Abstract. 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.

Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere in a changing climate – the “global carbon budget” – is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe and synthesize data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFOS) are based on energy statistics and cement production data, while emissions from land-use change (ELUC), mainly deforestation, are based on land use and land-use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly and its growth rate (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) and terrestrial CO2 sink (SLAND) are estimated with global process models constrained by observations. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the last decade available (2010–2019), EFOS was 9.6 ± 0.5 GtC yr−1 excluding the cement carbonation sink (9.4 ± 0.5 GtC yr−1 when the cement carbonation sink is included), and ELUC was 1.6 ± 0.7 GtC yr−1. For the same decade, GATM was 5.1 ± 0.02 GtC yr−1 (2.4 ± 0.01 ppm yr−1), SOCEAN 2.5 ±  0.6 GtC yr−1, and SLAND 3.4 ± 0.9 GtC yr−1, with a budget imbalance BIM of −0.1 GtC yr−1 indicating a near balance between estimated sources and sinks over the last decade. For the year 2019 alone, the growth in EFOS was only about 0.1 % with fossil emissions increasing to 9.9 ± 0.5 GtC yr−1 excluding the cement carbonation sink (9.7 ± 0.5 GtC yr−1 when cement carbonation sink is included), and ELUC was 1.8 ± 0.7 GtC yr−1, for total anthropogenic CO2 emissions of 11.5 ± 0.9 GtC yr−1 (42.2 ± 3.3 GtCO2). Also for 2019, GATM was 5.4 ± 0.2 GtC yr−1 (2.5 ± 0.1 ppm yr−1), SOCEAN was 2.6 ± 0.6 GtC yr−1, and SLAND was 3.1 ± 1.2 GtC yr−1, with a BIM of 0.3 GtC. The global atmospheric CO2 concentration reached 409.85 ± 0.1 ppm averaged over 2019. Preliminary data for 2020, accounting for the COVID-19-induced changes in emissions, suggest a decrease in EFOS relative to 2019 of about −7 % (median estimate) based on individual estimates from four studies of −6 %, −7 %, −7 % (−3 % to −11 %), and −13 %. Overall, the mean and trend in the components of the global carbon budget are consistently estimated over the period 1959–2019, but discrepancies of up to 1 GtC yr−1 persist for the representation of semi-decadal variability in CO2 fluxes. Comparison of estimates from diverse approaches and observations shows (1) no consensus in the mean and trend in land-use change emissions over the last decade, (2) a persistent low agreement between the different methods on the magnitude of the land CO2 flux in the northern extra-tropics, and (3) an apparent discrepancy between the different methods for the ocean sink outside the tropics, particularly in the Southern Ocean. This living data update documents changes in the methods and data sets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this data set (Friedlingstein et al., 2019; Le Quéré et al., 2018b, a, 2016, 2015b, a, 2014, 2013). The data presented in this work are available at https://doi.org/10.18160/gcp-2020 (Friedlingstein et al., 2020).

Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere – the “global carbon budget” – is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFF) are based on energy statistics and cement production data, while emissions from land use change (ELUC), mainly deforestation, are based on land use and land use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly and its growth rate (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) and terrestrial CO2 sink (SLAND) are estimated with global process models constrained by observations. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the last decade available (2009–2018), EFF was 9.5±0.5 GtC yr−1, ELUC 1.5±0.7 GtC yr−1, GATM 4.9±0.02 GtC yr−1 (2.3±0.01 ppm yr−1), SOCEAN 2.5±0.6 GtC yr−1, and SLAND 3.2±0.6 GtC yr−1, with a budget imbalance BIM of 0.4 GtC yr−1 indicating overestimated emissions and/or underestimated sinks. For the year 2018 alone, the growth in EFF was about 2.1 % and fossil emissions increased to 10.0±0.5 GtC yr−1, reaching 10 GtC yr−1 for the first time in history, ELUC was 1.5±0.7 GtC yr−1, for total anthropogenic CO2 emissions of 11.5±0.9 GtC yr−1 (42.5±3.3 GtCO2). Also for 2018, GATM was 5.1±0.2 GtC yr−1 (2.4±0.1 ppm yr−1), SOCEAN was 2.6±0.6 GtC yr−1, and SLAND was 3.5±0.7 GtC yr−1, with a BIM of 0.3 GtC. The global atmospheric CO2 concentration reached 407.38±0.1 ppm averaged over 2018. For 2019, preliminary data for the first 6–10 months indicate a reduced growth in EFF of +0.6 % (range of −0.2 % to 1.5 %) based on national emissions projections for China, the USA, the EU, and India and projections of gross domestic product corrected for recent changes in the carbon intensity of the economy for the rest of the world. Overall, the mean and trend in the five components of the global carbon budget are consistently estimated over the period 1959–2018, but discrepancies of up to 1 GtC yr−1 persist for the representation of semi-decadal variability in CO2 fluxes. A detailed comparison among individual estimates and the introduction of a broad range of observations shows (1) no consensus in the mean and trend in land use change emissions over the last decade, (2) a persistent low agreement between the different methods on the magnitude of the land CO2 flux in the northern extra-tropics, and (3) an apparent underestimation of the CO2 variability by ocean models outside the tropics. This living data update documents changes in the methods and data sets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this data set (Le Quéré et al., 2018a, b, 2016, 2015a, b, 2014, 2013). The data generated by this work are available at https://doi.org/10.18160/gcp-2019 (Friedlingstein et al., 2019).

The accuracy of chemical tracer simulations by atmospheric general circulation model (AGCM)-based chemistry-transport models (ACTMs) depends on the quality of AGCM transport properties, even when the meteorology is nudged towards the reanalysis fields. Here we show that significant improvements in tracer distribution are achieved when hybrid vertical coordinate is implemented in MIROC4.0 AGCM, compared to its predecessors AGCM5.7b based on sigma coordinate. Only explicitly resolved gravity waves are propagated into the stratosphere in MIROC4-ACTM. The MIROC4-ACTM produces "age-of-air" up to about 5 years in the tropical upper stratosphere (~1 hPa) and about 6 years in the polar middle stratosphere (~10 hPa), in agreement with observational estimates. Comparisons of MIROC4-ACTM simulation with observed sulphur hexafluoride (SF 6) in the troposphere also show remarkable improvements over the AGCM57b-ACTM simulation. MIROC4-ACTM is characterized by weaker convective mass flux and thus older age of air in the tropical troposphere, relative to AGCM57b-ACTM. The role of convective transport on tracer simulations is depicted using vertical cross-sections of 222 Rn (radon) distributions. Both the ACTM versions show similar results when compared with 222 Rn measurements at remote sites. All aspects of tracer transport in MIROC4-ACTM is promising for inverse modelling of greenhouse gases sources and sinks at reduced bias.

Methane (CH 4 ) is an important greenhouse gas and plays a significant role in tropospheric and stratospheric chemistry. Despite the relevance of methane (CH 4 ) in human-induced climate change and air pollution chemistry, there is no scientific consensus on the causes of changes in its growth rates and variability over the past three decades. We use a well-validated chemistry-transport model for simulating CH 4 concentration and estimation of regional CH 4 emissions by inverse modeling during 1988-2016. The control simulations are conducted using seasonally varying hydroxyl (OH) concentrations and assumed no interannual variability. Using inverse modeling of atmospheric observations, emission inventories, a wetland model, and a δ 13 C-CH 4 box model, we show that reductions in emissions from Europe and Russia since 1988, particularly from oil-gas exploitation and enteric fermentation, led to decreased CH 4 growth rates in the 1990s. This period was followed by a quasi-stationary state of CH 4 in the atmosphere during the early 2000s. CH 4 resumed growth from 2007, which we attribute to increases in emissions from coal mining mainly in China and the intensification of ruminant farming in tropical regions. A sensitivity simulation using interannually varying OH shows that regional emission estimates by inversion are unaffected for the mid-and high latitude areas. We show that meridional shift in CH 4 emissions toward the lower latitudes and the increase in CH 4 loss by hydroxyl (OH) over the tropics finely balance out, keeping the CH 4 gradients between the southern hemispheric tropical and polar sites relatively unchanged during 1988-2016. The latitudinal emissions shift is confirmed using the global distributions of the total column CH 4 observations via satellite remote sensing. During our analysis period, there is no evidence of emission enhancement due to climate warming, including the boreal regions. These findings highlight key sectors for effective emission reduction strategies toward climate change mitigation.Keywords atmospheric chemistry-transport model; inversion model; greenhouse gases; methane (CH 4

Methane (CH 4 ) has a large contribution to the global radiative budget and is responsible for about 0.5°C of present global warming over the period 1850 -1900(IPCC, 2021. Methane has a relatively short perturbation lifetime (12.4 years (Balcombe et al., 2018)) and high global warming potential (28-36 times that of CO 2 over a 100year period (IPCC, 2021)). As such, a decline in CH 4 emissions will rapidly reduce global CH 4 concentrations and mitigate the impact of climate change at decadal time scales (United Nations Environment Programme & Climate & Clean Air Coalition, 2021). However, any efforts to target CH 4 emissions reductions require a thorough understanding of the dominant CH 4 sources and sinks and their temporal and regional distribution and trends.Methane is produced in three ways-pyrogenically, thermogenically, or biogenically-from both anthropogenic and natural processes. Pyrogenic sources of CH 4 include biofuel combustion (e.g., wood burning for heating and cooking) and biomass burning (e.g., wildfires and peat fires). All pyrogenic sources produce CH 4 from the incomplete combustion of organic matter. Thermogenic CH 4 is produced from the breakdown of organic matter buried deep within the Earth's crust at high pressure and temperature. Although geological CH 4 is released naturally into the atmosphere through gas seeps, most is released through activities related to the exploration, mining, and transport of fossil fuels (Hmiel et al., 2020;Janssens-Maenhout et al., 2019;Petrenko et al., 2017). The majority of biogenic CH 4 is produced in anaerobic environments by the microbial mediated breakdown of organic matter. These environments include wetlands, inland waters, marine sediments, ruminants such as cattle, rice paddies, manure management and wastewater and landfill systems. Small quantities of CH4 are also produced from the aerobic bacterial metabolization of methylated compounds (e.g., Florez-Leiva et al., 2013) and even photochemically (Li et al., 2020). Counter-balancing these CH 4 sources are three chemically driven atmospheric sinks of CH 4 . The first two reactions with tropospheric OH radicals and tropospheric atomic chlorine account for ~88% (476 -677 Tg CH 4 yr −1 ) and ~2% (1-35 Tg CH 4 yr −1 ) of the total sink, respectively, with a third stratospheric sink (e.g., reaction with O('D), Cl and OH in the stratosphere) accounting for a further ~5% (12-37 Tg CH 4 yr −1 ) (Saunois et al., 2020). However, due to their highly reactive nature, the key reactants are inherently difficult to quantify, driving a significant level of uncertainty in the spatial and temporal distribution of atmospheric sink estimates (Zhao et al., 2019). Many fundamental aspects of the spatial distribution of OH are currently unresolved, for example, estimates of the interhemispheric gradient can vary from 0.85 to 1.4 (NH/SH) depending on the methodology

Abstract. About 70 % of the anthropogenic carbon dioxide (CO 2 ) is emitted from the megacities and urban areas of the world. In order to draw effective emission mitigation policies for combating future climate change as well as independently validating the emission inventories for constraining their large range of uncertainties, especially over major metropolitan areas of developing countries, there is an urgent need for greenhouse gas measurements over representative urban regions. India is a fast developing country, where fossil fuel emissions have increased dramatically in the last three decades and are predicted to continue to grow further by at least 6 % per year through to 2025. The CO 2 measurements over urban regions in India are lacking. To overcome this limitation, simultaneous measurements of CO 2 and carbon monoxide (CO) have been made at Ahmedabad, a major urban site in western India, using a state-of-the-art laser-based cavity ring down spectroscopy technique from November 2013 to May 2015. These measurements enable us to understand the diurnal and seasonal variations in atmospheric CO 2 with respect to its sources (both anthropogenic and biospheric) and biospheric sinks. The observed annual average concentrations of CO 2 and CO are 413.0 ± 13.7 and 0.50 ± 0.37 ppm respectively. Both CO 2 and CO show strong seasonality with lower concentrations (400.3 ± 6.8 and 0.19 ± 0.13 ppm) during the south-west monsoon and higher concentrations (419.6 ± 22.8 and 0.72 ± 0.68 ppm) during the autumn (SON) season. Strong diurnal variations are also observed for both the species. The common factors for the diurnal cycles of CO 2 and CO are vertical mixing and rush hour traffic, while the influence of biospheric fluxes is also seen in the CO 2 diurnal cycle. Using CO and CO 2 covariation, we differentiate the anthropogenic and biospheric components of CO 2 and found significant contributions of biospheric respiration and anthropogenic emissions in the late night (00:00-05:00 h, IST) and evening rush hours (18:00-22:00 h) respectively. We compute total yearly emissions of CO to be 69.2 ± 0.07 Gg for the study region using the observed CO : CO 2 correlation slope and bottom-up CO 2 emission inventory. This calculated emission of CO is 52 % larger than the estimated emission of CO by the emissions database for global atmospheric research (EDGAR) inventory. The observations of CO 2 have been compared with an atmospheric chemistry-transport model (ACTM), which incorporates various components of CO 2 fluxes. ACTM is able to capture the basic variabilities, but both diurnal and seasonal amplitudes are largely underestimated compared to the observations. We attribute this underestimation by the model to uncertainties in terrestrial biosphere fluxes and coarse model resolution. The fossil fuel signal from the model shows fairly good correlation with observed CO 2 variations, which supports the overall dominance of fossil fuel emissions over the biospheric fluxes in this urban region.

Up in the air Understanding ocean-atmospheric carbon dioxide (CO 2 ) fluxes in the Southern Ocean is necessary for quantifying the global CO 2 budget, but measurements in the harsh conditions there make collecting good data difficult, so a quantitative picture still is out of reach. Long et al . present measurements of atmospheric CO 2 concentrations made by aircraft and show that the annual net flux of carbon into the ocean south of 45°S is large, with stronger summertime uptake and less wintertime outgassing than other recent observations have indicated. —HJS