Belgian Assimilation System For Chemical ObsErvations Research Articles

Microwave radiometer observations of the ozone diurnal cycle and its short-term variability over Switzerland

Abstract. In Switzerland, two ground-based ozone microwave radiometers are operated in the vicinity of each other (ca. 40 km): the GROund-based Millimeter-wave Ozone Spectrometer (GROMOS) in Bern (Institute of Applied Physics) and the Stratospheric Ozone MOnitoring RAdiometer (SOMORA) in Payerne (MeteoSwiss). Recently, their calibration and retrieval algorithms have been fully harmonized, and updated time series are now available since 2009. Using these harmonized ozone time series, we investigate and cross-validate the strato–mesospheric ozone diurnal cycle derived from the two instruments and compare it with various model-based datasets: the dedicated GEOS-GMI Diurnal Ozone Climatology (GDOC) based on the Goddard Earth Observing System (GEOS-5) general circulation model, the Belgian Assimilation System for Chemical ObsErvations (BASCOE) – a chemical transport model driven by ERA5 dynamics, and a set of free-running simulations from the Whole Atmosphere Community Climate Model (WACCM). Overall, the two instruments show very similar ozone diurnal cycles at all seasons and pressure levels, and the models compare well with each other. There is a good agreement between the models and the measurements at most seasons and pressure levels, and the largest discrepancies can be explained by the limited vertical resolution of the microwave radiometers. However, as in a similar study over Mauna Loa, some discrepancies remain near the stratopause, at the transition region between ozone daytime accumulation and depletion. We report similar delays in the onset of the modelled ozone diurnal depletion in the lower mesosphere. Using the newly harmonized time series of GROMOS and SOMORA radiometers, we present the first observations of short-term (sub-monthly) ozone diurnal cycle variability at mid-latitudes. The short-term variability is observed in the upper stratosphere during wintertime, when the mean monthly cycle has a small amplitude and when the dynamics are more important. This is shown in the form of strong enhancements of the diurnal cycle, reaching up to 4–5 times the amplitude of the mean monthly cycle. We show that BASCOE is able to capture some of these events, and we present a case study of one such event following the minor sudden stratospheric warming of January 2015. Our analysis of this event supports the conclusions of a previous modelling study, attributing regional variability of the ozone diurnal cycle to regional anomalies in nitrogen oxide (NOx) concentrations. However, we also find periods with an enhanced diurnal cycle that do not show much change in NOx and where other processes might be dominant (e.g. atmospheric tides). Given its importance, we believe that the short-term variability of the ozone diurnal cycle should be further investigated over the globe, for instance using the BASCOE model.

Tropospheric ozone retrieval by a combination of TROPOMI/S5P measurements with BASCOE assimilated data

Abstract. We present a new tropospheric ozone dataset based on TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P) total ozone measurements combined with stratospheric ozone data from the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by assimilating ozone observations from the Microwave Limb Sounder (MLS). The BASCOE stratospheric data are interpolated to the S5P observations and subtracted from the TROPOMI total ozone data. The difference is equal to the tropospheric ozone residual column from the surface up to the tropopause. The tropospheric ozone columns are retrieved at the full spatial resolution of the TROPOMI sensor (5.5×3.5 km2) with daily global coverage. Compared to the Ozone Mapping and Profiler Suite Modern-Era Retrospective analysis for Research and Applications 2 (OMPS-MERRA-2) data, a global mean positive bias of 3.3 DU is found for the analysed period April 2018 to June 2020. A small negative bias of about −0.91 DU is observed in the tropics relative to the operational TROPOMI tropical tropospheric data based on the convective cloud differential (CCD) algorithm throughout the same period. The new tropospheric ozone data (S5P-BASCOE) are compared to a set of globally distributed ozonesonde data integrated up to the tropopause level. We found 2254 comparisons with cloud-free TROPOMI observations within 25 km of the stations. In the global mean, S5P-BASCOE deviates by 2.6 DU from the integrated ozonesondes. Depending on the latitude the S5P-BASCOE deviate from the sondes and between −4.8 and 7.9 DU, indicating a good agreement. However, some exceptional larger positive deviations up to 12 DU are found, especially in the northern polar regions (north of 70∘). The monthly mean tropospheric column and time series for selected areas showed the expected spatial and temporal pattern, such as the wave one structure in the tropics or the seasonal cycle, including a summer maximum, in the mid-latitudes.

OpenIFS/AC: atmospheric chemistry and aerosol in OpenIFS 43r3

Abstract. In this paper, we report on the first implementation of atmospheric chemistry and aerosol as part of the European Centre for Medium-Range Weather Forecasts (ECMWF) OpenIFS model. OpenIFS is a portable version of ECMWF's global numerical weather prediction model. Modules and input data for model cycle CY43R3, which have been developed as part of the Copernicus Atmosphere Monitoring Service (CAMS), have been ported to OpenIFS with the modified CB05 tropospheric chemistry scheme, the bulk bin tropospheric aerosol module, and the option to use Belgian Assimilation System for Chemical ObsErvations (BASCOE)-based stratospheric ozone chemistry. We give an overview of the model, and describe the datasets used for emissions and dry deposition, which are similar to those used in the model configuration applied to create the CAMS reanalysis. We evaluate two reference model configurations with and without the stratospheric chemistry extension against standard observational datasets for tropospheric ozone, surface carbon monoxide (CO), tropospheric nitrogen dioxide (NO2), and aerosol optical depth. The results give basic confidence in the model implementation and configuration. This OpenIFS version with atmospheric composition components is open to the scientific user community under a standard OpenIFS license.

Coupled Stratospheric Chemistry–Meteorology Data Assimilation. Part I: Physical Background and Coupled Modeling Aspects

A coupled stratospheric chemistry–meteorology model was developed by combining the Canadian operational weather prediction model Global Environmental Multiscale (GEM) with a comprehensive stratospheric photochemistry model from the Belgian Assimilation System for Chemical ObsErvations (BASCOE). The coupled model was called GEM-BACH for GEM-Belgian Atmospheric CHemistry. The coupling was made across a chemical interface that preserves time-splitting while being modular, allowing GEM to run with or without chemistry. An evaluation of the coupling was performed by comparing the coupled model, refreshed by meteorological analyses every 6 h, against the standard offline chemical transport model (CTM) approach. Results show that the dynamical meteorological consistency between meteorological analysis times far outweighs the error created by the jump resulting from the meteorological analysis increments at regular time intervals, irrespective of whether a 3D-Var or 4D-Var meteorological analysis is used. Arguments in favor of using the same horizontal resolution for chemistry, meteorology, and meteorological and chemical analysis increments are also presented. GEM-BACH forecasts refreshed by meteorological analyses every 6 h were compared against independent measurements of temperature, long-lived species, ozone and water vapor. The comparison showed a relatively good agreement throughout the stratosphere except for an upper-level warm temperature bias and an ozone deficit of nearly 15%. In particular, the coupled model simulation during an ozone hole event gives better ozone concentrations than a 4D-Var chemical assimilation at a lower resolution.

Technical note: Reanalysis of Aura MLS chemical 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.

Harmonisation and diagnostics of MIPAS ESA CH<sub>4</sub> and N<sub>2</sub>O profiles using data assimilation

Abstract. This paper discusses assimilation experiments of methane (CH4) and nitrous oxide (N2O) profiles retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). Here we focus on data versions 6 and 7 provided by the ESA processor. These data sets have been assimilated by the Belgian Assimilation System for Chemical ObsErvations (BASCOE). The CH4 and N2O retrieved profiles can oscillate, especially in the tropical lower stratosphere. Using the averaging kernels of the observations and a background error covariance matrix, which has previously been calibrated, allows the system to partly remedy this issue and provide assimilated fields that are more regular vertically. In general, there is a good agreement between the BASCOE analyses and independent observations from ACE–FTS (CH4 and N2O) and MLS (N2O), demonstrating the general good quality of CH4 and N2O retrievals provided by MIPAS ESA. Nevertheless, this study also identifies two issues in these data sets. First, time series of the observations show unexpected discontinuities due to an abrupt change in the gain of MIPAS band B, generally occurring after the instrument decontamination. Since the calibration is performed weekly, the abrupt change in the gain affects the measurements until the subsequent calibration is performed. Second, the correlations between BASCOE analyses and independent observations are poor in the lower stratosphere, especially in the tropics, probably due to the presence of outliers in the assimilated data. In this region, we recommend using MIPAS CH4 and N2O retrievals with caution.

C-IFS-CB05-BASCOE: stratospheric chemistry in the Integrated Forecasting System of ECMWF

Abstract. We present a model description and benchmark evaluation of an extension of the tropospheric chemistry module in the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF) with stratospheric chemistry, referred to as C-IFS-CB05-BASCOE (for brevity here referred to as C-IFS-TS). The stratospheric chemistry originates from the one used in the Belgian Assimilation System for Chemical ObsErvations (BASCOE), and is here combined with the modified CB05 chemistry module for the troposphere as currently used operationally in the Copernicus Atmosphere Monitoring Service (CAMS). In our approach either the tropospheric or stratospheric chemistry module is applied, depending on the altitude of each individual grid box with respect to the tropopause. An evaluation of a 2.5-year long C-IFS-TS simulation with respect to various satellite retrieval products and in situ observations indicates good performance of the system in terms of stratospheric ozone, and a general improvement in terms of stratospheric composition compared to the C-IFS predecessor model version. Possible issues with transport processes in the stratosphere are identified. This marks a key step towards a chemistry module within IFS that encompasses both tropospheric and stratospheric composition, and could expand the CAMS analysis and forecast capabilities in the near future.

EnKF and 4D-Var data assimilation with chemical transport model BASCOE (version 05.06)

Abstract. We compare two optimized chemical data assimilation systems, one based on the ensemble Kalman filter (EnKF) and the other based on four-dimensional variational (4D-Var) data assimilation, using a comprehensive stratospheric chemistry transport model (CTM). This work is an extension of the Belgian Assimilation System for Chemical ObsErvations (BASCOE), initially designed to work with a 4D-Var data assimilation. A strict comparison of both methods in the case of chemical tracer transport was done in a previous study and indicated that both methods provide essentially similar results. In the present work, we assimilate observations of ozone, HCl, HNO3, H2O and N2O from EOS Aura-MLS data into the BASCOE CTM with a full description of stratospheric chemistry. Two new issues related to the use of the full chemistry model with EnKF are taken into account. One issue is a large number of error variance parameters that need to be optimized. We estimate an observation error variance parameter as a function of pressure level for each observed species using the Desroziers method. For comparison purposes, we apply the same estimate procedure in the 4D-Var data assimilation, where both scale factors of the background and observation error covariance matrices are estimated using the Desroziers method. However, in EnKF the background error covariance is modelled using the full chemistry model and a model error term which is tuned using an adjustable parameter. We found that it is adequate to have the same value of this parameter based on the chemical tracer formulation that is applied for all observed species. This is an indication that the main source of model error in chemical transport model is due to the transport. The second issue in EnKF with comprehensive atmospheric chemistry models is the noise in the cross-covariance between species that occurs when species are weakly chemically related at the same location. These errors need to be filtered out in addition to a localization based on distance. The performance of two data assimilation methods was assessed through an 8-month long assimilation of limb sounding observations from EOS Aura MLS. This paper discusses the differences in results and their relation to stratospheric chemical processes. Generally speaking, EnKF and 4D-Var provide results of comparable quality but differ substantially in the presence of model error or observation biases. If the erroneous chemical modelling is associated with moderately fast chemical processes, but whose lifetimes are longer than the model time step, then EnKF performs better, while 4D-Var develops spurious increments in the chemically related species. If, however, the observation biases are significant, then 4D-Var is more robust and is able to reject erroneous observations while EnKF does not.

Copernicus stratospheric ozone service, 2009–2012: validation, system intercomparison and roles of input data sets

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 stratosphere, but this requires the assimilation of observations from nadir-looking instruments as well as the assimilation of profiles, which are well resolved vertically and extend into the lowermost stratosphere.

Comparison of the ensemble Kalman filter and 4D-Var assimilation methods using a stratospheric tracer transport model

Abstract. An ensemble Kalman filter (EnKF) assimilation method is applied to the tracer transport using the same stratospheric transport model as in the four-dimensional variational (4D-Var) assimilation system BASCOE (Belgian Assimilation System for Chemical ObsErvations). This EnKF version of BASCOE was built primarily to avoid the large costs associated with the maintenance of an adjoint model. The EnKF developed in BASCOE accounts for two adjustable parameters: a parameter α controlling the model error term and a parameter r controlling the observational error. The EnKF system is shown to be markedly sensitive to these two parameters, which are adjusted based on the monitoring of a χ2 test measuring the misfit between the control variable and the observations. The performance of the EnKF and 4D-Var versions was estimated through the assimilation of Aura-MLS (microwave limb sounder) ozone observations during an 8-month period which includes the formation of the 2008 Antarctic ozone hole. To ensure a proper comparison, despite the fundamental differences between the two assimilation methods, both systems use identical and carefully calibrated input error statistics. We provide the detailed procedure for these calibrations, and compare the two sets of analyses with a focus on the lower and middle stratosphere where the ozone lifetime is much larger than the observational update frequency. Based on the observation-minus-forecast statistics, we show that the analyses provided by the two systems are markedly similar, with biases less than 5% and standard deviation errors less than 10% in most of the stratosphere. Since the biases are markedly similar, they most probably have the same causes: these can be deficiencies in the model and in the observation data set, but not in the assimilation algorithm nor in the error calibration. The remarkably similar performance also shows that in the context of stratospheric transport, the choice of the assimilation method can be based on application-dependent factors, such as CPU cost or the ability to generate an ensemble of forecasts.

Technical Note: Spectral representation of spatial correlations in variational assimilation with grid point models and application to the Belgian Assimilation System for Chemical Observations (BASCOE)

Abstract. The formulation of the background error covariances represented in the spectral space is discussed in the context of univariate assimilation relying on a grid point model, leaving out all the aspects of balances between the different control variables needed in meteorological assimilation. The spectral transform operations are discussed in the case of a spherical harmonics basis and we stress that there is no need for an inverse spectral transform and of a Gaussian grid. The analysis increments are thus produced directly on the model grid. The practice of producing analysis increments on a horizontal Gaussian grid and then interpolating to an equally spaced grid is also shown to produce a degradation of the analysis. The method discussed in this paper allows the implementation of separable and non-separable spatial correlations. The separable formulation has been implemented in the Belgian Assimilation System for Chemical ObsErvations (BASCOE) and its impact on the assimilation of O3 observed by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is shown. To promote the use of this method by other non-meteorological variational systems and in particular chemistry, the Fortran code developed is made available to the community.

Evaluation of Ozone Analyses From UARS MLS Assimilation by BASCOE Between 1992 and 1997

We present the analyses of UARS MLS ozone data obtained by the Belgian Assimilation System for Chemical ObsErvations (BASCOE). This system, based on the 4D-var method, is dedicated to the assimilation of stratospheric chemistry observations. It uses a 3-D Chemical Transport Model (3D-CTM) including 57 chemical species with explicit calculation of stratospheric chemistry. The CTM is driven by ECMWF ERA-40 analyses of winds and temperature, with a horizontal grid of 3.75 in latitude by 5 in longitude, and with 37 pressure levels from the surface to 0.1 hPa. BASCOE has assimilated UARS MLS observations acquired during the period 1992-1997. We discuss how BASCOE is able to reproduce MLS data, and we evaluate the BASCOE analyses with respect to independent observations from UARS HALOE, ozonesondes, and ground-based lidars. An excellent agreement is found with independent observations (bias usually less than 10%), except in the lowermost stratosphere and in the Antarctic ozone hole. The performances of BASCOE ozone analyses are also compared to those of two other long-term ozone reanalyses; namely, ERA-40 and ERA-Interim, both from ECMWF. Finally, sensitivity test based on BASCOE free model runs suggest that ozone analyses during the ozone hole period would be greatly improved by driving BASCOE with the dynamical fields of the new ECMWF reanalyses ERA-Interim. This work is part of the Stratospheric Ozone Profile Record service raised by the GMES Service Element PROMOTE.