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The UV–Visible Working Group of the Network for the Detection of Atmospheric Composition Changes (NDACC) focuses on the monitoring of air-quality-related stratospheric and tropospheric trace gases in support of trend analysis, satellite validation and model studies. Tropospheric measurements are based on MAX-DOAS-type instruments that progressively emerged in the years 2010 onward. In the interest of improving the overall consistency of the NDACC MAX-DOAS network and facilitating its further extension to the benefit of satellite validation, the ESA initiated, in late 2016, the FRM4DOAS project, which aimed to set up the first centralised data processing system for MAX-DOAS-type instruments. Developed by a consortium of European scientists with proven expertise in measurements, data extraction algorithms and software design specialities, the system has now reached pre-operational status and has demonstrated its ability to deliver a set of quality-controlled atmospheric composition data products with a latency of one day. The processing system has been designed using a highly modular approach, making it easy to integrate new tools or processing updates. It incorporates advanced algorithms selected by community consensus for the retrieval of total ozone, lower tropospheric and stratospheric NO2 vertical profiles and formaldehyde profiles. The ozone and NO2 products are currently generated from a total of 22 stations and delivered daily to the NDACC rapid delivery (RD) repository, with an additional mirroring to the ESA Validation Data Centre (EVDC). Although it is still operated in a pre-operational/demonstrational mode, FRM4DOAS was already used for several validation and science studies, and it was also deployed in support of field campaigns for the validation of the TROPOMI and GEMS satellite missions. It recently went through a CEOS-FRM self-assessment process aiming at assessing the level of maturity of the service in terms of instrumentation, operations, data sampling, metrology and verification. Based on this evaluation, it falls under class C, which is a good rating but also implies that further improvements are needed to reach full compliance with FRM standards, i.e., class A. [ABSTRACT FROM AUTHOR]

We introduce NitroNet, a deep learning model for the prediction of tropospheric NO2 profiles from satellite column measurements. NitroNet is a neural network trained on synthetic NO2 profiles from the regional chemistry and transport model WRF-Chem, which was operated on a European domain for the month of May 2019. This WRF-Chem simulation was constrained by in situ and satellite measurements, which were used to optimize important simulation parameters (e.g. the boundary layer scheme). The NitroNet model receives NO2 vertical column densities (VCDs) from the TROPOspheric Monitoring Instrument (TROPOMI) and ancillary variables (meteorology, emissions, etc.) as input, from which it reproduces NO2 concentration profiles. Training of the neural network is conducted on a filtered dataset, meaning that NO2 profiles showing strong disagreement (>20 %) with colocated TROPOMI column measurements are discarded. We present a first evaluation of NitroNet over a variety of geographical and temporal domains (Europe, the US West Coast, India, and China) and different seasons. For this purpose, we validate the NO2 profiles predicted by NitroNet against satellite, in situ, and MAX-DOAS (Multi-Axis Differential Optical Absorption Spectroscopy) measurements. The training data were previously validated against the same datasets. During summertime, NitroNet shows small biases and strong correlations with all three datasets: a bias of +6.7% and R=0.95 for TROPOMI NO2 VCDs, a bias of -10.5% and R=0.75 for AirBase surface concentrations, and a bias of -34.3% to +99.6% with R=0.83 – 0.99 for MAX-DOAS measurements. In comparison to TROPOMI satellite data, NitroNet even shows significantly lower errors and stronger correlation than a direct comparison with WRF-Chem numerical results. During wintertime considerable low biases arise because the summertime/late-spring training data are not fully representative of all atmospheric wintertime characteristics (e.g. longer NO2 lifetimes). Nonetheless, the wintertime performance of NitroNet is surprisingly good and comparable to that of classic regional chemistry and transport models. NitroNet can demonstrably be used outside the geographic and temporal domain of the training data with only slight performance reductions. What makes NitroNet unique when compared to similar existing deep learning models is the inclusion of synthetic model data, which offers important benefits: due to the lack of NO2 profile measurements, models trained on empirical datasets are limited to the prediction of surface concentrations learned from in situ measurements. NitroNet, however, can predict full tropospheric NO2 profiles. Furthermore, in situ measurements of NO2 are known to suffer from biases, often larger than +20 %, due to cross-sensitivities to photooxidants, which other models trained on empirical data inevitably reproduce. [ABSTRACT FROM AUTHOR]

Since 2011, the Global Energy and Water cycle Exchanges (GEWEX) Water Vapor Assessment (G-VAP) has provided performance analyses for state-of-the-art reanalysis and satellite water vapour products to the GEWEX Data and Analysis Panel (GDAP) and the user community in general. A significant component of the work undertaken by G-VAP is to characterise the quality and uncertainty of these water vapour records to (i) ensure full exploitation and (ii) avoid incorrect use or interpretation of results. This study presents results from the second phase of G-VAP, where we have extended and expanded our analysis of total column water vapour (TCWV) from phase 1, in conjunction with updating the G-VAP archive. For version 2 of the archive, we consider 28 freely available and mature satellite and reanalysis data products, remapped to a regular longitude–latitude grid of 2° × 2° and on monthly time steps between January 1979 and December 2019. We first analysed all records for a "common" short period of 5 years (2005–2009), focusing on variability (spatial and seasonal) and deviation from the ensemble mean. We observed that clear-sky daytime-only satellite products were generally drier than the ensemble mean, and seasonal variability/disparity in several regions up to 12 kg m -2 related to original spatial resolution and temporal sampling. For 11 of the 28 data records, further analysis was undertaken between 1988–2014. Within this "long period", key results show (i) trends between - 1.18 ± 0.68 to 3.82 ± 3.94 kg m -2 per decade and - 0.39 ± 0.27 to 1.24 ± 0.85 kg m -2 per decade were found over ice-free global oceans and land surfaces, respectively, and (ii) regression coefficients of TCWV against surface temperatures of 6.17 ± 0.24 to 27.02 ± 0.51 % K -1 over oceans (using sea surface temperature) and 3.00 ± 0.17 to 7.77 ± 0.16 % K -1 over land (using surface air temperature). It is important to note that trends estimated within G-VAP are used to identify issues in the data records rather than analyse climate change. Additionally, breakpoints have been identified and characterised for both land and ocean surfaces within this period. Finally, we present a spatial analysis of correlations to six climate indices within the long period, highlighting regional areas of significant positive and negative correlation and the level of agreement among records. [ABSTRACT FROM AUTHOR]

We present a new method for estimating NOx emissions and effective lifetimes from large cities based on NO2 measurements from the TROPOspheric Monitoring Instrument (TROPOMI) (PAL dataset, May 2018–November 2021). As in previous studies, the estimate is based on the downwind plume evolution for different wind directions separately. The novelty of the presented approach lies in the simultaneous fit of downwind patterns for opposing wind directions, which makes the method far more robust (i.e., less prone to local minima with nonphysically high or low lifetimes) than a single exponential decay fit. In addition, the new method does not require the assumption of a city being a "point source" but also derives the spatial distribution of emissions. The method was successfully applied to 100 cities worldwide on a seasonal scale. Fitted emissions generally agree reasonably with the Emissions Database for Global Atmospheric Research (EDGAR) v6 (R=0.72) and are on average 14 % lower, while estimated uncertainties are still rather large (≈ 30 %–50 %). Lifetimes were found to be rather short (2.44 ± 0.68 h) and show no distinct dependency on season or latitude, which might be a consequence of discarding observations at high solar zenith angles (>65 °). The main limitations of this and similar methods are the underlying assumptions of steady state (meaning constant emissions, wind fields and chemical conditions) within about 100 km downwind from a city, which is probably a simplification that is too strong in order to reach higher accuracies. [ABSTRACT FROM AUTHOR]

Satellite-derived spatiotemporal patterns of nitrogen oxide (NO x) emissions can improve accuracy of emission inventories to better support air quality and climate research and policy studies. In this study, we develop a new method by coupling the chemical transport Model-Independent SATellite-derived Emission estimation Algorithm for Mixed-sources (MISATEAM) with a divergence method to map high-resolution NO x emissions across US cities using TROPOspheric Monitoring Instrument (TROPOMI) tropospheric nitrogen dioxide (NO 2) retrievals. The accuracy of the coupled method is validated through application to synthetic NO 2 observations from the NASA-Unified Weather Research and Forecasting (NU-WRF) model, with a horizontal spatial resolution of 4 km × 4 km for 33 large and mid-size US cities. Validation reveals excellent agreement between inferred and NU-WRF-provided emission magnitudes (R= 0.99, normalized mean bias, NMB = - 0.01) and a consistent spatial pattern when comparing emissions for individual grid cells (R=0.88±0.06). We then develop a TROPOMI-based database reporting annual emissions for 39 US cities at a horizontal spatial resolution of 0.05° × 0.05° from 2018 to 2021. This database demonstrates a strong correlation (R= 0.90) with the National Emission Inventory (NEI) but reveals some bias (NMB = - 0.24). There are noticeable differences in the spatial patterns of emissions in some cities. Our analysis suggests that uncertainties in TROPOMI-based emissions and potential misallocation of emissions and/or missing sources in bottom-up emission inventories both contribute to these differences. [ABSTRACT FROM AUTHOR]

We present a new method for estimating NOx emissions and effective lifetimes from large cities. As in previous studies, the estimate is based on the downwind plume evolution for different wind directions separately. The novelty of the presented approach lies in the simultaneous fit of downwind patterns for opposing wind directions, which makes the method far more robust (i.e. less prone to local minima with nonphysically high or low lifetimes) than a single exponential decay fit. In addition, the new method does not require the assumption of a city being a 'point source', but derives also the spatial distribution of emissions. The method was successfully applied to 100 cities worldwide on seasonal scale. Fitted emissions generally agree reasonably with EDGAR v6 (R=0.76) and are on average 16 % lower, while estimated uncertainties are still rather large (≈ 30–50 %). Lifetimes were found to be rather short (2.44±0.68 h) and show no distinct dependency on season or latitude, which might be a consequence of discarding observations at high solar zenith angles (>65°). Main limitations of this (and similar) methods are the underlying assumptions of steady state (meaning constant emissions, wind fields and chemical conditions) within about 100 km downwind from a city, which is probably a too strong simplification in order to reach higher accuracies. [ABSTRACT FROM AUTHOR]

We present WRF-Chem simulations over central Europe with a spatial resolution of 3 km × 3 km and focus on nitrogen dioxide (NO2). A regional emission inventory issued by the German Environmental Agency, with a spatial resolution of 1 km × 1 km, is used as input. We demonstrate by comparison of five different model setups that significant improvements in model accuracy can be achieved by choosing the appropriate boundary layer scheme, increasing vertical mixing strength, and/or tuning the temporal modulation of the emission data ("temporal profiles") driving the model. The model setup with improved vertical mixing is shown to produce the best results. Simulated NO2 surface concentrations are compared to measurements from a total of 275 in situ measurement stations in Germany, where the model was able to reproduce average noontime NO2 concentrations with a bias of ca. - 3 % and R=0.74. The best agreement is achieved when correcting for the presumed NOy cross sensitivity of the molybdenum-based in situ measurements by computing an NOy correction factor from modelled peroxyacetyl nitrate (PAN) and nitric acid (HNO3) mixing ratios. A comparison between modelled NO2 vertical column densities (VCDs) and satellite observations from TROPOMI (TROPOspheric Monitoring Instrument) is conducted with averaging kernels taken into account. Simulations and satellite observations are shown to agree with a bias of + 5.5 % and R=0.87 for monthly means. Lastly, simulated NO2 concentration profiles are compared to noontime NO2 profiles obtained from multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements at five locations in Europe. For stations within Germany, average biases of - 25.3 % to + 12.0 % were obtained. Outside of Germany, where lower-resolution emission data were used, biases of up to + 50.7 % were observed. Overall, the study demonstrates the high sensitivity of modelled NO2 to the mixing processes in the boundary layer and the diurnal distribution of emissions. [ABSTRACT FROM AUTHOR]

Since 2011 the Global Energy and Water cycle Exchanges (GEWEX) Water Vapor Assessment (G-VAP) has provided performance analyses for state-of-the-art reanalysis and satellite water vapour products to the GEWEX Data and Analysis Panel (GDAP) and the user community in general. A significant component of the work undertaken by G-VAP is to characterise the quality and uncertainty of these water vapour records to; i) ensure full exploitation and ii) avoid incorrect use or interpretation of results. This study presents results from the second phase of G-VAP, where we have extended and expanded our analysis of Total Column Water Vapour (TCWV) from phase 1, in conjunction with updating the G-VAP archive. For version 2 of the archive, we consider 28 freely available and mature satellite and reanalysis data products, remapped to a regular longitude-latitude grid of 2 × 2, and on monthly time steps between January 1979 and December 2019. We first analysed all records for a 'common' short period of five years (2005-2009), focusing on variability (spatial & seasonal) and deviation from the ensemble mean. We observed that clear-sky daytime-only satellite products were generally drier than the ensemble mean, and seasonal variability/disparity in several regions up to 12 kg/m2 related to original spatial resolution and temporal sampling. For 11 of the 28 data records, further analysis was undertaken between 1988-2014. Within this 'long period', key results show i) trends between -1.18±0.68 to 3.82±3.94 kg/m2/decade and -0.39±0.27 to 1.24±0.85 kg/m2/decade were found over ice-free global oceans and land surfaces respectively, and ii) regression coefficients of TWCV against surface temperatures of 6.17±0.24 to 27.02±0.51 %/K over oceans (using sea surface temperature) and 3.00±0.17 to 7.77±0.16 %/K over land (using surface air temperature). It is important to note that trends estimated within G-VAP are used to identify issues in the data records rather than analyse climate change. Additionally, breakpoints have been identified and characterised for both land and ocean surfaces within this period. Finally, we present a spatial analysis of correlations to six climate indices within the 'long period', highlighting regional areas of significant positive and negative correlation and the level of agreement among records. [ABSTRACT FROM AUTHOR]

Bromine monoxide (BrO) is a key radical in the atmosphere, influencing the chemical state of the atmosphere, most notably the abundance of ozone (O3). O3 depletion caused by the release of bromine has been observed and modeled in polar regions, salt pans, and in particular inside volcanic plumes. Furthermore, the molar ratio of BrO and SO2 – which can be detected simultaneously via spectroscopic measurements using the differential optical absorption spectroscopy (DOAS) method – is a proxy for the magmatic composition of a volcano and potentially an eruption forecast parameter. The detection of BrO in volcanic plumes from satellite spectroscopic observations is limited by the precision and sensitivity of the retrieval, which so far only allowed for the detection of BrO during major eruptions. The unprecedented spatial resolution of up to 3.5km×5.5km and the high signal-to-noise ratio of the TROPOspheric Monitoring Instrument (TROPOMI) on board Sentinel-5 Precursor (S-5P) enable observing and monitoring volcanic bromine release globally even for minor eruptions or even quiescent degassing. In this study, we investigate how far the BrO retrieval can be improved using TROPOMI data and how well BrO can be detected, even in small eruptions and during quiescent volcanic degassing. There are two steps for which improvements in accuracy are investigated and applied: the improvement and quantitative determination of (1) the detection limit of the DOAS BrO column retrieval and (2) the correction of the non-volcanic background BrO signal. First, the DOAS retrieval settings are varied, and their influence on accuracy and precision is investigated with respect to the detection limit and potential systematic influences. Based on these results, we propose a dedicated DOAS evaluation scheme optimized for the detection of BrO in volcanic plumes. For the DOAS retrieval, we propose the use of a large fit window from 323–360 nm , yielding a statistical uncertainty lower by a factor of 1.8 compared to previous BrO DOAS algorithms while not enhancing systematic influences. Second, the effect of the background BrO is reduced by a latitude-dependent empirical correction scheme correlated to cloud information as well as information on the O3 column. Via these improvements, the combined statistical and systematic uncertainties in the resulting BrO vertical column density is on the order of 7×1012moleculescm-2. We present a new and accurate retrieval algorithm of BrO columns from TROPOMI observations which allows for the detection of even slightly enhanced BrO amounts inside minor eruptive plumes of bromine-rich volcanoes. While designed specifically for TROPOMI observations, the retrieval algorithm is in general also applicable to other hyperspectral satellite observations. However, some parts might require adaptation. [ABSTRACT FROM AUTHOR]

Satellite-derived spatiotemporal patterns of nitrogen oxide (NOx) emissions can improve accuracy of emission inventories to better support air quality and climate research and policy studies. In this study, we develop a new method by coupling the chemical transport Model-Independent SATellite-derived Emission estimation Algorithm for Mixed-sources (MISATEAM) with a divergence method to map high-resolution NOx emissions across US cities using TROPOspheric Monitoring Instrument (TROPOMI) tropospheric nitrogen dioxide (NO2) retrievals. The accuracy of the coupled method is validated through application to synthetic NO2 observations from the NASA-Unified Weather Research and Forecasting (NU-WRF) model, with a horizontal spatial resolution of 4 km × 4 km for 33 large and mid-size US cities. Validation reveals excellent agreement between inferred and NU-WRF-provided emission magnitudes (R = 0.99, Normalized Mean Bias, NMB = −0.01) and a consistent spatial pattern when comparing emissions for individual grid cells (R = 0.88 ± 0.06). We then develop a TROPOMI-based database reporting annual emissions for 39 US cities at a horizontal spatial resolution of 0.05° × 0.05° from 2018 to 2021. This database demonstrates a strong correlation (R = 0.90) with the national emission inventory (NEI) but reveals some bias (NMB = −0.24). There are noticeable differences in the spatial patterns of emissions in some cities, which suggests potential misallocation of emissions and/or missing sources in bottom-up emission inventories. [ABSTRACT FROM AUTHOR]

Satellite-derived spatiotemporal patterns of nitrogen oxide (NOx) emissions can improve accuracy of emission inventories to better support air quality and climate research and policy studies. In this study, we develop a new method by coupling the chemical transport Model-Independent SATellite-derived Emission estimation Algorithm for Mixed-sources (MISATEAM) with a divergence method to map high-resolution NOx emissions across US cities using TROPOspheric Monitoring Instrument (TROPOMI) tropospheric nitrogen dioxide (NO2) retrievals. The accuracy of the coupled method is validated through application to synthetic NO2 observations from the NASA-Unified Weather Research and Forecasting (NU-WRF) model, with a horizontal spatial resolution of 4 km × 4 km for 33 large and mid-size US cities. Validation reveals excellent agreement between inferred and NU-WRF-provided emission magnitudes (R = 0.99, Normalized Mean Bias, NMB = −0.01) and a consistent spatial pattern when comparing emissions for individual grid cells (R = 0.88 ± 0.06). We then develop a TROPOMI-based database reporting annual emissions for 39 US cities at a horizontal spatial resolution of 0.05° × 0.05° from 2018 to 2021. This database demonstrates a strong correlation (R = 0.90) with the national emission inventory (NEI) but reveals some bias (NMB = −0.24). There are noticeable differences in the spatial patterns of emissions in some cities, which suggests potential misallocation of emissions and/or missing sources in bottom-up emission inventories. [ABSTRACT FROM AUTHOR]

We present a long-term data set of 1∘×1∘ monthly mean total column water vapour (TCWV) based on global measurements of the Ozone Monitoring Instrument (OMI) covering the time range from January 2005 to December 2020. In comparison to the retrieval algorithm of , several modifications and filters have been applied accounting for instrumental issues (such as OMI's "row anomaly") or the inferior quality of solar reference spectra. For instance, to overcome issues related to low-quality reference spectra, the daily solar irradiance spectrum is replaced by an annually varying mean earthshine radiance obtained in December over Antarctica. For the TCWV data set, we only consider measurements with an effective cloud fraction less than 20 %, an air mass factor (AMF) greater than 0.1, a snow- and ice-free ground pixel, and an OMI row that is not affected by the row anomaly over the complete time range of the data set. The individual TCWV measurements are then gridded to a regular 1∘×1∘ lattice, from which the monthly means are calculated. The investigation of sampling errors in the OMI TCWV data set shows that these are dominated by the clear-sky bias and cause on average deviations of around - 10 %, which is consistent with the findings of previous studies. However, the spatiotemporal sampling errors and those due to the row-anomaly filter are negligible. In a comprehensive intercomparison study, we demonstrate that the OMI TCWV data set is in good agreement with the global reference data sets of ERA5 (fifth-generation ECMWF atmospheric reanalysis), RSS SSM/I (Remote Sensing Systems Special Sensor Microwave Imager), and CM SAF/CCI TCWV-global (COMBI): over ocean the orthogonal distance regressions indicate slopes close to unity with very small offsets and high coefficients of determination of around 0.96. However, over land, distinctive positive deviations of more than + 10 kg m -2 are obtained for high TCWV values. These overestimations are mainly due to extreme overestimations of high TCWV values in the tropics, likely caused by uncertainties in the retrieval input data (surface albedo, cloud information) due to frequent cloud contamination in these regions. Similar results are found from intercomparisons with in situ radiosonde measurements from version 2 of the Integrated Global Radiosonde Archive (IGRA2) data set. Nevertheless, for TCWV values smaller than 25 kg m -2 , the OMI TCWV data set shows very good agreement with the global reference data sets. Furthermore, a temporal stability analysis proves that the OMI TCWV data set is consistent with the temporal changes in the reference data sets and shows no significant deviation trends. As the TCWV retrieval can be easily applied to further satellite missions, additional TCWV data sets can be created from past missions, such as the Global Ozone Monitoring Experiment-1 (GOME-1) or the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY); under consideration of systematic differences (e.g. due to different observation times), these data sets can be combined with the OMI TCWV data set in order to create a data record that would cover a time span from 1995 to the present. Moreover, the TCWV retrieval will also work for all missions dedicated to NO2 in the future, such as Sentinel-5 on MetOp-SG. The Max Planck Institute for Chemistry (MPIC) OMI total column water vapour (TCWV) climate data record (CDR) is available at 10.5281/zenodo.7973889. [ABSTRACT FROM AUTHOR]