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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]

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]

Chemical ozone destruction occurs over both polar regions in local winter-spring. In the Antarctic, essentially complete removal of lower-stratospheric ozone currently results in an ozone hole every year, whereas in the Arctic, ozone loss is highly variable and has until now been much more limited. Here we demonstrate that chemical ozone destruction over the Arctic in early 2011 was--for the first time in the observational record--comparable to that in the Antarctic ozone hole. Unusually long-lasting cold conditions in the Arctic lower stratosphere led to persistent enhancement in ozone-destroying forms of chlorine and to unprecedented ozone loss, which exceeded 80 per cent over 18-20 kilometres altitude. Our results show that Arctic ozone holes are possible even with temperatures much milder than those in the Antarctic. We cannot at present predict when such severe Arctic ozone depletion may be matched or exceeded., Since the emergence of the Antarctic 'ozone hole' in the 1980s (1) and elucidation of the chemical mechanisms (2-5) and meteorological conditions (6) involved in its formation, the likelihood of [...]

A TROPOspheric Monitoring Instrument (TROPOMI) validation campaign was held in the Netherlands based at the CESAR (Cabauw Experimental Site for Atmospheric Research) Observatory during September 2019. The TROpomi vaLIdation eXperiment (TROLIX-19) consisted of active and passive remote sensing platforms in conjunction with several balloon-borne and surface chemical (e.g. ozone and nitrogen dioxide) measurements. The goal of this joint NASA-KNMI geophysical validation campaign was to make intensive observations in the TROPOMI domain in order to be able to establish the quality of the L2 satellite data products under realistic conditions, such as non-idealized conditions with varying cloud cover and a range of atmospheric conditions at a rural site. The research presented here focuses on using ozone lidars from NASA’s Goddard Space Flight Center to better evaluate the characterization of ozone throughout TROLIX-19. Results of comparisons to the lidar systems with balloon, space-borne, and ground-based passive measurements are shown. In addition, results are compared to a global coupled chemistry meteorology model to illustrate the vertical variability and columnar amounts of both tropospheric and stratospheric ozone during the campaign period. [ABSTRACT FROM AUTHOR]

Nitrogen dioxide (NO2) is an important contributor to air pollution and can adversely affect human health1–9. A decrease in NO2 concentrations has been reported as a result of lockdown measures to reduce the spread of COVID-1910–20. Questions remain, however, regarding the relationship of satellite-derived atmospheric column NO2 data with health-relevant ambient ground-level concentrations, and the representativeness of limited ground-based monitoring data for global assessment. Here we derive spatially resolved, global ground-level NO2 concentrations from NO2 column densities observed by the TROPOMI satellite instrument at sufficiently fine resolution (approximately one kilometre) to allow assessment of individual cities during COVID-19 lockdowns in 2020 compared to 2019. We apply these estimates to quantify NO2 changes in more than 200 cities, including 65 cities without available ground monitoring, largely in lower-income regions. Mean country-level population-weighted NO2 concentrations are 29% ± 3% lower in countries with strict lockdown conditions than in those without. Relative to long-term trends, NO2 decreases during COVID-19 lockdowns exceed recent Ozone Monitoring Instrument (OMI)-derived year-to-year decreases from emission controls, comparable to 15 ± 4 years of reductions globally. Our case studies indicate that the sensitivity of NO2 to lockdowns varies by country and emissions sector, demonstrating the critical need for spatially resolved observational information provided by these satellite-derived surface concentration estimates.The satellite instrument TROPOMI is used to assess ambient NO2 levels at approximately one-kilometre resolution across 215 cities worldwide during COVID-19 lockdowns, finding about 30% lower NO2 concentrations in countries with strict lockdowns. [ABSTRACT FROM AUTHOR]

The Ozone Monitoring Instrument (OMI) was launched on July 15, 2004, with an expected mission lifetime of 5 years. After more than 17 years in orbit the instrument is still functioning satisfactorily, and in principle can continue doing so for many years more. In order to continue the datasets acquired by OMI and the Microwave Limb Sounder the mission was extended up to at least 2023. Actions have been taken to ensure the proper functioning of the OMI instrument operations, the data processing, and the calibration monitoring system until the eventual end of the mission. For the data processing a new level 0 to level 1b data processor was built based on the recent developments for Tropospheric Monitoring Instrument (TROPOMI). With corrections for the degradation of the instrument now included, it is feasible to generate a new data collection to supersede the current collection 3 data products. This paper describes the differences between the collection 3 and collection 4 data. It will be shown that the collection 4 L1b data is a clear improvement with respect to the previous collections. By correcting for the gentle optical and electronic aging that has occurred over the past 17 years, OMI's ability to make trend-quality ozone measurements has further improved. [ABSTRACT FROM AUTHOR]

Sentinel-5 Precursor (S-5P), launched in October 2017, carrying the TROPOspheric Monitoring Instrument (TROPOMI) nadir-viewing spectrometer, is the first mission of the Copernicus Programme dedicated to the monitoring of air quality, climate, and ozone. In the presented study, the TROPOMI tropospheric nitrogen dioxide (NO2) L2 product (OFFL v1.03.01; 3.5 km x 7 km at nadir observations) has been validated over strongly polluted urban regions by comparison with coincident high-resolution Airborne Prism EXperiment (APEX) remote sensing observations (~75 m x 120 m). Satellite products can be optimally assessed based on (APEX) airborne remote sensing observations as a large amount of satellite pixels can be fully mapped at high accuracy and in a relatively short time interval, reducing the impact of spatio-temporal mismatches. In the framework of the S5PVAL-BE campaign, the APEX imaging spectrometer has been deployed during four mapping flights (26-29 June 2019) over the two largest urban regions in Belgium, i.e. Brussels and Antwerp, in order to map the horizontal distribution of tropospheric NO2. For each flight, 10 to 20 TROPOMI pixels were fully covered by approximately 2800 to 4000 APEX measurements within each TROPOMI pixel. The TROPOMI and APEX NO2 vertical column density (VCD) retrieval schemes are similar in concept. Overall for the ensemble of the four flights, the standard TROPOMI NO2 VCD product is well correlated (R = 0.92) but biased negatively by -1.2 ± 1.2 x 1015 molec cm-2 or -14 % ± 12 %, on average, with respect to coincident APEX NO2 retrievals. When replacing the coarse 1° x 1° TM5-MP a priori NO2 profiles by NO2 profile shapes from the CAMS regional CTM ensemble at 0.1° x 0.1°, the slope increases by 11 % to 0.93, and the bias is reduced to -0.1 ± 1.0 x 1015 molec cm-2 or -1.0 % ± 12 %. When the absolute value of the difference is taken, the bias is 1.3 x 1015 molec cm-2 or 16 %, and 0.7 x 1015 molec cm-2 or 9 % on average, when comparing APEX NO2 VCDs with TM5-MP-based and CAMS-based NO2 VCDs, respectively. Both sets of retrievals are well within the accuracy requirement of a maximum bias of 25-50 % for the TROPOMI tropospheric NO2 product for all individual compared pixels. Additionally, the APEX data set allows the study of TROPOMI subpixel variability and impact of signal smoothing due to its finite satellite pixel size, typically coarser than fine-scale gradients in the urban NO2 field. The amount of underestimation of peak plume values and overestimation of urban background values in the TROPOMI data is in the order of 1-2 x 1015 molec cm-2 on average, or 10 %-20 %, in case of an urban scene. [ABSTRACT FROM AUTHOR]

After the launch of the Sentinel-5 Precursor satellite on 13 October 2017 its single payload, the Tropospheric Monitoring Instrument (TROPOMI), was commissioned during 6 months. In this time the instrument was tested and calibrated extensively. During this phase the geolocation calibration was validated using a dedicated measurement zoom mode. With the help of spacecraft manoeuvres the solar angle dependence of the irradiance radiometry was calibrated for both internal diffusers. This improved the results that were obtained on-ground significantly. Furthermore the orbital and long term stability was tested for electronic gains, offsets, non-linearity, the dark current and the output of the internal light sources. The CCD output gain of the UV, UVIS and NIR detectors shows drifts over time which can be corrected for in the L1b processor. In-flight measurements also revealed inconsistencies of the radiometric calibration and degradation of the UV spectrometer. Degradation is also detected for the internal solar diffusers. Since the start of the nominal operations (E2) phase in orbit 2818 on 30 April 2018, regularly scheduled calibration measurements on the eclipse side of the orbit are used for monitoring and updates to calibration key data. This article reports on the main results of the commissioning phase, the in-flight calibration and on the instrument's stability since launch. Insights from commissioning and in-flight monitoring led to updates to the Level 1b processor and its calibration key data. The updated processor is planned to be used for nominal processing from 2020 on. [ABSTRACT FROM AUTHOR]