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

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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: 1. the updated OMCLDO2 algorithm, which derives improved effective cloud parameters, 2. 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% V -40%] to [0% V 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% V 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).

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We present a 3-D climatology of the desert dust distribution over South and East Asia derived using CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) data. To distinguish desert dust from total aerosol load we apply a methodology developed in the framework of EARLINET (European Aerosol Research Lidar Network). The method involves the use of the particle linear depolarization ratio and updated lidar ratio values suitable for Asian dust, applied to multiyear CALIPSO observations (January 2007-December 2015). The resulting dust product provides information on the horizontal and vertical distribution of dust aerosols over South and East Asia along with the seasonal transition of dust transport pathways. Persistent high D-AOD (dust aerosol optical depth) values at 532 nm, of the order of 0.6, are present over the arid and semi-arid desert regions. Dust aerosol transport (range, height and intensity) is subject to high seasonality, with the highest values observed during spring for northern China (Taklimakan and Gobi deserts) and during summer over the Indian subcontinent (Thar Desert). Additionally, we decompose the CALIPSO AOD (aerosol optical depth) into dust and non-dust aerosol components to reveal the nondust AOD over the highly industrialized and densely populated regions of South and East Asia, where the non-dust aerosols yield AOD values of the order of 0.5. Furthermore, the CALIPSO-based short-term AOD and D-AOD time series and trends between January 2007 and December 2015 are calculated over South and East Asia and over selected subregions. Positive trends are observed over northwest and east China and the Indian subcontinent, whereas over southeast China trends are mostly negative. The calculated AOD trends agree well with the trends derived from Aqua MODIS (Moderate Resolution Imaging Spectroradiometer), although significant differences are observed over specific regions.

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The main objective of this thesis is to design a new aerosol layer height retrieval in order to improve the operational NO2 retrieval, both in the troposphere, from space-borne instruments for highly polluted events and under cloud-free conditions. This thesis focuses on the exploitation of the OMI satellite measurements acquired in the visible wavelength range (405-490 nm). In addition, we develop numerical methods and tools (e.g. machine learning) in order to support the operational processing of big data amounts from the forthcoming new-generation satellite instruments for air quality and climate research.@en

Sunlight scattering and absorption by aerosols perturb the atmospheric radiation. This brings both scientific and technical challenges to the research community. Aerosols are an important player in the climate system (Boucher et al., IPCC report, Chapter 5: Clouds and aerosols, 2015), and also affect satellite measurements of reflected sunlight. Because long-time series of OMI trace gas observations are so crucial for analysing the air pollution trends between urban and regional scales, the uncertainties due to aerosols must be reduced. While, overall, the horizontal distribution of aerosol optical thickness (AOT) can be relatively well described, uncertainties in aerosol layer height (ALH) significantly contribute to the overall uncertainty. In the absence of clouds, ALH remains the most important error source on the observations of trace gases in the troposphere (e.g. NO2, HCHO, SO2) from UV-Vis air quality space-borne sensors over areas dominated by high AOT (i.e. > 0.5), and absorbing particles (Krotkov et al., 2008; Boersma et al., 2011; Barkley et al., 2012; Hewson et al., 2015; Castellanos et al., 2015; Chimot et al., 2016). Because atmospheric models still have large uncertainties on the vertical distribution of aerosols the use of passive satellite measurements with global coverage, such as OMI, becomes advantageous. We have developed a unique Multilayer Perceptron Neural Network (NN) algorithm (i.e. machine learning) to retrieve ALH from the OMI 477 nm O2-O2 visible absorption band and over cloud-free scenes (Chimot et al., 2017a). This band has high sensitivity to strong aerosol loading and has fewer challenges than other bands (e.g. O2-A). This retrieval approach strongly benefits from a synergy with MODIS as prior AOT information is needed. We will present the evaluation of the OMI ALH performances over cloud-free scenes. A 3-year time series (2005- 2007) over the urban and large industrialized area of north-east China shows accuracy in the range of 260-800 m for scenes with AOT (550 nm) > 0.5 (Chimot et al., 2017a). In addition, comparisons with CALIOP aerosol observations demonstrate a high correlation of the spatial distributions (Chimot et al., 2017b). Furthermore, analyses of biomass burning episodes over South America and Russia suggest the strong potential of UV-visible passive satellite sensors to probe thick smoke layer height (Chimot et al., 2017b). Improvement of these retrievals can be obtained by reducing uncertainties on the assumed aerosol type and surface albedo. Preliminary yearly global maps of OMI aerosol layer height will be shown. Finally, we will discuss how this first development may support the correction of aerosol radiation effect on the retrieved OMI tropospheric NO2 product, a key element of fossil-fuel emissions. This work illustrates the possibility, in the future, to derive a long-time series aerosol layer height with global coverage and to analyse the aerosol radiative effects, over cloud-free scenes, from current and nextgeneration UV-visible satellites: e.g. OMI, TROPOMI on-board Sentinel-5-Precurosr, Sentinel-4, Sentinel-5. Moreover, the proposed machine learning technique is a promising asset for facing the challenge of big satellite data. @en

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.@en

This paper presents an exploratory study on the aerosol layer height (ALH) retrieval from the OMI 477nm 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,. Using MODIS Aqua(550nm) 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(550nm) ≥ 1. 0, are in the range of 260-800m (assuming single scattering albedo 0 Combining double low line 0. 95) and 180-310m (assuming 0 Combining double low line 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 ≤ 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 ± g 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 gO₂ absorption spectral band.

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The ability to monitor air quality and climate from UltraViolet-Visible (UV-Vis) satellite spectral measurements relies on accurate trace gas (e.g. NO2, SO2, HCHO, O3) columns combined with aerosol properties and vertical distribution. In the absence of clouds, the most important error source on the observations of trace gases in the troposphere are aerosols, since their scattering and absorbing properties modify the average light path followed by the detected photons. Large impacts due to their vertical distribution uncertainties remain when retrieving vertical column densities of trace gases from UV-Vis air quality space-borne sensors [Krotkov et al., 2008; Boersma et al., 2011; Barkley et al., 2012; Hewson et al., 2015; Castellanos et al., 2015; Chimot et al., 2016a]. Aerosols and trace gases share, over urban and industrialized areas, similar anthropogenic sources, and their concentrations, as shown by the satellite observations, often present significant correlations [Veefkind et al., 2011]. We have recently developed a Multilayer Perceptron Neural Network (NN) algorithm to retrieve Aerosol Layer Height (ALH) from the OMI 477 nm O2-O2 absorption band [Chimot et al., 2016b]. This algorithm represents aerosols in the troposphere as a single scattering layer defined by its mean altitude and homogeneous optical properties. This algorithm enables the link between the OMI O2-O2 slant column density derived from the 477 nm spectral measurements and the aerosol layer altitude. A prior information about the Aerosol Optical Thickness (AOT) is needed to distinguish the effects due to the amount of fine particles and their altitude. Therefore, the ALH retrieval strongly benefits from a synergy between OMI 477 nm O2-O2 spectral measurements and MODIS AOT product. Aerosol layer heights are currently retrieved with an uncertainty in the range of 260-800 m for scenes with AOT larger than 1. Improvement of these retrievals can be expected by improving assumptions on the aerosol single scattering albedo (impacts up to 600 m on average) and surface albedo (less than 200 m). We will present the results obtained for the first time on 3-year (2005-2007) cloud-free OMI observations over large urban and industrialized areas, in North-East Asia [Chimot et al., 2016b]. Some case studies, depicting the correlation between OMI ALH with collocated CALIPSO aerosol observations over some days of strong pollution in China and wildfires in 2012 in Russia, will also be presented. Finally, we will discuss how this product may be used for an explicit aerosol correction in the retrieval of trace gases from UV-Vis satellite sensor. The focus will be on tropospheric NO2 column, over scenes with a high aerosol loading. @en

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.@en

Numerous studies have drawn attention to the complexities related to the retrievals of tropospheric NO2 columns derived from satellite UltraViolet-Visible (UV-Vis) measurements in the presence of aerosols. Correction for aerosol effects will remain a challenge for the next generation of air quality satellite instruments such as TROPOMI on Sentinel-5 Precursor, Sentinel-4 and Sentinel-5. The Ozone Monitoring Instrument (OMI) instrument has provided daily global measurements of tropospheric NO2 for more than a decade. However, aerosols are not explicitly taken into account in the current operational OMI tropospheric NO2 retrieval chain (DOMINO v2 [Boersma et al., 2011]). Our study analyses 2 approaches for an operational aerosol correction, based on the use of the O2-O2 477 nm band. The 1st approach is the cloud-model based aerosol correction, also named “implicit aerosol correction”, and already used in the operational chain. The OMI O2-O2 cloud retrieval algorithm, based on the Differential Optical Absorption Spectroscopy (DOAS) approach, is applied both to cloudy and to cloud-free scenes with aerosols present. Perturbation of the OMI cloud retrievals over scenes dominated by aerosols has been observed in recent studies led by [Castellanos et al., 2015; Lin et al., 2015; Lin et al., 2014]. We investigated the causes of these perturbations by: (1) confronting the OMI tropospheric NO2, clouds and MODIS AQUA aerosol products; (2) characterizing the key drivers of the aerosol net effects, compared to a signal from clouds, in the UV-Vis spectra. This study has focused on large industrialised areas like East-China, over cloud-free scenes. One of the key findings is the limitation due to the coarse sampling of the employed cloud Look-Up Table (LUT) to convert the results of the applied DOAS fit into effective cloud fraction and pressure. This leads to an underestimation of tropospheric NO2 amount in cases of particles located at elevated altitude. A higher sampling of the variation of O2-O2 SCD and continuum reflectance as a function of effective cloud parameters in case of low effective cloud fraction values is requested for applying an aerosol correction. The updates of the OMI O2-O2 cloud algorithm, based on the scheduled new OMI cloud LUT, will be presented in terms of impacts of the effective cloud retrievals and reduced biases of tropospheric NO2 columns over cloud-free scenes dominated by aerosols in China. A 2nd approach is investigated, assuming a more explicit aerosol correction. Previous analyses pointed out that the O2-O2 spectra contain information about aerosols: the continuum reflectance is primarily constrained by the Aerosol Optical thickness (AOT) while the O2-O2 Slant Column Density (SCD) mostly results from the combination of AOT and aerosols altitude. We have developed a first prototype algorithm allowing to retrieve information about AOT and aerosol altitude from the O2-O2 DOAS fit. We will discuss preliminary sensitivities and the potential accuracy of the associated explicit aerosol correction, without the use of effective cloud parameters. @en