The information content of skylight polarisation in MAX-DOAS trace gas- and aerosol profiling applications 

Author(s):  
Jan-Lukas Tirpitz ◽  
Udo Frieß ◽  
Ulrich Platt

<p>Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a well-established measurement technique for the detection of atmospheric aerosol and trace gases: ultra-violet and visible radiation spectra of skylight are analyzed to obtain information on different atmospheric parameters. An appropriate set of spectra recorded under different viewing geometries ("Multi-Axis") allows retrieval of aerosol and trace gas vertical distributions as well as aerosol properties by applying numerical inversion methods. Currently one of the method’s major limitations in ground-based applications is the limited information contained in the measurements that reduces the sensitivity, particularly at higher altitudes.</p><p>It is well known but not yet used in MAX-DOAS profile retrievals that measuring skylight of different polarisation directions provides additional information: The degree of polarisation for instance strongly depends on the atmospheric aerosol content and the aerosol properties and – since the light path differs for the light of different polarisation -  the set of geometries available for the inversion is extended. We present a novel polarization-sensitive MAX-DOAS instrument (PMAX-DOAS) and a corresponding inversion algorithm, capable of using polarimetric information to significantly extend the information content of the measurements. The improvement over conventional “unpolarised” MAX-DOAS approaches will be discussed, based on both, synthetic data and real measurements.</p>

2020 ◽  
Author(s):  
Jan-Lukas Tirpitz ◽  
Udo Frieß ◽  
Ulrich Platt

<p>Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a well-established ground-based measurement technique for the detection of atmospheric aerosol and trace gases: ultra-violet and visible radiation spectra of skylight are analyzed to obtain information on different atmospheric parameters. An appropriate set of spectra recorded under different viewing geometries ("Multi-Axis") allows retrieval of aerosol and trace gas vertical distributions by applying numerical inversion methods. Currently one of the method’s major limitations is the limited information content in the measurements that reduces the sensitivity particularly at higher altitudes.</p><p>It is well known but not yet used in MAX-DOAS profile retrievals that measuring skylight of different polarisation directions provides additional information: the degree of polarisation for instance strongly depends on the atmospheric aerosol content and the aerosol properties and – since the light path (?) differs for light of different polarisation -  the set of geometries available for the inversion is extended. We present a novel polarization-sensitive MAX-DOAS instrument and a corresponding inversion algorithm, capable of using polarization information. Further, in contrast to existing MAX-DOAS algorithms consisting of separate aerosol and trace gas retrieval modules, our novel inversion scheme simultaneously retrieves aerosol and trace gas profiles of several species in a single step. The improvement over “unpolarised” MAX-DOAS approaches will be discussed, based on both, synthetic data and real measurements.</p>


2021 ◽  
Author(s):  
Jan-Lukas Tirpitz ◽  
Udo Frieß ◽  
Robert Spurr ◽  
Ulrich Platt

Abstract. Ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a widely-used measurement technique for the remote detection of atmospheric aerosol and trace gases. The technique relies on the analysis ultra-violet and visible radiation spectra of scattered sunlight (skylight) to obtain information on different atmospheric parameters. From an appropriate set of spectra recorded under different viewing directions (typically a group of observations at different elevation angles) the retrieval of aerosol and trace gas vertical distributions is achieved through numerical inversion methods. It is well known that the polarisation state of skylight is particularly sensitive to atmospheric aerosol content as well as aerosol properties, and that polarimetric measurement could therefore provide additional information for MAX-DOAS profile retrievals; however such measurement have not yet been used for this purpose. To address this issue, we have developed the RAPSODI (Retrieval of Atmospheric Parameters from Spectroscopic Observations using DOAS Instruments) algorithm. In contrast to existing MAX-DOAS algorithms, it can process polarimetric information, and it can retrieve simultaneously profiles of aerosols and various trace gases at multiple wavelengths in a single retrieval step; a further advantage is that it contains a Mie scattering model, allowing for the retrieval aerosol microphysical properties. The forward model component in RAPSODI is based on a linearized vector radiative transfer model with Jacobian facilities, and we have used this model to create a data base of synthetic measurements in order to carry out sensitivity analyses aimed at assessing the potential of polarimetric MAX-DOAS observations. We find that multispectral polarimetry significantly enhances the sensitivity, particularly to aerosol related quantities. Assuming typical viewing geometries, the degree of freedom for signal (DFS) increases by about 50 % and 70 % for aerosol vertical distributions and aerosol properties, respectively, and by approximately 10 % for trace gas vertical profiles. For an idealised scenario with a horizontally homogeneous atmosphere, our findings predict an improvement in the inversions results' accuracy (root-mean-square deviations to the true values) of about 60 % for aerosol VCDs as well as for aerosol surface concentrations, and by 40 % for aerosol properties. For trace gas VCDs, very little improvement is apparent, although the accuracy of trace gas surface concentrations improves by about 50 %.


2020 ◽  
Author(s):  
Jan-Lukas Tirpitz ◽  
Udo Frieß ◽  
François Hendrick ◽  
Carlos Alberti ◽  
Marc Allaart ◽  
...  

Abstract. Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a well-established ground-based measurement technique for the detection of aerosols and trace gases particularly in the boundary layer and the lower troposphere: ultraviolet- and visible radiation spectra of skylight are analysed to obtain information on different atmospheric parameters, integrated over the light path from space to the instrument. An appropriate set of spectra recorded under different viewing geometries ("Multi-Axis") allows retrieval of tropospheric aerosol and trace gas vertical distributions by applying numerical inversion methods. The second Cabauw Intercomparison of Nitrogen Dioxide measuring Instruments (CINDI-2) took place in Cabauw (The Netherlands) in September 2016 with the aim of assessing the consistency of MAX-DOAS measurements of tropospheric species (NO2, HCHO, O3, HONO, CHOCHO and O4). This was achieved through the coordinated operation of 36 spectrometers operated by 24 groups from all over the world, together with a wide range of supporting reference observations (in situ analysers, balloon sondes, lidars, Long-Path DOAS, sun photometer and others). In the presented study, the retrieved CINDI-2 MAX-DOAS trace gas (NO2, HCHO) and aerosol vertical profiles of 15 participating groups using different inversion algorithms are compared and validated against the colocated supporting observations. The profiles were found to be in good qualitative agreement: most participants obtained the same features in the retrieved vertical trace gas and aerosol distributions, however sometimes at different altitudes and of different intensity. Under clear sky conditions, the root-mean-square differences of aerosol optical thicknesses, trace gas (NO2, HCHO) vertical columns and surface concentrations among the results of individual participants vary between 0.01–0.1, (1.5–15) x 1014 molec cm-2 and (0.3–8) x 1010 molec cm-3, respectively. For the comparison against supporting observations, these values increase to 0.02–0.2, (11–55) x 1014 molec cm-2 and (0.8–9) x 1010 molec cm-3. It is likely that a large part of this increase is caused by imperfect spatio-temporal overlap of the different observations. In contrast to what is often assumed, the MAX-DOAS vertically integrated extinction profiles and the sun photometer total aerosol optical thickness were found to not necessarily being comparable quantities, unless information on the real aerosol vertical distribution is available to account for the low sensitivity of MAX-DOAS observations at higher altitudes.


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.


2005 ◽  
Vol 5 (5) ◽  
pp. 10747-10797
Author(s):  
A. Butz ◽  
H. Bösch ◽  
C. Camy-Peyret ◽  
M. Chipperfield ◽  
M. Dorf ◽  
...  

Abstract. Stratospheric O3 and NO2 abundances measured by different remote sensing instruments are inter-compared: (1) Line-of-sight absorptions and vertical profiles inferred from solar spectra in the ultra-violet (UV), visible and infrared (IR) wavelength ranges measured by the LPMA/DOAS (Limb Profile Monitor of the Atmosphere/Differential Optical Absorption Spectroscopy) balloon payload during balloon ascent/descent and solar occultation are examined with respect to internal consistency. (2) The balloon borne stratospheric profiles of O3 and NO2 are compared to collocated space-borne skylight limb observations of the Envisat/SCIAMACHY satellite instrument. The trace gas profiles are retrieved from SCIAMACHY spectra using different algorithms developed at the Universities of Bremen and Heidelberg and at the Harvard-Smithsonian Center for Astrophysics. A comparison scheme is used that accounts for the spatial and temporal mismatch as well as differing photochemical conditions between the balloon and satellite borne measurements. It is found that the balloon borne measurements internally agree to within ±10% and ±20% for O3 and NO2, respectively, whereas the agreement with the satellite is ±20% for both gases in the 20 km to 30 km altitude range and in general worse below 20 km.


2006 ◽  
Vol 6 (5) ◽  
pp. 1293-1314 ◽  
Author(s):  
A. Butz ◽  
H. Bösch ◽  
C. Camy-Peyret ◽  
M. Chipperfield ◽  
M. Dorf ◽  
...  

Abstract. Stratospheric O3 and NO2 abundances measured by different remote sensing instruments are inter-compared: (1) Line-of-sight absorptions and vertical profiles inferred from solar spectra in the ultra-violet (UV), visible and infrared (IR) wavelength ranges measured by the LPMA/DOAS (Limb Profile Monitor of the Atmosphere/Differential Optical Absorption Spectroscopy) balloon payload during balloon ascent/descent and solar occultation are examined with respect to internal consistency. (2) The balloon borne stratospheric profiles of O3 and NO2 are compared to collocated space-borne skylight limb observations of the Envisat/SCIAMACHY satellite instrument. The trace gas profiles are retrieved from SCIAMACHY spectra using different algorithms developed at the Universities of Bremen and Heidelberg and at the Harvard-Smithsonian Center for Astrophysics. A comparison scheme is used that accounts for the spatial and temporal mismatch as well as differing photochemical conditions between the balloon and satellite borne measurements. It is found that the balloon borne measurements internally agree to within ±10% and ±20% for O3 and NO2, respectively, whereas the agreement with the satellite is ±20% for both gases in the 20 km to 30 km altitude range and in general worse below 20 km.


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

Abstract. Ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a state of the art remote sensing technique for deriving vertical profiles of trace gases and aerosols. However, MAX-DOAS profile inversions under aerosol pollution scenarios are challenging because of the complex radiative transfer and limited information content of the measurements. In this study, the performances of two inversion algorithms were evaluated for various aerosol pollution scenarios based on synthetic slant column densities (SCDs) derived from radiative transfer simulations. One inversion algorithm is based on optimal estimation, the other uses a parameterized approach. In this analysis, 3 types of profile shapes for aerosols and NO2 were considered: exponential, Boltzmann, and Gaussian. First, the systematic deviations of the retrieved aerosol profiles from the input profiles were investigated. For most cases, the AODs of the retrieved profiles were found to be systematically lower than the input values, and the deviations increased with increasing AOD. Especially for the optimal estimation algorithm and for high AOD, these findings might explain part of the deviations between the AOD retrieved from MAX-DOAS and sun photometers in previous studies. For the optimal estimation algorithm the agreement with the input values can be improved by optimizing the covariance matrix of the a priori uncertainties. Second, the aerosol effects on the NO2 profile retrieval were tested. Here, especially for the optimal estimation algorithm, a systematic dependence on the NO2 VCD was found with a strong relative overestimation of the retrieved results for low NO2 VCDs and an underestimation for high NO2 VCDs. In contrast, the dependence on the aerosol profiles was found to be rather low. In general, both inversion schemes can well retrieve the near-surface values of aerosol extinction and trace gases concentrations.


2014 ◽  
Vol 8 (3) ◽  
pp. 143-149 ◽  
Author(s):  
Ferdinando De Tomasi ◽  
Maria Rita Perrone

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