Abstract. Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. Much effort is focused on the reduction of surface levels of ozone owing to its health and vegetation impacts, but recent efforts to achieve reductions in exposure at a country scale have proved difficult to achieve owing to increases in background ozone at the zonal hemispheric scale. There is also a growing realisation that the role of ozone as a short-lived climate pollutant could be important in integrated air quality climate change mitigation. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models. It takes the view that knowledge across the scales is important for dealing with air quality and climate change in a synergistic manner. The review shows that there remain a number of clear challenges for ozone such as explaining surface trends, incorporating new chemical understanding, ozone-climate coupling, and a better assessment of impacts. There is a clear and present need to treat ozone across the range of scales, a transboundary issue, but with an emphasis on the hemispheric scales. New observational opportunities are offered both by satellites and small sensors that bridge the scales.

Notable warming trends have been observed in the Arctic. Although increased human-induced emissions of long-lived greenhouse gases are certainly the main driving factor, air pollutants, such as aerosols and ozone, are also important. Air pollutants are transported to the Arctic, primarily from Eurasia, leading to high concentrations in winter and spring (Arctic haze). Local ship emissions and summertime boreal forest fires may also be important pollution sources. Aerosols and ozone could be perturbing the radiative budget of the Arctic through processes specific to the region: Absorption of solar radiation by aerosols is enhanced by highly reflective snow and ice surfaces; deposition of light-absorbing aerosols on snow or ice can decrease surface albedo; and tropospheric ozone forcing may also be contributing to warming in this region. Future increases in pollutant emissions locally or in mid-latitudes could further accelerate global warming in the Arctic

Abstract. Tentative estimates, using three-dimensional chemistry and transport models, have suggested small ozone increases in the upper troposphere resulting from current aircraft emissions, but have also concluded to significant deficiencies in today's models and to the need to improve them through comparison with extended data sets. The Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program was initiated in 1993 by European scientists, aircraft manufacturers, and airlines to collect experimental data. Its goal is to help understand the atmosphere and how it is changing under the influence of human activity, with particular interest in the effects of aircraft. MOZAIC consists of automatic and regular measurements of ozone and water vapor by five long range passenger airliners flying all over the world. The aim is not to detect direct effects of aircraft emissions on the ozone budget inside the air traffic corridors but to build a large database of measurements to allow studies of chemical and physical processes in the atmosphere, and hence to validate global chemistry transport models. MOZAIC data provide, in particular, detailed ozone and water vapor climatologies at 9-12 km where subsonic aircraft emit most of their exhaust and which is a very critical domain (e.g., radiatively and stratosphere/troposphere exchanges) still imperfectly described in existing models. This will be valuable to improve knowledge about the processes occuring in the upper troposphere and the lowermost stratosphere, and the model treatment of near tropopause chemistry and transport. During MOZAIC I (January 1993-September 1996), fully automatic devices were developed,

Abstract. This paper presents a summary of the work done within the European Union's Seventh Framework Programme project ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants). ECLIPSE had a unique systematic concept for designing a realistic and effective mitigation scenario for short-lived climate pollutants (SLCPs; methane, aerosols and ozone, and their precursor species) and quantifying its climate and air quality impacts, and this paper presents the results in the context of this overarching strategy. The first step in ECLIPSE was to create a new emission inventory based on current legislation (CLE) for the recent past and until 2050. Substantial progress compared to previous work was made by including previously unaccounted types of sources such as flaring of gas associated with oil production, and wick lamps. These emission data were used for present-day reference simulations with four advanced Earth system models (ESMs) and six chemistry transport models (CTMs). The model simulations were compared with a variety of ground-based and satellite observational data sets from Asia, Europe and the Arctic. It was found that the models still underestimate the measured seasonality of aerosols in the Arctic but to a lesser extent than in previous studies. Problems likely related to the emissions were identified for northern Russia and India, in particular. To estimate the climate impacts of SLCPs, ECLIPSE followed two paths of research: the first path calculated radiative Published by Copernicus Publications on behalf of the European Geosciences Union. A. Stohl et al.: Evaluating the climate and air quality impacts of short-lived pollutantsforcing (RF) values for a large matrix of SLCP species emissions, for different seasons and regions independently. Based on these RF calculations, the Global Temperature change Potential metric for a time horizon of 20 years (GTP 20 ) was calculated for each SLCP emission type. This climate metric was then used in an integrated assessment model to identify all emission mitigation measures with a beneficial air quality and short-term (20-year) climate impact. These measures together defined a SLCP mitigation (MIT) scenario. Compared to CLE, the MIT scenario would reduce global methane (CH 4 ) and black carbon (BC) emissions by about 50 and 80 %, respectively. For CH 4 , measures on shale gas production, waste management and coal mines were most important. For non-CH 4 SLCPs, elimination of high-emitting vehicles and wick lamps, as well as reducing emissions from gas flaring, coal and biomass stoves, agricultural waste, solvents and diesel engines were most important. These measures lead to large reductions in calculated surface concentrations of ozone and particulate matter. We estimate that in the EU, the loss of statistical life expectancy due to air pollution was 7.5 months in 2010, which will be reduced to 5.2 months by 2030 in the CLE scenario. The MIT scenario would reduce this value by another 0.9 to 4.3 months. Substantially larger reductions du...

Changes in baseline (here understood as representative of continental to hemispheric scales) tropospheric O₃ concentrations that have occurred at northern mid-latitudes over the past six decades are quantified from available measurement records with the goal of providing benchmarks to which retrospective model calculations of the global O₃ distribution can be compared. Eleven data sets (ten ground-based and one airborne) including six European (beginning in the 1950's and before), three North American (beginning in 1984) and two Asian (beginning in 1991) are analyzed. When the full time periods of the data records are considered a consistent picture emerges; O₃ has increased at all sites in all seasons at approximately 1% yr^−1 relative to the site's 2000 yr mixing ratio in each season. For perspective, this rate of increase sustained from 1950 to 2000 corresponds to an approximate doubling. There is little if any evidence for statistically significant differences in average rates of increase among the sites, regardless of varying length of data records. At most sites (most definitively at the European sites) the rate of increase has slowed over the last decade (possibly longer), to the extent that at present O₃ is decreasing at some sites in some seasons, particularly in summer. The average rate of increase before 2000 shows significant seasonal differences (1.08 ± 0.09, 0.89 ± 0.10, 0.85 ± 0.11 and 1.21 ± 0.12% yr^−1 in spring, summer, autumn and winter, respectively, over North America and Europe)

[1] A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by three different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NO y , mainly in form of PAN. Observed O 3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, was used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume was investigated using in situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18% in O 3 production and 24% in O 3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O 3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O 3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O 3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutant levels in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales (averaging 6.25 days) were derived from CO changes. Observed and simulated O 3 /CO correlations in the plume were also compared in order to evaluate the photochemistry in the model. Observed slopes change from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting a small underestimation in modeled photochemical O 3 production. The possible impact of this biomass burning plume on O 3 levels in the European boundary layer was also examined by running the model for a further 5 days and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O 3 increases and elevated CO levels. The model predicts significant changes in O 3 over the entire 10 day period due to photochemistry but the signal is largely lost because of the effects of dilution. However, measurements in several other BB plumes over Europe show that O 3 impact of Alaskan fires can be potentially significant over Europe.

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[1] In the summer of 2004 several separate field programs intensively studied the photochemical, heterogeneous chemical and radiative environment of the troposphere over North America, the North Atlantic Ocean, and western Europe. Previous studies have indicated that the transport of continental emissions, particularly from North America, influences the concentrations of trace species in the troposphere over the North Atlantic and Europe. An international team of scientists, representing over 100 laboratories, collaborated under the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) umbrella to coordinate the separate field programs in order to maximize the resulting advances in our understanding of regional air quality, the transport, chemical transformation and removal of aerosols, ozone, and their precursors during intercontinental transport, and the radiation balance of the troposphere. Participants utilized nine aircraft, one research vessel, several ground-based sites in North America and the Azores, a network of aerosol-ozone lidars in Europe, satellites, balloon borne sondes, and routine commercial aircraft measurements. In this special section, the results from a major fraction of those platforms are presented. This overview is aimed at providing operational and logistical information for those platforms, summarizing the principal findings and conclusions that have been drawn from the results, and directing readers to specific papers for further details.