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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Emissions and atmospheric concentrations of CH4 continue to increase, maintaining CH4 as 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 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 reducing uncertainties in the factors explaining the well-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 multi-disciplinary 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 gas 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 datasets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this edition benefits from important progress in estimating inland freshwater emissions, with better accounting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double accounting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double accounting that still exists (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 % are attributed to direct anthropogenic sources in the fossil, agriculture and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr-1or 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). 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 uncertainty in bottom-up and top-down budgets overlap. The latitudinal distribution from atmospheric inversion-based emissions indicates a predominance of tropical and southern hemisphere emissions (~65 % of the global budget, <30° N) compared to mid (30° N–60° N, ~30 % of emissions) and high-northern latitudes (60° N–90° N, ~4 % of global emissions). This latitudinal distribution is similar in the bottom-up budget though the bottom-up budget estimates slightly larger contributions for the mid and high-northern latitudes, and slightly smaller contributions from the tropics and southern hemisphere than the inversions. 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. 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). [ABSTRACT FROM AUTHOR]

Ignoring the diurnal cycle in surface-to-atmosphere CO2 fluxes leads to a systematic bias in CO2 mole fraction simulations sampled at daytime, because the daily mean flux systematically misses the CO2 uptake during the daytime hours. In an atmospheric inversion using daytime-selected CO2 measurements at most continental sites and not resolving diurnal cycles in the flux, this leads to systematic biases in the estimates of the annual sources and sinks of atmospheric CO2. This study focuses on quantifying the impact of this diurnal cycle effect on the annual carbon fluxes estimated with the CarboScope (CS) atmospheric inversion at regional, continental, and global scales for the period of time 2010–2020. Biogenic fluxes of hourly Net Ecosystem Exchange (NEE) obtained from the data-driven FLUXCOM estimates are used in the inversion together with global and regional atmospheric transport models. Differences between CO2 mixing ratios simulated with daily averaged and hourly NEE range between around -2.5 and 7 ppm averaged annually throughout a site network across the world. As a consequence, these differences lead to systematic biases in CO2 flux estimates when ignoring the diurnal variations of the CO2 flux in the atmospheric inversions. Although the impact on the global average of estimated annual flux is negligible (around 2 % of the overall land flux of -1.79 Pg C yr-1), we find significant biases in the annual flux budgets at continental and regional scales. For Europe, the annual mean difference in the fluxes arising from the diurnal cycle of CO2 represents around 48 % of the annual posterior fluxes (0.31 Pg C yr-1) estimated with CarboScope-Regional (CSR). Furthermore, the differences in NEE estimates calculated with CS increase the magnitude of the flux budgets for some regions such as northern American temperate and northern Africa by a factor of about 1.5. To the extent that FLUXOM diurnal cycles are realistic at all latitudes and for the station set used in our inversions here, we conclude that ignoring the diurnal variations in the land CO2 flux leads to overestimation of both CO2 sources in the tropical lands and CO2 sinks in the temperate zones. [ABSTRACT FROM AUTHOR]

A growing number of general circulation models are adapting interactive sulfur and aerosol schemes to improve the representation of relevant physical and chemical processes and associated feedbacks. They are motivated by investigations of climate response to major volcanic eruptions and potential solar geoengineering scenarios. However, uncertainties in these schemes are not well constrained. Stratospheric sulfate is modulated by emissions of sulfur-containing species of anthropogenic and natural origin, including volcanic activity. While the effects of volcanic eruptions have been studied in the framework of global model intercomparisons, the background conditions of the sulfur cycle have not been addressed in such a way. Here, we fill this gap by analyzing the distribution of the main sulfur species in nine global atmospheric aerosol models for a volcanically quiescent period. We use observational data to evaluate model results. Overall, models agree that the three dominant sulfur species in terms of burdens (sulfate aerosol, OCS, and SO 2) make up about 98 % stratospheric sulfur and 95 % tropospheric sulfur. However, models vary considerably in the partitioning between these species. Models agree that anthropogenic emission of SO 2 strongly affects the sulfate aerosol burden in the northern hemispheric troposphere, while its importance is very uncertain in other regions, where emissions are much lower. Sulfate aerosol is the main deposited species in all models, but the values deviate by a factor of 2. Additionally, the partitioning between wet and dry deposition fluxes is highly model dependent. Inter-model variability in the sulfur species is low in the tropics and increases towards the poles. Differences are largest in the dynamically active northern hemispheric extratropical region and could be attributed to the representation of the stratospheric circulation. The differences in the atmospheric sulfur budget among the models arise from the representation of both chemical and dynamical processes, whose interplay complicates the bias attribution. Several problematic points identified for individual models are related to the specifics of the chemistry schemes, model resolution, and representation of cross-tropopause transport in the extratropics. Further model intercomparison research is needed with a focus on the clarification of the reasons for biases, given the importance of this topic for the stratospheric aerosol injection studies. [ABSTRACT FROM AUTHOR]

Forest ecosystems play an important role in the global carbon (C) budget by sequestering a large fraction of anthropogenic carbon dioxide (CO 2) emissions and by acting as important methane (CH 4) sinks. The forest-floor greenhouse gas (GHG; CO 2 , CH 4 , and nitrous oxide (N 2 O)) flux, i.e., from soil and understory vegetation, is one of the major components to consider when determining the C or GHG budget of forests. Although winter fluxes are essential to determine the annual C budget, only very few studies have examined long-term, year-round forest-floor GHG fluxes. Thus, we aimed to (i) quantify seasonal and annual variations of forest-floor GHG fluxes; (ii) evaluate their drivers, including the effects of snow cover, timing, and amount of snowmelt; and (iii) calculate annual budgets of forest-floor GHG fluxes for a subalpine spruce forest in Switzerland. We measured GHG fluxes year-round during 4 years with four automatic large chambers at the ICOS Class 1 Ecosystem station Davos (CH-Dav). We applied random forest models to investigate environmental drivers and to gap-fill the flux time series. The forest floor emitted 2336 g CO 2 m -2 yr -1 (average over 4 years). Annual and seasonal forest-floor respiration responded most strongly to soil temperature and snow depth. No response of forest-floor respiration to leaf area index or photosynthetic photon flux density was observed, suggesting a strong direct control of soil environmental factors and a weak, or even lacking, indirect control of canopy biology. Furthermore, the forest floor was a consistent CH 4 sink (- 0.71 g CH 4 m -2 yr -1), with annual fluxes driven mainly by snow depth. Winter CO 2 fluxes were less important for the CO 2 budget (6.0 %–7.3 %), while winter CH 4 fluxes contributed substantially to the annual CH 4 budget (14.4 %–18.4 %). N 2 O fluxes were very low (0.007 g N 2 O m -2 yr -1), negligible for the forest-floor GHG budget at our site. In 2022, the warmest year on record with below-average precipitation at the Davos site, we observed a substantial increase in forest-floor respiration compared with other years. The mean forest-floor GHG budget indicated emissions of 2319 ± 200 g CO2eq. m -2 yr -1 (mean ± standard deviation (SD) over all years), with respiration fluxes dominating and CH 4 offsetting a very small proportion (0.8 %) of the CO 2 emissions. Due to the relevance of snow cover, we recommend year-round measurements of GHG fluxes with high temporal resolution. In a future with increasing temperatures and less snow cover due to climate change, we expect increased forest-floor respiration at this subalpine site modulating the carbon sink of the forest ecosystem. [ABSTRACT FROM AUTHOR]

We explore the impacts of the diurnal cycle, free-tropospheric (FT) humidity values, and interactive surface fluxes on the cloud system evolution of non-precipitating marine stratocumuli based on a large ensemble of large-eddy simulations. Cases are separated into three categories based on their degree of decoupling and cloud liquid water path (LWPc). A new budget analysis method is proposed to analyze the evolution of LWPc under both coupled and decoupled conditions. More coupled clouds start with relatively low LWPc and cloud fraction (f c) but experience the least decrease in LWPc and f c during the daytime. More decoupled clouds undergo greater daytime reduction in LWPc and f c, especially those with higher LWPc at sunrise because they suffer from faster weakening of a net radiative cooling. During the nighttime, a positive correlation between FT humidity and LWPc emerges, consistent with higher FT humidity reducing both radiative cooling and the humidity jump, both of which reduce entrainment and increase LWPc. The time rate of change in the LWPc is more likely to be negative for higher LWPc and greater inversion base height (z i), conditions under which entrainment dominates as turbulence develops. In the morning, the rate of the LWPc reduction depends on the LWPc at sunrise, z i, and the degree of decoupling, with distinct contributions from subsidence and radiation. Under well-mixed conditions, it takes about 10 h for the surface fluxes to offset 15 % of the changes in entrainment warming and drying, assuming no changes in transfer coefficients or surface wind speed. [ABSTRACT FROM AUTHOR]

The carbon monoxide (CO) in the marine boundary layer and in the surface waters and water column were measured along the western limb of the North Pacific from the Korean Peninsula to Alaska, USA, in summer 2012. The observation allows us to estimate the CO budgets in the surface mixed layer of the three distinct regimes: the East Sea (Sea of Japan) (ES), the Northwest Pacific (NP), and the Bering Sea (BS). CO photochemical production rates were 56(± 15) µ mol m -2 d -1 , 27(± 3) µ mol m -2 d -1 , and 26(± 2) µ mol m -2 d -1 , while microbial consumption rates were 30(± 8) µ mol m -2 d -1 , 24(± 5) µ mol m -2 d -1 , and 63(± 19) µ mol m -2 d -1 in the ES, NP, and BS, respectively, both of which are the dominant components of the CO budget in the ocean. The other two known components, air–sea gas exchange and downward mixing, remained negligible (less than 3 µ mol m -2 d -1) in all regimes. While the CO budget in the surface mixed layer of the NP was in balance, the CO production surpassed the consumption in the ES, and vice versa in the BS. The significant imbalances in the CO budget in the ES (25 ± 17 µ mol m -2 d -1) and the BS (40 ± 19 µ mol m -2 d -1) are suggested to be compensated by external physical transport such as lateral advection, subduction, or ventilation. Notably, the increase in the CO column burden correlated with the imbalance in the CO budget, highlighting the significant role of the physical transport in the marine CO cycles. Our observation, for the first time, underscores the potential importance of physical transport in driving CO dynamics in the marine environment. [ABSTRACT FROM AUTHOR]

In September 2020, a global aerosol forecasting model was implemented as an ensemble member of the National Oceanic and Atmospheric Administration (NOAA) National Centers for Environmental Prediction (NCEP) Global Ensemble Forecasting System (GEFS) v12.0.1 (hereafter referred to as "GEFS-Aerosols"). In this study, GEFS-Aerosols simulation results from 1 September 2019 to 30 September 2020 were evaluated using an aerosol budget analysis. These results were compared with results from other global models as well as reanalysis data. From this analysis, the global average lifetimes of black carbon (BC), organic carbon (OC), dust, sea salt, and sulfate are 4.06, 4.29, 4.59, 0.34, and 3.3 d, respectively, with the annual average loads of 0.14, 1.29, 4.52, 6.80, and 0.51 Tg. Compared with the National Aeronautics and Space Administration (NASA) Goddard Earth Observing System–Goddard Chemistry Aerosol and Radiation Transport (GEOS4-GOCART) model, the aerosols in GEFS-Aerosols have a relatively short lifetime because of the faster removal processes in GEFS-Aerosols. Meanwhile, in GEFS-Aerosols, aerosol emissions are the determining factor for the mass and composition of aerosols in the atmosphere. The size (bin) distribution of aerosol emissions is as important as its total emissions, especially in simulations of dust and sea salt. Moreover, most importantly, the strong monthly and interannual variations in natural sources of aerosols in GEFS-Aerosols suggest that improving the accuracy of the prognostic concentrations of aerosols is important for applying aerosol feedback to weather and climate predictions. [ABSTRACT FROM AUTHOR]