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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.

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.

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.

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.

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.

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.

We present an Observing System Simulation Experiment (OSSE) dedicated to the evaluation of the added value of the Sentinel-4 and Sentinel-5P missions for tropospheric nitrogen dioxide (NO2). Sentinel-4 is a geostationary (GEO) mission covering the European continent, providing observations with high temporal resolution (hourly). Sentinel-5P is a low Earth orbit (LEO) mission providing daily observations with a global coverage. The OSSE experiment has been carefully designed, with separate models for the simulation of observations and for the assimilation experiments and with conservative estimates of the total observation uncertainties. In the experiment we simulate Sentinel-4 and Sentinel-5P tropospheric NO2 columns and surface ozone concentrations at 7 by 7 km resolution over Europe for two 3-month summer and winter periods. The synthetic observations are based on a nature run (NR) from a chemistry transport model (MOCAGE) and error estimates using instrument characteristics. We assimilate the simulated observations into a chemistry transport model (LOTOS-EUROS) independent of the NR to evaluate their impact on modelled NO2 tropospheric columns and surface concentrations. The results are compared to an operational system where only ground-based ozone observations are ingested. Both instruments have an added value to analysed NO2 columns and surface values, reflected in decreased biases and improved correlations. The Sentinel-4 NO2 observations with hourly temporal resolution benefit modelled NO2 analyses throughout the entire day where the daily Sentinel-5P NO2 observations have a slightly lower impact that lasts up to 3–6 h after overpass. The evaluated benefits may be even higher in reality as the applied error estimates were shown to be higher than actual errors in the now operational Sentinel-5P NO2 products. We show that an accurate representation of the NO2 profile is crucial for the benefit of the column observations on surface values. The results support the need for having a combination of GEO and LEO missions for NO2 analyses in view of the complementary benefits of hourly temporal resolution (GEO, Sentinel-4) and global coverage (LEO, Sentinel-5P).

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.

We use the technique of Observing System Simulation Experiments (OSSEs) to quantify the impact of spaceborne carbon monoxide (CO) total column observations from the Sentinel-5 Precursor (S-5P) platform on tropospheric analyses and forecasts. We focus on Europe for the period of northern summer 2003, when there was a severe heat wave episode associated with extremely hot and dry weather conditions. We describe different elements of the OSSE: (i) the nature run (NR), i.e., the truth; (ii) the CO synthetic observations; (iii) the assimilation run (AR), where we assimilate the observations of interest; (iv) the control run (CR), in this study a free model run without assimilation; and (v) efforts to establish the fidelity of the OSSE results. Comparison of the results from AR and the CR, against the NR, shows that CO total column observations from S-5P provide a significant benefit (at the 99 % confidence level) at the surface, with the largest benefit occurring over land in regions far away from emission sources. Furthermore, the S-5P CO total column observations are able to capture phenomena such as the forest fires that occurred in Portugal during northern summer 2003. These results provide evidence of the benefit of S-5P observations for monitoring processes contributing to atmospheric pollution.

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.

We derive annual and seasonal global climatologies of tropospheric NO2 profiles from OMI cloudy observations for the year 2006 using the cloud-slicing method on six pressure levels centered at about 280, 380, 500, 620, 720 and 820 hPa. A comparison between OMI and the TM4 model tropospheric NO2 profiles reveals striking overall similarities, which confer great confidence to the cloud-slicing approach to provide details that pertain to annual as well as seasonal means, along with localized discrepancies that seem to probe into particular model processes. Anomalies detected at the lowest levels can be traced to deficiencies in the model surface emission inventory, at mid-tropospheric levels to convective transport and horizontal advective diffusion, and at the upper tropospheric levels to model lightning NOx production and the placement of deeply transported NO2 plumes such as from the Asian summer monsoon. The vertical information contained in the OMI cloud-sliced NO2 profiles provides a global observational constraint that can be used to evaluate chemistry transport models (CTMs) and guide the development of key parameterization schemes.

We present the new version (v14) of the BIRA-IASB algorithm for the retrieval of formaldehyde (H2CO) columns from spaceborne UV–visible sensors. Applied to OMI measurements from Aura and to GOME-2 measurements from MetOp-A and MetOp-B, this algorithm is used to produce global distributions of H2CO representative of mid-morning and early afternoon conditions. Its main features include (1) a new iterative DOAS scheme involving three fitting intervals to better account for the O2–O2 absorption, (2) the use of earthshine radiances averaged in the equatorial Pacific as reference spectra, and (3) a destriping correction and background normalisation resolved in the across-swath position. For the air mass factor calculation, a priori vertical profiles calculated by the IMAGES chemistry transport model at 09:30 and 13:30 LT are used. Although the resulting GOME-2 and OMI H2CO vertical columns are found to be highly correlated, some systematic differences are observed. Afternoon columns are generally larger than morning ones, especially in mid-latitude regions. In contrast, over tropical rainforests, morning H2CO columns significantly exceed those observed in the afternoon. These differences are discussed in terms of the H2CO column variation between mid-morning and early afternoon, using ground-based MAX-DOAS measurements available from seven stations in Europe, China and Africa. Validation results confirm the capacity of the combined satellite measurements to resolve diurnal variations in H2CO columns. Furthermore, vertical profiles derived from MAX-DOAS measurements in the Beijing area and in Bujumbura are used for a more detailed validation exercise. In both regions, we find an agreement better than 15 % when MAX-DOAS profiles are used as a priori for the satellite retrievals. Finally, regional trends in H2CO columns are estimated for the 2004–2014 period using SCIAMACHY and GOME-2 data for morning conditions, and OMI for early afternoon conditions. Consistent features are observed, such as an increase of the columns in India and central–eastern China, and a decrease in the eastern US and Europe. We find that the higher horizontal resolution of OMI combined with a better sampling and a more favourable illumination at midday allow for more significant trend estimates, especially over Europe and North America. Importantly, in some parts of the Amazonian forest, we observe with both time series a significant downward trend in H2CO columns, spatially correlated with areas affected by deforestation.

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.

A new ozone climatology, based on ozonesonde and satellite measurements, spanning the altitude region between the earth's surface and ~60 km is presented (TpO3 climatology). This climatology is novel in that the ozone profiles are categorized according to calendar month, latitude and local tropopause heights. Compared to the standard latitude–month categorization, this presentation improves the representativeness of the ozone climatology in the upper troposphere and the lower stratosphere (UTLS). The probability distribution of tropopause heights in each latitude–month bin provides additional climatological information and allows transforming/comparing the TpO3 climatology to a standard climatology of zonal mean ozone profiles. The TpO3 climatology is based on high-vertical-resolution measurements of ozone from the satellite-based Stratospheric Aerosol and Gas Experiment II (in 1984 to 2005) and from balloon-borne ozonesondes from 1980 to 2006. The main benefits of the TpO3 climatology are reduced standard deviations on climatological ozone profiles in the UTLS, partial characterization of longitudinal variability, and characterization of ozone profiles in the presence of double tropopauses. The first successful application of the TpO3 climatology as a priori in ozone profile retrievals from Ozone Monitoring Instrument on board the Earth Observing System (EOS) Aura satellite shows an improvement of ozone precision in UTLS of up to 10% compared with the use of conventional climatologies. In addition to being advantageous for use as a priori in satellite retrieval algorithms, the TpO3 climatology might be also useful for validating the representation of ozone in climate model simulations.

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.

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.

Following the launch of several satellite ultraviolet and visible spectrometers including the Ozone Monitoring Instrument (OMI), much has been learned about the global distribution of nitrogen dioxide (NO2). NO2, which is mostly anthropogenic in origin, absorbs solar radiation at ultraviolet and visible wavelengths. We parameterized NO2 absorption for fast radiative transfer calculations. Using this parameterization with cloud, surface, and NO2 information from different sensors in the NASA A-train constellation of satellites and NO2 profiles from the Global Modeling Initiative (GMI), we compute the global distribution of net atmospheric heating (NAH) due to tropospheric NO2 for January and July 2005. The globally-averaged NAH values due to tropospheric NO2 are very low: they are about 0.05 W/m2. While the impact of NO2 on the global radiative forcing is small, locally it can produce instantaneous net atmospheric heating of 2–4 W/m2 in heavily polluted areas. We assess the impact of clouds and find that they reduce the globally-averaged NAH values by 5–6% only. However, because most of NO2 is contained in the boundary layer in polluted regions, the cloud shielding effect can significantly reduce the net atmospheric heating due to tropospheric NO2 (up to 50%). We examine the effect of diurnal variations in NO2 emissions and chemistry on net atmospheric heating and find only a small impact of these on the daily-averaged heating (11–14% at the most). We also examine the sensitivity of NO2 absorption to various geophysical conditions. Effects of the vertical distributions of cloud optical depth and NO2 on net atmospheric heating and downwelling radiance are simulated in detail for various scenarios including vertically-inhomogeneous convective clouds observed by CloudSat. The maximum effect of NO2 on downwelling radiance occurs when the NO2 is located in the middle part of the cloud where the optical extinction peaks.

Airborne sunphotometer measurements are used to evaluate retrievals of extinction aerosol optical depth (AOD) from spatially coincident and temporally near-coincident measurements by the Ozone Monitoring Instrument (OMI) aboard the Aura satellite during the March 2006 Megacity Initiative-Local And Global Research Observations/Phase B of the Intercontinental Chemical Transport Experiment (MILAGRO/INTEX-B). The 14-channel NASA Ames Airborne Tracking Sunphotometer (AATS) flew on nine missions over the Gulf of Mexico and four in or near the Mexico City area. Retrievals of AOD from near-coincident AATS and OMI measurements are compared for three flights over the Gulf of Mexico for flight segments when the aircraft flew at altitudes 60–70 m above sea level, and for one flight over the Mexico City area where the aircraft was restricted to altitudes ~320–800 m above ground level over the rural area and ~550–750 m over the city. OMI-measured top of atmosphere (TOA) reflectances are routinely inverted to yield aerosol products such as AOD and aerosol absorption optical depth (AAOD) using two different retrieval algorithms: a near-UV (OMAERUV) and a multiwavelength (OMAERO) technique. This study uses the archived Collection 3 data products from both algorithms. In particular, AATS and OMI AOD comparisons are presented for AATS data acquired in 20 OMAERUV retrieval pixels (15 over water) and 19 OMAERO pixels (also 15 over water). At least four pixels for one of the over-water coincidences and all pixels for the over-land case were cloud-free. Coincident AOD retrievals from 17 pixels of the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard Aqua are available for two of the over-water flights and are shown to agree with AATS AODs to within root mean square (RMS) differences of 0.00–0.06, depending on wavelength. Near-coincident ground-based AOD measurements from ground-based sun/sky radiometers operated as part of the Aerosol Robotic Network (AERONET) at three sites in and near Mexico City are also shown and are generally consistent with the AATS AODs (which exclude any AOD below the aircraft) both in magnitude and spectral dependence. The OMAERUV algorithm retrieves AODs corresponding to a non-absorbing aerosol model for all three over-water comparisons whereas the OMAERO algorithm retrieves best-fit AODs corresponding to an absorbing biomass-burning aerosol model for two of the three over-water cases. For the four cloud-free pixels in one over-water coincidence (10 March), the OMAERUV retrievals underestimate the AATS AODs by ~0.20, which exceeds the expected retrieval uncertainty, but retrieved AODs agree with AATS values within uncertainties for the other two over-water events. When OMAERO retrieves AODs corresponding to a biomass-burning aerosol over water, the values significantly overestimate the AATS AODs (by up to 0.55). For the Mexico City coincidence, comparisons are presented for a non-urban region ~50–70 km northeast of the city and for a site near the center of the city. OMAERUV retrievals are consistent with AERONET AOD magnitudes for the non-urban site, but are nearly double the AATS and AERONET AODs (with differences of up to 0.29) in the center of the city. Corresponding OMAERO retrievals exceed the AATS and/or AERONET AODs by factors of 3 to 10.

Ozone Monitoring Instrument (OMI), launched in July 2004, is dedicated to the monitoring of the Earth's ozone, air quality and climate. OMI is the successor of the Total Ozone Mapping Spectrometer (TOMS) instruments and provides among other atmospheric and radiometric quantities the total column of ozone (TOC), the surface ultraviolet (UV) irradiance at several wavelengths, the erythemal dose rates and the erythemal daily doses. The main objective of this work is to compare OMI data with data from ground-based instruments in order to use OMI products (collection 2) for scientific studies. The Laboratoire d'Optique Atmosphérique (LOA) located in Villeneuve d'Ascq (VdA) in the north of France performs solar UV measurements using a spectroradiometer. The site of Briançon in the French Southern Alps is also equipped with a spectroradiometer operated by Interaction Rayonnement Solaire Atmosphère (IRSA). The OMI total ozone column data is obtained from the OMI-TOMS and OMI-DOAS algorithms. The comparison between the TOC retrieved with ground-based measurements and OMI-TOMS data shows good agreement at both sites for all sky conditions with a relative difference for most of points better than 5%. For OMI-DOAS data, the agreement is generally better than 7% and these data show a significant dependence on solar zenith angle. Comparisons of spectral UV on clear sky conditions are also satisfying with relative differences smaller than 10% except at solar zenith angles larger than 65°. On the contrary, results of comparisons of the erythemal dose rates and erythemal daily doses for clear sky show that OMI overestimates surface UV doses at VdA by about 15% and that on cloudy skies, the bias increases. At Briançon, such a bias is observed if data corresponding to snow-covered surface are excluded.

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.