In support of the first Tropospheric Ozone Assessment Report (TOAR) a relational database of global surface ozone observations has been developed and populated with hourly measurement data and enhanced metadata. A comprehensive suite of ozone data products including standard statistics, health and vegetation impact metrics, and trend information, are made available through a common data portal and a web interface. These data form the basis of the TOAR analyses focusing on human health, vegetation, and climate relevant ozone issues, which are part of this special feature.Cooperation among many data centers and individual researchers worldwide made it possible to build the world's largest collection of in-situ hourly surface ozone data covering the period from 1970 to 2015. By combining the data from almost 10,000 measurement sites around the world with global metadata information, new analyses of surface ozone have become possible, such as the first globally consistent characterisations of measurement sites as either urban or rural/remote. Exploitation of these global metadata allows for new insights into the global distribution, and seasonal and long-term changes of tropospheric ozone and they enable TOAR to perform the first, globally consistent analysis of present-day ozone concentrations and recent ozone changes with relevance to health, agriculture, and climate.Considerable effort was made to harmonize and synthesize data formats and metadata information from various networks and individual data submissions. Extensive quality control was applied to identify questionable and erroneous data, including changes in apparent instrument offsets or calibrations. Such data were excluded from TOAR data products. Limitations of a posteriori data quality assurance are discussed. As a result of the work presented here, global coverage of surface ozone data for scientific analysis has been significantly extended. Yet, large gaps remain in the surface observation network both in Schultz et al: Tropospheric Ozone Assessment Report Art. 58, page 2 of 26 terms of regions without monitoring, and in terms of regions that have monitoring programs but no public access to the data archive. Therefore future improvements to the database will require not only improved data harmonization, but also expanded data sharing and increased monitoring in data-sparse regions.

Extracting globally representative trend information from lower tropospheric ozone observations is extremely difficult due to the highly variable distribution and interannual variability of ozone, and the ongoing shift of ozone precursor emissions from high latitudes to low latitudes. Here we report surface ozone trends at 27 globally distributed remote locations (20 in the Northern Hemisphere, 7 in the Southern Hemisphere), focusing on continuous time series that extend from the present back to at least 1995. While these sites are only representative of less than 25% of the global surface area, this analysis provides a range of regional long-term ozone trends for the evaluation of global chemistry-climate models. Trends are based on monthly mean ozone anomalies, and all sites have at least 20 years of data, which improves the likelihood that a robust trend value is due to changes in ozone precursor emissions and/or forced climate change rather than naturally occurring climate variability. Since 1995, the Northern Hemisphere sites are nearly evenly split between positive and negative ozone trends, while 5 of 7 Southern Hemisphere sites have positive trends. Positive trends are in the range of 0.5-2 ppbv decade-1 , with ozone increasing at Mauna Loa by roughly 50% since the late 1950s. Two high elevation Alpine sites, discussed by previous assessments, exhibit decreasing ozone trends in contrast to the positive trend observed by IAGOS commercial aircraft in the European lower free-troposphere. The Alpine sites frequently sample polluted European boundary layer air, especially in summer, and can only be representative of lower free tropospheric ozone if the data are carefully filtered to avoid boundary layer air. The highly variable ozone trends at these 27 surface sites are not necessarily indicative of free tropospheric trends, which have been overwhelmingly positive since the mid-1990s, as shown by recent studies of ozonesonde and aircraft observations.

Abstract. 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.

Abstract. Aerosol observations above the Southern Ocean and Antarctic sea ice are scarce. Measurements of aerosols and atmospheric composition were made in East Antarctic pack ice on board the Australian icebreaker Aurora Australis during the spring of 2012. One particle formation event was observed during the 32 days of observations. This event occurred on the only day to exhibit extended periods of global irradiance in excess of 600 W m −2 . Within the single air mass influencing the measurements, number concentrations of particles larger than 3 nm (CN 3 ) 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 mercurydriven 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 ≥ 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.

We demonstrate the ability of atmospheric radon concentrations to reliably and unambiguously identify local and remote terrestrial influences on an air mass, and thereby the potential for alteration of trace gas composition by anthropogenic and biogenic processes. Based on high accuracy (lower limit of detection 10-40 mBq m -3 ), high temporal resolution (hourly) measurements of atmospheric radon concentration we describe, apply and evaluate a simple two-step method for identifying and characterising constituent mole fractions in baseline air. The technique involves selecting a radon-based threshold concentration to identify the "cleanest" (least terrestrially influenced) air masses, and then performing an outlier removal step based on the distribution of constituent mole fractions in the identified clean air masses. The efficacy of this baseline selection technique is tested at three contrasting WMO GAW stations: Cape Grim (a coastal low-altitude site), Mauna Loa (a remote high-altitude island site), and Jungfraujoch (a continental high-altitude site). At Cape Grim and Mauna Loa the two-step method is at least as effective as more complicated methods employed to characterise baseline conditions, some involving up to nine steps. While it is demonstrated that Jungfraujoch air masses rarely meet the baseline criteria of the more remote sites, a selection method based on a variable monthly radon threshold is shown to produce credible "near baseline" characteristics. The seasonal peak-to-peak amplitude of recent monthly baseline CO 2 mole fraction deviations from the long-term trend at Cape Grim, Mauna Loa and Jungfraujoch are estimated to be 1.1, 6.0 and 8.1 ppm, respectively.