scholarly journals Retrieval of O3, NO2, BrO and OClO Columns from Ground-Based Zenith Scattered Light DOAS Measurements in Summer and Autumn over the Northern Tibetan Plateau

2021 ◽  
Vol 13 (21) ◽  
pp. 4242
Author(s):  
Siyang Cheng ◽  
Jianzhong Ma ◽  
Xiangdong Zheng ◽  
Myojeong Gu ◽  
Sebastian Donner ◽  
...  

Ground-based zenith scattered light differential optical absorption spectroscopy (DOAS) measurements were performed in summer and autumn (27 May–30 November) 2020 at Golmud (94°54′ E, 36°25′ N; 2807.6 m altitude) to investigate the abundances and temporal variations of ozone (O3) and its depleting substances over the northern Tibetan Plateau (TP). The differential slant column densities (dSCDs) of O3, nitrogen dioxide (NO2), bromine monoxide (BrO), and chlorine dioxide (OClO) were simultaneously retrieved from scattered solar spectra in the zenith direction during the twilight period. The O3 vertical column densities (VCDs) were derived by applying the Langley plot method, for which we investigated the sensitivities to the chosen wavelength, the a-priori O3 profile and the aerosol extinction profile used in O3 air mass factor (AMF) simulation as well as the selected solar zenith angle (SZA) range. The mean O3 VCDs from June to November 2020 are 7.21 × 1018 molec·cm−2 and 7.18 × 1018 molec·cm−2 at sunrise and sunset, respectively. The derived monthly variations of the O3 VCDs, ranging from a minimum of 6.9 × 1018 molec·cm−2 in October to 7.5 × 1018 molec·cm−2 in November, well matched the OMI satellite product, with a correlation coefficient R = 0.98. The NO2 VCDs at SZA = 90°, calculated by a modified Langley plot method, were systematically larger at sunset than at sunrise as expected with a pm/am ratio of ~1.56. The maximum of the monthly NO2 VCDs, averaged between sunrise and sunset, was 3.40 × 1015 molec·cm−2 in July. The overall trends of the NO2 VCDs were gradually decreasing with the time and similarly observed by the ground-based zenith DOAS and OMI. The average level of the BrO dSCD90°–80° (i.e., dSCD between 90° and 80° SZA) was 2.06 × 1014 molec·cm−2 during the period of June–November 2020. The monthly BrO dSCD90°–80° presented peaks in August and July for sunrise and sunset, respectively, and slowly increased after October. During the whole campaign period, the OClO abundance was lower than the detection limit of the instrument. This was to be expected because during that season the stratospheric temperatures were above the formation temperature of polar stratospheric clouds. Nevertheless, this finding is still of importance, because it indicates that the OClO analysis works well and is ready to be used during periods when enhanced OClO abundances can be expected. As a whole, ground-based zenith DOAS observations can serve as an effective way to measure the columns of O3 and its depleting substances over the TP. The aforementioned results are helpful in investigating stratospheric O3 chemistry over the third pole of the world.

2010 ◽  
Vol 3 (3) ◽  
pp. 631-653 ◽  
Author(s):  
J. Puķīte ◽  
S. Kühl ◽  
T. Deutschmann ◽  
U. Platt ◽  
T. Wagner

Abstract. Methods of UV/VIS absorption spectroscopy to determine the constituents in the Earth's atmosphere from measurements of scattered light are often based on the Beer-Lambert law, like e.g. Differential Optical Absorption Spectroscopy (DOAS). While the Beer-Lambert law is strictly valid for a single light path only, the relation between the optical depth and the concentration of any absorber can be approximated as linear also for scattered light observations at a single wavelength if the absorption is weak. If the light path distribution is approximated not to vary with wavelength, also linearity between the optical depth and the product of the cross-section and the concentration of an absorber can be assumed. These assumptions are widely made for DOAS applications for scattered light observations. For medium and strong absorption of scattered light (e.g. along very long light-paths like in limb geometry) the relation between the optical depth and the concentration of an absorber is no longer linear. In addition, for broad wavelength intervals the differences in the travelled light-paths at different wavelengths become important, especially in the UV, where the probability for scattering increases strongly with decreasing wavelength. However, the DOAS method can be extended to cases with medium to strong absorptions and for broader wavelength intervals by the so called air mass factor modified (or extended) DOAS and the weighting function modified DOAS. These approaches take into account the wavelength dependency of the slant column densities (SCDs), but also require a priori knowledge for the air mass factor or the weighting function from radiative transfer modelling. We describe an approach that considers the fitting results obtained from DOAS, the SCDs, as a function of wavelength and vertical optical depth and expands this function into a Taylor series of both quantities. The Taylor coefficients are then applied as additional fitting parameters in the DOAS analysis. Thus the variability of the SCD in the fit window is determined by the retrieval itself. This new approach provides a description of the SCD the exactness of which depends on the order of the Taylor expansion, and is independent from any assumptions or a priori knowledge of the considered absorbers. In case studies of simulated and measured spectra in the UV range (332–357 nm), we demonstrate the improvement by this approach for the retrieval of vertical profiles of BrO from the SCIAMACHY limb observations. The results for BrO obtained from the simulated spectra are closer to the true profiles, when applying the new method for the SCDs of ozone, than when the standard DOAS approach is used. For the measured spectra the agreement with validation measurements is also improved significantly, especially for cases with strong ozone absorption. While the focus of this article is on the improvement of the BrO profile retrieval from the SCIAMACHY limb measurements, the novel approach may be applied to a wide range of DOAS retrievals.


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.


2020 ◽  
Vol 13 (11) ◽  
pp. 6271-6292
Author(s):  
Wenjing Su ◽  
Cheng Liu ◽  
Ka Lok Chan ◽  
Qihou Hu ◽  
Haoran Liu ◽  
...  

Abstract. We present an improved TROPOspheric Monitoring Instrument (TROPOMI) retrieval of formaldehyde (HCHO) over China. The new retrieval optimizes the slant column density (SCD) retrieval and air mass factor (AMF) calculation for TROPOMI observations of HCHO over China. Retrieval of HCHO differential SCDs (DSCDs) is improved using the basic optical differential spectroscopy (BOAS) technique resulting in lower noise and smaller random error, while AMFs are improved with a priori HCHO profiles from a higher resolution regional chemistry transport model. Compared to the operational product, the new TROPOMI HCHO retrieval shows better agreement with ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements in Beijing. The improvements are mainly related to the AMF calculation with more precise a priori profiles in winter. Using more precise a priori profiles in general reduces HCHO vertical column densities (VCDs) by 52.37 % (± 27.09 %) in winter. Considering the aerosol effect in AMF calculation reduces the operational product by 11.46 % (± 1.48 %) and our retrieval by 17.61 % (± 1.92 %) in winter. The improved and operational HCHO are also used to investigate the spatial–temporal characteristics of HCHO over China. The result shows that both improved and operational HCHO VCDs reach maximum in summer and minimum in winter. High HCHO VCDs mainly located over populated areas, i.e., Sichuan Basin and central and eastern China, indicate a significant contribution of anthropogenic emissions. The hotspots are more obvious on the map of the improved HCHO retrieval than the operational product. The result indicates that the improved TROPOMI HCHO retrieval is more suitable for the analysis of regional- and city-scale pollution in China.


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.


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):  
Steven Compernolle ◽  
Tijl Verhoelst ◽  
Gaia Pinardi ◽  
José Granville ◽  
Daan Hubert ◽  
...  

Abstract. The QA4ECV version 1.1 stratospheric and tropospheric NO2 vertical column density (VCD) climate data records (CDR) from the satellite sensor OMI are validated, using NDACC zenith scattered light DOAS (ZSL-DOAS) and Multi Axis-DOAS (MAX-DOAS) data as a reference. The QA4ECV OMI stratospheric VCD 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 Pmolec cm-2 up to −10 Pmolec cm-2 (−40 %) in one extreme high-pollution case. QA4ECV OMI tropospheric VCD has a negative bias with respect to the MAX-DOAS data (−1 to −4 Pmolec cm-2), a feature also found for the OMI OMNO2 standard data product. The tropospheric VCD discrepancies between satellite and ground-based data exceed by far 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 to the difference in vertical smoothing and a priori profile assumptions.


2020 ◽  
Author(s):  
Sebastian Iancu

<p>Atmospheric pollution has a well-known impact on the human life, thus observing the emissions of trace gases is an important part of monitoring the atmospheric composition. This paper aims to determine the vertical column densities (VCDs) of Nitrogen Dioxide (NO<sub>2</sub>) and Sulfur Dioxide (SO<sub>2</sub>). These quantities will be used to calculate emissions of these pollutants quantified using a ground based mobile remote sensing technique that relies on scattered light DOAS (Differential Optical Absorption Spectroscopy) measurements. This method will be implemented using the SWING (Small Whiskbroom Imager for atmospheric compositioN monitorinG). The instrument is designed to perform airborne measurements, but for the purpose of this paper it was adapted for ground-based use by the National Institute for Aerospace Research (INCAS) in Bucharest, Romania. The source aimed to be quantified is the city of Bucharest, specifically the total emissions generated by the traffic and industry within the city. The measurements will be performed during the Spring of 2020 between February and April. The experimental setup consists of the SWING that will be mounted on the roof of a car, which allows to perform measurements along the ring road of Bucharest. There will be presented results from several days of measurements from a total of 150 hours of driving in terms of differential slant column densities (DSCDs), vertical column densities (VCDs) and quantified emissions of NO­<sub>2</sub> and SO<sub>2</sub>. This study will also be used for the fine tuning of the SWING operational parameters for use on UAV platforms in future measurement campaigns.</p>


2005 ◽  
Vol 5 (4) ◽  
pp. 1015-1025 ◽  
Author(s):  
M. Coldewey-Egbers ◽  
M. Weber ◽  
L. N. Lamsal ◽  
R. de Beek ◽  
M. Buchwitz ◽  
...  

Abstract. A new algorithm approach called Weighting Function Differential Optical Absorption Spectroscopy (WFDOAS) is presented which has been developed to retrieve total ozone columns from nadir observations of the Global Ozone Monitoring Experiment. By fitting the vertically integrated ozone weighting function rather than ozone cross-section to the sun-normalized radiances, a direct retrieval of vertical column amounts is possible. The new WFDOAS approach takes into account the slant path wavelength modulation that is usually neglected in the standard DOAS approach using single airmass factors. This paper focuses on the algorithm description and error analysis, while in a companion paper by Weber et al. (2004) a detailed validation with groundbased measurements is presented. For the first time several auxiliary quantities directly derived from the GOME spectral range such as cloud-top-height and cloud fraction (O2-A band) and effective albedo using the Lambertian Equivalent Reflectivity (LER) near 377nm are used in combination as input to the ozone retrieval. In addition the varying ozone dependent contribution to the Raman correction in scattered light known as Ring effect has been included. The molecular ozone filling-in that is accounted for in the new algorithm has the largest contribution to the improved total ozone results from WFDOAS compared to the operational product. The precision of the total ozone retrieval is estimated to be better than 3% for solar zenith angles below 80°.


2004 ◽  
Vol 4 (4) ◽  
pp. 4915-4944
Author(s):  
M. Coldewey-Egbers ◽  
M. Weber ◽  
L. N. Lamsal ◽  
R. de Beek ◽  
M. Buchwitz ◽  
...  

Abstract. A new algorithm approach called Weighting Function Differential Optical Absorption Spectroscopy (WFDOAS) is presented which has been developed to retrieve total ozone columns from nadir observations of the Global Ozone Monitoring Experiment. By fitting the vertically integrated ozone weighting function rather than ozone cross-section to the sun-normalized radiances, a direct retrieval of vertical column amounts is possible. The new WFDOAS approach takes into account the slant path wavelength modulation that is usually neglected in the standard DOAS approach using single airmass factors. This paper focuses on the algorithm description and error analysis, while in a companion paper by Weber et al. (2004) a detailed validation with groundbased measurements is presented. For the first time several auxiliary quantities directly derived from the GOME spectral range such as cloud-top-height and cloud fraction (O2-A band) and effective albedo using the Lambertian Equivalent Reflectivity (LER) near 377 nm are used in combination as input to the ozone retrieval. In addition the varying ozone dependent contribution to the Raman correction in scattered light known as Ring effect has been included. Detailed investigations have been performed concerning the influence of the molecular ozone filling-in as part of the Ring effect. The precision of the total ozone retrieval is estimated to be better than 3% for solar zenith angles below 80°.


2009 ◽  
Vol 2 (6) ◽  
pp. 2919-2982 ◽  
Author(s):  
J. Puķīte ◽  
S. Kühl ◽  
T. Deutschmann ◽  
U. Platt ◽  
T. Wagner

Abstract. Methods of UV/VIS absorption spectroscopy to determine the constituents in the Earth's atmosphere from measurements of scattered light are often based on the Beer-Lambert law, like e.g. Differential Optical Absorption Spectroscopy (DOAS). Therefore they are strictly valid for weak absorptions and narrow wavelength intervals (strictly only for monochromatic radiation). For medium and strong absorption (e.g. along very long light-paths like in limb geometry) the relation between the optical depth and the concentration of an absorber is not linear anymore. As well, for large wavelength intervals the wavelength dependent differences in the travelled light-paths become important, especially in the UV, where the probability for scattering increases strongly with decreasing wavelength. However, by taking into account these dependencies, the applicability of the DOAS method can be extended also to cases with medium to strong absorptions and for broader wavelength intervals. Common approaches for this correction are the so called air mass factor modified (or extended) DOAS and the weighting function modified DOAS. These approaches take into account the wavelength dependency of the slant column densities (SCDs), but also require a-priori knowledge for the air mass factor or the weighting function calculation by radiative transfer modelling. We describe an approach that considers the fitting results obtained from DOAS, the SCDs, as a function of wavelength and vertical optical depth and expands this function into a Taylor series of both quantities. The Taylor coefficients are then applied as additional fitting parameters in the DOAS analysis. Thus the variability of the SCD in the fit window is determined by the retrieval itself. This new approach gives a description of the SCD that is as close to reality as desired (depending on the order of the Taylor expansion), and is independent from any assumptions or a-priori knowledge of the considered absorbers. In case studies for simulated and measured spectra in the UV (332–357 nm), we demonstrate the improvement by this approach for the retrieval of vertical profiles of BrO from the SCIAMACHY limb observations. Compared to the standard DOAS approach, the results for BrO obtained from the simulated spectra are closer to the true profile, when applying the new method for the SCDs of ozone. Also for the measured spectra the agreement with validation measurements is improved significantly, especially for cases with strong ozone absorption. While the focus of this article is on the improvement of the BrO profile retrieval from the SCIAMACHY limb measurements, the novel approach may be applied for a wide range of DOAS retrievals.


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