Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios — which differ in fossil fuel and microbial emissions — to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain

[1] Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions scenarios, broadly representing ''optimistic,'' ''likely,'' and ''pessimistic'' options, are compared to a base year 2000 simulation. This base case realistically represents the current global distribution of tropospheric ozone. A further set of simulations considers the influence of climate change over the same time period by forcing the central emissions scenario with a surface warming of around 0.7K. The use of a large multimodel ensemble allows us to identify key areas of uncertainty and improves the robustness of the results. Ensemble mean changes in tropospheric ozone burden between 2000 and 2030 for the 3 scenarios range from a 5% decrease, through a 6% increase, to a 15% increase. The intermodel uncertainty (±1 standard deviation) associated with these values is about ±25%. Model outliers have no significant influence on the ensemble mean results. Combining ozone and methane changes, the three scenarios produce radiative forcings of À50, 180, and 300 mW m À2, compared to a CO 2 forcing over the same time period of 800-1100 mW m À2 . These values indicate the importance of air pollution emissions in short-to medium-term climate forcing and the potential for stringent/lax control measures to improve/worsen future climate forcing. The model sensitivity of ozone to imposed climate change varies between models but modulates zonal mean mixing ratios by ±5 ppbv via a variety of feedback mechanisms, in particular those involving water vapor and stratosphere-troposphere exchange. This level of climate change also reduces the methane lifetime by around 4%.

[1] We use 23 atmospheric chemistry transport models to calculate current and future (2030) deposition of reactive nitrogen (NO y , NH x ) and sulfate (SO x ) to land and ocean surfaces. The models are driven by three emission scenarios: (1) current air quality legislation (CLE); (2) an optimistic case of the maximum emissions reductions currently technologically feasible (MFR); and (3) the contrasting pessimistic IPCC SRES A2 scenario. An extensive evaluation of the present-day deposition using nearly all information on wet deposition available worldwide shows a good agreement with observations in Europe and North America, where 60-70% of the model-calculated wet deposition rates agree to within ±50% with quality-controlled measurements. Models systematically overestimate NH x deposition in South Asia, and underestimate NO y deposition in East Asia. We show that there are substantial differences among models for the removal mechanisms of NO y , NH x , and SO x , leading to ±1 s variance in total deposition fluxes of about 30% in the anthropogenic emissions regions, and up to a factor of 2 outside. In all cases the mean model constructed from the ensemble calculations is among the best when comparing to measurements. Currently, 36-51% of all NO y , NH x , and SO x is deposited over the ocean, and 50-80% of the fraction of deposition on land falls on natural (nonagricultural) vegetation. Currently, 11% of the world's natural vegetation receives nitrogen deposition in excess of the ''critical load'' threshold of 1000 mg(N) m À2 yr À1 . The regions most affected are the United States (20% of vegetation), western Europe (30%), eastern Europe (80%), South Asia (60%), East Asia

Abstract. An earth system model (MIROC-ESM 2010) is fully described in terms of each model component and their interactions. Results for the CMIP5 (Coupled Model Intercomparison Project phase 5) historical simulation are presented to demonstrate the model's performance from several perspectives: atmosphere, ocean, sea-ice, land-surface, ocean and terrestrial biogeochemistry, and atmospheric chemistry and aerosols. An atmospheric chemistry coupled version of MIROC-ESM (MIROC-ESM-CHEM 2010) reasonably reproduces transient variations in surface air temperatures for the period 1850-2005, as well as the presentday climatology for the zonal-mean zonal winds and temperatures from the surface to the mesosphere. The historical evolution and global distribution of column ozone and the amount of tropospheric aerosols are reasonably simulated in the model based on the Representative Concentration Pathways' (RCP) historical emissions of these precursors. The simulated distributions of the terrestrial and marine biogeochemistry parameters agree with recent observations, which is encouraging to use the model for future global change projections.

Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337 ± 23 Tg, the ensemble mean burden for 1850 time slice is ~30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16%) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18%) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40–150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly