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Denitrification within the stratospheric vortex is a crucial process for Antarctic ozone hole formation, resulting in an analogous stratospheric “nitrogen hole”. Sedimentation of large nitric acid trihydrate polar stratospheric cloud particles within the Antarctic polar stratospheric vortex that form during winter depletes the inner vortex of nitrogen oxides. Here, 2018–2021 daily TROPOspheric Monitoring Instrument (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 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 the two main regimes is a third regime of coherent patterns in the total nitrogen dioxide column–total ozone column phase space – defined here as “mixing lines”. 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 is 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 polar stratospheric denitrification processes, vortex dynamics, and long-term monitoring of Antarctic ozone hole conditions.

Abstract We have analyzed Sentinel‐5 Precursor TROPOspheric Monitoring Instrument (TROPOMI) data over the Copperbelt mining region (Democratic Republic of Congo and Zambia). Despite high background values, annual 2019–2022 means of TROPOMI NO2 (nitrogen dioxide) show local enhancements consistent with six point sources (four copper/cobalt mines, two cities) where high‐emission industrial activities take place. We have quantified annual NOx (nitrogen oxides) emissions from these point sources, identified temporal trends in emissions, and found strong correlations with production data from colocated mines and one oil refinery. The Copernicus Atmosphere Monitoring Service Global Anthropogenic (CAMS‐GLOB‐ANT) version 5 inventory underpredicts TROPOMI‐derived emissions and lacks the temporal trends observed in TROPOMI and mine/refinery production. These results demonstrate the potential for satellite monitoring of mining and other industrial activities, often unreported or underestimated, which impact the air quality of local communities. This is particularly important for Africa, where mining is increasing aggressively.

The purpose of this study is to investigate the ability of the Sentinel-5P TROPOspheric Monitoring Instrument (TROPOMI) to derive accurate geometrical features of lofted aerosol layers, selecting the Mediterranean Basin as the study area. Comparisons with ground-based correlative measurements constitute a key component in the validation of passive and active satellite aerosol products. For this purpose, we use ground-based observations from quality-controlled lidar stations reporting to the European Aerosol Research Lidar Network (EARLINET). An optimal methodology for validation purposes has been developed and applied using the EARLINET optical profiles and TROPOMI aerosol products, aiming at the in-depth evaluation of the TROPOMI aerosol layer height (ALH) product for the period 2018 to 2022 over the Mediterranean Basin. Seven EARLINET stations were chosen, taking into consideration their proximity to the sea, which provided 63 coincident aerosol cases for the satellite retrievals. In the following, we present the first validation results for the TROPOMI/S5P ALH using the optimized EARLINET lidar products employing the automated validation chain designed for this purpose. The quantitative validation at pixels over the selected EARLINET stations illustrates that the TROPOMI ALH product is consistent with the EARLINET lidar products, with a high correlation coefficient R=0.82 (R=0.51) and a mean bias of -0.51±0.77 km and -2.27±1.17 km over ocean and land, respectively. Overall, it appears that aerosol layer altitudes retrieved from TROPOMI are systematically lower than altitudes from the lidar retrievals. High-albedo scenes, as well as low-aerosol-load scenes, are the most challenging for the TROPOMI retrieval algorithm, and these results testify to the need to further investigate the underlying cause. This work provides a clear indication that the TROPOMI ALH product can under certain conditions achieve the required threshold accuracy and precision requirements of 1 km, especially when only ocean pixels are included in the comparison analysis. Furthermore, we describe and analyse three case studies in detail, one dust and two smoke episodes, in order to illustrate the strengths and limitations of the TROPOMI ALH product and demonstrate the presented validation methodology. The present analysis provides important additions to the existing validation studies that have been performed so far for the TROPOMI S5P ALH product, which were based only on satellite-to-satellite comparisons.

DISAMAR (determining instrument specifications and analysing methods for atmospheric retrieval) is a computer model developed to simulate retrievals of properties of atmospheric trace gases, aerosols, clouds, and the ground surface from passive remote sensing observations in a wavelength range from 270 to 2400 nm. It is being used for the TROPOMI/Sentinel-5P and Sentinel-4/5 missions to derive Level-1b product specifications. DISAMAR uses the doubling–adding method and the layer-based orders of scattering method for radiative transfer calculations. It can perform retrievals using three different approaches: optimal estimation (OE), differential optical absorption spectroscopy (DOAS), and the combination of DOAS and OE, called DISMAS (differential and smooth absorption separated). The derivatives, which are needed in the OE and DISMAS retrievals, are derived in a semi-analytical way from the adding formulae. DISAMAR uses plane-parallel homogeneous atmospheric layers with a pseudo-spherical correction for large solar zenith angles. DISAMAR has various novel features and diverse retrieval possibilities, such as retrieving aerosol layer heights and ozone vertical profiles. This paper provides an overview of the DISAMAR model version 4.1.5 without treating all the details. We focus on the principle of the layer-based orders of scattering method, the calculation of the semi-analytical derivatives, and the DISMAS retrieval method, and it is to our knowledge the first time that these methods are described. We demonstrate some applications of DISMAS and the derivatives.

The aim of this paper is to highlight how TROPOspheric Monitoring Instrument (TROPOMI) trace gas data can best be used and interpreted to understand event-based impacts on air quality from regional to city scales around the globe. For this study, we present the observed changes in the atmospheric column amounts of five trace gases (NO2, SO2, CO, HCHO, and CHOCHO) detected by the Sentinel-5P TROPOMI instrument and driven by reductions in anthropogenic emissions due to COVID-19 lockdown measures in 2020. We report clear COVID-19-related decreases in TROPOMI NO2 column amounts on all continents. For megacities, reductions in column amounts of tropospheric NO2 range between 14 % and 63 %. For China and India, supported by NO2 observations, where the primary source of anthropogenic SO2 is coal-fired power generation, we were able to detect sector-specific emission changes using the SO2 data. For HCHO and CHOCHO, we consistently observe anthropogenic changes in 2-week-averaged column amounts over China and India during the early phases of the lockdown periods. That these variations over such a short timescale are detectable from space is due to the high resolution and improved sensitivity of the TROPOMI instrument. For CO, we observe a small reduction over China, which is in concert with the other trace gas reductions observed during lockdown; however, large interannual differences prevent firm conclusions from being drawn. The joint analysis of COVID-19-lockdown-driven reductions in satellite-observed trace gas column amounts using the latest operational and scientific retrieval techniques for five species concomitantly is unprecedented. However, the meteorologically and seasonally driven variability of the five trace gases does not allow for drawing fully quantitative conclusions on the reduction in anthropogenic emissions based on TROPOMI observations alone. We anticipate that in future the combined use of inverse modeling techniques with the high spatial resolution data from S5P/TROPOMI for all observed trace gases presented here will yield a significantly improved sector-specific, space-based analysis of the impact of COVID-19 lockdown measures as compared to other existing satellite observations. Such analyses will further enhance the scientific impact and societal relevance of the TROPOMI mission.

Nitrogen dioxide (NO2) is one of the main data products measured by the Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor (S5P) satellite, which combines a high signal-to-noise ratio with daily global coverage and high spatial resolution. TROPOMI provides a valuable source of information to monitor emissions from local sources such as power plants, industry, cities, traffic and ships, and variability of these sources in time. Validation exercises of NO2 v1.2–v1.3 data, however, have revealed that TROPOMI's tropospheric vertical column densities (VCDs) are too low by up to 50 % over highly polluted areas. These findings are mainly attributed to biases in the cloud pressure retrieval, the surface albedo climatology and the low resolution of the a priori profiles derived from global simulations of the TM5-MP chemistry model. This study describes improvements in the TROPOMI NO2 retrieval leading to version v2.2, operational since 1 July 2021. Compared to v1.x, the main changes are the following. (1) The NO2-v2.2 data are based on version-2 level-1b (ir)radiance spectra with improved calibration, which results in a small and fairly homogeneous increase in the NO2 slant columns of 3 % to 4 %, most of which ends up as a small increase in the stratospheric columns. (2) The cloud pressures are derived with a new version of the FRESCO cloud retrieval already introduced in NO2-v1.4, which led to a lowering of the cloud pressure, resulting in larger tropospheric NO2 columns over polluted scenes with a small but non-zero cloud coverage. (3) For cloud-free scenes a surface albedo correction is introduced based on the observed reflectance, which also leads to a general increase in the tropospheric NO2 columns over polluted scenes of order 15 %. (4) An outlier removal was implemented in the spectral fit, which increases the number of good-quality retrievals over the South Atlantic Anomaly region and over bright clouds where saturation may occur. (5) Snow/ice information is now obtained from ECMWF weather data, increasing the number of valid retrievals at high latitudes. On average the NO2-v2.2 data have tropospheric VCDs that are between 10 % and 40 % larger than the v1.x data, depending on the level of pollution and season; the largest impact is found at mid and high latitudes in wintertime. This has brought these tropospheric NO2 closer to Ozone Monitoring Instrument (OMI) observations. Ground-based validation shows on average an improvement of the negative bias of the stratospheric (from −6 % to −3 %), tropospheric (from −32 % to −23 %) and total (from −12 % to −5 %) columns. For individual measurement stations, however, the picture is more complex, in particular for the tropospheric and total columns.

Ozone in the troposphere affects humans and ecosystems as a pollutant and as a greenhouse gas. Observing, understanding and modelling this dual role, as well as monitoring effects of international regulations on air quality and climate change, however, challenge measurement systems to operate at opposite ends of the spatio-temporal scale ladder. Aboard the ESA/EU Copernicus Sentinel-5 Precursor (S5P) satellite launched in October 2017, the TROPOspheric Monitoring Instrument (TROPOMI) aspires to take the next leap forward by measuring ozone and its precursors at unprecedented horizontal resolution until at least the mid-2020s. In this work, we assess the quality of TROPOMI's first release (V01.01.05–08) of tropical tropospheric ozone column (TrOC) data. Derived with the convective cloud differential (CCD) method, TROPOMI daily TrOC data represent the 3 d moving mean ozone column between the surface and 270 hPa under clear-sky conditions gridded at 0.5∘ latitude by 1∘ longitude resolution. Comparisons to almost 2 years of co-located SHADOZ ozonesonde and satellite data (Aura OMI and MetOp-B GOME-2) conclude to TROPOMI biases between −0.1 and +2.3 DU (<+13 %) when averaged over the tropical belt. The field of the bias is essentially uniform in space (deviations DU) and stable in time at the 1.5–2.5 DU level. However, the record is still fairly short, and continued monitoring will be key to clarify whether observed patterns and stability persist, alter behaviour or disappear. Biases are partially due to TROPOMI and the reference data records themselves, but they can also be linked to systematic effects of the non-perfect co-locations. Random uncertainty due to co-location mismatch contributes considerably to the 2.6–4.6 DU (∼14 %–23 %) statistical dispersion observed in the difference time series. We circumvent part of this problem by employing the triple co-location analysis technique and infer that TROPOMI single-measurement precision is better than 1.5–2.5 DU (∼8 %–13 %), in line with uncertainty estimates reported in the data files. Hence, the TROPOMI precision is judged to be 20 %–25 % better than for its predecessors OMI and GOME-2B, while sampling at 4 times better spatial resolution and almost 2 times better temporal resolution. Using TROPOMI tropospheric ozone columns at maximal resolution nevertheless requires consideration of correlated errors at small scales of up to 5 DU due to the inevitable interplay of satellite orbit and cloud coverage. Two particular types of sampling error are investigated, and we suggest how these can be identified or remedied. Our study confirms that major known geophysical patterns and signals of the tropical tropospheric ozone field are imprinted in TROPOMI's 2-year data record. These include the permanent zonal wave-one pattern, the pervasive annual and semiannual cycles, the high levels of ozone due to biomass burning around the Atlantic basin, and enhanced convective activity cycles associated with the Madden–Julian Oscillation over the Indo-Pacific warm pool. TROPOMI's combination of higher precision and higher resolution reveals details of these patterns and the processes involved, at considerably smaller spatial and temporal scales and with more complete coverage than contemporary satellite sounders. If the accuracy of future TROPOMI data proves to remain stable with time, these hold great potential to be included in Climate Data Records, as well as serve as a travelling standard to interconnect the upcoming constellation of air quality satellites in geostationary and low Earth orbits.

The global fire emission inventories depend on ground and airborne measurements of species-specific emission factors (EFs), which translate dry matter losses due to fires to actual trace gas and aerosol emissions. The EFs of nitrogen oxides (NOx) and carbon monoxide (CO) can function as a proxy for combustion efficiency to distinguish flaming from smoldering combustion. The uncertainties in these EFs remain large as they are limited by the spatial and temporal representativeness of the measurements. The global coverage of satellite observations has the advantage of filling this gap, making these measurements highly complementary to ground-based or airborne data. We present a new analysis of biomass burning pollutants using space-borne data to investigate the spatiotemporal efficiency of fire combustion. Column measurements of nitrogen dioxide and carbon monoxide (XNO2 and XCO) from the TROPOspheric Monitoring Instrument (TROPOMI) are used to quantify the relative atmospheric enhancements of these species over different fire-prone regions around the world. We find spatial and temporal patterns in the ΔXNO2 ∕ ΔXCO ratio that point to distinct differences in biomass burning behavior. Such differences are induced by the burning phase of the fire (e.g., high-temperature flaming vs. low-temperature smoldering combustion) and burning practice (e.g., the combustion of logs, coarse woody debris and soil organic matter vs. the combustion of fine fuels such as savanna grasses). The sampling techniques and the signal-to-noise ratio of the retrieved ΔXNO2 ∕ ΔXCO signals were quantified with WRF-Chem experiments and showed similar distinct differences in combustion types. The TROPOMI measurements show that the fraction of surface smoldering combustion is much larger for the boreal forest fires in the upper Northern Hemisphere and peatland fires in Indonesia. These types of fires cause a much larger increase (3 to 6 times) in ΔXCO relative to ΔXNO2 than elsewhere in the world. The high spatial and temporal resolution of TROPOMI also enables the detection of spatial gradients in combustion efficiency at smaller regional scales. For instance, in the Amazon, we found higher combustion efficiency (up to 3-fold) for savanna fires than for the nearby tropical deforestation fires. Out of two investigated fire emission products, the TROPOMI measurements support the broad spatial pattern of combustion efficiency rooted in GFED4s. Meanwhile, TROPOMI data also add new insights into regional variability in combustion characteristics that are not well represented in the different emission inventories, which can help the fire modeling community to improve their representation of the spatiotemporal variability in EFs.

This paper reports on consolidated ground-based validation results of the atmospheric NO2 data produced operationally since April 2018 by the TROPOspheric Monitoring Instrument (TROPOMI) on board of the ESA/EU Copernicus Sentinel-5 Precursor (S5P) satellite. Tropospheric, stratospheric, and total NO2 column data from S5P are compared to correlative measurements collected from, respectively, 19 Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS), 26 Network for the Detection of Atmospheric Composition Change (NDACC) Zenith-Scattered-Light DOAS (ZSL-DOAS), and 25 Pandonia Global Network (PGN)/Pandora instruments distributed globally. The validation methodology gives special care to minimizing mismatch errors due to imperfect spatio-temporal co-location of the satellite and correlative data, e.g. by using tailored observation operators to account for differences in smoothing and in sampling of atmospheric structures and variability and photochemical modelling to reduce diurnal cycle effects. Compared to the ground-based measurements, S5P data show, on average, (i) a negative bias for the tropospheric column data, of typically −23 % to −37 % in clean to slightly polluted conditions but reaching values as high as −51 % over highly polluted areas; (ii) a slight negative median difference for the stratospheric column data, of about −0.2 Pmolec cm−2, i.e. approx. −2 % in summer to −15 % in winter; and (iii) a bias ranging from zero to −50 % for the total column data, found to depend on the amplitude of the total NO2 column, with small to slightly positive bias values for columns below 6 Pmolec cm−2 and negative values above. The dispersion between S5P and correlative measurements contains mostly random components, which remain within mission requirements for the stratospheric column data (0.5 Pmolec cm−2) but exceed those for the tropospheric column data (0.7 Pmolec cm−2). While a part of the biases and dispersion may be due to representativeness differences such as different area averaging and measurement times, it is known that errors in the S5P tropospheric columns exist due to shortcomings in the (horizontally coarse) a priori profile representation in the TM5-MP chemical transport model used in the S5P retrieval and, to a lesser extent, to the treatment of cloud effects and aerosols. Although considerable differences (up to 2 Pmolec cm−2 and more) are observed at single ground-pixel level, the near-real-time (NRTI) and offline (OFFL) versions of the S5P NO2 operational data processor provide similar NO2 column values and validation results when globally averaged, with the NRTI values being on average 0.79 % larger than the OFFL values.

The ultraviolet (UV) Absorbing Aerosol Index (AAI) is widely used as an indicator for the presence of absorbing aerosols in the atmosphere. Here we consider the TROPOMI AAI based on the 340 nm/380 nm wavelength pair. We investigate the effects of clouds on the AAI observed at small and large scales. The large-scale effects are studied using an aggregate of TROPOMI measurements over an area mostly devoid of absorbing aerosols (Pacific Ocean). The study reveals that several structural features can be distinguished in the AAI, such as the cloud bow, viewing zenith angle dependence, sunglint, and a previously unexplained increase in AAI values at extreme viewing and solar geometries. We explain these features in terms of the bidirectional reflectance distribution function (BRDF) of the scene in combination with the different ratios of diffuse and direct illumination of the surface at 340 and 380 nm. To reduce the dependency on the BRDF and homogenize the AAI distribution across the orbit, we present three different AAI retrieval models: the traditional Lambertian scene model (LSM), a Lambertian cloud model (LCM), and a scattering cloud model (SCM). We perform a model study to assess the propagation of errors in auxiliary databases used in the cloud models. The three models are then applied to the same low-aerosol region. Results show that using the LCM and SCM gives on average a higher AAI than the LSM. Additionally, a more homogeneous distribution is retrieved across the orbit. At the small scale, related to the high spatial resolution of TROPOMI, strong local increases and decreases in AAI are observed in the presence of clouds. The BRDF effect presented here is a first step – more research is needed to explain the small-scale cloud effects on the AAI.

Airborne and ground-based Pandora spectrometer NO2 column measurements were collected during the 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) in the New York City/Long Island Sound region, which coincided with early observations from the Sentinel-5P TROPOspheric Monitoring Instrument (TROPOMI) instrument. Both airborne- and ground-based measurements are used to evaluate the TROPOMI NO2 Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NO2. First, airborne and Pandora TrVCs are compared to evaluate the uncertainty of the airborne TrVC and establish the spatial representativeness of the Pandora observations. The 171 coincidences between Pandora and airborne TrVCs are found to be highly correlated (r2= 0.92 and slope of 1.03), with the largest individual differences being associated with high temporal and/or spatial variability. These reference measurements (Pandora and airborne) are complementary with respect to temporal coverage and spatial representativity. Pandora spectrometers can provide continuous long-term measurements but may lack areal representativity when operated in direct-sun mode. Airborne spectrometers are typically only deployed for short periods of time, but their observations are more spatially representative of the satellite measurements with the added capability of retrieving at subpixel resolutions of 250 m × 250 m over the entire TROPOMI pixels they overfly. Thus, airborne data are more correlated with TROPOMI measurements (r2=0.96) than Pandora measurements are with TROPOMI (r2=0.84). The largest outliers between TROPOMI and the reference measurements appear to stem from too spatially coarse a priori surface reflectivity (0.5∘) over bright urban scenes. In this work, this results during cloud-free scenes that, at times, are affected by errors in the TROPOMI cloud pressure retrieval impacting the calculation of tropospheric air mass factors. This factor causes a high bias in TROPOMI TrVCs of 4 %–11 %. Excluding these cloud-impacted points, TROPOMI has an overall low bias of 19 %–33 % during the LISTOS timeframe of June–September 2018. Part of this low bias is caused by coarse a priori profile input from the TM5-MP model; replacing these profiles with those from a 12 km North American Model–Community Multiscale Air Quality (NAMCMAQ) analysis results in a 12 %–14 % increase in the TrVCs. Even with this improvement, the TROPOMI-NAMCMAQ TrVCs have a 7 %–19 % low bias, indicating needed improvement in a priori assumptions in the air mass factor calculation. Future work should explore additional impacts of a priori inputs to further assess the remaining low biases in TROPOMI using these datasets.

The TROPOspheric Monitoring Instrument (TROPOMI) level-2 aerosol layer height (ALH) product has now been released to the general public. This product is retrieved using TROPOMI's measurements of the oxygen A-band, radiative transfer model (RTM) calculations augmented by neural networks and an iterative optimal estimation technique. The TROPOMI ALH product will deliver ALH estimates over cloud-free scenes over the ocean and land that contain aerosols above a certain threshold of the measured UV aerosol index (UVAI) in the ultraviolet region. This paper provides background for the ALH product and explores its quality by comparing ALH estimates to similar quantities derived from spaceborne lidars observing the same scene. The spaceborne lidar chosen for this study is the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission, which flies in formation with NASA's A-train constellation since 2006 and is a proven source of data for studying ALHs. The influence of the surface and clouds is discussed, and the aspects of the TROPOMI ALH algorithm that will require future development efforts are highlighted. A case-by-case analysis of the data from the four selected cases (mostly around the Saharan region with approximately 800 co-located TROPOMI pixels and CALIOP profiles in June and December 2018) shows that ALHs retrieved from TROPOMI using the operational Sentinel-5 Precursor Level-2 ALH algorithm is lower than CALIOP aerosol extinction heights by approximately 0.5 km. Looking at data beyond these cases, it is clear that there is a significant difference when it comes to retrievals over land, where these differences can easily go over 1 km on average.

The Tropospheric Monitoring Instrument (TROPOMI), aboard the Sentinel-5 Precursor (S5P) satellite, launched on 13 October 2017, provides measurements of atmospheric trace gases and of cloud and aerosol properties at an unprecedented spatial resolution of approximately 7×3.5 km2 (approx. 5.5×3.5 km2 as of 6 August 2019), achieving near-global coverage in 1 d. The retrieval of nitrogen dioxide (NO2) concentrations is a three-step procedure: slant column density (SCD) retrieval, separation of the SCD in its stratospheric and tropospheric components, and conversion of these into vertical column densities. This study focusses on the TROPOMI NO2 SCD retrieval: the retrieval method used, the stability of the SCDs and the SCD uncertainties, and a comparison with the Ozone Monitoring Instrument (OMI) NO2 SCDs. The statistical uncertainty, based on the spatial variability of the SCDs over a remote Pacific Ocean sector, is 8.63 µmol m−2 for all pixels (9.45 µmol m−2 for clear-sky pixels), which is very stable over time and some 30 % less than the long-term average over OMI–QA4ECV data (since the pixel size reduction TROPOMI uncertainties are ∼8 % larger). The SCD uncertainty reported by the differential optical absorption spectroscopy (DOAS) fit is about 10 % larger than the statistical uncertainty, while for OMI–QA4ECV the DOAS uncertainty is some 20 % larger than its statistical uncertainty. Comparison of the SCDs themselves over the Pacific Ocean, averaged over 1 month, shows that TROPOMI is about 5 % higher than OMI–QA4ECV, which seems to be due mainly to the use of the so-called intensity offset correction in OMI–QA4ECV but not in TROPOMI: turning that correction off means about 5 % higher SCDs. The row-to-row variation in the SCDs of TROPOMI, the “stripe amplitude”, is 2.15 µmol m−2, while for OMI–QA4ECV it is a factor of ∼2 (∼5) larger in 2005 (2018); still, a so-called stripe correction of this non-physical across-track variation is useful for TROPOMI data. In short, TROPOMI shows a superior performance compared with OMI–QA4ECV and operates as anticipated from instrument specifications. The TROPOMI data used in this study cover 30 April 2018 up to 31 January 2020.

To retrieve aerosol properties from satellite measurements of the oxygen A-band in the near-infrared, a line-by-line radiative transfer model implementation requires a large number of calculations. These calculations severely restrict a retrieval algorithm's operational capability as it can take several minutes to retrieve the aerosol layer height for a single ground pixel. This paper proposes a forward modelling approach using artificial neural networks to speed up the retrieval algorithm. The forward model outputs are trained into a set of neural network models to completely replace line-by-line calculations in the operational processor. Results comparing the forward model to the neural network alternative show an encouraging outcome with good agreement between the two when they are applied to retrieval scenarios using both synthetic and real measured spectra from TROPOMI (TROPOspheric Monitoring Instrument) on board the European Space Agency (ESA) Sentinel-5 Precursor mission. With an enhancement of the computational speed by 3 orders of magnitude, TROPOMI's operational aerosol layer height processor is now able to retrieve aerosol layer heights well within operational capacity.

Global mapping of satellite tropospheric NO2 vertical column density (VCD), a key gas in air quality monitoring, requires accurate retrievals over complex urban and industrialized areas and under any atmospheric conditions. The high abundance of aerosol particles in regions dominated by anthropogenic fossil fuel combustion, e.g. megacities, and/or biomass-burning episodes, affects the space-borne spectral measurement. Minimizing the tropospheric NO2 VCD biases caused by aerosol scattering and absorption effects is one of the main retrieval challenges from air quality satellite instruments. In this study, the reference Ozone Monitoring Instrument (OMI) DOMINO-v2 product was reprocessed over cloud-free scenes, by applying new aerosol correction parameters retrieved from the 477 nm O2−O2 band, over eastern China and South America for 2 years (2006–2007). These new parameters are based on two different and separate algorithms developed during the last 2 years in view of an improved use of the OMI 477 nm O2−O2 band: the updated OMCLDO2 algorithm, which derives improved effective cloud parameters, the aerosol neural network (NN), which retrieves explicit aerosol parameters by assuming a more physical aerosol model. The OMI aerosol NN is a step ahead of OMCLDO2 because it primarily estimates an explicit aerosol layer height (ALH), and secondly an aerosol optical thickness τ for cloud-free observations. Overall, it was found that all the considered aerosol correction parameters reduce the biases identified in DOMINO-v2 over scenes in China with high aerosol abundance dominated by fine scattering and weakly absorbing particles, e.g. from [-20%:-40%] to [0 %:20 %] in summertime. The use of the retrieved OMI aerosol parameters leads in general to a more explicit aerosol correction and higher tropospheric NO2 VCD values, in the range of [0 %:40 %], than from the implicit correction with the updated OMCLDO2. This number overall represents an estimation of the aerosol correction strategy uncertainty nowadays for tropospheric NO2 VCD retrieval from space-borne visible measurements. The explicit aerosol correction theoretically includes a more realistic consideration of aerosol multiple scattering and absorption effects, especially over scenes dominated by strongly absorbing particles, where the correction based on OMCLDO2 seems to remain insufficient. However, the use of ALH and τ from the OMI NN aerosol algorithm is not a straightforward operation and future studies are required to identify the optimal methodology. For that purpose, several elements are recommended in this paper. Overall, we demonstrate the possibility of applying a more explicit aerosol correction by considering aerosol parameters directly derived from the 477 nm O2−O2 spectral band, measured by the same satellite instrument. Such an approach can, in theory, easily be transposed to the new-generation of space-borne instruments (e.g. TROPOMI on board Sentinel-5 Precursor), enabling a fast reprocessing of tropospheric NO2 data over cloud-free scenes (cloudy pixels need to be filtered out), as well as for other trace gas retrievals (e.g. SO2, HCHO).

The absorbing aerosol index (AAI) is a qualitative parameter directly calculated from satellite-measured reflectance. Its sensitivity to absorbing aerosols in combination with a long-term data record since 1978 makes it an important parameter for climate research. In this study, we attempt to quantify aerosol absorption by retrieving the single-scattering albedo (ω0) at 550 nm from the satellite-measured AAI. In the first part of this study, AAI sensitivity studies are presented exclusively for biomass-burning aerosols. Later on, we employ a radiative transfer model (DISAMAR) to simulate the AAI measured by the Ozone Monitoring Instrument (OMI) in order to derive ω0 at 550 nm. Inputs for the radiative transfer calculations include satellite measurement geometry and surface conditions from OMI, aerosol optical thickness (τ) from the Moderate Resolution Imaging Spectroradiometer (MODIS) and aerosol microphysical parameters from the AErosol RObotic NETwork (AERONET), respectively. This approach is applied to the Chile wildfires for the period from 26 to 30 January 2017, when the OMI-observed AAI of this event reached its peak. The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) overpasses missed the evolution of the smoke plume over the research region; therefore the aerosol profile is parameterized. The simulated plume is at an altitude of 4.5–4.9 km, which is in good agreement with available CALIOP backscatter coefficient measurements. The data may contain pixels outside the plume, so an outlier detection criterion is applied. The results show that the AAI simulated by DISAMAR is consistent with satellite observations. The correlation coefficients fall into the range between 0.85 and 0.95. The retrieved mean ω0 at 550 nm for the entire plume over the research period from 26 to 30 January 2017 varies from 0.81 to 0.87, whereas the nearest AERONET station reported ω0 between 0.89 and 0.92. The difference in geolocation between the AERONET site and the plume, the assumption of homogeneous plume properties, the lack of the aerosol profile information and the uncertainties in the inputs for radiative transfer calculation are primarily responsible for this discrepancy in ω0.

This paper presents a weighted least squares approach to retrieve aerosol layer height from top-of-atmosphere reflectance measurements in the oxygen A band (758–770 nm) over bright surfaces. A property of the measurement error covariance matrix is discussed, due to which photons travelling from the surface are given a higher preference over photons that scatter back from the aerosol layer. This is a potential source of biases in the estimation of aerosol properties over land, which can be mitigated by revisiting the design of the measurement error covariance matrix. The alternative proposed in this paper, which we call the dynamic scaling method, introduces a scene-dependent and wavelength-dependent modification in the measurement signal-to-noise ratio in order to influence this matrix. This method is generally applicable to other retrieval algorithms using weighted least squares. To test this method, synthetic experiments are done in addition to application to GOME-2A and GOME-2B measurements of the oxygen A band over the August 2010 Russian wildfires and the October 2017 Portugal wildfire plume over western Europe.

A global picture of atmospheric aerosol vertical distribution with a high temporal resolution is of key importance not only for climate, cloud formation, and air quality research studies but also for correcting scattered radiation induced by aerosols in absorbing trace gas retrievals from passive satellite sensors. Aerosol layer height (ALH) was retrieved from the OMI 477 nm O2 − O2 band and its spatial pattern evaluated over selected cloud-free scenes. Such retrievals benefit from a synergy with MODIS data to provide complementary information on aerosols and cloudy pixels. We used a neural network approach previously trained and developed. Comparison with CALIOP aerosol level 2 products over urban and industrial pollution in eastern China shows consistent spatial patterns with an uncertainty in the range of 462–648 m. In addition, we show the possibility to determine the height of thick aerosol layers released by intensive biomass burning events in South America and Russia from OMI visible measurements. A Saharan dust outbreak over sea is finally discussed. Complementary detailed analyses show that the assumed aerosol properties in the forward modelling are the key factors affecting the accuracy of the results, together with potential cloud residuals in the observation pixels. Furthermore, we demonstrate that the physical meaning of the retrieved ALH scalar corresponds to the weighted average of the vertical aerosol extinction profile. These encouraging findings strongly suggest the potential of the OMI ALH product, and in more general the use of the 477 nm O2 − O2 band from present and future similar satellite sensors, for climate studies as well as for future aerosol correction in air quality trace gas retrievals.

This overview paper highlights the successes of the Ozone Monitoring Instrument (OMI) on board the Aura satellite spanning a period of nearly 14 years. Data from OMI has been used in a wide range of applications and research resulting in many new findings. Due to its unprecedented spatial resolution, in combination with daily global coverage, OMI plays a unique role in measuring trace gases important for the ozone layer, air quality, and climate change. With the operational very fast delivery (VFD; direct readout) and near real-time (NRT) availability of the data, OMI also plays an important role in the development of operational services in the atmospheric chemistry domain.

Retrieving aerosol optical thickness and aerosol layer height over a bright surface from measured top-of-atmosphere reflectance spectrum in the oxygen A band is known to be challenging, often resulting in large errors. In certain atmospheric conditions and viewing geometries, a loss of sensitivity to aerosol optical thickness has been reported in the literature. This loss of sensitivity has been attributed to a phenomenon known as critical surface albedo regime, which is a range of surface albedos for which the top-of-atmosphere reflectance has minimal sensitivity to aerosol optical thickness. This paper extends the concept of critical surface albedo for aerosol layer height retrievals in the oxygen A band, and discusses its implications. The underlying physics are introduced by analysing the top-of-atmosphere reflectance spectrum as a sum of atmospheric path contribution and surface contribution, obtained using a radiative transfer model. Furthermore, error analysis of an aerosol layer height retrieval algorithm is conducted over dark and bright surfaces to show the dependence on surface reflectance. The analysis shows that the derivative with respect to aerosol layer height of the atmospheric path contribution to the top-of-atmosphere reflectance is opposite in sign to that of the surface contribution – an increase in surface brightness results in a decrease in information content. In the case of aerosol optical thickness, these derivatives are anti-correlated, leading to large retrieval errors in high surface albedo regimes. The consequence of this anti-correlation is demonstrated with measured spectra in the oxygen A band from the GOME-2 instrument on board the Metop-A satellite over the 2010 Russian wildfires incident.

The Dutch–Finnish Ozone Monitoring Instrument (OMI) is an imaging spectrograph flying on NASA's EOS Aura satellite since 15 July 2004. OMI is primarily used to map trace-gas concentrations in the Earth's atmosphere, obtaining mid-resolution (0.4–0.6 nm) ultraviolet–visible (UV–VIS; 264–504 nm) spectra at multiple (30–60) simultaneous fields of view. Assessed via various approaches that include monitoring of radiances from selected ocean, land ice and cloud areas, as well as measurements of line profiles in the solar spectra, the instrument shows low optical degradation and high wavelength stability over the mission lifetime. In the regions relatively free from the slowly unraveling row anomaly (RA) the OMI irradiances have degraded by 3–8 %, while radiances have changed by 1–2 %. The long-term wavelength calibration of the instrument remains stable to 0.005–0.020 nm.

This paper presents an exploratory study on the aerosol layer height (ALH) retrieval from the OMI 477 nm O2 − O2 spectral band. We have developed algorithms based on the multilayer perceptron (MLP) neural network (NN) approach and applied them to 3-year (2005–2007) OMI cloud-free scenes over north-east Asia, collocated with MODIS Aqua aerosol product. In addition to the importance of aerosol altitude for climate and air quality objectives, our long-term motivation is to evaluate the possibility of retrieving ALH for potential future improvements of trace gas retrievals (e.g. NO2, HCHO, SO2) from UV–visible air quality satellite measurements over scenes including high aerosol concentrations. This study presents a first step of this long-term objective and evaluates, from a statistic point of view, an ensemble of OMI ALH retrievals over a long time period of 3 years covering a large industrialized continental region. This ALH retrieval relies on the analysis of the O2 − O2 slant column density (SCD) and requires an accurate knowledge of the aerosol optical thickness, τ. Using MODIS Aqua τ(550 nm) as a prior information, absolute seasonal differences between the LIdar climatology of vertical Aerosol Structure for space-based lidar simulation (LIVAS) and average OMI ALH, over scenes with MODIS τ(550 nm) ≥ 1. 0, are in the range of 260–800 m (assuming single scattering albedo ω0 = 0. 95) and 180–310 m (assuming ω0 = 0. 9). OMI ALH retrievals depend on the assumed aerosol single scattering albedo (sensitivity up to 660 m) and the chosen surface albedo (variation less than 200 m between OMLER and MODIS black-sky albedo). Scenes with τ ≤ 0. 5 are expected to show too large biases due to the little impact of particles on the O2 − O2 SCD changes. In addition, NN algorithms also enable aerosol optical thickness retrieval by exploring the OMI reflectance in the continuum. Comparisons with collocated MODIS Aqua show agreements between −0. 02 ± 0. 45 and −0. 18 ± 0. 24, depending on the season. Improvements may be obtained from a better knowledge of the surface albedo and higher accuracy of the aerosol model. Following the previous work over ocean of Park et al.(2016), our study shows the first encouraging aerosol layer height retrieval results over land from satellite observations of the 477 nm O2 − O2 absorption spectral band.

The OMI (Ozone Monitoring Instrument on board NASA's Earth Observing System (EOS) Aura satellite) OMCLDO2 cloud product supports trace gas retrievals of for example ozone and nitrogen dioxide. The OMCLDO2 algorithm derives the effective cloud fraction and effective cloud pressure using a DOAS (differential optical absorption spectroscopy) fit of the O2–O2 absorption feature around 477 nm. A new version of the OMI OMCLDO2 cloud product is presented that contains several improvements, of which the introduction of a temperature correction on the O2–O2 slant columns and the updated look-up tables have the largest impact. Whereas the differences in the effective cloud fraction are on average limited to 0.01, the differences of the effective cloud pressure can be up to 200 hPa, especially at cloud fractions below 0.3. As expected, the temperature correction depends on latitude and season. The updated look-up tables have a systematic effect on the cloud pressure at low cloud fractions. The improvements at low cloud fractions are very important for the retrieval of trace gases in the lower troposphere, for example for nitrogen dioxide and formaldehyde. The cloud pressure retrievals of the improved algorithm are compared with ground-based radar–lidar observations for three sites at mid-latitudes. For low clouds that have a limited vertical extent the comparison yields good agreement. For higher clouds, which are vertically extensive and often contain several layers, the satellite retrievals give a lower cloud height. For high clouds, mixed results are obtained.

The Ozone Monitoring Instrument (OMI) onboard NASA's Aura satellite has been providing global observations of the ozone layer and key atmospheric pollutant gases, such as nitrogen dioxide (NO2) and sulfur dioxide (SO2), since October 2004. The data products from the same instrument provide consistent spatial and temporal coverage and permit the study of anthropogenic and natural emissions on local-to-global scales. In this paper, we examine changes in SO2 and NO2 over some of the world's most polluted industrialized regions during the first decade of OMI observations. In terms of regional pollution changes, we see both upward and downward trends, sometimes in opposite directions for NO2 and SO2, for different study areas. The trends are, for the most part, associated with economic and/or technological changes in energy use, as well as regional regulatory policies. Over the eastern US, both NO2 and SO2 levels decreased dramatically from 2005 to 2015, by more than 40 and 80 %, respectively, as a result of both technological improvements and stricter regulations of emissions. OMI confirmed large reductions in SO2 over eastern Europe's largest coal-fired power plants after installation of flue gas desulfurization devices. The North China Plain has the world's most severe SO2 pollution, but a decreasing trend has been observed since 2011, with about a 50 % reduction in 2012–2015, due to an economic slowdown and government efforts to restrain emissions from the power and industrial sectors. In contrast, India's SO2 and NO2 levels from coal power plants and smelters are growing at a fast pace, increasing by more than 100 and 50 %, respectively, from 2005 to 2015. Several SO2 hot spots observed over the Persian Gulf are probably related to oil and gas operations and indicate a possible underestimation of emissions from these sources in bottom-up emission inventories. Overall, OMI observations have proved valuable in documenting rapid changes in air quality over different parts of the world during last decade. The baseline established during the first 11 years of OMI is indispensable for the interpretation of air quality measurements from current and future satellite atmospheric composition missions.

The Ozone Monitoring Instrument (OMI) has provided daily global measurements of tropospheric NO2 for more than a decade. Numerous studies have drawn attention to the complexities related to measurements of tropospheric NO2 in the presence of aerosols. Fine particles affect the OMI spectral measurements and the length of the average light path followed by the photons. However, they are not explicitly taken into account in the current operational OMI tropospheric NO2 retrieval chain (DOMINO – Derivation of OMI tropospheric NO2) product. Instead, the operational OMI O2 − O2 cloud retrieval algorithm is applied both to cloudy and to cloud-free scenes (i.e. clear sky) dominated by the presence of aerosols. This paper describes in detail the complex interplay between the spectral effects of aerosols in the satellite observation and the associated response of the OMI O2 − O2 cloud retrieval algorithm. Then, it evaluates the impact on the accuracy of the tropospheric NO2 retrievals through the computed Air Mass Factor (AMF) with a focus on cloud-free scenes. For that purpose, collocated OMI NO2 and MODIS (Moderate Resolution Imaging Spectroradiometer) Aqua aerosol products are analysed over the strongly industrialized East China area. In addition, aerosol effects on the tropospheric NO2 AMF and the retrieval of OMI cloud parameters are simulated. Both the observation-based and the simulation-based approach demonstrate that the retrieved cloud fraction increases with increasing Aerosol Optical Thickness (AOT), but the magnitude of this increase depends on the aerosol properties and surface albedo. This increase is induced by the additional scattering effects of aerosols which enhance the scene brightness. The decreasing effective cloud pressure with increasing AOT primarily represents the shielding effects of the O2 − O2 column located below the aerosol layers. The study cases show that the aerosol correction based on the implemented OMI cloud model results in biases between −20 and −40 % for the DOMINO tropospheric NO2 product in cases of high aerosol pollution (AOT ≥ 0.6) at elevated altitude. These biases result from a combination of the cloud model error, used in the presence of aerosols, and the limitations of the current OMI cloud Look-Up-Table (LUT). A new LUT with a higher sampling must be designed to remove the complex behaviour between these biases and AOT. In contrast, when aerosols are relatively close to the surface or mixed with NO2, aerosol correction based on the cloud model results in an overestimation of the DOMINO tropospheric NO2 column, between 10 and 20 %. These numbers are in line with comparison studies between ground-based and OMI tropospheric NO2 measurements in the presence of high aerosol pollution and particles located at higher altitudes. This highlights the need to implement an improved aerosol correction in the computation of tropospheric NO2 AMFs.

An algorithm setup for the operational Aerosol Layer Height product for TROPOMI on the Sentinel-5 Precursor mission is described and discussed, applied to GOME-2A data, and evaluated with lidar measurements. The algorithm makes a spectral fit of reflectance at the O2 A band in the near-infrared and the fit window runs from 758 to 770 nm. The aerosol profile is parameterised by a scattering layer with constant aerosol volume extinction coefficient and aerosol single scattering albedo and with a fixed pressure thickness. The algorithm's target parameter is the height of this layer. In this paper, we apply the algorithm to observations from GOME-2A in a number of systematic and extensive case studies, and we compare retrieved aerosol layer heights with lidar measurements. Aerosol scenes cover various aerosol types, both elevated and boundary layer aerosols, and land and sea surfaces. The aerosol optical thicknesses for these scenes are relatively moderate. Retrieval experiments with GOME-2A spectra are used to investigate various sensitivities, in which particular attention is given to the role of the surface albedo. From retrieval simulations with the single-layer model, we learn that the surface albedo should be a fit parameter when retrieving aerosol layer height from the O2 A band. Current uncertainties in surface albedo climatologies cause biases and non-convergences when the surface albedo is fixed in the retrieval. Biases disappear and convergence improves when the surface albedo is fitted, while precision of retrieved aerosol layer pressure is still largely within requirement levels. Moreover, we show that fitting the surface albedo helps to ameliorate biases in retrieved aerosol layer height when the assumed aerosol model is inaccurate. Subsequent retrievals with GOME-2A spectra confirm that convergence is better when the surface albedo is retrieved simultaneously with aerosol parameters. However, retrieved aerosol layer pressures are systematically low (i.e., layer high in the atmosphere) to the extent that retrieved values no longer realistically represent actual extinction profiles. When the surface albedo is fixed in retrievals with GOME-2A spectra, convergence deteriorates as expected, but retrieved aerosol layer pressures become much higher (i.e., layer lower in atmosphere). The comparison with lidar measurements indicates that retrieved aerosol layer heights are indeed representative of the underlying profile in that case. Finally, subsequent retrieval simulations with two-layer aerosol profiles show that a model error in the assumed profile (two layers in the simulation but only one in the retrieval) is partly absorbed by the surface albedo when this parameter is fitted. This is expected in view of the correlations between errors in fit parameters and the effect is relatively small for elevated layers (less than 100 hPa). If one of the scattering layers is near the surface (boundary layer aerosols), the effect becomes surprisingly large, in such a way that the retrieved height of the single layer is above the two-layer profile. Furthermore, we find that the retrieval solution, once retrieval converges, hardly depends on the starting values for the fit. Sensitivity experiments with GOME-2A spectra also show that aerosol layer height is indeed relatively robust against inaccuracies in the assumed aerosol model, even when the surface albedo is not fitted. We show spectral fit residuals, which can be used for further investigations. Fit residuals may be partly explained by spectroscopic uncertainties, which is suggested by an experiment showing the improvement of convergence when the absorption cross section is scaled in agreement with Butz et al. (2013) and Crisp et al. (2012), and a temperature offset to the a priori ECMWF temperature profile is fitted. Retrieved temperature offsets are always negative and quite large (ranging between −4 and −8 K), which is not expected if temperature offsets absorb remaining inaccuracies in meteorological data. Other sensitivity experiments investigate fitting of stray light and fluorescence emissions. We find negative radiance offsets and negative fluorescence emissions, also for non-vegetated areas, but from the results it is not clear whether fitting these parameters improves the retrieval. Based on the present results, the operational baseline for the Aerosol Layer Height product currently will not fit the surface albedo. The product will be particularly suited for elevated, optically thick aerosol layers. In addition to its scientific value in climate research, anticipated applications of the product for TROPOMI are providing aerosol height information for aviation safety and improving interpretation of the Absorbing Aerosol Index.

An improved nitrogen dioxide (NO2) slant column density retrieval for the Ozone Monitoring Instrument (OMI) in the 405–465 nm spectral region is presented. Since the launch of OMI on board NASA's EOS-Aura satellite in 2004, differential optical absorption spectroscopy (DOAS) retrievals of NO2 slant column densities have been the starting point for the KNMI DOMINO and NASA SP NO2 vertical column data as well as the OMI NO2 data of some other institutes. However, recent intercomparisons between NO2 retrievals from OMI and other UV/Vis and limb spectrometers, as well as ground-based measurements, suggest that OMI stratospheric NO2 is biased high. This study revises and, for the first time, fully documents the OMI NO2 retrieval in detail. The representation of the OMI slit function to convolve high-resolution reference spectra onto the relevant spectral grid is improved. The window used for the wavelength calibration is optimised, leading to much-reduced fitting errors. Ozone and water vapour spectra used in the fit are updated, reflecting the recently improved knowledge of their absorption cross section in the literature. The improved spectral fit also accounts for absorption by the O2–O2 collision complex and by liquid water over clear-water areas. The main changes in the improved spectral fitting result from the updates related to the wavelength calibration: the RMS error of the fit is reduced by 23% and the NO2 slant column by 0.85 × 1015 molec cm−2, independent of latitude, solar zenith angle and NO2 value. Including O2–O2 and liquid water absorption and updating the O3 and water vapour cross-section spectra further reduces NO2 slant columns on average by 0.35 × 1015 molec cm−2, accompanied by a further 9% reduction in the RMS error of the fit. The improved OMI NO2 slant columns are consistent with independent NO2 retrievals from other instruments to within a range that can be explained by photochemically driven diurnal increases in stratospheric NO2 and by small differences in fitting window and approach. The revisions indicate that current OMI NO2 slant columns suffered mostly from an additive positive offset, which is removed by the improved wavelength calibration and representation of the OMI slit function. It is therefore anticipated that the improved NO2 slant columns are most important to retrievals of spatially homogeneous stratospheric NO2 rather than to heterogeneous tropospheric NO2.

We have assessed the sensitivity of the operational Ozone Monitoring Instrument (OMI) ozone profile retrieval algorithm to a number of a priori and radiative transfer assumptions. We studied the effect of stray light correction, surface albedo assumptions and a priori ozone profiles on the retrieved ozone profile. Then, we studied how to modify the algorithm to improve the retrieval of tropospheric ozone. We found that stray light corrections have a significant effect on the retrieved ozone profile but mainly at high altitudes. Surface albedo assumptions, on the other hand, have the largest impact at the lowest layers. Choice of an ozone profile climatology which is used as a priori information has small effects on the retrievals at all altitudes. However, the usage of climatological a priori covariance matrix has a significant effect. Based on these sensitivity tests, we made several modifications to the retrieval algorithm: the a priori ozone climatology was replaced with a new tropopause-dependent climatology, the a priori covariance matrix was calculated from the climatological ozone variability values, and the surface albedo was assumed to be linearly dependent on wavelength in the 311.5–330 nm channel. As expected, we found that the a priori covariance matrix basically defines the vertical distribution of degrees of freedom for a retrieval. Moreover, our case study over Europe showed that the modified version produced over 10% smaller ozone abundances in the troposphere which reduced the systematic overestimation of ozone in the retrieval algorithm and improved correspondence with Infrared Atmospheric Sounding Instrument (IASI) retrievals. The comparison with ozonesonde measurements over North America showed that the operational retrieval performed better in the upper troposphere/lower stratosphere (UTLS), whereas the modified version improved the retrievals in the lower troposphere and upper stratosphere. These comparisons showed that the systematic biases in the OMI ozone profile retrievals are not caused by the a priori information but by some still unidentified problem in the radiative transfer modelling. Instead, the a priori information pushes the systematically wrong ozone profiles towards the true values. The smaller weight of the a priori information in the modified retrieval leads to better visibility of tropospheric ozone structures, because it has a smaller tendency to damp the variability of the retrievals in the troposphere. In summary, the modified retrieval unmasks systematic problems in the radiative transfer/instrument model and is more sensitive to tropospheric ozone variation; that is, it is able to capture the tropospheric ozone morphology better.

Satellite instruments are nowadays successfully utilised for measuring atmospheric aerosol in many applications as well as in research. Therefore, there is a growing need for rigorous error characterisation of the measurements. Here, we introduce a methodology for quantifying the uncertainty in the retrieval of aerosol optical thickness (AOT). In particular, we concentrate on two aspects: uncertainty due to aerosol microphysical model selection and uncertainty due to imperfect forward modelling. We apply the introduced methodology for aerosol optical thickness retrieval of the Ozone Monitoring Instrument (OMI) on board NASA's Earth Observing System (EOS) Aura satellite, launched in 2004. We apply statistical methodologies that improve the uncertainty estimates of the aerosol optical thickness retrieval by propagating aerosol microphysical model selection and forward model error more realistically. For the microphysical model selection problem, we utilise Bayesian model selection and model averaging methods. Gaussian processes are utilised to characterise the smooth systematic discrepancies between the measured and modelled reflectances (i.e. residuals). The spectral correlation is composed empirically by exploring a set of residuals. The operational OMI multi-wavelength aerosol retrieval algorithm OMAERO is used for cloud-free, over-land pixels of the OMI instrument with the additional Bayesian model selection and model discrepancy techniques introduced here. The method and improved uncertainty characterisation is demonstrated by several examples with different aerosol properties: weakly absorbing aerosols, forest fires over Greece and Russia, and Sahara desert dust. The statistical methodology presented is general; it is not restricted to this particular satellite retrieval application.

Peak stratospheric chlorofluorocarbon (CFC) and other ozone depleting substance (ODS) concentrations were reached in the mid- to late 1990s. Detection and attribution of the expected recovery of the stratospheric ozone layer in an atmosphere with reduced ODSs as well as efforts to understand the evolution of stratospheric ozone in the presence of increasing greenhouse gases are key current research topics. These require a critical examination of the ozone changes with an accurate knowledge of the spatial (geographical and vertical) and temporal ozone response. For such an examination, it is vital that the quality of the measurements used be as high as possible and measurement uncertainties well quantified. In preparation for the 2014 United Nations Environment Programme (UNEP)/World Meteorological Organization (WMO) Scientific Assessment of Ozone Depletion, the SPARC/IO3C/IGACO-O3/NDACC (SI2N) Initiative was designed to study and document changes in the global ozone profile distribution. This requires assessing long-term ozone profile data sets in regards to measurement stability and uncertainty characteristics. The ultimate goal is to establish suitability for estimating long-term ozone trends to contribute to ozone recovery studies. Some of the data sets have been improved as part of this initiative with updated versions now available. This summary presents an overview of stratospheric ozone profile measurement data sets (ground and satellite based) available for ozone recovery studies. Here we document measurement techniques, spatial and temporal coverage, vertical resolution, native units and measurement uncertainties. In addition, the latest data versions are briefly described (including data version updates as well as detailing multiple retrievals when available for a given satellite instrument). Archive location information for each data set is also given.

Satellite remote sensing is increasingly being used to monitor air quality over localized sources such as the Canadian oil sands. Following an initial study, significantly low biases have been identified in current NO2 and SO2 retrieval products from the Ozone Monitoring Instrument (OMI) satellite sensor over this location resulting from a combination of its rapid development and small spatial scale. Air mass factors (AMFs) used to convert line-of-sight "slant" columns to vertical columns were re-calculated for this region based on updated and higher resolution input information including absorber profiles from a regional-scale (15 km × 15 km resolution) air quality model, higher spatial and temporal resolution surface reflectivity, and an improved treatment of snow. The overall impact of these new Environment Canada (EC) AMFs led to substantial increases in the peak NO2 and SO2 average vertical column density (VCD), occurring over an area of intensive surface mining, by factors of 2 and 1.4, respectively, relative to estimates made with previous AMFs. Comparisons are made with long-term averages of NO2 and SO2 (2005–2011) from in situ surface monitors by using the air quality model to map the OMI VCDs to surface concentrations. This new OMI-EC product is able to capture the spatial distribution of the in situ instruments (slopes of 0.65 to 1.0, correlation coefficients of >0.9). The concentration absolute values from surface network observations were in reasonable agreement, with OMI-EC NO2 and SO2 biased low by roughly 30%. Several complications were addressed including correction for the interference effect in the surface NO2 instruments and smoothing and clear-sky biases in the OMI measurements. Overall these results highlight the importance of using input information that accounts for the spatial and temporal variability of the location of interest when performing retrievals.

We describe a new algorithm for the retrieval of nitrogen dioxide (NO2) vertical columns from nadir-viewing satellite instruments. This algorithm (SP2) is the basis for the Version 2.1 OMI This algorithm (SP2) is the basis for the Version 2.1 Ozone Monitoring Instrument (OMI) NO2 Standard Product and features a novel method for separating the stratospheric and tropospheric columns. NO2 Standard Product and features a novel method for separating the stratospheric and tropospheric columns. The approach estimates the stratospheric NO2 directly from satellite data without using stratospheric chemical transport models or assuming any global zonal wave pattern. Tropospheric NO2 columns are retrieved using air mass factors derived from high-resolution radiative transfer calculations and a monthly climatology of NO2 profile shapes. We also present details of how uncertainties in the retrieved columns are estimated. The sensitivity of the retrieval to assumptions made in the stratosphere–troposphere separation is discussed and shown to be small, in an absolute sense, for most regions. We compare daily and monthly mean global OMI NO2 retrievals using the SP2 algorithm with those of the original Version 1 Standard Product (SP1) and the Dutch DOMINO product. The SP2 retrievals yield significantly smaller summertime tropospheric columns than SP1, particularly in polluted regions, and are more consistent with validation studies. SP2 retrievals are also relatively free of modeling artifacts and negative tropospheric NO2 values. In a reanalysis of an INTEX-B validation study, we show that SP2 largely eliminates an ~20% discrepancy that existed between OMI and independent in situ springtime NO2 SP1 measurements.

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

We retrieve slant column NO2 from the super-zoom mode of the Ozone Monitoring Instrument (OMI) to explore its utility for understanding NOx emissions and variability. Slant column NO2 is operationally retrieved from OMI (Boersma et al., 2007; Bucsela et al., 2006) with a nadir footprint of 13 × 24 km2, the result of averaging eight detector elements on board the instrument. For 85 orbits in late 2004, OMI reported observations from individual "super-zoom" detector elements (spaced at 13 × 3 km2 at nadir). We assess the spatial response of these individual detector elements in-flight and determine an upper-bound on spatial resolution of 9 km, in good agreement with on-ground calibration (7 km FWHM). We determine the precision of the super-zoom mode to be 2.1 × 1015 molecules cm−2, approximately a factor of √8 lower than an identical retrieval at operational scale as expected if random noise dominates the uncertainty. We retrieve slant column NO2 over the Satpura power plant in India; Seoul, South Korea; Dubai, United Arab Emirates; and a set of large point sources on the Rihand Reservoir in India using differential optical absorption spectroscopy (DOAS). Over these sources, the super-zoom mode of OMI observes variation in slant column NO2 of up to 30 × the instrumental precision within one operational footprint.

We present an improved tropospheric nitrogen dioxide column retrieval algorithm (DOMINO v2.0) for OMI based on better air mass factors (AMFs) and a correction for across-track stripes resulting from calibration errors in the OMI backscattered reflectances. Since October 2004, NO2 retrievals from the Ozone Monitoring Instrument (OMI), a UV/Vis nadir spectrometer onboard NASA's EOS-Aura satellite, have been used with success in several scientific studies focusing on air quality monitoring, detection of trends, and NOx emission estimates. Dedicated evaluations of previous DOMINO tropospheric NO2 retrievals indicated their good quality, but also suggested that the tropospheric columns were susceptible to high biases (by 0–40%), probably because of errors in the air mass factor calculations. Here we update the DOMINO air mass factor approach. We calculate a new look-up table (LUT) for altitude-dependent AMFs based on more realistic atmospheric profile parameters, and include more surface albedo and surface pressure reference points than before. We improve the sampling of the TM4 model, resulting in a priori NO2 profiles that are better mixed throughout the boundary layer. We evaluate the NO2 profiles simulated with the improved TM4 sampling as used in the AMF calculations and show that they are highly consistent with in situ NO2 measurements from aircraft during the INTEX-A and INTEX-B campaigns in 2004 and 2006. Our air mass factor calculations are further updated by the implementation of a high-resolution terrain height and a high-resolution surface albedo climatology based on OMI measurements. Together with a correction for across-track stripes, the overall impact of the improved terrain height and albedo descriptions is modest (2 simulated aloft, where sensitivity to NO2 is higher, and amount to reductions in tropospheric NO2 columns of up to 20% in winter, and 10% in summer over extended polluted areas. We investigate the impact of aerosols on the NO2 retrieval, and based on a comparison of concurrent retrievals of clouds from OMI and aerosols from MODIS Aqua, we find empirical evidence that OMI cloud retrievals are sensitive to the presence of scattering aerosols. It follows that an implicit correction for the effects of aerosols occurs through the aerosol-induced cloud parameters in DOMINO, and we show that such an empirical correction amounts to a 20 %AMF reduction in summer and ±10% changes in winter over the eastern United States.

The spatial and temporal correlations between concurrent satellite observations of aerosol optical thickness (AOT) from the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric columns of nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) from the Ozone Monitoring Instrument (OMI) are used to infer information on the global composition of aerosol particles. When averaging the satellite data over large regions and longer time periods, we find significant correlation between MODIS AOT and OMI trace gas columns for various regions in the world. This shows that these enhanced aerosol and trace gas concentrations originate from common sources, such as fossil fuel combustion, biomass burning, and organic compounds released from the biosphere. This leads us to propose that satellite-inferred AOT to NO2 ratios for regions with comparable photochemical regimes can be used as indicators for the relative regional pollution control of combustion processes. Indeed, satellites observe low AOT to NO2 ratios over the eastern United States and western Europe, and high AOT to NO2 ratios over comparably industrialized regions in eastern Europe and China. Emission databases and OMI SO2 observations over these regions suggest a much stronger sulfur contribution to aerosol formation than over the well-regulated areas of the eastern United States and western Europe. Furthermore, satellite observations show AOT to NO2 ratios are a factor 100 higher over biomass burning regions than over industrialized areas, reflecting the unregulated burning practices with strong primary particle emissions in the tropics compared to the heavily controlled combustion processes in the industrialized Northern Hemisphere. Simulations with a global chemistry transport model (GEOS-Chem) capture most of these variations, although on regional scales significant differences are found. Wintertime aerosol concentrations show strongest correlations with NO2 throughout most of the Northern Hemisphere. During summertime, AOT is often (also) correlated with enhanced HCHO concentrations, reflecting the importance of secondary organic aerosol formation in that season. We also find significant correlations between AOT and HCHO over biomass burning regions, the tropics in general, and over industrialized regions in southeastern Asia. The distinct summertime maximum in AOT (0.4 at 550 nm) and HCHO over the southeastern United States strengthens existing hypotheses that local emissions of volatile organic compounds lead to the formation of secondary organic aerosols there. GEOS-Chem underestimates the AOT over the southeastern United States by a factor of 2, most likely due to too strong precipitation and too low SOA yield in the model.

The Ozone Monitoring Instrument (OMI) is an imaging UV-VIS solar backscatter spectrometer and is designed and used primarily to retrieve trace gases like O3 and NO2 from the measured Earth reflectance spectrum in the UV-visible (270–500 nm). However, also aerosols are an important science target of OMI. The multi-wavelength algorithm is used to retrieve aerosol parameters from OMI spectral reflectance measurements in up to 20 wavelength bands. A Principal Component Analysis (PCA) is performed to quantify the information content of OMI reflectance measurements on aerosols and to assess the capability of the multi-wavelength algorithm to discern various aerosol types. This analysis is applied to synthetic reflectance measurements for desert dust, biomass burning aerosols, and weakly absorbing anthropogenic aerosol with a variety of aerosol optical thicknesses, aerosol layer altitudes, refractive indices and size distributions. The range of aerosol parameters considered covers the natural variability of tropospheric aerosols. This theoretical analysis is performed for a large number of scenarios with various geometries and surface albedo spectra for ocean, soil and vegetation. When the surface albedo spectrum is accurately known and clouds are absent, OMI reflectance measurements have 2 to 4 degrees of freedom that can be attributed to aerosol parameters. This information content depends on the observation geometry and the surface albedo spectrum. An additional wavelength band is evaluated, that comprises the O2-O2 absorption band at a wavelength of 477 nm. It is found that this wavelength band adds significantly more information than any other individual band.

We present a new algorithm for the near-real time retrieval – within 3 h of the actual satellite measurement – of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). The retrieval is based on the combined retrieval-assimilation-modelling approach developed at KNMI for off-line tropospheric NO2 from the GOME and SCIAMACHY satellite instruments. We have adapted the off-line system such that the required a priori information – profile shapes and stratospheric background NO2 – is now immediately available upon arrival (within 80 min of observation) of the OMI NO2 slant columns and cloud data at KNMI. Slant columns for NO2 are retrieved using differential optical absorption spectroscopy (DOAS) in the 405–465 nm range. Cloud fraction and cloud pressure are provided by a new cloud retrieval algorithm that uses the absorption of the O2-O2 collision complex near 477 nm. On-line availability of stratospheric slant columns and NO2 profiles is achieved by running the TM4 chemistry transport model (CTM) forward in time based on forecast ECMWF meteo and assimilated NO2 information from all previously observed orbits. OMI NO2 slant columns, after correction for spurious across-track variability, show a random error for individual pixels of approximately 0.7×1015 molec cm−2. Cloud parameters from OMI's O2-O2 algorithm have similar frequency distributions as retrieved from SCIAMACHY's Fast Retrieval Scheme for Cloud Observables (FRESCO) for August 2006. On average, OMI cloud fractions are higher by 0.011, and OMI cloud pressures exceed FRESCO cloud pressures by 60 hPa. A sequence of OMI observations over Europe in October 2005 shows OMI's capability to track changeable NOx air pollution from day to day in cloud-free situations.