Data assimilation of stratospheric constituents: a review

International audienceThe data assimilation of stratospheric constituents is reviewed. The data assimilation method is introduced, with particular consideration to its application to stratospheric constituent measurements. Differences from meteorological data assimilation are outlined. Historically, two approaches have been used to carry out constituent assimilation. One approach has carried constituent assimilation out as part of a numerical weather prediction system; the other has carried it out in a standalone chemical model, often with a more sophisticated representation of chemical processes. Whereas the aim of the numerical weather prediction approach has been to improve weather forecasts, the aims of the chemical model approach have included providing chemical forecasts and analyses of chemical constituents. A range of constituent assimilation systems developed in these two areas is presented and strengths and weaknesses discussed. The use of stratospheric constituent data assimilation to evaluate models, observations and analyses, and to provide analyses of constituents, monitor ozone, and make ozone forecasts is discussed. Finally, the current state of affairs is assessed, future directions are discussed, and potential key drivers identified

A 3D-CTM with detailed online PSC-microphysics: analysis of the Antarctic winter 2003 by comparison with satellite observations

International audienceWe present the first detailed microphysical simulations which are performed online within the framework of a global 3-D chemical transport model (CTM) with full chemistry. The model describes the formation and evolution of four types of polar stratospheric cloud (PSC) particles. Aerosol freezing and other relevant microphysical processes are treated in a full explicit way. Each particle type is described by a binned size distribution for the number density and chemical composition. This set-up allows for an accurate treatment of sedimentation and for detailed calculation of surface area densities and optical properties. Simulations are presented for the Antarctic winter of 2003 and comparisons are made to a diverse set of satellite observations (optical and chemical measurements of POAM III and MIPAS) to illustrate the capabilities of the model. This study shows that a combined resolution approach where microphysical processes are simulated in coarse-grained conditions gives good results for PSC formation and its large-scale effect on the chemical environment through processes such as denitrification, dehydration and ozone loss. It is also shown that the influence of microphysical parameters can be measured directly from these processes

4D-Var Assimilation of MIPAS chemical observations: ozone and nitrogen dioxide analyses

International audienceThis paper discusses the global analyses of stratospheric ozone (O3) and nitrogen dioxide (NO2) obtained by the Belgian Assimilation System for Chemical Observations from Envisat (BASCOE). Based on a chemistry transport model (CTM) and the 4-dimensional variational (4D-Var) method, BASCOE has assimilated chemical observations of O3, NO2, HNO3, N2O, CH4 and H2O, made between July 2002 and March 2004 by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard the European Space Agency (ESA) Environment Satellite (ENVISAT). This corresponds to the entire period during which MIPAS was operating at its nominal resolution. Our analyses are evaluated against assimilated MIPAS data and independent HALOE (HALogen Occultation Experiment) and POAM-III (Polar Ozone and Aerosol Measurement) satellite data. A good agreement is generally found between the analyses and these datasets, in both cases within the estimated error bars of the observations. The benefit of data assimilation is also evaluated using a BASCOE free model run. For O3, the gain from the assimilation is significant during ozone hole conditions, and in the lower stratosphere. Elsewhere, the free model run is within the MIPAS uncertainties and the assimilation does not provide significant improvement. For NO2, the gain from the assimilation is realized through most of the stratosphere. Using the BASCOE analyses, we estimate the differences between MIPAS data and independent data from HALOE and POAM-III, and find results close to those obtained by classical validation methods involving only direct measurement-to-measurement comparisons. Our results extend and reinforce previous MIPAS data validation efforts by taking account of a much larger variety of atmospheric states and measurement conditions. This study discusses possible further developments of the BASCOE data assimilation system; these concern the horizontal resolution, a better filtering of NO2 observations, and the photolysis calculation near the lid of the model. The ozone analyses are publicly available via the PROMOTE project http://www.gse-promote.org)

Harmonisation and diagnostics of MIPAS ESA CH4 and N2O profiles using data assimilation

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

Global observations of tropospheric BrO columns using GOME-2 satellite data

Measurements from the GOME-2 satellite instrument have been analyzed for tropospheric BrO using a residual technique that combines measured BrO columns and estimates of the stratospheric BrO content from a climatological approach driven by O<sub>3</sub> and NO<sub>2</sub> observations. Comparisons between the GOME-2 results and BrO vertical columns derived from correlative ground-based and SCIAMACHY nadir observations, present a good level of consistency. We show that the adopted technique enables separation of stratospheric and tropospheric fractions of the measured total BrO columns and allows quantitative study of the BrO plumes in polar regions. While some satellite observed plumes of enhanced BrO can be explained by stratospheric descending air, we show that most BrO hotspots are of tropospheric origin, although they are often associated to regions with low tropopause heights as well. Elaborating on simulations using the <i>p</i>-TOMCAT tropospheric chemical transport model, this result is found to be consistent with the mechanism of bromine release through sea salt aerosols production during blowing snow events. No definitive conclusion can be drawn however on the importance of blowing snow sources in comparison to other bromine release mechanisms. Outside polar regions, evidence is provided for a global tropospheric BrO background with column of 1–3 × 10<sup>13</sup> molec cm<sup>−2</sup>, consistent with previous estimates

Comprehensive evaluation of the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis against independent observations: Reactive gases

The Copernicus Atmosphere Monitoring Service (CAMS) is operationally providing forecast and reanalysis products of air quality and atmospheric composition. In this article, we present an extended evaluation of the CAMS global reanalysis data set of four reactive gases, namely, ozone (O-3), carbon monoxide (CO), nitrogen dioxide (NO2), and formaldehyde (HCHO), using multiple independent observations. Our results show that the CAMS model system mostly provides a stable and accurate representation of the global distribution of reactive gases over time. Our findings highlight the crucial impact of satellite data assimilation and emissions, investigated through comparison with a model run without assimilated data. Stratospheric and tropospheric O-3 are mostly well constrained by the data assimilation, except over Antarctica after 2012/2013 due to changes in the assimilated data. Challenges remain for O-3 in the Tropics and high-latitude regions during winter and spring. At the surface and for short-lived species (NO2), data assimilation is less effective. Total column CO in the CAMS reanalysis is well constrained by the assimilated satellite data. The control run, however, shows large overestimations of total column CO in the Southern Hemisphere and larger year-to-year variability in all regions. Concerning the long-term stability of the CAMS model, we note drifts in the time series of biases for surface O-3 and CO in the Northern midlatitudes and Tropics and for NO2 over East Asia, which point to biased emissions. Compared to the previous Monitoring Atmospheric Composition and Climate reanalysis, changes in the CAMS chemistry module and assimilation system helped to reduce biases and enhance the long-term temporal consistency of model results for the CAMS reanalysis

Technical note: Reanalysis of Aura MLS chemical observations

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 201