The TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel 5 Precursor (S5-P) satellite provides methane (CH₄) measurements with high accuracy and exceptional temporal and spatial resolution and sampling. TROPOMI CH₄ measurements are highly valuable to constrain emissions inventories and for trend analysis, with strict requirements on the data quality. This study describes the improvements that we have implemented to retrieve CH₄ from TROPOMI using the RemoTeC full-physics algorithm. The updated retrieval algorithm features a constant regularization scheme of the inversion that stabilizes the retrieval and yields less scatter in the data and includes a higher resolution surface altitude database. We have tested the impact of three state-of-the-art molecular spectroscopic databases (HITRAN 2008, HITRAN 2016 and Scientific Exploitation of Operational Missions – Improved Atmospheric Spectroscopy Databases SEOM-IAS) and found that SEOM-IAS provides the best fitting results. The most relevant update in the TROPOMI XCH₄ data product is the implementation of an a posteriori correction fully independent of any reference data that is more accurate and corrects for the underestimation at low surface albedo scenes and the overestimation at high surface albedo scenes. After applying the correction, the albedo dependence is removed to a large extent in the TROPOMI versus satellite (Greenhouse gases Observing SATellite – GOSAT) and TROPOMI versus ground-based observations (Total Carbon Column Observing Network – TCCON) comparison, which is an independent verification of the correction scheme. We validate 2 years of TROPOMI CH₄ data that show the good agreement of the updated TROPOMI CH₄ with TCCON (−3.4 ± 5.6 ppb) and GOSAT (−10.3 ± 16.8 ppb) (mean bias and standard deviation). Low- and high-albedo scenes as well as snow-covered scenes are the most challenging for the CH₄ retrieval algorithm, and although the a posteriori correction accounts for most of the bias, there is a need to further investigate the underlying cause.

Global observations of tropospheric nitrogen dioxide (NO₂) columns have been shown to be feasible from space, but consistent multi-sensor records do not yet exist, nor are they covered by planned activities at the international level. Harmonised, multi-decadal records of NO₂ columns and their associated uncertainties can provide crucial information on how the emissions and concentrations of nitrogen oxides evolve over time. Here we describe the development of a new, community best-practice NO₂ retrieval algorithm based on a synthesis of existing approaches. Detailed comparisons of these approaches led us to implement an enhanced spectral fitting method for NO₂, a 1° × 1° TM5-MP data assimilation scheme to estimate the stratospheric background and improve air mass factor calculations. Guided by the needs expressed by data users, producers, and WMO GCOS guidelines, we incorporated detailed per-pixel uncertainty information in the data product, along with easily traceable information on the relevant quality aspects of the retrieval. We applied the improved QA4ECV NO₂ algorithm to the most current level-1 data sets to produce a complete 22-year data record that includes GOME (1995–2003), SCIAMACHY (2002–2012), GOME-2(A) (2007 onwards) and OMI (2004 onwards). The QA4ECV NO₂ spectral fitting recommendations and TM5-MP stratospheric column and air mass factor approach are currently also applied to S5P-TROPOMI. The uncertainties in the QA4ECV tropospheric NO₂ columns amount to typically 40 % over polluted scenes. The first validation results of the QA4ECV OMI NO₂ columns and their uncertainties over Tai'an, China, in June 2006 suggest a small bias (−2 %) and better precision than suggested by uncertainty propagation. We conclude that our improved QA4ECV NO₂ long-term data record is providing valuable information to quantitatively constrain emissions, deposition, and trends in nitrogen oxides on a global scale.

As atmospheric methane concentrations increase at record pace, it is critical to identify individual emission sources with high potential for mitigation. Here, we leverage the synergy between satellite instruments with different spatiotemporal coverage and resolution to detect and quantify emissions from individual landfills. We use the global surveying Tropospheric Monitoring Instrument (TROPOMI) to identify large emission hot spots and then zoom in with high-resolution target-mode observations from the GHGSat instrument suite to identify the responsible facilities and characterize their emissions. Using this approach, we detect and analyze strongly emitting landfills (3 to 29 t hour ⁻¹ ) in Buenos Aires, Delhi, Lahore, and Mumbai. Using TROPOMI data in an inversion, we find that city-level emissions are 1.4 to 2.6 times larger than reported in commonly used emission inventories and that the landfills contribute 6 to 50% of those emissions. Our work demonstrates how complementary satellites enable global detection, identification, and monitoring of methane superemitters at the facility level.

Air mass factor (AMF) calculation is the largest source of uncertainty in NO₂ and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (< 0.2) and the choice of aerosol correction introduces an average uncertainty of 50 % for situations with high pollution and high aerosol loading. Our work shows that structural uncertainty in AMF calculations is significant and that it is mainly caused by the assumptions and choices made to represent the state of the atmosphere. In order to decide which approach and which ancillary data are best for AMF calculations, we call for well-designed validation exercises focusing on polluted conditions in which AMF structural uncertainty has the highest impact on NO₂ and HCHO retrievals.

Nitrogen dioxide (NO₂) is a regulated air pollutant that is of particular concern in many cities, where concentrations are high. Emissions of nitrogen oxides to the atmosphere lead to the formation of ozone and particulate matter, with adverse impacts on human health and ecosystems. The effects of emissions are often assessed through modeling based on inventories relying on indirect information that is often outdated or incomplete. Here we show that NO₂ measurements from the new, high-resolution TROPOMI satellite sensor can directly determine the strength and distribution of emissions from Paris. From the observed build-up of NO₂ pollution, we find highest emissions on cold weekdays in February 2018, and lowest emissions on warm weekend days in spring 2018. The new measurements provide information on the spatio-temporal distribution of emissions within a large city, and suggest that Paris emissions in 2018 are only 5–15% below inventory estimates for 2011–2012, reflecting the difficulty of meeting NO_x emission reduction targets.

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^∘ × 2.5^∘ horizontal resolution. We compare the results to an inversion using the sparser but more mature GOSAT satellite retrievals and to 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 inference 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^∘ × 2.5^∘ scale of the inversion and large spatial inhomogeneity in the number of observations make it less useful than GOSAT for quantifying emissions at that scale. 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.