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.

The global methane (CH₄) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH₄ over the past decade. Emissions and concentrations of CH₄ are continuing to increase, making CH₄ the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH₄ sources that overlap geographically, and from the destruction of CH₄ by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH₄ yr⁻¹, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 Tg CH₄ yr⁻¹, range 596–884) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the individual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (∼ 64 % of the global budget, < 30° N) as compared to mid (∼ 32 %, 30–60° N) and high northern latitudes (∼ 4 %, 60–90° N). Top-down inversions consistently infer lower emissions in China (∼ 58 Tg CH₄ yr⁻¹, range 51–72, −14 %) and higher emissions in Africa (86 Tg CH₄ yr⁻¹, range 73–108, +19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30–40 % on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (http://doi.org/10.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project.

The Community Earth System Model version 2 (CESM2) includes a detailed representation of chemistry throughout the atmosphere in the Community Atmosphere Model with chemistry and Whole Atmosphere Community Climate Model configurations. These model configurations use the Model for Ozone and Related chemical Tracers (MOZART) family of chemical mechanisms, covering the troposphere, stratosphere, mesosphere, and lower thermosphere. The new MOZART tropospheric chemistry scheme (T1) has a number of updates over the previous version (MOZART‐4) in CESM, including improvements to the oxidation of isoprene and terpenes, organic nitrate speciation, and aromatic speciation and oxidation and thus improved representation of ozone and secondary organic aerosol precursors. An evaluation of the present‐day simulations of CESM2 being provided for Climate Model Intercomparison Project round 6 (CMIP6) is presented. These simulations, using the anthropogenic and biomass burning emissions from the inventories specified for CMIP6, as well as online calculation of emissions of biogenic compounds, lightning NO, dust, and sea salt, indicate an underestimate of anthropogenic emissions of a variety of compounds, including carbon monoxide and hydrocarbons. The simulation of surface ozone in the southeast United States is improved over previous model versions, largely due to the improved representation of reactive nitrogen and organic nitrate compounds resulting in a lower ozone production rate than in CESM1 but still overestimates observations in summer. The simulation of tropospheric ozone agrees well with ozonesonde observations in many parts of the globe. The comparison of NO_xand PAN to aircraft observations indicates the model simulates the nitrogen budget well.

Using observations from the Cheeka Peak Observatory in northwestern Washington State during March‐April, 1997, we show that Asian anthropogenic emissions significantly impact the concentrations of a large number of atmospheric species in the air arriving to North America during spring. Isentropic back‐trajectories can be used to identify possible times when this impact will be felt, however trajectories alone are not sufficient to indicate the presence of Asian pollutants. Detailed chemical and meteorological data from one of these periods (March 29th, 1997) indicates that the surface emissions were lifted into the free troposphere over Asia and then transported to North America in ∼6 days.

Gas and particle measurements are described for optically thick regional hazes, dominated by aged smoke from biomass burning, in the cerrado and rain forested regions of Brazil. The hazes tended to be evenly mixed from the surface to the trade wind inversion at 3–4 km in altitude. The properties of aged gases and particles in the regional hazes were significantly different from those of young smoke (<4 min old). As the smoke aged, the total amount of carbon in non‐methane hydrocarbon species (C<11) was depleted by about one third due to transformations into CO₂, CO, and reactive molecules, and removed by dry deposition and/or by conversion to particulate matter. As the smoke particles aged, their sizes increased significantly due to coagulation and mass growth by secondary species (e.g., ammonium, organic acids and sulfate). During aging, condensation and gas‐to‐particle conversion of inorganic and organic vapors increased the aerosol mass by ∼20–40%. One third to one half of this mass growth likely occurred in the first few hours of aging due to the condensation of large organic molecules. The remaining mass growth was probably associated with photochemical and cloud‐processing mechanisms operating over several days. Changes in particle sizes and compositions during aging had a large impact on the optical properties of the aerosol. Over a 2 to 4 day period, the fine particle mass‐scattering efficiency and single‐scattering albedo increased by 1 m²g⁻¹, and ∼0.06, respectively. Conversely, the Angstrom coefficient, backscatter ratio, and mass absorption efficiency decreased significantly with age.

We analyzed the measurements of ozone (O₃) and its precursors made at rural/suburban sites downwind of four large Chinese cities – Beijing, Shanghai, Guangzhou and Lanzhou, to elucidate their pollution characteristics, regional transport, in situ production, and impacts of heterogeneous processes. The same measurement techniques and observation-based model were used to minimize uncertainties in comparison of the results due to difference in methodologies. All four cities suffered from serious O₃ pollution but showed different precursor distributions. The model-calculated in situ O₃ production rates were compared with the observed change rates to infer the relative contributions of on-site photochemistry and transport. At the rural site downwind of Beijing, export of the well-processed urban plumes contributed to the extremely high O₃ levels (up to an hourly value of 286 ppbv), while the O₃ pollution observed at suburban sites of Shanghai, Guangzhou and Lanzhou was dominated by intense in situ production. The O₃ production was in a volatile organic compound (VOC)-limited regime in both Shanghai and Guangzhou, and a NO_x-limited regime in Lanzhou. The key VOC precursors are aromatics and alkenes in Shanghai, and aromatics in Guangzhou. The potential impacts on O₃ production of several heterogeneous processes, namely, hydrolysis of dinitrogen pentoxide (N₂O₅), uptake of hydro peroxy radical (HO₂) on particles and surface reactions of NO₂ forming nitrous acid (HONO), were assessed. The analyses indicate the varying and considerable impacts of these processes in different areas of China depending on the atmospheric abundances of aerosol and NO_x, and suggest the urgent need to better understand these processes and represent them in photochemical models.