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We present the first global glyoxal (CHOCHO) tropospheric column product derived from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor satellite. Atmospheric glyoxal results from the oxidation of other non-methane volatile organic compounds (NMVOCs) and from direct emissions caused by combustion processes. Therefore, this product is a useful indicator of VOC emissions. It is generated with an improved version of the BIRA-IASB scientific retrieval algorithm relying on the differential optical absorption spectroscopy (DOAS) approach. Among the algorithmic updates, the DOAS fit now includes corrections to mitigate the impact of spectral misfits caused by scene brightness inhomogeneity and strong NO2 absorption. The product comes along with a full error characterization, which allows for providing random and systematic error estimates for every observation. Systematic errors are typically in the range of 1 ×1014–3 ×1014 molec. cm−2 (∼30 %–70 % in emission regimes) and originate mostly from a priori data uncertainties and spectral interferences with other absorbing species. The latter may be at the origin, at least partly, of an enhanced glyoxal signal over equatorial oceans, and further investigation is needed to mitigate them. Random errors are large (>6×1014 molec. cm−2) but can be reduced by averaging observations in space and/or time. Benefiting from a high signal-to-noise ratio and a large number of small-size observations, TROPOMI provides glyoxal tropospheric column fields with an unprecedented level of detail. Using the same retrieval algorithmic baseline, glyoxal column data sets are also generated from the Ozone Monitoring Instrument (OMI) on Aura and from the Global Ozone Monitoring Experiment-2 (GOME-2) on board Metop-A and Metop-B. Those four data sets are intercompared over large-scale regions worldwide and show a high level of consistency. The satellite glyoxal columns are also compared to glyoxal columns retrieved from ground-based Multi-AXis DOAS (MAX-DOAS) instruments at nine stations in Asia and Europe. In general, the satellite and MAX-DOAS instruments provide consistent glyoxal columns both in terms of absolute values and variability. Correlation coefficients between TROPOMI and MAX-DOAS glyoxal columns range between 0.61 and 0.87. The correlation is only poorer at one mid-latitude station, where satellite data appear to be biased low during wintertime. The mean absolute glyoxal columns from satellite and MAX-DOAS generally agree well for low/moderate columns with differences of less than 1×1014 molec. cm−2. A larger bias is identified at two sites where the MAX-DOAS columns are very large. Despite this systematic bias, the consistency of the satellite and MAX-DOAS glyoxal seasonal variability is high.

Since May 2017 and August 2018, two ground-based MAX-DOAS (multi-axis differential optical absorption spectroscopy) instruments have been continuously recording daytime spectral UV–visible measurements in the northwest (University of Natural Resources and Life Sciences (BOKU) site) and south (Arsenal site), respectively, of the Vienna city center (Austria). In this study, vertical aerosol extinction (AE) profiles, aerosol optical depth (AOD), and near-surface AE are retrieved from MAX-DOAS measurements recorded on cloud-free days applying the Bremen Optimal estimation REtrieval for Aerosols and trace gaseS (BOREAS) algorithm. Measurements of atmospheric profiles of pressure and temperature obtained from routinely performed sonde ascents are used to calculate box-air-mass factors and weighting functions for different seasons. The performance of BOREAS was evaluated against co-located ceilometer, sun photometer, and in situ instrument observations covering all four seasons. The results show that the vertical AE profiles retrieved from the BOKU UV–visible MAX-DOAS observations are in very good agreement with data from the co-located ceilometer, reaching correlation coefficients (R) of 0.936–0.996 (UV) and 0.918–0.999 (visible) during the fall, winter, and spring seasons. Moreover, AE extracted using the lowest part of MAX-DOAS vertical profiles (up to 100 m above ground) is highly consistent with near-surface ceilometer AE (R>0.865 and linear regression slopes of 0.815–1.21) during the fall, winter, and spring seasons. A strong correlation is also found for the BOREAS-based AODs when compared to the AERONET ones. Notably, the highest correlation coefficients (R=0.953 and R=0.939 for UV and visible, respectively) were identified for the fall season. While high correlation coefficients are generally found for the fall, winter, and spring seasons, the results are less reliable for measurements taken during summer. For the first time, the spatial variability of AOD and near-surface AE over the urban environment of Vienna is assessed by analyzing the retrieved and evaluated BOREAS aerosol profiling products in terms of different azimuth angles of the two MAX-DOAS instruments and for different seasons. We found that the relative differences of averaged AOD between different azimuth angles are 7–13 %, depending on the season. Larger relative differences of up to 32 % are found for near-surface AE in the different azimuthal directions. This study revealed the strong capability of BOREAS to retrieve AE profiles, AOD, and near-surface AE over urban environments and demonstrated its use for identifying the spatial variability of aerosols in addition to the temporal variation.

In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97∘ N, 4.93∘ E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen collision complex (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region, and NO2 in an additional (smaller) wavelength range in the visible region. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in a unique set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the selected reference (which is obtained from the median of either all data sets or a subset), and the rms error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the consistency between all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques.

We present different methods for in-field elevation calibration of MAX-DOAS (Multi AXis Differential Optical Absorption Spectroscopy) instruments that were applied and inter-compared during the second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2). One necessary prerequisite of consistent MAX-DOAS retrievals is a precise and accurate calibration of the elevation angles of the different measuring systems. Therefore, different methods for this calibration were applied to several instruments during the campaign, and the results were inter-compared. This work first introduces and explains the different methods, namely far- and near-lamp measurements, white-stripe scans, horizon scans and sun scans, using data and results for only one (mainly the Max Planck Institute for Chemistry) instrument. In the second part, the far-lamp measurements and the horizon scans are examined for all participating groups. Here, the results for both methods are first inter-compared for the different instruments; secondly, the two methods are compared amongst each other. All methods turned out to be well-suited for the calibration of the elevation angles of MAX-DOAS systems, with each of them having individual advantages and drawbacks. Considering the results of this study, the systematic uncertainties of the methods can be estimated as ±0.05∘ for the far-lamp measurements and the sun scans, ±0.25∘ for the horizon scans, and around ±0.1∘ for the white-stripe and near-lamp measurements. When comparing the results of far-lamp and horizon-scan measurements, a spread of around 0.9∘ in the elevation calibrations is found between the participating instruments for both methods. This spread is of the order of a typical field of view (FOV) of a MAX-DOAS instrument and therefore affecting the retrieval results. Further, consistent (wavelength dependent) offsets of 0.32∘ and 0.40∘ between far-lamp measurements and horizon scans are found, which can be explained by the fact that, despite the flat topography around the measurement site, obstacles such as trees might mark the visible horizon during daytime. The observed wavelength dependence can be explained by surface albedo effects. Lastly, the results are discussed and recommendations for future campaigns are given.

A novel imaging-DOAS (differential optical absorption spectroscopy) instrument IMPACT (Imaging MaPper for AtmospheriC observaTions) is presented combining full-azimuthal pointing (360∘) with a large vertical coverage (∼41∘). Complete panoramic scans are acquired at a temporal resolution of ∼15 min, enabling the retrieval of NO2 vertical profiles over the entire panorama around the measurement site. IMPACT showed excellent agreement (correlation >99 %) with coincident multiaxis DOAS (MAX-DOAS) measurements during the Second Cabauw Intercomparison of Nitrogen Dioxide measuring Instruments (CINDI-2) campaign. The temporal variability of NO2 slant columns within a typical MAX-DOAS vertical scanning sequence could be resolved and was as large as 20 % in a case study under good viewing conditions. The variation of corresponding profiles and surface concentrations was even larger (40 %). This variability is missed when retrieving trace gas profiles based on standard MAX-DOAS measurements. The azimuthal distribution of NO2 around the measurement site showed inhomogeneities (relative differences) up to 120 % (on average 35 %) on short timescales (individual panoramic scans). This is more than expected for the semirural location. We explain this behavior by the transport of pollution. Exploiting the instrument's advantages, the plume's trajectory during a prominent transport event could be reconstructed. Finally, the potential for retrieving information about the aerosol phase function from O4 slant columns along multiple almucantar scans of IMPACT is demonstrated, with promising results for future studies.

Nitrogen dioxide (NO2), produced as a result of fossil fuel combustion, biomass burning, lightning, and soil emissions, is a key urban and rural tropospheric pollutant. In this case study, ground-based remote sensing has been coupled with the in situ network in Vienna, Austria, to investigate NO2 distributions in the planetary boundary layer. Near-surface and path-averaged NO2 mixing ratios within the metropolitan area of Vienna are estimated from car DOAS (differential optical absorption spectroscopy) zenith-sky and tower DOAS horizon observations. The latter configuration is innovative in the sense that it obtains horizontal measurements at more than a hundred different azimuthal angles – within a 360∘ rotation taking less than half an hour. Spectral measurements were made with a DOAS instrument on nine days in April, September, October, and November 2015 in the zenith-sky mode and on five days in April and May 2016 in the off-axis mode. The analysis of tropospheric NO2 columns from the car measurements and O4 normalized NO2 path averages from the tower observations provide interesting insights into the spatial and temporal NO2 distribution over Vienna. Integrated column amounts of NO2 from both DOAS-type measurements are converted into mixing ratios by different methods. The estimation of near-surface NO2 mixing ratios from car DOAS tropospheric NO2 vertical columns is based on a linear regression analysis including mixing height and other meteorological parameters that affect the dilution and reactivity in the planetary boundary layer – a new approach for such conversion. Path-averaged NO2 mixing ratios are calculated from tower DOAS NO2 slant column densities by taking into account topography and geometry. Overall, lap averages of near-surface NO2 mixing ratios obtained from car DOAS zenith-sky measurements, around a circuit in Vienna, are in the range of 3.8 to 26.1 ppb and in good agreement with values obtained from in situ NO2 measurements for days with wind from the southeast. Path-averaged NO2 mixing ratios at 160 m above the ground as derived from the tower DOAS measurements are between 2.5 and 9 ppb on two selected days with different wind conditions and pollution levels and show similar spatial distribution as seen in the car DOAS zenith-sky observations. We conclude that the application of the two methods to obtain near-surface and path-averaged NO2 mixing ratios is promising for this case study.

In this study, mixing ratios of NO2 (XNO2) and HCHO (XHCHO) in the free troposphere are derived from two multi-axis differential optical absorption spectroscopy (MAX-DOAS) data sets collected at Zugspitze (2650 m a.s.l., Germany) and Pico Espejo (4765 m a.s.l., Venezuela). The estimation of NO2 and HCHO mixing ratios is based on the modified geometrical approach, which assumes a single-scattering geometry and a scattering point altitude close to the instrument altitude. Firstly, the horizontal optical path length (hOPL) is obtained from O4 differential slant column densities (DSCDs) in the horizontal (0°) and vertical (90°) viewing directions. Secondly, XNO2 and XHCHO are estimated from the NO2 and HCHO DSCDs at the 0° and 90° viewing directions and averaged along the obtained hOPLs. As the MAX-DOAS instrument was performing measurements in the ultraviolet region, wavelength ranges of 346–372 and 338–357 nm are selected for the DOAS analysis to retrieve NO2 and HCHO DSCDs, respectively. In order to compare the measured O4 DSCDs and moreover to perform some sensitivity tests, the radiative transfer model SCIATRAN with adapted altitude settings for mountainous terrain is operated to simulate synthetic spectra, on which the DOAS analysis is also applied. The overall agreement between measured and synthetic O4 DSCDs is better for the higher Pico Espejo station than for Zugspitze. Further sensitivity analysis shows that a change in surface albedo (from 0.05 to 0.7) can influence the O4 DSCDs, with a larger absolute difference observed for the horizontal viewing direction. Consequently, the hOPL can vary by about 5 % throughout the season, for example when winter snow cover fully disappears in summer. Typical values of hOPLs during clear-sky conditions are 19 km (14 km) at Zugspitze and 34 km (26.5 km) at Pico Espejo when using the 346–372 (338–357 nm) fitting window. The estimated monthly values of XNO2 (XHCHO), averaged over these hOPLs during clear-sky conditions, are in the range of 60–100 ppt (500–950 ppt) at Zugspitze and 8.5–15.5 ppt (255–385 ppt) at Pico Espejo. Interestingly, multi-year-averaged monthly means of XNO2 and XHCHO increase towards the end of the dry season at the Pico Espejo site, suggesting that both trace gases are frequently lifted above the boundary layer as a result of South American biomass burning.

Satellite observations from the SCIAMACHY, GOME-2 and OMI spectrometers have been used to retrieve atmospheric columns of glyoxal (CHOCHO) with the DOAS method. High CHOCHO levels were found over regions with large biogenic and pyrogenic emissions, and hot-spots have been identified over areas of anthropogenic activities. This study focuses on the development of an improved retrieval for CHOCHO from measurements by the OMI instrument. From sensitivity tests, a fitting window and a polynomial degree are determined. Two different approaches to reduce the interference of liquid water absorption over oceanic regions are evaluated, achieving significant reduction of the number of negative columns over clear water regions. The impact of using different absorption cross-sections for water vapour is evaluated and only small differences are found. Finally, a high-temperature (boundary layer ambient: 294 K) absorption cross-section of nitrogen dioxide (NO2) is introduced in the DOAS retrieval to account for potential interferences of NO2 over regions with large anthropogenic emissions, leading to improved fit quality over these areas. A comparison with vertical CHOCHO columns retrieved from GOME-2 and SCIAMACHY measurements over continental regions is performed, showing overall good consistency. However, SCIAMACHY CHOCHO columns are systematically higher than those obtained from the other instruments. Using the new OMI CHOCHO data set, the link between fires and glyoxal columns is investigated for two selected regions in Africa. In addition, mapped averages are computed for a fire event in Russia between mid-July and mid-August 2010. In both cases, enhanced CHOCHO levels are found in close spatial and temporal proximity to elevated levels of MODIS fire radiative power, demonstrating that pyrogenic emissions can be clearly identified in the new OMI CHOCHO product.

Nitrogen oxides (NOx) play key roles in atmospheric chemistry, air pollution, and climate. While the largest fraction of these reactive gases is released by anthropogenic emission sources, a significant amount can be attributed to vegetation fires. In this study, NO2 from GOME-2 on board EUMETSAT's MetOp-A and OMI on board NASA's Aura as well as fire radiative power (FRP) from the measurements of MODIS on board NASA's Terra and Aqua satellites are used to derive fire emission rates (FERs) of NOx for different types of vegetation using a simple statistical approach. Monthly means of tropospheric NO2 vertical columns (TVC NO2) have been analyzed for their temporal correlation with the monthly means of FRP for five consecutive years from 2007 to 2011 on a horizontal 1° × 1° grid. The strongest correlation is found to be largely confined to tropical and subtropical regions, which account for more than 80% of yearly burned area, on average, globally. In these regions, the seasonal variation of fire intensity, expressed by the FRP data, is similar to the pattern of TVC NO2. As chemical models typically require values for the amount of NOx being released as a function of time, we have converted the retrieved TVC NO2 into production rates of NOx from fire (Pf) by assuming a constant lifetime of NOx. The comparison between Pf and NOx emissions from the Global Fire Emissions Database (GFEDv3.1) over 5 characteristic biomass burning regions in the tropics and subtropics shows good agreement. By separating the monthly means of Pf and FRP according to land cover type, FERs of NOx could be derived for different biomes. The estimated FERs for the dominating types of vegetation burned are lowest for open shrublands and savannas (0.28–1.03 g NOx s−1 MW−1) and highest for croplands and woody savannas (0.82–1.56 g NOx s−1 MW−1). This analysis demonstrates that the strong empirical relationship between TVC NO2 and FRP and the following simplified assumptions are a useful tool for the characterization of NOx emission rates from vegetation fires in the tropics and subtropics. Possible factors affecting the magnitude of the obtained values are discussed.

The aim of this study is to investigate the influence of the spatial resolution of a digital elevation map (DEM) on the three-dimensional (3-D) radiative transfer performance for both spectral ultraviolet (UV) irradiance and actinic flux at 305 nm. Model simulations were performed for clear sky conditions for three case studies: the first and second one using three sites in the Innsbruck area and the third one using three sites at the Sonnblick observatory and surrounding area. It was found that the DEM resolution may change the altitude at some locations by up to 500 m, resulting in changes in the sky obscured by the horizon of up to 15%. The geographical distribution of UV irradiance and actinic flux shows that with larger pixel size, uncertainties in UV irradiance and actinic flux determination of up to 100% are possible. These large changes in incident irradiance and actinic flux with changing pixel size are strongly connected to shading effects. The effect of the DEM pixel size on irradiance and actinic flux was studied at the six locations, and it was found that significant increases in irradiance and actinic flux with increasing DEM pixel size occurred at one valley location at high solar zenith angles in the Innsbruck area as well as for one steep valley location in the Sonnblick area. This increase in irradiance and actinic flux with increasing DEM resolution is most likely to be connected to shading effects affecting the reflections from the surroundings.