Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. CH4 is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2), and both emissions and atmospheric concentrations of CH4 have continued to increase since 2007 after a temporary pause. The relative importance of CH4 emissions compared to those of CO2 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in quantifying the factors responsible for the observed atmospheric growth rate arise from diverse, geographically overlapping CH4 sources and from the uncertain magnitude and temporal change in the destruction of CH4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise, and update the global CH4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH4 budget, integrating results of top-down CH4 emission estimates (based on in situ and Greenhouse Gases Observing SATellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full data sets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this 2025 edition benefits from important progress in estimating inland freshwater emissions, with better counting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double counting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double counting that may exist (average of 23 Tg CH4 yr−1). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH4 yr−1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH4 yr−1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH4 yr−1 or ∼ 65 % is attributed to direct anthropogenic sources in the fossil, agriculture, and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr−1 or 63 %–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH4 yr−1 (range 9–40). The 2020 emission rate is the highest of the period and reaches 608 Tg CH4 yr−1 (range 581–627), which is 12 % higher than the average emissions in the 2000s. Since 2012, global direct anthropogenic CH4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH4 yr−1) larger global emissions (669 Tg CH4 yr−1, range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH4 yr−1 in Saunois et al. (2016, 2020) respectively), and for the first time uncertainties in bottom-up and top-down budgets overlap. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. The tropospheric loss of methane, as the main contributor to methane lifetime, has been estimated at 563 [510–663] Tg CH4 yr−1 based on chemistry–climate models. These values are slightly larger than for 2000–2009 due to the impact of the rise in atmospheric methane and remaining large uncertainty (∼ 25 %). The total sink of CH4 is estimated at 633 [507–796] Tg CH4 yr−1 by the bottom-up approaches and at 554 [550–567] Tg CH4 yr−1 by top-down approaches. However, most of the top-down models use the same OH distribution, which introduces less uncertainty to the global budget than is likely justified. For 2010–2019, agriculture and waste contributed an estimated 228 [213–242] Tg CH4 yr−1 in the top-down budget and 211 [195–231] Tg CH4 yr−1 in the bottom-up budget. Fossil fuel emissions contributed 115 [100–124] Tg CH4 yr−1 in the top-down budget and 120 [117–125] Tg CH4 yr−1 in the bottom-up budget. Biomass and biofuel burning contributed 27 [26–27] Tg CH4 yr−1 in the top-down budget and 28 [21–39] Tg CH4 yr−1 in the bottom-up budget. We identify five major priorities for improving the CH4 budget: (i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH4 based on a robust classification of different types of emitting ecosystems; (ii) further development of process-based models for inland-water emissions; (iii) intensification of CH4 observations at local (e.g. FLUXNET-CH4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture, and landfills) to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GKQ9-2RHT (Martinez et al., 2024).

This review summarizes the rapid advances in direct practical methods to quantify and reduce agricultural methane emissions worldwide. Major tasks are location, identification, quantification and distinction between different specific sources (often multiple emitters such as manure pools, animal housing, biodigesters and landfills are co-located). Emission reduction, facilitated by developing methodologies for locating hot spots, is the least-cost choice for action, especially from manure stores, biodigesters and from controlling biomass burning. Agricultural methane can also be used to generate electricity or, in appropriate circumstances, can be destroyed by oxidation. It may be possible to cut North American, East Asian and European emissions sharply and rapidly. In Africa and South Asia, emissions from crop waste and food waste in landfills, also a source of air pollution, can be sharply and quickly reduced. Globally, cutting total annual agricultural and waste emissions by a third would demand reductions of very approximately 75 Tg yr −1 . Apportioned by source type, notional cuts might be 30–40 Tg yr −1 from livestock and manure, 5-10 Tg yr −1 from rice cultivation and 20 Tg yr −1 or more from specifically agricultural waste.

From 2020, the atmospheric methane burden has grown at the fastest rate in the detailed observational record. This rise has been accompanied by an unprecedented plunge in d13C(CH4). The causes of recent accelerated growth are as yet uncertain but the geographic spread of growth and the rapid isotopic plunge suggest strong rises in isotopically light emissions from both Tropical and Boreal wetlands. These emissions may be due to rising precipitation and temperatures in parts of the tropics, and by rising temperatures in northern Canada, Siberia, and Europe. Over the longer period since 2007, methane’s actual growth is comparable to methane’s growth in the ‘worst case’ very high baseline emission scenario RCP8.5 (8.5 W/m2 forcing increase relative to pre-industrial). If the recent trend were to continue for more than another decade it could make the 2°C target as hard to achieve as the 1.5°C target is now. Natural feedbacks to climate warming in wetlands need to be included in future modelling and should be incorporated in climate modelling projects such as CMIP7. Methane’s recent accelerated growth also has wide implications for climate negotiations as it reduces the permissible total anthropogenic greenhouse gas emissions if the Paris Agreement is to be achieved. Strong growth in non-anthropogenic methane emissions, driven by feedback impacts on natural and quasi-natural sources, was not expected in modelling at the time of the Paris Agreement and shows the urgency of improving our understanding of the feedback impacts of climate change. The simplest way to limit methane’s growth is for all nations, including non-signatory countries, to cut anthropogenic emissions urgently and sharply, meeting or exceeding the targets of the Global Methane Pledge.

Rapid warming in the Arctic has the potential to release vast reservoirs of carbon into the atmosphere as methane (CH4) resulting in a strong positive climate feedback. This raises the concern that, after a period of near-zero growth in atmospheric CH4 burden from 1999 to 2006, the increase since then may be in part related to increased Arctic emissions. Measurements of CH4 in background air samples provide useful, direct information to determine if Arctic CH4 emissions are increasing. One sensitive first-order indicator for large emission change is the Interpolar Difference, that is the difference in surface atmospheric annual means between polar northern and southern zones (53°–90°), which has varied interannually, but did not increase from 1992 to 2019. The Interpolar Difference has increased moderately during 2020–2022 when the global CH4 burden increased significantly, but not yet to its peak values in the late-1980s. For quantitative assessment of changing Arctic CH4 emissions, the atmospheric measurements must be combined with an atmospheric tracer transport model. Based on multiple studies including some using CH4 isotopes, it is clear that most of the increase in global atmospheric CH4 burden is driven by increased emissions from microbial sources in the tropics, and that Arctic emissions have not increased significantly since the beginning of our measurement record in 1983 through 2022.

This paper highlights the main findings of the eighteenth annual Greenhouse Gas Bulletin (https://library.wmo.int/index.php?lvl=notice_display&id=22149) of the World Meteorological Organization (WMO). The results are based on research and observations performed by laboratories contributing to the WMO Global Atmosphere Watch (GAW) Programme (https://community.wmo.int/activity-areas/gaw).The Bulletin presents global analyses of observational data collected according to GAW recommended practices and submitted to the World Data Center for Greenhouse Gases (WDCGG). Bulletins are prepared by the WMO/GAW Scientific Advisory Group on Greenhouse Gases in collaboration with WDCGG.Observations used for the global analysis are from more than 100 marine and terrestrial sites worldwide for CO2 and CH4 and at a smaller number of sites for other greenhouse gases. The globally averaged surface mole fractions calculated from this in situ network reached new highs in 2021, with CO2 at 415.7 ± 0.2 ppm, CH4 at 1908 ± 2 ppb and N2O at 334.0 ± 0.1 ppb. These values constitute, respectively, 149%, 262% and 124% of pre-industrial (before 1750) levels. The increase in CO2 from 2020 to 2021 was equal to that observed from 2019 to 2020 and larger than the average annual growth rate over the last decade. For CH4, the increase from 2020 to 2021 was higher than that observed from 2019 to 2020 and considerably higher than the average annual growth rate over the last decade. For N2O, the increase from 2020 to 2021 was slightly higher than that observed from 2019 to 2020 and also higher than the average annual growth rate over the last decade.The Bulletin highlights the exceptional growth of CH4 in 2020 and 2021. The causes of these exceptional increases are still being investigated though analyses of measurements of atmospheric CH4 abundance and its stable carbon isotope ratio 13C/12C indicate that the increase in CH4 since 2007 is associated mostly with biogenic processes, but the relative contributions of anthropogenic and natural sources to this increase are unclear.The Bulletin further highlights that the accuracy of emissions estimates from atmospheric measurements depends on the geometry of the surface network, pointing to the large observational gaps in tropical regions and the interior of the Asian continent. The tropics accommodate not only highly uncertain emissions from natural wetlands, but also the atmospheric hydroxyl radical sink of CH4, which is largest there. Surface measurements provide limited information to distinguish between increasing surface emissions and decreasing atmospheric sinks, which could both explain the increasing atmospheric CH4 abundance.WMO is working with the broader greenhouse gas community to develop a framework for sustained, internationally coordinated global greenhouse gas monitoring. These efforts are envisaged to result in an internationally coordinated approach to observing network design and acquisition, international exchange and use of the observations. It is foreseen that this will result in the expansion of the in-situ network, especially in currently undersampled regions and lead to reduced uncertainties in the quantification of the net atmospheric balance of CH4 and other greenhouse gases.

Atmospheric methane's rapid growth from late 2006 is unprecedented in the observational record. Assessment of atmospheric methane data attributes a large fraction of this atmospheric growth to increased natural emissions over the tropics, which appear to be responding to changes in anthropogenic climate forcing. Isotopically lighter measurements of delta(13)C(CH4 )are consistent with the recent atmospheric methane growth being mainly driven by an increase in emissions from microbial sources, particularly wetlands. The global methane budget is currently in disequilibrium and new inputs are as yet poorly quantified. Although microbial emissions from agriculture and waste sources have increased between 2006 and 2022 by perhaps 35 Tg/yr, with wide uncertainty, approximately another 35-45 Tg/yr of the recent net growth in methane emissions may have been driven by natural biogenic processes, especially wetland feedbacks to climate change. A model comparison shows that recent changes may be comparable or greater in scale and speed than methane's growth and isotopic shift during past glacial/interglacial termination events. It remains possible that methane's current growth is within the range of Holocene variability, but it is also possible that methane's recent growth and isotopic shift may indicate a large-scale reorganization of the natural climate and biosphere is under way.

This study investigates atmospheric δ13CH4 trends, as produced by a global atmospheric transport model using CH4 inversions from CarbonTracker-Europe CH4 for 2000–2020, and compares them to observations. The CH4 inversions include the grouping of the emissions both by δ13CH4 isotopic signatures and process type to investigate the effect, and to estimate the CH4 magnitudes and model CH4 and δ13CH4 trends. In addition to inversion results, simulations of the global atmospheric transport model were performed with modified emissions. The estimated global CH4 trends for oil and gas were found to increase more than coal compared to the priors from 2000–2006 to 2007–2020. Estimated trends for coal emissions at 30∘ N–60∘ N are less than 50% of those from priors. Estimated global CH4 rice emissions trends are opposite to priors, with the largest contribution from the EQ to 60∘ N. The results of this study indicate that optimizing wetland emissions separately produces better agreement with the observed δ13CH4 trend than optimizing all biogenic emissions simultaneously. This study recommends optimizing separately biogenic emissions with similar isotopic signature to wetland emissions. In addition, this study suggests that fossil-based emissions were overestimated by 9% after 2012 and biogenic emissions are underestimated by 8% in the inversion using EDGAR v6.0 as priors.

Sulfur hexafluoride (SF6) is the most potent greenhouse gas (GHG), and its atmospheric abundance, albeit small, has been increasing rapidly. Although SF6 is used to assess atmospheric transport modeling and its emissions influence the climate for millennia, SF6 emission magnitudes and distributions have substantial uncertainties. In this study, we used NOAA's ground-based and airborne measurements of SF6 to estimate SF6 emissions from the United States between 2007 and 2018. Our results suggest a substantial decline of US SF6 emissions, a trend also reported in the US Environmental Protection Agency's (EPA) national inventory submitted under the United Nations Framework Convention on Climate Change (UNFCCC), implying that US mitigation efforts have had some success. However, the magnitudes of annual emissions derived from atmospheric observations are 40 %–250 % higher than the EPA's national inventory and substantially lower than the Emissions Database for Global Atmospheric Research (EDGAR) inventory. The regional discrepancies between the atmosphere-based estimate and EPA's inventory suggest that emissions from electric power transmission and distribution (ETD) facilities and an SF6 production plant that did not or does not report to the EPA may be underestimated in the national inventory. Furthermore, the atmosphere-based estimates show higher emissions of SF6 in winter than in summer. These enhanced wintertime emissions may result from increased maintenance of ETD equipment in southern states and increased leakage through aging brittle seals in ETD in northern states during winter. The results of this study demonstrate the success of past US SF6 emission mitigations and suggest that substantial additional emission reductions might be achieved through efforts to minimize emissions during servicing or through improving sealing materials in ETD.

Methane is a major greenhouse gas (GHG) that has contributed to one third of the warming induced by all GHGs since the preindustrial era (IPCC, 2021). Reliable quantification of methane emissions is critical for tracking progress towards methane mitigation, especially for the countries that join the Global Methane Pledge and that have firm plans for reducing methane emissions over the next decades, such as the US. In this study, we quantified US methane emissions using inverse modeling of ground- and airborne- methane measurements made from the NOAA Greenhouse Gas Reference Network for 2007 – 2021. We conducted 12 inversion runs using two high-resolution transport models (HYSPLIT-NAMs and WRF-STILT), three background estimates, and two prior emission fields. Multiple estimates of wetland emissions were considered and subtracted from our inversion-derived total emission estimates. Our derived anthropogenic emissions show a consistent increasing trend after 2015 across our inversion ensemble members and a seasonal cycle in emission magnitude that repeats every year during our study period. Both the trend and seasonal variation seem to correlate with US natural gas consumption. A similar seasonal variability has been reported previously, but only on an urban scale; this is the first time it has been derived on a national scale. Furthermore, we also compared our estimates with US EPA’s national GHG inventory reporting and investigated the impact of the COVID-19 pandemic on emissions in 2020 relative to 2019 and 2021.

Atmospheric concentrations of methane, a powerful greenhouse gas, have strongly increased since 2007. Measurements of stable carbon isotopes of methane can constrain emissions if the isotopic compositions are known; however, isotopic compositions of methane emissions from wetlands are poorly constrained despite their importance. Here, we use a process-based biogeochemistry model to calculate the stable carbon isotopic composition of global wetland methane emissions. We estimate a mean global signature of −61.3 ± 0.7‰ and find that tropical wetland emissions are enriched by ~11‰ relative to boreal wetlands. Our model shows improved resolution of regional, latitudinal and global variations in isotopic composition of wetland emissions. Atmospheric simulation scenarios with the improved wetland isotopic composition suggest that increases in atmospheric methane since 2007 are attributable to rising microbial emissions. Our findings substantially reduce uncertainty in the stable carbon isotopic composition of methane emissions from wetlands and improve understanding of the global methane budget.

Abstract. Sulfur hexafluoride (SF6) is the most potent greenhouse gas and its atmospheric abundance, albeit small, has been increasing rapidly. Although SF6 is used to assess atmospheric transport modeling and influences the climate for millennia, SF6 emission magnitudes and distributions have substantial uncertainties. In this study, we used NOAA’s ground-based and airborne measurements of SF6 to estimate SF6 emissions from the U.S. between 2007 and 2018. The substantial decline in U.S. SF6 emissions derived from atmospheric observations agrees with the reported trend in the U.S. Environmental Protection Agency (EPA)’s national inventory submitted under the United Nations Framework on Climate Change, suggesting mitigation efforts have had some success. However, the magnitudes of derived annual emissions are 40–250 % higher than the EPA national inventory and substantially lower than the Emissions Database for Global Atmospheric Research inventory. The regional discrepancies between atmosphere-based estimate and EPA’s inventory suggest that emissions from electric power transmission and distribution (ETD) facilities and an SF6 production plant that did not or do not report to EPA may be underestimated in the national inventory. Furthermore, the atmosphere-based estimates show higher winter than summer emissions of SF6. These enhanced wintertime emissions may result from increased maintenance of ETD equipment in southern states and increased leakage through aging brittle seals in ETD in northern states in winter. These results demonstrate the success of past U.S. SF6 emission mitigations, and suggest substantial additional emission reductions might be achieved through efforts to minimize emissions during servicing or through improving sealing materials in ETD.

Atmospheric nitrous oxide (N2O) contributes to global warming and stratospheric ozone depletion, so reducing uncertainty in estimates of emissions from different sources is important for climate policy. In this study, we simulate atmospheric N2O using an atmospheric chemistry-transport model (ACTM), and the results are first compared with the in situ measurements. Five combinations of known (a priori) N2O emissions due to natural soil, agricultural land, other human activities, and sea–air exchange are used. The N2O lifetime is 127.6 ± 4.0 yr in the control ACTM simulation (range indicates interannual variability). Regional N2O emissions are optimized using Bayesian inverse modeling for 84 partitions of the globe at monthly intervals, using measurements at 42 sites around the world covering 1997–2019. The best estimated global land and ocean emissions are 12.99 ± 0.22 TgN yr−1 and 2.74 ± 0.27 TgN yr−1, respectively, for 2000–2009, and 14.30 ± 0.20 TgN yr−1 and 2.91 ± 0.27 TgN yr−1, respectively, for 2010–2019. On regional scales, we find that the most recent ocean emission estimation, with lower emissions in the Southern Ocean regions, fits better with that predicted by the inversions. Marginally higher (lower) emissions than the inventory/model for the tropical (extratropical) land regions are estimated and validated using independent aircraft observations. Global land and ocean emission variabilities show a statistically significant correlation with El Niño Southern Oscillation (ENSO). Analysis of regional land emissions shows increases over America (Temperate North, Central, and Tropical), Central Africa, and Asia (South, East, and Southeast) between the 2000s and 2010s. Only Europe as a whole recorded a slight decrease in N2O emissions due to the chemical industry. Our inversions suggest revisions to seasonal emission variations for three of the 15 land regions (East Asia, Temperate North America, and Central Africa), and the Southern Ocean region. The terrestrial ecosystem model (Vegetation Integrative SImulator for Trace Gases) can simulate annual total emissions in agreement with the observed N2O growth rate since 1978, but the lag-time scales of N2O emissions from nitrogen fertilizer application may need to be revised.

Nitrous oxide (N 2 O) is the third most important anthropogenic greenhouse gas and a major ozone‐depleting substance. Its main sources include anthropogenic activities (mostly agriculture) and natural emissions from ocean and soils. However, emission estimates for individual sources are highly variable due to uncertainties in N 2 O lifetime estimates and partitioning among sources. We derive annual global N 2 O emissions for 1990–2019 using NOAA Global Monitoring Laboratory (GML) surface N 2 O observations and the N 2 O lifetime calculated in the NASA GEOS‐5 chemistry climate model. The inferred global mean N 2 O emissions has gradually increased from ∼15.8 TgN/yr in the early 1990s to ∼17.8 TgN/yr in the 2010s. This implies that anthropogenic N 2 O emissions have grown rapidly from ∼6.7 TgN/yr in the 1990s to about ∼8.7 TgN/yr in the 2010s, a ∼30% increase. With specially designed N 2 O isotopic tracers in 3‐D GEOSCCM, we estimate that, on global average, stratospheric enrichment contributes about +7.7‰/yr, +7.6‰/yr, +8.0‰/yr to tropospheric δ 15 N α , δ 15 N β , and δ 18 O budget, respectively. To balance the global mean isotopic signature for pre‐industrial terrestrial sources of δ 15 N α ∼ 6.7‰, δ 15 N β ∼ −12.6‰, δ 18 O ∼ 35.4‰, our 3‐dimensional isotopic budget simulation using the GEOSCCM suggests global mean anthropogenic isotopic signatures in the recent decades are δ 15 N α ∼ −18‰, δ 15 N β ∼ −20‰, δ 18 O ∼ 19‰. These anthropogenic isotopic estimates are significantly lighter than results from one‐box atmospheric model‐based estimates with the largest difference seen for δ 15 N β . More surface isotopic measurements are needed to better quantify the N 2 O isotopic signatures.

We have constructed an atmospheric inversion framework based on TM5-4DVAR to jointly assimilate measurements of methane and delta C-13 of methane in order to estimate source-specific methane emissions. Here we present global emission estimates from this framework for the period 1999-2016. We assimilate a newly constructed, multi-agency database of CH4 and delta C-13 measurements. We find that traditional CH4-only atmospheric inversions are unlikely to estimate emissions consistent with atmospheric delta C-13 data, and assimilating delta C-13 data is necessary to derive emissions consistent with both measurements. Our framework attributes ca. 85 % of the post-2007 growth in atmospheric methane to microbial sources, with about half of that coming from the tropics between 23.5 degrees N and 23.5 degrees S. This contradicts the attribution of the recent growth in the methane budget of the Global Carbon Project (GCP). We find that the GCP attribution is only consistent with our top-down estimate in the absence of delta C-13 data. We find that at global and continental scales, delta C-13 data can separate microbial from fossil methane emissions much better than CH4 data alone, and at smaller scales this ability is limited by the current delta C-13 measurement coverage. Finally, we find that the largest uncertainty in using delta C-13 data to separate different methane source types comes from our knowledge of atmospheric chemistry, specifically the distribution of tropospheric chlorine and the isotopic discrimination of the methane sink.

This study investigates the contribution of different CH4 sources to the seasonal cycle of δ13C during 2000–2012 by using the TM5 atmospheric transport model, including spatially varying information on isotopic signatures. The TM5 model is able to produce the background seasonality of δ13C, but the discrepancies compared to the observations arise from incomplete representation of the emissions and their source-specific signatures. Seasonal cycles of δ13C are found to be an inverse of CH4 cycles in general, but the anti-correlations between CH4 and δ13C are imperfect and experience a large variation (p=−0.35 to −0.91) north of 30° S. We found that wetland emissions are an important driver in the δ13C seasonal cycle in the Northern Hemisphere and Tropics, and in the Southern Hemisphere Tropics, emissions from fires contribute to the enrichment of δ13C in July–October. The comparisons to the observations from 18 stations globally showed that the seasonal cycle of EFMM emissions in the EDGAR v5.0 inventory is more realistic than in v4.3.2. At northern stations (north of 55° N), modeled δ13C amplitudes are generally smaller by 12–68%, mainly because the model could not reproduce the strong depletion in autumn. This indicates that the CH4 emission magnitude and seasonal cycle of wetlands may need to be revised. In addition, results from stations in northern latitudes (19–40° N) indicate that the proportion of biogenic to fossil-based emissions may need to be revised, such that a larger portion of fossil-based emissions is needed during summer.

Mixing of neighboring data points in a sequence is a common, but understudied, effect in physical experiments. This can occur in the measurement apparatus (if material from multiple time points is pulled into a measurement chamber simultaneously, for instance) or the system itself, e.g., via diffusion of isotopes in an ice sheet. We propose a model-free technique to detect this kind of local mixing in time-series data using an information-theoretic technique called permutation entropy. By varying the temporal resolution of the calculation and analyzing the patterns in the results, we can determine whether the data are mixed locally, and on what scale. This can be used by practitioners to choose appropriate lower bounds on scales at which to measure or report data. After validating this technique on several synthetic examples, we demonstrate its effectiveness on data from a chemistry experiment, methane records from Mauna Loa, and an Antarctic ice core.

Atmospheric CH4 is arguably the most interesting of the anthropogenically influenced, long-lived greenhouse gases. It has a diverse suite of sources, each presenting its own challenges in quantifying emissions, and while its main sink, atmospheric oxidation initiated by reaction with hydroxyl radical (OH), is well-known, determining the magnitude and trend in this and other smaller sinks remains challenging. Here, we provide an overview of the state of knowledge of the dynamic atmospheric CH4 budget of sources and sinks determined from measurements of CH4 and δ13CCH4 in air samples collected predominantly at background air sampling sites. While nearly four decades of direct measurements provide a strong foundation of understanding, large uncertainties in some aspects of the global CH4 budget still remain. More complete understanding of the global CH4 budget requires significantly more observations, not just of CH4 itself, but other parameters to better constrain key, but still uncertain, processes like wetlands and sinks. This article is part of a discussion meeting issue 'Rising methane: is warming feeding warming? (part 1)'.

The mean age since air was last at the Northern Hemisphere (NH) midlatitude surface is a fundamental property of tropospheric transport. Here we approximate the mean age in terms of an "SF6 age" (Gamma SF6), derived from surface and aircraft measurements of SF6 that are broader in spatial scope and cover a longer time period (1997-2018) than considered previously. At the surface, Gamma SF6 increases from near-zero values north of 30 degrees N to similar to 1.5 years over the Southern Hemisphere (SH) extratropics, with the largest meridional gradients occurring in the tropics. By comparison, vertical gradients in Gamma SF6 are weak throughout, with only slight increases/decreases with height in the NH/SH. The broader spatial coverage of the measurements reveals strong variations in the seasonal cycle of Gamma SF6 within the (sub)tropics that are weaker over the Atlantic and Pacific oceans, compared to over the Indian Ocean. Observations from 2000 to 2018 reveal that the SF6 age at sites in the SH has been decreasing by similar to 0.12 years/dec. However, this decrease is not due to changes in transport but, rather, is likely related to changes in emissions, which have increased globally and reportedly shifted from northern midlatitudes into the subtropics. Simulations, which reproduce the SF6 age trends, show no decreases in an age-of-air tracer, reinforcing the fact that Gamma SF6 represents only an approximation to the mean age. Finally, the modeled SF6 ages are older than observed, by similar to 0.3-0.4 years throughout the southern extratropics. We show that this bias is partly related to an overestimation in simulated SF6 near emissions regions, likely reflecting a combination of uncertainties in emissions and model transport.