An improved divergence method has been developed to estimate annual methane (CH4) emissions from TROPOspheric Monitoring Instrument (TROPOMI) observations. It has been applied to the period of 2018 to 2021 over the Middle East, where the orography is complicated, and the mean mixing ratio of methane (XCH4) might be affected by albedos or aerosols over some locations. To adapt to extreme changes of terrain over mountains or coasts, winds are used with their divergent part removed. A temporal filter is introduced to identify highly variable emissions and to further exclude fake sources caused by retrieval artifacts. We compare our results to widely used bottom-up anthropogenic emission inventories: Emissions Database for Global Atmospheric Research (EDGAR), Community Emissions Data System (CEDS), and Global Fuel Exploitation Inventory (GFEI) over several regions representing various types of sources. The NOx emissions are from EDGAR and Daily Emissions Constrained by Satellite Observations (DECSO), and the industrial heat sources identified by Visible Infrared Imaging Radiometer Suite (VIIRS) are further used to better understand our resulting methane emissions. Our results indicate possibly large underestimations of methane emissions in metropolises like Tehran (up to 50 %) and Isfahan (up to 70 %) in Iran. The derived annual methane emissions from oil/gas production near the Caspian Sea in Turkmenistan are comparable to GFEI but more than 2 times higher than EDGAR and CEDS in 2019. Large discrepancies in the distribution of methane sources in Riyadh and its surrounding areas are found between EDGAR, CEDS, GFEI, and our emissions. The methane emission from oil/gas production to the east of Riyadh seems to be largely overestimated by EDGAR and CEDS, while our estimates as well as GFEI and DECSO NOx indicate much lower emissions from industrial activities. On the other hand, regions like Iran, Iraq, and Oman are dominated by sources from oil and gas exploitation that probably include more irregular releases of methane, with the result that our estimates, which include only invariable sources, are lower than the bottom-up emission inventories.@en

We present a new divergence method to estimated methane (CH₄) emissions from satellite observed mean mixing ratio of methane (XCH₄) by deriving the regional enhancement of XCH₄ in the Planetary Boundary Layer (PBL). The applicability is proven by comparing the estimated emissions with its known emission inventory from a 3-month GEOS-Chem simulation. When applied to TROPOspheric Monitoring Instrument observations, sources from well-known oil/gas production areas, livestock farms and wetlands in Texas become clearly visible in the emission maps. The calculated yearly averaged total CH₄ emission over the Permian Basin is 3.06 (2.82, 3.78) Tg a⁻¹ for 2019, which is consistent with previous studies and double that of EDGAR v4.3.2 for 2012. Sensitivity tests on PBL heights, on the derived regional background and on wind speeds suggest our divergence method is quite robust. It is also a fast and simple method to estimate the CH₄ emissions globally.

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Satellite retrieval of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO₂) is critical for NO_x pollution and impact evaluation. For regions with high aerosol loadings, the retrieval accuracy is greatly affected by whether aerosol optical effects are treated implicitly (as additional effective clouds) or explicitly, among other factors. Our previous POMINO algorithm explicitly accounts for aerosol effects to improve the retrieval, especially in polluted situations over China, by using aerosol information from GEOS-Chem simulations with further monthly constraints by MODIS/Aqua aerosol optical depth (AOD) data. Here we present a major algorithm update, POMINO v1.1, by constructing a monthly climatological dataset of aerosol extinction profiles, based on level 2 CALIOP/CALIPSO data over 2007-2015, to better constrain the modeled aerosol vertical profiles. We find that GEOS-Chem captures the month-to-month variation in CALIOP aerosol layer height (ALH) but with a systematic underestimate by about 300-600 m (season and location dependent), due to a too strong negative vertical gradient of extinction above 1 km. Correcting the model aerosol extinction profiles results in small changes in retrieved cloud fraction, increases in cloud-top pressure (within 2 %-6 % in most cases), and increases in tropospheric NO₂ VCD by 4 %-16 % over China on a monthly basis in 2012. The improved NO₂ VCDs (in POMINO v1.1) are more consistent with independent ground-based MAX-DOAS observations (R²=0.80, NMB =-3.4 %, for 162 pixels in 49 days) than POMINO (R²=0.80, NMB =-9.6 %), DOMINO v2 (R²=0.68, NMB =-2.1 %), and QA4ECV (R²=0.75, NMB =-22.0 %) are. Especially on haze days, R² reaches 0.76 for POMINO v1.1, much higher than that for POMINO (0.68), DOMINO v2 (0.38), and QA4ECV (0.34). Furthermore, the increase in cloud pressure likely reveals a more realistic vertical relationship between cloud and aerosol layers, with aerosols situated above the clouds in certain months span id=page2 instead of always below the clouds. The POMINO v1.1 algorithm is a core step towards our next public release of the data product (POMINO v2), and it will also be applied to the recently launched S5P-TROPOMI sensor.

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