MAX-DOAS NO2 profile retrieval over Minsk: 3 years of observation

Author(s):  
Ilya Bruchkouski ◽  
Siarhei Barodka ◽  
Yang Wang

<p>For NO<sub>2</sub> monitoring by MAX-DOAS method, the automated instrument MARS-B based on the spectrograph ORIEL MS257 with a Peltier-cooled CCD-array detector Andor Technology DV-420 OE (number of active pixels is 1024×256, working temperature is -40 ºC) has been employed. The MARS-B instrument records the spectra of scattered sunlight in the range of elevation angles 0º – 90º within vertical angle aperture of 1.3º in spectral range 340-400 nm with FWHM = 0.32 nm and is operating without mechanical shutter. Radiation input system is working without optical fiber and spectrograph unit has open-air design, spectrograph unit is temperature-stabilized at level 40 ± 0.5 ºC. The MARS-B instrument successfully took part in MAD-CAT (2013) and CINDI-2 (2016) international inter-comparison campaigns.</p><p>Since 2017 MARS-B instrument is performing spectra registering over Minsk (National Ozone Monitoring Research and Education Centre, Minsk, Belarus) using multi-axis geometry of observations during daytime and zenith geometry in twilights. More than 4.5 millions of day-time spectra aiming to retrieve differential slant columns of ozone, nitrogen dioxide and oxygen dimer have been processed by DOAS method. Total nitrogen dioxide columns have been retrieved by PriAM algorithm which is based on optimal estimation method.</p><p>Continuous 3-year MAX-DOAS measurements (nitrogen dioxide vertical column, near-surface nitrogen dioxide concentrations, aerosol optical depth) over Minsk in period of 2017 - 2019 will be presented, compared with data of impact gas analyzers and satellite data, analyzed and discussed. Also, zenith twilights measurements will be processed aiming to retrieve stratospheric nitrogen dioxide and ozone columns for comparison with different parameters of solar activity.</p>

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.


2020 ◽  
Author(s):  
Yang Wang ◽  
Arnoud Apituley ◽  
Alkiviadis Bais ◽  
Steffen Beirle ◽  
Nuria Benavent ◽  
...  

Abstract. We present the inter-comparison of delta slant column densities (SCDs) and vertical profiles of nitrous acid (HONO) derived from measurements of different MAX-DOAS instruments and using different inversion algorithms during the Second Cabauw Inter-comparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2), in September 2016, at Cabauw, The Netherlands (51.97° N, 4.93° E). Systematic discrepancies of HONO delta SCDs are observed in the range of ±0.3 × 1015 molecules cm−2, which is half of the typical random discrepancy of 0.6 × 1015 molecules cm−2. For a typical high HONO delta SCD of 2 × 1015 molecules cm−2, the relative systematic and random discrepancies are about 15 % and 30 %, respectively. The inter-comparison of HONO profiles shows that both systematic and random discrepancies of HONO VCDs and near-surface volume mixing ratios (VMRs) are mostly in the range of ~ ±0.5 × 1015 molecules cm−2 and ~ ±0.1 ppb (typically ~ 20 %). Further we find that the discrepancies of the retrieved HONO profiles are dominated by discrepancies of the HONO delta SCDs. The profile retrievals only contribute to the discrepancies of the HONO profiles by ~ 5 %. However, some data sets with substantial larger discrepancies than the typical values indicate that inappropriate implementations of profile inversion algorithms and configurations of radiative transfer models in the profile retrievals can also be an important uncertainty source. In addition, estimations of measurement uncertainties of HONO dSCDs, which can significantly impact profile retrievals using the optimal estimation method, need to consider not only DOAS fit errors, but also atmospheric variability, especially for an instrument with a DOAS fit error lower than ~ 3 × 1015 molecules cm−2. The MAX-DOAS results during the CINDI-2 campaign indicate that the peak HONO levels (e.g. near-surface VMRs of ~ 0.4 ppb) often appeared in the early morning and below 0.2 km. The near-surface VMRs retrieved from the MAX-DOAS observations are compared with those measured using a co-located long-path DOAS instrument. The systematic differences are smaller than 0.15 ppb and 0.07 ppb during early morning and around noon, respectively. Since true HONO values at high altitudes are not known in the absence of real measurements, in order to evaluate the abilities of profile inversion algorithms to respond to different HONO profile shapes, we performed sensitivity studies using synthetic HONO delta SCDs simulated by a radiative transfer model with assumed HONO profiles. The tests indicate that the profile inversion algorithms based on the optimal estimation method with proper configurations can well reproduce the different HONO profile shapes. Therefore we conclude that the feature of HONO accumulated near the surface derived from MAX-DOAS measurements are expected to well represent the ambient HONO profiles.


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 ◽  
Vol 13 (9) ◽  
pp. 5087-5116 ◽  
Author(s):  
Yang Wang ◽  
Arnoud Apituley ◽  
Alkiviadis Bais ◽  
Steffen Beirle ◽  
Nuria Benavent ◽  
...  

Abstract. We present the inter-comparison of delta slant column densities (SCDs) and vertical profiles of nitrous acid (HONO) derived from measurements of different multi-axis differential optical absorption spectroscopy (MAX-DOAS) instruments and using different inversion algorithms during the Second Cabauw Inter-comparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) in September 2016 at Cabauw, the Netherlands (51.97∘ N, 4.93∘ E). The HONO vertical profiles, vertical column densities (VCDs), and near-surface volume mixing ratios are compared between different MAX-DOAS instruments and profile inversion algorithms for the first time. Systematic and random discrepancies of the HONO results are derived from the comparisons of all data sets against their median values. Systematic discrepancies of HONO delta SCDs are observed in the range of ±0.3×1015 molec. cm−2, which is half of the typical random discrepancy of 0.6×1015 molec. cm−2. For a typical high HONO delta SCD of 2×1015 molec. cm−2, the relative systematic and random discrepancies are about 15 % and 30 %, respectively. The inter-comparison of HONO profiles shows that both systematic and random discrepancies of HONO VCDs and near-surface volume mixing ratios (VMRs) are mostly in the range of ∼±0.5×1014 molec. cm−2 and ∼±0.1 ppb (typically ∼20 %). Further we find that the discrepancies of the retrieved HONO profiles are dominated by discrepancies of the HONO delta SCDs. The profile retrievals only contribute to the discrepancies of the HONO profiles by ∼5 %. However, some data sets with substantially larger discrepancies than the typical values indicate that inappropriate implementations of profile inversion algorithms and configurations of radiative transfer models in the profile retrievals can also be an important uncertainty source. In addition, estimations of measurement uncertainties of HONO dSCDs, which can significantly impact profile retrievals using the optimal estimation method, need to consider not only DOAS fit errors, but also atmospheric variability, especially for an instrument with a DOAS fit error lower than ∼3×1014 molec. cm−2. The MAX-DOAS results during the CINDI-2 campaign indicate that the peak HONO levels (e.g. near-surface VMRs of ∼0.4 ppb) often appeared in the early morning and below 0.2 km. The near-surface VMRs retrieved from the MAX-DOAS observations are compared with those measured using a co-located long-path DOAS instrument. The systematic differences are smaller than 0.15 and 0.07 ppb during early morning and around noon, respectively. Since true HONO values at high altitudes are not known in the absence of real measurements, in order to evaluate the abilities of profile inversion algorithms to respond to different HONO profile shapes, we performed sensitivity studies using synthetic HONO delta SCDs simulated by a radiative transfer model with assumed HONO profiles. The tests indicate that the profile inversion algorithms based on the optimal estimation method with proper configurations can reproduce the different HONO profile shapes well. Therefore we conclude that the features of HONO accumulated near the surface derived from MAX-DOAS measurements are expected to represent the ambient HONO profiles well.


2018 ◽  
Vol 11 (12) ◽  
pp. 6833-6859 ◽  
Author(s):  
Tim Bösch ◽  
Vladimir Rozanov ◽  
Andreas Richter ◽  
Enno Peters ◽  
Alexei Rozanov ◽  
...  

Abstract. We present a new MAX-DOAS profiling algorithm for aerosols and trace gases, BOREAS, which utilizes an iterative solution method including Tikhonov regularization and the optimal estimation technique. The aerosol profile retrieval is based on a novel approach in which the absorption depth of O4 is directly used in order to retrieve extinction coefficient profiles instead of the commonly used perturbation theory method. The retrieval of trace gases is done with the frequently used optimal estimation method but significant improvements are presented on how to deal with wrongly weighted a priori constraints and for scenarios in which the a priori profile is inaccurate. Performance tests are separated into two parts. First, we address the general sensitivity of the retrieval to the example of synthetic data calculated with the radiative transfer model SCIATRAN. In the second part of the study, we demonstrate BOREAS profiling accuracy by validating the results with the help of ancillary measurements carried out during the CINDI-2 campaign in Cabauw, the Netherlands, in 2016. The synthetic sensitivity tests indicate that the regularization between measurement and a priori constraints is insufficient when knowledge of the true state of the atmosphere is poor. We demonstrate a priori pre-scaling and extensive regularization tests as a tool for the optimization of retrieved profiles. The comparison of retrieval results with in situ, ceilometer, NO2 lidar, sonde and long-path DOAS measurements during the CINDI-2 campaign always shows high correlations with coefficients greater than 0.75. The largest differences can be found in the morning hours, when the planetary boundary layer is not yet fully developed and the concentration of trace gases and aerosol, as a result of a low night-time boundary layer having formed, is focused in a shallow, near-surface layer.


2021 ◽  
Vol 13 (10) ◽  
pp. 1865
Author(s):  
Gabriel Calassou ◽  
Pierre-Yves Foucher ◽  
Jean-François Léon

Stack emissions from the industrial sector are a subject of concern for air quality. However, the characterization of the stack emission plume properties from in situ observations remains a challenging task. This paper focuses on the characterization of the aerosol properties of a steel plant stack plume through the use of hyperspectral (HS) airborne remote sensing imagery. We propose a new method, based on the combination of HS airborne acquisition and surface reflectance imagery derived from the Sentinel-2 Multi-Spectral Instrument (MSI). The proposed method detects the plume footprint and estimates the surface reflectance under the plume, the aerosol optical thickness (AOT), and the modal radius of the plume. Hyperspectral surface reflectances are estimated using the coupled non-negative matrix factorization (CNMF) method combining HS and MSI data. The CNMF reduces the error associated with estimating the surface reflectance below the plume, particularly for heterogeneous classes. The AOT and modal radius are retrieved using an optimal estimation method (OEM), based on the forward model and allowing for uncertainties in the observations and in the model parameters. The a priori state vector is provided by a sequential method using the root mean square error (RMSE) metric, which outperforms the previously used cluster tuned matched filter (CTMF). The OEM degrees of freedom are then analysed, in order to refine the mask plume and to enhance the quality of the retrieval. The retrieved mean radii of aerosol particles in the plume is 0.125 μμm, with an uncertainty of 0.05 μμm. These results are close to the ultra-fine mode (modal radius around 0.1 μμm) observed from in situ measurements within metallurgical plant plumes from previous studies. The retrieved AOT values vary between 0.07 (near the source point) and 0.01, with uncertainties of 0.005 for the darkest surfaces and above 0.010 for the brightest surfaces.


2008 ◽  
Vol 2 (2) ◽  
pp. 167-178 ◽  
Author(s):  
G. H. Gudmundsson ◽  
M. Raymond

Abstract. An optimal estimation method for simultaneously determining both basal slipperiness and basal topography from variations in surface flow velocity and topography along a flow line on ice streams and ice sheets is presented. We use Bayesian inference to update prior statistical estimates for basal topography and slipperiness using surface measurements along a flow line. Our main focus here is on how errors and spacing of surface data affect estimates of basal quantities and on possibly aliasing/mixing between basal slipperiness and basal topography. We find that the effects of spatial variations in basal topography and basal slipperiness on surface data can be accurately separated from each other, and mixing in retrieval does not pose a serious problem. For realistic surface data errors and density, small-amplitude perturbations in basal slipperiness can only be resolved for wavelengths larger than about 50 times the mean ice thickness. Bedrock topography is well resolved down to horizontal scale equal to about one ice thickness. Estimates of basal slipperiness are not significantly improved by accurate prior estimates of basal topography. However, retrieval of basal slipperiness is found to be highly sensitive to unmodelled errors in basal topography.


2012 ◽  
Vol 12 (10) ◽  
pp. 4607-4617 ◽  
Author(s):  
M. D. Rowe ◽  
J. A. Perlinger

Abstract. Air-water exchange fluxes of persistent, bioaccumulative and toxic (PBT) substances are frequently estimated using the Whitman two-film (W2F) method, but micrometeorological flux measurements of these compounds over water are rarely attempted. We measured air-water exchange fluxes of hexachlorobenzene (HCB) and polychlorinated biphenyls (PCBs) on 14 July 2006 in Lake Superior using the modified Bowen ratio (MBR) method. Measured fluxes were compared to estimates using the W2F method, and to estimates from an Internal Boundary Layer Transport and Exchange (IBLTE) model that implements the NOAA COARE bulk flux algorithm and gas transfer model. We reveal an inaccuracy in the estimate of water vapor transfer velocity that is commonly used with the W2F method for PBT flux estimation, and demonstrate the effect of use of an improved estimation method. Flux measurements were conducted at three stations with increasing fetch in offshore flow (15, 30, and 60 km) in southeastern Lake Superior. This sampling strategy enabled comparison of measured and predicted flux, as well as modification in near-surface atmospheric concentration with fetch, using the IBLTE model. Fluxes estimated using the W2F model were compared to fluxes measured by MBR. In five of seven cases in which the MBR flux was significantly greater than zero, concentration increased with fetch at 1-m height, which is qualitatively consistent with the measured volatilization flux. As far as we are aware, these are the first reported ship-based micrometeorological air-water exchange flux measurements of PCBs.


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