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2021 Articolo in rivista open access

Phosgene distribution derived from MIPAS ESA v8 data: intercomparisons and trends

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) measured the middle-infrared limb emission spectrum of the atmosphere from 2002 to 2012 on board ENVISAT, a polar-orbiting satellite. Recently, the European Space Agency (ESA) completed the final reprocessing of MIPAS measurements, using version 8 of the level 1 and level 2 processors, which include more accurate models, processing strategies, and auxiliary data. The list of retrieved gases has been extended, and it now includes a number of new species with weak emission features in the MIPAS spectral range. The new retrieved trace species include carbonyl chloride (COCl2), also called phosgene. Due to its toxicity, its use has been reduced over the years; however, it is still used by chemical industries for several applications. Besides its direct injection in the troposphere, stratospheric phosgene is mainly produced from the photolysis of CCl4, a molecule present in the atmosphere because of human activity. Since phosgene has a long stratospheric lifetime, it must be carefully monitored as it is involved in the ozone destruction cycles, especially over the winter polar regions.In this paper we exploit the ESA MIPAS version 8 data in order to discuss the phosgene distribution, variability, and trends in the middle and lower stratosphere and in the upper troposphere. The zonal averages show that phosgene volume mixing ratio is larger in the stratosphere, with a peak of 40 pptv (parts per trillion by volume) between 50 and 30 hPa at equatorial latitudes, while at middle and polar latitudes it varies from 10 to 25 pptv. A moderate seasonal variability is observed in polar regions, mostly between 80 and 50 hPa. The comparison of MIPAS-ENVISAT COCl2 v8 profiles with the ones retrieved from MIPAS balloon and ACE-FTS (Atmospheric Chemistry Experiment - Fourier Transform Spectrometer) measurements highlights a negative bias of about 2 pptv, mainly in polar and mid-latitude regions. Part of this bias is attributed to the fact that the ESA level 2 v8 processor uses an updated spectroscopic database. For the trend computation, a fixed pressure grid is used to interpolate the phosgene profiles, and, for each pressure level, VMR (volume mixing ratio) monthly averages are computed in pre-defined 10? wide latitude bins. Then, for each latitudinal bin and pressure level, a regression model has been fitted to the resulting time series in order to derive the atmospheric trends. We find that the phosgene trends are different in the two hemispheres. The analysis shows that the stratosphere of the Northern Hemisphere is characterized by a negative trend of about -7 pptv per decade, while in the Southern Hemisphere phosgene mixing ratios increase with a rate of the order of +4 pptv per decade. This behavior resembles the stratospheric trend of CCl4, which is the main stratospheric source of COCl2. In the upper troposphere a positive trend is found in both hemispheres.

atmospheric phosgene MIPAS measurements phosgene trend climate change
2021 Articolo in rivista open access

The ESA MIPAS/Envisat level2-v8 dataset: 10 years of measurements retrieved with ORM v8.22

Bianca Maria Dinelli ; Piera Raspollini ; Marco Gai ; Luca Sgheri ; Marco Ridolfi ; Simone Ceccherini ; Flavio Barbara ; Nicola Zoppetti ; Elisa Castelli ; Enzo Papandrea ; Paolo Pettinari ; Angelika Dehn ; Anu Dudhia ; Michael Kiefer ; Alessandro Piro ; JeanMarie Flaud ; Manuel LópezPuertas ; David Moore ; John Remedios ; Massimo Bianchini

The observations acquired during the full mission of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, aboard the European Space Agency Environmental Satellite (Envisat), have been analysed with version 8.22 of the Optimised Retrieval Model (ORM), originally developed as the scientific prototype of the ESA level-2 processor for MIPAS observations. The results of the analyses have been included into the MI- PAS level-2 version 8 (level2-v8) database containing atmospheric fields of pressure, temperature, and volume mixing ratio (VMR) of MIPAS main targets H2 O, O3 , HNO3 , CH4 , N2 O, and NO2 , along with the minor gases CFC- 11, ClONO2 , N2 O5 , CFC-12, COF2 , CCl4 , CF4 , HCFC-22, C2 H2 , CH3 Cl, COCl2 , C2 H6 , OCS, and HDO. The database covers all the measurements acquired by MIPAS in the nominal measurement mode of the full resolution (FR) part of the mission (from July 2002 to March 2004) and all the observation modes of the optimised resolution (OR) part (from January 2005 to April 2012). The number of species included in the MIPAS level2-v8 dataset makes it of particular importance for the studies of stratospheric chemistry. The database is considered by ESA the final release of the MIPAS level-2 products.The ORM algorithm is operated at the vertical grid coincident to the tangent altitudes of the observations or to a subset of them, spanning (in the nominal mode) the alti- tude range from 6 to 68km in the FR phase and from 6 to 70 km in the OR period. In the latitude domain, FR profiles are spaced by about 4.7o, while the OR profiles are spaced by about 3.7o. For each retrieved species, the auxiliary data and the retrieval choices are described. Each product is characterised in terms of the retrieval error, spatial resolution, and "useful" vertical range in both phases of the MIPAS mission. These depend on the characteristics of the measurements (spectral and vertical resolution of the measurements), the retrieval choices (number of spectral points in- cluded in the analyses, number of altitudes included in the vertical retrieval grid), and the information content of the measurements for each trace species. For temperature, water vapour, ozone, and nitric acid, the number of degrees of freedom is significantly larger in the OR phase than in the FR one, mainly due to the finer vertical measurement grid. In the FR phase, some trace species are characterised by a smaller retrieval error with respect to the OR phase, mainly due to the larger number of spectral points used in the analyses, along with the reduced vertical resolution. The way of handling possible caveats (negative VMR, vertical grid representation) is discussed. The quality of the retrieved profiles is assessed through four criteria, two providing information on the successful convergence of the retrieval iterations, one on the capability of the retrieval to reproduce the measurements, and one on the presence of outliers. An easy way to identify and filter the problematic profiles with the informa- tion contained in the output files is provided. MIPAS level2- v8 data are available to the scientific community through the ESA portal (https://doi.org/10.5270/EN1-c8hgqx4).

composizione atmosferica MIPAS
2020 Abstract in Atti di convegno metadata only access

ESA Version 8 reprocessing of the 10 years of MIPAS on ENVISAT measurements

P Raspollini ; F Barbara ; M Bianchini ; M Birk ; S Ceccherini ; A Dehn ; M Gai ; B M Dinelli ; A Dudhia ; J M Flaud ; M Hoepfner ; D Hubert ; A Keppens ; M Kiefer ; A Kleinert ; D Moore ; E Papandrea ; G Perron ; A Piro ; M LópezPuertas ; H Oelhaf ; P Pettinari ; J Remedios ; M Ridolfi ; L Sgheri ; G Wagner ; G Wetzel ; N Zoppetti

MIPAS is a Fourier Transform spectrometer that measured the atmospheric limb emission spectra in the middle infrared on board the ENVISAT satellite. These measurements allowed the global monitoring of the three-dimensional (latitude, longitude and altitude) distribution of concentrations of many species, during both day and night, for 10 years, from July 2002 to April 2012. Being a limb sounding instrument, the focus of MIPAS measurements was the study of the atmosphere from the upper troposphere to the stratosphere and above, up to the mesosphere. The interest in these measurements goes beyond the end of the mission, as they can be used in long time series of data to determine changes in our planet's climate. To this purpose, it is therefore important to continue improving their quality. The quality of MIPAS L2 products depends on the quality of the L1 products, on the L2 model accuracy, on the quality of auxiliary data, particularly on spectroscopic data. For the last reanalysis of the whole MIPAS mission, a significant effort was made by the MIPAS Quality Working Group, supported by ESA, to improve both L1 and L2 processors, as well as spectroscopy, with the objectives of obtaining L2 products with increased accuracy, better temporal stability, and a larger number of retrieved species. Here we present the full mission dataset, including vertical profiles of 21 trace species plus temperature, obtained by applying the latest version of ESA L2 processor (ORM V8) to the MIPAS L1 data obtained with version 8 of the L1 processor. The impact of the improvements of both L1 and L2 processors on the quality of the L2 products is presented, as well as results of the validation against independent correlative measurements.

MIPAS Atmospheric composition Level 2 data quality
2019 Poster / Abstract non pubblicati in atti di convegno restricted access

Assessment of quality of MIPAS ESA L2 products

P. Raspollini ; F. Barbara ; M. Bianchini ; M. Birk ; S. Ceccherini ; A. Dehn ; M. Gai ; B. M. Dinelli ; A. Dudhia ; J. M. Flaud ; M. Hoepfner ; D. Hubert ; A. Keppens ; M. Kiefer ; A. Kleinert ; D. Moore ; E. Papandrea ; G. Perron ; A. Piro ; M. López-Puertas ; H. Oelhaf ; P. Pettinari ; J. Remedios ; M. Ridolfi ; L. Sgheri ; G. Wagner ; G. Wetzel ; N. Zoppetti

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is a limb-viewing infrared Fourier transform spectrometer that operated from 2002 to 2012 onboard the ENVISAT satellite. The analysis of MIPAS measurements allows to study the temporal evolution of numerous species of interest for the study of the ozone in the stratosphere, pollutants and many green-house gases. The objective of the MIPAS Quality Working Group is to improve the quality of the MIPAS products through a fruitful collaboration among spectroscopists, Level 1, Level 2, and validation teams. A large effort has recently led to implement significant improvements in both ESA Level 1 and Level 2 processors, as well as in spectroscopic database and in some absorption cross-sections in order to improve the quality of the products. In addition to the products already present in the V7 dataset (temperature and the VMR of H2O, O3, HNO3, CH4, N2O, NO2, CFC-11, CFC-12, N2O5, ClONO2, HCFC-22, COF2, CF4, HCN and CCl4), the VMR of six additional species (OCS, CH3Cl, HDO, C2H2, C2H6, COCl2) will be provided in V8 dataset. In order to evaluate the impact of the changes in the products before full mission reprocessing, the analysis of the performances of the products of the modified L1 and L2 processors, as well as the auxiliary data, has been performed on a Diagnostic DataSet (DDS). The orbits of the DDS have been chosen in coincidence with correlative measurements for performing also a preliminary assessment of the accuracy of the products and to evaluate possible changes in the drift. With respect to V7 products, main improvements consist in a reduction of the temperature bias in the first part of the mission, a reduction of the discontinuities in CH4 and N2O time series due to daily gain upgrade, a better filtering of clouds and a better handling of horizontal inhomogeneities.The results of the assessment of the quality of MIPAS measurements will be shown, as well as the study of the temporal evolution and variability of all species. We will also investigate the spatial, seasonal, and interannual variations in the distribution of these species.

MIPAS Quality Assessment
2019 Poster / Abstract non pubblicati in atti di convegno restricted access

Preliminary assessment of the quality of Methyl chloride (CH3Cl) from MIPAS on ENVISAT measurements

P Raspollini ; F Barbara ; M Bianchini ; S Ceccherini ; A Dehn ; M Gai ; B M Dinelli ; A Dudhia ; JM Flaud ; M Höpfner ; M Kiefer ; D Moore ; A Piro ; M LópezPuertas ; H Oelhaf ; P Pettinari ; J Remedios ; M Ridolfi ; L Sgheri ; G Wetzel ; N Zoppetti

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is a limb-viewing infrared Fourier transform spectrometer that operated from 2002 to 2012 on board the ENVISAT satellite. The fruitful collaboration among spectroscopists, Level 1, Level 2, and validation teams in the frame of the MIPAS Quality Working Group has recently led to the implementation of significant changes in both ESA Level 1 and Level 2 processors, as well as in the spectroscopic database and in some absorption cross-sections. In addition to the products already present in V7 dataset (temperature and the VMR of H2O, O3, HNO3, CH4, N2O, NO2, CFC-11, CFC-12, N2O5, ClONO2, HCFC-22, COF2, CF4, HCN and CCl4), the VMR of six additional species (OCS, CH3Cl, HDO, C2H2, C2H6, COCl2) will be provided in V8 dataset.Among the new species, methyl chloride (CH3Cl) is of great interest in stratospheric ozone chemistry since it is the most abundant chlorine-containing gas in the troposphere and, in contrast to other relatively long-lived ozone-depleting gases, it has both natural and anthropogenic sources, with the known emission being mainly natural (tropical plants, biomass burning, the ocean, salt marshes and fungi). Since it is not controlled under the Montreal Protocol, its importance is expected to increase in the coming decades as emission controls alter the relative contributions from natural and anthropogenic halogen sources.In this paper we present a preliminary assessment of the quality of the MIPAS CH3Cl data, in terms of precision, accuracy and vertical resolution, and we investigate the spatial and seasonal variations in the distribution of CH3Cl in the upper troposphere/lower stratosphere (UTLS).

MIPAS Methyl chloride Quality Assessment
2018 Presentazione / Comunicazione non pubblicata (convegno, evento, webinar...) restricted access

Quality assessment of MIPAS ESA V8 products before full mission reprocessing

Raspollini Piera ; Barbara Flavio ; Bianchini Massimo ; Birk Manfred ; Castelli Elisa ; Ceccherini Simone ; Dehn Angelika ; Gai Marco ; Dinelli Bianca Maria ; Dudhia Anu ; Flaud JeanMarie ; Hoepfner Michael ; Hubert Daan ; Keppens Arno ; Kiefer Michael ; Kleinert Anne ; Moore David ; Papandrea Enzo ; Perron Gaetan ; Piro Alessandro ; LopezPuertas Manuel ; Oelhaf Hermann ; Pettinari Paolo ; Remedios John ; Ridolfi Marco ; Sgheri Luca ; Wagner Georg ; Wetzel Gerald ; Zoppetti Nicola

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is a limb-viewing infrared Fourier transform spectrometer that operated from 2002 to 2012 onboard the ENVISAT satellite. The maintenance and the upgrade of both L1 and L2 ESA processors are accomplished by the Quality Working Group, where a fruitful collaboration among Level 1, Level 2 and validation teams can be exploited. Recently both ESA L1 and L2 processors have been updated, as well as the spectroscopic database and some absorption cross-sections. In addition to the products already present in the current release (V7) of ESA MIPAS data (temperature and the VMR of H2O, O3, HNO3, CH4, N2O, NO2, CFC-11, CFC-12, N2O5, ClONO2, HCFC-22, COF2, CF4, HCN and CCl4), the VMR of six additional species (OCS, CH3Cl, HDO, C2H2, C2H6, COCl2) will be provided in V8 dataset. In preparation of V8 full mission reprocessing, three Diagnostic Datasets have been generated to check the performances of all L1, L2 processors and the new auxiliary data.The analysis of these Diagnostic Datasets and the comparison with previous full mission dataset V7 will be used to perform a first assessment of the quality of the new V8 products. In the paper special focus will be given to the new species.

MIPAS ENVISAT ESA V8 Products