Abstract. European scale harmonized monitoring of atmospheric composition was initiated in the early 1970s, and the activity has generated a comprehensive dataset (available at http://www.emep.int) which allows the evaluation of regional and spatial trends of air pollution during a period of nearly 40 yr. Results from the monitoring made within EMEP, the European Monitoring and Evaluation Programme, show large reductions in ambient concentrations and deposition of sulphur species during the last decades. Reductions are in the order of 70-90 % since the year 1980, and correspond well with reported emission changes. Also reduction in emissions of nitrogen oxides (NO x ) are reflected in the measurements, with an average decrease of nitrogen dioxide and nitrate in precipitation by about 23 % and 25 % respectively since 1990. Only minor reductions are however seen since the late 1990s. The concentrations of total nitrate in air have decreased on average only by 8 % since 1990, and fewer sites show a significant trend. A majority of the EMEP sites show a decreasing trend in reduced nitrogen both in air and precipitation on the order of 25 % since 1990. Deposition of base cations has decreased during the past 30 yr, and the pH in precipitation has increased across Europe. Large inter annual variations in the particulate matter mass concentrations reflect meteorological variability, but still there is a relatively clear overall decrease at several sites during the last decade. With few observations going back to the 1990s, the observed chemical composition is applied to document a change in particulate matter (PM) mass even since 1980. These data indicate an overall reduction of about 5 µg m −3 from sulphate alone. Despite the significant reductions in sulphur emissions, sulphate still remains one of the single most important compounds contributing to regional scale aerosol mass concentration. Long-term ozone trends at EMEP sites show a mixed pattern. The year-to-year variability in ozone due to varying meteorological conditions is substantial, making it hard to separate the trends caused by emission change from other effects. For the Nordic countries the data indicate a reduced occurrence of very low concentrations. The most pronounced change in the frequency distribution is seen at sites in the UK and the Netherlands, showing a reduction in the higher values. Smaller changes are seen in Germany, while in Switzerland and Austria, no change is seen in the frequency distribution of ozone. The lack of long-term data series is a major obstacle for studying trends in volatile organic compounds (VOC). The scatter in the data is large, and significant changes are only found for certain components and stations. Concentrations of the heavy metals lead and cadmium have decreased in both air and precipitation during the last 20 yr, with reductions in the order of 80-90 % for Pb and 64-84 % for Cd (precipitation and air respectively). The measurements of total gaseous mercury indicate a dramatic decrease in concentrations during ...

Abstract. In spring 2006, the European Arctic was abnormally warm, setting new historical temperature records. During this warm period, smoke from agricultural fires in Eastern Europe intruded into the European Arctic and caused the most severe air pollution episodes ever recorded there. This paper confirms that biomass burning (BB) was indeed the source of the observed air pollution, studies the transport of the smoke into the Arctic, and presents an overview of the observations taken during the episode. Fire detections from the MODIS instruments aboard the Aqua and Terra satellites were used to estimate the BB emissions. The FLEX-PART particle dispersion model was used to show that the smoke was transported to Spitsbergen and Iceland, which was confirmed by MODIS retrievals of the aerosol optical depth (AOD) and AIRS retrievals of carbon monoxide (CO) total columns. Concentrations of halocarbons, carbon dioxide and CO, as well as levoglucosan and potassium, measured at Zeppelin mountain near NyÅlesund, were used to further corroborate the BB source of the smoke at Spitsbergen. The ozone (O 3 ) and CO concentrations were the highest ever observed at the Zeppelin station, and gaseous elemental mercury was also elevated. A new O 3 record was also set at a station on Iceland. The smoke was strongly absorbingblack carbon concentrations were the highest ever recorded Correspondence to: A. Stohl (ast@nilu.no) at Zeppelin -and strongly perturbed the radiation transmission in the atmosphere: aerosol optical depths were the highest ever measured at NyÅlesund. We furthermore discuss the aerosol chemical composition, obtained from filter samples, as well as the aerosol size distribution during the smoke event. Photographs show that the snow at a glacier on Spitsbergen became discolored during the episode and, thus, the snow albedo was reduced. Samples of this polluted snow contained strongly elevated levels of potassium, sulphate, nitrate and ammonium ions, thus relating the discoloration to the deposition of the smoke aerosols. This paper shows that, to date, BB has been underestimated as a source of aerosol and air pollution for the Arctic, relative to emissions from fossil fuel combustion. Given its significant impact on air quality over large spatial scales and on radiative processes, the practice of agricultural waste burning should be banned in the future.

This study quantifies the present-day global and regional distributions (2010–2014) and trends (2000–2014) for five ozone metrics relevant for short-term and long-term human exposure. These metrics, calculated by the Tropospheric Ozone Assessment Report, are: 4thhighest daily maximum 8-hour ozone (4MDA8); number of days with MDA8 > 70 ppb (NDGT70), SOMO35 (annual Sum of Ozone Means Over 35 ppb) and two seasonally averaged metrics (3MMDA1; AVGMDA8). These metrics were explored at ozone monitoring sites worldwide, which were classified as urban or non-urban based on population and nighttime lights data.Present-day distributions of 4MDA8 and NDGT70, determined predominantly by peak values, are similar with highest levels in western North America, southern Europe and East Asia. For the other three metrics, distributions are similar with North–South gradients more prominent across Europe and Japan. Between 2000 and 2014, significant negative trends in 4MDA8 and NDGT70 occur at most US and some European sites. In contrast, significant positive trends are found at many sites in South Korea and Hong Kong, with mixed trends across Japan. The other three metrics have similar, negative trends for many non-urban North American and some European and Japanese sites, and positive trends across much of East Asia. Globally, metrics at many sites exhibit non-significant trends. At 59% of all sites there is a common direction and significance in the trend across all five metrics, whilst 4MDA8 and NDGT70 have a common trend at ~80% of all sites. Sensitivity analysis shows AVGMDA8 trends differ with averaging period (warm season or annual). Trends are unchanged at many sites when a 1995–2014 period is used; although fewer sites exhibit non-significant trends. Over the longer period 1970–2014, most Japanese sites exhibit positive 4MDA8/SOMO35 trends. Insufficient data exist to characterize ozone trends for the rest of Asia and other world regions.

Abstract. Ozone levels in Europe are changing. Emissions of ozone precursors from Europe (NO x , CO and nonmethane hydrocarbons) have been substantially reduced over the last 10-15 years, but changes in ozone levels cannot be explained by changes in European emissions alone. The observed ozone trends at many European sites are only partially reproduced by global or regional photochemistry models, and possible reasons for this are discussed.In order to further explain the European trends in ozone since 1990, the EMEP regional photochemistry model has been run for the years 1990 and 1995-2002. The EMEP model is a regional model centred over Europe but the model domain also includes most of the North Atlantic and the polar region. Climatological ozone data are used as initial and lateral boundary concentrations. Model results are compared to measurements over this timespan of 12 years. Possible causes for the measured trends in European surface ozone have been investigated using model sensitivity runs perturbing emissions and lateral boundary concentrations. The increase in winter ozone partially, and the decrease in the magnitude of high ozone episodes, is attributed to the decrease in ozone precursor emissions since 1990 by the model. Furthermore, the model calculations indicate that the emission reductions have resulted in a marked decrease in summer ozone in major parts of Europe, in particular in Germany. Such a trend in summer ozone is likely to be difficult to identify from the measurements alone because of large inter-annual variability.

Abstract. In spring 2006, the European Arctic was abnormally warm, setting new historical temperature records. During this warm period, smoke from agricultural fires in Eastern Europe intruded into the European Arctic and caused the most severe air pollution episodes ever recorded there. This paper confirms that biomass burning (BB) was indeed the source of the observed air pollution, studies the transport of the smoke into the Arctic, and presents an overview of the observations taken during the episode. Fire detections from the MODIS instruments aboard the Aqua and Terra satellites were used to estimate the BB emissions. The FLEXPART particle dispersion model was used to show that the smoke was transported to Spitsbergen and Iceland, which was confirmed by MODIS retrievals of the aerosol optical depth (AOD) and AIRS retrievals of carbon monoxide (CO) total columns. Concentrations of halocarbons, carbon dioxide and CO, as well as levoglucosan and potassium, measured at Zeppelin mountain near Ny Ålesund, were used to further corroborate the BB source of the smoke at Spitsbergen. The ozone (O3) and CO concentrations were the highest ever observed at the Zeppelin station, and gaseous elemental mercury was also enhanced. A new O3 record was also set at a station on Iceland. The smoke was strongly absorbing – black carbon concentrations were the highest ever recorded at Zeppelin –, and strongly perturbed the radiation transmission in the atmosphere: aerosol optical depths were the highest ever measured at Ny Ålesund. We furthermore discuss the aerosol chemical composition, obtained from filter samples, as well as the aerosol size distribution during the smoke event. Photographs show that the snow at a glacier on Spitsbergen became discolored during the episode and, thus, the snow albedo was reduced. Samples of this polluted snow contained strongly enhanced levels of potassium, sulphate, nitrate and ammonium ions, thus relating the discoloration to the deposition of the smoke aerosols. This paper shows that, to date, BB has been underestimated as a source of aerosol and air pollution for the Arctic, relative to emissions from fossil fuel combustion. Given its significant impact on air quality over large spatial scales and on radiative processes, the practice of agricultural waste burning should be banned in the future.