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We use 2021 TROPOMI and GOSAT satellite observations of atmospheric methane in an analytical inversion to quantify national methane emissions from South America at up to 25 km × 25 km resolution. From the inversion, we derive optimal posterior estimates of methane emissions, adjusting a combination of national anthropogenic emission inventories reported by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC), the UNFCCC-based Global Fuel Exploitation Inventory (GFEIv2), and the Emissions Database for Global Atmospheric Research (EDGARv7) as prior estimates. We also evaluate two alternative wetland emission inventories (WetCHARTs and LPJ-wsl) as prior estimates. Our best posterior estimates for wetland emissions are consistent with previous inventories for the Amazon but lower for the Pantanal and higher for the Paraná. Our best posterior estimate of South American anthropogenic emissions is 48 (41–56) Tg a−1, where numbers in parentheses are the range from our inversion ensemble. This is 55 % higher than our prior estimate and is dominated by livestock (65 % of anthropogenic total). We find that TROPOMI and GOSAT observations can effectively optimize and separate national emissions by sector for 10 of the 13 countries and territories in the region, 7 of which account for 93 % of continental anthropogenic emissions: Brazil (19 (16–23) Tg a−1), Argentina (9.2 (7.9–11) Tg a−1), Venezuela (7.0 (5.5–9.9) Tg a−1), Colombia (5.0 (4.4–6.7) Tg a−1), Peru (2.4 (1.6–3.9) Tg a−1), Bolivia (0.96 (0.66–1.2) Tg a−1), and Paraguay (0.93 (0.88–1.0) Tg a−1). Our estimates align with the prior estimates for Brazil, Bolivia, and Paraguay but are significantly higher for other countries. Emissions in all countries are dominated by livestock (mainly enteric fermentation) except for oil–gas in Venezuela and landfills in Peru. Methane intensities from the oil–gas industry are high in Venezuela (33 %), Colombia (6.5 %), and Argentina (5.9 %). The livestock sector shows the largest difference between our top-down estimate and the UNFCCC prior estimates, and even countries using complex bottom-up methods report UNFCCC emissions significantly lower than our posterior estimate. These discrepancies could stem from underestimations in IPCC-recommended bottom-up calculations or uncertainties in the inversion from aggregation error and the prior spatial distribution of emissions.

Recent analyses show the importance of methane shortwave absorption, which many climate models lack. In particular, Allen et al. (2023) used idealized climate model simulations to show that methane shortwave absorption mutes up to 30 % of the surface warming and 60 % of the precipitation increase associated with its longwave radiative effects. Here, we explicitly quantify the radiative and climate impacts due to shortwave absorption of the present-day methane perturbation. Our results corroborate the hypothesis that present-day methane shortwave absorption mutes the warming effects of longwave absorption. For example, the global mean cooling in response to the present-day methane shortwave absorption is -0.10±0.07 K, which offsets 28 % (7 %–55 %) of the surface warming associated with present-day methane longwave radiative effects. The precipitation increase associated with the longwave radiative effects of the present-day methane perturbation (0.012±0.006 mm d−1) is also muted by shortwave absorption but not significantly so (-0.008±0.009 mm d−1). The unique responses to methane shortwave absorption are related to its negative top-of-the-atmosphere effective radiative forcing but positive atmospheric heating and in part to methane's distinctive vertical atmospheric solar heating profile. We also find that the present-day methane shortwave radiative effects, relative to its longwave radiative effects, are about 5 times larger than those under idealized carbon dioxide perturbations. Additional analyses show consistent but non-significant differences between the longwave versus shortwave radiative effects for both methane and carbon dioxide, including a stronger (negative) climate feedback when shortwave radiative effects are included (particularly for methane). We conclude by reiterating that methane remains a potent greenhouse gas.

We quantify 2019 annual mean methane emissions in the contiguous US (CONUS) at 0.25° × 0.3125° resolution by inverse analysis of atmospheric methane columns measured by the Tropospheric Monitoring Instrument (TROPOMI). A gridded version of the US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) serves as the basis for the prior estimate for the inversion. We optimize emissions and quantify observing system information content for an eight-member inversion ensemble through analytical minimization of a Bayesian cost function. We achieve high resolution with a reduced-rank characterization of the observing system that optimally preserves information content. Our optimal (posterior) estimate of anthropogenic emissions in CONUS is 30.9 (30.0–31.8) Tg a−1, where the values in parentheses give the spread of the ensemble. This is a 13 % increase from the 2023 GHGI estimate for CONUS in 2019. We find emissions for livestock of 10.4 (10.0–10.7) Tg a−1, for oil and gas of 10.4 (10.1–10.7) Tg a−1, for coal of 1.5 (1.2–1.9) Tg a−1, for landfills of 6.9 (6.4–7.5) Tg a−1, for wastewater of 0.6 (0.5–0.7), and for other anthropogenic sources of 1.1 (1.0–1.2) Tg a−1. The largest increase relative to the GHGI occurs for landfills (51 %), with smaller increases for oil and gas (12 %) and livestock (11 %). These three sectors are responsible for 89 % of posterior anthropogenic emissions in CONUS. The largest decrease (28 %) is for coal. We exploit the high resolution of our inversion to quantify emissions from 70 individual landfills, where we find emissions are on median 77 % larger than the values reported to the EPA's Greenhouse Gas Reporting Program (GHGRP), a key data source for the GHGI. We attribute this underestimate to overestimated recovery efficiencies at landfill gas facilities and to under-accounting of site-specific operational changes and leaks. We also quantify emissions for the 48 individual states in CONUS, which we compare to the GHGI's new state-level inventories and to independent state-produced inventories. Our posterior emissions are on average 27 % larger than the GHGI in the largest 10 methane-producing states, with the biggest upward adjustments in states with large oil and gas emissions, including Texas, New Mexico, Louisiana, and Oklahoma. We also calculate emissions for 95 geographically diverse urban areas in CONUS. Emissions for these urban areas total 6.0 (5.4–6.7) Tg a−1 and are on average 39 (27–52) % larger than a gridded version of the 2023 GHGI, which we attribute to underestimated landfill and gas distribution emissions.

We present a user-friendly, cloud-based facility for quantifying methane emissions with 0.25∘ × 0.3125∘ (≈ 25 km × 25 km) resolution by inverse analysis of satellite observations from the TROPOspheric Monitoring Instrument (TROPOMI). The facility is built on an Integrated Methane Inversion optimal estimation workflow (IMI 1.0) and supported for use on the Amazon Web Services (AWS) cloud. It exploits the GEOS-Chem chemical transport model and TROPOMI data already resident on AWS, thus avoiding cumbersome big-data download. Users select a region and period of interest, and the IMI returns an analytical solution for the Bayesian optimal estimate of period-average emissions on the 0.25∘ × 0.3125∘ grid including error statistics, information content, and visualization code for inspection of results. The inversion uses an advanced research-grade algorithm fully documented in the literature. An out-of-the-box inversion with rectilinear grid and default prior emission estimates can be conducted with no significant learning curve. Users can also configure their inversions to infer emissions for irregular regions of interest, swap in their own prior emission inventories, and modify inversion parameters. Inversion ensembles can be generated at minimal additional cost once the Jacobian matrix for the analytical inversion has been constructed. A preview feature allows users to determine the TROPOMI information content for their region and time period of interest before actually performing the inversion. The IMI is heavily documented and is intended to be accessible by researchers and stakeholders with no expertise in inverse modelling or high-performance computing. We demonstrate the IMI's capabilities by applying it to estimate methane emissions from the US oil-producing Permian Basin in May 2018.

By regulating the global transport of heat, freshwater, and carbon, the Atlantic meridional overturning circulation (AMOC) serves as an important component of the climate system. During the late 20th and early 21st centuries, indirect observations and models suggest a weakening of the AMOC. Direct AMOC observations also suggest a weakening during the early 21st century but with substantial interannual variability. Long-term weakening of the AMOC has been associated with increasing greenhouse gases (GHGs), but some modeling studies suggest the build up of anthropogenic aerosols (AAs) may have offset part of the GHG-induced weakening. Here, we quantify 1900–2020 AMOC variations and assess the driving mechanisms in state-of-the-art climate models from the Coupled Model Intercomparison Project phase 6 (CMIP6). The CMIP6 forcing (GHGs, anthropogenic and volcanic aerosols, solar variability, and land use and land change) multi-model mean shows negligible AMOC changes up to ∼ 1950, followed by robust AMOC strengthening during the second half of the 20th century (∼ 1950–1990) and weakening afterwards (1990–2020). These multi-decadal AMOC variations are related to changes in North Atlantic atmospheric circulation, including an altered sea level pressure gradient, storm track activity, surface winds, and heat fluxes, which drive changes in the subpolar North Atlantic surface density flux. To further investigate these AMOC relationships, we perform a regression analysis and decompose these North Atlantic climate responses into an anthropogenic aerosol-forced component and a subsequent AMOC-related feedback. Similar to previous studies, CMIP6 GHG simulations yield robust AMOC weakening, particularly during the second half of the 20th century. Changes in natural forcings, including solar variability and volcanic aerosols, yield negligible AMOC changes. In contrast, CMIP6 AA simulations yield robust AMOC strengthening (weakening) in response to increasing (decreasing) anthropogenic aerosols. Moreover, the CMIP6 all-forcing AMOC variations and atmospheric circulation responses also occur in the CMIP6 AA simulations, which suggests these are largely driven by changes in anthropogenic aerosol emissions. More specifically, our results suggest that AMOC multi-decadal variability is initiated by North Atlantic aerosol optical thickness perturbations to net surface shortwave radiation and sea surface temperature (and hence sea surface density), which in turn affect sea level pressure gradient and surface wind and – via latent and sensible heat fluxes – sea surface density flux through its thermal component. AMOC-related feedbacks act to reinforce this aerosol-forced AMOC response, largely due to changes in sea surface salinity (and hence sea surface density), with temperature-related (and cloud-related) feedbacks acting to mute the initial response. Although aspects of the CMIP6 all-forcing multi-model mean response resembles observations, notable differences exist. This includes CMIP6 AMOC strengthening from ∼ 1950 to 1990, when the indirect estimates suggest AMOC weakening. The CMIP6 multi-model mean also underestimates the observed increase in North Atlantic ocean heat content, and although the CMIP6 North Atlantic atmospheric circulation responses – particularly the overall patterns – are similar to observations, the simulated responses are weaker than those observed, implying they are only partially externally forced. The possible causes of these differences include internal climate variability, observational uncertainties, and model shortcomings, including excessive aerosol forcing. A handful of CMIP6 realizations yield AMOC evolution since 1900 similar to the indirect observations, implying the inferred AMOC weakening from 1950 to 1990 (and even from 1930 to 1990) may have a significant contribution from internal (i.e., unforced) climate variability. Nonetheless, CMIP6 models yield robust, externally forced AMOC changes, the bulk of which are due to anthropogenic aerosols.

We examine the potential for global detection of methane plumes from individual point sources with the new generation of spaceborne imaging spectrometers (EnMAP, PRISMA, EMIT, SBG, CHIME) scheduled for launch in 2019–2025. These instruments are designed to map the Earth's surface at high spatial resolution (30 m×30 m) and have a spectral resolution of 7–10 nm in the 2200–2400 nm band that should also allow useful detection of atmospheric methane. We simulate scenes viewed by EnMAP (10 nm spectral resolution, 180 signal-to-noise ratio) using the EnMAP end-to-end simulation tool with superimposed methane plumes generated by large-eddy simulations. We retrieve atmospheric methane and surface reflectivity for these scenes using the IMAP-DOAS optimal estimation algorithm. We find an EnMAP precision of 3 %–7 % for atmospheric methane depending on surface type. This allows effective single-pass detection of methane point sources as small as 100 kg h−1 depending on surface brightness, surface homogeneity, and wind speed. Successful retrievals over very heterogeneous surfaces such as an urban mosaic require finer spectral resolution. We tested the EnMAP capability with actual plume observations over oil/gas fields in California from the Airborne Visible/Infrared Imaging Spectrometer – Next Generation (AVIRIS-NG) sensor (3 m×3 m pixel resolution, 5 nm spectral resolution, SNR 200–400), by spectrally and spatially downsampling the AVIRIS-NG data to match EnMAP instrument specifications. Results confirm that EnMAP can successfully detect point sources of ∼100 kg h−1 over bright surfaces. Source rates inferred with a generic integrated mass enhancement (IME) algorithm were lower for EnMAP than for AVIRIS-NG. Better agreement may be achieved with a more customized IME algorithm. Our results suggest that imaging spectrometers in space could play an important role in the future for quantifying methane emissions from point sources worldwide.

Methane emissions from oil/gas fields originate from a large number of relatively small and densely clustered point sources. A small fraction of high-mode emitters can make a large contribution to the total methane emission. Here we conduct observation system simulation experiments (OSSEs) to examine the potential of recently launched or planned satellites to detect and locate these high-mode emitters through measurements of atmospheric methane columns. We simulate atmospheric methane over a generic oil/gas field (20–500 production sites of different size categories in a 50×50 km2 domain) for a 1-week period using the WRF-STILT meteorological model with 1.3×1.3 km2 horizontal resolution. The simulations consider many random realizations for the occurrence and distribution of high-mode emitters in the field by sampling bimodal probability density functions (PDFs) of emissions from individual sites. The atmospheric methane fields for each realization are observed virtually with different satellite and surface observing configurations. Column methane enhancements observed from satellites are small relative to instrument precision, even for high-mode emitters, so an inverse analysis is necessary. We compare L1 and L2 regularizations and show that L1 regularization effectively provides sparse solutions for a bimodally distributed variable and enables the retrieval of high-mode emitters. We find that the recently launched TROPOMI instrument (low Earth orbit, 7×7 km2 nadir pixels, daily return time) and the planned GeoCARB instrument (geostationary orbit, 2.7×3.0 km2 pixels, 2 times or 4 times per day return times) are successful (> 80 % detection rate, 50×50 km2 domain as long as skies are clear. They are unsuccessful for denser fields. GeoCARB does not benefit significantly from more frequent observations (4 times per day vs. 2 times per day) because of a temporal error correlation in the inversion, unless under partly cloudy conditions where more frequent observation increases the probability of clear sky. It becomes marginally successful when allowing a 5 km error tolerance for localization. A next-generation geostationary satellite instrument with 1.3×1.3 km2 pixels, hourly return time, and 1 ppb precision can successfully detect and locate the high-mode emitters for a dense field with up to 500 sites in the 50×50 km2 domain. The capabilities of TROPOMI and GeoCARB can be usefully augmented with a surface air observation network of 5–20 sites, and in turn the satellite instruments increase the detection capability that can be achieved from the surface sites alone.

Anthropogenic methane emissions originate from a large number of fine-scale and often transient point sources. Satellite observations of atmospheric methane columns are an attractive approach for monitoring these emissions but have limitations from instrument precision, pixel resolution, and measurement frequency. Dense observations will soon be available in both low-Earth and geostationary orbits, but the extent to which they can provide fine-scale information on methane sources has yet to be explored. Here we present an observation system simulation experiment (OSSE) to assess the capabilities of different satellite observing system configurations. We conduct a 1-week WRF-STILT simulation to generate methane column footprints at 1.3 × 1.3 km2 spatial resolution and hourly temporal resolution over a 290 × 235 km2 domain in the Barnett Shale, a major oil and gas field in Texas with a large number of point sources. We sub-sample these footprints to match the observing characteristics of the recently launched TROPOMI instrument (7 × 7 km2 pixels, 11 ppb precision, daily frequency), the planned GeoCARB instrument (2.7 × 3.0 km2 pixels, 4 ppb precision, nominal twice-daily frequency), and other proposed observing configurations. The information content of the various observing systems is evaluated using the Fisher information matrix and its eigenvalues. We find that a week of TROPOMI observations should provide information on temporally invariant emissions at ∼ 30 km spatial resolution. GeoCARB should provide information available on temporally invariant emissions ∼ 2–7 km spatial resolution depending on sampling frequency (hourly to daily). Improvements to the instrument precision yield greater increases in information content than improved sampling frequency. A precision better than 6 ppb is critical for GeoCARB to achieve fine resolution of emissions. Transient emissions would be missed with either TROPOMI or GeoCARB. An aspirational high-resolution geostationary instrument with 1.3 × 1.3 km2 pixel resolution, hourly return time, and 1 ppb precision would effectively constrain the temporally invariant emissions in the Barnett Shale at the kilometer scale and provide some information on hourly variability of sources.

A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons. Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly −10 to 20%, with over- and underestimates of radiative cooling at lower and higher solar zenith angle, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15% as solar zenith angle decreases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing.

Simulated multi-model "diversity" in aerosol direct radiative forcing estimates is often perceived as a measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated "host-model uncertainties" are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in twelve participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is −4.47 Wm−2 and the inter-model standard deviation is 0.55 Wm−2, corresponding to a relative standard deviation of 12%. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.04 Wm−2, and the standard deviation increases to 1.01 W−2, corresponding to a significant relative standard deviation of 97%. However, the top-of-atmosphere forcing variability owing to absorption (subtracting the scattering case from the case with scattering and absorption) is low, with absolute (relative) standard deviations of 0.45 Wm−2 (8%) clear-sky and 0.62 Wm−2 (11%) all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the AeroCom Direct Effect experiment demonstrates that host model uncertainties could explain about 36% of the overall sulfate forcing diversity of 0.11 Wm−2 in the AeroCom Direct Radiative Effect experiment. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus cloud decks or areas with poorly constrained surface albedos, such as sea ice. Our results demonstrate that host model uncertainties are an important component of aerosol forcing uncertainty that require further attention.

Tropospheric aerosols emitted from biomass burning reduce solar radiation at the surface and locally heat the atmosphere. Equilibrium simulations using an atmospheric general circulation model (GFDL AGCM) indicate that strong atmospheric absorption from these particles can cool the surface and increase upward motion and low-level convergence over southern Africa during the dry season. These changes increase sea level pressure over land in the biomass burning region and spin-up the hydrologic cycle by increasing clouds, atmospheric water vapor, and, to a lesser extent, precipitation. Cloud increases serve to reinforce the surface radiative cooling tendency of the aerosol. Conversely, if the climate over southern Africa were hypothetically forced by high loadings of scattering aerosol, then the change in the low-level circulation and increased subsidence would serve to decrease clouds, precipitation, and atmospheric water vapor. Surface cooling associated with scattering-only aerosols is mitigated by warming from cloud decreases. The direct and semi-direct climate impacts of biomass burning aerosol over southern Africa are sensitive to the total amount of aerosol absorption and how clouds change in response to the aerosol-induced heating of the atmosphere.