scholarly journals Retrieval of absolute SO<sub>2</sub> column amounts from scattered-light spectra – Implications for the evaluation of data from automated DOAS Networks

Author(s):  
Peter Lübcke ◽  
Johannes Lampel ◽  
Santiago Arellano ◽  
Nicole Bobrowski ◽  
Florian Dinger ◽  
...  

Abstract. Scanning Differential Optical Absorption Spectroscopy (DOAS) networks using scattered solar radiation have become an increasingly important tool for monitoring volcanic sulphur dioxide (SO2) emissions. In order to get absolute column densities (CDs), the DOAS evaluation requires a Fraunhofer Reference Spectrum (FRS) that is free of absorption structures of the trace gas of interest. At volcanoes, this requirement can be formulated in a weaker form, if there is a plume free viewing direction within the spectra of a scan through the complete sky. In this case, it is possible to use a specific viewing direction (e.g. zenith) as FRS and correcting for possible plume contamination in the FRS by calculating and subtracting an SO2 offset (e.g. the lowest SO2 CD) from all viewing directions of the respective scan. This procedure is followed in the standard evaluations of data from the Network for Observation of Volcanic and Atmospheric Change (NOVAC). While this procedure is very efficient in removing Fraunhofer structures and instrumental effects it has the disadvantage that one can never be sure that there is no SO2 from the plume in the FRS. Therefore, using a modelled FRS (based on a high-resolution Solar atlas) is of great advantage. We followed this approach and investigated an SO2 retrieval algorithm using a modelled FRS. In this manuscript, we present results from two volcanoes that are monitored by NOVAC stations and which also often show a large volcanic plume. Results from a DOAS SO2 evaluation using a modelled FRS are presented for data from Nevado del Ruiz (Colombia) recorded between January 2010 and June 2012 and from Tungurahua (Ecuador) recorded between January 2009 and December 2011. Instrumental effects were identified with help of a Principal Component Analysis (PCA) of the residual structures of the DOAS evaluation. The SO2 retrieval performed extraordinarily well with an SO2 DOAS retrieval error of 1−2 × 1016 [molecules/cm2]. Compared to a regular evaluation (using a FRS recorded directly before the scan), we found systematic differences of the differential Slant Column Density (dSCD) of only up to 15 % when looking at the variation of the SO2 within one scan. The major advantage of our new retrieval is that it yields absolute SO2 CDs and that it does not require complicated instrumental calibration in the field, since the method exploits the information available in the measurements.

2016 ◽  
Vol 9 (12) ◽  
pp. 5677-5698 ◽  
Author(s):  
Peter Lübcke ◽  
Johannes Lampel ◽  
Santiago Arellano ◽  
Nicole Bobrowski ◽  
Florian Dinger ◽  
...  

Abstract. Scanning spectrometer networks using scattered solar radiation in the ultraviolet spectral region have become an increasingly important tool for monitoring volcanic sulfur dioxide (SO2) emissions. Often measured spectra are evaluated using the differential optical absorption spectroscopy (DOAS) technique. In order to obtain absolute column densities (CDs), the DOAS evaluation requires a Fraunhofer reference spectrum (FRS) that is free of absorption structures of the trace gas of interest. For measurements at volcanoes such a FRS can be readily obtained if the scan (i.e. series of measurements at different elevation angles) includes viewing directions where the plume is not seen. In this case, it is possible to use these viewing directions (e.g. zenith) as FRS. Possible contaminations of the FRS by the plume can then be corrected by calculating and subtracting an SO2 offset (e.g. the lowest SO2 CD) from all viewing directions of the respective scan. This procedure is followed in the standard evaluations of data from the Network for Observation of Volcanic and Atmospheric Change (NOVAC). While this procedure is very efficient in removing Fraunhofer structures and instrumental effects it has the disadvantage that one can never be sure that there is no SO2 from the plume in the FRS. Therefore, using a modelled FRS (based on a high-resolution solar atlas) has a great advantage. We followed this approach and investigated an SO2 retrieval algorithm using a modelled FRS. In this paper, we present results from two volcanoes that are monitored by NOVAC stations and which frequently emit large volcanic plumes: Nevado del Ruiz (Colombia) recorded between January 2010 and June 2012 and from Tungurahua (Ecuador) recorded between January 2009 and December 2011. Instrumental effects were identified with help of a principal component analysis (PCA) of the residual structures of the DOAS evaluation. The SO2 retrieval performed extraordinarily well with an SO2 DOAS retrieval error of 1 − 2 × 1016 [molecules cm−2]. Compared to a standard evaluation, we found systematic differences of the differential slant column density (dSCD) of only up to  ≈ 15 % when looking at the variation of the SO2 within one scan. The major advantage of our new retrieval is that it yields absolute SO2 CDs and that it does not require complicated instrumental calibration in the field (e.g. by employing calibration cells or broadband light sources), since the method exploits the information available in the measurements.We compared our method to an evaluation that is similar to the NOVAC approach, where a spectrum that is recorded directly before the scan is used as an FRS and an SO2 CD offset is subtracted from all retrieved dSCD in the scan to correct for possible SO2 contamination of the FRS. The investigation showed that 21.4 % of the scans (containing significant amounts of SO2) at Nevado del Ruiz and 7 % of the scans at Tungurahua showed much larger SO2 CDs when evaluated using modelled FRS (more than a factor of 2). For standard evaluations the overall distribution of the SO2 CDs in a scan can in some cases indicate whether the plume affects all viewing directions and thus these scans need to be discarded for NOVAC emission rate evaluation. However, there are other cases where this is not possible and thus the reported SO2 emission rates would be underestimated. The new method can be used to identify these cases and thus it can considerably improve SO2 emission budgets.


2015 ◽  
Vol 8 (6) ◽  
pp. 2417-2435 ◽  
Author(s):  
F. Tack ◽  
F. Hendrick ◽  
F. Goutail ◽  
C. Fayt ◽  
A. Merlaud ◽  
...  

Abstract. We present an algorithm for retrieving tropospheric nitrogen dioxide (NO2) vertical column densities (VCDs) from ground-based zenith–sky (ZS) measurements of scattered sunlight. The method is based on a four-step approach consisting of (1) the differential optical absorption spectroscopy (DOAS) analysis of ZS radiance spectra using a fixed reference spectrum corresponding to low NO2 absorption, (2) the determination of the residual amount in the reference spectrum using a Langley-plot-type method, (3) the removal of the stratospheric content from the daytime total measured slant column based on stratospheric VCDs measured at sunrise and sunset, and simulation of the rapid NO2 diurnal variation, (4) the retrieval of tropospheric VCDs by dividing the resulting tropospheric slant columns by appropriate air mass factors (AMFs). These steps are fully characterized and recommendations are given for each of them. The retrieval algorithm is applied on a ZS data set acquired with a multi-axis (MAX-) DOAS instrument during the Cabauw (51.97° N, 4.93° E, sea level) Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI) held from 10 June to 21 July 2009 in the Netherlands. A median value of 7.9 × 1015 molec cm−2 is found for the retrieved tropospheric NO2 VCDs, with maxima up to 6.0 × 1016 molec cm−2. The error budget assessment indicates that the overall error σTVCD on the column values is less than 28%. In the case of low tropospheric contribution, σTVCD is estimated to be around 39% and is dominated by uncertainties in the determination of the residual amount in the reference spectrum. For strong tropospheric pollution events, σTVCD drops to approximately 22% with the largest uncertainties on the determination of the stratospheric NO2 abundance and tropospheric AMFs. The tropospheric VCD amounts derived from ZS observations are compared to VCDs retrieved from off-axis and direct-sun measurements of the same MAX-DOAS instrument as well as to data from a co-located Système d'Analyse par Observations Zénithales (SAOZ) spectrometer. The retrieved tropospheric VCDs are in good agreement with the different data sets with correlation coefficients and slopes close to or larger than 0.9. The potential of the presented ZS retrieval algorithm is further demonstrated by its successful application on a 2-year data set, acquired at the NDACC (Network for the Detection of Atmospheric Composition Change) station Observatoire de Haute Provence (OHP; Southern France).


2015 ◽  
Vol 8 (1) ◽  
pp. 935-985
Author(s):  
F. Tack ◽  
F. Hendrick ◽  
F. Goutail ◽  
C. Fayt ◽  
A. Merlaud ◽  
...  

Abstract. We present an algorithm for retrieving tropospheric nitrogen dioxide (NO2) vertical column densities (VCDs) from ground-based zenith-sky (ZS) measurements of scattered sunlight. The method is based on a four-step approach consisting of (1) the Differential Optical Absorption Spectroscopy (DOAS) analysis of ZS radiance spectra using a fixed reference spectrum corresponding to low NO2 absorption, (2) the determination of the residual amount in the reference spectrum using a Langley-plot-type method, (3) the removal of the stratospheric content from the daytime total measured slant column based on stratospheric VCDs measured at sunrise and sunset, and simulation of the rapid NO2 diurnal variation, (4) the retrieval of tropospheric VCDs by dividing the resulting tropospheric slant columns by appropriate air mass factors (AMFs). These steps are fully characterized and recommendations are given for each of them. The retrieval algorithm is applied on a ZS dataset acquired with a Multi-AXis (MAX-) DOAS instrument during the Cabauw (51.97° N, 4.93° E, sea level) Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI) held from the 10 June to the 21 July 2009 in the Netherlands. A median value of 7.9 × 1015 molec cm−2 is found for the retrieved tropospheric NO2 VCDs, with maxima up to 6.0 × 1016 molec cm−2. The error budget assessment indicates that the overall error σTVCD on the column values is less than 28%. In case of low tropospheric contribution, σTVCD is estimated to be around 39% and is dominated by uncertainties in the determination of the residual amount in the reference spectrum. For strong tropospheric pollution events, σTVCD drops to approximately 22% with the largest uncertainties on the determination of the stratospheric NO2 abundance and tropospheric AMFs. The tropospheric VCD amounts derived from ZS observations are compared to VCDs retrieved from off-axis and direct-sun measurements of the same MAX-DOAS instrument as well as to data from a co-located Système d'Analyse par Observations Zénithales (SAOZ) spectrometer. The retrieved tropospheric VCDs are in good agreement with the different datasets with correlation coefficients and slopes close to or larger than 0.9. The potential of the presented ZS retrieval algorithm is further demonstrated by its successful application on a 2 year dataset, acquired at the NDACC (Network for the Detection of Atmospheric Composition Change) station Observatoire de Haute Provence (OHP; Southern France).


2006 ◽  
Vol 6 (11) ◽  
pp. 3517-3534 ◽  
Author(s):  
M. P. Barkley ◽  
U. Frieß ◽  
P. S. Monks

Abstract. Satellite measurements of atmospheric CO2 concentrations are a rapidly evolving area of scientific research which can help reduce the uncertainties in the global carbon cycle fluxes and provide insight into surface sources and sinks. One of the emerging CO2 measurement techniques is a relatively new retrieval algorithm called Weighting Function Modified Differential Optical Absorption Spectroscopy (WFM-DOAS) that has been developed by Buchwitz et al. (2000). This algorithm is designed to measure the total columns of CO2 (and other greenhouse gases) through the application to spectral measurements in the near infrared (NIR), made by the SCIAMACHY instrument on-board ENVISAT. The algorithm itself is based on fitting the logarithm of a model reference spectrum and its derivatives to the logarithm of the ratio of a measured nadir radiance and solar irradiance spectrum. In this work, a detailed error assessment of this technique has been conducted and it has been found necessary to include suitable a priori information within the retrieval in order to minimize the errors on the retrieved CO2 columns. Hence, a more flexible implementation of the retrieval technique, called Full Spectral Initiation (FSI) WFM-DOAS, has been developed which generates a reference spectrum for each individual SCIAMACHY observation using the estimated properties of the atmosphere and surface at the time of the measurement. Initial retrievals over Siberia during the summer of 2003 show that the measured CO2 columns are not biased from the input a priori data and that whilst the monthly averaged CO2 distributions contain a high degree of variability, they also contain interesting spatial features.


2021 ◽  
Author(s):  
Nicolas Theys ◽  
Vitali Fioletov ◽  
Can Li ◽  
Isabelle De Smedt ◽  
Christophe Lerot ◽  
...  

Abstract. Sensitive and accurate detection of sulfur dioxide (SO2) from space is important for monitoring and estimating global sulfur emissions. Inspired by detection methods applied in the thermal infrared, we present here a new scheme to retrieve SO2 columns from satellite observations of ultraviolet back-scattered radiances. The retrieval is based on a measurement error covariance matrix to fully represent the SO2-free radiance variability, so that the SO2 slant column density is the only retrieved parameter of the algorithm. We demonstrate this approach, named COBRA, on measurements from the TROPOspheric Monitoring Instrument (TROPOMI) aboard the Sentinel-5 Precursor (S-5P) satellite. We show that the method reduces significantly both the noise and biases present in the current TROPOMI operational DOAS SO2 retrievals. The performance of this technique is also benchmarked against that of the Principal Component Algorithm (PCA) approach. We find that the quality of the data is similar and even slightly better with the proposed COBRA approach. The ability of the algorithm to retrieve SO2 accurately is also further supported by comparison with ground-based observations. We illustrate the great sensitivity of the method with a high-resolution global SO2 map, considering two and a half years of TROPOMI data. In addition to the known sources, we detect many new SO2 emission hotspots worldwide. For the largest sources, we use the COBRA data to estimate SO2 emission rates. Results are comparable to other recently published TROPOMI-based SO2 emissions estimates, but the associated uncertainties are significantly lower than with the operational data. Next, for a limited number of weak sources, we demonstrate the potential of our data for quantifying SO2 emissions with a detection limit of about 8 kt yr-1, a factor of 4 better than the emissions derived from the Ozone Monitoring Instrument (OMI). We anticipate that the systematic use of our TROPOMI COBRA SO2 column data set at a global scale will allow identifying and quantifying missing sources, and help improving SO2 emission inventories.


2006 ◽  
Vol 6 (2) ◽  
pp. 2765-2807 ◽  
Author(s):  
M. P. Barkley ◽  
U. Frieß ◽  
P. S. Monks

Abstract. Satellite measurements of atmospheric CO2 concentrations are a rapidly evolving area of scientific research which can help reduce the uncertainties in the global carbon cycle fluxes and provide insight into surface sources and sinks. One of the emerging CO2 measurement techniques is a relatively new retrieval algorithm called Weighting Function Modified Differential Optical Absorption Spectroscopy (WFM-DOAS) that has been developed by Buchwitz et al. (2000). This algorithm is designed to measure the total columns of CO2 (and other greenhouse gases) through the application to spectral measurements in the near infrared (NIR), made by the SCIAMACHY instrument on-board ENVISAT. The algorithm itself is based on fitting the logarithm of a model reference spectrum and its derivatives to the logarithm of the ratio of a measured nadir radiance and solar irradiance spectrum. In this work, a detailed error assessment of this technique has been conducted and it has been found necessary to include suitable a priori information within the retrieval in order to minimize the errors on the retrieved CO2 columns. Hence, a new CO2 retrieval algorithm called Full Spectral Initiation (FSI) WFM-DOAS has been developed which generates a reference spectrum for each individual SCIAMACHY observation using the known properties of the atmosphere and surface at the time of the measurement. Initial retrievals over Siberia during the summer of 2003 show that the measured CO2 columns are not biased from the input a priori data and that whilst the monthly averaged CO2 distributions contain a high degree of variability, they also contain significant spatial features.


2021 ◽  
Vol 21 (22) ◽  
pp. 16727-16744
Author(s):  
Nicolas Theys ◽  
Vitali Fioletov ◽  
Can Li ◽  
Isabelle De Smedt ◽  
Christophe Lerot ◽  
...  

Abstract. Sensitive and accurate detection of sulfur dioxide (SO2) from space is important for monitoring and estimating global sulfur emissions. Inspired by detection methods applied in the thermal infrared, we present here a new scheme to retrieve SO2 columns from satellite observations of ultraviolet back-scattered radiances. The retrieval is based on a measurement error covariance matrix to fully represent the SO2-free radiance variability, so that the SO2 slant column density is the only retrieved parameter of the algorithm. We demonstrate this approach, named COBRA, on measurements from the TROPOspheric Monitoring Instrument (TROPOMI) aboard the Sentinel-5 Precursor (S-5P) satellite. We show that the method reduces significantly both the noise and biases present in the current TROPOMI operational DOAS SO2 retrievals. The performance of this technique is also benchmarked against that of the principal component algorithm (PCA) approach. We find that the quality of the data is similar and even slightly better with the proposed COBRA approach. The ability of the algorithm to retrieve SO2 accurately is further supported by comparison with ground-based observations. We illustrate the great sensitivity of the method with a high-resolution global SO2 map, considering 2.5 years of TROPOMI data. In addition to the known sources, we detect many new SO2 emission hotspots worldwide. For the largest sources, we use the COBRA data to estimate SO2 emission rates. Results are comparable to other recently published TROPOMI-based SO2 emissions estimates, but the associated uncertainties are significantly lower than with the operational data. Next, for a limited number of weak sources, we demonstrate the potential of our data for quantifying SO2 emissions with a detection limit of about 8 kt yr−1, a factor of 4 better than the emissions derived from the Ozone Monitoring Instrument (OMI). We anticipate that the systematic use of our TROPOMI COBRA SO2 column data set at a global scale will allow missing sources to be identified and quantified and help improve SO2 emission inventories.


2021 ◽  
Vol 13 (1) ◽  
pp. 152
Author(s):  
Haklim Choi ◽  
Xiong Liu ◽  
Gonzalo Gonzalez Abad ◽  
Jongjin Seo ◽  
Kwang-Mog Lee ◽  
...  

Clouds act as a major reflector that changes the amount of sunlight reflected to space. Change in radiance intensity due to the presence of clouds interrupts the retrieval of trace gas or aerosol properties from satellite data. In this paper, we developed a fast and robust algorithm, named the fast cloud retrieval algorithm, using a triplet of wavelengths (469, 477, and 485 nm) of the O2–O2 absorption band around 477 nm (CLDTO4) to derive the cloud information such as cloud top pressure (CTP) and cloud fraction (CF) for the Geostationary Environment Monitoring Spectrometer (GEMS). The novel algorithm is based on the fact that the difference in the optical path through which light passes with regard to the altitude of clouds causes a change in radiance due to the absorption of O2–O2 at the three selected wavelengths. To reduce the time required for algorithm calculations, the look-up table (LUT) method was applied. The LUT was pre-constructed for various conditions of geometry using Vectorized Linearized Discrete Ordinate Radiative Transfer (VLIDORT) to consider the polarization of the scattered light. The GEMS was launched in February 2020, but the observed data of GEMS have not yet been widely released. To evaluate the performance of the algorithm, the retrieved CTP and CF using observational data from the Global Ozone Monitoring Experiment-2 (GOME-2), which cover the spectral range of GEMS, were compared with the results of the Fast Retrieval Scheme for Clouds from the Oxygen A band (FRESCO) algorithm, which is based on the O2 A-band. There was good agreement between the results, despite small discrepancies for low clouds.


Mathematics ◽  
2020 ◽  
Vol 8 (11) ◽  
pp. 1970
Author(s):  
Jun-Kyu Park ◽  
Suwoong Lee ◽  
Aaron Park ◽  
Sung-June Baek

In spectroscopy, matching a measured spectrum to a reference spectrum in a large database is often computationally intensive. To solve this problem, we propose a novel fast search algorithm that finds the most similar spectrum in the database. The proposed method is based on principal component transformation and provides results equivalent to the traditional full search method. To reduce the search range, hierarchical clustering is employed, which divides the spectral data into multiple clusters according to the similarity of the spectrum, allowing the search to start at the cluster closest to the input spectrum. Furthermore, a pilot search was applied in advance to further accelerate the search. Experimental results show that the proposed method requires only a small fraction of the computational complexity required by the full search, and it outperforms the previous methods.


2021 ◽  
Vol 13 (11) ◽  
pp. 2098
Author(s):  
Yuanyuan Qian ◽  
Yuhan Luo ◽  
Fuqi Si ◽  
Haijin Zhou ◽  
Taiping Yang ◽  
...  

Global measurements of total ozone are necessary to evaluate ozone hole recovery above Antarctica. The Environmental Trace Gases Monitoring Instrument (EMI) onboard GaoFen 5, launched in May 2018, was developed to measure and monitor the global total ozone column (TOC) and distributions of other trace gases. In this study, some of the first global TOC results of the EMI using the differential optical absorption spectroscopy (DOAS) method and validation with ground-based TOC measurements and data derived from Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI) observations are presented. Results show that monthly average EMI TOC data had a similar spatial distribution and a high correlation coefficient (R ≥ 0.99) with both OMI and TROPOMI TOC. Comparisons with ground-based measurements from the World Ozone and Ultraviolet Radiation Data Centre also revealed strong correlations (R > 0.9). Continuous zenith sky measurements from zenith scattered light differential optical absorption spectroscopy instruments in Antarctica were also used for validation (R = 0.9). The EMI-derived observations were able to account for the rapid change in TOC associated with the sudden stratospheric warming event in October 2019; monthly average TOC in October 2019 was 45% higher compared to October 2018. These results indicate that EMI TOC derived using the DOAS method is reliable and has the potential to be used for global TOC monitoring.


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