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The Monitoring Atmospheric Composition and Climate (MACC) project represents the European Union's Copernicus Atmosphere Monitoring Service (CAMS) (http://www.copernicus.eu/), which became fully operational during 2015. The global near-real-time MACC model production run for aerosol and reactive gases provides daily analyses and 5-day forecasts of atmospheric composition fields. It is the only assimilation system worldwide that is operational to produce global analyses and forecasts of reactive gases and aerosol fields. We have investigated the ability of the MACC analysis system to simulate tropospheric concentrations of reactive gases covering the period between 2009 and 2012. A validation was performed based on carbon monoxide (CO), nitrogen dioxide (NO2) and ozone (O3) surface observations from the Global Atmosphere Watch (GAW) network, the O3 surface observations from the European Monitoring and Evaluation Programme (EMEP) and, furthermore, NO2 tropospheric columns, as well as CO total columns, derived from satellite sensors. The MACC system proved capable of reproducing reactive gas concentrations with consistent quality; however, with a seasonally dependent bias compared to surface and satellite observations – for northern hemispheric surface O3 mixing ratios, positive biases appear during the warm seasons and negative biases during the cold parts of the year, with monthly modified normalised mean biases (MNMBs) ranging between −30 and 30 % at the surface. Model biases are likely to result from difficulties in the simulation of vertical mixing at night and deficiencies in the model's dry deposition parameterisation. Observed tropospheric columns of NO2 and CO could be reproduced correctly during the warm seasons, but are mostly underestimated by the model during the cold seasons, when anthropogenic emissions are at their highest level, especially over the US, Europe and Asia. Monthly MNMBs of the satellite data evaluation range from values between −110 and 40 % for NO2 and at most −20 % for CO, over the investigated regions. The underestimation is likely to result from a combination of errors concerning the dry deposition parameterisation and certain limitations in the current emission inventories, together with an insufficiently established seasonality in the emissions.

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.