scholarly journals Intercomparison of MAX-DOAS Vertical Profile Retrieval Algorithms: Studies using Synthetic Data

2018 ◽  
Author(s):  
Udo Frieß ◽  
Steffen Beirle ◽  
Leonardo Alvarado Bonilla ◽  
Tim Bösch ◽  
Martina M. Friedrich ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Trace Gases ◽  
Estimation Method ◽  
Synthetic Data ◽  
Optimal Estimation ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Vertical Profiles ◽  
Retrieval Algorithms ◽  
Transfer Modelling

Abstract. Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a widely used measurement technique for the detection of a variety of atmospheric trace gases. Using inverse modelling, the observation of trace gas column densities along different lines of sight enables the retrieval of aerosol and trace gas vertical profiles in the atmospheric boundary layer using appropriate retrieval algorithms. In this study, the ability of eight profile retrieval algorithms to reconstruct vertical profiles is assessed on the basis of synthetic measurements. Five of the algorithms are based on the optimal estimation method, two on parametrised approaches, and one using an analytical approach without involving any radiative transfer modelling. The synthetic measurements consist of the median of simulated slant column densities of O4 at 360 nm and 477 nm, as well as of HCHO at 343 nm and NO2 at 477 nm, from seven datasets simulated by five different radiative transfer models. Simulations are performed for a combination of 10 trace gas and 11 aerosol profiles, as well as 11 elevation angles, 3 solar 10 zenith and 3 relative azimuth angles. Overall, the results from the different algorithms show moderate to good performance for the retrieval of vertical profiles, surface concentrations and total columns. Except for some outliers, the root mean squares difference between true and retrieved state ranges between (0:05–0:1) km1 for aerosol extinction, and (2:5–5:0) × 1010 molec/cm3 for HCHO and NO2 concentrations.

scholarly journals Intercomparison of MAX-DOAS vertical profile retrieval algorithms: studies using synthetic data

2019 ◽  
Vol 12 (4) ◽  
pp. 2155-2181 ◽  
Author(s):  
Udo Frieß ◽  
Steffen Beirle ◽  
Leonardo Alvarado Bonilla ◽  
Tim Bösch ◽  
Martina M. Friedrich ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Trace Gases ◽  
Estimation Method ◽  
Synthetic Data ◽  
Optimal Estimation ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Vertical Profiles ◽  
Retrieval Algorithms ◽  
Mean Square Difference

Abstract. Multi-axis differential optical absorption spectroscopy (MAX-DOAS) is a widely used measurement technique for the detection of a variety of atmospheric trace gases. Using inverse modelling, the observation of trace gas column densities along different lines of sight enables the retrieval of aerosol and trace gas vertical profiles in the atmospheric boundary layer using appropriate retrieval algorithms. In this study, the ability of eight profile retrieval algorithms to reconstruct vertical profiles is assessed on the basis of synthetic measurements. Five of the algorithms are based on the optimal estimation method, two on parametrised approaches, and one using an analytical approach without involving any radiative transfer modelling. The synthetic measurements consist of the median of simulated slant column densities of O4 at 360 and 477 nm, as well as of HCHO at 343 nm and NO2 at 477 nm, from seven datasets simulated by five different radiative transfer models. Simulations are performed for a combination of 10 trace gas and 11 aerosol profiles, as well as 11 elevation angles, three solar zenith, and three relative azimuth angles. Overall, the results from the different algorithms show moderate to good performance for the retrieval of vertical profiles, surface concentrations, and total columns. Except for some outliers, the root-mean-square difference between the true and retrieved state ranges between (0.05–0.1) km−1 for aerosol extinction and (2.5–5.0) ×1010 molec cm−3 for HCHO and NO2 concentrations.

scholarly journals Inter-comparison of MAX-DOAS measurements of tropospheric HONO slant column densities and vertical profiles during the CINDI-2 campaign

2020 ◽  
Vol 13 (9) ◽  
pp. 5087-5116 ◽  
Author(s):  
Yang Wang ◽  
Arnoud Apituley ◽  
Alkiviadis Bais ◽  
Steffen Beirle ◽  
Nuria Benavent ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Estimation Method ◽  
Optimal Estimation ◽  
Early Morning ◽  
Optical Absorption Spectroscopy ◽  
Data Sets ◽  
Vertical Profiles ◽  
Near Surface ◽  
Mixing Ratios ◽  
Profile Inversion

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.

scholarly journals Technical note: Evaluation of profile retrievals of aerosols and trace gases for MAX-DOAS measurements under different aerosol scenarios based on radiative transfer simulations

2021 ◽  
Vol 21 (17) ◽  
pp. 12867-12894
Author(s):  
Xin Tian ◽  
Yang Wang ◽  
Steffen Beirle ◽  
Pinhua Xie ◽  
Thomas Wagner ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Trace Gases ◽  
Optimal Estimation ◽  
Estimation Algorithm ◽  
Optical Absorption Spectroscopy ◽  
Limited Information ◽  
Inversion Algorithm ◽  
Vertical Column ◽  
Near Surface ◽  
Aerosol Pollution

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.

scholarly journals Inter-comparison of MAX-DOAS measurements of tropospheric HONO slant column densities and vertical profiles during the CINDI-2 Campaign

2020 ◽  
Author(s):  
Yang Wang ◽  
Arnoud Apituley ◽  
Alkiviadis Bais ◽  
Steffen Beirle ◽  
Nuria Benavent ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Estimation Method ◽  
Optimal Estimation ◽  
Early Morning ◽  
Radiative Transfer Model ◽  
Measuring Instruments ◽  
Transfer Model ◽  
Vertical Profiles ◽  
Near Surface ◽  
Profile Inversion

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.

scholarly journals Impact of 3D Cloud Structures on the Atmospheric Trace Gas Products from UV-VIS Sounders – Part I: Synthetic dataset for validation of trace gas retrieval algorithms

2021 ◽  
Author(s):  
Claudia Emde ◽  
Huan Yu ◽  
Arve Kylling ◽  
Michel van Roozendael ◽  
Kerstin Stebel ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
3D Structure ◽  
Three Dimensional ◽  
Synthetic Data ◽  
Synthetic Dataset ◽  
Trace Gas ◽  
Transfer Model ◽  
Retrieval Error ◽  
Retrieval Algorithms ◽  
The Impact

Abstract. Retrievals of trace gas concentrations from satellite observations are mostly performed for clear regions or regions with low cloud coverage. However, even fully clear pixels can be affected by clouds in the vicinity, either by shadowing or by scattering of radiation from clouds in the clear region. Quantifying the error of retrieved trace gas concentrations due to cloud scattering is a difficult task. One possibility is to generate synthetic data by three-dimensional (3D) radiative transfer simulations using realistic 3D atmospheric input data, including 3D cloud structures. Retrieval algorithms may be applied on the synthetic data and comparison to the known input trace gas concentrations yields the retrieval error due to cloud scattering. In this paper we present a comprehensive synthetic dataset which has been generated using the Monte Carlo radiative transfer model MYSTIC. The dataset includes simulated spectra in two spectral ranges (400–500 nm and the O2A-band from 755–775 nm). Moreover it includes layer air mass factors (layer-AMF) calculated at 460 nm. All simulations are performed for a fixed background atmosphere for various sun positions, viewing directions and surface albedos. Two cloud setups are considered: The first includes simple box-clouds with various geometrical and optical thicknesses. This can be used to systematically investigate the sensitivity of the retrieval error on solar zenith angle, surface albedo and cloud parameters. Corresponding 1D simulations are also provided. The second includes realistic three-dimensional clouds from an ICON large eddy simulation (LES) for a region covering Germany and parts of surrounding countries. The scene includes cloud types typical for central Europe such as shallow cumulus, convective cloud cells, cirrus, and stratocumulus. This large dataset can be used to quantify the trace gas concentration retrieval error statistically. Along with the dataset the impact of horizontal photon transport on reflectance spectra and layer-AMFs is analyzed for the box-cloud scenarios. Moreover, the impact of 3D cloud scattering on the NO2 vertical column density (VCD) retrieval is presented for a specific LES case. We find that the retrieval error is largest in cloud shadow regions, where the NO2 VCD is underestimated by more than 20 %. The dataset is available for the scientific community to assess the behavior of trace gas retrieval algorithms and cloud correction schemes in cloud conditions with 3D structure.

Retrieval of vertical concentration profiles from OSIRIS UV–visible limb spectra

2002 ◽  
Vol 80 (4) ◽  
pp. 409-434 ◽  
Author(s):  
K Strong ◽  
B M Joseph ◽  
R Dosanjh ◽  
I C McDade ◽  
C A McLinden ◽  
...  
Keyword(s):  
Optical Absorption ◽  
Absorption Spectroscopy ◽  
Optimal Estimation ◽  
Gas Absorption ◽  
Forward Model ◽  
Differential Optical Absorption Spectroscopy ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Vertical Profiles ◽  
Uv Visible

The OSIRIS instrument, launched on the Odin satellite in February 2001, includes an optical spectrograph that will record UV–visible spectra of sunlight scattered from the limb over a range of tangent heights. These spectra will be used to retrieve vertical profiles of ozone, NO2, OClO, BrO, NO3, O2, and aerosols, for the investigation of both stratospheric and mesospheric processes, particularly those related to ozone chemistry. In this work, the retrieval of vertical profiles of trace-gas concentrations from OSIRIS limb-radiance spectra is described. A forward model has been developed to simulate these spectra, and it consists of a single-scattering radiative-transfer model with partial spherical geometry, trace-gas absorption, Mie scattering by stratospheric aerosols, a Lambertian surface contribution, and OSIRIS instrument response and noise. Number-density profiles have been retrieved by using optimal estimation (OE) to combine an a priori profile with the information from sets of synthetic ``measurements''. For ozone, OE has been applied both to limb radiances at one or more discrete wavelengths and to effective-column abundances retrieved over a broad spectral range using differential optical absorption spectroscopy (DOAS). The results suggest that, between 15 and 35 km, ozone number densities can be retrieved to 10% accuracy or better on 1 and 2 km grids and to 5% on a 5 km grid. The combined DOAS-OE approach has also been used to retrieve NO2 number densities, yielding 13% accuracy or better for altitudes from 18 to 36 km on a 2 km grid. Differential optical absorption spectroscopy – optimal estimation retrievals of BrO and OClO reproduce the true profiles above 15 km in the noise-free case, but the quality of the retrievals is highly sensitive to noise on the simulated OSIRIS spectra because of the weak absorption of these two gases. The development of inversion methods for the retrieval of trace-gas concentrations from OSIRIS spectra is continuing, and a number of future improvements to the forward model and refinements of the retrieval algorithms are identified. PACS Nos.: 42.68Mj, 94.10Dy

scholarly journals Quantification and parameterization of non-linearity effects by higher order sensitivity terms in scattered light Differential Optical Absorption Spectroscopy

2016 ◽  
Author(s):  
Jānis Puķīte ◽  
Thomas Wagner
Keyword(s):  
Radiative Transfer ◽  
Optical Absorption ◽  
Absorption Spectroscopy ◽  
Scattered Light ◽  
Higher Order ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Non Linear ◽  
Linear Effects ◽  
Transfer Modelling

Abstract. We address the application of Differential Optical Absorption Spectroscopy (DOAS) of scattered light observations in the presence of strong absorbers (in particular ozone), for which the absorption optical depth is a non-linear function of the trace gas concentration. This is the case, because Beer-Lambert law generally does not hold for scattered light measurements due to many light paths contributing to the measurement. While in many cases linear approximation can be made, for scenarios with strong absorptions non-linear effects cannot always be neglected. This is especially the case for observation geometries, for which the light contributing to the measurement is crossing the atmosphere under spatially well separated paths differing strongly in length and location, like e.g. in limb geometry. In these cases, often full retrieval algorithms are applied to address the non-linearities requiring iterative forward modelling of absorption spectra involving time consuming wavelength by wavelength radiative transfer modelling. In this study, we propose to describe the non-linear effects by additional sensitivity parameters that can be used e.g. to build up a look up table. Together with widely used box air mass factors (effective light paths) describing the linear response to the increase in the trace gas amount, the higher order sensitivity parameters eliminate the need for repeating the radiative transfer modelling when modifying the absorption scenario even in presence of a strong absorption background. While the higher order absorption structures can be described as separate fit parameters in the spectral analysis (so called DOAS fit), in practice their quantitative evaluation requires good measurement quality (typically better than that available from current measurements). Therefore, we introduce an iterative retrieval algorithm correcting for the higher or- der absorption structures not yet considered in the DOAS fit as well as the absorption dependence on temperature and scattering processes.

scholarly journals Retrieval of tropospheric aerosol, NO<sub>2</sub> and HCHO vertical profiles from MAX-DOAS observations over Thessaloniki, Greece

2021 ◽  
Author(s):  
Dimitris Karagkiozidis ◽  
Martina Michaela Friedrich ◽  
Steffen Beirle ◽  
Alkiviadis Bais ◽  
François Hendrick ◽  
...  
Keyword(s):  
Estimation Method ◽  
Correlation Coefficients ◽  
Scaling Factor ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Systematic Bias ◽  
Vertical Profiles ◽  
Ancillary Data ◽  
Tropospheric Aerosol ◽  
Good Agreement

Abstract. In this study we focus on the retrieval of aerosol and trace gas vertical profiles from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations for the first time over Thessaloniki, Greece. We use two independent inversion algorithms for the profile retrievals: The Mexican MAX-DOAS Fit (MMF) and the Mainz Profile Algorithm (MAPA). The former is based on the Optimal Estimation Method (OEM), while the latter follows a parameterization approach. We evaluate the performance of MMF and MAPA and we validate their retrieved products with ancillary data measured by other co-located reference instruments. We find an excellent agreement between the tropospheric column densities of NO2 retrieved by MMF and MAPA (Slope = 1.009, Pearson's correlation coefficient R = 0.982) and a good correlation for the case of HCHO (R = 0.927). For aerosols, we find better agreement for the aerosol optical depths (AODs) in the visible (i.e., at 477 nm), compared to the UV (360 nm) and we show that the agreement strongly depends on the O4 scaling factor that is used in the analysis. The trace gas differential slant column densities (dSCDs), simulated by the forward models, are also in good agreement, except for HCHO, where larger scatter is observed due to the increased spectral noise of the measurements in the UV. The agreement for NO2 and HCHO surface concentrations is similar to the comparison of the integrated columns with slightly decreased correlation coefficients. The AODs retrieved by the MAX-DOAS are validated by comparing them with AOD values measured by a CIMEL sun-photometer and a Brewer spectrophotometer. Four different flagging schemes were applied to the data in order to evaluate their performance. Qualitatively, a generally good agreement is observed for both wavelengths, but we find a systematic bias from the CIMEL and Brewer measurements, due to the limited sensitivity of the MAX-DOAS in retrieving information at higher altitudes, especially in the UV. An in-depth validation of the aerosol vertical profiles retrieved by the MAX-DOAS is not possible since only in very few cases the true aerosol profile is known during the period of study. However, we examine four cases, where the MAX-DOAS provided a generally good estimation of the shape of the profiles retrieved by a co-located multi-wavelength lidar system. The NO2 surface concentrations are validated against in situ observations and the comparison of both MMF and MAPA revealed good agreement with correlation coefficients of R = 0.78 and R = 0.73, respectively. Finally, the effect of the O4 scaling factor is investigated by intercomparing the integrated columns retrieved by the two algorithms and also by comparing the AODs derived by MAPA for different values of the scaling factor with AODs measured by the CIMEL and the Brewer.

scholarly journals Quantification and parametrization of non-linearity effects by higher-order sensitivity terms in scattered light differential optical absorption spectroscopy

2016 ◽  
Vol 9 (5) ◽  
pp. 2147-2177 ◽  
Author(s):  
Jānis Puķīte ◽  
Thomas Wagner
Keyword(s):  
Radiative Transfer ◽  
Optical Absorption ◽  
Absorption Spectroscopy ◽  
Scattered Light ◽  
Higher Order ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Non Linear ◽  
Linear Effects ◽  
Transfer Modelling

Abstract. We address the application of differential optical absorption spectroscopy (DOAS) of scattered light observations in the presence of strong absorbers (in particular ozone), for which the absorption optical depth is a non-linear function of the trace gas concentration. This is the case because Beer–Lambert law generally does not hold for scattered light measurements due to many light paths contributing to the measurement. While in many cases linear approximation can be made, for scenarios with strong absorptions non-linear effects cannot always be neglected. This is especially the case for observation geometries, for which the light contributing to the measurement is crossing the atmosphere under spatially well-separated paths differing strongly in length and location, like in limb geometry. In these cases, often full retrieval algorithms are applied to address the non-linearities, requiring iterative forward modelling of absorption spectra involving time-consuming wavelength-by-wavelength radiative transfer modelling. In this study, we propose to describe the non-linear effects by additional sensitivity parameters that can be used e.g. to build up a lookup table. Together with widely used box air mass factors (effective light paths) describing the linear response to the increase in the trace gas amount, the higher-order sensitivity parameters eliminate the need for repeating the radiative transfer modelling when modifying the absorption scenario even in the presence of a strong absorption background. While the higher-order absorption structures can be described as separate fit parameters in the spectral analysis (so-called DOAS fit), in practice their quantitative evaluation requires good measurement quality (typically better than that available from current measurements). Therefore, we introduce an iterative retrieval algorithm correcting for the higher-order absorption structures not yet considered in the DOAS fit as well as the absorption dependence on temperature and scattering processes.

3D Remote Sensing of Trace Gas Distributions with HAIDI (Heidelberg Airborne Imaging DOAS Instrument) - Power Plant and Ship Emissions observed during the EMeRGe Campaigns

2021 ◽  
Author(s):  
Katja Bigge ◽  
Udo Frieß ◽  
Denis Pöhler ◽  
Ulrich Platt
Keyword(s):  
Remote Sensing ◽  
Radiative Transfer ◽  
Power Plants ◽  
Trace Gases ◽  
Trace Gas ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
Flight Altitude ◽  
Airborne Imaging

&lt;p&gt;&lt;span&gt;Compared to ground-based or satellite measurements, atmospheric observations based on aircraft missions have many advantages, such as the potential to observe a large atmospheric volume using remote sensing measurements, among which Differential Optical Absorption Spectroscopy (DOAS) is a well established method for the observation of integrated trace gas concentrations along the light path. However, the interpretation of remote spectroscopic measurements using scattered sunlight is complicated due to the lack of prior knowledge on the light paths between sun and detector, and thus on the observed air volume. Using radiative transfer calculations, quantities commonly derived from DOAS measurements are integrated vertical columns of various trace gases, providing no information about their vertical distribution.&lt;/span&gt;&lt;/p&gt;&lt;p&gt;&lt;span&gt;On the ground, tomographic approaches have been used to reconstruct the spatial distribution of trace gases by using multiple viewing directions and detectors. &lt;!-- Bislang eigentlich h&amp;#246;chstens 2D (P&amp;#246;hler et al) oder 1D (MAX-DOAS Profil-retrieval) --&gt;HAIDI, the Heidelberg Airborne Imaging DOAS Instrument, was designed to transfer this concept to the air. In addition to its excellent temporal and spatial resolution (40 m x 40 m at 1.5 km flight altitude, 266 m x 266 m at 10 km flight altitude, at 10 ms temporal resolution), HAIDI uses three separate scanning telescopes aimed at +/-45&amp;#176; forward- and backward looking angles and the nadir direction. In combination with a 3D radiative transfer model, this allows a reconstruction of the 3D distribution of the detected trace gases in the vicinity of the flight track.&lt;/span&gt;&lt;/p&gt;&lt;p&gt;&lt;span&gt;HAIDI joined the EMerGe (Effect of Megacities on the Transport and transformation of Pollutants on the Regional to Global Scales) missions on HALO, the High Altitude and LOng range research aircraft based at DLR (German Aerospace Center) in Oberpfaffenhofen, Germany. The EMerGe missions targeted the emission outflows of megacities to investigate their compositions and the atmospheric impact of urban pollution in Europe (July 2017) and Asia (March 2018). HAIDI observed a number of trace gases such as NO&lt;sub&gt;2,&lt;/sub&gt; SO&lt;sub&gt;2&lt;/sub&gt; and HCHO. For NO&lt;sub&gt;2&lt;/sub&gt; and SO&lt;sub&gt;2&lt;/sub&gt; in particular, strong plumes originating from power plants and ships were found, which were then used for inversion of the 3D distribution of the plume and emission estimation. Here we present the method and results of the HAIDI measurements during the EMeRGe missions.&lt;/span&gt;&lt;/p&gt;

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