret our observations. GEOS-Chem sensitivity runs identify the emission sources influencing the seasonal variation of CO. At both Paris and Jungfraujoch, the surface seasonality is mainly driven by anthropogenic emissions, while the total column seasonality is also controlled by air masses transported from distant sources. At Wollongong, where the CO seasonality is mainly affected by biomass burning, no time shift is observed between surface measurements and total column data.

Formic acid (HCOOH) is one of the most abundant volatile organic compounds in the atmosphere. It is a major contributor to rain acidity in remote areas. There are, however, large uncertainties on the sources and sinks of HCOOH and therefore HCOOH is misrepresented by global chemistry-transport models. This work presents global distributions from 2008 to 2014 as derived from the measurements of the Infrared Atmospheric Sounding Interferometer (IASI), based on conversion factors between brightness temperature differences and representative retrieved total columns over seven regions: Northern Africa, southern Africa, Amazonia, Atlantic, Australia, Pacific, and Russia. The dependence of the measured HCOOH signal on the thermal contrast is taken into account in the conversion method. This conversion presents errors lower than 20 % for total columns ranging between 0.5 and 1 x 1016 molec cm−2 but reaches higher values, up to 78 %, for columns that are lower than 0.3 x 1016 molec cm−2. Signatures from biomass burning events are highlighted, such as in the Southern Hemisphere and in Russia, as well as biogenic emission sources, e.g., over the eastern USA. A comparison between 2008 and 2014 with ground-based Fourier transform infrared spectroscopy (FTIR) measurements obtained at four locations (Maido and Saint-Denis at La Réunion, Jungfraujoch, and Wollongong) is shown. Although IASI columns are found to correlate well with FTIR data, a large bias (> 100 %) is found over the two sites at La Réunion. A better agreement is found at Wollongong with a negligible bias. The comparison also highlights the difficulty of retrieving total columns from IASI measurements over mountainous regions such as Jungfraujoch. A comparison of the retrieved columns with the global chemistry-transport model IMAGESv2 is also presented, showing good representation of the seasonal and interannual cycles over America, Australia, Asia, and Siberia. A global model underestimation of the distribution and

The biogenic emissions of isoprene and monoterpenes are one of the main drivers of atmospheric photochemistry, including oxidant and secondary organic aerosol production. In this paper, the emission rates of isoprene and monoterpenes from Australian vegetation are investigated for the first time using the Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGANv2.1); the CSIRO chemical transport model; and atmospheric observations of isoprene, monoterpenes and isoprene oxidation products (methacrolein and methyl vinyl ketone). Observations from four field campaigns during three different seasons are used, covering urban, coastal suburban and inland forest areas. The observed concentrations of isoprene and monoterpenes were of a broadly similar magnitude, which may indicate that southeast Australia holds an unusual position where neither chemical species dominates. The model results overestimate the observed atmospheric concentrations of isoprene (up to a factor of 6) and underestimate the monoterpene concentrations (up to a factor of 4). This may occur because the emission rates currently used in MEGANv2.1 for Australia are drawn mainly from young eucalypt trees (< 7 years), which may emit more isoprene than adult trees. There is no single increase/decrease factor for the emissions which suits all seasons and conditions studied. There is a need for further field measurements of in situ isoprene and monoterpene emission fluxes in Australia.

Smoke plumes from fires contain atmospheric pollutants that can be transported to populated areas and effect regional air quality. In this paper, the characteristics and impact of the fire plumes from a major fire event that occurred in October 2013 (17-26) in the New South Wales (NSW) in Australia, near the populated areas of Sydney and Wollongong, are studied. Measurements from the Fourier Transform InfraRed (FTIR) spectrometer located at the University of Wollongong allowed a calculation of specific emission factors (EFs) in terms of grams per kilogram of dry fuel burned: 1640 g kg-1 of carbon dioxide; 107 g kg-1 of carbon monoxide; 7.8 g kg-1 of methane and 0.16 g kg-1 of nitrous oxide. These EFs have then been used to calculate daily fire emissions for the NSW fire event using the APIFLAME emissions' model, leading to an increase of 54% of CO emitted compared to calculations with EFs from Akagi et al. (2011), widely used in the literature. Simulations have been conducted for this event using the regional chemistry-transport model (CTM) CHIMERE, allowing the first evaluation of its regional impact. Fire emissions are assumed well mixed into the boundary layer. The model simulations have been evaluated compared to measurements at the NSW air quality stations. The mean correlation coefficients (R) are 0.44 for PM10, 0.60 for PM2.5 and 0.79 for CO, with a negative bias for CO (-14%) and a positive bias for PM2.5 (64%). The model shows higher performance for lower boundary layer heights and wind speeds. According to the observations, 7 days show concentrations exceeding the air quality Australian national standards for PM10, 8 days for PM2.5. In the simulations, 5 days are correctly simulated for PM10, 8 days for PM2.5. For PM10, the model predicts 1 additional day of exceedance (one false detection). During this fire episode, inner Sydney is affected during 5 days by PM exceedances, that are mainly attributed to organic carbon in the model simulations. To evaluate

Marine nitrogen fixation is co-limited by the supply of iron (Fe) and phosphorus in large regions of the global ocean. The deposition of soluble aerosol Fe can initiate nitrogen fixation and trigger toxic algal blooms in nitrate-poor tropical waters. We present dry season soluble Fe data from the Savannah Fires in the Early Dry Season (SAFIRED) campaign in northern Australia that reflects coincident dust and biomass burning sources of soluble aerosol Fe. The mean soluble and total aerosol Fe concentrations were 40 and 500 ng m-3 respectively. Our results show that while biomass burning species may not be a direct source of soluble Fe, biomass burning may substantially enhance the solubility of mineral dust. We observed fractional Fe solubility up to 12% in mixed aerosols. Thus, Fe in dust may be more soluble in the tropics compared to higher latitudes due to higher concentrations of biomass-burning-derived reactive organic species in the atmosphere. In addition, biomass-burning-derived particles can act as a surface for aerosol Fe to bind during atmospheric transport and subsequently be released to the ocean upon deposition. As the aerosol loading is dominated by biomass burning emissions over the tropical waters in the dry season, additions of biomass-burning-derived soluble Fe could have harmful consequences for initiating nitrogen-fixing toxic algal blooms. Future research is required to quantify biomass-burning-derived particle sources of soluble Fe over tropical waters.

Formic acid (HCOOH) is one of the most abundant volatile organic compounds in the atmosphere. It is a major contributor to rain acidity in remote areas. There are, however, large uncertainties on the sources and sinks of HCOOH and therefore HCOOH is misrepresented by global chemistry-transport models. This work presents global distributions from 2008 to 2014 as derived from the measurements of the Infrared Atmospheric Sounding Interferometer (IASI), based on conversion factors between brightness temperature differences and representative retrieved total columns over seven regions: Northern Africa, southern Africa, Amazonia, Atlantic, Australia, Pacific, and Russia. The dependence of the measured HCOOH signal on the thermal contrast is taken into account in the conversion method. This conversion presents errors lower than 20 % for total columns ranging between 0.5 and 1 x 1016 molec cm−2 but reaches higher values, up to 78 %, for columns that are lower than 0.3 x 1016 molec cm−2. Signatures from biomass burning events are highlighted, such as in the Southern Hemisphere and in Russia, as well as biogenic emission sources, e.g., over the eastern USA. A comparison between 2008 and 2014 with ground-based Fourier transform infrared spectroscopy (FTIR) measurements obtained at four locations (Maido and Saint-Denis at La Réunion, Jungfraujoch, and Wollongong) is shown. Although IASI columns are found to correlate well with FTIR data, a large bias (> 100 %) is found over the two sites at La Réunion. A better agreement is found at Wollongong with a negligible bias. The comparison also highlights the difficulty of retrieving total columns from IASI measurements over mountainous regions such as Jungfraujoch. A comparison of the retrieved columns with the global chemistry-transport model IMAGESv2 is also presented, showing good representation of the seasonal and interannual cycles over America, Australia, Asia, and Siberia. A global model underestimation of the distribution and

The biogenic emissions of isoprene and monoterpenes are one of the main drivers of atmospheric photochemistry, including oxidant and secondary organic aerosol production. In this paper, the emission rates of isoprene and monoterpenes from Australian vegetation are investigated for the first time using the Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGANv2.1); the CSIRO chemical transport model; and atmospheric observations of isoprene, monoterpenes and isoprene oxidation products (methacrolein and methyl vinyl ketone). Observations from four field campaigns during three different seasons are used, covering urban, coastal suburban and inland forest areas. The observed concentrations of isoprene and monoterpenes were of a broadly similar magnitude, which may indicate that southeast Australia holds an unusual position where neither chemical species dominates. The model results overestimate the observed atmospheric concentrations of isoprene (up to a factor of 6) and underestimate the monoterpene concentrations (up to a factor of 4). This may occur because the emission rates currently used in MEGANv2.1 for Australia are drawn mainly from young eucalypt trees (< 7 years), which may emit more isoprene than adult trees. There is no single increase/decrease factor for the emissions which suits all seasons and conditions studied. There is a need for further field measurements of in situ isoprene and monoterpene emission fluxes in Australia.

Marine nitrogen fixation is co-limited by the supply of iron (Fe) and phosphorus in large regions of the global ocean. The deposition of soluble aerosol Fe can initiate nitrogen fixation and trigger toxic algal blooms in nitrate-poor tropical waters. We present dry season soluble Fe data from the Savannah Fires in the Early Dry Season (SAFIRED) campaign in northern Australia that reflects coincident dust and biomass burning sources of soluble aerosol Fe. The mean soluble and total aerosol Fe concentrations were 40 and 500 ng m-3 respectively. Our results show that while biomass burning species may not be a direct source of soluble Fe, biomass burning may substantially enhance the solubility of mineral dust. We observed fractional Fe solubility up to 12% in mixed aerosols. Thus, Fe in dust may be more soluble in the tropics compared to higher latitudes due to higher concentrations of biomass-burning-derived reactive organic species in the atmosphere. In addition, biomass-burning-derived particles can act as a surface for aerosol Fe to bind during atmospheric transport and subsequently be released to the ocean upon deposition. As the aerosol loading is dominated by biomass burning emissions over the tropical waters in the dry season, additions of biomass-burning-derived soluble Fe could have harmful consequences for initiating nitrogen-fixing toxic algal blooms. Future research is required to quantify biomass-burning-derived particle sources of soluble Fe over tropical waters.

Formic acid (HCOOH) is one of the most abundant volatile organic compounds in the atmosphere. It is a major contributor to rain acidity in remote areas. There are, however, large uncertainties on the sources and sinks of HCOOH and therefore HCOOH is misrepresented by global chemistry-transport models. This work presents global distributions from 2008 to 2014 as derived from the measurements of the Infrared Atmospheric Sounding Interferometer (IASI), based on conversion factors between brightness temperature differences and representative retrieved total columns over seven regions: Northern Africa, southern Africa, Amazonia, Atlantic, Australia, Pacific, and Russia. The dependence of the measured HCOOH signal on the thermal contrast is taken into account in the conversion method. This conversion presents errors lower than 20 % for total columns ranging between 0.5 and 1 x 1016 molec cm−2 but reaches higher values, up to 78 %, for columns that are lower than 0.3 x 1016 molec cm−2. Signatures from biomass burning events are highlighted, such as in the Southern Hemisphere and in Russia, as well as biogenic emission sources, e.g., over the eastern USA. A comparison between 2008 and 2014 with ground-based Fourier transform infrared spectroscopy (FTIR) measurements obtained at four locations (Maido and Saint-Denis at La Réunion, Jungfraujoch, and Wollongong) is shown. Although IASI columns are found to correlate well with FTIR data, a large bias (> 100 %) is found over the two sites at La Réunion. A better agreement is found at Wollongong with a negligible bias. The comparison also highlights the difficulty of retrieving total columns from IASI measurements over mountainous regions such as Jungfraujoch. A comparison of the retrieved columns with the global chemistry-transport model IMAGESv2 is also presented, showing good representation of the seasonal and interannual cycles over America, Australia, Asia, and Siberia. A global model underestimation of the distribution and

The biogenic emissions of isoprene and monoterpenes are one of the main drivers of atmospheric photochemistry, including oxidant and secondary organic aerosol production. In this paper, the emission rates of isoprene and monoterpenes from Australian vegetation are investigated for the first time using the Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGANv2.1); the CSIRO chemical transport model; and atmospheric observations of isoprene, monoterpenes and isoprene oxidation products (methacrolein and methyl vinyl ketone). Observations from four field campaigns during three different seasons are used, covering urban, coastal suburban and inland forest areas. The observed concentrations of isoprene and monoterpenes were of a broadly similar magnitude, which may indicate that southeast Australia holds an unusual position where neither chemical species dominates. The model results overestimate the observed atmospheric concentrations of isoprene (up to a factor of 6) and underestimate the monoterpene concentrations (up to a factor of 4). This may occur because the emission rates currently used in MEGANv2.1 for Australia are drawn mainly from young eucalypt trees (< 7 years), which may emit more isoprene than adult trees. There is no single increase/decrease factor for the emissions which suits all seasons and conditions studied. There is a need for further field measurements of in situ isoprene and monoterpene emission fluxes in Australia.