scholarly journals Tropospheric nitrogen dioxide column retrieval from ground-based zenith–sky DOAS observations

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).


2014 ◽  
Vol 7 (3) ◽  
pp. 3021-3073 ◽  
Author(s):  
M. Grossi ◽  
P. Valks ◽  
D. Loyola ◽  
B. Aberle ◽  
S. Slijkhuis ◽  
...  

Abstract. The knowledge of the total column water vapour (TCWV) global distribution is fundamental for climate analysis and weather monitoring. In this work, we present the retrieval algorithm used to derive the operational TCWV from the GOME-2 sensors and perform an extensive inter-comparison and validation in order to estimate their absolute accuracy and long-term stability. We use the recently reprocessed data sets retrieved by the GOME-2 instruments aboard EUMETSAT's MetOp-A and MetOp-B satellites and generated by DLR in the framework of the O3M-SAF using the GOME Data Processor (GDP) version 4.7. The retrieval algorithm is based on a classical Differential Optical Absorption Spectroscopy (DOAS) method and combines H2O/O2 retrieval for the computation of the trace gas vertical column density. We introduce a further enhancement in the quality of the H2O column by optimizing the cloud screening and developing an empirical correction in order to eliminate the instrument scan angle dependencies. We evaluate the overall consistency between about 8 months measurements from the newer GOME-2 instrument on the MetOp-B platform with the GOME-2/MetOp-A data in the overlap period. Furthermore, we compare GOME-2 results with independent TCWV data from ECMWF and with SSMIS satellite measurements during the full period January 2007–August 2013 and we perform a validation against the combined SSM/I + MERIS satellite data set developed in the framework of the ESA DUE GlobVapour project. We find global mean biases as small as ± 0.03 g cm−2 between GOME-2A and all other data sets. The combined SSM/I-MERIS sample is typically drier than the GOME-2 retrievals (−0.005 g cm−2), while on average GOME-2 data overestimate the SSMIS measurements by only 0.028 g cm−2. However, the size of some of these biases are seasonally dependent. Monthly average differences can be as large as 0.1 g cm−2, based on the analysis against SSMIS measurements, but are not as evident in the validation with the ECMWF and the SSM/I + MERIS data. Studying two exemplary months, we estimate regional differences and identify a very good agreement between GOME-2 total columns and all three independent data sets, especially for land areas, although some discrepancies over ocean and over land areas with high humidity and a relatively large surface albedo are also present.


2014 ◽  
Vol 7 (11) ◽  
pp. 4009-4022 ◽  
Author(s):  
H. Diémoz ◽  
A. M. Siani ◽  
A. Redondas ◽  
V. Savastiouk ◽  
C. T. McElroy ◽  
...  

Abstract. A new algorithm to retrieve nitrogen dioxide (NO2) column densities using MKIV ("Mark IV") Brewer spectrophotometers is described. The method includes several improvements, such as a more recent spectroscopic data set, the reduction of measurement noise, interference by other atmospheric species and instrumental settings, and a better determination of the zenith sky air mass factor. The technique was tested during an ad hoc calibration campaign at the high-altitude site of Izaña (Tenerife, Spain) and the results of the direct sun and zenith sky geometries were compared to those obtained by two reference instruments from the Network for the Detection of Atmospheric Composition Change (NDACC): a Fourier Transform Infrared Radiometer (FTIR) and an advanced visible spectrograph (RASAS-II) based on the differential optical absorption spectrometry (DOAS) technique. To determine the extraterrestrial constant, an easily implementable extension of the standard Langley technique for very clean sites without tropospheric NO2 was developed which takes into account the daytime linear drift of stratospheric nitrogen dioxide due to photochemistry. The measurement uncertainty was thoroughly determined by using a Monte Carlo technique. Poisson noise and wavelength misalignments were found to be the most influential contributors to the overall uncertainty, and possible solutions are proposed for future improvements. The new algorithm is backward-compatible, thus allowing for the reprocessing of historical data sets.


2009 ◽  
Vol 9 (14) ◽  
pp. 4827-4840 ◽  
Author(s):  
M. L. Melamed ◽  
R. Basaldud ◽  
R. Steinbrecher ◽  
S. Emeis ◽  
L. G. Ruíz-Suárez ◽  
...  

Abstract. This work presents ground based differential optical absorption spectroscopy (DOAS) measurements of nitrogen dioxide (NO2) during the MILAGRO field campaign in March 2006 at the Tenango del Aire research site located to the southeast of Mexico City. The DOAS NO2 column density measurements are used in conjunction with ceilometer, meteorological and surface nitric oxide (NO), nitrogen oxides (NOx) and total reactive nitrogen (NOy) measurements to analyze pollution transport events to the southeast of Mexico City during the MILARGO field campaign. The study divides the data set into three case study pollution transport events that occurred at the Tenango del Aire research site. The unique data set is then used to provide an in depth analysis of example days of each of the pollution transport events. An in depth analysis of 13 March 2006, a Case One day, shows the transport of several air pollution plumes during the morning through the Tenango del Aire research site when southerly winds are present and demonstrates how DOAS tropospheric NO2 vertical column densities (VCD), surface NO2 mixing ratios and ceilometer data are used to determine the vertical homogeneity of the pollution layer. The analysis of 18 March 2006, a Case Two day, shows that when northerly winds are present for the entire day, the air at the Tenango del Aire research site is relatively clean and no major pollution plumes are detected. Case 3 days are characterized by relatively clean air throughout the morning with large DOAS NO2 enhancements detected in the afternoon. The analysis of 28 March 2006 show the DOAS NO2 enhancements are likely due to lightning activity and demonstrate how suitable ground-based DOAS measruements are for monitoring anthropogenic and natural pollution sources that reside above the mixing layer.


2020 ◽  
Author(s):  
Sebastian Iancu

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


2015 ◽  
Vol 8 (3) ◽  
pp. 1111-1133 ◽  
Author(s):  
M. Grossi ◽  
P. Valks ◽  
D. Loyola ◽  
B. Aberle ◽  
S. Slijkhuis ◽  
...  

Abstract. Knowledge of the total column water vapour (TCWV) global distribution is fundamental for climate analysis and weather monitoring. In this work, we present the retrieval algorithm used to derive the operational TCWV from the GOME-2 sensors aboard EUMETSAT's MetOp-A and MetOp-B satellites and perform an extensive inter-comparison in order to evaluate their consistency and temporal stability. For the analysis, the GOME-2 data sets are generated by DLR in the framework of the EUMETSAT O3M-SAF project using the GOME Data Processor (GDP) version 4.7. The retrieval algorithm is based on a classical Differential Optical Absorption Spectroscopy (DOAS) method and combines a H2O and O2 retrieval for the computation of the trace gas vertical column density. We introduce a further enhancement in the quality of the H2O total column by optimizing the cloud screening and developing an empirical correction in order to eliminate the instrument scan angle dependencies. The overall consistency between measurements from the newer GOME-2 instrument on board of the MetOp-B platform and the GOME-2/MetOp-A data is evaluated in the overlap period (December 2012–June 2014). Furthermore, we compare GOME-2 results with independent TCWV data from the ECMWF ERA-Interim reanalysis, with SSMIS satellite measurements during the full period January 2007–June 2014 and against the combined SSM/I + MERIS satellite data set developed in the framework of the ESA DUE GlobVapour project (January 2007–December 2008). Global mean biases as small as ±0.035 g cm−2 are found between GOME-2A and all other data sets. The combined SSM/I-MERIS sample and the ECMWF ERA-Interim data set are typically drier than the GOME-2 retrievals, while on average GOME-2 data overestimate the SSMIS measurements by only 0.006 g cm−2. However, the size of these biases is seasonally dependent. Monthly average differences can be as large as 0.1 g cm−2, based on the analysis against SSMIS measurements, which include only data over ocean. The seasonal behaviour is not as evident when comparing GOME-2 TCWV to the ECMWF ERA-Interim and the SSM/I+MERIS data sets, since the different biases over land and ocean surfaces partly compensate each other. Studying two exemplary months, we estimate regional differences and identify a very good agreement between GOME-2 total columns and all three data sets, especially for land areas, although some discrepancies (bias larger than ±0.5 g cm−2) over ocean and over land areas with high humidity or a relatively large surface albedo are observed.


2009 ◽  
Vol 9 (11) ◽  
pp. 3641-3662 ◽  
Author(s):  
D. Chen ◽  
B. Zhou ◽  
S. Beirle ◽  
L. M. Chen ◽  
T. Wagner

Abstract. Zenith-sky scattered sunlight observations using differential optical absorption spectroscopy (DOAS) technique were carried out in Shanghai, China (31.3° N, 121.5° E) since December 2006. At this polluted urban site, the measurements provided NO2 total columns in the daytime. Here, we present a new method to extract time series of tropospheric vertical column densities (VCDs) of NO2 from these observations. The derived tropospheric NO2 VCDs are important quantities for the estimation of emissions and for the validation of satellite observations. Our method makes use of assumptions on the relative NO2 height profiles and the diurnal variation of stratospheric NO2 VCDs. The main error sources arise from the uncertainties in the estimated stratospheric slant column densities (SCDs) and the determination of tropospheric NO2 air mass factor (AMF). For a polluted site like Shanghai, the accuracy of our method is conservatively estimated to be <25% for solar zenith angle (SZA) lower than 70°. From simultaneously performed long-path DOAS measurements, the NO2 surface concentrations at the same site were observed and the corresponding tropospheric NO2 VCDs were estimated using the assumed seasonal NO2 profiles in the planetary boundary layer (PBL). By making a comparison between the tropospheric NO2 VCDs from zenith-sky and long-path DOAS measurements, it is found that the former provides more realistic information about total tropospheric pollution than the latter, so it's more suitable for satellite data validation. A comparison between the tropospheric NO2 VCDs from ground-based zenith-sky measurements and SCIAMACHY was also made. Satellite validation for a strongly polluted area is highly needed, but exhibits also a great challenge. Our comparison shows good agreement, considering in particular the different spatial resolutions between the two measurements. Remaining systematic deviations are most probably related to the uncertainties of satellite data caused by the assumptions on aerosol properties as well as the layer heights of aerosols and NO2.


2015 ◽  
Vol 8 (12) ◽  
pp. 12663-12707 ◽  
Author(s):  
T. E. Taylor ◽  
C. W. O'Dell ◽  
C. Frankenberg ◽  
P. Partain ◽  
H. Q. Cronk ◽  
...  

Abstract. The objective of the National Aeronautics and Space Administration's (NASA) Orbiting Carbon Observatory-2 (OCO-2) mission is to retrieve the column-averaged carbon dioxide (CO2) dry air mole fraction (XCO2) from satellite measurements of reflected sunlight in the near-infrared. These estimates can be biased by clouds and aerosols within the instrument's field of view (FOV). Screening of the most contaminated soundings minimizes unnecessary calls to the computationally expensive Level 2 (L2) XCO2 retrieval algorithm. Hence, robust cloud screening methods have been an important focus of the OCO-2 algorithm development team. Two distinct, computationally inexpensive cloud screening algorithms have been developed for this application. The A-Band Preprocessor (ABP) retrieves the surface pressure using measurements in the 0.76 μm O2 A-band, neglecting scattering by clouds and aerosols, which introduce photon path-length (PPL) differences that can cause large deviations between the expected and retrieved surface pressure. The Iterative Maximum A-Posteriori (IMAP) Differential Optical Absorption Spectroscopy (DOAS) Preprocessor (IDP) retrieves independent estimates of the CO2 and H2O column abundances using observations taken at 1.61 μm (weak CO2 band) and 2.06 μm (strong CO2 band), while neglecting atmospheric scattering. The CO2 and H2O column abundances retrieved in these two spectral regions differ significantly in the presence of cloud and scattering aerosols. The combination of these two algorithms, which key off of different features in the spectra, provides the basis for cloud screening of the OCO-2 data set. To validate the OCO-2 cloud screening approach, collocated measurements from NASA's Moderate Resolution Imaging Spectrometer (MODIS), aboard the Aqua platform, were compared to results from the two OCO-2 cloud screening algorithms. With tuning to allow throughputs of &amp;simeq; 30 %, agreement between the OCO-2 and MODIS cloud screening methods is found to be &amp;simeq; 85 % over four 16-day orbit repeat cycles in both the winter (December) and spring (April–May) for OCO-2 nadir-land, glint-land and glint-water observations. No major, systematic, spatial or temporal dependencies were found, although slight differences in the seasonal data sets do exist and validation is more problematic with increasing solar zenith angle and when surfaces are covered in snow and ice and have complex topography. To further analyze the performance of the cloud screening algorithms, an initial comparison of OCO-2 observations was made to collocated measurements from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). These comparisons highlight the strength of the OCO-2 cloud screening algorithms in identifying high, thin clouds but suggest some difficulty in identifying some clouds near the surface, even when the optical thicknesses are greater than 1.


2013 ◽  
Vol 6 (1) ◽  
pp. 167-185 ◽  
Author(s):  
G. Pinardi ◽  
M. Van Roozendael ◽  
N. Abuhassan ◽  
C. Adams ◽  
A. Cede ◽  
...  

Abstract. We present intercomparison results for formaldehyde (HCHO) slant column measurements performed during the Cabauw Intercomparison campaign of Nitrogen Dioxide measuring Instruments (CINDI) that took place in Cabauw, the Netherlands, in summer 2009. During two months, nine atmospheric research groups simultaneously operated MAX-DOAS (MultiAXis Differential Optical Absorption Spectroscopy) instruments of various designs to record UV-visible spectra of scattered sunlight at different elevation angles that were analysed using common retrieval settings. The resulting HCHO data set was found to be highly consistent, the mean difference between instruments generally not exceeding 15% or 7.5 × 1015 molec cm−2, for all viewing elevation angles. Furthermore, a sensitivity analysis was performed to investigate the uncertainties in the HCHO slant column retrieval when varying key input parameters such as the molecular absorption cross sections, correction terms for the Ring effect or the width and position of the fitting interval. This study led to the identification of potentially important sources of errors associated with cross-correlation effects involving the Ring effect, O4, HCHO and BrO cross sections and the DOAS closure polynomial. As a result, a set of updated recommendations was formulated for HCHO slant column retrieval in the 336.5–359 nm wavelength range. To conclude, an error budget is proposed which distinguishes between systematic and random uncertainties. The total systematic error is estimated to be of the order of 20% and is dominated by uncertainties in absorption cross sections and related spectral cross-correlation effects. For a typical integration time of one minute, random uncertainties range between 5 and 30%, depending on the noise level of individual instruments.


2017 ◽  
Vol 10 (1) ◽  
pp. 119-153 ◽  
Author(s):  
Nicolas Theys ◽  
Isabelle De Smedt ◽  
Huan Yu ◽  
Thomas Danckaert ◽  
Jeroen van Gent ◽  
...  

Abstract. The TROPOspheric Monitoring Instrument (TROPOMI) onboard the Copernicus Sentinel-5 Precursor (S-5P) platform will measure ultraviolet earthshine radiances at high spectral and improved spatial resolution (pixel size of 7 km  ×  3.5 km at nadir) compared to its predecessors OMI and GOME-2. This paper presents the sulfur dioxide (SO2) vertical column retrieval algorithm implemented in the S-5P operational processor UPAS (Universal Processor for UV/VIS Atmospheric Spectrometers) and comprehensively describes its various retrieval steps. The spectral fitting is performed using the differential optical absorption spectroscopy (DOAS) method including multiple fitting windows to cope with the large range of atmospheric SO2 columns encountered. It is followed by a slant column background correction scheme to reduce possible biases or across-track-dependent artifacts in the data. The SO2 vertical columns are obtained by applying air mass factors (AMFs) calculated for a set of representative a priori profiles and accounting for various parameters influencing the retrieval sensitivity to SO2. Finally, the algorithm includes an error analysis module which is fully described here. We also discuss verification results (as part of the algorithm development) and future validation needs of the TROPOMI SO2 algorithm.


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