scholarly journals Observations of the vertical distributions of summertime atmospheric pollutants and the corresponding ozone production in Shanghai, China

2017 ◽  
Vol 17 (23) ◽  
pp. 14275-14289 ◽  
Author(s):  
Chengzhi Xing ◽  
Cheng Liu ◽  
Shanshan Wang ◽  
Ka Lok Chan ◽  
Yang Gao ◽  
...  

Abstract. Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) and lidar measurements were performed in Shanghai, China, during May 2016 to investigate the vertical distribution of summertime atmospheric pollutants. In this study, vertical profiles of aerosol extinction coefficient, nitrogen dioxide (NO2) and formaldehyde (HCHO) concentrations were retrieved from MAX-DOAS measurements using the Heidelberg Profile (HEIPRO) algorithm, while vertical distribution of ozone (O3) was obtained from an ozone lidar. Sensitivity study of the MAX-DOAS aerosol profile retrieval shows that the a priori aerosol profile shape has significant influences on the aerosol profile retrieval. Aerosol profiles retrieved from MAX-DOAS measurements with Gaussian a priori profile demonstrate the best agreements with simultaneous lidar measurements and vehicle-based tethered-balloon observations among all a priori aerosol profiles. Tropospheric NO2 vertical column densities (VCDs) measured with MAX-DOAS show a good agreement with OMI satellite observations with a Pearson correlation coefficient (R) of 0.95. In addition, measurements of the O3 vertical distribution indicate that the ozone productions do not only occur at surface level but also at higher altitudes (about 1.1 km). Planetary boundary layer (PBL) height and horizontal and vertical wind field information were integrated to discuss the ozone formation at upper altitudes. The results reveal that enhanced ozone concentrations at ground level and upper altitudes are not directly related to horizontal and vertical transportation. Similar patterns of O3 and HCHO vertical distributions were observed during this campaign, which implies that the ozone productions near the surface and at higher altitudes are mainly influenced by the abundance of volatile organic compounds (VOCs) in the lower troposphere.

2017 ◽  
Author(s):  
Chengzhi Xing ◽  
Cheng Liu ◽  
Shanshan Wang ◽  
Ka Lok Chan ◽  
Yang Gao ◽  
...  

Abstract. Ground based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) and lidar measurements were performed in Shanghai, China during May 2016 to investigate the summertime atmospheric pollutants vertical distribution. In this study, vertical profiles of aerosol extinction coefficient, nitrogen dioxide (NO2) and formaldehyde (HCHO) concentrations were retrieved from MAX-DOAS measurement using the Heidelberg Profile (HeiPro) algorithm, while vertical distribution of ozone (O3) was obtained from an ozone lidar. Sensitivity study of the MAX-DOAS aerosol profile retrieval shows that the a priori aerosol profile shape has significant influences on the aerosol profile retrieval. Aerosol profiles retrieved from MAX-DOAS measurements with Gaussian a priori demonstrate the best agreements with simultaneous lidar measurements and vehicle-based tethered-balloon observations among all a priori aerosol profiles. MAX-DOAS measured tropospheric NO2Vertical Column Densities (VCDs) show a good agreement with OMI satellite observations with Pearson correlation coefficient (R) of 0.95. In addition, measurements of the O3 vertical distribution indicate that the ozone productions do not only occur at surface level but also at higher altitudes (about 1.1 km). Planetary boundary layer (PBL) height, horizontal and vertical wind fields information were integrated to discuss the ozone formation at upper altitudes. The results reveal that enhanced ozone concentrations at ground and upper altitudes are not directly related to horizontal and vertical transportations. Similar patterns of O3 and HCHO vertical distributions were observed during this campaign, which implies that the ozone productions near to the surface and at higher altitudes are mainly influenced by the abundance of volatile organic compounds (VOCs) in the lower troposphere.


2021 ◽  
Author(s):  
Vinod Kumar ◽  
Julia Remmers ◽  
Steffen Beirle ◽  
Astrid Kerkweg ◽  
Jos Lelieveld ◽  
...  

<p>Regional atmospheric chemistry models are adopted for simulating concentrations of atmospheric components at high resolution and quantifying the impact of localized emissions (e.g. industrial and urban clusters) on the non-linear chemical processes, e.g. ozone production. However, their evaluation is challenging due to the limited availability of high spatiotemporally resolved reference datasets. For the same reason, the vertical distribution of pollutants simulated by the model is especially arduous to assess.</p><p>Here, we present regional atmospheric chemistry model studies with spatial resolution up to 2.2 × 2.2 km<sup>2</sup> focused around Germany for May 2018 using the MECO(n) model system. Using a network of surface concentration measurements at background, near traffic and industrial locations, we evaluate the spatial distribution of NO<sub>2</sub> simulated by the model. The highly resolved model together with a comparable resolution and up-to-date input emissions inventory, was found to perform best in reproducing the spatial distribution of NO<sub>2</sub> surface volume mixing ratios (VMRs). We propose a computationally efficient approach to account for the diurnal and day of the week variability of input anthropogenic emissions (e.g. from road transport), which proved to be crucial for resolving the temporal variability of NO<sub>2</sub> surface VMRs.</p><p>The simulated NO<sub>2</sub> tropospheric vertical column densities were evaluated by employing the measurements of a 4-azimuth MAX-DOAS instrument in Mainz. Generally, such comparisons do not account for the spatial sensitivity volume of the MAX-DOAS measurements, the change of sensitivity within this volume and the spatial heterogeneity of NO<sub>2</sub>. We therefore apply a consistent approach of comparison of the differential slant column densities (dSCDs), which overcomes these limitations. Moreover, the dSCDs are obtained for several elevation and azimuth angles, which are characterized by distinctive sensitivity for different vertical levels within the boundary layer and different horizontal representativeness. Hence, also an evaluation of the model in simulating the vertical distribution of NO<sub>2</sub> can be performed with this approach using continuous MAX-DOAS measurements spanning long time periods. We found that the model performs well with respect to the measured dSCDs at low elevation angles (< 8°) with an overall bias between +14 and -9%, and Pearson correlation coefficients between 0.5 and 0.8 for the different azimuth viewing directions.</p>


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.


2020 ◽  
Vol 20 (11) ◽  
pp. 6973-6990 ◽  
Author(s):  
Jianzhong Ma ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Junli Jin ◽  
Siyang Cheng ◽  
...  

Abstract. Mt. Waliguan Observatory (WLG) is a World Meteorological Organization (WMO) Global Atmosphere Watch (GAW) global baseline station in China. WLG is located at the northeastern part of the Tibetan Plateau (36∘17′ N, 100∘54′ E, 3816 m a.s.l.) and is representative of the pristine atmosphere over the Eurasian continent. We made long-term ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements at WLG during the period 2012–2015. In this study, we retrieve the differential slant column densities (dSCDs) and estimate the tropospheric background mixing ratios of different trace gases, including NO2, SO2, HCHO, and BrO, using the measured spectra at WLG. Averaging of 10 original spectra is found to be an “optimum option” for reducing both the statistical error of the spectral retrieval and systematic errors in the analysis. The dSCDs of NO2, SO2, HCHO, and BrO under clear-sky and low-aerosol-load conditions are extracted from measured spectra at different elevation angles at WLG. By performing radiative transfer simulations with the model TRACY-2, we establish approximate relationships between the trace gas dSCDs at 1∘ elevation angle and the corresponding average tropospheric background volume mixing ratios. Mixing ratios of these trace gases in the lower troposphere over WLG are estimated to be in a range of about 7 ppt (January) to 100 ppt (May) for NO2, below 0.5 ppb for SO2, between 0.4 and 0.9 ppb for HCHO, and lower than 0.3 ppt for BrO. The chemical box model simulations constrained by the NO2 concentration from our MAX-DOAS measurements show that there is a little net ozone loss (−0.8 ppb d−1) for the free-tropospheric conditions and a little net ozone production (0.3 ppb d−1) for the boundary layer conditions over WLG during summertime. Our study provides valuable information and data sets for further investigating tropospheric chemistry in the background atmosphere and its links to anthropogenic activities.


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

<p>Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of aerosols, tropospheric nitrogen dioxide (NO<sub>2</sub>) and formaldehyde (HCHO) have been carried out in Uccle, Brussels, during two years (March 2018 – 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<sup>o</sup>). 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  concentrations (VMRs) and vertical column densities (VCDs) are retrieved in ten different azimuthal directions.</p><p>The present work focuses on the seasonal horizontal variation of NO<sub>2 </sub>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  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  vertical profile information derived from the MAX-DOAS measurements, we show that a persistent systematic underestimation of the TROPOMI  data can be explained by uncertainties in the a-priori NO<sub>2</sub> profile shape in the satellite retrieval. A similar validation study for TROPOMI HCHO is currently under progress and preliminary results will be presented.</p><p><strong>References:</strong></p><p>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, 1521–1532, https://doi.org/10.5194/amt-6-1521-2013, 2013.</p>


2020 ◽  
Author(s):  
Maria Razi ◽  
Steffen Dörner ◽  
Vinod Kumar ◽  
Sebastian Donner ◽  
Noor Ahmad ◽  
...  

<p>Lahore, megacity of Pakistan with more than 11 million inhabitants is a strong emission source of atmospheric pollutants. We present results of a top-down emission procedure for NOx and SO<sub>2</sub> for Lahore, based on car multi-axis differential optical absorption spectroscopy (car-MAX-DOAS) observations. Additionally, the total flux of HCHO from the city is determined which can be seen as an indicator for VOC emissions. Results from two extensive campaigns, which took place in summer 2017 and spring 2018 will be presented. From the measured spectra, we retrieve the vertically integrated concentration (the so-called tropospheric vertical column density, VCD) of the trace gases along the driving route by using the so-called geometric approximation method. By combining these observations with ECMWF Re-Analysis wind data, the total fluxes of NO<sub>x</sub>, SO<sub>2</sub> and HCHO from the city of Lahore are estimated. From both measurement campaigns, we also analyzed the seasonal variability of the above-mentioned species.</p><p>Derived NOx and SO<sub>2</sub> emissions are compared to the bottom-up emission inventory EDGAR. Spatial disributions of the tropospheric NO<sub>2</sub> and SO<sub>2</sub> VCDs observed by car MAX-DOAS are compared with those simulated using a coupled regional-global model system (MECO(n)). We find that, the model is able to account for the spatial variablity but the VCDs are systematically underestimated by the regional model. Finally, derived NOx emissions are also compared to the emissions estimated from TROPOMI satellite observations.</p>


2020 ◽  
Vol 20 (13) ◽  
pp. 8017-8045 ◽  
Author(s):  
Steven Compernolle ◽  
Tijl Verhoelst ◽  
Gaia Pinardi ◽  
José Granville ◽  
Daan Hubert ◽  
...  

Abstract. The QA4ECV (Quality Assurance for Essential Climate Variables) version 1.1 stratospheric and tropospheric NO2 vertical column density (VCD) climate data records (CDRs) from the OMI (Ozone Monitoring Instrument) satellite sensor are validated using NDACC (Network for the Detection of Atmospheric Composition Change) zenith-scattered light differential optical absorption spectroscopy (ZSL-DOAS) and multi-axis DOAS (MAX-DOAS) data as a reference. The QA4ECV OMI stratospheric VCDs have a small bias of ∼0.2 Pmolec.cm-2 (5 %–10 %) and a dispersion of 0.2 to 1 Pmolec.cm-2 with respect to the ZSL-DOAS measurements. QA4ECV tropospheric VCD observations from OMI are restricted to near-cloud-free scenes, leading to a negative sampling bias (with respect to the unrestricted scene ensemble) of a few peta molecules per square centimetre (Pmolec.cm-2) up to −10 Pmolec.cm-2 (−40 %) in one extreme high-pollution case. The QA4ECV OMI tropospheric VCD has a negative bias with respect to the MAX-DOAS data (−1 to −4 Pmolec.cm-2), which is a feature also found for the OMI OMNO2 standard data product. The tropospheric VCD discrepancies between satellite measurements and ground-based data greatly exceed the combined measurement uncertainties. Depending on the site, part of the discrepancy can be attributed to a combination of comparison errors (notably horizontal smoothing difference error), measurement/retrieval errors related to clouds and aerosols, and the difference in vertical smoothing and a priori profile assumptions.


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