Atmospheric methane grew very rapidly in 2014 (12.7 ± 0.5 ppb/year), 2015 (10.1 ± 0.7 ppb/year), 2016 (7.0 ± 0.7 ppb/year), and 2017 (7.7 ± 0.7 ppb/year), at rates not observed since the 1980s. The increase in the methane burden began in 2007, with the mean global mole fraction in remote surface background air rising from about 1,775 ppb in 2006 to 1,850 ppb in 2017. Simultaneously the 13C/12C isotopic ratio (expressed as δ13CCH4) has shifted, now trending negative for more than a decade. The causes of methane's recent mole fraction increase are therefore either a change in the relative proportions (and totals) of emissions from biogenic and thermogenic and pyrogenic sources, especially in the tropics and subtropics, or a decline in the atmospheric sink of methane, or both. Unfortunately, with limited measurement data sets, it is not currently possible to be more definitive. The climate warming impact of the observed methane increase over the past decade, if continued at >5 ppb/year in the coming decades, is sufficient to challenge the Paris Agreement, which requires sharp cuts in the atmospheric methane burden. However, anthropogenic methane emissions are relatively very large and thus offer attractive targets for rapid reduction, which are essential if the Paris Agreement aims are to be attained.

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 ...

Anthropogenic mercury emissions are transported through the atmosphere as gaseous elemental mercury (Hg(0)) prior to deposition to Earth's surface. Strong seasonality in atmospheric Hg(0) concentrations in the Northern Hemisphere has been explained by two factors: anthropogenic Hg(0) emissions are thought to peak in winter due to higher energy consumption, and atmospheric oxidation rates of Hg(0) are faster in summer. Oxidationdriven Hg(0) seasonality should be equally pronounced in the Southern Hemisphere, which is inconsistent with observations of constant year-round Hg(0) levels. Here, we assess the role of Hg(0) uptake by vegetation as an alternative mechanism for driving Hg(0) seasonality. We find that at terrestrial sites in the Northern Hemisphere, Hg(0) co-varies with CO2, which is

The profound changes in global SO2 emissions over the last decades have affected atmospheric composition on a regional and global scale with large impact on air quality, atmospheric deposition and the radiative forcing of sulfate aerosols. Reproduction of historical atmospheric pollution levels based on global aerosol models and emission changes is crucial to prove that such models are able to predict future scenarios. Here, we analyze consistency of trends in observations of sulfur components in air and precipitation from major regional networks and estimates from six different global aerosol models from 1990 until 2015. There are large interregional differences in the sulfur trends consistently captured by the models and observations, especially for North America and Europe. Europe had the largest reductions in sulfur emissions in the first part of the period while the highest reduction came later in North America and East Asia. The uncertainties in both the emissions and the representativity of the observations are larger in Asia. However, emissions from East Asia clearly increased from 2000 to 2005 followed by a decrease, while in India a steady increase over the whole period has been observed and modelled. The agreement between a bottom-up approach, which uses emissions and process-based chemical transport models, with independent observations gives an improved confidence in the understanding of the atmospheric sulfur budget.

[1] Large sets of filtered actinometer, filtered pyrheliometer and Sun photometer measurements have been carried out over the past 30 years by various groups at different Arctic and Antarctic sites and for different time periods. They were examined to estimate ensemble average, long-term trends of the summer background aerosol optical depth AOD(500 nm) in the polar regions (omitting the data influenced by Arctic haze and volcanic eruptions). The trend for the Arctic was estimated to be between À1.6% and À2.0% per year over 30 years, depending on location. No significant trend was observed for Antarctica. The time patterns of AOD(500 nm) and Å ngström's parameters a and b measured with Sun photometers during the last 20 years at various Arctic and Antarctic sites are also presented. They give a measure of the large variations of these parameters due to El Chichon, Pinatubo, and Cerro Hudson volcanic particles, Arctic haze episodes most frequent in winter and spring, and the transport of Asian dust and boreal smokes to the Arctic region. Evidence is also shown of marked differences between the aerosol optical parameters measured at coastal and high-altitude sites in Antarctica. In situ optical and chemical composition parameters of aerosol particles measured at Arctic and Antarctic sites are also examined to achieve more complete information on the multimodal size distribution shape parameters and their radiative properties. A characterization of aerosol radiative parameters is also defined by plotting the daily mean values of a as a function of AOD(500 nm), separately for the two polar regions, allowing the identification of different clusters related to fifteen aerosol classes, for which the spectral values of complex refractive index and single scattering albedo were evaluated. Citation: Tomasi, C., et al. (2007), Aerosols in polar regions: A historical overview based on optical depth and in situ observations,