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Monitoring the spatial distribution and trends in surface greenhouse gas (GHG) fluxes, as well as flux attribution to natural and anthropogenic processes, is essential to track progress under the Paris Agreement and to inform its global stocktake. This study updates earlier syntheses (Petrescu et al., 2020, 2021, 2023), provides a consolidated synthesis of CH4 emissions using bottom-up (BU) and top-down (TD) approaches for the European Union (EU), and is expanded to include seven additional countries with large anthropogenic and/or natural emissions (the USA, Brazil, China, India, Indonesia, Russia, and the Democratic Republic of the Congo (DR Congo)). Our aim is to demonstrate the use of different emission estimates to help improve national GHG emission inventories for a diverse geographical range of stakeholders. We use updated national GHG inventories (NGHGIs) reported by Annex I parties under the United Nations Framework Convention on Climate Change (UNFCCC) in 2023 and the latest available biennial update reports (BURs) reported by non-Annex I parties. Comparing NGHGIs with other approaches highlights that different system boundaries are a key source of divergence. A key system boundary difference is whether anthropogenic and natural fluxes are included and, if they are, how fluxes belonging to these two sources are partitioned. Over the studied period, the total CH4 emission estimates in the EU, the USA, and Russia show a steady decreasing trend since 1990, while for the non-Annex I emitters analyzed in this study, Brazil, China, India, Indonesia, and DR Congo, CH4 emissions have generally increased. Quantitatively, in the EU the mean of 2015–2020 anthropogenic UNFCCC NGHGIs (15±1.8 Tg CH4 yr−1) and the mean of the BU CH4 emissions (17.8 (16–19) Tg CH4 yr−1) generally agree on the magnitude, while inversions show higher emission estimates (medians of 21 (19–22) Tg CH4 yr−1 and 24 (22–25) Tg CH4 yr−1 for the three regional and six global inversions, respectively), as they include natural emissions, which for the EU were quantified at 6.6 Tg CH4 yr−1 (Petrescu et al., 2023). Similarly, for the other Annex I parties in this study (the USA and Russia), the gap between the BU anthropogenic and total TD emissions is partly explained by the natural emissions. For the non-Annex I parties, anthropogenic CH4 estimates from UNFCCC BURs show large differences compared to the other global-inventory-based estimates and even more compared to atmospheric ones. This poses an important potential challenge to monitoring the progress of the global CH4 pledge and the global stocktake. Our analysis provides a useful baseline to prepare for the influx of inventories from non-Annex I parties as regular reporting starts under the enhanced transparency framework of the Paris Agreement. By systematically comparing the BU and TD methods, this study provides recommendations for more robust comparisons of available data sources and hopes to steadily engage more parties in using observational methods to complement their UNFCCC inventories, as well as considering their natural emissions. With anticipated improvements in atmospheric modeling and observations, as well as modeling of natural fluxes, future development needs to resolve knowledge gaps in the BU and TD approaches and to better quantify the remaining uncertainty. TD methods may emerge as a powerful tool to help improve NGHGIs of CH4 emissions, but further confidence is needed in the comparability and robustness of the estimates. The referenced datasets related to figures are available at https://doi.org/10.5281/zenodo.12818506 (Petrescu et al., 2024).

Abstract Various fire emission estimates for southern Africa during 2019, derived with multiple burned area data sets with resolutions ranging from 500 to 20 m, are evaluated using satellite carbon monoxide (CO) observations. Southern African emissions derived from burned area generated by 20 m Sentinel‐2 satellite imagery are up to 120% higher than other estimates because small fires are better detected with a higher‐resolution satellite instrument. A comprehensive comparison between simulated and observed atmospheric CO indicates that the Sentinel‐2 burned area data significantly improves emission estimates, with up to 15% reduction in CO concentration biases in comparison to emissions based on coarser resolution burned area data. We also found that the temporal lag between emissions and atmospheric CO concentrations during the peak fire month was related to atmospheric transport. These findings emphasize the importance of utilizing higher‐resolution satellite instruments in accurately estimating emissions and understanding the impact of small fires on global climate.

A reduction in anthropogenic methane emissions is vital to limit near-term global warming. A small number of so-called super-emitters is responsible for a disproportionally large fraction of total methane emissions. Since late 2017, the TROPOspheric Monitoring Instrument (TROPOMI) has been in orbit, providing daily global coverage of methane mixing ratios at a resolution of up to 7×5.5 km2, enabling the detection of these super-emitters. However, TROPOMI produces millions of observations each day, which together with the complexity of the methane data, makes manual inspection infeasible. We have therefore designed a two-step machine learning approach using a convolutional neural network to detect plume-like structures in the methane data and subsequently apply a support vector classifier to distinguish the emission plumes from retrieval artifacts. The models are trained on pre-2021 data and subsequently applied to all 2021 observations. We detect 2974 plumes in 2021, with a mean estimated source rate of 44 t h−1 and 5–95th percentile range of 8–122 t h−1. These emissions originate from 94 persistent emission clusters and hundreds of transient sources. Based on bottom-up emission inventories, we find that most detected plumes are related to urban areas and/or landfills (35 %), followed by plumes from gas infrastructure (24 %), oil infrastructure (21 %), and coal mines (20 %). For 12 (clusters of) TROPOMI detections, we tip and cue the targeted observations and analysis of high-resolution satellite instruments to identify the exact sources responsible for these plumes. Using high-resolution observations from GHGSat, PRISMA, and Sentinel-2, we detect and analyze both persistent and transient facility-level emissions underlying the TROPOMI detections. We find emissions from landfills and fossil fuel exploitation facilities, and for the latter, we find up to 10 facilities contributing to one TROPOMI detection. Our automated TROPOMI-based monitoring system in combination with high-resolution satellite data allows for the detection, precise identification, and monitoring of these methane super-emitters, which is essential for mitigating their emissions.

Knowledge of the spatial distribution of the fluxes of greenhouse gases (GHGs) and their temporal variability as well as flux attribution to natural and anthropogenic processes is essential to monitoring the progress in mitigating anthropogenic emissions under the Paris Agreement and to inform its global stocktake. This study provides a consolidated synthesis of CH4 and N2O emissions using bottom-up (BU) and top-down (TD) approaches for the European Union and UK (EU27 + UK) and updates earlier syntheses (Petrescu et al., 2020, 2021). The work integrates updated emission inventory data, process-based model results, data-driven sector model results and inverse modeling estimates, and it extends the previous period of 1990–2017 to 2019. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported by parties under the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. Uncertainties in NGHGIs, as reported to the UNFCCC by the EU and its member states, are also included in the synthesis. Variations in estimates produced with other methods, such as atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), arise from diverse sources including within-model uncertainty related to parameterization as well as structural differences between models. By comparing NGHGIs with other approaches, the activities included are a key source of bias between estimates, e.g., anthropogenic and natural fluxes, which in atmospheric inversions are sensitive to the prior geospatial distribution of emissions. For CH4 emissions, over the updated 2015–2019 period, which covers a sufficiently robust number of overlapping estimates, and most importantly the NGHGIs, the anthropogenic BU approaches are directly comparable, accounting for mean emissions of 20.5 Tg CH4 yr−1 (EDGARv6.0, last year 2018) and 18.4 Tg CH4 yr−1 (GAINS, last year 2015), close to the NGHGI estimates of 17.5±2.1 Tg CH4 yr−1. TD inversion estimates give higher emission estimates, as they also detect natural emissions. Over the same period, high-resolution regional TD inversions report a mean emission of 34 Tg CH4 yr−1. Coarser-resolution global-scale TD inversions result in emission estimates of 23 and 24 Tg CH4 yr−1 inferred from GOSAT and surface (SURF) network atmospheric measurements, respectively. The magnitude of natural peatland and mineral soil emissions from the JSBACH–HIMMELI model, natural rivers, lake and reservoir emissions, geological sources, and biomass burning together could account for the gap between NGHGI and inversions and account for 8 Tg CH4 yr−1. For N2O emissions, over the 2015–2019 period, both BU products (EDGARv6.0 and GAINS) report a mean value of anthropogenic emissions of 0.9 Tg N2O yr−1, close to the NGHGI data (0.8±55 % Tg N2O yr−1). Over the same period, the mean of TD global and regional inversions was 1.4 Tg N2O yr−1 (excluding TOMCAT, which reported no data). The TD and BU comparison method defined in this study can be operationalized for future annual updates for the calculation of CH4 and N2O budgets at the national and EU27 + UK scales. Future comparability will be enhanced with further steps involving analysis at finer temporal resolutions and estimation of emissions over intra-annual timescales, which is of great importance for CH4 and N2O, and may help identify sector contributions to divergence between prior and posterior estimates at the annual and/or inter-annual scale. Even if currently comparison between CH4 and N2O inversion estimates and NGHGIs is highly uncertain because of the large spread in the inversion results, TD inversions inferred from atmospheric observations represent the most independent data against which inventory totals can be compared. With anticipated improvements in atmospheric modeling and observations, as well as modeling of natural fluxes, TD inversions may arguably emerge as the most powerful tool for verifying emission inventories for CH4, N2O and other GHGs. The referenced datasets related to figures are visualized at https://doi.org/10.5281/zenodo.7553800 (Petrescu et al., 2023).

A new method is presented for estimating urban hydroxyl radical (OH) concentrations using the downwind decay of the ratio of nitrogen dioxide over carbon monoxide column-mixing ratios (XNO2/XCO) retrieved from the Tropospheric Monitoring Instrument (TROPOMI). The method makes use of plumes simulated by the Weather Research and Forecast model (WRF-Chem) using passive-tracer transport, instead of the encoded chemistry, in combination with auxiliary input variables such as Copernicus Atmospheric Monitoring Service (CAMS) OH, Emission Database for Global Atmospheric Research v4.3.2 (EDGAR) NOx and CO emissions, and National Center for Environmental Protection (NCEP)-based meteorological data. NO2 and CO mixing ratios from the CAMS reanalysis are used as initial and lateral boundary conditions. WRF overestimates NO2 plumes close to the center of the city by 15 % to 30 % in summer and 40 % to 50 % in winter compared to TROPOMI observations over Riyadh. WRF-simulated CO plumes differ by 10 % with TROPOMI in both seasons. The differences between WRF and TROPOMI are used to optimize the OH concentration, NOx, CO emissions and their backgrounds using an iterative least-squares method. To estimate OH, WRF is optimized using (a) TROPOMI XNO2/XCO and (b) TROPOMI-derived XNO2 only. For summer, both the NO2/CO ratio optimization and the XNO2 optimization increase the prior OH from CAMS by 32 ± 5.3 % and 28.3 ± 3.9 %, respectively. EDGAR NOx and CO emissions over Riyadh are increased by 42.1 ± 8.4 % and 101 ± 21 %, respectively, in summer. In winter, the optimization method doubles the CO emissions while increasing OH by ∼ 52 ± 14 % and reducing NOx emissions by 15.5 ± 4.1 %. TROPOMI-derived OH concentrations and the pre-existing exponentially modified Gaussian function fit (EMG) method differ by 10 % in summer and winter, confirming that urban OH concentrations can be reliably estimated using the TROPOMI-observed NO2/CO ratio. Additionally, our method can be applied to a single TROPOMI overpass, allowing one to analyze day-to-day variability in OH, NOx and CO emission.

Atmospheric inversions are used to constrain emissions of trace gases using atmospheric mole-fraction measurements. The four-dimensional variational (4DVAR) inversion approach allows optimization of emissions at a higher temporal and spatial resolution than ensemble or analytical approaches but provides limited opportunities for scalable parallelization because it is an iterative optimization method. Multidecadal variational inversions are needed to optimally extract information from the long measurement records of long-lived atmospheric trace gases like carbon dioxide and methane. However, the wall time needed – up to months – complicates these multidecadal inversions. The physical parallelization (PP) method introduced by Chevallier (2013) addresses this problem for carbon dioxide inversions by splitting the period of the chemical transport model into blocks and running them in parallel. Here, we present a new implementation of the PP method which is suitable for methane inversions accounting for the chemical sink of methane. The performance of the PP method is tested in an 11-year inversion using a TM5-4DVAR inversion setup that assimilates surface observations to optimize methane emissions at grid scale. Our PP implementation improves the wall time performance by a factor of 5 and shows excellent agreement with a full serial inversion in an identical configuration (global mean emissions difference =0.06 % with an interannual variation correlation R=0.99; regional mean emission difference % and interannual variation R>0.94). The wall time improvement of the PP method increases with the size of the inversion period. The PP method is planned to be used in future releases of the Copernicus Atmosphere Monitoring Service (CAMS) multidecadal methane reanalysis.

In this study, an extension on the previously reported status of the COllaborative Carbon Column Observing Network's (COCCON) calibration procedures incorporating refined methods is presented. COCCON is a global network of portable Bruker EM27/SUN FTIR spectrometers for deriving column-averaged atmospheric abundances of greenhouse gases. The original laboratory open-path lamp measurements for deriving the instrumental line shape (ILS) of the spectrometer from water vapour lines have been refined and extended to the secondary detector channel incorporated in the EM27/SUN spectrometer for detection of carbon monoxide (CO). The refinements encompass improved spectroscopic line lists for the relevant water lines and a revision of the laboratory pressure measurements used for the analysis of the spectra. The new results are found to be in good agreement with those reported by Frey et al. (2019) and discussed in detail. In addition, a new calibration cell for ILS measurements was designed, constructed and put into service. Spectrometers calibrated since January 2020 were tested using both methods for ILS characterization, open-path (OP) and cell measurements. We demonstrate that both methods can detect the small variations in ILS characteristics between different spectrometers, but the results of the cell method indicate a systematic bias of the OP method. Finally, a revision and extension of the COCCON network instrument-to-instrument calibration factors for XCO2, XCO and XCH4 is presented, incorporating 47 new spectrometers (of 83 in total by now). This calibration is based on the reference EM27/SUN spectrometer operated by the Karlsruhe Institute of Technology (KIT) and spectra collected by the collocated TCCON station Karlsruhe. Variations in the instrumental characteristics of the reference EM27/SUN from 2014 to 2017 were detected, probably arising from realignment and the dual-channel upgrade performed in early 2018. These variations are considered in the evaluation of the instrument-specific calibration factors in order to keep all tabulated calibration results consistent.

Atmospheric inversion approaches are expected to play a critical role in future observation-based monitoring systems for surface fluxes of greenhouse gases (GHGs), pollutants and other trace gases. In the past decade, the research community has developed various inversion software, mainly using variational or ensemble Bayesian optimization methods, with various assumptions on uncertainty structures and prior information and with various atmospheric chemistry–transport models. Each of them can assimilate some or all of the available observation streams for its domain area of interest: flask samples, in situ measurements or satellite observations. Although referenced in peer-reviewed publications and usually accessible across the research community, most systems are not at the level of transparency, flexibility and accessibility needed to provide the scientific community and policy makers with a comprehensive and robust view of the uncertainties associated with the inverse estimation of GHG and reactive species fluxes. Furthermore, their development, usually carried out by individual research institutes, may in the future not keep pace with the increasing scientific needs and technical possibilities. We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is primarily a programming protocol to allow various inversion bricks to be exchanged among researchers. In practice, the ensemble of bricks makes a flexible, transparent and open-source Python-based tool to estimate the fluxes of various GHGs and reactive species both at the global and regional scales. It will allow for running different atmospheric transport models, different observation streams and different data assimilation approaches. This adaptability will allow for a comprehensive assessment of uncertainty in a fully consistent framework. We present here the main structure and functionalities of the system, and we demonstrate how it operates in a simple academic case.

The global fire emission inventories depend on ground and airborne measurements of species-specific emission factors (EFs), which translate dry matter losses due to fires to actual trace gas and aerosol emissions. The EFs of nitrogen oxides (NOx) and carbon monoxide (CO) can function as a proxy for combustion efficiency to distinguish flaming from smoldering combustion. The uncertainties in these EFs remain large as they are limited by the spatial and temporal representativeness of the measurements. The global coverage of satellite observations has the advantage of filling this gap, making these measurements highly complementary to ground-based or airborne data. We present a new analysis of biomass burning pollutants using space-borne data to investigate the spatiotemporal efficiency of fire combustion. Column measurements of nitrogen dioxide and carbon monoxide (XNO2 and XCO) from the TROPOspheric Monitoring Instrument (TROPOMI) are used to quantify the relative atmospheric enhancements of these species over different fire-prone regions around the world. We find spatial and temporal patterns in the ΔXNO2 ∕ ΔXCO ratio that point to distinct differences in biomass burning behavior. Such differences are induced by the burning phase of the fire (e.g., high-temperature flaming vs. low-temperature smoldering combustion) and burning practice (e.g., the combustion of logs, coarse woody debris and soil organic matter vs. the combustion of fine fuels such as savanna grasses). The sampling techniques and the signal-to-noise ratio of the retrieved ΔXNO2 ∕ ΔXCO signals were quantified with WRF-Chem experiments and showed similar distinct differences in combustion types. The TROPOMI measurements show that the fraction of surface smoldering combustion is much larger for the boreal forest fires in the upper Northern Hemisphere and peatland fires in Indonesia. These types of fires cause a much larger increase (3 to 6 times) in ΔXCO relative to ΔXNO2 than elsewhere in the world. The high spatial and temporal resolution of TROPOMI also enables the detection of spatial gradients in combustion efficiency at smaller regional scales. For instance, in the Amazon, we found higher combustion efficiency (up to 3-fold) for savanna fires than for the nearby tropical deforestation fires. Out of two investigated fire emission products, the TROPOMI measurements support the broad spatial pattern of combustion efficiency rooted in GFED4s. Meanwhile, TROPOMI data also add new insights into regional variability in combustion characteristics that are not well represented in the different emission inventories, which can help the fire modeling community to improve their representation of the spatiotemporal variability in EFs.

The TROPOspheric Monitoring Instrument (TROPOMI) provides observations of atmospheric methane (CH4) at an unprecedented combination of high spatial resolution and daily global coverage. Hu et al. (2018) reported unexpectedly large methane enhancements over South Sudan in these observations. Here we assess methane emissions from the wetlands of South Sudan using 2 years (December 2017–November 2019) of TROPOMI total column methane observations. We estimate annual wetland emissions of 7.4 ± 3.2 Tg yr−1, which agrees with the multiyear GOSAT inversions of Lunt et al. (2019) but is an order of magnitude larger than estimates from wetland process models. This disagreement may be explained by the underestimation (by up to 4 times) of inundation extent by the hydrological schemes used in those models. We investigate the seasonal cycle of the emissions and find the lowest emissions during the June–August season when the process models show the largest emissions. Using satellite-altimetry-based river water height measurements, we infer that this seasonal mismatch is likely due to a seasonal mismatch in inundation extent. In models, inundation extent is controlled by regional precipitation scaled to static wetland extent maps, whereas the actual inundation extent is driven by water inflow from rivers like the White Nile and the Sobat. We find the lowest emissions in the highest precipitation and lowest temperature season (June–August, JJA) when models estimate large emissions. In general, our emission estimates show better agreement in terms of both seasonal cycle and annual mean with model estimates that use a stronger temperature dependence. This suggests that temperature might be a stronger control for the South Sudan wetlands emissions than currently assumed by models. Our findings demonstrate the use of satellite instruments for quantifying emissions from inaccessible and uncertain tropical wetlands, providing clues for the improvement of process models and thereby improving our understanding of the currently uncertain contribution of wetlands to the global methane budget.

This work documents and evaluates the tropospheric gas-phase chemical mechanism MOGUNTIA in the three-dimensional chemistry transport model TM5-MP. Compared to the modified CB05 (mCB05) chemical mechanism previously used in the model, MOGUNTIA includes a detailed representation of the light hydrocarbons (C1–C4) and isoprene, along with a simplified chemistry representation of terpenes and aromatics. Another feature implemented in TM5-MP for this work is the use of the Rosenbrock solver in the chemistry code, which can replace the classical Euler backward integration method of the model. Global budgets of ozone (O3), carbon monoxide (CO), hydroxyl radicals (OH), nitrogen oxides (NOx), and volatile organic compounds (VOCs) are analyzed, and their mixing ratios are compared with a series of surface, aircraft, and satellite observations for the year 2006. Both mechanisms appear to be able to satisfactorily represent observed mixing ratios of important trace gases, with the MOGUNTIA chemistry configuration yielding lower biases than mCB05 compared to measurements in most of the cases. However, the two chemical mechanisms fail to reproduce the observed mixing ratios of light VOCs, indicating insufficient primary emission source strengths, oxidation that is too fast, and/or a low bias in the secondary contribution to C2–C3 organics via VOC atmospheric oxidation. Relative computational memory and time requirements of the different model configurations are also compared and discussed. Overall, the MOGUNTIA scheme simulates a large suite of oxygenated VOCs that are observed in the atmosphere at significant levels. This significantly expands the possible applications of TM5-MP.

This study investigates the use of co-located nitrogen dioxide (NO2) and carbon monoxide (CO) retrievals from the TROPOMI satellite to improve the quantification of burning efficiency and emission factors (EFs) over the megacities of Tehran, Mexico City, Cairo, Riyadh, Lahore, and Los Angeles. Efficient combustion is characterized by high NOx (NO+NO2) and low CO emissions, making the NO2∕CO ratio a useful proxy for combustion efficiency (CE). The local enhancement of CO and NO2 above megacities is well captured by TROPOMI at short averaging times compared with previous satellite missions. In this study, the upwind background and plume rotation methods are used to investigate the accuracy of satellite-derived ΔNO2∕ΔCO ratios. The column enhancement ratios derived using these two methods vary by 5 % to 20 % across the selected megacities. TROPOMI-derived column enhancement ratios are compared with emission ratios from the EDGAR v4.3.2 (Emission Database for Global Atmospheric Research v4.3.2) and the MACCity (Monitoring Atmospheric Chemistry and Climate and CityZen) 2018 emission inventories. TROPOMI correlates strongly (r=0.85 and 0.7) with EDGAR and MACCity, showing the highest emission ratio for Riyadh and lowest emission ratio for Lahore. However, inventory-derived emission ratios are 60 % to 85 % higher than TROPOMI column enhancement ratios across the six megacities. The short lifetime of NO2 and the different vertical sensitivity of TROPOMI NO2 and CO explain most of this difference. We present a method to translate TROPOMI-retrieved column enhancement ratios into corresponding emission ratios, thereby accounting for these influences. Except for Los Angeles and Lahore, TROPOMI-derived emission ratios are close (within 10 % to 25 %) to MACCity values. For EDGAR, however, emission ratios are ∼65 % higher for Cairo and 35 % higher for Riyadh. For Los Angeles, EDGAR and MACCity are a factor of 2 and 3 higher than TROPOMI respectively. The air quality monitoring networks in Los Angeles and Mexico City are used to validate the use of TROPOMI. For Mexico City and Los Angeles, these measurements are consistent with TROPOMI-derived emission ratios, demonstrating the potential of TROPOMI with respect to monitoring burning efficiency.

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4 yr−1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr−1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30∘ N) compared to mid-latitudes (∼ 30 %, 30–60∘ N) and high northern latitudes (∼ 4 %, 60–90∘ N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4 yr−1 by 8 Tg CH4 yr−1, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GCP-CH4-2019 (Saunois et al., 2020) and from the Global Carbon Project.

Methane (CH4) is an important greenhouse gas, and its atmospheric budget is determined by interacting sources and sinks in a dynamic global environment. Methane observations indicate that after almost a decade of stagnation, from 2006, a sudden and continuing global mixing ratio increase took place. We applied a general circulation model to simulate the global atmospheric budget, variability, and trends of methane for the period 1997–2016. Using interannually constant CH4 a priori emissions from 11 biogenic and fossil source categories, the model results are compared with observations from 17 Advanced Global Atmospheric Gases Experiment (AGAGE) and National Oceanic and Atmospheric Administration (NOAA) surface stations and intercontinental Civil Aircraft for the Regular observation of the atmosphere Based on an Instrumented Container (CARIBIC) flights, with > 4800 CH4 samples, gathered on > 320 flights in the upper troposphere and lowermost stratosphere. Based on a simple optimization procedure, methane emission categories have been scaled to reduce discrepancies with the observational data for the period 1997–2006. With this approach, the all-station mean dry air mole fraction of 1780 nmol mol−1 could be improved from an a priori root mean square deviation (RMSD) of 1.31 % to just 0.61 %, associated with a coefficient of determination (R2) of 0.79. The simulated a priori interhemispheric difference of 143.12 nmol mol−1 was improved to 131.28 nmol mol−1, which matched the observations quite well (130.82 nmol mol−1). Analogously, aircraft measurements were reproduced well, with a global RMSD of 1.1 % for the measurements before 2007, with even better results on a regional level (e.g., over India, with an RMSD of 0.98 % and R2=0.65). With regard to emission optimization, this implied a 30.2 Tg CH4 yr−1 reduction in predominantly fossil-fuel-related emissions and a 28.7 Tg CH4 yr−1 increase of biogenic sources. With the same methodology, the CH4 growth that started in 2007 and continued almost linearly through 2013 was investigated, exploring the contributions by four potential causes, namely biogenic emissions from tropical wetlands, from agriculture including ruminant animals, and from rice cultivation, and anthropogenic emissions (fossil fuel sources, e.g., shale gas fracking) in North America. The optimization procedure adopted in this work showed that an increase in emissions from shale gas (7.67 Tg yr−1), rice cultivation (7.15 Tg yr−1), and tropical wetlands (0.58 Tg yr−1) for the period 2006–2013 leads to an optimal agreement (i.e., lowest RMSD) between model results and observations.

The TROPOspheric Monitoring Instrument (TROPOMI), launched 13 October 2017, has been measuring carbon monoxide (CO) concentrations in the Earth's atmosphere since early November 2017. In the first measurements, TROPOMI was able to measure CO concentrations of the high-pollution event in India of November 2017. In this paper, we studied the extent of the pollution in India, comparing the TROPOMI CO with modeled data from the Weather Research and Forecasting model (WRF) to identify the most important sources contributing to the high pollution, both at ground level and in the total column. We investigated the period 11–19 November 2017. We found that residential and commercial combustion was a much more important source of CO pollution than the post-monsoon crop burning during this period, which is in contrast to what media suggested and some studies on aerosol emissions found. Also, the high pollution was not limited to Delhi and its direct neighborhood but the accumulation of pollution extended over the whole Indo-Gangetic Plain (IGP) due to the unfavorable weather conditions in combination with extensive emissions. From the TROPOMI data and WRF simulations, we observed a buildup of CO during 11–14 November and a decline in CO after 15 November. The meteorological conditions, characterized by low wind speeds and shallow atmospheric boundary layers, were most likely the primary explanation for the temporal accumulation and subsequent dispersion of regionally emitted CO in the atmosphere. This emphasizes the important role of atmospheric dynamics in determining the air quality conditions at ground level and in the total column. Due to its rapidly growing population and economy, India is expected to encounter similar pollution events more often in future post-monsoon and winter seasons unless significant policy measures are taken to reduce residential and commercial emissions.

The Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor satellite provides measurements of carbon monoxide (CO) total column concentrations based on earthshine radiance measurements in the 2.3 µm spectral range with a spatial resolution of 7 km×7 km and daily global coverage. Due to the high accuracy of the observations, CO pollution can be detected over cities and industrial areas using single orbit overpasses. In this study, we analyzed local CO enhancements in an area around Iran from 1 November to 20 December 2017. We employed the Weather Research and Forecasting (WRF) model v3.8.1 using the EDGAR v4.2 emission inventory and evaluated CO emissions from the cities of Tehran, Yerevan, Urmia, and Tabriz on a spatial resolution comparable to that of TROPOMI. For background conditions, the WRF simulation agrees well with TROPOMI CO, with a mean difference of 5.7 %. However, the emissions for the city area had to be significantly increased in order to match the observations. Moreover, significant differences at the sub-city scale remain. To match the TROPOMI CO observations around the Armenian city of Yerevan, it is necessary to introduce CO emissions along a southeast arterial road of Yerevan. Overall, this hints at deficits in the EDGAR inventory in the region around Iran and indicates TROPOMI's capability to identify localized CO pollution on sub-city scales, which at the same time challenges current atmospheric modeling at high spatial and temporal resolution.

Temperature exerts strong controls on the incidence and severity of fire. All else equal, warming is expected to increase fire-related carbon emissions, and thereby atmospheric CO2. But the magnitude of this feedback is very poorly known. We use a single-box model of the land biosphere to quantify this positive feedback from satellite-based estimates of biomass burning emissions for 2000–2014 CE and from sedimentary charcoal records for the millennium before the industrial period. We derive an estimate of the centennial-scale feedback strength of 6.5 ± 3.4 ppm CO2 per degree of land temperature increase, based on the satellite data. However, this estimate is poorly constrained, and is largely driven by the well-documented dependence of tropical deforestation and peat fires (primarily anthropogenic) on climate variability patterns linked to the El Niño–Southern Oscillation. Palaeo-data from pre-industrial times provide the opportunity to assess the fire-related climate–carbon-cycle feedback over a longer period, with less pervasive human impacts. Past biomass burning can be quantified based on variations in either the concentration and isotopic composition of methane in ice cores (with assumptions about the isotopic signatures of different methane sources) or the abundances of charcoal preserved in sediments, which reflect landscape-scale changes in burnt biomass. These two data sources are shown here to be coherent with one another. The more numerous data from sedimentary charcoal, expressed as normalized anomalies (fractional deviations from the long-term mean), are then used – together with an estimate of mean biomass burning derived from methane isotope data – to infer a feedback strength of 5.6 ± 3.2 ppm CO2 per degree of land temperature and (for a climate sensitivity of 2.8 K) a gain of 0.09 ± 0.05. This finding indicates that the positive carbon cycle feedback from increased fire provides a substantial contribution to the overall climate–carbon-cycle feedback on centennial timescales. Although the feedback estimates from palaeo- and satellite-era data are in agreement, this is likely fortuitous because of the pervasive influence of human activities on fire regimes during recent decades.

The growth of mega-cities leads to air quality problems directly affecting the citizens. Satellite measurements are becoming of higher quality and quantity, which leads to more accurate satellite retrievals of enhanced air pollutant concentrations over large cities. In this paper, we compare and discuss both an existing and a new method for estimating urban-scale trends in CO emissions using multi-year retrievals from the MOPITT satellite instrument. The first method is mainly based on satellite data, and has the advantage of fewer assumptions, but also comes with uncertainties and limitations as shown in this paper. To improve the reliability of urban-to-regional scale emission trend estimation, we simulate MOPITT retrievals using the Weather Research and Forecast model with chemistry core (WRF-Chem). The difference between model and retrieval is used to optimize CO emissions in WRF-Chem, focusing on the city of Madrid, Spain. This method has the advantage over the existing method in that it allows both a trend analysis of CO concentrations and a quantification of CO emissions. Our analysis confirms that MOPITT is capable of detecting CO enhancements over Madrid, although significant differences remain between the yearly averaged model output and satellite measurements (R2 = 0.75) over the city. After optimization, we find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory. The MOPITT-derived emission adjustments lead to better agreement with the European emission inventory TNO-MAC-III for both years. This suggests that the downward trend in CO emissions over Madrid is overestimated in EdgarV4.2 and more realistically represented in TNO-MACC-III. However, our satellite and model based emission estimates have large uncertainties, around 20 % for 2002 and 50 % for 2006.

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4 yr−1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

We present a global distribution of surface methane (CH4) emission estimates for 2000–2012 derived using the CarbonTracker Europe-CH4 (CTE-CH4) data assimilation system. In CTE-CH4, anthropogenic and biospheric CH4 emissions are simultaneously estimated based on constraints of global atmospheric in situ CH4 observations. The system was configured to either estimate only anthropogenic or biospheric sources per region, or to estimate both categories simultaneously. The latter increased the number of optimizable parameters from 62 to 78. In addition, the differences between two numerical schemes available to perform turbulent vertical mixing in the atmospheric transport model TM5 were examined. Together, the system configurations encompass important axes of uncertainty in inversions and allow us to examine the robustness of the flux estimates. The posterior emission estimates are further evaluated by comparing simulated atmospheric CH4 to surface in situ observations, vertical profiles of CH4 made by aircraft, remotely sensed dry-air total column-averaged mole fraction (XCH4) from the Total Carbon Column Observing Network (TCCON), and XCH4 from the Greenhouse gases Observing Satellite (GOSAT). The evaluation with non-assimilated observations shows that posterior XCH4 is better matched with the retrievals when the vertical mixing scheme with faster interhemispheric exchange is used. Estimated posterior mean total global emissions during 2000–2012 are 516 ± 51 Tg CH4 yr−1, with an increase of 18 Tg CH4 yr−1 from 2000–2006 to 2007–2012. The increase is mainly driven by an increase in emissions from South American temperate, Asian temperate and Asian tropical TransCom regions. In addition, the increase is hardly sensitive to different model configurations ( 4 yr−1 difference), and much smaller than suggested by EDGAR v4.2 FT2010 inventory (33 Tg CH4 yr−1), which was used for prior anthropogenic emission estimates. The result is in good agreement with other published estimates from inverse modelling studies (16–20 Tg CH4 yr−1). However, this study could not conclusively separate a small trend in biospheric emissions (−5 to +6.9 Tg CH4 yr−1) from the much larger trend in anthropogenic emissions (15–27 Tg CH4 yr−1). Finally, we find that the global and North American CH4 balance could be closed over this time period without the previously suggested need to strongly increase anthropogenic CH4 emissions in the United States. With further developments, especially on the treatment of the atmospheric CH4 sink, we expect the data assimilation system presented here will be able to contribute to the ongoing interpretation of changes in this important greenhouse gas budget.

The aim of this paper is to present an overview of inverse modeling methods that have been developed over the years for estimating the global sources and sinks of CH4. It provides insight into how techniques and estimates have evolved over time and what the remaining shortcomings are. As such, it serves a didactical purpose of introducing apprentices to the field, but it also takes stock of developments so far and reflects on promising new directions. The main focus is on methodological aspects that are particularly relevant for CH4, such as its atmospheric oxidation, the use of methane isotopologues, and specific challenges in atmospheric transport modeling of CH4. The use of satellite retrievals receives special attention as it is an active field of methodological development, with special requirements on the sampling of the model and the treatment of data uncertainty. Regional scale flux estimation and attribution is still a grand challenge, which calls for new methods capable of combining information from multiple data streams of different measured parameters. A process model representation of sources and sinks in atmospheric transport inversion schemes allows the integrated use of such data. These new developments are needed not only to improve our understanding of the main processes driving the observed global trend but also to support international efforts to reduce greenhouse gas emissions.

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, 4 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 Tropospheric Monitoring Instrument (TROPOMI) spectrometer is the single payload of the Copernicus Sentinel 5 Precursor (S5P) mission. It measures Earth radiance spectra in the shortwave infrared spectral range around 2.3 µm with a dedicated instrument module. These measurements provide carbon monoxide (CO) total column densities over land, which for clear sky conditions are highly sensitive to the tropospheric boundary layer. For cloudy atmospheres over land and ocean, the column sensitivity changes according to the light path through the atmosphere. In this study, we present the physics-based operational S5P algorithm to infer atmospheric CO columns satisfying the envisaged accuracy (

The distribution of methane (CH4) in the stratosphere can be a major driver of spatial variability in the dry-air column-averaged CH4 mixing ratio (XCH4), which is being measured increasingly for the assessment of CH4 surface emissions. Chemistry-transport models (CTMs) therefore need to simulate the tropospheric and stratospheric fractional columns of XCH4 accurately for estimating surface emissions from XCH4. Simulations from three CTMs are tested against XCH4 observations from the Total Carbon Column Network (TCCON). We analyze how the model–TCCON agreement in XCH4 depends on the model representation of stratospheric CH4 distributions. Model equivalents of TCCON XCH4 are computed with stratospheric CH4 fields from both the model simulations and from satellite-based CH4 distributions from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) and MIPAS CH4 fields adjusted to ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. Using MIPAS-based stratospheric CH4 fields in place of model simulations improves the model–TCCON XCH4 agreement for all models. For the Atmospheric Chemistry Transport Model (ACTM) the average XCH4 bias is significantly reduced from 38.1 to 13.7 ppb, whereas small improvements are found for the models TM5 (Transport Model, version 5; from 8.7 to 4.3 ppb) and LMDz (Laboratoire de Météorologie Dynamique model with zooming capability; from 6.8 to 4.3 ppb). Replacing model simulations with MIPAS stratospheric CH4 fields adjusted to ACE-FTS reduces the average XCH4 bias for ACTM (3.3 ppb), but increases the average XCH4 bias for TM5 (10.8 ppb) and LMDz (20.0 ppb). These findings imply that model errors in simulating stratospheric CH4 contribute to model biases. Current satellite instruments cannot definitively measure stratospheric CH4 to sufficient accuracy to eliminate these biases. Applying transport diagnostics to the models indicates that model-to-model differences in the simulation of stratospheric transport, notably the age of stratospheric air, can largely explain the inter-model spread in stratospheric CH4 and, hence, its contribution to XCH4. Therefore, it would be worthwhile to analyze how individual model components (e.g., physical parameterization, meteorological data sets, model horizontal/vertical resolution) impact the simulation of stratospheric CH4 and XCH4.

High-precision analyses of the isotopic composition of methane in ambient air can potentially be used to discriminate between different source categories. Due to the complexity of isotope ratio measurements, such analyses have generally been performed in the laboratory on air samples collected in the field. This poses a limitation on the temporal resolution at which the isotopic composition can be monitored with reasonable logistical effort. Here we present the performance of a dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique for in situ analysis of the isotopic composition of methane under field conditions. Both systems were deployed at the Cabauw Experimental Site for Atmospheric Research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months. The IRMS and QCLAS instruments were in excellent agreement with a slight systematic offset of (+0.25 ± 0.04) ‰ for δ13C and (−4.3 ± 0.4) ‰ for δD. This was corrected for, yielding a combined dataset with more than 2500 measurements of both δ13C and δD. The high-precision and high-temporal-resolution dataset not only reveals the overwhelming contribution of isotopically depleted agricultural CH4 emissions from ruminants at the Cabauw site but also allows the identification of specific events with elevated contributions from more enriched sources such as natural gas and landfills. The final dataset was compared to model calculations using the global model TM5 and the mesoscale model FLEXPART-COSMO. The results of both models agree better with the measurements when the TNO-MACC emission inventory is used in the models than when the EDGAR inventory is used. This suggests that high-resolution isotope measurements have the potential to further constrain the methane budget when they are performed at multiple sites that are representative for the entire European domain.

This study investigates the constraint provided by greenhouse gas measurements from space on surface fluxes. Imperfect knowledge of the light path through the atmosphere, arising from scattering by clouds and aerosols, can create biases in column measurements retrieved from space. To minimize the impact of such biases, ratios of total column retrieved CH4 and CO2 (Xratio) have been used. We apply the ratio inversion method described in Pandey et al. (2015) to retrievals from the Greenhouse Gases Observing SATellite (GOSAT). The ratio inversion method uses the measured Xratio as a weak constraint on CO2 fluxes. In contrast, the more common approach of inverting proxy CH4 retrievals (Frankenberg et al., 2005) prescribes atmospheric CO2 fields and optimizes only CH4 fluxes. The TM5–4DVAR (Tracer Transport Model version 5–variational data assimilation system) inverse modeling system is used to simultaneously optimize the fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy inversions using model-derived CO2 mixing ratios (XCO2model) from CarbonTracker and the Monitoring Atmospheric Composition and Climate (MACC) Reanalysis CO2 product. The performance of the inverse models is evaluated using measurements from three aircraft measurement projects. Xratio and XCO2model are compared with TCCON retrievals to quantify the relative importance of errors in these components of the proxy XCH4 retrieval (XCH4proxy). We find that the retrieval errors in Xratio (mean = 0.61 %) are generally larger than the errors in XCO2model (mean = 0.24 and 0.01 % for CarbonTracker and MACC, respectively). On the annual timescale, the CH4 fluxes from the different satellite inversions are generally in agreement with each other, suggesting that errors in XCO2model do not limit the overall accuracy of the CH4 flux estimates. On the seasonal timescale, however, larger differences are found due to uncertainties in XCO2model, particularly over Australia and in the tropics. The ratio method stays closer to the a priori CH4 flux in these regions, because it is capable of simultaneously adjusting the CO2 fluxes. Over tropical South America, comparison to independent measurements shows that CO2 fields derived from the ratio method are less realistic than those used in the proxy method. However, the CH4 fluxes are more realistic, because the impact of unaccounted systematic uncertainties is more evenly distributed between CO2 and CH4. The ratio inversion estimates an enhanced CO2 release from tropical South America during the dry season of 2010, which is in accordance with the findings of Gatti et al. (2014) and Van der Laan et al. (2015). The performance of the ratio method is encouraging, because despite the added nonlinearity due to the assimilation of Xratio and the significant increase in the degree of freedom by optimizing CO2 fluxes, still consistent results are obtained with respect to other CH4 inversions.

Data assimilation systems allow for estimating surface fluxes of greenhouse gases from atmospheric concentration measurements. Good knowledge about fluxes is essential to understand how climate change affects ecosystems and to characterize feedback mechanisms. Based on the assimilation of more than 1 year of atmospheric in situ concentration measurements, we compare the performance of two established data assimilation models, CarbonTracker and TM5-4DVar (Transport Model 5 – Four-Dimensional Variational model), for CO2 flux estimation. CarbonTracker uses an ensemble Kalman filter method to optimize fluxes on ecoregions. TM5-4DVar employs a 4-D variational method and optimizes fluxes on a 6° × 4° longitude–latitude grid. Harmonizing the input data allows for analyzing the strengths and weaknesses of the two approaches by direct comparison of the modeled concentrations and the estimated fluxes. We further assess the sensitivity of the two approaches to the density of observations and operational parameters such as the length of the assimilation time window. Our results show that both models provide optimized CO2 concentration fields of similar quality. In Antarctica CarbonTracker underestimates the wintertime CO2 concentrations, since its 5-week assimilation window does not allow for adjusting the distant surface fluxes in response to the detected concentration mismatch. Flux estimates by CarbonTracker and TM5-4DVar are consistent and robust for regions with good observation coverage, regions with low observation coverage reveal significant differences. In South America, the fluxes estimated by TM5-4DVar suffer from limited representativeness of the few observations. For the North American continent, mimicking the historical increase of the measurement network density shows improving agreement between CarbonTracker and TM5-4DVar flux estimates for increasing observation density.

We present a method for assimilating total column CH4 : CO2 ratio measurements from satellites for inverse modeling of CH4 and CO2 fluxes using the variational approach. Unlike conventional approaches, in which retrieved CH4 : CO2 are multiplied by model-derived total column CO2 and only the resulting CH4 is assimilated, our method assimilates the ratio of CH4 and CO2 directly and is therefore called the ratio method. It is a dual tracer inversion, in which surface fluxes of CH4 and CO2 are optimized simultaneously. The optimization of CO2 fluxes turns the hard constraint of prescribing model-derived CO2 fields into a weak constraint on CO2, which allows us to account for uncertainties in CO2. The method has been successfully tested in a synthetic inversion setup. We show that the ratio method is able to reproduce assumed true CH4 and CO2 fluxes starting from a prior, which is derived by perturbing the true fluxes randomly. We compare the performance of the ratio method with that of the traditional proxy approach and the use of only surface measurements for estimating CH4 fluxes. Our results confirm that the optimized CH4 fluxes are sensitive to the treatment of CO2, and that hard constraints on CO2 may significantly compromise results that are obtained for CH4. We find that the relative performance of ratio and proxy methods have a regional dependence. The ratio method performs better than the proxy method in regions where the CO2 fluxes are most uncertain. However, both ratio and proxy methods perform better than the surface-measurement-only inversion, confirming the potential of spaceborne measurements for accurately determining fluxes of CH4 and other greenhouse gases (GHGs).

The GHG-CCI project (http://www.esa-ghg-cci.org/) is one of several projects of the European Space Agency’s (ESA) Climate Change Initiative (CCI). The goal of the CCI is to generate and deliver data sets of various satellite-derived Essential Climate Variables (ECVs) in line with GCOS (Global Climate Observing System) requirements. The “ECV Greenhouse Gases” (ECV GHG) is the global distribution of important climate relevant gases – namely atmospheric CO2 and CH4 - with a quality sufficient to obtain information on regional CO2 and CH4 sources and sinks. The main goal of GHG-CCI is to generate long-term highly accurate and precise time series of global near-surface-sensitive satellite observations of CO2 and CH4, i.e., XCO2 and XCH4, starting with the launch of ESA’s ENVISAT satellite. These products are currently retrieved from SCIAMACHY/ENVISAT (2002-2012) and TANSO-FTS/GOSAT (2009-today) nadir mode observations in the near-infrared/shortwave-infrared spectral region. In addition, other sensors (e.g., IASI and MIPAS) and viewing modes (e.g., SCIAMACHY solar occultation) are also considered and in the future also data from other satellites. The GHG-CCI data products and related documentation are freely available via the GHG-CCI website and yearly updates are foreseen. Here we present an overview about the latest data set (Climate Research Data Package No. 2 (CRDP#2)) and summarize key findings from using satellite CO2 and CH4 retrievals to improve our understanding of the natural and anthropogenic sources and sinks of these important atmospheric greenhouse gases. We also shortly mention ongoing activities related to validation and initial user assessment of CRDP#2 and future plans.

Over the last decade, global-scale data sets of atmospheric water vapor isotopologues (HDO) have become available from different remote sensing instruments. Due to the observational geometry and the spectral ranges that are used, few satellites sample water isotopologues in the lower troposphere, where the bulk of hydrological processes within the atmosphere take place. Here, we compare three satellite HDO data sets, two from the Tropospheric Emission Spectrometer (TES retrieval version 4 and 5) and one from SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY), with results from the atmospheric global circulation model ECHAM4 (European Centre HAMburg 4). We examine a list of known isotopologue effects to qualitatively benchmark the various observational data sets. TES version 5 (TESV5), TES version 4 (TESV4), SCIAMACHY, ECHAM, and ECHAM convolved with averaging kernels of TES version 5 (ECHAMAK5) successfully reproduced a number of established isotopologue effects such as the latitude effect, the amount effect, and the continental effect. The improvement of TESV5 over TESV4 is confirmed by the steeper latitudinal gradient at higher latitudes in agreement with SCIAMACHY. Also the representation of other features of the water isotopologue cycle, such as the seasonally varying signal in the tropics due to the movement of the Intertropical Convergence Zone (ITCZ), is improved in TESV5 and SCIAMACHY compared to TESV4. A known humidity bias due to the cross correlation of H2O and HDO measurements, which is of particular importance for instruments with low sensitivity close to the surface, was analyzed by applying either a humidity bias correction or a suitable a posteriori analysis. We suggest that the qualitative and quantitative tests carried out in this study could become benchmark tests for evaluation of future satellite isotopologue data sets.

Two years of satellite observations were used to quantify methane emissions from coal mines in Queensland, the largest coal-producing state in Australia. The six analyzed surface and underground coal mines are estimated to emit 570 ± 98 Gg a -1 in 2018-2019. Together, they account for 7% of the national coal production while emitting 55 ± 10% of the reported methane emission from coal mining in Australia. Our results indicate that for two of the three locations, our satellite-based estimates are significantly higher than reported to the Australian government. Most remarkably, 40% of the quantified emission came from a single surface mine (Hail Creek) located in a methane-rich coal basin. Our findings call for increased monitoring and investment in methane recovery technologies for both surface and underground mines.

Southeast Australia experienced intensive and geographically extensive wildfires during the 2019-2020 summer season 1,2 . The fires released substantial amounts of carbon dioxide into the atmosphere 3 . However, existing emission estimates based on fire inventories are uncertain 4 , and vary by up to a factor of four for this event. Here we constrain emission estimates with the help of satellite observations of carbon monoxide 5 , an analytical Bayesian inversion 6 and observed ratios between emitted carbon dioxide and carbon monoxide 7 . We estimate emissions of carbon dioxide to be 715 teragrams (range 517-867) from November 2019 to January 2020. This is more than twice the estimate derived by five different fire inventories 8-12 , and broadly consistent with estimates based on a bottom-up bootstrap analysis of this fire episode 13 . Although fires occur regularly in the savannas in northern Australia, the recent episodes were extremely large in scale and intensity, burning unusually large areas of eucalyptus forest in the southeast 13 . The fires were driven partly by climate change 14,15 , making better-constrained emission estimates particularly important. This is because the build-up of atmospheric carbon dioxide may become increasingly dependent on fire-driven climate-carbon feedbacks, as highlighted by this event 16 ., (© 2021. The Author(s), under exclusive licence to Springer Nature Limited.)

Quantifying natural geological sources of methane (CH 4 ) allows to improve the assessment of anthropogenic emissions to the atmosphere from fossil fuel industries. The global CH 4 flux of geological gas is, however, an object of debate. Recent fossil ( 14 C-free) CH 4 measurements in preindustrial-era ice cores suggest very low global geological emissions (~ 1.6 Tg year -1 ), implying a larger fossil fuel industry source. This is however in contrast with previously published bottom-up and top-down geo-emission estimates (~ 45 Tg year -1 ) and even regional-scale emissions of ~ 1-2 Tg year -1 . Here we report on significant geological CH 4 emissions from the Lusi hydrothermal system (Indonesia), measured by ground-based and satellite (TROPOMI) techniques. Both techniques indicate a total CH 4 output of ~ 0.1 Tg year -1 , equivalent to the minimum value of global geo-emission derived by ice core 14 CH 4 estimates. Our results are consistent with the order of magnitude of the emission factors of large seeps used in global bottom-up estimates, and endorse a substantial contribution from natural Earth's CH 4 degassing. The preindustrial ice core assessments of geological CH 4 release may be underestimated and require further study. Satellite measurements can help to test geological CH 4 emission factors and explain the gap between the contrasting estimates.

Using new satellite observations and atmospheric inverse modeling, we report methane emissions from the Permian Basin, which is among the world's most prolific oil-producing regions and accounts for >30% of total U.S. oil production. Based on satellite measurements from May 2018 to March 2019, Permian methane emissions from oil and natural gas production are estimated to be 2.7 ± 0.5 Tg a -1 , representing the largest methane flux ever reported from a U.S. oil/gas-producing region and are more than two times higher than bottom-up inventory-based estimates. This magnitude of emissions is 3.7% of the gross gas extracted in the Permian, i.e., ~60% higher than the national average leakage rate. The high methane leakage rate is likely contributed by extensive venting and flaring, resulting from insufficient infrastructure to process and transport natural gas. This work demonstrates a high-resolution satellite data-based atmospheric inversion framework, providing a robust top-down analytical tool for quantifying and evaluating subregional methane emissions., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).)

Methane emissions due to accidents in the oil and natural gas sector are very challenging to monitor, and hence are seldom considered in emission inventories and reporting. One of the main reasons is the lack of measurements during such events. Here we report the detection of large methane emissions from a gas well blowout in Ohio during February to March 2018 in the total column methane measurements from the spaceborne Tropospheric Monitoring Instrument (TROPOMI). From these data, we derive a methane emission rate of 120 ± 32 metric tons per hour. This hourly emission rate is twice that of the widely reported Aliso Canyon event in California in 2015. Assuming the detected emission represents the average rate for the 20-d blowout period, we find the total methane emission from the well blowout is comparable to one-quarter of the entire state of Ohio's reported annual oil and natural gas methane emission, or, alternatively, a substantial fraction of the annual anthropogenic methane emissions from several European countries. Our work demonstrates the strength and effectiveness of routine satellite measurements in detecting and quantifying greenhouse gas emission from unpredictable events. In this specific case, the magnitude of a relatively unknown yet extremely large accidental leakage was revealed using measurements of TROPOMI in its routine global survey, providing quantitative assessment of associated methane emissions.

Several viable but conflicting explanations have been proposed to explain the recent ~8 p.p.b. per year increase in atmospheric methane after 2006, equivalent to net emissions increase of ~25 Tg CH 4 per year. A concurrent increase in atmospheric ethane implicates a fossil source; a concurrent decrease in the heavy isotope content of methane points toward a biogenic source, while other studies propose a decrease in the chemical sink (OH). Here we show that biomass burning emissions of methane decreased by 3.7 (±1.4) Tg CH 4 per year from the 2001-2007 to the 2008-2014 time periods using satellite measurements of CO and CH 4 , nearly twice the decrease expected from prior estimates. After updating both the total and isotopic budgets for atmospheric methane with these revised biomass burning emissions (and assuming no change to the chemical sink), we find that fossil fuels contribute between 12-19 Tg CH 4 per year to the recent atmospheric methane increase, thus reconciling the isotopic- and ethane-based results.

Year-to-year variations in the atmospheric methane (CH 4 ) growth rate show significant correlation with climatic drivers. The second half of 2010 and the first half of 2011 experienced the strongest La Niña since the early 1980s, when global surface networks started monitoring atmospheric CH 4 mole fractions. We use these surface measurements, retrievals of column-averaged CH 4 mole fractions from GOSAT, new wetland inundation estimates, and atmospheric δ 13 C-CH 4 measurements to estimate the impact of this strong La Niña on the global atmospheric CH 4 budget. By performing atmospheric inversions, we find evidence of an increase in tropical CH 4 emissions of ∼6-9 TgCH 4 yr -1 during this event. Stable isotope data suggest that biogenic sources are the cause of this emission increase. We find a simultaneous expansion of wetland area, driven by the excess precipitation over the Tropical continents during the La Niña. Two process-based wetland models predict increases in wetland area consistent with observationally-constrained values, but substantially smaller per-area CH 4 emissions, highlighting the need for improvements in such models. Overall, tropical wetland emissions during the strong La Niña were at least by 5% larger than the long-term mean.