scholarly journals Advanced NO<sub>2</sub> retrieval technique for the Brewer spectrophotometer applied to the 20-year record in Rome, Italy

2021 ◽  
Vol 13 (10) ◽  
pp. 4929-4950
Author(s):  
Henri Diémoz ◽  
Anna Maria Siani ◽  
Stefano Casadio ◽  
Anna Maria Iannarelli ◽  
Giuseppe Rocco Casale ◽  
...  

Abstract. A re-evaluated data set of nitrogen dioxide (NO2) column densities over Rome for the years 1996 to 2017 is here presented. This long-term record is obtained from ground-based direct sun measurements with a MkIV Brewer spectrophotometer (serial number #067) and further reprocessed using a novel algorithm. Compared to the original Brewer algorithm, the new method includes updated NO2 absorption cross sections and Rayleigh scattering coefficients, and it accounts for additional atmospheric compounds and instrumental artefacts, such as the spectral transmittance of the filters, the alignment of the wavelength scale, and internal temperature. Moreover, long-term changes in the Brewer radiometric sensitivity are tracked using statistical methods for in-field calibration. The resulting series presents only a few (about 30) periods with missing data longer than 1 week and features NO2 retrievals for more than 6100 d, covering nearly 80 % of the considered 20-year period. The high quality of the data is demonstrated by two independent comparisons. In the first intensive campaign, Brewer #067 is compared against another Brewer (#066), recently calibrated at the Izaña Atmospheric Observatory through the Langley method and there compared to reference instrumentation from the Network for the Detection of Atmospheric Composition Change (NDACC). Data from this campaign show a highly significant Pearson's correlation coefficient of 0.90 between the two series of slant column densities (SCDs), slope 0.98 and offset 0.05 DU (Dobson units; 1.3×1015 molec.cm-2). The average bias between the vertical column densities is 0.03 DU (8.1×1014 molec.cm-2), well within the combined uncertainty of both instruments. Brewer #067 is also independently compared with new-generation instrumentation, a co-located Pandora spectrometer (#117), over a 1-year-long period (2016–2017) at Sapienza University of Rome, showing linear correlation indices above 0.96 between slant column densities, slope of 0.97, and offset of 0.02 DU (5.4×1014 molec.cm-2). The average bias between vertical column densities is negligible (−0.002 DU or -5.4×1013 molec.cm-2). This, incidentally, represents the first intercomparison of NO2 retrievals between a MkIV Brewer and a Pandora instrument. Owing to its accuracy and length, the Brewer data set collected in Rome can be useful for satellite calibration/validation exercises, comparison with photochemical models, and better aerosol optical depth estimates (NO2 optical depth climatology). In addition, it can be employed to identify long-term trends in NO2 column densities in a metropolitan environment, over two decades witnessing important changes in environmental policies, emission loads and composition, and the effect of a worldwide economic recession, to offer just a few examples. The method can be replicated on the more than 80 MkIV spectrophotometers operating worldwide in the frame of the international Brewer network. The NO2 data set described in this paper can be freely accessed at https://doi.org/10.5281/zenodo.4715219 (Diémoz and Siani, 2021).

2021 ◽  
Author(s):  
Henri Diémoz ◽  
Anna Maria Siani ◽  
Stefano Casadio ◽  
Anna Maria Iannarelli ◽  
Giuseppe Rocco Casale ◽  
...  

Abstract. A re-evaluated data set of nitrogen dioxide (NO2) column densities over Rome for the years 1996 to 2017 is here presented. This long-term record is obtained from ground-based direct sun measurements with a MkIV Brewer spectrophotometer (#067), further reprocessed using a novel algorithm. Compared to the original Brewer algorithm, the new method includes updated NO2 absorption cross sections and Rayleigh scattering coefficients, and accounts for additional atmospheric compounds and instrumental artefacts, such as the spectral transmittance of the filters, the alignment of the wavelength scale and internal temperature. Moreover, long-term changes in the Brewer radiometric sensitivity are tracked using statistical methods for in-field calibration. The resulting series presents only few (about 30) periods with missing data longer than one week and features NO2 retrievals in more than 6100 days, covering nearly 80 % of the considered 20-year period. The high quality of the data is demonstrated by two independent comparisons. In a first intensive campaign, Brewer #067 is compared against another Brewer (#066), recently calibrated at the Izaña Atmospheric Observatory through the Langley method and there compared to reference instrumentation from the Network for the Detection of Atmospheric Composition Change (NDACC). Data from this campaign show a highly significant Pearson's correlation coefficient of 0.90 between the two series of slant column densities, slope 0.98 and offset 0.05 DU (1.3 × 1015 molec cm−2). The average bias between the vertical column densities is 0.03 DU (8.1 ×1014 molec cm−2), well within the combined uncertainty of both instruments. Brewer #067 is also independently compared with new-generation instrumentation, a co-located Pandora spectrometer (#117), over a 1-year long period (2016–2017) at Sapienza University of Rome, showing linear correlation indices above 0.96 between slant column densities, slope of 0.97 and offset of 0.02 DU (5.4 × 1014 molec cm−2). The average bias between vertical column densities is negligible (−0.002 DU or −5.4 × 1013 molec cm−2). This, incidentally, represents the first intercomparison of NO2 retrievals between a MkIV Brewer and a Pandora instrument. Owing to its accuracy and length, the Brewer data set collected in Rome can be useful for satellite cal/val exercises, comparison with photochemical models, and for better aerosol optical depth estimates (NO2 optical depth climatology). In addition, it can be employed to identify long-term trends in NO2 column densities over a metropolitan environment, during two decades witnessing important changes in environmental policies, emission loads and composition, and the effect of a worldwide economic recession, to offer just a few examples. The method can be replicated on the more than 80 MkIV spectrophotometers operating worldwide in the frame of the international Brewer network. The NO2 data set described in this manuscript can be freely accessed at https://doi.org/10.5281/zenodo.4715219 (Diémoz and Siani, 2021).


2010 ◽  
Vol 10 (8) ◽  
pp. 20405-20460
Author(s):  
F. Hendrick ◽  
J.-P. Pommereau ◽  
F. Goutail ◽  
R. D. Evans ◽  
D. Ionov ◽  
...  

Abstract. Accurate long-term monitoring of total ozone is one of the most important requirements for identifying possible natural or anthropogenic changes in the composition of the stratosphere. For this purpose, the NDACC (Network for the Detection of Atmospheric Composition Change) UV-visible Working Group has made recommendations for improving and homogenizing the retrieval of total ozone columns from twilight zenith-sky visible spectrometers. These instruments, deployed all over the world in about 35 stations, allow measurements of total ozone twice daily with little sensitivity to stratospheric temperature and cloud cover. The NDACC recommendations address both the DOAS retrieval parameters and the calculation of air mass factors (AMF) needed for the conversion of O3 slant column densities into vertical column amounts. The most important improvement is the use of O3 AMF look-up tables calculated using the TOMS V8 O3 profile climatology, that allows accounting for the dependence of the O3 AMF on the seasonal and latitudinal variations of the O3 vertical distribution. To investigate their impact on the retrieved ozone columns, the recommendations have been applied to measurements from the NDACC/SAOZ (Système d'Analyse par Observation Zénithale) network. The revised SAOZ ozone data from eight stations covering all latitude regions have been compared to TOMS, GOME-GDP4, SCIAMACHY-TOSOMI, OMI-TOMS, and OMI-DOAS satellite overpass observations, as well as to those of collocated Dobson and Brewer instruments. A significant improvement is obtained after applying the new O3 AMFs, although systematic seasonal differences between SAOZ and all other instruments remain. These are shown to mainly originate from i) the temperature dependence of the ozone absorption cross sections in the UV being not or improperly corrected by some retrieval algorithms, and ii) the longitudinal differences in tropospheric ozone column being ignored by zonal climatologies. For those measurements sensitive to stratospheric temperature like TOMS, OMI-TOMS, Dobson and Brewer, the application of a temperature correction results in the almost complete removal of the seasonal difference with SAOZ, improving significantly the consistency between all ground-based and satellite total ozone observations.


2011 ◽  
Vol 11 (12) ◽  
pp. 5975-5995 ◽  
Author(s):  
F. Hendrick ◽  
J.-P. Pommereau ◽  
F. Goutail ◽  
R. D. Evans ◽  
D. Ionov ◽  
...  

Abstract. Accurate long-term monitoring of total ozone is one of the most important requirements for identifying possible natural or anthropogenic changes in the composition of the stratosphere. For this purpose, the NDACC (Network for the Detection of Atmospheric Composition Change) UV-visible Working Group has made recommendations for improving and homogenizing the retrieval of total ozone columns from twilight zenith-sky visible spectrometers. These instruments, deployed all over the world in about 35 stations, allow measuring total ozone twice daily with limited sensitivity to stratospheric temperature and cloud cover. The NDACC recommendations address both the DOAS spectral parameters and the calculation of air mass factors (AMF) needed for the conversion of O3 slant column densities into vertical column amounts. The most important improvement is the use of O3 AMF look-up tables calculated using the TOMS V8 (TV8) O3 profile climatology, that allows accounting for the dependence of the O3 AMF on the seasonal and latitudinal variations of the O3 vertical distribution. To investigate their impact on the retrieved ozone columns, the recommendations have been applied to measurements from the NDACC/SAOZ (Système d'Analyse par Observation Zénithale) network. The revised SAOZ ozone data from eight stations deployed at all latitudes have been compared to TOMS, GOME-GDP4, SCIAMACHY-TOSOMI, SCIAMACHY-OL3, OMI-TOMS, and OMI-DOAS satellite overpass observations, as well as to those of collocated Dobson and Brewer instruments at Observatoire de Haute Provence (44° N, 5.5° E) and Sodankyla (67° N, 27° E), respectively. A significantly better agreement is obtained between SAOZ and correlative reference ground-based measurements after applying the new O3 AMFs. However, systematic seasonal differences between SAOZ and satellite instruments remain. These are shown to mainly originate from (i) a possible problem in the satellite retrieval algorithms in dealing with the temperature dependence of the ozone cross-sections in the UV and the solar zenith angle (SZA) dependence, (ii) zonal modulations and seasonal variations of tropospheric ozone columns not accounted for in the TV8 profile climatology, and (iii) uncertainty on the stratospheric ozone profiles at high latitude in the winter in the TV8 climatology. For those measurements mostly sensitive to stratospheric temperature like TOMS, OMI-TOMS, Dobson and Brewer, or to SZA like SCIAMACHY-TOSOMI, the application of temperature and SZA corrections results in the almost complete removal of the seasonal difference with SAOZ, improving significantly the consistency between all ground-based and satellite total ozone observations.


2014 ◽  
Vol 14 (15) ◽  
pp. 7909-7927 ◽  
Author(s):  
Y. Kanaya ◽  
H. Irie ◽  
H. Takashima ◽  
H. Iwabuchi ◽  
H. Akimoto ◽  
...  

Abstract. We conducted long-term network observations using standardized Multi-Axis Differential optical absorption spectroscopy (MAX-DOAS) instruments in Russia and ASia (MADRAS) from 2007 onwards and made the first synthetic data analysis. At seven locations (Cape Hedo, Fukue and Yokosuka in Japan, Hefei in China, Gwangju in Korea, and Tomsk and Zvenigorod in Russia) with different levels of pollution, we obtained 80 927 retrievals of tropospheric NO2 vertical column density (TropoNO2VCD) and aerosol optical depth (AOD). In the technique, the optimal estimation of the TropoNO2VCD and its profile was performed using aerosol information derived from O4 absorbances simultaneously observed at 460–490 nm. This large data set was used to analyze NO2 climatology systematically, including temporal variations from the seasonal to the diurnal scale. The results were compared with Ozone Monitoring Instrument (OMI) satellite observations and global model simulations. Two NO2 retrievals of OMI satellite data (NASA ver. 2.1 and Dutch OMI NO2 (DOMINO) ver. 2.0) generally showed close correlations with those derived from MAX-DOAS observations, but had low biases of up to ~50%. The bias was distinct when NO2 was abundantly present near the surface and when the AOD was high, suggesting a possibility of incomplete accounting of NO2 near the surface under relatively high aerosol conditions for the satellite observations. Except for constant biases, the satellite observations showed nearly perfect seasonal agreement with MAX-DOAS observations, suggesting that the analysis of seasonal features of the satellite data were robust. Weekend reduction in the TropoNO2VCD found at Yokosuka and Gwangju was absent at Hefei, implying that the major sources had different weekly variation patterns. While the TropoNO2VCD generally decreased during the midday hours, it increased exceptionally at urban/suburban locations (Yokosuka, Gwangju, and Hefei) during winter. A global chemical transport model, MIROC-ESM-CHEM (Model for Interdisciplinary Research on Climate–Earth System Model–Chemistry), was validated for the first time with respect to background NO2 column densities during summer at Cape Hedo and Fukue in the clean marine atmosphere.


2018 ◽  
Vol 11 (6) ◽  
pp. 3339-3350 ◽  
Author(s):  
Andreas Schneider ◽  
Tobias Borsdorff ◽  
Joost aan de Brugh ◽  
Haili Hu ◽  
Jochen Landgraf

Abstract. A new data set of vertical column densities of the water vapour isotopologues H2O and HDO from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument for the whole of the mission period from January 2003 to April 2012 is presented. The data are retrieved from reflectance measurements in the spectral range 2339 to 2383 nm with the Shortwave Infrared CO Retrieval (SICOR) algorithm, ignoring atmospheric light scattering in the measurement simulation. The retrievals are validated with ground-based Fourier transform infrared measurements obtained within the Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) project. A good agreement for low-altitude stations is found with an average bias of −3.6×1021 for H2O and −1.0×1018 molec cm−2 for HDO. The a posteriori computed δD shows an average bias of −8 ‰, even though polar stations have a larger negative bias. The latter is due to the large amount of sensor noise in SCIAMACHY in combination with low albedo and high solar zenith angles. To demonstrate the benefit of accounting for light scattering in the retrieval, the quality of the data product fitting effective cloud parameters simultaneously with trace gas columns is evaluated in a dedicated case study for measurements round high-altitude stations. Due to a large altitude difference between the satellite ground pixel and the mountain station, clear-sky scenes yield a large bias, resulting in a δD bias of 125 ‰. When selecting scenes with optically thick clouds within 1000 m above or below the station altitude, the bias in a posteriori δD is reduced from 125 to 44 ‰. The insights from the present study will also benefit the analysis of the data from the new Sentinel-5 Precursor mission.


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).


2013 ◽  
Vol 13 (17) ◽  
pp. 8643-8650 ◽  
Author(s):  
B. J. Connor ◽  
T. Mooney ◽  
G. E. Nedoluha ◽  
J. W. Barrett ◽  
A. Parrish ◽  
...  

Abstract. We present a re-analysis of upper stratospheric ClO measurements from the ground-based millimeter-wave instrument from January 1992 to February 2012. These measurements are made as part of the Network for the Detection of Atmospheric Composition Change (NDACC) from Mauna Kea, Hawaii, (19.8° N, 204.5° E). Here, we use daytime and nighttime measurements together to form a day–night spectrum, from which the difference in the day and night profiles is retrieved. These results are then compared to the day–night difference profiles from the Upper Atmosphere Research Satellite (UARS) and Aura Microwave Limb Sounder (MLS) instruments. We also compare them to our previous analyses of the same data, in which we retrieved the daytime ClO profile. The major focus will be on comparing the year-to-year and long-term changes in ClO derived by the two analysis methods, and comparing these results to the long-term changes reported by others. We conclude that the re-analyzed data set has less short-term variability and exhibits a more constant long-term trend that is more consistent with other observations. Data from 1995 to 2012 indicate a linear decline of mid-stratospheric ClO of 0.64 ± 0.15% yr−1 (2σ).


2018 ◽  
Author(s):  
Robin Wing ◽  
Alain Hauchecorne ◽  
Philippe Keckhut ◽  
Sophie Godin-Beekmann ◽  
Sergey Khaykin ◽  
...  

Abstract. The objective of this paper and its companion (Wing et al., 2018b) is to show that ground based lidar temperatures are a stable, accurate and precise dataset for use in validating satellite temperatures at high vertical resolution. Long-term lidar observations of the middle atmosphere have been conducted at the Observatoire de Haute-Provence (OHP), located in southern France (43.93° N, 5.71° E), since 1978. Making use of 20 years of high-quality co-located lidar measurements we have shown that lidar temperatures calculated using the Rayleigh technique at 532 nm are statistically identical to lidar temperatures calculated from the non-absorbing 355 nm channel of a Differential Absorption Lidar (DIAL) system. This result is of interest to members of the Network for the Detection of Atmospheric Composition Change (NDACC) ozone lidar community seeking to produce validated temperature products. Additionally, we have addressed previously published concerns of lidar-satellite relative warm bias in comparisons of Upper Mesospheric and Lower Thermospheric (UMLT) temperature profiles. We detail a data treatment algorithm which minimizes known errors due to data selection procedures, a priori choices, and initialization parameters inherent in the lidar retrieval. Our algorithm results in a median cooling of the lidar calculated absolute temperature profile by 20 K at 90 km altitude with respect to the standard OHP NDACC lidar temperature algorithm. The confidence engendered by the long-term cross-validation of two independent lidars and the improved lidar temperature dataset is exploited in (Wing et al., 2018b) for use in multi-year satellite validations.


2018 ◽  
Author(s):  
Andreas Schneider ◽  
Tobias Borsdorff ◽  
Joost aan de Brugh ◽  
Haili Hu ◽  
Jochen Landgraf

Abstract. A new data set of vertical column densities of the water vapour isotopologues H₂O and HDO from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) instrument for the whole mission period from January 2003 to April 2012 is presented. The data are retrieved from reflectance measurements in the spectral range 2339 nm to 2383 nm with the Shortwave Infrared CO Retrieval (SICOR) algorithm, ignoring atmospheric light scattering in the measurement simulation. The retrievals are validated with ground-based Fourier transform infrared measurements obtained within the Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) project. A good agreement for low-altitude stations is found with an average bias of −3.6·1021 molec cm−2 for HO and −1.0·1018molec cm−2 for HDO. The a posteriori computed δD shows an average bias of −8 ‰, even though polar stations have a larger negative bias. The latter is due to large sensor noise of SCIAMACHY in combination with low albedo and high solar zenith angles. To demonstrate the benefit of accounting for light scattering in the retrieval, the quality of the data product fitting effective cloud parameters simultaneously with trace gas columns is evaluated in a dedicated case study for measurements round high altitude stations. Due to a large altitude difference between the satellite ground pixel and the mountain station, clear sky scenes yield a large bias, resulting in a δD bias of 125 ‰. When selecting scenes with optically thick clouds within 1000 m above or below the station altitude, the bias in a posteriori δD is reduced from 125 ‰ to 44 ‰. The insights from the present study will also benefit the analysis of the data from the new Sentinel 5 Precursor mission.


1999 ◽  
Vol 17 (2) ◽  
pp. 231-241 ◽  
Author(s):  
K. Petzoldt

Abstract. Total ozone anomalies (deviation from the long-term mean) are created by anomalous circulation patterns. The dynamically produced ozone anomalies can be estimated from known circulation parameters in the layer between the tropopause and the middle stratosphere by means of statistics. Satellite observations of ozone anomalies can be compared with those expected from dynamics. Residual negative anomalies may be due to chemical ozone destruction. The statistics are derived from a 14 year data set of TOMS (Total Ozone Mapping Spectrometer January 1979-Dec. 1992) and corresponding 300 hPa geopotential (for the tropopause height) together with 30 hPa temperature (for stratospheric waves) at 60°N. The correlation coefficient for the linear multiple regression between total ozone (dependent variable) and the dynamical parameters (independent variables) is 0.88 for the zonal deviations in the winter of the Northern Hemisphere. Zonal means are also significantly dependent on circulation parameters, besides showing the known negative trend function of total ozone observed by TOMS. The significant linear trend for 60°N is \\sim3 DU/year in the winter months taking into account the dependence on the dynamics between the tropopause region and the mid-stratosphere. The highest correlation coefficient for the monthly mean total ozone anomalies is reached in November with 0.94.Key words. Atmospheric composition and structure (middle atmosphere · composition and chemistry) · Meteorology and atmospheric dynamics (middle atmosphere dynamics).


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