scholarly journals Horizontal distribution of tropospheric NO<sub>2</sub> and aerosols derived by dual-scan multi-wavelength MAX-DOAS measurements in Uccle, Belgium

2021 ◽  
Author(s):  
Ermioni Dimitropoulou ◽  
Francois Hendrick ◽  
Martina Michaela Friedrich ◽  
Frederik Tack ◽  
Gaia Pinardi ◽  
...  

Abstract. Dual-scan ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of tropospheric nitrogen dioxide (NO2) and aerosols have been carried out in Uccle (50.8° N, 4.35° E; Brussels region, Belgium) for two years, from March 2018 to February 2020. The MAX-DOAS instrument has been operating in both UV and Visible wavelength ranges in a dual-scan configuration consisting of two sub-modes: (1) an elevation scan in a fixed viewing azimuthal direction and (2) an azimuthal scan in a fixed low elevation angle (2°). By analyzing the O4 and NO2 dSCDs at six different wavelength intervals along every azimuthal direction and by applying a new Optimal-Estimation-based inversion approach, the horizontal distribution of the NO2 near-surface concentrations and vertical column densities (VCDs) and the aerosols near-surface extinction coefficient are retrieved along ten azimuthal directions. The retrieved horizontal NO2 concentration profiles allow the identification of the main NO2 hotspots in the Brussels area. Correlative comparisons of the retrieved horizontal NO2 distribution have been conducted with airborne, mobile, and satellite datasets, and overall a good agreement is found. The comparison with TROPOMI observations reveals that the characterization of the horizontal distribution of tropospheric NO2 VCDs by ground-based measurements, the appropriate sampling of TROPOMI pixels, and an adequate a priori NO2 profile shape in TROPOMI retrievals lead to a better consistency between satellite and ground-based datasets.

2020 ◽  
Author(s):  
Ermioni Dimitropoulou ◽  
François Hendrick ◽  
Gaia Pinardi ◽  
Martina M. Friedrich ◽  
Alexis Merlaud ◽  
...  

Abstract. Ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of aerosols and tropospheric nitrogen dioxide (NO2) were carried out in Uccle (50.8° N, 4.35° E) Brussels, during one year from March 2018 until March 2019. The instrument was operated in both UV and visible (Vis) wavelength ranges in a dual-scan configuration consisting of two sub-modes: (1) an elevation scan in a fixed viewing azimuthal direction (the so-called main azimuthal direction) pointing to the Northeast and (2) an azimuthal scan in a fixed low elevation angle (2°). By applying a vertical profile inversion algorithm in the main azimuthal direction and a parameterization technique in the other azimuthal directions, near-surface NO2 concentrations (VMRs) and vertical column densities (VCDs) were retrieved in ten different azimuthal directions. The dual-scan MAX-DOAS dataset allows partly resolving the horizontal distribution of NO2 around the measurement site and studying its seasonal variations. Furthermore, we show that measuring the tropospheric NO2 VCDs in different azimuthal directions improves the spatial colocation with measurements from the Sentinel-5 Precursor (S5P), leading to a reduction of the spread in validation results. By using NO2 vertical profile information derived from the MAX-DOAS measurements, we also resolve a systematic underestimation in S5P NO2 data due to the use of inadequate a-priori NO2 profile shape data in the satellite retrieval.


2020 ◽  
Author(s):  
Ermioni Dimitropoulou ◽  
Francois Hendrick ◽  
Martine M. Friedrich ◽  
Gaia Pinardi ◽  
Frederik Tack ◽  
...  

&lt;p&gt;Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of aerosols, tropospheric nitrogen dioxide (NO&lt;sub&gt;2&lt;/sub&gt;) and formaldehyde (HCHO) have been carried out in Uccle, Brussels, during two years (March 2018 &amp;#8211; March 2020). The MAX-DOAS instrument has been operating in both UV and visible (Vis) wavelength ranges in a dual-scan configuration consisting of two sub-modes: (1) an elevation scan in a fixed viewing azimuthal direction (the so-called main azimuthal direction) pointing and (2) an azimuthal scan in a fixed low elevation angle (2&lt;sup&gt;o&lt;/sup&gt;). By applying a vertical profile inversion algorithm in the main azimuthal direction and an adapted version of the parameterization technique proposed by Sinreich et al. (2013) in the other azimuthal directions, near-surface &amp;#160;concentrations (VMRs) and vertical column densities (VCDs) are retrieved in ten different azimuthal directions.&lt;/p&gt;&lt;p&gt;The present work focuses on the seasonal horizontal variation of NO&lt;sub&gt;2 &lt;/sub&gt;and HCHO around the measurement site. The observations show a clear seasonal cycle of these trace gases. An important application of the dual-scan MAX-DOAS measurements is the validation of satellite missions with high spatial resolution, such as TROPOMI/S5P. Measuring the tropospheric &amp;#160;VCDs in different azimuthal directions is shown to improve the spatial colocation with satellite measurements leading to a better agreement between both datasets. By using &amp;#160;vertical profile information derived from the MAX-DOAS measurements, we show that a persistent systematic underestimation of the TROPOMI &amp;#160;data can be explained by uncertainties in the a-priori NO&lt;sub&gt;2&lt;/sub&gt; profile shape in the satellite retrieval. A similar validation study for TROPOMI HCHO is currently under progress and preliminary results will be presented.&lt;/p&gt;&lt;p&gt;&lt;strong&gt;References:&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;Sinreich, R., Merten, A., Molina, L., and Volkamer, R.: Parameterizing radiative transfer to convert MAX-DOAS dSCDs into near-surface box-averaged mixing ratios, Atmos. Meas. Tech., 6, 1521&amp;#8211;1532, https://doi.org/10.5194/amt-6-1521-2013, 2013.&lt;/p&gt;


2020 ◽  
Vol 13 (10) ◽  
pp. 5165-5191 ◽  
Author(s):  
Ermioni Dimitropoulou ◽  
François Hendrick ◽  
Gaia Pinardi ◽  
Martina M. Friedrich ◽  
Alexis Merlaud ◽  
...  

Abstract. Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of aerosols and tropospheric nitrogen dioxide (NO2) were carried out in Uccle (50.8∘ N, 4.35∘ E), Brussels, during 1 year from March 2018 until March 2019. The instrument was operated in both the UV and visible wavelength ranges in a dual-scan configuration consisting of two sub-modes: (1) an elevation scan in a fixed viewing azimuthal direction (the so-called main azimuthal direction) pointing to the northeast and (2) an azimuthal scan in a fixed low elevation angle (2∘). By applying a vertical profile inversion algorithm in the main azimuthal direction and a parameterization technique in the other azimuthal directions, near-surface NO2 volume mixing ratios (VMRs) and vertical column densities (VCDs) were retrieved in 10 different azimuthal directions. The dual-scan MAX-DOAS dataset allows for partly resolving the horizontal distribution of NO2 around the measurement site and studying its seasonal variations. Furthermore, we show that measuring the tropospheric NO2 VCDs in different azimuthal directions improves the spatial colocation with measurements from the Sentinel-5 Precursor (S5P), leading to a reduction of the spread in validation results. By using NO2 vertical profile information derived from the MAX-DOAS measurements, we also resolve a systematic underestimation in S5P NO2 data due to the use of inadequate a priori NO2 profile shape data in the satellite retrieval.


2021 ◽  
Vol 21 (17) ◽  
pp. 12867-12894
Author(s):  
Xin Tian ◽  
Yang Wang ◽  
Steffen Beirle ◽  
Pinhua Xie ◽  
Thomas Wagner ◽  
...  

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.


2021 ◽  
Author(s):  
Xin Tian ◽  
Yang Wang ◽  
Steffen Beirle ◽  
Pinhua Xie ◽  
Thomas Wagner ◽  
...  

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. One inversion algorithm is based on optimal estimation, the other uses a parameterized approach. In this analysis, 3 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. Especially for the optimal estimation algorithm and for high AOD, these findings might explain part of the deviations between the AOD retrieved from MAX-DOAS and sun photometers in previous studies. 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. In general, both inversion schemes can well retrieve the near-surface values of aerosol extinction and trace gases concentrations.


2017 ◽  
Vol 10 (1) ◽  
pp. 119-153 ◽  
Author(s):  
Nicolas Theys ◽  
Isabelle De Smedt ◽  
Huan Yu ◽  
Thomas Danckaert ◽  
Jeroen van Gent ◽  
...  

Abstract. The TROPOspheric Monitoring Instrument (TROPOMI) onboard the Copernicus Sentinel-5 Precursor (S-5P) platform will measure ultraviolet earthshine radiances at high spectral and improved spatial resolution (pixel size of 7 km  ×  3.5 km at nadir) compared to its predecessors OMI and GOME-2. This paper presents the sulfur dioxide (SO2) vertical column retrieval algorithm implemented in the S-5P operational processor UPAS (Universal Processor for UV/VIS Atmospheric Spectrometers) and comprehensively describes its various retrieval steps. The spectral fitting is performed using the differential optical absorption spectroscopy (DOAS) method including multiple fitting windows to cope with the large range of atmospheric SO2 columns encountered. It is followed by a slant column background correction scheme to reduce possible biases or across-track-dependent artifacts in the data. The SO2 vertical columns are obtained by applying air mass factors (AMFs) calculated for a set of representative a priori profiles and accounting for various parameters influencing the retrieval sensitivity to SO2. Finally, the algorithm includes an error analysis module which is fully described here. We also discuss verification results (as part of the algorithm development) and future validation needs of the TROPOMI SO2 algorithm.


2019 ◽  
Vol 12 (1) ◽  
pp. 211-236 ◽  
Author(s):  
Frederik Tack ◽  
Alexis Merlaud ◽  
Andreas C. Meier ◽  
Tim Vlemmix ◽  
Thomas Ruhtz ◽  
...  

Abstract. We present an intercomparison study of four airborne imaging DOAS instruments, dedicated to the retrieval and high-resolution mapping of tropospheric nitrogen dioxide (NO2) vertical column densities (VCDs). The AROMAPEX campaign took place in Berlin, Germany, in April 2016 with the primary objective to test and intercompare the performance of experimental airborne imagers. The imaging DOAS instruments were operated simultaneously from two manned aircraft, performing synchronised flights: APEX (VITO–BIRA-IASB) was operated from DLR's DO-228 D-CFFU aircraft at 6.2 km in altitude, while AirMAP (IUP-Bremen), SWING (BIRA-IASB), and SBI (TNO–TU Delft–KNMI) were operated from the FUB Cessna 207T D-EAFU at 3.1 km. Two synchronised flights took place on 21 April 2016. NO2 slant columns were retrieved by applying differential optical absorption spectroscopy (DOAS) in the visible wavelength region and converted to VCDs by the computation of appropriate air mass factors (AMFs). Finally, the NO2 VCDs were georeferenced and mapped at high spatial resolution. For the sake of harmonising the different data sets, efforts were made to agree on a common set of parameter settings, AMF look-up table, and gridding algorithm. The NO2 horizontal distribution, observed by the different DOAS imagers, shows very similar spatial patterns. The NO2 field is dominated by two large plumes related to industrial compounds, crossing the city from west to east. The major highways A100 and A113 are also identified as line sources of NO2. Retrieved NO2 VCDs range between 1×1015 molec cm−2 upwind of the city and 20×1015 molec cm−2 in the dominant plume, with a mean of 7.3±1.8×1015 molec cm−2 for the morning flight and between 1 and 23×1015 molec cm−2 with a mean of 6.0±1.4×1015 molec cm−2 for the afternoon flight. The mean NO2 VCD retrieval errors are in the range of 22 % to 36 % for all sensors. The four data sets are in good agreement with Pearson correlation coefficients better than 0.9, while the linear regression analyses show slopes close to unity and generally small intercepts.


2017 ◽  
Vol 10 (5) ◽  
pp. 1831-1857 ◽  
Author(s):  
Andreas Carlos Meier ◽  
Anja Schönhardt ◽  
Tim Bösch ◽  
Andreas Richter ◽  
André Seyler ◽  
...  

Abstract. In this study we report on airborne imaging DOAS measurements of NO2 from two flights performed in Bucharest during the AROMAT campaign (Airborne ROmanian Measurements of Aerosols and Trace gases) in September 2014. These measurements were performed with the Airborne imaging Differential Optical Absorption Spectroscopy (DOAS) instrument for Measurements of Atmospheric Pollution (AirMAP) and provide nearly gapless maps of column densities of NO2 below the aircraft with a high spatial resolution of better than 100 m. The air mass factors, which are needed to convert the measured differential slant column densities (dSCDs) to vertical column densities (VCDs), have a strong dependence on the surface reflectance, which has to be accounted for in the retrieval. This is especially important for measurements above urban areas, where the surface properties vary strongly. As the instrument is not radiometrically calibrated, we have developed a method to derive the surface reflectance from intensities measured by AirMAP. This method is based on radiative transfer calculation with SCIATRAN and a reference area for which the surface reflectance is known. While surface properties are clearly apparent in the NO2 dSCD results, this effect is successfully corrected for in the VCD results. Furthermore, we investigate the influence of aerosols on the retrieval for a variety of aerosol profiles that were measured in the context of the AROMAT campaigns. The results of two research flights are presented, which reveal distinct horizontal distribution patterns and strong spatial gradients of NO2 across the city. Pollution levels range from background values in the outskirts located upwind of the city to about 4  ×  1016 molec cm−2 in the polluted city center. Validation against two co-located mobile car-DOAS measurements yields good agreement between the datasets, with correlation coefficients of R =  0.94 and R =  0.85, respectively. Estimations on the NOx emission rate of Bucharest for the two flights yield emission rates of 15.1 ± 9.4 and 13.6 ± 8.4 mol s−1, respectively.


2019 ◽  
Vol 12 (1) ◽  
pp. 599-606 ◽  
Author(s):  
Hitoshi Irie ◽  
Hossain Mohammed Syedul Hoque ◽  
Alessandro Damiani ◽  
Hiroshi Okamoto ◽  
Al Mashroor Fatmi ◽  
...  

Abstract. The first intensive multicomponent ground-based remote-sensing observations by sky radiometer and multi-axis differential optical absorption spectroscopy (MAX-DOAS) were performed simultaneously at the SKYNET Phimai site located in central Thailand (15.18∘ N, 102.56∘ E) from January to April 2016. The period corresponds to the dry season associated with intense biomass burning (BB) activity around the site. The near-surface concentration of formaldehyde (HCHO) retrieved from MAX-DOAS was found to be a useful tracer for absorption aerosols from BB plumes, when BB was the dominant source of HCHO and absorption aerosols over other sources. As the HCHO concentration tripled from 3 to 9 ppbv, the ratio of gaseous glyoxal to HCHO concentrations in daytime decreased from ∼0.04 to ∼0.03, responding presumably to the increased contribution of volatile organic compound emissions from BB. In addition, clear increases in aerosol absorption optical depths (AAODs) retrieved from sky radiometer observations were seen with the HCHO enhancement. At a HCHO of 9 ppbv, AAOD at a wavelength of 340 nm reached as high as ∼0.15±0.03. The wavelength dependence of AAODs at 340–870 nm was quantified by the absorption Ångström exponent (AAE), providing evidence for the presence of brown carbon aerosols at an AAE of 1.5±0.2. Thus, our multicomponent observations around central Thailand are expected to provide unique constraints for understanding physical–chemical–optical properties of BB plumes.


2017 ◽  
Vol 10 (9) ◽  
pp. 3133-3149 ◽  
Author(s):  
Nickolay A. Krotkov ◽  
Lok N. Lamsal ◽  
Edward A. Celarier ◽  
William H. Swartz ◽  
Sergey V. Marchenko ◽  
...  

Abstract. We describe the new version 3.0 NASA Ozone Monitoring Instrument (OMI) standard nitrogen dioxide (NO2) products (SPv3). The products and documentation are publicly available from the NASA Goddard Earth Sciences Data and Information Services Center (https://disc.gsfc.nasa.gov/datasets/OMNO2_V003/summary/). The major improvements include (1) a new spectral fitting algorithm for NO2 slant column density (SCD) retrieval and (2) higher-resolution (1° latitude and 1.25° longitude) a priori NO2 and temperature profiles from the Global Modeling Initiative (GMI) chemistry–transport model with yearly varying emissions to calculate air mass factors (AMFs) required to convert SCDs into vertical column densities (VCDs). The new SCDs are systematically lower (by ∼ 10–40 %) than previous, version 2, estimates. Most of this reduction in SCDs is propagated into stratospheric VCDs. Tropospheric NO2 VCDs are also reduced over polluted areas, especially over western Europe, the eastern US, and eastern China. Initial evaluation over unpolluted areas shows that the new SPv3 products agree better with independent satellite- and ground-based Fourier transform infrared (FTIR) measurements. However, further evaluation of tropospheric VCDs is needed over polluted areas, where the increased spatial resolution and more refined AMF estimates may lead to better characterization of pollution hot spots.


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