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  • 1
    Online Resource
    Online Resource
    American Association for the Advancement of Science (AAAS) ; 2019
    In:  Science Advances Vol. 5, No. 11 ( 2019-11)
    In: Science Advances, American Association for the Advancement of Science (AAAS), Vol. 5, No. 11 ( 2019-11)
    Abstract: Satellite observations of nitrogen dioxide (NO 2 ) provide valuable information on the location and strength of NO x emissions, but spatial resolution is limited by horizontal transport and smearing of temporal averages due to changing wind fields. In this study, we map NO x emissions on high spatial resolution from TROPOMI observations of NO 2 combined with wind fields based on the continuity equation. The divergence of horizontal fluxes proves to be highly sensitive for point sources like exhaust stacks. Thus, NO x emissions from individual power plants can be resolved and quantified even on top of considerably high urban pollution from the Saudi Arabian capital city Riyadh. This allows us to catalog NO x emissions from large point sources globally, as demonstrated for South Africa and Germany, with a detection limit of about 0.11 kg/s down to 0.03 kg/s for ideal conditions.
    Type of Medium: Online Resource
    ISSN: 2375-2548
    Language: English
    Publisher: American Association for the Advancement of Science (AAAS)
    Publication Date: 2019
    detail.hit.zdb_id: 2810933-8
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  • 2
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 14, No. 11 ( 2021-11-22), p. 7297-7327
    Abstract: Abstract. Launched in October 2017, the TROPOspheric Monitoring Instrument (TROPOMI) aboard Sentinel-5 Precursor provides the potential to monitor air quality over point sources across the globe with a spatial resolution as high as 5.5 km × 3.5 km (7 km × 3.5 km before 6 August 2019). The DLR nitrogen dioxide (NO2) retrieval algorithm for the TROPOMI instrument consists of three steps: the spectral fitting of the slant column, the separation of stratospheric and tropospheric contributions, and the conversion of the slant column to a vertical column using an air mass factor (AMF) calculation. In this work, an improved DLR tropospheric NO2 retrieval algorithm from TROPOMI measurements over Europe is presented. The stratospheric estimation is implemented using the STRatospheric Estimation Algorithm from Mainz (STREAM), which was developed as a verification algorithm for TROPOMI and does not require chemistry transport model data as input. A directionally dependent STREAM (DSTREAM) is developed to correct for the dependency of the stratospheric NO2 on the viewing geometry by up to 2×1014 molec./cm2. Applied to synthetic TROPOMI data, the uncertainty in the stratospheric column is 3.5×1014 molec./cm2 in the case of significant tropospheric sources. Applied to actual measurements, the smooth variation of stratospheric NO2 at low latitudes is conserved, and stronger stratospheric variation at higher latitudes is captured. For AMF calculation, the climatological surface albedo data are replaced by geometry-dependent effective Lambertian equivalent reflectivity (GE_LER) obtained directly from TROPOMI measurements with a high spatial resolution. Mesoscale-resolution a priori NO2 profiles are obtained from the regional POLYPHEMUS/DLR chemistry transport model with the TNO-MACC emission inventory. Based on the latest TROPOMI operational cloud parameters, a more realistic cloud treatment is provided by a Clouds-As-Layers (CAL) model, which treats the clouds as uniform layers of water droplets, instead of the Clouds-As-Reflecting-Boundaries (CRB) model, in which clouds are simplified as Lambertian reflectors. For the error analysis, the tropospheric AMF uncertainty, which is the largest source of NO2 uncertainty for polluted scenarios, ranges between 20 % and 50 %, leading to a total uncertainty in the tropospheric NO2 column in the 30 %–60 % range. From a validation performed with ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, the new DLR tropospheric NO2 data show good correlations for nine European urban/suburban stations, with an average correlation coefficient of 0.78. The implementation of the algorithm improvements leads to a decrease of the relative difference from −55.3 % to −34.7 % on average in comparison with the DLR reference retrieval. When the satellite averaging kernels are used to remove the contribution of a priori profile shape, the relative difference decreases further to ∼ −20 %.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2505596-3
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  • 3
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Atmospheric Measurement Techniques Vol. 12, No. 3 ( 2019-03-19), p. 1785-1806
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 12, No. 3 ( 2019-03-19), p. 1785-1806
    Abstract: Abstract. The Mainz profile algorithm (MAPA) derives vertical profiles of aerosol extinction and trace gas concentrations from MAX-DOAS measurements of slant column densities under multiple elevation angles. This paper presents (a) a detailed description of the MAPA (v0.98), (b) results for the CINDI-2 campaign, and (c) sensitivity studies on the impact of a priori assumptions such as flag thresholds. Like previous profile retrieval schemes developed at MPIC, MAPA is based on a profile parameterization combining box profiles, which also might be lifted, and exponential profiles. But in contrast to previous inversion schemes based on least-square fits, MAPA follows a Monte Carlo approach for deriving those profile parameters yielding best match to the MAX-DOAS observations. This is much faster and directly provides physically meaningful distributions of profile parameters. In addition, MAPA includes an elaborated flagging scheme for the identification of questionable or dubious results. The AODs derived with MAPA for the CINDI-2 campaign show good agreement with AERONET if a scaling factor of 0.8 is applied for O4, and the respective NO2 and HCHO surface mixing ratios match those derived from coincident long-path DOAS measurements. MAPA results are robust with respect to modifications of the a priori MAPA settings within plausible limits.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2505596-3
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 17 ( 2021-08-31), p. 12867-12894
    Abstract: Abstract. Ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a state-of-the-art remote sensing technique for deriving vertical profiles of trace gases and aerosols. However, MAX-DOAS profile inversions under aerosol pollution scenarios are challenging because of the complex radiative transfer and limited information content of the measurements. In this study, the performances of two inversion algorithms were evaluated for various aerosol pollution scenarios based on synthetic slant column densities (SCDs) derived from radiative transfer simulations. Compared to previous studies, in our study, much larger ranges of aerosol optical depth (AOD) and NO2 vertical column densities (VCDs) are covered. One inversion algorithm is based on optimal estimation; the other uses a parameterized approach. In this analysis, three types of profile shapes for aerosols and NO2 were considered: exponential, Boltzmann, and Gaussian. First, the systematic deviations of the retrieved aerosol profiles from the input profiles were investigated. For most cases, the AODs of the retrieved profiles were found to be systematically lower than the input values, and the deviations increased with increasing AOD. In particular for the optimal estimation algorithm and for high AOD, these findings are consistent with the results in previous studies. The assumed single scattering albedo (SSA) and asymmetry parameter (AP) have a systematic influence on the aerosol retrieval. However, for most cases the influence of the assumed SSA and AP on the retrieval results are rather small (compared to other uncertainties). For the optimal estimation algorithm, the agreement with the input values can be improved by optimizing the covariance matrix of the a priori uncertainties. Second, the aerosol effects on the NO2 profile retrieval were tested. Here, especially for the optimal estimation algorithm, a systematic dependence on the NO2 VCD was found, with a strong relative overestimation of the retrieved results for low NO2 VCDs and an underestimation for high NO2 VCDs. In contrast, the dependence on the aerosol profiles was found to be rather low. Interestingly, the results for both investigated wavelengths (360 and 477 nm) were found to be rather similar, indicating that the differences in the radiative transfer between both wavelengths have no strong effect. In general, both inversion schemes can retrieve the near-surface values of aerosol extinction and trace gas concentrations well.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 14, No. 1 ( 2021-02-01), p. 769-783
    Abstract: Abstract. In urban areas, road traffic is a dominant source of nitrogen oxides (NOx=NO+NO2). Although the emissions from individual vehicles are regulated by the European emission standards, real driving emissions often exceed these limits. In this study, two multi-axis differential optical absorption spectroscopy (MAX-DOAS) instruments on opposite sides of the motorway were used to measure the NO2 absorption caused by road traffic at the A60 motorway close to Mainz, Germany. In combination with wind data, the total NOx emissions for the occurring traffic volume can be estimated. Hereto, the ozone-dependent photochemical equilibrium between NO and NO2 is considered. We show that for 10 May 2019 the measured emissions exceed the maximum expected emissions calculated from the European emission standards for standardised test cycles by a factor of 11±7. One major advantage of the method used here is that MAX-DOAS measurements are very sensitive to the integrated NO2 concentration close to the surface. Thus, all emitted NO2 molecules are detected independently from their altitude, and therefore the whole emission plume originating from the nearby motorway is captured, which is a key advantage compared to other approaches such as in situ measurements.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2505596-3
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 12, No. 5 ( 2019-05-14), p. 2745-2817
    Abstract: Abstract. In this study the consistency between MAX-DOAS measurements and radiative transfer simulations of the atmospheric O4 absorption is investigated on 2 mainly cloud-free days during the MAD-CAT campaign in Mainz, Germany, in summer 2013. In recent years several studies indicated that measurements and radiative transfer simulations of the atmospheric O4 absorption can only be brought into agreement if a so-called scaling factor (〈1) is applied to the measured O4 absorption. However, many studies, including those based on direct sunlight measurements, came to the opposite conclusion, that there is no need for a scaling factor. Up to now, there is no broad consensus for an explanation of the observed discrepancies between measurements and simulations. Previous studies inferred the need for a scaling factor from the comparison of the aerosol optical depths derived from MAX-DOAS O4 measurements with that derived from coincident sun photometer measurements. In this study a different approach is chosen: the measured O4 absorption at 360 nm is directly compared to the O4 absorption obtained from radiative transfer simulations. The atmospheric conditions used as input for the radiative transfer simulations were taken from independent data sets, in particular from sun photometer and ceilometer measurements at the measurement site. This study has three main goals: first all relevant error sources of the spectral analysis, the radiative transfer simulations and the extraction of the input parameters used for the radiative transfer simulations are quantified. One important result obtained from the analysis of synthetic spectra is that the O4 absorptions derived from the spectral analysis agree within 1 % with the corresponding radiative transfer simulations at 360 nm. Based on the results from sensitivity studies, recommendations for optimised settings for the spectral analysis and radiative transfer simulations are given. Second, the measured and simulated results are compared for 2 selected cloud-free days with similar aerosol optical depths but very different aerosol properties. On 18 June, measurements and simulations agree within their (rather large) uncertainties (the ratio of simulated and measured O4 absorptions is found to be 1.01±0.16). In contrast, on 8 July measurements and simulations significantly disagree: for the middle period of that day the ratio of simulated and measured O4 absorptions is found to be 0.82±0.10, which differs significantly from unity. Thus, for that day a scaling factor is needed to bring measurements and simulations into agreement. Third, recommendations for further intercomparison exercises are derived. One important recommendation for future studies is that aerosol profile data should be measured at the same wavelengths as the MAX-DOAS measurements. Also, the altitude range without profile information close to the ground should be minimised and detailed information on the aerosol optical and/or microphysical properties should be collected and used. The results for both days are inconsistent, and no explanation for a O4 scaling factor could be derived in this study. Thus, similar but more extended future studies should be performed, including more measurement days and more instruments. Also, additional wavelengths should be included.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2505596-3
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  • 7
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 2 ( 2020-02-13), p. 685-712
    Abstract: Abstract. 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.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2505596-3
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  • 8
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 15, No. 4 ( 2022-02-24), p. 987-1006
    Abstract: Abstract. We present a formalism that relates the vertical column density (VCD) of the oxygen collision complex O2–O2 (denoted as O4 below) to surface (2 m) values of temperature and pressure, based on physical laws. In addition, we propose an empirical modification which also accounts for surface relative humidity (RH). This allows for simple and quick calculation of the O4 VCD without the need for constructing full vertical profiles. The parameterization reproduces the true O4 VCD, as derived from vertically integrated profiles, within -0.7±1.2% (mean ± SD) for Weather Research and Forecasting (WRF) simulations around Germany, 0.2±1.8 % for global reanalysis data (ERA5), and -0.3±1.4% for Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) radiosonde measurements around the world. When applied to measured surface values, uncertainties of 1 K, 1 hPa, and 16 % for temperature, pressure, and RH correspond to relative uncertainties of the O4 VCD of 0.3 %, 0.2 %, and 1 %, respectively. The proposed parameterization thus provides a simple and accurate formula for the calculation of the O4 VCD which is expected to be useful in particular for MAX-DOAS applications.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2505596-3
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  • 9
    Online Resource
    Online Resource
    Copernicus GmbH ; 2021
    In:  Earth System Science Data Vol. 13, No. 6 ( 2021-06-24), p. 2995-3012
    In: Earth System Science Data, Copernicus GmbH, Vol. 13, No. 6 ( 2021-06-24), p. 2995-3012
    Abstract: Abstract. We present version 1.0 of a global catalog of NOx emissions from point sources, derived from TROPOspheric Monitoring Instrument (TROPOMI) measurements of tropospheric NO2 for 2018–2019. The identification of sources and quantification of emissions are based on the divergence (spatial derivative) of the mean horizontal flux, which is highly sensitive for point sources like power plant exhaust stacks. The catalog lists 451 locations which could be clearly identified as NOx point sources by a fully automated algorithm, while ambiguous cases as well as area sources such as megacities are skipped. A total of 242 of these point sources could be automatically matched to power plants. Other NOx point sources listed in the catalog are metal smelters, cement plants, or industrial areas. The four largest localized NOx emitters are all coal combustion plants in South Africa. About 1/4 of all detected point sources are located in the Indian subcontinent and are mostly associated with power plants. The catalog is incomplete, mainly due to persisting gaps in the TROPOMI NO2 product at some coastlines, inaccurate or complex wind fields in coastal and mountainous regions, and high noise in the divergence maps for high background pollution. The derived emissions are generally too low, lacking a factor of about 2 up to 8 for extreme cases. This strong low bias results from combination of different effects, most of all a strong underestimation of near-surface NO2 in TROPOMI NO2 columns. Still, the catalog has high potential for checking and improving emission inventories, as it provides accurate and independent up-to-date information on the location of sources of NOx and thus also CO2. The catalog of NOx emissions from point sources is freely available at https://doi.org/10.26050/WDCC/Quant_NOx_TROPOMI (Beirle et al., 2020).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2475469-9
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 7 ( 2021-04-07), p. 5315-5353
    Abstract: Abstract. We used a global long-term (1995–2015) data set of total column water vapour (TCWV) derived from satellite observations to quantify to which extent the temporal patterns of various teleconnections can be identified in this data set. To our knowledge, such a comprehensive global TCWV data set was rarely used for teleconnection studies. One important property of the TCWV data set is that it is purely based on observational data. We developed a new empirical method to decide whether a teleconnection index is significantly detected in the global data set. We compared our new method to well-established hypothesis tests and found good agreement with the results of our approach. Based on our empirical method more than 40 teleconnection indices were significantly detected in the global TCWV data set derived from satellite observations. In addition to the satellite data we also applied our method to other global data sets derived from ERA-Interim. One important finding is that the spatial patterns obtained for the ERA TCWV data are very similar to the observational TCWV data set indicating a high consistency between the satellite and ERA data. Moreover, similar results are also found for two selections of ERA data (either all data or mainly clear-sky data). This finding indicates that the clear-sky bias of the satellite data set is negligible for the results of this study. However, for some indices, also systematic differences in the spatial patterns between the satellite and model data set were found probably indicating possible shortcomings in the model data. For most “traditional” teleconnection data sets (surface temperature, surface pressure, geopotential heights and meridional winds at different altitudes) a smaller number of significant teleconnection indices was found than for the TCWV data sets, while for zonal winds at different altitudes, the number of significant teleconnection indices (up to 〉 50) was higher. The strongest teleconnection signals were found in the data sets of tropospheric geopotential heights and surface pressure. In all global data sets, no “other indices” (solar variability, stratospheric AOD or hurricane frequency) were significantly detected. Since many teleconnection indices are strongly correlated, we also applied our method to a set of orthogonalised indices, which represent the dominant independent temporal teleconnection patterns. The number of significantly detected orthogonalised indices (20) was found to be much smaller than for the original indices (42). Based on the orthogonalised indices we derived the global spatial distribution of the cumulative effect of teleconnections. The strongest effect on the TCWV is found in the tropics and high latitudes.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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