L'assimilation de données permet de combiner d'une manière optimale un modèle numérique décrivant l'évolution de la composition chimique de l'atmosphère et les mesures disponibles. Dans cette thèse, l'assimilation de données est utilisée afin de caractériser les distributions troposphériques et stratosphériques de l'ozone (O3) et du monoxyde de carbone (CO). Le Modèle de Chimie Transport (CTM) MOCAGE (MOdèle de Chimie Atmosphérique à Grande échelle) est utilisé dans une configuration à deux domaines imbriqués avec les résolutions de 2◦ (global) et de 0.2◦ (régional). La technique variationnelle du 3D-FGAT est utilisée pour toutes les études que constituent cette thèse. Nous avons évalué la complémentarité des mesures satellites au limbe et au nadir aujourd'hui disponibles pour la caractérisation de l'UTLS (Haute Troposphère Basse Stratosphère) en assimilant ces deux types de mesures simultanément. Nous nous sommes en particulier intéressé à la propagation de l'information provenant des mesures assimilés dans le modèle et plus particulièrement, aux impacts de l'assimilation de mesures stratosphérique d'ozone en troposphère aux moyennes latitudes. Les principaux objectifs de cette thèse ont été de montrer la valeur ajoutée de l'augmentation de la résolution modèle pour l'assimilation de données et les effets synergiques de l'assimilation combinée d'un sondeur au limbe et au nadir. Des développements au niveau du système d'assimilation en domaine imbriqué à 0.2◦ ont été effectués. L'assimilation des données dans le domaine global est maintenant prise en compte et les conditions aux bords provenant des champs assimilés montre un impact significatif sur le domaine imbriqué. Dans un premier temps, nous avons assimilé les profils d'ozone stratosphériques mesurés au limbe provenant de MLS (Microwave Limb Sounder) afin d'étudier deux cas d'échange entre la Stratosphère et la Troposphère (STE). / Data assimilation combines in an optimal way a numerical model describing the evolution of the atmospheric chemical composition and the available trace gases measurements. In this thesis, data assimilation is used to characterize the ozone (O3) and the carbon monoxide (CO) distributions in the stratosphere and in the troposphere. The Chemistry Transport Model (CTM) MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle) is used in a configuration with two nested domains at 2◦ (global) and at 0.2◦ (regional). To perform the assimilation experiments a 3D-FGAT variational method is used. We evaluate the complementarity of limb and nadir measurements available at the present day at characterizing the UTLS (Upper Troposphere Lower Stratosphere) region by assimilating simultaneously the two type of measurements. We particularly focus on the impacts of data assimilation of stratospheric ozone measurements on troposphere and conversely of tropospheric data assimilation on stratosphere. Showing the added value of the increased horizontal resolution in the UTLS assimilated fields and the synergistic effects of limb and nadir assimilation were the main objectives of this work. Development in the assimilation system have been made in the assimilation system with the nested domain. Data assimilation in the global domain is now taken in account and the boundary condition from the assimilated fields show significant impacts on the regional domain. Firstly, we assimilate stratospheric ozone profiles from MLS (Microwave Limb Sounder) to investigate two Stratosphere-Troposphere Exchange (STE) case studies. .

This study examines the long-term record of lower stratospheric water vapor focusing on the 20-year data record from the Stratospheric Aerosol and Gas Experiment II (SAGE II). The SAGE II zonal monthly mean water vapor data was enhanced to include the aerosol heavy late 1980s through the use of aerosol extinction filtering of the data. Comparisons between the SAGE II lower stratospheric water vapor and the Limb Infrared Monitor of the Stratosphere (LIMS), the Microwave Limb Sounder (MLS), and HALogen Occultation Experiment (HALOE) are performed. This study further focuses on the minimum lower stratospheric water vapor (i.e., hygropause) and on the dehydration seen in the hygropause with examination of the transport barrier at both the tropical tropopause and the tropopause folding region between the tropics and extra-tropics that would account for this decadal variation. The effects of aerosol contamination on the SAGE II water vapor retrievals from four volcanic eruptions from 1984 to 1992 were examined, leading to a four level filtering of the SAGE II water vapor data to allow retention of good data from early in the data record. With the improved filtered water vapor data, monthly and seasonal time series analyses show a significant decadal variation in the lower stratosphere for all months where the satellite coverage provided data from the late 1980s to the early 2000s. This decadal variation documents a decrease in the water vapor from below approximately 25 km to below the tropopause with this decrease seen in the hygropause from the tropics to the poles. Analysis of the hygropause for all months provided a statistically significant consistent neutral or decreasing value in the long-term water vapor minimum. March was shown to be the seasonal minimum in the hygropause over this 20-year low aerosol record, followed by a discontinuity in the minimum abundance after 2000. Three transport pathways for transport of water vapor from the moist troposphere to the lower stratosphere include the tropical tropopause, isentropic transport at the sub-tropical jet locations, and meridional transport from the tropics to the midlatitudes above the hygropause. The tropical tropopause temperatures were examined using the new Modern Era Retrospective-analysis for Research and Applications (MERRA) data set. Analysis showed a significant decrease in the tropical and sub-tropical tropopause temperatures over the 20-year timeframe for the DJF season preceding the March minimum. The lower temperatures would provide a colder "cold trap" at the tropopause, further "freeze drying" the air seasonally transported from the upper troposphere to the lower stratosphere, providing the long-term dehydration in the hygropause and lower stratosphere. The Ertel's Potential Vorticity (EPV or PV) was examined as a proxy for the sub-tropical jet movement towards the poles over this long-term record. Changes in this pathway location may affect the efficiency of isentropic transport of moist tropospheric air into the lower stratosphere at these higher latitudes. Analysis using the MERRA zonal EPV and maximum zonal Uwind data showed a statistically significant shift in the locations of the contours towards the SH poles over this 20-year timeframe for the DJF, DJFM seasons and the month of December. The meridional winds above the tropopause show an increase over the 20-year record covered by SAGE II water vapor data. These increasing winds are consistent with the increase in the Brewer-Dobson circulation shown in other studies. The colder tropopause temperatures along with the increasing Brewer-Dobson circulation just above the tropopause, are the likely cause for the decreasing water vapor trend as seen in the SAGE II March hygropause over the 20-years from 1986-2005.

Afin de mieux comprendre les processus responsables de la distribution de l'ozone (O3) dans la haute troposphère (UT) tropicale, cette thèse étudie différents aspects du transport de la pollution depuis les régions sources jusque dans l'UT. La première étude repose sur les observations spatiales IASI qui identifient un évènement de transport de masses d'air enrichies en O3 dans l'UT depuis l'Afrique vers l'Inde. Pour la saison de pré-mousson de tels enrichissement d'O3 dans l'UT au-dessus de l'Océan Indien sont essentiellement attribués à des intrusions stratosphériques. Afin de déterminer son origine des simulations ont été effectuées permettant d'exclure une origine stratosphérique et montrent l'impact prépondérant des NOx produit par les éclairs (LiNOx) en Afrique pour expliquer cet enrichissement d'O3. Cette étude pourra être étendue à d'autres saisons, pour consolider les conclusions obtenues dans le cadre du projet INDOEX. La deuxième partie porte sur l'étude de l'impact d'un système convectif très profond sur la composition de l'UT pendant la mousson asiatique d'été. La simulation avec un traceur passif montre la capacité du système situé le long de l'Himalaya centrale à soulever des masses d'air polluées jusqu'à 100 hPa, altitudes auxquelles la pollution est transportée rapidement par la circulation de l'anticyclone de la mousson asiatique. Confirmant le conduit privilégié de transport vers l'UTLS identifié par Bergman et al. 2013. Cependant l'activation du schéma chimique montre une surestimation des LiNOx produites, un ajustement de leur paramétrisation devra être effectué ainsi que des simulations de sensibilité pour correctement quantifier la production d'O3. Ce travail prend place dans des problématiques actuellement au centre d'une collaboration internationale, ACAM (Atmospheric Composition and the Asian Monsoon) visant à étudier les interactions complexes de la mousson asiatique d'été entre dynamique et chimie, jusqu'à l'échelle du changement climatique. / To better understand the processes controling for the distribution of upper tropospheric (UT) ozone (O3) in the tropics, this thesis examines different aspects of pollution transport from sources regions to UT level, through two case studies that take place in the still debated issues.. First study is based on IASI space observations identified an event of transport of UT enriched O3 air masses from Africa to India. During the pre-monsoon season, events of O3 enrichment in UT above the Indian Ocean were essentially attributed to stratospherics intrusions. Simulations have been used to determine its origin, it excludes a stratospheric origin for the event and indicates a probable important contribution by lightning (LiNOx) that occurs over Africa regions. This study could be extended to the whole region and other seasons with a focus on the spring season in order to complete the conclusions obtained during the INDOEX program. The second part focuses on the characterisation of the impact of a deep convective system upon the UTLS composition during the asian summer monsoon. Simulation with a passive tracer highlights the potential of the convective system located over the central Himalaya foothills, to uplift polluted air masses in UTLS to 100 hPa, where the pollutants are rapidly transported by the asian monsoon anticyclone circulation. In agreement with transport pipe towards the UTLS identified by Bergman et al. 2013. However simulation including reactive chemistry show an overestimation by the model of the amount of LiNOx produced, so an adjustment of their parameterization must be made and sensitivity analysis are foreseen to determine precisely O3 production. This study is established in connection with actual major problematic at the center of general debate of the international collaboration. Like ACAM (Atmospheric Composition and the Asian Monsoon) whose targeting the complexe interaction of asian summer monsoon to atmospheric dynamics and chemistry, as well as climate change impact.