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Clouds in Antarctica are key elements that affect radiative forcing and thus Antarctic climate evolution. Although the vast majority of clouds are composed of ice crystals, a non-negligible fraction constitutes supercooled liquid water (SLW; water held in liquid form below 0 °C). Numerical weather prediction models have great difficulty in forecasting SLW clouds over Antarctica, favouring ice at the expense of liquid water and therefore incorrectly estimating the cloud radiative forcing. Remote-sensing observations of SLW clouds have been carried out for several years at Concordia Station (75° S, 123° E; 3233 m above mean sea level), combining active lidar measurements (SLW cloud detection) and passive HAMSTRAD microwave measurements (liquid water path, LWP). The present project aimed at in situ observations of SLW clouds using sondes developed by the company Anasphere, specifically designed for SLW content (SLWC) measurements. These SLWC sondes were coupled to standard meteorological pressure–temperature–humidity sondes from Vaisala and released under meteorological balloons. During the 2021–2022 summer campaign, 15 launches were made, of which 7 were scientifically exploitable above a height of 400 m above ground level, a threshold height imposed by the time the SLWC sonde takes to stabilize after launch. The three main outcomes from our analyses are as follows: (a) the first in situ observations so far of SLW clouds in Antarctica with SLWC sondes; (b) on average, the consistency of SLW cloud heights as observed by in situ sondes and remote-sensing lidar; and (c) the liquid water path (vertically integrated SLWC) deduced by the sondes being generally equal to or greater than the LWP remotely sensed by HAMSTRAD. In general, the SLW clouds were observed in a layer close to saturation (U > 80 %) or saturated (U ∼ 100 %–105 %) just below or at the lowermost part of the entrainment zone, or capping inversion zone, which exists at the top of the planetary boundary layer and is characterized by an inflection point in the potential temperature vertical profile. Our results are consistent with the theoretical view that SLW clouds form and remain at the top of the planetary boundary layer.

Clouds affect the Earth climate with an impact that depends on the cloud nature (solid and/or liquid water). Although the Antarctic climate is changing rapidly, cloud observations are sparse over Antarctica due to few ground stations and satellite observations. The Concordia station is located on the eastern Antarctic Plateau (75∘ S, 123∘ E; 3233 m above mean sea level), one of the driest and coldest places on Earth. We used observations of clouds, temperature, liquid water, and surface irradiance performed at Concordia during four austral summers (December 2018–2021) to analyse the link between liquid water and temperature and its impact on surface irradiance in the presence of supercooled liquid water (liquid water for temperature less than 0 ∘C) clouds (SLWCs). Our analysis shows that, within SLWCs, temperature logarithmically increases from −36.0 to −16.0 ∘C when liquid water path increases from 1.0 to 14.0 g m−2. The SLWC radiative forcing is positive and logarithmically increases from 0.0 to 70.0 W m−2 when liquid water path increases from 1.2 to 3.5 g m−2. This is mainly due to the downward longwave component that logarithmically increases from 0 to 90 W m−2 when liquid water path increases from 1.0 to 3.5 g m−2. The attenuation of shortwave incoming irradiance (that can reach more than 100 W m−2) is almost compensated for by the upward shortwave irradiance because of high values of surface albedo. Based on our study, we can extrapolate that, over the Antarctic continent, SLWCs have a maximum radiative forcing that is rather weak over the eastern Antarctic Plateau (0 to 7 W m−2) but 3 to 5 times larger over West Antarctica (0 to 40 W m−2), maximizing in summer and over the Antarctic Peninsula.

Geostationary meteorological satellites are unique tools to monitor atmospheric aerosols from space. The observation of the Earth several times per hour allows these types of imaging systems to provide high-temporal-resolution observations of these suspended particles, which are of interest for research and operational topics, including climate, air quality, numerical weather prediction, and volcanic risk management. However, some challenges need to be addressed to achieve the sub-daily retrieval of aerosol properties mainly due to the varying sensitivity of geostationary imagers to aerosols during the day. In this article we propose a new algorithm named iAERUS-GEO (instantaneous Aerosol and surfacE Retrieval Using Satellites in GEOstationary orbit) that estimates the diurnal evolution of aerosol optical depth (AOD) over land and ocean from the Meteosat Second Generation (MSG) satellite. This is achieved by the use of an optimal-estimation method combined with several aerosol models and other features, including the daily retrieval of the surface reflectance directionality using Kalman filtering. AOD estimates provided by iAERUS-GEO every 15 min – the acquisition frequency of the Spinning Enhanced Visible InfraRed Imager (SEVIRI) on MSG – are assessed with collocated reference aerosol observations. First, comparison to AERONET ground-based data proves the overall satisfactory accuracy of iAERUS-GEO over land, with the exception of some higher biases found over bright surfaces and for high scattering angles. The confidence measure provided by iAERUS-GEO is proved useful to filter these less satisfactory retrievals that generally arise due to a low information content on aerosols provided by SEVIRI. Second, comparison to the GRASP/POLDER satellite product shows similar scores for the two aerosol data sets, with a significantly larger number of retrievals for iAERUS-GEO. This added value – which we illustrate here by inspecting the sub-daily variation in AOD over selected regions – allows geostationary satellites to break the temporal barrier set by traditional aerosol remote sensing from the low Earth orbit. Furthermore, the aerosol retrievals presented in this work are expected to be improved in the near future thanks to the enhanced sensing capabilities of the upcoming Meteosat Third Generation Imager mission.

This paper presents the first results about the assimilation of CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) extinction coefficient measurements onboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite in the MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle) chemistry transport model of Météo-France. This assimilation module is an extension of the aerosol optical depth (AOD) assimilation system already presented by Sič et al. (2016). We focus on the period of the TRAQA (TRAnsport à longue distance et Qualité de l’Air dans le bassin méditerranéen) field campaign that took place during summer 2012. This period offers the opportunity to have access to a large set of aerosol observations from instrumented aircraft, balloons, satellite and ground-based stations. We evaluate the added value of CALIOP assimilation with respect to the model free run by comparing both fields to independent observations issued from the TRAQA field campaign. In this study we focus on the desert dust outbreak which happened during late June 2012 over the Mediterranean Basin (MB) during the TRAQA campaign. The comparison with the AERONET (Aerosol Robotic Network) AOD measurements shows that the assimilation of CALIOP lidar observations improves the statistics compared to the model free run. The correlation between AERONET and the model (assimilation) is 0.682 (0.753); the bias and the root mean square error (RMSE), due to CALIOP assimilation, are reduced from −0.063 to 0.048 and from 0.183 to 0.148, respectively. Compared to MODIS (Moderate-resolution Imaging Spectroradiometer) AOD observations, the model free run shows an underestimation of the AOD values, whereas the CALIOP assimilation corrects this underestimation and shows a quantitative good improvement in terms of AOD maps over the MB. The correlation between MODIS and the model (assimilation) during the dust outbreak is 0.47 (0.52), whereas the bias is −0.18 (−0.02) and the RMSE is 0.36 (0.30). The comparison of in situ aircraft and balloon measurements to both modelled and assimilated outputs shows that the CALIOP lidar assimilation highly improves the model aerosol field. The evaluation with the LOAC (Light Optical Particle Counter) measurements indicates that the aerosol vertical profiles are well simulated by the direct model but with a general underestimation of the aerosol number concentration, especially in the altitude range 2–5 km. The CALIOP assimilation improves these results by a factor of 2.5 to 5. Analysis of the vertical distribution of the desert aerosol concentration shows that the aerosol dust transport event is well captured by the model but with an underestimated intensity. The assimilation of CALIOP observations allows the improvement of the geographical representation of the event within the model as well as its intensity by a factor of 2 in the altitude range 1–5 km.

A comprehensive analysis of the water budget over the Dome C (Concordia, Antarctica) station has been performed during the austral summer 2018–2019 as part of the Year of Polar Prediction (YOPP) international campaign. Thin (∼100 m deep) supercooled liquid water (SLW) clouds have been detected and analysed using remotely sensed observations at the station (tropospheric depolarization lidar, the H2O Antarctica Microwave Stratospheric and Tropospheric Radiometer (HAMSTRAD), net surface radiation from the Baseline Surface Radiation Network (BSRN)), radiosondes, and satellite observations (CALIOP, Cloud-Aerosol LIdar with Orthogonal Polarization/CALIPSO, Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observations) combined with a specific configuration of the numerical weather prediction model: ARPEGE-SH (Action de Recherche Petite Echelle Grande Echelle – Southern Hemisphere). The analysis shows that SLW clouds were present from November to March, with the greatest frequency occurring in December and January when ∼50 % of the days in summer time exhibited SLW clouds for at least 1 h. Two case studies are used to illustrate this phenomenon. On 24 December 2018, the atmospheric planetary boundary layer (PBL) evolved following a typical diurnal variation, which is to say with a warm and dry mixing layer at local noon thicker than the cold and dry stable layer at local midnight. Our study showed that the SLW clouds were observed at Dome C within the entrainment and the capping inversion zones at the top of the PBL. ARPEGE-SH was not able to correctly estimate the ratio between liquid and solid water inside the clouds with the liquid water path (LWP) strongly underestimated by a factor of 1000 compared to observations. The lack of simulated SLW in the model impacted the net surface radiation that was 20–30 W m−2 higher in the BSRN observations than in the ARPEGE-SH calculations, mainly attributable to the BSRN longwave downward surface radiation being 50 W m−2 greater than that of ARPEGE-SH. The second case study took place on 20 December 2018, when a warm and wet episode impacted the PBL with no clear diurnal cycle of the PBL top. SLW cloud appearance within the entrainment and capping inversion zones coincided with the warm and wet event. The amount of liquid water measured by HAMSTRAD was ∼20 times greater in this perturbed PBL than in the typical PBL. Since ARPEGE-SH was not able to accurately reproduce these SLW clouds, the discrepancy between the observed and calculated net surface radiation was even greater than in the typical PBL case, reaching +50 W m−2, mainly attributable to the downwelling longwave surface radiation from BSRN being 100 W m−2 greater than that of ARPEGE-SH. The model was then run with a new partition function favouring liquid water for temperatures below −20 down to −40 ∘C. In this test mode, ARPEGE-SH has been able to generate SLW clouds with modelled LWP and net surface radiation consistent with observations during the typical case, whereas, during the perturbed case, the modelled LWP was 10 times less than the observations and the modelled net surface radiation remained lower than the observations by ∼50 W m−2. Accurately modelling the presence of SLW clouds appears crucial to correctly simulate the surface energy budget over the Antarctic Plateau.

We present an observing simulated system experiment (OSSE) dedicated to evaluate the potential added value from the Sentinel-4 and the Sentinel-5P observations on tropospheric ozone composition. For this purpose, the ozone data of Sentinel-4 (Ultraviolet Visible Near-infrared) and Sentinel-5P (TROPOspheric Monitoring Instrument) on board a geostationary (GEO) and a low-Earth-orbit (LEO) platform, respectively, have been simulated using the DISAMAR inversion package for the summer 2003. To ensure the robustness of the results, the OSSE has been configured with conservative assumptions. We simulate the reality by combining two chemistry transport models (CTMs): the LOng Term Ozone Simulation – EURopean Operational Smog (LOTOS-EUROS) and the Transport Model version 5 (TM5). The assimilation system is based on a different CTM, the MOdèle de Chimie Atmosphérique à Grande Echelle (MOCAGE), combined with the 3-D variational technique. The background error covariance matrix does not evolve in time and its variance is proportional to the field values. The simulated data are formed of six eigenvectors to minimize the size of the dataset by removing the noise-dominated part of the observations. The results show that the satellite data clearly bring direct added value around 200 hPa for the whole assimilation period and for the whole European domain, while a likely indirect added value is identified but not for the whole period and domain at 500 hPa, and to a lower extent at 700 hPa. In addition, the ozone added value from Sentinel-5P (LEO) appears close to that from Sentinel-4 (GEO) in the free troposphere (200–500 hPa) in our OSSE. The outcome of our study is a result of the OSSE design and the choice within each of the components of the system.

We present an Observing System Simulation Experiment (OSSE) dedicated to the evaluation of the added value of the Sentinel-4 and Sentinel-5P missions for tropospheric nitrogen dioxide (NO2). Sentinel-4 is a geostationary (GEO) mission covering the European continent, providing observations with high temporal resolution (hourly). Sentinel-5P is a low Earth orbit (LEO) mission providing daily observations with a global coverage. The OSSE experiment has been carefully designed, with separate models for the simulation of observations and for the assimilation experiments and with conservative estimates of the total observation uncertainties. In the experiment we simulate Sentinel-4 and Sentinel-5P tropospheric NO2 columns and surface ozone concentrations at 7 by 7 km resolution over Europe for two 3-month summer and winter periods. The synthetic observations are based on a nature run (NR) from a chemistry transport model (MOCAGE) and error estimates using instrument characteristics. We assimilate the simulated observations into a chemistry transport model (LOTOS-EUROS) independent of the NR to evaluate their impact on modelled NO2 tropospheric columns and surface concentrations. The results are compared to an operational system where only ground-based ozone observations are ingested. Both instruments have an added value to analysed NO2 columns and surface values, reflected in decreased biases and improved correlations. The Sentinel-4 NO2 observations with hourly temporal resolution benefit modelled NO2 analyses throughout the entire day where the daily Sentinel-5P NO2 observations have a slightly lower impact that lasts up to 3–6 h after overpass. The evaluated benefits may be even higher in reality as the applied error estimates were shown to be higher than actual errors in the now operational Sentinel-5P NO2 products. We show that an accurate representation of the NO2 profile is crucial for the benefit of the column observations on surface values. The results support the need for having a combination of GEO and LEO missions for NO2 analyses in view of the complementary benefits of hourly temporal resolution (GEO, Sentinel-4) and global coverage (LEO, Sentinel-5P).

In the framework of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr, last access: 22 June 2018) project, we study the evolution of surface ozone over the Mediterranean Basin (MB) with a focus on summertime over the time period 2000–2100, using the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) outputs from 13 models. We consider three different periods (2000, 2030 and 2100) and the four Representative Concentration Pathways (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) to study the changes in the future ozone and its budget. We use a statistical approach to compare and discuss the results of the models. We discuss the behavior of the models that simulate the surface ozone over the MB. The shape of the annual cycle of surface ozone simulated by ACCMIP models is similar to the annual cycle of the ozone observations, but the model values are biased high. For the summer, we found that most of the models overestimate surface ozone compared to observations over the most recent period (1990–2010). Compared to the reference period (2000), we found a net decrease in the ensemble mean surface ozone over the MB in 2030 (2100) for three RCPs: −14 % (−38 %) for RCP2.6, −9 % (−24 %) for RCP4.5 and −10 % (−29 %) for RCP6.0. The surface ozone decrease over the MB for these scenarios is much more pronounced than the relative changes of the global tropospheric ozone burden. This is mainly due to the reduction in ozone precursors and to the nitrogen oxide (NOx = NO + NO2)-limited regime over the MB. For RCP8.5, the ensemble mean surface ozone is almost constant over the MB from 2000 to 2100. We show how the future climate change and in particular the increase in methane concentrations can offset the benefits from the reduction in emissions of ozone precursors over the MB.

We use the technique of Observing System Simulation Experiments (OSSEs) to quantify the impact of spaceborne carbon monoxide (CO) total column observations from the Sentinel-5 Precursor (S-5P) platform on tropospheric analyses and forecasts. We focus on Europe for the period of northern summer 2003, when there was a severe heat wave episode associated with extremely hot and dry weather conditions. We describe different elements of the OSSE: (i) the nature run (NR), i.e., the truth; (ii) the CO synthetic observations; (iii) the assimilation run (AR), where we assimilate the observations of interest; (iv) the control run (CR), in this study a free model run without assimilation; and (v) efforts to establish the fidelity of the OSSE results. Comparison of the results from AR and the CR, against the NR, shows that CO total column observations from S-5P provide a significant benefit (at the 99 % confidence level) at the surface, with the largest benefit occurring over land in regions far away from emission sources. Furthermore, the S-5P CO total column observations are able to capture phenomena such as the forest fires that occurred in Portugal during northern summer 2003. These results provide evidence of the benefit of S-5P observations for monitoring processes contributing to atmospheric pollution.

Since the 1970s, the French space agency CNES has developed boundary-layer pressurised balloons (BLPBs) with the capability to transport lightweight scientific payloads at isopycnic level and offer a quasi-Lagrangian sampling of the lower atmosphere over very long distances and durations (up to several weeks).Electrochemical concentration cell (ECC) ozonesondes are widely used under small sounding balloons. However, their autonomy is limited to a few hours owing to power consumption and electrolyte evaporation. An adaptation of the ECC sonde has been developed specifically for long-duration BLPB flights. Compared to conventional ECC sondes, the main feature is the possibility of programming periodic measurement sequences (with possible remote control during the flight). To increase the ozonesonde autonomy, the strategy has been adopted of short measurement sequences (2–3 min) regularly spaced in time (e.g. every 15 min). The rest of the time, the sonde pump is turned off. Results of preliminary ground-based tests are first presented. In particular, the sonde was able to provide correct ozone concentrations against a reference UV-absorption ozone analyser every 15 min for 4 days. Then we illustrate results from 16 BLBP flights launched over the western Mediterranean during three summer field campaigns of the ChArMEx project (http://charmex.lsce.ipsl.fr): TRAQA in 2012, and ADRIMED and SAFMED in 2013. BLPB drifting altitudes were in the range 0.25–3.2 km. The longest flight lasted more than 32 h and covered more than 1000 km. Satisfactory data were obtained when compared to independent ozone measurements close in space and time. The quasi-Lagrangian measurements allowed a first look at ozone diurnal evolution in the marine boundary layer as well as in the lower free troposphere. During some flight segments, there was indication of photochemical ozone production in the marine boundary layer or even in the free troposphere, at rates ranging from 1 to 2 ppbv h −1, which is slower than previously found in the boundary layer over land in the same region.

In this study, we describe the development of the aerosol optical depth (AOD) assimilation module in the chemistry transport model (CTM) MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle). Our goal is to assimilate the spatially averaged 2-D column AOD data from the National Aeronautics and Space Administration (NASA) Moderate-resolution Imaging Spectroradiometer (MODIS) instrument, and to estimate improvements in a 3-D CTM assimilation run compared to a direct model run. Our assimilation system uses 3-D-FGAT (first guess at appropriate time) as an assimilation method and the total 3-D aerosol concentration as a control variable. In order to have an extensive validation dataset, we carried out our experiment in the northern summer of 2012 when the pre-ChArMEx (CHemistry and AeRosol MEditerranean EXperiment) field campaign TRAQA (TRAnsport à longue distance et Qualité de l'Air dans le bassin méditerranéen) took place in the western Mediterranean basin. The assimilated model run is evaluated independently against a range of aerosol properties (2-D and 3-D) measured by in situ instruments (the TRAQA size-resolved balloon and aircraft measurements), the satellite Spinning Enhanced Visible and InfraRed Imager (SEVIRI) instrument and ground-based instruments from the Aerosol Robotic Network (AERONET) network. The evaluation demonstrates that the AOD assimilation greatly improves aerosol representation in the model. For example, the comparison of the direct and the assimilated model run with AERONET data shows that the assimilation increased the correlation (from 0.74 to 0.88), and reduced the bias (from 0.050 to 0.006) and the root mean square error in the AOD (from 0.12 to 0.07). When compared to the 3-D concentration data obtained by the in situ aircraft and balloon measurements, the assimilation consistently improves the model output. The best results as expected occur when the shape of the vertical profile is correctly simulated by the direct model. We also examine how the assimilation can influence the modelled aerosol vertical distribution. The results show that a 2-D continuous AOD assimilation can improve the 3-D vertical profile, as a result of differential horizontal transport of aerosols in the model.

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.

Pollution aerosols strongly influence the composition of the Western Mediterranean basin, but at present little is known on their optical properties. We report in this study in situ observations of the single scattering albedo (ω) of pollution aerosol plumes measured over the Western Mediterranean basin during the TRAQA (TRansport and Air QuAlity) airborne campaign in summer 2012. Cases of pollution export from different source regions around the basin and at different altitudes between ∼ 160 and 3500 m above sea level were sampled during the flights. Data from this study show a large variability of ω, with values between 0.84–0.98 at 370 nm and 0.70–0.99 at 950 nm. The single scattering albedo generally decreases with the wavelength, with some exception associated to the mixing of pollution with sea spray or dust particles over the sea surface. The lowest values of ω (0.84–0.70 between 370 and 950 nm) are measured in correspondence of a fresh plume possibly linked to ship emissions over the basin. The range of variability of ω observed in this study seems to be independent of the source region around the basin, as well as of the altitude and aging time of the plumes. The observed variability of ω reflects in a large variability for the complex refractive index of pollution aerosols, which is estimated to span in the large range 1.41–1.77 and 0.002–0.097 for the real and the imaginary parts, respectively, between 370 and 950 nm. Radiative calculations in clear-sky conditions were performed with the GAME radiative transfer model to test the sensitivity of the aerosol shortwave Direct Radiative Effect (DRE) to the variability of ω as observed in this study. Results from the calculations suggest up to a 50 and 30 % change of the forcing efficiency (FE), i.e. the DRE per unit of optical depth, at the surface (−160/−235 W m−2 τ−1 at 60° solar zenith angle) and at the Top-Of-Atmosphere (−137/−92 W m−2 τ−1) for ω varying between its maximum and minimum value. This induces a change of up to an order of magnitude (+23/+143 W m−2 τ−1) for the radiative effect within the atmosphere.

We conduct analyses to assess how characteristics of observations of ozone and its precursors affect air quality forecasting and research. To carry out this investigation, we use a photochemical box model and its adjoint integrated with a Lagrangian 4D-variational data assimilation system. Using this framework in conjunction with pseudo-observations, we perform an ozone precursor source inversion and estimate surface emissions. We then assess the resulting improvement in ozone air quality prediction. We use an analytical model to conduct uncertainty analyses. Using this analytical tool, we address some key questions regarding how the characteristics of observations affect ozone precursor emission inversion and in turn ozone prediction. These questions include what the effect is of choosing which species to observe, of varying amounts of observation noise, of changing the observing frequency and the observation time during the diurnal cycle, and of how these different scenarios interact with different photochemical regimes. In our investigation we use three observed species scenarios: CO and NO2; ozone, CO, and NO2; and HCHO, CO and NO2. The photochemical model was set up to simulate a range of summertime polluted environments spanning NOx-(NO and NO2)-limited to volatile organic compound (VOC)-limited conditions. We find that as the photochemical regime changes, here is a variation in the relative importance of trace gas observations to be able to constrain emission estimates and to improve the subsequent ozone forecasts. For example, adding ozone observations to an NO2 and CO observing system is found to decrease ozone prediction error under NOx- and VOC-limited regimes, and complementing the NO2 and CO system with HCHO observations would improve ozone prediction in the transitional regime and under VOC-limited conditions. We found that scenarios observing ozone and HCHO with a relative observing noise of lower than 33 % were able to achieve ozone prediction errors of lower than 5 ppbv (parts per billion by volume). Further, only observing intervals of 3 h or shorter were able to consistently achieve ozone prediction errors of 5 ppbv or lower across all photochemical regimes. Making observations closer to the prediction period and either in the morning or afternoon rush hour periods made greater improvements for ozone prediction: 0.2–0.3 ppbv for the morning rush hour and from 0.3 to 0.8 ppbv for the afternoon compared to only 0–0.1 ppbv for other times of the day. Finally, we made two complementary analyses that show that our conclusions are insensitive to the assumed diurnal emission cycle and to the choice of which VOC species emission to estimate using our framework. These questions will address how different types of observing platform, e.g. geostationary satellites or ground monitoring networks, could support future air quality research and forecasting.

In this study we present airborne observations of aerosol and trace gases obtained over the sea in the western Mediterranean basin during the TRAQA (TRansport and Air QuAlity) and SAFMED (Secondary Aerosol Formation in the MEDiterranean) campaigns in summer 2012 and 2013. A total of 23 vertical profiles were measured up to 5000 m above sea level over an extended area (40–45° N and 2° W–12° E) including the Gulf of Genoa, southern France, the Gulf of Lion, and the Spanish coast. During TRAQA and SAFMED the study area experienced a wide range of meteorological conditions which favoured pollution export from different sources located around the basin. Also, several events of dust outflows were measured during the campaigns. Observations from the present study show that continental pollution largely affects the western Mediterranean both close to coastal regions and in the open sea as far as ~ 250 km from the coastline. The measured aerosol scattering coefficient varies between ~ 20 and 120 Mm−1, while carbon monoxide (CO) and ozone (O3) mixing ratios are in the range of 60–165 and 30–85 ppbv, respectively. Pollution reaches 3000–4000 m in altitude and presents a very complex and highly stratified structure characterized by fresh and aged layers both in the boundary layer and in the free troposphere. Within pollution plumes the measured particle concentration in the Aitken (0.004–0.1 μm) and accumulation (0.1–1.0 μm) modes is between ~ 30 and 5000–6000 scm−3 (standard cm−3), which is comparable to the aerosol concentration measured in continental areas under pollution conditions. Additionally, our measurements indicate the presence of highly concentrated Aitken layers (10 000–15 000 scm−3) observed both close to the surface and in the free troposphere, possibly linked to the influence of new particle formation (NPF) episodes over the basin.

Validation results from a comparison between Measurement Of Pollution In The Troposphere (MOPITT) V5 Near InfraRed (NIR) carbon monoxide (CO) total column measurements and Measurement of Ozone and Water Vapour on Airbus in-service Aircraft (MOZAIC)/In-Service Aircraft for a Global Observing System (IAGOS) aircraft measurements are presented. A good agreement is found between MOPITT and MOZAIC/IAGOS measurements, consistent with results from earlier studies using different validation data and despite large variability in MOPITT CO total columns along the spatial footprint of the MOZAIC/IAGOS measurements. Validation results improve when taking the large spatial footprint of the MOZAIC/IAGOS data into account. No statistically significant drift was detected in the validation results over the period 2002–2010 at global, continental and local (airport) scales. Furthermore, for those situations where MOZAIC/IAGOS measurements differed from the MOPITT a priori, the MOPITT measurements clearly outperformed the MOPITT a priori data, indicating that MOPITT NIR retrievals add value to the MOPITT a priori. Results from a high spatial resolution simulation of the chemistry-transport model MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle) showed that the most likely explanation for the large MOPITT variability along the MOZAIC-IAGOS profile flight path is related to spatio-temporal CO variability, which should be kept in mind when using MOZAIC/IAGOS profile measurements for validating satellite nadir observations.

The space and time variabilities of methane (CH4) total column and upper tropospheric mixing ratios are analysed above the Mediterranean Basin (MB) as part of the Chemical and Aerosol Mediterranean Experiment (ChArMEx) programme. Since the analysis of the mid-to-upper tropospheric CH4 distribution from spaceborne sensors and model outputs is challenging, we have adopted a climatological approach and have used a wide variety of data sets. We have combined spaceborne measurements from the Thermal And Near infrared Sensor for carbon Observations – Fourier Transform Spectrometer (TANSO-FTS) instrument on the Greenhouse gases Observing SATellite (GOSAT) satellite, the Atmospheric InfraRed Spectrometer (AIRS) on the AURA platform and the Infrared Atmospheric Sounder Interferometer (IASI) instrument aboard the MetOp-A platform with model results from the Chemical Transport Model (CTM) MOCAGE, and the Chemical Climate Models (CCMs) CNRM-AOCCM and LMDz-OR-INCA (according to different emission scenarios). In order to minimize systematic errors in the spaceborne measurements, we have only considered maritime pixels over the MB. The period of interest spans from 2008 to 2011 considering satellite and MOCAGE data and, regarding the CCMs, from 2001 to 2010. Although CH4 is a long-lived tracer with lifetime of ~12 years and is supposed to be well mixed in the troposphere, an east–west gradient in CH4 is observed and modelled in the mid-to-upper troposphere with a maximum in the Western MB in all seasons except in summer when CH4 accumulates above the Eastern MB. The peak-to-peak amplitude of the east–west seasonal variation in CH4 above the MB in the upper troposphere (300 hPa) is weak but almost twice as great in the satellite measurements (~25 ppbv) as in the model data (~15 ppbv). The maximum of CH4 in summer above the eastern MB can be explained by a series of dynamical processes only occurring in summer. The Asian monsoon traps and uplifts high amounts of CH4 to the upper troposphere where they build up. The Asian Monsoon Anticyclone redistributes these elevated CH4 amounts towards North Africa and the Middle East to finally reach and descend in the eastern MB. In the lower troposphere, the CH4 variability is mainly driven by the local sources of emission in the vicinity of the MB.

This paper presents a validation of a method to derive the vertical profile of carbon monoxide (CO) from its total column using data assimilation. We choose version 3 of MOPITT CO total columns to validate the proposed method. MOPITT products have the advantage of providing both the vertical profiles and the total columns of CO. Furthermore, this version has been extensively validated by comparison with many independent data sets, and has been used in many scientific studies. The first step of the paper consists in the specification of the observation errors based on the chi-square (χ2) test. The observations have been binned according to three types: over land during daytime, over land during night-time, and over sea. Their respective errors using the χ2 metric have been found to be 8, 11 and 7%. In the second step, the CO total columns, with their specified errors, are used within the assimilation system to estimate the vertical profiles. These are compared to the retrieved profiles of MOPITT V3 at global and regional scales. Generally, the two data sets show similar patterns and good agreement at both scales. Nevertheless, total column analyses slightly overestimate CO concentrations compared to MOPITT observations. The mean bias between both data sets is +15 and +12% at 700 and 250 hPa, respectively. In the third step, the assimilation of total column has been compared to the assimilation of MOPITT vertical profiles. The differences between both analyses are very small. In terms longitude–latitude maps, the mean bias between the two data sets is +6 and +8% at the pressure levels 700 and 200 hPa, respectively. In terms of zonal means, the CO distribution is similar for both analyses, with a mean bias which does not exceed 12%. Finally, the two analyses have been validated using independent observations from the aircraft-based MOZAIC program in terms of vertical profiles over eight airports. Over most airports, both analyses agree well with aircraft profiles. For more than 50% of recorded measurements, the difference between the analyses and MOZAIC does not exceed 5 ppbv (parts per billion by volume).

Ozone is a tropospheric pollutant and plays a key role in determining the air quality that affects human wellbeing. In this study, we compare the capability of two hypothetical grating spectrometers onboard a geostationary (GEO) satellite to sense ozone in the lowermost troposphere (surface and the 0–1 km column). We consider 1 week during the Northern Hemisphere summer simulated by a chemical transport model, and use the two GEO instrument configurations to measure ozone concentration (1) in the thermal infrared (GEO TIR) and (2) in the thermal infrared and the visible (GEO TIR+VIS). These configurations are compared against each other, and also against an ozone reference state and a priori ozone information. In a first approximation, we assume clear sky conditions neglecting the influence of aerosols and clouds. A number of statistical tests are used to assess the performance of the two GEO configurations. We consider land and sea pixels and whether differences between the two in the performance are significant. Results show that the GEO TIR+VIS configuration provides a better representation of the ozone field both for surface ozone and the 0–1 km ozone column during the daytime especially over land.

The tropical deep overshooting convection is known to be most intense above continental areas such as South America, Africa, and the maritime continent. However, its impact on the tropical tropopause layer (TTL) at global scale remains debated. In our analysis, we use the 8-year Microwave Limb Sounder (MLS) water vapour (H2O), cloud ice-water content (IWC), and temperature data sets from 2005 to date, to highlight the interplays between these parameters and their role in the water vapour variability in the TTL, and separately in the northern and southern tropics. In the tropical upper troposphere (177 hPa), continents, including the maritime continent, present the night-time (01:30 local time, LT) peak in the water vapour mixing ratio characteristic of the H2O diurnal cycle above tropical land. The western Pacific region, governed by the tropical oceanic diurnal cycle, has a daytime maximum (13:30 LT). In the TTL (100 hPa) and tropical lower stratosphere (56 hPa), South America and Africa differ from the maritime continent and western Pacific displaying a daytime maximum of H2O. In addition, the relative amplitude between day and night is found to be systematically higher by 5–10% in the southern tropical upper troposphere and 1–3% in the TTL than in the northern tropics during their respective summer, indicative of a larger impact of the convection on H2O in the southern tropics. Using a regional-scale approach, we investigate how mechanisms linked to the H2O variability differ in function of the geography. In summary, the MLS water vapour and cloud ice-water observations demonstrate a clear contribution to the TTL moistening by ice crystals overshooting over tropical land regions. The process is found to be much more effective in the southern tropics. Deep convection is responsible for the diurnal temperature variability in the same geographical areas in the lowermost stratosphere, which in turn drives the variability of H2O.

This study tests a novel methodology to add value to satellite data sets. This methodology, data fusion, is similar to data assimilation, except that the background model-based field is replaced by a satellite data set, in this case AIRS (Atmospheric Infrared Sounder) carbon monoxide (CO) measurements. The observational information comes from CO measurements with lower spatial coverage than AIRS, namely, from TES (Tropospheric Emission Spectrometer) and MLS (Microwave Limb Sounder). We show that combining these data sets with data fusion uses the higher spectral resolution of TES to extend AIRS CO observational sensitivity to the lower troposphere, a region especially important for air quality studies. We also show that combined CO measurements from AIRS and MLS provide enhanced information in the UTLS (upper troposphere/lower stratosphere) region compared to each product individually. The combined AIRS–TES and AIRS–MLS CO products are validated against DACOM (differential absorption mid-IR diode laser spectrometer) in situ CO measurements from the INTEX-B (Intercontinental Chemical Transport Experiment: MILAGRO and Pacific phases) field campaign and in situ data from HIPPO (HIAPER Pole-to-Pole Observations) flights. The data fusion results show improved sensitivities in the lower and upper troposphere (20–30% and above 20%, respectively) as compared with AIRS-only version 5 CO retrievals, and improved daily coverage compared with TES and MLS CO data.

We study the carbon monoxide (CO) variability in the last decade measured by NASA's Atmospheric InfraRed Sounder (AIRS) on the Earth Observing System (EOS)/Aqua satellite. The focus of this study is to analyze CO variability and short-term trends separately for background CO and fresh CO emissions based on a new statistical approach. The AIRS Level 2 (L2) retrieval algorithm utilizes cloud clearing to treat cloud contaminations in the signals, and this increases the data coverage significantly to a yield of more than 50% of the total measurements. We first study if the cloud clearing affects CO retrievals and the subsequent trend studies by using the collocated Moderate Resolution Imaging Spectroradiometer (MODIS) cloud mask to identify AIRS clear sky scenes. We then carry out a science analysis using AIRS CO data individually for the clear and cloud-cleared scenes to identify any potential effects due to cloud clearing. We also introduce a new technique to separate background and recently emitted CO observations, which aims to constrain emissions using only satellite CO data. We validate the CO variability of the recent emissions estimated from AIRS against other emission inventory databases (i.e., Global Fire Emissions Database – GFED3 and the MACC/CityZEN UE – MACCity) and calculate that the correlation coefficients between the AIRS CO recently emitted and the emission inventory databases are 0.726 for the Northern Hemisphere (NH) and 0.915 for the Southern Hemisphere (SH). The high degree of agreement between emissions identified using only AIRS CO and independent inventory sources demonstrates the validity of this approach to separate recent emissions from the background CO using one satellite data set.

The behavior of the extratropical transition layer (ExTL) is investigated using a chemistry transport model (CTM) and analyses derived from assimilation of MLS (Microwave Limb Sounder) O3 and MOPITT (Measurements Of Pollution In The Troposphere) CO data. We firstly focus on a stratosphere–troposphere exchange (STE) case study that occurred on 15 August 2007 over the British Isles (50° N, 10° W). We evaluate the effect of data assimilation on the O3–CO correlations. It is shown that data assimilation disrupts the relationship in the transition region. When MLS O3 is assimilated, CO and O3 values are not consistent between each other, leading to unphysical correlations at the STE location. When MLS O3 and MOPITT CO assimilated fields are taken into account in the diagnostics the relationship happens to be more physical. We then use O3–CO correlations to quantify the effect of data assimilation on the height and depth of the ExTL. When the free-model run O3 and CO fields are used in the diagnostics, the ExTL distribution is found 1.1 km above the thermal tropopause and is 2.6 km wide (2σ). MOPITT CO analyses only slightly sharpen (by −0.02 km) and lower (by −0.2 km) the ExTL distribution. MLS O3 analyses provide an expansion (by +0.9 km) of the ExTL distribution, suggesting a more intense O3 mixing. However, the MLS O3 analyses ExTL distribution shows a maximum close to the thermal tropopause and a mean location closer to the thermal tropopause (+0.45 km). When MLS O3 and MOPITT CO analyses are used together, the ExTL shows a mean location that is the closest to the thermal tropopause (+0.16 km). We also extend the study at the global scale on 15 August 2007 and for the month of August 2007. MOPITT CO analyses still show a narrower chemical transition between stratosphere and troposphere than the free-model run. MLS O3 analyses move the ExTL toward the troposphere and broaden it. When MLS O3 analyses and MOPITT CO analyses are used together, the ExTL matches the thermal tropopause poleward of 50°.

The SPIRALE and SWIR balloon-borne instruments were launched in the Arctic polar region (near Kiruna, Sweden, 67.9° N–21.1° E) during summer on 7 and 24 August 2009 and on 14 August 2009, respectively. The SPIRALE instrument performed in situ measurements of several trace gases including CO and O3 at altitudes between 9 and 34 km, with very high vertical resolution (∼ 5 m). The SWIR-balloon instrument measured total and partial column of several species including CO. The CO stratospheric profile from SPIRALE for 7 August 2009 shows some specific structures with large concentrations in the low levels (potential temperatures between 320 and 380 K, i.e. 10–14 km height). These structures are not present in the CO vertical profile of SPIRALE for 24 August 2009, for which the volume mixing ratios are typical from polar latitudes (∼ 30 ppb). CO total columns retrieved from the IASI-MetOp satellite sounder for the three dates of flights are used to understand this CO variability. SPIRALE and SWIR CO partial columns between 9 and 34 km are compared, allowing us to confirm that the enhancement of CO is localised in the stratosphere. The measurements are also investigated in terms of CO:O3 correlations and using several modelling approaches (trajectory calculations, potential vorticity fields, results of chemistry transport model) in order to characterize the origin of the air masses sampled. The emission sources are qualified in terms of source type (fires, urban pollution) using NH3 and CO measurements from IASI-MetOp and fires detection from MODIS on board the TERRA/AQUA satellite. The results give strong evidence that the unusual abundance of CO on 7 August is due to surface pollution plumes from East Asia and North America transporting to the upper troposphere and then entering the lower stratosphere by isentropic advection. This study strengthens evidence that the composition of low polar stratosphere in summer may be affected by anthropogenic surface emissions through long-range transport.

We assimilate stratospheric ozone profiles from MLS (Microwave Limb Sounder) into the MOCAGE Chemistry Transport Model (CTM) to study Stratosphere-Troposphere Exchange (STE). This study uses two horizontal grid resolutions of 2° and 0.2°. The combined impacts of MLS ozone assimilation and high horizontal resolution are illustrated in two case studies where STE events occurred (23 June 2009 and 17 July 2009). At high resolution the filamentary structures of stratospheric air which characterise STE events are captured by the model. To test the impact of the assimilation and the resolution, we compare model outputs from different experiments (high resolution and low resolution; MLS assimilation run and free run) with independent data (MOZAIC aircraft ozone data; WOUDC ozone sonde network data). MLS ozone analyses show a better description of the Upper Troposphere Lower Stratosphere (UTLS) region and the stratospheric intrusions than the free model run. In particular, at high horizontal resolution the MLS ozone analyses present realistic filamentary ozone structures in the UTLS and laminae structures in the ozone profile. Despite a low aspect ratio between horizontal resolution and vertical resolution in the UTLS at high horizontal resolution, MLS ozone analyses improve the vertical structures of the ozone fields. Results from backward trajectories and ozone forecasts show that assimilation at high horizontal resolution of MLS ozone profiles between 10 hPa and 215 hPa has an impact on tropospheric ozone.

This paper presents observing system simulation experiments (OSSEs) to compare the relative capabilities of two geostationary thermal infrared (TIR) instruments to measure ozone (O3) and carbon monoxide (CO) for monitoring air quality (AQ) over Europe. The primary motivation of this study is to use OSSEs to assess how these infrared instruments can constrain different errors affecting AQ hindcasts and forecasts (emissions, meteorology, initial condition and the 3 parameters together). The first instrument (GEO-TIR) has a configuration optimized to monitor O3 and CO in the lowermost troposphere (LmT; defined to be the atmosphere between the surface and 3 km), and the second instrument (GEO-TIR2) is designed to monitor temperature and humidity. Both instruments measure radiances in the same spectral TIR band. Results show that GEO-TIR could have a significant impact (GEO-TIR is closer to the reference atmosphere than GEO-TIR2) on the analyses of O3 and CO LmT column. The information added by the measurements for both instruments is mainly over the Mediterranean Basin and some impact can be found over the Atlantic Ocean and Northern Europe. The impact of GEO-TIR is mainly above 1 km for O3 and CO but can also improve the surface analyses for CO. The analyses of GEO-TIR2 show low impact for O3 LmT column but a significant impact (although still lower than for GEO-TIR) for CO above 1 km. The results of this study indicate the beneficial impact from an infrared instrument (GEO-TIR) with a capability for monitoring O3 and CO concentrations in the LmT, and quantify the value of this information for constraining AQ models.

This paper describes the capabilities of a nadir thermal infrared (TIR) sensor proposed for deployment onboard a geostationary platform to monitor ozone (O3) and carbon monoxide (CO) for air quality (AQ) purposes. To assess the capabilities of this sensor we perform idealized retrieval studies considering typical atmospheric profiles of O3 and CO over Europe with different instrument configuration (signal to noise ratio, SNR, and spectral sampling interval, SSI) using the KOPRA forward model and the KOPRA-fit retrieval scheme. We then select a configuration, referred to as GEO-TIR, optimized for providing information in the lowermost troposphere (LmT; 0–3 km in height). For the GEO-TIR configuration we obtain ~1.5 degrees of freedom for O3 and ~2 for CO at altitudes between 0 and 15 km. The error budget of GEO-TIR, calculated using the principal contributions to the error (namely, temperature, measurement error, smoothing error) shows that information in the LmT can be achieved by GEO-TIR. We also retrieve analogous profiles from another geostationary infrared instrument with SNR and SSI similar to the Meteosat Third Generation Infrared Sounder (MTG-IRS) which is dedicated to numerical weather prediction, referred to as GEO-TIR2. We quantify the added value of GEO-TIR over GEO-TIR2 for a realistic atmosphere, simulated using the chemistry transport model MOCAGE (MOdèle de Chimie Atmospherique à Grande Echelle). Results show that GEO-TIR is able to capture well the spatial and temporal variability in the LmT for both O3 and CO. These results also provide evidence of the significant added value in the LmT of GEO-TIR compared to GEO-TIR2 by showing GEO-TIR is closer to MOCAGE than GEO-TIR2 for various statistical parameters (correlation, bias, standard deviation).

During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA) project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons) and points to some of the important findings discussed in more detail in other papers in this special issue. The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow. Mineral dust was found to be the most abundant and ubiquitous aerosol type in the atmosphere over Western Africa. Data collected within AMMA indicate that injection of dust to altitudes favourable for long-range transport (i.e. in the upper Sahelian planetary boundary layer) can occur behind the leading edge of mesoscale convective system (MCS) cold-pools. Research within AMMA also provides the first estimates of secondary organic aerosols across the West African Sahel and have shown that organic mass loadings vary between 0 and 2 μg m−3 with a median concentration of 1.07 μg m−3. The vertical distribution of nucleation mode particle concentrations reveals that significant and fairly strong particle formation events did occur for a considerable fraction of measurement time above 8 km (and only there). Very low concentrations were observed in general in the fresh outflow of active MCSs, likely as the result of efficient wet removal of aerosol particles due to heavy precipitation inside the convective cells of the MCSs. This wet removal initially affects all particle size ranges as clearly shown by all measurements in the vicinity of MCSs.

This paper presents an evaluation of a new linear parameterization valid for the troposphere and the stratosphere, based on a first order approximation of the carbon monoxide (CO) continuity equation. This linear scheme (hereinafter noted LINCO) has been implemented in the 3-D Chemical Transport Model (CTM) MOCAGE (MOdèle de Chimie Atmospherique Grande Echelle). First, a one and a half years of LINCO simulation has been compared to output obtained from a detailed chemical scheme output. The mean differences between both schemes are about ±25 ppbv (part per billion by volume) or 15% in the troposphere and ±10 ppbv or 100% in the stratosphere. Second, LINCO has been compared to diverse observations from satellite instruments covering the troposphere (Measurements Of Pollution In The Troposphere: MOPITT) and the stratosphere (Microwave Limb Sounder: MLS) and also from aircraft (Measurements of ozone and water vapour by Airbus in-service aircraft: MOZAIC programme) mostly flying in the upper troposphere and lower stratosphere (UTLS). In the troposphere, the LINCO seasonal variations as well as the vertical and horizontal distributions are quite close to MOPITT CO observations. However, a bias of ~−40 ppbv is observed at 700 Pa between LINCO and MOPITT. In the stratosphere, MLS and LINCO present similar large-scale patterns, except over the poles where the CO concentration is underestimated by the model. In the UTLS, LINCO presents small biases less than 2% compared to independent MOZAIC profiles. Third, we assimilated MOPITT CO using a variational 3D-FGAT (First Guess at Appropriate Time) method in conjunction with MOCAGE for a long run of one and a half years. The data assimilation greatly improves the vertical CO distribution in the troposphere from 700 to 350 hPa compared to independent MOZAIC profiles. At 146 hPa, the assimilated CO distribution is also improved compared to MLS observations by reducing the bias up to a factor of 2 in the tropics. This study confirms that the linear scheme is able to simulate reasonably well the CO distribution in the troposphere and in the lower stratosphere. Therefore, the low computing cost of the linear scheme opens new perspectives to make free runs and CO data assimilation runs at high resolution and over periods of several years.

This paper presents a comprehensive characterization of a very deep stratospheric intrusion which occurred over the British Isles on 15 August 2007. The signature of this event is diagnosed using ozonesonde measurements over Lerwick, UK (60.14° N, 1.19° W) and is also well characterized using meteorological analyses from the global operational weather prediction model of Météo-France, ARPEGE. Modelled as well as assimilated fields of both ozone (O3) and carbon monoxide (CO) have been used in order to better document this event. O3 and CO from Aura/MLS and Terra/MOPITT instruments, respectively, are assimilated into the three-dimensional chemical transport model MOCAGE of Météo-France using a variational 3-D-FGAT (First Guess at Appropriate Time) method. The validation of O3 and CO assimilated fields is done using self-consistency diagnostics and by comparison with independent observations such as MOZAIC (O3 and CO), AIRS (CO) and OMI (O3). It particularly shows in the upper troposphere and lower stratosphere region that the assimilated fields are closer to MOZAIC than the free model run. The O3 bias between MOZAIC and the analyses is −11.5 ppbv with a RMS of 22.4 ppbv and a correlation coefficient of 0.93, whereas between MOZAIC and the free model run, the corresponding values are 33 ppbv, 38.5 ppbv and 0.83, respectively. In the same way, for CO, the bias, RMS and correlation coefficient between MOZAIC and the analyses are −3.16 ppbv, 13 ppbv and 0.79, respectively, whereas between MOZAIC and the free model they are 6.3 ppbv, 16.6 ppbv and 0.71, respectively. The paper also presents a demonstration of the capability of O3 and CO assimilated fields to better describe a stratosphere-troposphere exchange (STE) event in comparison with the free run modelled O3 and CO fields. Although the assimilation of MLS data improves the distribution of O3 above the tropopause compared to the free model run, it is not sufficient to reproduce the STE event well. Assimilated MOPITT CO allows a better qualitative description of the stratospheric intrusion event. The MOPITT CO analyses appear more promising than the MLS O3 analyses in terms of their ability to capture a deep STE event. Therefore, the results of this study open the perspectives for using MOPITT CO in the STE studies.

The mechanisms of transport on annual, semi-annual and quasi-biennial time scales in the equatorial (10° S–10° N) stratosphere are investigated using the nitrous oxide (N2O) measurements of the space-borne ODIN Sub-Millimetre Radiometer from November 2001 to June 2005, and the simulations of the three-dimensional chemical transport models MOCAGE and SLIMCAT. Both models are forced with analyses from the European Centre for Medium-range Weather Forecast, but the vertical transport is derived either from the forcing analyses by solving the continuity equation (MOCAGE), or from diabatic heating rates using a radiation scheme (SLIMCAT). The N2O variations in the mid-to-upper stratosphere at levels above 32 hPa are generally well captured by the models though significant differences appear with the observations as well as between the models, attributed to the difficulty of capturing correctly the slow upwelling associated with the Brewer-Dobson circulation. However, in the lower stratosphere, below 32 hPa, the observed variations are shown to be mainly seasonal with peak amplitude at 400–450 K (~17.5–19 km), totally missed by the models. The minimum N2O in June, out of phase by two months with the known minimum seasonal upwelling associated with the Brewer-Dobson circulation and moreover amplified over the Western Pacific compared to Africa is incompatible with the seasonal change of upwelling evoked to explain the O3 annual cycle in the same altitude range (Randel et al., 2007). Unless the 1.5 ppbv amplitude of N2O annual cycle in the upper troposphere is totally wrong, the explanation of the observed N2O annual cycle of 15 ppbv in the lower stratosphere requires another mechanism. A possible candidate for that might be the existence of a downward time-averaged mass flux above specific regions, as shown by Sherwood (2000) over Indonesia, required for compensating the energy sink resulting from the deep overshooting of cold and heavy air at high altitude over intense convective areas. But, since global models do currently not capture this subsidence, it must be recognised that a full explanation of the observations cannot be provided for the moment. However, the coincidence of the peak contrast between the Western Pacific and Africa with the maximum overshooting volume in May reported by the Tropical Rainfall Measuring Mission (TRMM) Precipitation Radar, suggests a strong influence of deep convection on the chemical composition of the tropical lower stratosphere up to 500 K (21 km).

In this paper we use the total columns of nitrous oxide (N2O) as retrieved from the radiance spectra as measured by the Infrared Atmospheric Sounding Interferometer (IASI) instrument aboard the MetOp-A platform and distributed by the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT) during the March–May (MAM) 2008 period. Since the total column of N2O reflects concentrations in the middle troposphere, cloud-free columnar N2O measurements are used to assess transport processes in the equatorial band (10° S–10° N). We compare the measured data set with the outputs produced by the 3-D chemical-transport model MOCAGE during the period MAM 2002–2004. To reflect MAM 2008 concentrations, MOCAGE results have been scaled by a factor 1.0125 in order to represent the change in concentration of N2O since 2004. IASI N2O equatorial measurements show a maximum over Africa (4.96×10−3 kg m−2) and a minimum over South America (4.86×10−3 kg m−2) in reasonable agreement with the outputs from MOCAGE despite the fact that emissions of N2O are more intense over America than over Africa. The amplitude of the longitudinal variation of total column N2O along the equatorial band is twice as intense in the measurements (~1.6%) than as in the model calculations (~0.8%), and much greater than the IASI mean random error (0.16–0.33%). A difference between the two data sets is observed above the Western Pacific (110° E–150° E) with a marked minimum in IASI compared to MOCAGE. Recent theoretical studies (Ricaud et al., 2007 and 2009) have shown the potentially important effect of the Walker and the Hadley cells on the tropospheric distribution of N2O in producing a local maximum in N2O above Africa. Based on equatorial total columns of N2O retrieved from IASI, our results are consistent with the fact that Africa is a zone of convergence of airmasses coming from different convective regions whilst Western Pacific behaves more like a divergence zone.

The transport pathways of carbon monoxide (CO) in the African Upper Troposphere (UT) during the West African Monsoon (WAM) is investigated through the assimilation of CO observations by the Aura Microwave Limb Sounder (MLS) in the MOCAGE Chemistry Transport Model (CTM). The assimilation setup, based on a 3-D First Guess at Assimilation Time (3-D-FGAT) variational method is described. Comparisons between the assimilated CO fields and in situ airborne observations from the MOZAIC program between Europe and both Southern Africa and Southeast Asia show an overall good agreement around the lowermost pressure level sampled by MLS (~215 hPa). The 4-D assimilated fields averaged over the month of July 2006 have been used to determine the main dynamical processes responsible for the transport of CO in the African UT. The studied period corresponds to the second AMMA (African Monsoon Multidisciplinary Analyses) aircraft campaign. At 220 hPa, the CO distribution is characterized by a latitudinal maximum around 5° N mostly driven by convective uplift of air masses impacted by biomass burning from Southern Africa, uplifted within the WAM region and vented predominantly southward by the upper branch of the winter hemisphere Hadley cell. Above 150 hPa, the African CO distribution is characterized by a broad maximum over northern Africa. This maximum is mostly controlled by the large scale UT circulation driven by the Asian Summer Monsoon (ASM) and characterized by the Asian Monsoon Anticyclone (AMA) centered at 30° N and the Tropical Easterly Jet (TEJ) on the southern flank of the anticyclone. Asian pollution uplifted to the UT over large region of Southeast Asia is trapped within the AMA and transported by the anticyclonic circulation over Northeast Africa. South of the AMA, the TEJ is responsible for the tranport of CO-enriched air masses from India and Southeast Asia over Africa. Using the high time resolution provided by the 4-D assimilated fields, we give evidence that the variability of the African CO distribution above 150 hPa and north of the WAM region is mainly driven by the synoptic dynamical variability of both the AMA and the TEJ.

The mechanism of troposphere-stratosphere exchange in the tropics was investigated from space-borne observations of the horizontal distributions of tropospheric-origin long-lived species, nitrous oxide (N2O), methane (CH4) and carbon monoxide (CO), from 150 to 70 hPa in March-April-May by the ODIN/Sub-Millimeter Radiometer (SMR), the Upper Atmosphere Research Satellite (UARS)/Halogen Occultation Experiment (HALOE) and the TERRA/Measurements Of Pollution In The Troposphere (MOPITT) instruments in 2002–2004, completed by recent observations of the AURA/Microwave Limb Sounder (MLS) instrument during the same season in 2005. The vertical resolution of the satellite measurements ranges from 2 to 4 km. The analysis has been performed on isentropic surfaces: 400 K (lower stratosphere) for all the species and 360 K (upper troposphere) only for CO. At 400 K (and 360 K for CO), all gases show significant longitudinal variations with peak-to-trough values of ~5–11 ppbv for N2O, 0.07–0.13 ppmv for CH4, and ~10 ppbv for CO (~40 ppbv at 360 K). The maximum amounts are primarily located over Africa and, depending on the species, secondary more or less pronounced maxima are reported above northern South America and South-East Asia. The lower stratosphere over the Western Pacific deep convective region where the outgoing longwave radiation is the lowest, the tropopause the highest and the coldest, appears as a region of minimum concentration of tropospheric trace species. The possible impact on trace gas concentration at the tropopause of the inhomogeneous distribution and intensity of the sources, mostly continental, of the horizontal and vertical transports in the troposphere, and of cross-tropopause transport was explored with the MOCAGE Chemistry Transport Model. In the simulations, significant longitudinal variations were found on the medium-lived CO (2-month lifetime) with peak-to-trough value of ~20 ppbv at 360 K and ~10 ppbv at 400 K, slightly weaker than observations. However, the CH4 (8–10 year lifetime) and N2O (130-year lifetime) longitudinal variations are significantly weaker than observed: peak-to-trough values of ~0.02 ppmv for CH4 and 1–2 ppbv for N2O at 400 K. The large longitudinal contrast of N2O and CH4 concentrations reported by the space-borne instruments at the tropopause and in the lower stratosphere not captured by the model thus requires another explanation. The suggestion is of strong overshooting over land convective regions, particularly Africa, very consistent with the space-borne Tropical Rainfall Measuring Mission (TRMM) radar maximum overshooting features over the same region during the same season. Compared to observations, the MOCAGE model forced by ECMWF analyses is found to ignore these fast local uplifts, but to overestimate the average uniform vertical transport in the UTLS at all longitudes in the tropics.

We present the configuration of the Météo-France Chemistry and Transport Model (CTM) MOCAGE-Climat that will be dedicated to the study of chemistry and climate interactions. MOCAGE-Climat is a state-of-the-art CTM that simulates the global distribution of ozone and its precursors (82 chemical species) both in the troposphere and the stratosphere, up to the mid-mesosphere (~70 km). Surface processes (emissions, dry deposition), convection, and scavenging are explicitly described in the model that has been driven by the ECMWF operational analyses of the period 2000–2005, on T21 and T42 horizontal grids and 60 hybrid vertical levels, with and without a procedure that reduces calculations in the boundary layer, and with on-line or climatological deposition velocities. Model outputs have been compared to available observations, both from satellites (TOMS, HALOE, SMR, SCIAMACHY, MOPITT) and in-situ instrument measurements (ozone sondes, MOZAIC and aircraft campaigns) at climatological timescales. The distribution of long-lived species is in fair agreement with observations in the stratosphere putting aside the shortcomings associated with the large-scale circulation. The variability of the ozone column, both spatially and temporarily, is satisfactory. However, because the Brewer-Dobson circulation is too fast, too much ozone is accumulated in the lower to mid-stratosphere at the end of winter. Ozone in the UTLS region does not show any systematic bias. In the troposphere better agreement with ozone sonde measurements is obtained at mid and high latitudes than in the tropics and differences with observations are the lowest in summer. Simulations using a simplified boundary layer lead to larger ozone differences between the model and the observations up to the mid-troposphere. NOx in the lowest troposphere is in general overestimated, especially in the winter months over the Northern Hemisphere, which may result from a positive bias in OH. Dry deposition fluxes of O3 and nitrogen species are within the range of values reported by recent inter-comparison model exercises. The use of climatological deposition velocities versus deposition velocities calculated on-line had greatest impact on HNO3 and NO2 in the troposphere.

This paper reports on the transport of ozone (O3) and related species over the North Atlantic ocean and its impact on Europe. Measurements of nitrogen dioxide (NO2) and carbon monoxide (CO) columns from the GOME and MOPITT satellite instruments, respectively, are used in conjunction with the GEOS-CHEM global model of transport and tropospheric chemistry to identify the major events of long range transport that reach Europe over the course of summer 2000. Sensitivity model simulations are used to analyse observed O3 distributions with respect to the impact of long range transport events. For that purpose, we used in-situ O3 observations taken at the mountain site of Jungfraujoch as well as O3 vertical profiles taken in the vicinity of central European cities. Over the course of summer 2000, we identified 9 major episodes of transatlantic pollution transport; 7 events are associated with transient cyclones while 2 events occur through zonal transport (e.g. by advection in the strong low-level westerly winds established in summer between the Azores anticyclone and transient cyclones). We find that on average three episodes occur per month with the strongest ones being in June. The number and frequency of long range transport events that reach Europe are driven by the position and strength of the Azores anticyclone. Model sensitivity simulations indicate that the summer mean North American O3 contribution ranges from 3 to 5 ppb (7–11%) in the planetary boundary layer and 10 to 13 ppb (18–23%) in the middle and upper troposphere. During particular episodes, North American sources can result in O3 enhancements up to 25–28 ppb in the layer between 800–600 hPa and 10–12 ppb in the boundary layer. The impact of the zonal transport events on O3 distribution over Europe is more clearly seen below 700 hPa as they tend to transport pollution at lower levels while the events associated with transient cyclones are more likely to have an impact on the middle and upper troposphere (i.e. above 600 hPa). The air mass origins found in the GEOS-CHEM model are clearly confirmed by back trajectory analyses. During most of the 9 events, a strong contribution in North American O3 is in general associated with only little European O3 and vice-versa (in particular at the Jungfraujoch). A substantial North American contribution (e.g., 30% or higher) to O3 over Europe does not always result in pronounced O3 enhancements in the observations during our period of study.

The Lagrangian particle dispersion model FLEXPART coupled with daily active fire products provided by the MODIS instrument was used to forecast the intrusions of the southern hemispheric fire plumes in the Northern Hemisphere during the AMMA (African Monsoon Multidisciplinary Analysis) fourth airborne campaign from 25 July to 31 August 2006 (Special Operation Period SOP2_a2). The imprint of the biomass burning plumes over the Gulf of Guinea showed a well marked intraseasonal variability which is controlled by the position and strength of the southern hemispheric African Easterly Jet (AEJ-S). Three different periods were identified which correspond to active and break phases of the AEJ-S: 25 July–2 August (active phase), 3 August–8 August (break phase) and 9 August–31 August (active phase). During the AEJ-S active phases, the advection of the biomass burning plumes out over the Atlantic ocean was efficient in the mid-troposphere. During the AEJ-S break phases, pollutants emitted by fires were trapped over the continent where they accumulated. The continental circulation increased the possibility for the biomass burning plumes to reach the convective regions located further north. As a consequence, biomass burning plumes were found in the upper troposphere over the Gulf of Guinea during the AEJ-S break phase. Observational evidences from the ozonesounding network at Cotonou and the carbon monoxide measured by MOPITT confirmed the alternation of the AEJ-S phases with low ozone and CO in the mid-troposphere over the Gulf of Guinea during the break phase.

This study presents an experimental analysis from aircraft measurements above the Pyrenees chain during the PYREX experiment. The Pyrenees chain, roughly WE oriented, is a major barrier for northerly and southerly airflows. We present a case of southerly flow (15 October 1990) and three successive cases of northerly flows above the Pyrenees (14, 15 and 16 November 1990) documented by two aircraft. The aircraft have described a vertical cross section perpendicular to the Pyrenean ridge. This area is described via the thermodynamical and dynamical fields which have a horizontal resolution of 10 km. Three methods for computing the vertical velocity of the air are presented. The horizontal advection terms which play a role in the budget equations are also evaluated. The altitude turbulence zone of 15 October are shown via turbulent fluxes, turbulent kinetic energy (TKE), dissipation rate of TKE and inertial length-scale. A comparison of results obtained by eddy-correlation and inertial-dissipation method is presented. The experimental results show a warm and dry downdraft for the southerly flow with large values for advection terms. All the mountain wave cases are also shown to present an important dynamical perturbation just above the Pyrenees at upper altitudes.