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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.

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 forcing (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 (GTP20) 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 (CH4) and black carbon (BC) emissions by about 50 and 80 %, respectively. For CH4, measures on shale gas production, waste management and coal mines were most important. For non-CH4 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 due to the mitigation are found for China (1.8 months) and India (11–12 months). The climate metrics cannot fully quantify the climate response. Therefore, a second research path was taken. Transient climate ensemble simulations with the four ESMs were run for the CLE and MIT scenarios, to determine the climate impacts of the mitigation. In these simulations, the CLE scenario resulted in a surface temperature increase of 0.70 ± 0.14 K between the years 2006 and 2050. For the decade 2041–2050, the warming was reduced by 0.22 ± 0.07 K in the MIT scenario, and this result was in almost exact agreement with the response calculated based on the emission metrics (reduced warming of 0.22 ± 0.09 K). The metrics calculations suggest that non-CH4 SLCPs contribute ~ 22 % to this response and CH4 78 %. This could not be fully confirmed by the transient simulations, which attributed about 90 % of the temperature response to CH4 reductions. Attribution of the observed temperature response to non-CH4 SLCP emission reductions and BC specifically is hampered in the transient simulations by small forcing and co-emitted species of the emission basket chosen. Nevertheless, an important conclusion is that our mitigation basket as a whole would lead to clear benefits for both air quality and climate. The climate response from BC reductions in our study is smaller than reported previously, possibly because our study is one of the first to use fully coupled climate models, where unforced variability and sea ice responses cause relatively strong temperature fluctuations that may counteract (and, thus, mask) the impacts of small emission reductions. The temperature responses to the mitigation were generally stronger over the continents than over the oceans, and with a warming reduction of 0.44 K (0.39–0.49) K the largest over the Arctic. Our calculations suggest particularly beneficial climate responses in southern Europe, where surface warming was reduced by about 0.3 K and precipitation rates were increased by about 15 (6–21) mm yr−1 (more than 4 % of total precipitation) from spring to autumn. Thus, the mitigation could help to alleviate expected future drought and water shortages in the Mediterranean area. We also report other important results of the ECLIPSE project.

The concentrations of sulfate, black carbon (BC) and other aerosols in the Arctic are characterized by high values in late winter and spring (so-called Arctic Haze) and low values in summer. Models have long been struggling to capture this seasonality and especially the high concentrations associated with Arctic Haze. In this study, we evaluate sulfate and BC concentrations from eleven different models driven with the same emission inventory against a comprehensive pan-Arctic measurement data set over a time period of 2 years (2008–2009). The set of models consisted of one Lagrangian particle dispersion model, four chemistry transport models (CTMs), one atmospheric chemistry-weather forecast model and five chemistry climate models (CCMs), of which two were nudged to meteorological analyses and three were running freely. The measurement data set consisted of surface measurements of equivalent BC (eBC) from five stations (Alert, Barrow, Pallas, Tiksi and Zeppelin), elemental carbon (EC) from Station Nord and Alert and aircraft measurements of refractory BC (rBC) from six different campaigns. We find that the models generally captured the measured eBC or rBC and sulfate concentrations quite well, compared to previous comparisons. However, the aerosol seasonality at the surface is still too weak in most models. Concentrations of eBC and sulfate averaged over three surface sites are underestimated in winter/spring in all but one model (model means for January–March underestimated by 59 and 37 % for BC and sulfate, respectively), whereas concentrations in summer are overestimated in the model mean (by 88 and 44 % for July–September), but with overestimates as well as underestimates present in individual models. The most pronounced eBC underestimates, not included in the above multi-site average, are found for the station Tiksi in Siberia where the measured annual mean eBC concentration is 3 times higher than the average annual mean for all other stations. This suggests an underestimate of BC sources in Russia in the emission inventory used. Based on the campaign data, biomass burning was identified as another cause of the modeling problems. For sulfate, very large differences were found in the model ensemble, with an apparent anti-correlation between modeled surface concentrations and total atmospheric columns. There is a strong correlation between observed sulfate and eBC concentrations with consistent sulfate/eBC slopes found for all Arctic stations, indicating that the sources contributing to sulfate and BC are similar throughout the Arctic and that the aerosols are internally mixed and undergo similar removal. However, only three models reproduced this finding, whereas sulfate and BC are weakly correlated in the other models. Overall, no class of models (e.g., CTMs, CCMs) performed better than the others and differences are independent of model resolution.

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).

Air pollution in the Arctic caused by local emission sources is a challenge that is important but often overlooked. Local Arctic air pollution can be severe and significantly exceed air quality standards, impairing public health and affecting ecosystems. Specifically in the wintertime, pollution can accumulate under inversion layers. However, neither the contributing emission sources are well identified and quantified nor the relevant atmospheric mechanisms forming pollution are well understood. In the summer, boreal forest fires cause high levels of atmospheric pollution. Despite the often high exposure to air pollution, there are neither specific epidemiological nor toxicological health impact studies in the Arctic. Hence, effects on the local population are difficult to estimate at present. Socioeconomic development of the Arctic is already occurring and expected to be significant in the future. Arctic destination shipping is likely to increase with the development of natural resource extraction, and tourism might expand. Such development will not only lead to growth in the population living in the Arctic but will likely increase emission types and magnitudes. Present‐day inventories show a large spread in the amount and location of emissions representing a significant source of uncertainty in model predictions that often deviate significantly from observations. This is a challenge for modeling studies that aim to assess the impacts of within Arctic air pollution. Prognoses for the future are hence even more difficult, given the additional uncertainty of estimating emissions based on future Arctic economic development scenarios. Key Points Local Arctic air pollution is among the most severe world wide Arctic meteorological conditions exacerbate air pollution and create unique pollution formation mechanisms Future economic activities in the Arctic are expected to increase local air pollution

A model intercomparison activity was inspired by the large suite of observations of atmospheric composition made during the International Polar Year (2008) in the Arctic. Nine global and two regional chemical transport models participated in this intercomparison and performed simulations for 2008 using a common emissions inventory to assess the differences in model chemistry and transport schemes. This paper summarizes the models and compares their simulations of ozone and its precursors and presents an evaluation of the simulations using a variety of surface, balloon, aircraft and satellite observations. Each type of measurement has some limitations in spatial or temporal coverage or in composition, but together they assist in quantifying the limitations of the models in the Arctic and surrounding regions. Despite using the same emissions, large differences are seen among the models. The cloud fields and photolysis rates are shown to vary greatly among the models, indicating one source of the differences in the simulated chemical species. The largest differences among models, and between models and observations, are in NOy partitioning (PAN vs. HNO3) and in oxygenated volatile organic compounds (VOCs) such as acetaldehyde and acetone. Comparisons to surface site measurements of ethane and propane indicate that the emissions of these species are significantly underestimated. Satellite observations of NO2 from the OMI (Ozone Monitoring Instrument) have been used to evaluate the models over source regions, indicating anthropogenic emissions are underestimated in East Asia, but fire emissions are generally overestimated. The emission factors for wildfires in Canada are evaluated using the correlations of VOCs to CO in the model output in comparison to enhancement factors derived from aircraft observations, showing reasonable agreement for methanol and acetaldehyde but underestimate ethanol, propane and acetone, while overestimating ethane emission factors.

We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high latitudes (> 50° N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, ΔO3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.47 to 7.00 pptv ppbv−1) than GEOS5-forced models (1.87 to 3.28 pptv ppbv−1), which we show is likely linked to differences in efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from towards the Arctic using a Lagrangian chemical transport model show that 4-day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HOx from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high-latitude tropospheric ozone during summer.

Lidar and in situ observations performed during the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, Climate, Chemistry, Aerosols and Transport (POLARCAT) campaign are reported here in terms of statistics to characterize aerosol properties over northern Europe using daily airborne measurements conducted between Svalbard and Scandinavia from 30 March to 11 April 2008. It is shown that during this period a rather large number of aerosol layers was observed in the troposphere, with a backscatter ratio at 532 nm of 1.2 (1.5 below 2 km, 1.2 between 5 and 7 km and a minimum in between). Their sources were identified using multispectral backscatter and depolarization airborne lidar measurements after careful calibration analysis. Transport analysis and comparisons between in situ and airborne lidar observations are also provided to assess the quality of this identification. Comparison with level 1 backscatter observations of the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) were carried out to adjust CALIOP multispectral observations to airborne observations on a statistical basis. Recalibration for CALIOP daytime 1064 nm signals leads to a decrease of their values by about 30%, possibly related to the use of the version 3.0 calibration procedure. No recalibration is made at 532 nm even though 532 nm scattering ratios appear to be biased low (−8%) because there are also significant differences in air mass sampling between airborne and CALIOP observations. Recalibration of the 1064 nm signal or correction of −5% negative bias in the 532 nm signal both could improve the CALIOP aerosol colour ratio expected for this campaign. The first hypothesis was retained in this work. Regional analyses in the European Arctic performed as a test emphasize the potential of the CALIOP spaceborne lidar for further monitoring in-depth properties of the aerosol layers over Arctic using infrared and depolarization observations. The CALIOP April 2008 global distribution of the aerosol backscatter reveal two regions with large backscatter below 2 km: the northern Atlantic between Greenland and Norway, and northern Siberia. The aerosol colour ratio increases between the source regions and the observations at latitudes above 70° N are consistent with a growth of the aerosol size once transported to the Arctic. The distribution of the aerosol optical properties in the mid-troposphere supports the known main transport pathways between the mid-latitudes and the Arctic.

Over the Mediterranean region, elevated tropospheric ozone (O3) values are recorded, especially in summer. We use the thermal Infrared Atmospheric Sounding Interferometer (IASI) and the Weather Research and Forecasting Model with Chemistry (WRF-Chem) to understand and interpret the factors and emission sources responsible for the high O3 concentrations observed in the Mediterranean troposphere. Six years (2008–2013) of IASI data have been analyzed and results show consistent maxima during summer, with an increase of up to 22% in the [0–8] km O3 column in the eastern part of the basin compared to the middle of the basin. We focus on summer 2010 to investigate the processes that contribute to these summer maxima. Using two modeled O3 tracers (inflow to the model domain and local anthropogenic emissions), we show that, between the surface and 2 km, O3 is mostly formed from anthropogenic emissions, while above 4 km it is mostly transported from outside the domain or from stratospheric origins. Evidence of stratosphere-to-troposphere exchange (STE) events in the eastern part of the basin is shown, and corresponds to a low water vapor mixing ratio and high potential vorticity.

Arctic sea ice has decreased dramatically in the past few decades and the Arctic is increasingly open to transit shipping and natural resource extraction. However, large knowledge gaps exist regarding composition and impacts of emissions associated with these activities. Arctic hydrocarbon extraction is currently under development owing to the large oil and gas reserves in the region. Transit shipping through the Arctic as an alternative to the traditional shipping routes is currently underway. These activities are expected to increase emissions of air pollutants and climate forcers (e.g., aerosols, ozone) in the Arctic troposphere significantly in the future. The authors present the first measurements of these activities off the coast of Norway taken in summer 2012 as part of the European Arctic Climate Change, Economy, and Society (ACCESS) project. The objectives include quantifying the impact that anthropogenic activities will have on regional air pollution and understanding the connections to Arctic climate. Trace gas and aerosol concentrations in pollution plumes were measured, including emissions from different ship types and several offshore extraction facilities. Emissions originating from industrial activities (smelting) on the Kola Peninsula were also sampled. In addition, pollution plumes originating from Siberian biomass burning were probed in order to put the emerging local pollution within a broader context. In the near future these measurements will be combined with model simulations to quantify the influence of local anthropogenic activities on Arctic composition. Here the authors present the scientific objectives of the ACCESS aircraft experiment and the the meteorological conditions during the campaign, and they highlight first scientific results from the experiment.