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Tropical tropospheric ozone (TTO) is important for the global radiation budget because the longwave radiative effect of tropospheric ozone is higher in the tropics than midlatitudes. In recent decades the TTO burden has increased, partly due to the ongoing shift of ozone precursor emissions from midlatitude regions toward the Equator. In this study, we assess the distribution and trends of TTO using ozone profiles measured by high-quality in situ instruments from the IAGOS (In-Service Aircraft for a Global Observing System) commercial aircraft, the SHADOZ (Southern Hemisphere ADditional OZonesondes) network, and the ATom (Atmospheric Tomographic Mission) aircraft campaign, as well as six satellite records reporting tropical tropospheric column ozone (TTCO): TROPOspheric Monitoring Instrument (TROPOMI), Ozone Monitoring Instrument (OMI), OMI/Microwave Limb Sounder (MLS), Ozone Mapping Profiler Suite (OMPS)/Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), Cross-track Infrared Sounder (CrIS), and Infrared Atmospheric Sounding Interferometer (IASI)/Global Ozone Monitoring Experiment 2 (GOME2). With greater availability of ozone profiles across the tropics we can now demonstrate that tropical India is among the most polluted regions (e.g., western Africa, tropical South Atlantic, Southeast Asia, Malaysia and Indonesia), with present-day 95th percentile ozone values reaching 80 nmol mol -1 in the lower free troposphere, comparable to midlatitude regions such as northeastern China and Korea. In situ observations show that TTO increased between 1994 and 2019, with the largest mid- and upper-tropospheric increases above India, Southeast Asia, and Malaysia and Indonesia (from 3.4 ± 0.8 to 6.8 ± 1.8 nmol mol -1 decade -1), reaching 11 ± 2.4 and 8 ± 0.8 nmol mol -1 decade -1 close to the surface (India and Malaysia–Indonesia, respectively). The longest continuous satellite records only span 2004–2019 but also show increasing ozone across the tropics when their full sampling is considered, with maximum trends over Southeast Asia of 2.31 ± 1.34 nmol mol -1 decade -1 (OMI) and 1.69 ± 0.89 nmol mol -1 decade -1 (OMI/MLS). In general, the sparsely sampled aircraft and ozonesonde records do not detect the 2004–2019 ozone increase, which could be due to the genuine trends on this timescale being masked by the additional uncertainty resulting from sparse sampling. The fact that the sign of the trends detected with satellite records changes above three IAGOS regions, when their sampling frequency is limited to that of the in situ observations, demonstrates the limitations of sparse in situ sampling strategies. This study exposes the need to maintain and develop high-frequency continuous observations (in situ and remote sensing) above the tropical Pacific Ocean, the Indian Ocean, western Africa, and South Asia in order to estimate accurate and precise ozone trends for these regions. In contrast, Southeast Asia and Malaysia–Indonesia are regions with such strong increases in ozone that the current in situ sampling frequency is adequate to detect the trends on a relatively short 15-year timescale. [ABSTRACT FROM AUTHOR]

An improved divergence method has been developed to estimate annual methane (CH 4) 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 (XCH 4) 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 NO x 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 NO x 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. [ABSTRACT FROM AUTHOR]

The Sentinel-5 Precursor (S5P) satellite operated by the European Space Agency has carried the TROPOspheric Monitoring Instrument (TROPOMI) on a Sun-synchronous low-Earth orbit since 13 October 2017. The S5P mission has acquired more than 5 years of TROPOMI nadir ozone profile data retrieved from the level 0 to 1B processor version 2.0 and the level 1B to 2 optimal-estimation-based processor version 2.4.0. The latter is described in detail in this work, followed by the geophysical validation of the resulting ozone profiles for the period May 2018 to April 2023. Comparison of TROPOMI ozone profile data to co-located ozonesonde and lidar measurements used as references concludes to a median agreement better than 5 % to 10 % in the troposphere. The bias goes up to - 15 % in the upper stratosphere (35–45 km) where it can exhibit vertical oscillations. The comparisons show a dispersion of about 30 % in the troposphere and 10 % to 20 % in the upper troposphere to lower stratosphere and in the middle stratosphere, which is close to mission requirements. Chi-square tests of the observed differences confirm on average the validity of the ex ante (prognostic) satellite and ground-based data uncertainty estimates in the middle stratosphere above about 20 km. Around the tropopause and below, the mean chi-square value increases up to about four, meaning that the ex ante TROPOMI uncertainty is underestimated. The information content of the ozone profile retrieval is characterised by about five to six vertical subcolumns of independent information and a vertical sensitivity (i.e. the fraction of the information that originates from the measurement) nearly equal to unity at altitudes from about 20 to 50 km, decreasing rapidly at altitudes above and below. The barycentre of the retrieved information is usually close to the nominal retrieval altitude in the 20–50 km altitude range, with positive and negative offsets of up to 10 km below and above this range, respectively. The effective vertical resolution of the profile retrieval usually ranges within 10–15 km, with a minimum close to 7 km in the middle stratosphere. Increased sensitivities and higher effective vertical resolutions are observed at higher solar zenith angles (above about 60°), as can be expected, and correlate with higher retrieved ozone concentrations. The vertical sensitivity of the TROPOMI tropospheric ozone retrieval is found to depend on the solar zenith angle, which translates into a seasonal and meridian dependence of the bias with respect to reference measurements. A similar although smaller effect can be seen for the viewing zenith angle. Additionally, the bias is negatively correlated with the surface albedo for the lowest three ozone subcolumns (0–18 km), despite the albedo's apparently slightly positive correlation with the retrieval degrees of freedom in the signal. For the 5 years of TROPOMI ozone profile data that are available now, an overall positive drift is detected for the same three subcolumns, while a negative drift is observed above (24–32 km), resulting in a negligible vertically integrated drift. [ABSTRACT FROM AUTHOR]

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 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 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 GEFI but more than two times higher than EDGAR and CEDS in 2019. Large discrepancies of 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 in the east to Riyadh seems to be largely overestimated by EDGAR and CEDS, while our estimates, and also GFEI and DECSO NOX indicate much lower emissions from industry activities. On the other hand, regions like Iran, Iraq, and Oman are dominated by sources from oil and gas exploitation that probably includes more irregular releases of methane, with the result that our estimates, that include only invariable sources, are lower than the bottom-up emission inventories. [ABSTRACT FROM AUTHOR]

The Sentinel-5 Precursor (S5P) satellite operated by the European Space Agency (ESA) carries the TROPOspheric Monitoring Instrument (TROPOMI) on a Sun-synchronous low-Earth orbit since October 13, 2017. The S5P mission has acquired more than five years of TROPOMI nadir ozone profile data retrieved from the Level-0-to-1B processor version 2.0 and the Level-1B-to-2 Optimal Estimation based processor version 2.4.0. The latter is described in detail in this work, followed by the geophysical validation of the resulting ozone profiles for the period May 2018 to April 2023. Comparison of TROPOMI ozone profile data to co-located ozonesonde and lidar measurements used as references, concludes to a median agreement better than 5 to 10 % in the troposphere. The bias goes up to -15 % in the upper stratosphere (35-45 km) where it can exhibit vertical oscillations. The comparisons show a dispersion of about 30 % in the troposphere and 10 to 20 % in the upper troposphere to lower stratosphere (UTLS) and in the middle stratosphere, which is close to mission requirements. Chi-square tests of the observed differences confirm on average the validity of the ex-ante (prognostic) satellite and ground-based data uncertainty estimates in the middle stratosphere, above about 20 km. Around the tropopause and below, the mean chi-square value increases up to about four, meaning that the ex-ante TROPOMI uncertainty is underestimated. The information content of the ozone profile retrieval is characterised by about five to six vertical sub-columns of independent information and a vertical sensitivity nearly equal to unity at altitudes from about 20 to 50 km, decreasing rapidly at altitudes above and below. The barycentre of the retrieved information is usually close to the nominal retrieval altitude in the 20-50 km altitude range, with positive and negative offsets of up to 10 km below and above this range, respectively. The effective vertical resolution of the profile retrieval usually ranges within 10-15 km, with a minimum close to 7 km in the middle stratosphere. Increased sensitivity and higher effective vertical resolution are observed at higher solar zenith angle (SZA, above about 60°C), as can be expected, and correlate with higher retrieved ozone concentrations. The vertical sensitivity of the TROPOMI tropospheric ozone amount is found to depend on solar zenith angle, which translates into a seasonal and meridian dependence of its bias with respect to reference measurements. A similar although smaller effect can be seen for the viewing zenith angle (VZA). Additionally, the bias is negatively correlated with the surface albedo for the 6-12 km ozone subcolumn, despite the latter's apparently slightly positive correlation with the retrieval degrees of freedom in the signal. For the five years of TROPOMI ozone profile data that are available now, an overall positive drift is detected for the lowest three subcolumns (0-18 km), while a negative drift is observed for the two subcolumns above (18-32 km), resulting in a negligible vertically integrated drift. [ABSTRACT FROM AUTHOR]

Denitrification of the stratospheric vortex is a crucial process for the Antarctic Ozone Hole formation resulting in an analogous stratospheric "Nitrogen Hole". Here, 2018–2021 daily TROPOMI measurements are used for the first time for a detailed characterization of this Nitrogen Hole. Nitrogen dioxide total columns exhibit strong spatiotemporal and seasonal variations associated with both photochemistry as well as transport and mixing processes. Combined with total ozone column data two main regimes are identified: inner-vortex ozone and nitrogen dioxide depleted air and outer-vortex air enhanced in ozone and nitrogen dioxide. Within the vortex total ozone and total stratospheric nitrogen dioxide are strongly correlated which is much less evident outside of the vortex. Connecting both main regimes are what is defined here as "mixing lines", a third regime of coherent patterns in the total nitrogen dioxide column – total ozone column phase space. These mixing lines exist because of differences in three dimensional variations of nitrogen dioxide and ozone thereby providing information about vortex dynamics and cross-vortex edge mixing. On the other hand, interannual variability of nitrogen dioxide – total ozone characteristics are rather small except in 2019 when the vortex was unusually unstable. Overall, the results show that daily stratospheric nitrogen dioxide column satellite measurements provide an innovative means for characterizing and Polar stratospheric denitrification processes and vortex dynamics and potentially long term monitoring if the total nitrogen column data record is extended with past satellite observations. [ABSTRACT FROM AUTHOR]