Abstract. We present a consistent intercomparison of the mean age of air (AoA) according to five modern reanalyses: the European Centre for Medium-Range Weather Forecasts Interim Reanalysis (ERA-Interim), the Japanese Meteorological Agency's Japanese 55-year Reanalysis (JRA-55), the National Centers for Environmental Prediction Climate Forecast System Reanalysis (CFSR) and the National Aeronautics and Space Administration's Modern Era Retrospective analysis for Research and Applications version 1 (MERRA) and version 2 (MERRA-2). The modeling tool is a kinematic transport model driven only by the surface pressure and wind fields. It is validated for ERA-I through a comparison with the AoA computed by another transport model. The five reanalyses deliver AoA which differs in the worst case by 1 year in the tropical lower stratosphere and more than 2 years in the upper stratosphere. At all latitudes and altitudes, MERRA-2 and MERRA provide the oldest values (∼5–6 years in midstratosphere at midlatitudes), while JRA-55 and CFSR provide the youngest values (∼4 years) and ERA-I delivers intermediate results. The spread of AoA at 50 hPa is as large as the spread obtained in a comparison of chemistry–climate models. The differences between tropical and midlatitude AoA are in better agreement except for MERRA-2. Compared with in situ observations, they indicate that the upwelling is too fast in the tropical lower stratosphere. The spread between the five simulations in the northern midlatitudes is as large as the observational uncertainties in a multidecadal time series of balloon observations, i.e., approximately 2 years. No global impact of the Pinatubo eruption can be found in our simulations of AoA, contrary to a recent study which used a diabatic transport model driven by ERA-I and JRA-55 winds and heating rates. The time variations are also analyzed through multiple linear regression analyses taking into account the seasonal cycles, the quasi-biennial oscillation and the linear trends over four time periods. The amplitudes of AoA seasonal variations in the lower stratosphere are significantly larger when using MERRA and MERRA-2 than with the other reanalyses. The linear trends of AoA using ERA-I confirm those found by earlier model studies, especially for the period 2002–2012, where the dipole structure of the latitude–height distribution (positive in the northern midstratosphere and negative in the southern midstratosphere) also matches trends derived from satellite observations of SF6. Yet the linear trends vary substantially depending on the considered period. Over 2002–2015, the ERA-I results still show a dipole structure with positive trends in the Northern Hemisphere reaching up to 0.3 yr dec−1. No reanalysis other than ERA-I finds any dipole structure of AoA trends. The signs of the trends depend strongly on the input reanalysis and on the considered period, with values above 10 hPa varying between approximately −0.4 and 0.4 yr dec−1. Using ERA-I and CFSR, the 2002–2015 trends are negative above 10 hPa, but using the three other reanalyses these trends are positive. Over the whole period (1989–2015) each reanalysis delivers opposite trends; i.e., AoA is mostly increasing with CFSR and ERA-I but mostly decreasing with MERRA, JRA-55 and MERRA-2. In view of this large disagreement, we urge great caution for studies aiming to assess AoA trends derived only from reanalysis winds. We briefly discuss some possible causes for the dependency of AoA on the input reanalysis and highlight the need for complementary intercomparisons using diabatic transport models.

Abstract. We report on an evaluation of tropospheric ozone and its precursor gases in three atmospheric chemistry versions as implemented in the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS), referred to as IFS(CB05BASCOE), IFS(MOZART) and IFS(MOCAGE). While the model versions were forced with the same overall meteorology, emissions, transport and deposition schemes, they vary largely in their parameterisations describing atmospheric chemistry, including the organics degradation, heterogeneous chemistry and photolysis, as well as chemical solver. The model results from the three chemistry versions are compared against a range of aircraft field campaigns, surface observations, ozone-sondes and satellite observations, which provides quantification of the overall model uncertainty driven by the chemistry parameterisations. We find that they produce similar patterns and magnitudes for carbon monoxide (CO) and ozone (O3), as well as a range of non-methane hydrocarbons (NMHCs), with averaged differences for O3 (CO) within 10 % (20 %) throughout the troposphere. Most of the divergence in the magnitude of CO and NMHCs can be explained by differences in OH concentrations, which can reach up to 50 %, particularly at high latitudes. There are also comparatively large discrepancies between model versions for NO2, SO2 and HNO3, which are strongly influenced by secondary chemical production and loss. Other common biases in CO and NMHCs are mainly attributed to uncertainties in their emissions. This configuration of having various chemistry versions within IFS provides a quantification of uncertainties induced by chemistry modelling in the main CAMS global trace gas products beyond those that are constrained by data assimilation.

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.

We present a model description and bench-

Abstract. This paper evaluates and discusses the quality of the stratospheric ozone analyses delivered in near real time by the MACC (Monitoring Atmospheric Composition and Climate) project during the 3-year period between September 2009 and September 2012. Ozone analyses produced by four different chemical data assimilation (CDA) systems are examined and compared: the Integrated Forecast System coupled to the Model for OZone And Related chemical Tracers (IFS-MOZART); the Belgian Assimilation System for Chemical ObsErvations (BASCOE); the Synoptic Analysis of Chemical Constituents by Advanced Data Assimilation (SACADA); and the Data Assimilation Model based on Transport Model version 3 (TM3DAM). The assimilated satellite ozone retrievals differed for each system; SACADA and TM3DAM assimilated only total ozone observations, BASCOE assimilated profiles for ozone and some related species, while IFS-MOZART assimilated both types of ozone observations. All analyses deliver total column values that agree well with ground-based observations (biases < 5 %) and have a realistic seasonal cycle, except for BASCOE analyses, which underestimate total ozone in the tropics all year long by 7 to 10 %, and SACADA analyses, which overestimate total ozone in polar night regions by up to 30 %. The validation of the vertical distribution is based on independent observations from ozonesondes and the ACE-FTS (Atmospheric Chemistry Experiment -Fourier Transform Spectrometer) satellite instrument. It cannot be performed with TM3DAM, which is designed only to deliver analyses of total ozone columns. Vertically alternating positive and negative biases are found in the IFS-MOZART analyses as well as an overestimation of 30 to 60 % in the polar lower stratosphere during polar ozone depletion events. SACADA underestimates lower stratospheric ozone by up to 50 % during these events above the South Pole and overestimates it by approximately the same amount in the tropics. The three-dimensional (3-D) analyses delivered by BASCOE are found to have the best quality among the three systems resolving the vertical dimension, with biases not exceeding 10 % all year long, at all stratospheric levels and in all latitude bands, except in the tropical lowermost stratosphere.The northern spring 2011 period is studied in more detail to evaluate the ability of the analyses to represent the exceptional ozone depletion event, which happened above the Arctic in March 2011. Offline sensitivity tests are performed during this month and indicate that the differences between the forward models or the assimilation algorithms are much less important than the characteristics of the assimilated data sets. They also show that IFS-MOZART is able to deliver realistic analyses of ozone both in the troposphere and in the stratoPublished by Copernicus Publications on behalf of the European Geosciences Union. sphere, but this requires the assimilation of observations from nadir-looking instruments as well as the assimilation of profiles, which are well resolved vertically an...