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Emissions from biomass burning (BB) are a key source of atmospheric tracer gases that affect the atmospheric carbon cycle. We developed four sets of global BB emissions estimates (named GlcGlob, GlcGeoc, McdGlob, and McdGeoc) using a bottom-up approach and by combining the remote sensing products related to fire distribution with two aboveground biomass (AGB) and two land cover classification (LCC) distributions. The sensitivity of the estimates of BB emissions to the AGB and LCC data was evaluated using the carbon monoxide (CO) emissions associated with each BB estimate. Using the AGB and/or LCC data led to substantially different spatial estimates of CO emissions, with a large (factor of approximately 3) spread of estimates for the mean annual CO emissions: 526±53, 219±35, 624±57, and 293±44 Tg CO yr−1 for GlcGlob, GlcGeoc, McdGlob, and McdGeoc, respectively, and 415±47 Tg CO yr−1 for their ensemble average (EsmAve). We simulated atmospheric CO variability at an approximately 2.5∘ grid using an atmospheric tracer transport model and the BB emissions estimates and compared it with ground-based and satellite observations. At ground-based observation sites during fire seasons, the impact of intermittent fire events was poorly defined in our simulations due to the coarse resolution, which obscured temporal and spatial variability in the simulated atmospheric CO concentration. However, when compared at the regional and global scales, the distribution of atmospheric CO concentrations in the simulations shows substantial differences among the estimates of BB emissions. These results indicate that the estimates of BB emissions are highly sensitive to the AGB and LCC data.

The Arctic is particularly sensitive to global warming and the effects of the increasing temperatures can already be detected in this region by occurring events such as thawing permafrost and decreasing Arctic sea ice area. One of the possible consequences is the risk of enhanced regional greenhouse gas emissions such as methane (CH4) due to the exposure of large terrestrial carbon pools or subsea permafrost which have previously been shielded by ice and frozen soil. Various sources, both natural and anthropogenic, are presently emitting methane in the Arctic. Natural sources include wetlands and other freshwater biomes, as well as the ocean and biomass burning. Despite the relatively small population in this region, CH4 emissions due to human activities are also significant. The main anthropogenic sources are the extraction and distribution of fossil fuels in the Arctic nations and, to a lesser extent, livestock activities and waste management. However, assessing the amount of CH4 emissions in the Arctic and their contribution to the global budget still remains challenging due to the difficulties in carrying out accurate measurements in such remote areas. Besides, high variations in the spatial distribution of methane sources and a poor understanding of the effects of ongoing changes in carbon decomposition, vegetation and hydrology also complicate the assessment.Therefore, the aim of this work is to reduce uncertainties on methane emissions in high northern latitudes. In order to achieve that, an inverse modeling approach has been implemented by using observational data sets of CH4 concentrations obtained at 42 surface stations located in different Arctic regions for the period from 2008 to 2019, the atmospheric transport model FLEXPART, as well as available bottom-up estimates of methane emissions provided by process-based surface models and CH4 emission inventories. The results have been analysed with regards to seasonal and inter-annual fluctuations, spatial differences and trends over the period of study.

The climate change impact of methane is significant and the recent increase in its atmospheric concentrations raises great concerns. Across Canada, methane emissions are unevenly distributed with a large part attributed to the Western Canadian Sedimentary Basin (WCSB), which is the fourth largest reserve of fossil fuels in the world. The WCSB extends from northeastern British Columbia to southwestern Manitoba, encompassing Alberta and southern Saskatchewan. The extraction of hydrocarbons mostly takes place in the provinces of Alberta and Saskatchewan and is a large source of methane.According to recent international agreements, the Government of Canada has committed to reducing methane emissions by 40 to 45% by 2025 based on 2012 levels. However, a recent study using atmospheric measurements of methane concentrations in the region showed that methane emissions from the oil and gas sector might be nearly twice that reported in Canada’s National Inventory (Chan et al., 2020). More investigations are required to better understand the discrepancy between these two estimates.In this study, we use atmospheric observations of δ13C measured successively at three locations across the WCSB between 2016 and 2020 to help identify the influence of different types of methane sources across the provinces of Alberta and Saskatchewan. We compare our atmospheric measurements with compilations and isotope contour maps of fugitive methane from energy facilities across the basin. Combining these measurements with trajectories computed with the HYSPLIT model developed by NOAA, we show a gradient in the methane isotopic signature across Alberta: methane being more depleted in southwestern Saskatchewan than northwestern Alberta. We also used the HYSPLIT5-STILT dispersion model to derive footprints during our measurements and estimate methane contributions of these two provinces using an optimization based on the isotopic measurements. Chan et al. 2020

The Arctic is a critical area in terms of global warming. Not only are the rising temperatures already causing changes in the natural conditions of this region, but the high potential of increased methane (CH4) regional emissions are also likely to intensify global warming even stronger in the near term.This future effect consists in the thawing and destabilization of inland and sub-sea permafrost that enhance the release of methane into the atmosphere from extensive CH4 and organic carbon pools which have so far been shielded by ice and frozen soil. Moreover, the high latitude regions are already playing a key role in the global CH4-budget because of such large sources as wetlands and freshwater lakes in addition to human activities, predominantly the fossil fuel industry of the Arctic nations.However, the level of scientific understanding of the actual contribution of Arctic methane emissions to the global CH4-budget is still relatively immature. Besides the difficulties in carrying out measurements in such remote areas, this is due to a high inhomogeneity in the spatial distribution of methane sources and sinks as well as to ongoing changes in hydrology, vegetation and carbon decomposition.Therefore, the aim of this work is to reduce the uncertainties about methane sources and sinks in the Arctic region during the most recent years by using an atmospheric approach, in order to improve the quality of the assessment of the local and global impacts.To do so, the data of atmospheric CH4 concentrations measured at about 30 stations located in different Arctic nations have been analysed in regard to the trends, seasonal fluctuations and spatial patterns that they demonstrate as well as their link to regional emissions.

The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. Current top-down estimates of the global and regional CH4 budget using 3D models usually apply prescribed OH fields and attribute model–observation mismatches almost exclusively to CH4 emissions, leaving the uncertainties due to prescribed OH fields less quantified. Here, using a variational Bayesian inversion framework and the 3D chemical transport model LMDz, combined with 10 different OH fields derived from chemistry–climate models (Chemistry–Climate Model Initiative, or CCMI, experiment), we evaluate the influence of OH burden, spatial distribution, and temporal variations on the global and regional CH4 budget. The global tropospheric mean CH4-reaction-weighted [OH] ([OH]GM-CH4) ranges 10.3–16.3×105 molec cm−3 across 10 OH fields during the early 2000s, resulting in inversion-based global CH4 emissions between 518 and 757  Tg yr−1. The uncertainties in CH4 inversions induced by the different OH fields are similar to the CH4 emission range estimated by previous bottom-up syntheses and larger than the range reported by the top-down studies. The uncertainties in emissions induced by OH are largest over South America, corresponding to large inter-model differences of [OH] in this region. From the early to the late 2000s, the optimized CH4 emissions increased by 22±6  Tg yr−1 (17–30  Tg yr−1), of which ∼25  % (on average) offsets the 0.7  % (on average) increase in OH burden. If the CCMI models represent the OH trend properly over the 2000s, our results show that a higher increasing trend of CH4 emissions is needed to match the CH4 observations compared to the CH4 emission trend derived using constant OH. This study strengthens the importance of reaching a better representation of OH burden and of OH spatial and temporal distributions to reduce the uncertainties in the global and regional CH4 budgets.

Aircraft-based measurements of methane (CH4) and other air pollutants in the Athabasca Oil Sands Region (AOSR) were made during a summer intensive field campaign between 13 August and 7 September 2013 in support of the Joint Canada–Alberta Implementation Plan for Oil Sands Monitoring. Chemical signatures were used to identify CH4 sources from tailings ponds (BTEX VOCs), open pit surface mines (NOy and rBC) and elevated plumes from bitumen upgrading facilities (SO2 and NOy). Emission rates of CH4 were determined for the five primary surface mining facilities in the region using two mass-balance methods. Emission rates from source categories within each facility were estimated when plumes from the sources were spatially separable. Tailings ponds accounted for 45 % of total CH4 emissions measured from the major surface mining facilities in the region, while emissions from operations in the open pit mines accounted for ∼ 50 %. The average open pit surface mining emission rates ranged from 1.2 to 2.8 t of CH4 h−1 for different facilities in the AOSR. Amongst the 19 tailings ponds, Mildred Lake Settling Basin, the oldest pond in the region, was found to be responsible for the majority of tailings ponds emissions of CH4 ( > 70 %). The sum of measured emission rates of CH4 from the five major facilities, 19.2 ± 1.1 t CH4 h−1, was similar to a single mass-balance determination of CH4 from all major sources in the AOSR determined from a single flight downwind of the facilities, 23.7 ± 3.7 t CH4 h−1. The measured hourly CH4 emission rate from all facilities in the AOSR is 48 ± 8 % higher than that extracted for 2013 from the Canadian Greenhouse Gas Reporting Program, a legislated facility-reported emissions inventory, converted to hourly units. The measured emissions correspond to an emissions rate of 0.17 ± 0.01 Tg CH4 yr−1 if the emissions are assumed as temporally constant, which is an uncertain assumption. The emission rates reported here are relevant for the summer season. In the future, effort should be devoted to measurements in different seasons to further our understanding of the seasonal parameters impacting fugitive emissions of CH4 and to allow for better estimates of annual emissions and year-to-year variability.

North American ecosystems absorb more CO2 from the atmosphere during El Niño than during La Niña periods., Long-term atmospheric CO2 mole fraction and δ13CO2 observations over North America document persistent responses to the El Niño–Southern Oscillation. We estimate these responses corresponded to 0.61 (0.45 to 0.79) PgC year−1 more North American carbon uptake during El Niño than during La Niña between 2007 and 2015, partially offsetting increases of net tropical biosphere-to-atmosphere carbon flux around El Niño. Anomalies in derived North American net ecosystem exchange (NEE) display strong but opposite correlations with surface air temperature between seasons, while their correlation with water availability was more constant throughout the year, such that water availability is the dominant control on annual NEE variability over North America. These results suggest that increased water availability and favorable temperature conditions (warmer spring and cooler summer) caused enhanced carbon uptake over North America near and during El Niño.

We present the Facility Level and Area Methane (CH4) Emissions inventory for the Greater Toronto Area (FLAME-GTA). We estimate that total emissions of CH4 in the GTA, the most populous metropolitan area in Canada, are about 86 ± 38 Gg/yr. The FLAME-GTA estimate is within uncertainty of, but lower in magnitude than the existing gridded inventories provided by the Emissions Database for Global Atmospheric Research (EDGAR v 5.0), and by Environment and Climate Change Canada's Air Quality Research Division (ECCC - AQRD) that estimate emissions of 96 ± 48 Gg/yr and 143 ± 71 Gg/yr in the GTA region, respectively. Using a Lagrangian transport model, we predict atmospheric mixing ratios based on different emission inventories and compare the predictions with in situ measurements available from an observatory within the GTA for January–March in both 2015 and 2016. Due to the strong influence of local sources on our observations only a subregion of our GTA inventory is evaluated. These results identify the need for a more extensive measurement network and an improved atmospheric transport modeling effort for further evaluation of the emission inventories.

Existing estimates of methane (CH4) fluxes from North American wetlands vary widely in both magnitude and distribution. In light of these differences, this study uses atmospheric CH4 observations from the US and Canada to analyze seven different bottom-up, wetland CH4 estimates reported in a recent model comparison project. We first use synthetic data to explore whether wetland CH4 fluxes are detectable at atmospheric observation sites. We find that the observation network can detect aggregate wetland fluxes from both eastern and western Canada but generally not from the US. Based upon these results, we then use real data and inverse modeling results to analyze the magnitude, seasonality, and spatial distribution of each model estimate. The magnitude of Canadian fluxes in many models is larger than indicated by atmospheric observations. Many models predict a seasonality that is narrower than implied by inverse modeling results, possibly indicating an oversensitivity to air or soil temperatures. The LPJ-Bern and SDGVM models have a geographic distribution that is most consistent with atmospheric observations, depending upon the region and season. These models utilize land cover maps or dynamic modeling to estimate wetland coverage while most other models rely primarily on remote sensing inundation data.

The Canadian Arctic (> 60 ∘ N, 60–141 ∘ W) may undergo drastic changes if the Arctic warming trend continues. For methane ( CH4 ), Arctic reservoirs are large and widespread, and the climate feedbacks from such changes may be potentially substantial. Current bottom-up and top-down estimates of the regional CH4 flux range widely. This study analyzes the recent observations of atmospheric CH4 from five arctic monitoring sites and presents estimates of the regional CH4 fluxes for 2012–2015. The observational data reveal sizeable synoptic summertime enhancements in the atmospheric CH4 that are distinguishable from background variations, which indicate strong regional fluxes (primarily wetland and biomass burning CH4 emissions) around Behchoko and Inuvik in the western Canadian Arctic. Three regional Bayesian inversion modelling systems with two Lagrangian particle dispersion models and three meteorological datasets are applied to estimate fluxes for the Canadian Arctic and show relatively robust results in amplitude and temporal variations across different transport models, prior fluxes, and subregion masking. The estimated mean total CH4 flux for the entire Canadian Arctic is 1.8±0.6 Tg CH4 yr −1 . The flux estimate is partitioned into biomass burning of 0.3±0.1 Tg CH4 yr −1 and the remaining natural (wetland) flux of 1.5±0.5 Tg CH4 yr −1 . The summer natural CH4 flux estimates clearly show inter-annual variability that is positively correlated with surface temperature anomalies. The results indicate that years with warmer summer conditions result in more wetland CH4 emissions. More data and analysis are required to statistically characterize the dependence of regional CH4 fluxes on the climate in the Arctic. These Arctic measurement sites will aid in quantifying the inter-annual variations and long-term trends in CH4 emissions in the Canadian Arctic.

Resolving the discrepancies between NEE estimates based upon (1) ground studies and (2) atmospheric inversion results, demands increasingly sophisticated techniques. In this paper we present a high-resolution inversion based upon a regional meteorology model (RAMS) and an underlying biosphere (SiB3) model, both running on an identical 40 km grid over most of North America. Current operational systems like CarbonTracker as well as many previous global inversions including the Transcom suite of inversions have utilized inversion regions formed by collapsing biome-similar grid cells into larger aggregated regions. An extreme example of this might be where corrections to NEE imposed on forested regions on the east coast of the United States might be the same as that imposed on forests on the west coast of the United States while, in reality, there likely exist subtle differences in the two areas, both natural and anthropogenic. Our current inversion framework utilizes a combination of previously employed inversion techniques while allowing carbon flux corrections to be biome independent. Temporally and spatially high-resolution results utilizing biome-independent corrections provide insight into carbon dynamics in North America. In particular, we analyze hourly CO2 mixing ratio data from a sparse network of eight towers in North America for 2004. A prior estimate of carbon fluxes due to Gross Primary Productivity (GPP) and Ecosystem Respiration (ER) is constructed from the SiB3 biosphere model on a 40 km grid. A combination of transport from the RAMS and the Parameterized Chemical Transport Model (PCTM) models is used to forge a connection between upwind biosphere fluxes and downwind observed CO2 mixing ratio data. A Kalman filter procedure is used to estimate weekly corrections to biosphere fluxes based upon observed CO2. RMSE-weighted annual NEE estimates, over an ensemble of potential inversion parameter sets, show a mean estimate 0.57 Pg/yr sink in North America. We perform the inversion with two independently derived boundary inflow conditions and calculate jackknife-based statistics to test the robustness of the model results. We then compare final results to estimates obtained from the CarbonTracker inversion system and at the Southern Great Plains flux site. Results are promising, showing the ability to correct carbon fluxes from the biosphere models over annual and seasonal time scales, as well as over the different GPP and ER components. Additionally, the correlation of an estimated sink of carbon in the South Central United States with regional anomalously high precipitation in an area of managed agricultural and forest lands provides interesting hypotheses for future work.

International audience; Anthropogenic mercury emissions are transported through the atmosphere as gaseous elemental mercury (Hg(0)) before they are deposited 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. Oxidation-driven 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 CO$_2$, which is known to exhibit a minimum in summer when CO$_2$ is assimilated by vegetation. The amplitude of seasonal oscillations in the atmospheric Hg(0) concentration increases with latitude and is larger at inland terrestrial sites than coastal sites. Using satellite data, we find that the photosynthetic activity of vegetation correlates with Hg(0) levels at individual sites and across continents. We suggest that terrestrial vegetation acts as a global Hg(0) pump, which can contribute to seasonal variations of atmospheric Hg(0), and that decreasing Hg(0) levels in the Northern Hemisphere over the past 20 years can be partly attributed to increased terrestrial net primary production.

Aircraft-based measurements of methane (CH4) and other air pollutants in the Athabasca Oil Sands Region (AOSR) were made during a summer intensive field campaign between August 13 and September 7 2013, in support of the Joint Canada–Alberta Implementation Plan for Oil Sands Monitoring. Chemical signatures were used to identify CH4 sources from tailings ponds (BTEX VOC's), open-pit surface mines (NOy and rBC) and elevated plumes from bitumen upgrading facilities (SO2 and NOy). Emission rates of CH4 were determined for the five primary surface mining facilities in the region using two mass balance methods. Emission rates from source categories within each facility were estimated when plumes from the sources were spatially separable. Tailings ponds accounted for 45 % of total CH4 emissions measured from the major surface mining facilities in the region while emissions from operations in the open pit mines accounted for ~ 50 %. The average open pit surface mining emission rates ranged from 1.2 to 2.8 tonnes of CH4 hr−1 for different facilities in the AOSR. Amongst the 19 tailings ponds, Mildred Lake Settling Basin, the oldest pond in the region, was found to be responsible for the majority of tailings ponds emissions of CH4 (> 70 %). The sum of measured emission rates of CH4 from the five major facilities, 19.2 ± 1.1 tonnes CH4 hr−1, was similar to a single mass balance determination of CH4 from all major sources in the AOSR determined from a single flight downwind of the facilities, 23.7 ± 3.7 tonnes CH4 hr−1. The measured hourly CH4 emission rate from all facilities in the AOSR is 48 ± 8 % higher than that extracted for 2013 from the Canadian Green House Gas Reporting Program, a legislated facility-reported Emissions Inventory, converted to hourly units. The measured emissions correspond to an emissions rate of 0.17 ± 0.01 Tg CH4 yr−1, if the emissions are assumed temporally constant, an uncertain assumption. The emission rates reported here are relevant for the summer season. In future, effort should be devoted to measurements in different seasons to further our understanding of seasonal parameters impacting fugitive emissions of CH4 and to allow better estimates of annual emissions and year to year variability.

We present methane (CH4) flux estimates for 2005 to 2013 from a Bayesian inversion focusing on the high northern latitudes (north of 50° N). Our inversion is based on atmospheric transport modelled by the Lagrangian particle dispersion model FLEXPART and CH4 observations from 17 in situ and five discrete flask-sampling sites distributed over northern North America and Eurasia. CH4 fluxes are determined at monthly temporal resolution and on a variable grid with maximum resolution of 1° × 1°. Our inversion finds a CH4 source from the high northern latitudes of 82 to 84 Tg yr−1, constituting ∼ 15 % of the global total, compared to 64 to 68 Tg yr−1 (∼ 12 %) in the prior estimates. For northern North America, we estimate a mean source of 16.6 to 17.9 Tg yr−1, which is dominated by fluxes in the Hudson Bay Lowlands (HBL) and western Canada, specifically the province of Alberta. Our estimate for the HBL, of 2.7 to 3.4 Tg yr−1, is close to the prior estimate (which includes wetland fluxes from the land surface model, LPX-Bern) and to other independent inversion estimates. However, our estimate for Alberta, of 5.0 to 5.8 Tg yr−1, is significantly higher than the prior (which also includes anthropogenic sources from the EDGAR-4.2FT2010 inventory). Since the fluxes from this region persist throughout the winter, this may signify that the anthropogenic emissions are underestimated. For northern Eurasia, we find a mean source of 52.2 to 55.5 Tg yr−1, with a strong contribution from fluxes in the Western Siberian Lowlands (WSL) for which we estimate a source of 19.3 to 19.9 Tg yr−1. Over the 9-year inversion period, we find significant year-to-year variations in the fluxes, which in North America, and specifically in the HBL, appear to be driven at least in part by soil temperature, while in the WSL, the variability is more dependent on soil moisture. Moreover, we find significant positive trends in the CH4 fluxes in North America of 0.38 to 0.57 Tg yr−2, and northern Eurasia of 0.76 to 1.09 Tg yr−2. In North America, this could be due to an increase in soil temperature, while in North Eurasia, specifically Russia, the trend is likely due, at least in part, to an increase in anthropogenic sources.

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 (similar to 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 TgCH(4) 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 TgCH(4) 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 (similar to 64% of the global budget, amp;lt;30 degrees N) as compared to mid (similar to 32 %, 30-60 degrees N) and high northern latitudes (similar to 4 %, 60-90 degrees N). Top-down inversions consistently infer lower emissions in China (similar to 58 TgCH(4) yr(-1), range 51-72, -14 %) and higher emissions in Africa (86 TgCH(4) 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. Funding Agencies|Swiss National Science Foundation; NASA [NNX14AF93G, NNX14AO73G]; National Environmental Science Program - Earth Systems and Climate Change Hub; European Commission [283576, 633080]; ESA Climate Change Initiative Greenhouse Gases Phase 2 project; US Department of Energy, BER [DE-AC02-05CH11231]; FAO member countries; Environment Research and Technology Development Fund of the Ministry of the Environment, Japan [2-1502]; ERC [322998]; NERC [NE/J00748X/1]; Swedish Research Council VR; Research Council of Norway [244074]; NSF [1243232, 1243220]; National Science and Engineering Research Council of Canada (NSERC); Chinas QianRen Program; CSIRO Australia; Australian Bureau of Meteorology; Australian Institute of Marine Science; Australian Antarctic Division; NOAA USA; Meteorological Service of Canada; National Aeronautic and Space Administration (NASA) [NAG5-12669, NNX07AE89G, NNX11AF17G, NNX07AE87G, NNX07AF09G, NNX11AF15G, NNX11AF16G]; Department of Energy and Climate Change (DECC, UK) [GA01081]; Commonwealth Scientific and Industrial Research Organization (CSIRO Australia); Bureau of Meteorology (Australia); Joint DECC/Defra Met Office Hadley Centre Climate Programme [GA01101]