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Global high-resolution observations of atmospheric composition from satellites can greatly improve our understanding of surface emissions through inverse analyses. Variational inverse methods can optimize surface emissions at any resolution but do not readily quantify the error and information content of the posterior solution. The information content of satellite data may be much lower than its coverage would suggest because of failed retrievals, instrument noise, and error correlations that propagate through the inversion. Analytical solution of the inverse problem provides closed-form characterization of posterior error statistics and information content but requires the construction of the Jacobian matrix that relates emissions to atmospheric concentrations. Building the Jacobian matrix is computationally expensive at high resolution because it involves perturbing each emission element, typically individual grid cells, in the atmospheric transport model used as the forward model for the inversion. We propose and analyze two methods, reduced dimension and reduced rank, to construct the Jacobian matrix at greatly decreased computational cost while retaining information content. Both methods are two-step iterative procedures that begin from an initial native-resolution estimate of the Jacobian matrix constructed at no computational cost by assuming that atmospheric concentrations are most sensitive to local emissions. The reduced-dimension method uses this estimate to construct a Jacobian matrix on a multiscale grid that maintains a high resolution in areas with high information content and aggregates grid cells elsewhere. The reduced-rank method constructs the Jacobian matrix at native resolution by perturbing the leading patterns of information content given by the initial estimate. We demonstrate both methods in an analytical Bayesian inversion of Greenhouse Gases Observing Satellite (GOSAT) methane data with augmented information content over North America in July 2009. We show that both methods reproduce the results of the native-resolution inversion while achieving a factor of 4 improvement in computational performance. The reduced-dimension method produces an exact solution at a lower spatial resolution, while the reduced-rank method solves the inversion at native resolution in areas of high information content and defaults to the prior estimate elsewhere.

We present a versatile, powerful, and user-friendly chemical data assimilation toolkit for simultaneously optimizing emissions and concentrations of chemical species based on atmospheric observations from satellites or suborbital platforms. The CHemistry and Emissions REanalysis Interface with Observations (CHEEREIO) exploits the GEOS-Chem chemical transport model and a localized ensemble transform Kalman filter algorithm (LETKF) to determine the Bayesian optimal (posterior) emissions and/or concentrations of a set of species based on observations and prior information using an easy-to-modify configuration file with minimal changes to the GEOS-Chem or LETKF code base. The LETKF algorithm readily allows for nonlinear chemistry and produces flow-dependent posterior error covariances from the ensemble simulation spread. The object-oriented Python-based design of CHEEREIO allows users to easily add new observation operators such as for satellites. CHEEREIO takes advantage of the Harmonized Emissions Component (HEMCO) modular structure of input data management in GEOS-Chem to update emissions from the assimilation process independently from the GEOS-Chem code. It can seamlessly support GEOS-Chem version updates and is adaptable to other chemical transport models with similar modular input data structure. A post-processing suite combines ensemble output into consolidated NetCDF files and supports a wide variety of diagnostic data and visualizations. We demonstrate CHEEREIO's capabilities with an out-of-the-box application, assimilating global methane emissions and concentrations at weekly temporal resolution and 2 ∘ × 2.5 ∘ spatial resolution for 2019 using TROPOspheric Monitoring Instrument (TROPOMI) satellite observations. CHEEREIO achieves a 50-fold improvement in computational performance compared to the equivalent analytical inversion of TROPOMI observations. [ABSTRACT FROM AUTHOR]

Satellite observations of dry-column methane mixing ratios (XCH 4) from shortwave infrared (SWIR) solar backscatter radiation provide a powerful resource to quantify methane emissions in service of climate action. The TROPOspheric Monitoring Instrument (TROPOMI), launched in October 2017, provides global daily coverage at a 5.5 × 7 km 2 (nadir) pixel resolution, but its methane retrievals can suffer from biases associated with SWIR surface albedo, scattering from aerosols and cirrus clouds, and across-track variability (striping). The Greenhouse gases Observing SATellite (GOSAT) instrument, launched in 2009, has better spectral characteristics and its methane retrieval is much less subject to biases, but its data density is 250 times sparser than TROPOMI. Here, we present a blended TROPOMI + GOSAT methane product obtained by training a machine learning (ML) model to predict the difference between TROPOMI and GOSAT co-located measurements, using only predictor variables included in the TROPOMI retrieval, and then applying the correction to the complete TROPOMI record from April 2018 to present. We find that the largest corrections are associated with coarse aerosol particles, high SWIR surface albedo, and across-track pixel index. Our blended product corrects a systematic difference between TROPOMI and GOSAT over water, and it features corrections exceeding 10 ppb over arid land, persistently cloudy regions, and high northern latitudes. It reduces the TROPOMI spatially variable bias over land (referenced to GOSAT data) from 14.3 to 10.4 ppb at a 0.25 ∘ × 0.3125 ∘ resolution. Validation with Total Carbon Column Observing Network (TCCON) ground-based column measurements shows reductions in variable bias compared with the original TROPOMI data from 4.7 to 4.4 ppb and in single-retrieval precision from 14.5 to 11.9 ppb. TCCON data are all in locations with a SWIR surface albedo below 0.4 (where TROPOMI biases tend to be relatively low), but they confirm the dependence of TROPOMI biases on SWIR surface albedo and coarse aerosol particles, as well as the reduction of these biases in the blended product. Fine-scale inspection of the Arabian Peninsula shows that a number of hotspots in the original TROPOMI data are removed as artifacts in the blended product. The blended product also corrects striping and aerosol/cloud biases in single-orbit TROPOMI data, enabling better detection and quantification of ultra-emitters. Residual coastal biases can be removed by applying additional filters. The ML method presented here can be applied more generally to validate and correct data from any new satellite instrument by reference to a more established instrument. [ABSTRACT FROM AUTHOR]

We quantify weekly methane emissions at 0.25 ∘ × 0.3125 ∘ (≈25 × 25 km 2) resolution from the Permian Basin, the largest oil production basin in the US, by inverse analysis of satellite observations from the TROPOspheric Monitoring Instrument (TROPOMI) from May 2018 to October 2020. The mean oil and gas emission from the region (± standard deviation of weekly estimates) was 3.7 ± 0.9 Tg a -1 , higher than previous TROPOMI inversion estimates that may have used biased prior emissions or background assumptions. We find strong week-to-week variability in emissions superimposed on longer-term trends, and these are consistent with independent inferences of temporal emission variability from tower, aircraft, and multispectral satellite data. New well development and natural gas spot price were significant drivers of variability in emissions over our study period but the concurrent 50 % increase in oil and gas production was not. The methane intensity (methane emitted per unit of methane gas produced) averaged 4.6 % ± 1.3 % and steadily decreased from 5 %–6 % in 2018 to 3 %–4 % in 2020. While the decreasing trend suggests improvement in operator practices during the study period, methane emissions from the Permian Basin remained high, with methane intensity an order of magnitude above the industry target of <0.2 %. Our success in using TROPOMI satellite observations for weekly estimates of emissions from a major oil production basin shows promise for application to near-real-time monitoring in support of climate change mitigation efforts. [ABSTRACT FROM AUTHOR]

We present a versatile, powerful, and user-friendly chemical data assimilation toolkit for simultaneously optimizing emissions and concentrations of chemical species based on atmospheric observations from satellites or suborbital platforms. The CHemistry and Emissions REanalysis Interface with Observations (CHEEREIO) exploits the GEOS-Chem chemical transport model and a localized ensemble transform Kalman filter algorithm (LETKF) to determine the Bayesian optimal (posterior) emissions and/or concentrations of a set of species based on observations and prior information, using an easy-to-modify configuration file with minimal changes to the GEOS-Chem or LETKF code base. The LETKF algorithm readily allows for non-linear chemistry and produces flow-dependent posterior error covariances from the ensemble simulation spread. The object-oriented Python-based design of CHEEREIO allows users to easily add new observation operators such as for satellites. CHEEREIO takes advantage of the HEMCO modular structure of input data management in GEOS-Chem to update emissions from the assimilation process independently from the GEOS-Chem code. It can seamlessly support GEOS-Chem version updates and is adaptable to other chemical transport models with similar modular input data structure. A postprocessing suite combines ensemble output into consolidated NetCDF files and supports a wide variety of diagnostic data and visualizations. We demonstrate CHEEREIO's capabilities with an out-of-the-box application, assimilating global methane emissions and concentrations at weekly temporal resolution and 2°x2.5° spatial resolution for 2019 using TROPOMI satellite observations. CHEEREIO achieves a 50-fold improvement in computational performance compared to the equivalent analytical inversion of TROPOMI observations. [ABSTRACT FROM AUTHOR]

We use 2019 TROPOMI satellite observations of atmospheric methane in an analytical inversion to quantify methane emissions from the Middle East and North Africa at up to ~25 km × 25 km resolution, using spatially allocated national UNFCCC reports as prior estimates for the fuel sector. Our resulting best estimate of anthropogenic emissions for the region is 35 % higher than the prior bottom-up estimate (+103 % for gas, +53 % for waste, +49 % for livestock, −14 % for oil) with large variability across countries. Oil and gas account for 38 % of total anthropogenic emissions in the region. TROPOMI observations can effectively optimize and separate national emissions by sector for most of the 23 countries in the region, with 6 countries accounting for most of total anthropogenic emissions including Iran (5.3 (5.0–5.5) Tg a−1; best estimate and uncertainty range), Turkmenistan (4.4 (2.8–5.1) Tg a−1), Saudi Arabia (4.3 (2.4–6.0) Tg a−1), Algeria (3.5 (2.4–4.4) Tg a−1), Egypt (3.4 (2.5–4.0) Tg a−1) , and Turkey (3.0 (2.0–4.1) Tg a−1). Most oil/gas emissions are from the production (upstream) subsector, but Iran, Turkmenistan, and Saudi Arabia have large gas emissions from transmission and distribution subsectors. We identify a high number of annual oil/gas emission hotspots in Turkmenistan, Algeria, Oman, and offshore in the Persian Gulf. We show that oil/gas methane emissions for individual countries are not related to production, invalidating a basic premise in the construction of activity-based bottom-up inventories. Instead, local infrastructure and management practices appear to be key drivers of oil/gas emissions, emphasizing the need for including top-down information from atmospheric observations in the construction of oil/gas emission inventories. We examined the methane intensity, defined as the upstream oil/gas emission per unit of methane gas produced, as a measure of the potential for decreasing emissions from the oil/gas sector, and using as reference the 0.2 % target set by industry. We find that the methane intensity in most countries is considerably higher than this target, reflecting leaky infrastructure combined with deliberate venting or incomplete flaring of gas. However, we also find that Kuwait, Saudi Arabia, and Qatar meet the industry target and thus show that the target is achievable through capture of associated gas, modern infrastructure, and concentration of operations. Decreasing methane intensities across the Middle East and North Africa to 0.2 % would achieve a 90 % decrease in oil/gas upstream emissions and a 26 % decrease of total anthropogenic methane emissions in the region, making a significant contribution toward the Global Methane Pledge. [ABSTRACT FROM AUTHOR]

We quantify weekly methane emissions at 0.25°×0.3125° (≈25×25 km²) resolution from the Permian Basin, the largest oil production basin in the United States, by inverse analysis of satellite observations from the TROPOspheric Monitoring Instrument (TROPOMI) from May 2018 to October 2020. The mean oil and gas emission from the region (± standard deviation of weekly estimates) was 3.7 ± 0.9 Tg a-1, higher than previous TROPOMI inversion estimates that may have used too-low prior emissions or biased background assumptions. We find strong week-to-week variability in emissions superimposed on longer-term trends, and these are consistent with independent inferences of temporal emission variability from tower, aircraft, and multispectral satellite data. New well development and local natural gas spot price were significant drivers of variability in emissions over our study period, but the concurrent 50 % increase in oil and gas production was not. The methane intensity (methane emitted per unit of methane gas produced) averaged 4.6 % ± 1.3 % and steadily decreased over the period from 5–6 % in 2018 to 3–4 % in 2020. While the decreasing trend suggests improvement in operator practices during the study period, methane emissions from the Permian Basin remained high, with methane intensity an order of magnitude above recent industry targets of <0.2 %. Our success in using TROPOMI satellite observations for weekly estimates of emissions from a major oil production basin shows promise for application to near-real-time monitoring in support of climate change mitigation efforts. [ABSTRACT FROM AUTHOR]

We quantify methane emissions in China and the contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. The inversion uses as prior estimate the national sector-resolved anthropogenic emission inventory reported by the Chinese government to the United Nations Framework Convention on Climate Change (UNFCCC) and thus serves as a direct evaluation of that inventory. Emissions are optimized with a Gaussian mixture model (GMM) at up to 0.25o×0.3125o resolution. The optimization is done analytically assuming lognormally distributed errors on prior emissions. Errors and information content on the optimal estimates are obtained directly from the analytical solution and also through a 36-member inversion ensemble. Our optimal estimate for total anthropogenic emissions in China is 65.0 (57.7-68.4) Tg a-1, where parentheses indicate uncertainty range. Contributions from individual sectors include 16.6 (15.6-17.6) Tg a-1 for coal, 2.3 (1.8-2.5) for oil, 0.29 (0.23-0.32) for gas, 17.8 (15.1-21.0) for livestock, 9.3 (8.2-9.9) for waste, 11.9 (10.7-12.7) for rice paddies, and 6.7 (5.8-7.1) for other sources. Our estimate is 21% higher than the Chinese inventory reported to the UNFCCC (53.6 Tg a-1), reflecting upward corrections to emissions from oil (+147%), gas (+61%), livestock (+37%), waste (+41%), and rice paddies (+34%), but downward correction for coal (-15%). It is also higher than previous inverse studies (43-62 Tg a-1) that used the much sparser GOSAT satellite observations and were conducted at coarser resolution. We are in particular better able to separate coal and rice emissions. Our higher livestock emissions are attributed largely to northern China where GOSAT has little sensitivity. Our higher waste emissions reflect at least in part a rapid growth in wastewater treatment in China. Underestimate of oil emissions in the UNFCCC report appears to reflect unaccounted super-emitting facilities. Gas emissions in China are mostly from distribution, in part because of low emission factors from production and in part because 42% of the gas is imported. Our estimate of emissions per unit of domestic gas production indicates a low life-cycle loss rate of 1.7 (1.3-1.9) %, which would imply net climate benefits from the current coal-to-gas energy transition in China. However, this small loss rate is somewhat misleading considering China's high gas imports, including from Turkmenistan where emission per unit of gas production is very high. [ABSTRACT FROM AUTHOR]

We quantify methane emissions and their 2010-2017 trends by sector in the contiguous United States (CONUS), Canada, and Mexico by inverse analysis of in situ (GLOBALVIEWplus CH4 ObsPack) and satellite (GOSAT) atmospheric methane observations. The inversion uses as prior estimate the national anthropogenic emission inventories for the three countries reported by the US Environmental Protection Agency (EPA), Environment and Climate Change Canada (ECCC), and the Instituto Nacional de Ecologia y Cambio Climatico (INECC) in Mexico to the United Nations Framework Convention on Climate Change (UNFCCC), and thus serves as an evaluation of these inventories in terms of their magnitudes and trends. Emissions are optimized with a Gaussian mixture model (GMM) at 0.5°Ã—0.625° resolution and for individual years. Optimization is done analytically using log-normal error forms. This yields closed-form statistics of error estimates and information content on the posterior (optimized) estimates, allows better representation of the high tail of the emission distribution, and enables construction of a large ensemble of inverse solutions using different observations and assumptions. We find that GOSAT and in situ observations are largely consistent and complementary in the optimization of methane emissions for North America. Mean 2010-2017 anthropogenic emissions from our base GOSAT + in situ inversion, with ranges from the inversion ensemble, are 36.9 (32.5-37.8) Tg a-1 for CONUS, 5.3 (3.6-5.7) Tg a-1 for Canada, and 6.0 (4.7-6.1) Tg a-1 for Mexico. These are higher than the most recent reported national inventories of 26.0 Tg a-1 for the US (EPA), 4.0 Tg a-1 for Canada (ECCC), and 5.0 Tg a-1 for Mexico (INECC). The correction in all three countries is largely driven by a factor of 2 underestimate in emissions from the oil sector with major contributions from the south-central US, western Canada, and southeast Mexico. Total CONUS anthropogenic emissions in our inversion peak in 2014, in contrast to the EPA report of a steady decreasing trend over 2010-2017. This reflects combined effects of increases in emissions from the oil and landfill sectors, decrease from the gas, and flat emissions from the livestock and coal sectors. We find decreasing trends in Canadian and Mexican anthropogenic methane emissions over the 2010-2017 period, mainly driven by oil and gas emissions. Our best estimates of mean 2010-2017 wetland emissions are 8.4 (6.4-10.6) Tg a-1 for CONUS, 9.9 (7.8-12.0) Tg a-1 for Canada, and 0.6 (0.4-0.6) Tg a-1 for Mexico. Wetland emissions in CONUS show an increasing trend of 2.6 (1.7-3.8) % a-1 over 2010-2017 correlated with precipitation. [ABSTRACT FROM AUTHOR]

We evaluate the global atmospheric methane column retrievals from the new TROPOMI satellite instrument and apply them to a global inversion of methane sources for 2019 at 2° x 2.5° horizontal resolution. We compare the results to an inversion using the sparser but more mature GOSAT satellite retrievals, as well as a joint inversion using both TROPOMI and GOSAT. Validation of TROPOMI and GOSAT with TCCON ground-based measurements of methane columns, after correcting for retrieval differences in prior vertical profiles and averaging kernels using the GEOS-Chem chemical transport model, shows global biases of -2.7 ppbv for TROPOMI and -1.0 ppbv for GOSAT, and regional biases of 6.7 ppbv for TROPOMI and 2.9 ppbv for GOSAT. Intercomparison of TROPOMI and GOSAT shows larger regional discrepancies exceeding 20 ppbv, mostly over regions with low surface albedo in the shortwave infrared where the TROPOMI retrieval may be biased. Our inversion uses an analytical solution to the Bayesian optimization of methane sources, thus providing an explicit characterization of error statistics and information content together with the solution. TROPOMI has ~100 times more observations than GOSAT but error correlation on the 2° x 2.5° scale of the inversion and large spatial variations of the number of observations make it less useful than GOSAT for quantifying emissions at that resolution. Finer-scale regional inversions would take better advantage of the TROPOMI data density. The TROPOMI and GOSAT inversions show consistent downward adjustments of global oil/gas emissions relative to a prior estimate based on national inventory reports to the United Nations Framework Convention on Climate Change, but consistent increases in the south-central US and in Venezuela. Global emissions from livestock (the largest anthropogenic source) are adjusted upward by TROPOMI and GOSAT relative to the EDGAR v4.3.2 prior estimate. We find large artifacts in the TROPOMI inversion over Southeast China, where seasonal rice emissions are particularly high but in phase with extensive cloudiness, and where coal emissions may be misallocated. Future advances in the TROPOMI retrieval together with finer-scale inversions and improved accounting of error correlations should enable improved exploitation of TROPOMI observations to quantify and attribute methane emissions on the global scale. [ABSTRACT FROM AUTHOR]

Global high-resolution observations of atmospheric composition from satellites can greatly improve our understanding of surface emissions through inverse analyses. Variational inverse methods can optimize surface emissions at any resolution but do not readily quantify the error and information content of the posterior solution. In fact, the information content of satellite data may be orders of magnitude lower than its coverage suggests because of failed retrievals, instrument noise, and error correlations that propagate through the inversion. Analytical solution to the inverse problem provides closed-form characterization of posterior error statistics and information content but requires the construction of the Jacobian matrix that relates emissions to atmospheric concentrations. Building the Jacobian matrix is computationally expensive at high resolution because it involves perturbing each emission element, typically individual grid cells, in the atmospheric transport model used as forward model for the inversion. We propose and analyze two methods, reduced-dimension and reduced-rank, to construct the Jacobian matrix at greatly decreased computational cost while retaining information content. Both methods begin from an initial native-resolution estimate of the Jacobian matrix constructed at no computational cost by assuming that atmospheric concentrations are most sensitive to local emissions. The reduced-dimension method uses this estimate to construct a Jacobian matrix on a multiscale grid that maintains high resolution in areas with high information content and aggregates grid cells elsewhere. The reduced-rank method constructs the Jacobian matrix at native resolution by perturbing the leading patterns of information content given by the initial estimate. We demonstrate both methods in an analytical Bayesian inversion of GOSAT methane satellite data with augmented information content over North America in July 2009. We show that both methods reproduce the results of the native-resolution inversion while achieving a factor of 4 improvement in computational performance. The reduced-dimension method produces an exact solution at lower spatial resolution while the reduced-rank method solves the inversion at native resolution in areas of high information content and defaults to the prior estimate elsewhere. [ABSTRACT FROM AUTHOR]

We use satellite (GOSAT) and in situ (GLOBALVIEWplus CH4 ObsPack) observations of atmospheric methane in a joint global inversion of methane sources, sinks, and trends for the 2010-2017 period. The inversion is done by analytical solution to the Bayesian optimization problem, yielding closed-form estimates of information content to assess the consistency and complementarity (or redundancy) of the satellite and in situ datasets. We find that GOSAT and in situ observations are to a large extent complementary, with GOSAT providing a stronger overall constraint on the global methane distributions, but in situ observations being more important for northern mid-latitudes and for relaxing global error correlations between methane emissions and the main methane sink (oxidation by OH radicals). The GOSAT observations achieve 212 independent pieces of information (DOFS) for quantifying mean 2010-2017 anthropogenic emissions on 1009 global model grid elements, and a DOFS of 122 for 2010-2017 emission trends. Adding the in situ data increases the DOFS by about 20-30%, to 262 and 161 respectively for mean emissions and trends. Our joint inversion finds that oil/gas emissions in the US and Canada are underestimated relative to the values reported by these countries to the United Nations Framework Convention on Climate Change (UNFCCC) and used here as prior estimates, while coal emissions in China are overestimated. Wetland emissions in North America are much lower than in the mean WetCHARTs inventory used as prior estimate. Oil/gas emissions in the US increase over the 2010-2017 period but decrease in Canada and Europe. Our joint GOSAT+in situ inversion yields a global methane emission of 551 Tg a-1 averaged over 2010-2017 and a methane lifetime of 11.2 years against oxidation by tropospheric OH (86% of the methane sink). [ABSTRACT FROM AUTHOR]

The article discusses that Methane is a potent greenhouse gas with a relatively short average atmospheric residence time of about a decade and is also a precursor of tropospheric ozone; and mentions the rapid increase in oil and natural gas (O/G) production in the U.S. since around 2005, driven primarily by hydraulic fracturing and horizontal drilling, has led to major concerns about increasing methane emissions and adverse climate impacts.