scholarly journals Evaluation of Water Vapour Assimilation in the Tropical Upper Troposphere and Lower Stratosphere by a Chemical Transport Model

2016 ◽  
Author(s):  
S. Payra ◽  
P. Ricaud ◽  
R. Abida ◽  
L. El Amraoui ◽  
J.-L. Attié ◽  
...  
Keyword(s):  
Water Vapour ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Model Space ◽  
Global Scale ◽  
Chemical Transport Model ◽  
Data Set ◽  
Upper Troposphere ◽  
Sensitivity Studies

Abstract. The present analysis deals with one of the most debated aspect of the studies on the Upper Troposphere/Lower Stratosphere (UTLS), namely the budget of the water vapour (H2O) at the tropical tropopause. Within the French project "Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics" (TRO-pico), a global-scale analysis has been set up based on space-borne observations, model and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa hPa range from August 2011 to March 2013 with an assimilation window of 1 hour. Diagnostics are developed to assess the quality of the assimilated H2O fields depending on several parameters: model error, observation minus analysis and forecast. Comparison with an independent source of H2O measurements in the UTLS based on the spaceborne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses are also shown. Sensitivity studies of the analyzed fields have been performed by: 1) considering periods when no MLS measurements are available and 2) using another MLS version 4.2 H2O data. The studies have been performed within 3 different spaces in time and space coincidences with MLS and MIPAS observations and with the model outputs and at 3 different levels: 121 hPa (upper troposphere), 100 hPa (tropopause), and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the “true” atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent to assess the behaviour of the analyses at 121 and 100 hPa particularly over intense convective areas as the Southern American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the great improvement on the H2O analyses in the tropical UTLS when assimilating spaceborne measurements of better quality particularly over the convective areas.

scholarly journals Evaluation of water vapour assimilation in the tropical upper troposphere and lower stratosphere by a chemical transport model

2016 ◽  
Vol 9 (9) ◽  
pp. 4355-4373 ◽  
Author(s):  
Swagata Payra ◽  
Philippe Ricaud ◽  
Rachid Abida ◽  
Laaziz El Amraoui ◽  
Jean-Luc Attié ◽  
...  
Keyword(s):  
Water Vapour ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Model Space ◽  
Global Scale ◽  
Chemical Transport Model ◽  
Data Set ◽  
Upper Troposphere ◽  
Sensitivity Studies

Abstract. The present analysis deals with one of the most debated aspects of the studies on the upper troposphere/lower stratosphere (UTLS), namely the budget of water vapour (H2O) at the tropical tropopause. Within the French project “Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics” (TRO-pico), a global-scale analysis has been set up based on space-borne observations, models and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa range from August 2011 to March 2013 with an assimilation window of 1 h. Diagnostics based on observations minus analysis and forecast are developed to assess the quality of the assimilated H2O fields. Comparison with an independent source of H2O measurements in the UTLS based on the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses is also shown. Sensitivity studies of the analysed fields have been performed by (1) considering periods when no MLS measurements are available and (2) using H2O data from another MLS version (4.2). The studies have been performed within three different spaces in time and space coincidences with MLS (hereafter referred to as MLS space) and MIPAS (MIPAS space) observations and with the model (model space) outputs and at three different levels: 121 hPa (upper troposphere), 100 hPa (tropopause) and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the reference atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but are consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent assessment of the behaviour of the analyses at 121 and 100 hPa, particularly over intense convective areas as the South American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the improvement on the H2O analyses in the tropical UTLS when assimilating space-borne measurements of better quality, particularly over the convective areas.

scholarly journals The SPARC water vapour assessment II: profile-to-profile and climatological comparisons of stratospheric <i>δ</i>D(H<sub>2</sub>O) observations from satellite

2019 ◽  
Vol 19 (4) ◽  
pp. 2497-2526 ◽  
Author(s):  
Charlotta Högberg ◽  
Stefan Lossow ◽  
Farahnaz Khosrawi ◽  
Ralf Bauer ◽  
Kaley A. Walker ◽  
...  
Keyword(s):  
Water Vapour ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Isotopic Ratio ◽  
Michelson Interferometer ◽  
Data Sets ◽  
Comprehensive Overview ◽  
Data Set ◽  
Upper Troposphere ◽  
Modelling Studies

Abstract. Within the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), we evaluated five data sets of δD(H2O) obtained from observations by Odin/SMR (Sub-Millimetre Radiometer), Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding), and SCISAT/ACE-FTS (Science Satellite/Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) using profile-to-profile and climatological comparisons. These comparisons aimed to provide a comprehensive overview of typical uncertainties in the observational database that could be considered in the future in observational and modelling studies. Our primary focus is on stratospheric altitudes, but results for the upper troposphere and lower mesosphere are also shown. There are clear quantitative differences in the measurements of the isotopic ratio, mainly with regard to comparisons between the SMR data set and both the MIPAS and ACE-FTS data sets. In the lower stratosphere, the SMR data set shows a higher depletion in δD than the MIPAS and ACE-FTS data sets. The differences maximise close to 50 hPa and exceed 200 ‰. With increasing altitude, the biases decrease. Above 4 hPa, the SMR data set shows a lower δD depletion than the MIPAS data sets, occasionally exceeding 100 ‰. Overall, the δD biases of the SMR data set are driven by HDO biases in the lower stratosphere and by H2O biases in the upper stratosphere and lower mesosphere. In between, in the middle stratosphere, the biases in δD are the result of deviations in both HDO and H2O. These biases are attributed to issues with the calibration, in particular in terms of the sideband filtering, and uncertainties in spectroscopic parameters. The MIPAS and ACE-FTS data sets agree rather well between about 100 and 10 hPa. The MIPAS data sets show less depletion below approximately 15 hPa (up to about 30 ‰), due to differences in both HDO and H2O. Higher up this behaviour is reversed, and towards the upper stratosphere the biases increase. This is driven by increasing biases in H2O, and on occasion the differences in δD exceed 80 ‰. Below 100 hPa, the differences between the MIPAS and ACE-FTS data sets are even larger. In the climatological comparisons, the MIPAS data sets continue to show less depletion in δD than the ACE-FTS data sets below 15 hPa during all seasons, with some variations in magnitude. The differences between the MIPAS and ACE-FTS data have multiple causes, such as differences in the temporal and spatial sampling (except for the profile-to-profile comparisons), cloud influence, vertical resolution, and the microwindows and spectroscopic database chosen. Differences between data sets from the same instrument are typically small in the stratosphere. Overall, if the data sets are considered together, the differences in δD among them in key areas of scientific interest (e.g. tropical and polar lower stratosphere, lower mesosphere, and upper troposphere) are too large to draw robust conclusions on atmospheric processes affecting the water vapour budget and distribution, e.g. the relative importance of different mechanisms transporting water vapour into the stratosphere.

scholarly journals Intercomparison and evaluation of satellite peroxyacetyl nitrate observations in the upper troposphere – lower stratosphere

2016 ◽  
Author(s):  
R. J. Pope ◽  
N. A. D. Richards ◽  
M. P. Chipperfield ◽  
D. P. Moore ◽  
S. A. Monks ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Regional Distribution ◽  
Michelson Interferometer ◽  
Lower Atmosphere ◽  
Chemical Transport Model ◽  
Peroxyacetyl Nitrate ◽  
Subsequent Formation ◽  
Upper Troposphere

Abstract. Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NOx and subsequent formation of O3 in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere – lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board ENVISAT from the Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology and the Department of Physics and Astronomy, University of Leicester (UoL). Retrieving PAN from MIPAS is challenging due to the weak signal in the measurements and contamination from other species. Therefore, we compare the two MIPAS datasets with observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), insitu aircraft data and the TOMCAT 3-D chemical transport model. MIPAS shows peak UTLS PAN concentrations over the biomass burning regions (e.g. ranging from 150 to > 200 pptv at 150 hPa) and during the summertime Asian monsoon as enhanced convection aids the vertical transport of PAN from the lower atmosphere. At 150 hPa, we find significant differences between the two MIPAS datasets in the tropics, where IMK PAN concentrations are larger by 50–100 pptv. Comparisons between MIPAS and ACE-FTS show better agreement with the UoL MIPAS PAN concentrations at 200 hPa, but with mixed results above this altitude. TOMCAT generally captures the magnitude and structure of climatological aircraft PAN profiles within the observational variability allowing it to be used to investigate the MIPAS PAN differences. TOMCAT-MIPAS comparisons show that the model is both positively (UoL) and negatively (IMK) biased against the satellite products. These results show that satellite PAN observations are able to detect realistic spatial variations in PAN in the UTLS, but further work is needed to resolve differences in existing retrievals to allow quantitative use of the products.

scholarly journals Intercomparison and evaluation of satellite peroxyacetyl nitrate observations in the upper troposphere–lower stratosphere

2016 ◽  
Vol 16 (21) ◽  
pp. 13541-13559 ◽  
Author(s):  
Richard J. Pope ◽  
Nigel A. D. Richards ◽  
Martyn P. Chipperfield ◽  
David P. Moore ◽  
Sarah A. Monks ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Regional Distribution ◽  
Michelson Interferometer ◽  
Lower Atmosphere ◽  
Chemical Transport Model ◽  
Peroxyacetyl Nitrate ◽  
Subsequent Formation ◽  
Upper Troposphere

Abstract. Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NOx and subsequent formation of O3 in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere–lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board Envisat from the Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology, and the Department of Physics and Astronomy, University of Leicester (UoL). Retrieving PAN from MIPAS is challenging due to the weak signal in the measurements and contamination from other species. Therefore, we compare the two MIPAS datasets with observations from the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS), in situ aircraft data and the 3-D chemical transport model TOMCAT. MIPAS shows peak UTLS PAN concentrations over the biomass burning regions (e.g. ranging from 150 to  >  200 pptv at 150 hPa) and during the summertime Asian monsoon as enhanced convection aids the vertical transport of PAN from the lower atmosphere. At 150 hPa, we find significant differences between the two MIPAS datasets in the tropics, where IMK PAN concentrations are larger by 50–100 pptv. Comparisons between MIPAS and ACE-FTS show better agreement with the UoL MIPAS PAN concentrations at 200 hPa, but with mixed results above this altitude. TOMCAT generally captures the magnitude and structure of climatological aircraft PAN profiles within the observational variability allowing it to be used to investigate the MIPAS PAN differences. TOMCAT–MIPAS comparisons show that the model is both positively (UoL) and negatively (IMK) biased against the satellite products. These results indicate that satellite PAN observations are able to detect realistic spatial variations in PAN in the UTLS, but further work is needed to resolve differences in existing retrievals to allow quantitative use of the products.

scholarly journals Modeling the transport of very short-lived substances into the tropical upper troposphere and lower stratosphere

2009 ◽  
Vol 9 (5) ◽  
pp. 18511-18543 ◽  
Author(s):  
J. Aschmann ◽  
B. M. Sinnhuber ◽  
E. L. Atlas ◽  
S. M. Schauffler
Keyword(s):  
Large Scale ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport Model ◽  
Heating Rates ◽  
Model Calculations ◽  
Upper Troposphere ◽  
Mass Fluxes ◽  
Tropical Upper Troposphere

Abstract. The transport of very short-lived substances into the tropical upper troposphere and lower stratosphere is investigated by a three-dimensional chemical transport model using archived convective updraft mass fluxes (or detrainment rates) from the European Centre for Medium-Range Weather Forecast's ERA-Interim reanalysis. Large-scale vertical velocities are calculated from diabatic heating rates. With this approach we explicitly model the large scale subsidence in the tropical troposphere with convection taking place in fast and isolated updraft events. The model calculations agree generally well with observations of bromoform and methyl iodide from aircraft campaigns and with ozone and water vapor from sonde and satellite observations. Using a simplified treatment of dehydration and bromine product gas washout we give a range of 1.6 to 3 ppt for the contribution of bromoform to stratospheric bromine, assuming a uniform source in the boundary layer of 1 ppt. We show that the most effective region for VSLS transport into the stratosphere is the West Pacific, accounting for about 55% of the bromine from bromoform transported into the stratosphere under the supposition of a uniformly distributed source.

scholarly journals The SPARC water vapour assessment II: Profile-to-profile and climatological comparisons of stratospheric <i>δ</i>D(H<sub>2</sub>O) observations from satellite

2018 ◽  
Author(s):  
Charlotta Högberg ◽  
Stefan Lossow ◽  
Ralf Bauer ◽  
Kaley A. Walker ◽  
Patrick Eriksson ◽  
...  
Keyword(s):  
Water Vapour ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Isotopic Ratio ◽  
Michelson Interferometer ◽  
Data Sets ◽  
Data Set ◽  
Spectroscopic Database ◽  
Temporal And Spatial ◽  
Chemistry Experiment

Abstract. Within the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), we have evaluated five data sets of δD(H2O) obtained from observations of Odin/SMR (Sub-Millimetre Radiometer), Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) and SCISAT/ACE-FTS (Science Satellite/Atmospheric Chemistry Experiment-Fourier Transform Spectrometer) using profile-to-profile and climatological comparisons. Our focus is on stratospheric altitudes, but results from the upper troposphere to the lower mesosphere are provided. There are clear quantitative differences in the measurements of the isotopic ratio, which primarily concerns the comparisons to the SMR data set. In the lower stratosphere, this data set shows a higher depletion than the MIPAS and ACE-FTS data sets. The differences maximise close to 50 hPa and exceed 200 per mille. With increasing altitude, the biases typically decrease. Above 4 hPa, the SMR data set shows a lower depletion than the MIPAS data sets, on occasion exceeding 100 per mille. Overall, the δD biases of the SMR data set are driven by HDO biases in the lower stratosphere and by H2O biases in the upper stratosphere and lower mesosphere. In between, in the middle stratosphere, the biases in δD are a combination of deviations in both HDO and H2O. These biases are attributed to issues with the calibration, in particular in terms of the sideband filtering for H2O, and uncertainties in spectroscopic parameters. The MIPAS and ACE-FTS data sets agree rather well between about 100 hPa and 10 hPa. The MIPAS data sets show less depletion below about 15 hPa (up to about 30 per mille), due to differences in both HDO and H2O. Higher up the picture is reversed, and towards the upper stratosphere the biases typically increase. This is driven by increasing biases in H2O and on occasion the differences in δD exceed 80 per mille. Below 100 hPa, the differences between the MIPAS and ACE-FTS data sets are even larger. In the climatological comparisons, the MIPAS data sets continue to show less depletion than the ACE-FTS data sets below 15 hPa during all seasons, with some variations in magnitude. The differences between the MIPAS and ACE-FTS data come from different aspects, such as differences in the temporal and spatial sampling (except for the profile-to-profile comparisons), cloud influence, vertical resolution, and the microwindows and spectroscopic database chosen. Differences between data sets from the same instrument are typically small in the stratosphere.

scholarly journals Tropospheric mixing and parametrization of unresolved convection as implemented into the Chemical Lagrangian Model of the Stratosphere (CLaMS)

2018 ◽  
Author(s):  
Paul Konopka ◽  
Mengchu Tao ◽  
Felix Ploeger ◽  
Mohamadou Diallo ◽  
Martin Riese
Keyword(s):  
Lower Stratosphere ◽  
Transport Model ◽  
Longwave Radiation ◽  
Vertical Transport ◽  
Lagrangian Model ◽  
Data Set ◽  
Numerical Diffusion ◽  
Upper Troposphere ◽  
Good Ability ◽  
Observation Network

Abstract. Inaccurate representation of mixing in chemistry transport model, mainly suffering from an excessive numerical diffusion, strongly influences the quantitative estimates of the stratosphere-troposphere exchange (STE). The Lagrangian view of transport offers an alternative to exploit the numerical diffusion for parametrization of the physical mixing. Here, we follow this concept and discuss how to extend the representation of tropospheric transport in the Chemical Lagrangian Model of the Stratosphere (CLaMS). Although the current transport scheme in CLaMS shows good ability of representing transport of tracers in the stably stratified stratosphere (Pommrich et al., (2014) and the references therein), there are deficiencies in representation of the effects of convective uplift and mixing due to weak vertical stability in the troposphere. We show how the CLaMS transport scheme was modified by including additional tropospheric mixing and vertical transport due to unresolved convection by parametrizing these processes in terms of the dry and moist Brunt-Vaisala frequency, respectively. The regions with enhanced vertical transport in the novel CLaMS simulation covering the 2005-08 period coincide with regions of enhanced convection as diagnosed from the satellite observations of the Outgoing Longwave Radiation (OLR). We analyze how well this approach improves the CLaMS representation of CO2 in the upper troposphere and lower stratosphere, in particular the propagation of the CO2 seasonal cycle from the Planetary Boundary Layer (PBL) into the lower stratosphere. The CO2 values in the PBL are specified by the CarbonTracker data set (version CT2013B) and the Comprehensive Observation Network for TRace gases by AIrLiner (CONTRAIL) observations are used to validate the model. The proposed extension of tropospheric transport increases the tropospheric influence in the middle and upper troposphere and at the same time influences the STE. The effect on mean age away from the troposphere in the deep stratosphere is weak.

scholarly journals Sulfur dioxide (SO<sub>2</sub>) from MIPAS in the upper troposphere and lower stratosphere 2002–2012

2015 ◽  
Vol 15 (12) ◽  
pp. 7017-7037 ◽  
Author(s):  
M. Höpfner ◽  
C. D. Boone ◽  
B. Funke ◽  
N. Glatthor ◽  
U. Grabowski ◽  
...  
Keyword(s):  
Sulfur Dioxide ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Michelson Interferometer ◽  
Volcanic Eruptions ◽  
Aerosol Layer ◽  
Mixing Ratio ◽  
So2 Emissions ◽  
Data Set ◽  
Upper Troposphere

Abstract. Vertically resolved distributions of sulfur dioxide (SO2) with global coverage in the height region from the upper troposphere to ~20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70–100 pptv and by a vertical resolution ranging from 3 to 5 km. Comparison with observations by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) revealed a slightly varying bias with altitude of −20 to 50 pptv for the MIPAS data set in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within −10 to 20 pptv in the altitude range of 10–20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS data set with in situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than 30 volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS). Emitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period – Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 – derived lifetimes of SO2 for the altitude ranges 10–14, 14–18 and 18–22 km are 13.3 ± 2.1, 23.6 ± 1.2 and 32.3 ± 5.5 days respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual cycle at northern mid- and high latitudes with maximum values in summer and an amplitude of about 30 pptv. At higher altitudes of about 16–18 km, enhanced mixing ratios of SO2 can be found in the regions of the Asian and the North American monsoons in summer – a possible connection to an aerosol layer discovered by Vernier et al. (2011b) in that region.

scholarly journals Technical note: Reanalysis of Aura MLS chemical observations

2019 ◽  
Vol 19 (21) ◽  
pp. 13647-13679 ◽  
Author(s):  
Quentin Errera ◽  
Simon Chabrillat ◽  
Yves Christophe ◽  
Jonas Debosscher ◽  
Daan Hubert ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Polar Vortex ◽  
Methyl Chloride ◽  
Technical Note ◽  
Chemical Transport Model ◽  
Stratospheric Polar Vortex ◽  
Upper Troposphere ◽  
Independent Observations

Abstract. This paper presents a reanalysis of the atmospheric chemical composition from the upper troposphere to the lower mesosphere from August 2004 to December 2017. This reanalysis is produced by the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by the chemical observations from the Microwave Limb Sounder (MLS) on board the Aura satellite. BASCOE is based on the ensemble Kalman filter (EnKF) method and includes a chemical transport model driven by the winds and temperature from the ERA-Interim meteorological reanalysis. The model resolution is 3.75∘ in longitude, 2.5∘ in latitude and 37 vertical levels from the surface to 0.1 hPa with 25 levels above 100 hPa. The outputs are provided every 6 h. This reanalysis is called BRAM2 for BASCOE Reanalysis of Aura MLS, version 2. Vertical profiles of eight species from MLS version 4 are assimilated and are evaluated in this paper: ozone (O3), water vapour (H2O), nitrous oxide (N2O), nitric acid (HNO3), hydrogen chloride (HCl), chlorine oxide (ClO), methyl chloride (CH3Cl) and carbon monoxide (CO). They are evaluated using independent observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) and N2O observations from a different MLS radiometer than the one used to deliver the standard product and ozonesondes. The evaluation is carried out in four regions of interest where only selected species are evaluated. These regions are (1) the lower-stratospheric polar vortex where O3, H2O, N2O, HNO3, HCl and ClO are evaluated; (2) the upper-stratospheric–lower-mesospheric polar vortex where H2O, N2O, HNO3 and CO are evaluated; (3) the upper troposphere–lower stratosphere (UTLS) where O3, H2O, CO and CH3Cl are evaluated; and (4) the middle stratosphere where O3, H2O, N2O, HNO3, HCl, ClO and CH3Cl are evaluated. In general BRAM2 reproduces MLS observations within their uncertainties and agrees well with independent observations, with several limitations discussed in this paper (see the summary in Sect. 5.5). In particular, ozone is not assimilated at altitudes above (i.e. pressures lower than) 4 hPa due to a model bias that cannot be corrected by the assimilation. MLS ozone profiles display unphysical oscillations in the tropical UTLS, which are corrected by the assimilation, allowing a good agreement with ozonesondes. Moreover, in the upper troposphere, comparison of BRAM2 with MLS and independent observations suggests a positive bias in MLS O3 and a negative bias in MLS H2O. The reanalysis also reveals a drift in MLS N2O against independent observations, which highlights the potential use of BRAM2 to estimate biases between instruments. BRAM2 is publicly available and will be extended to assimilate MLS observations after 2017.

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