Une grande partie de la variabilité naturelle de l’atmosphère et du climat est liée à la variabilité solaire. L’un des modes d’action du forçage solaire repose sur des perturbations de la moyenne atmosphère (stratosphère, mésosphère), notamment par l’intermédiaire de variations d’ozone (processus photochimiques) qui ensuite se propagent dans la troposphère jusqu’à la surface. La thèse se focalise sur la première étape de ce mode d’action, i.e. les perturbations de l’ozone associées à la variabilité solaire et plus particulièrement aux échelles de temps du cycle à 27 jours. Cette relation entre ozone et variabilité solaire est étudiée non seulement à partir de plusieurs séries temporelles de données satellitaires (MLS et GOMOS) mais également de résultats d’un modèle de chimie-climat (LMDz-Reprobus) sur des fenêtres d’analyse variant de 1 à 15 ans. La sensibilité moyenne d’ozone au cycle solaire à 27 jours (% de variation d’ozone pour 1% de variation du forçage solaire) se caractérise par des valeurs positives de 10 à 1 hPa avec un maximum de 0.4 vers 3 hPa. Cette sensibilité varie beaucoup selon la taille de la fenêtre d’analyse au point d’être masquée par la variabilité dynamique, même pendant les périodes de forte activité solaire. La dispersion des résultats apparaît aussi anti-corrélée à l’amplitude des fluctuations solaires rotationnelles qui est liée à la phase du cycle solaire à 11 ans. Dans la mésosphère, l’ozone est anti-corrélé à la variabilité solaire avec un maximum autour de 80 km. Il correspond exactement à l’altitude où la réponse de OH (le radical dominant dans la destruction de l’ozone mésosphérique) à la variabilité solaire est maximum. / A large part of the natural variability of the atmosphere and climate is related to solar variability. One of the forcing mechanisms of solar variability is based on perturbations of the middle atmosphere (stratosphere, mesosphere), particularly through ozone variations (photochemical processes), that then propagate through the troposphere to the surface. The thesis focuses on the first stage of this forcing mechanism, i.e. perturbations of ozone associated with solar variability and more specifically at the 27-day solar rotational time scales. The relationship between ozone and solar variability is studied not only using several time series of satellite data (MLS and GOMOS) but also results of a chemistry-climate model (LMDz-Reprobus) over analysis windows varying from 1 to 15 years. The mean ozone sensitivity to the 27-day solar cycle (% of ozone variation for 1% change in solar forcing) is characterized by positive values from 10 to 1 hPa with a maximum of 0.4 at 3 hPa. This sensitivity varies strongly depending on the size of the analysis window indicating that the solar signal can be masked by the dynamical variability, even during periods of strong solar activity. The dispersion of the results is found to be anti-correlated with the amplitude of the solar rotational fluctuations that are related to the phase of the 11-year solar cycle. In the mesosphere, ozone is found to be anti-correlated with solar variability with a maximum around 80 km. This corresponds exactly to the altitude of the maximum in the solar-induced enhancement of OH, the dominant radical in the destruction of mesospheric ozone.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第21579号 / 理博第4486号 / 新制||理||1644(附属図書館) / 京都大学大学院理学研究科地球惑星科学専攻 / (主査)教授 橋口 浩之, 教授 塩谷 雅人, 教授 秋友 和典 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

The ionosphere-thermosphere can be considered to a certain degree as a system, which is externally-driven by the extreme-ultraviolet solar radiation. The main components in the regular variation are connected to the solar cycle, solar rotation and the diurnal cycle. However, anomalies and periodicities of several days, which cannot be related to changes in the solar activity at all times, were detected in ionospheric parameters. It is assumed that the total variation in the ionosphere is partly forced by waves coming from below. This thesis provides a clearer picture of the seasonal changes of wave phenomena observed in the ionosphere and its possible relation to lower atmospheric structures. Since such global disturbances in the middle atmosphere are termed as planetary waves (PW), such features in the ionosphere are declared as planetary wave type oscillations (PWTO), although a direct connection is excluded.Northern hemispheric maps of the Total Electron Content (TEC) derived from GPS-signals that are currently used for monitoring the ionospheric F-region in relation to space weather provide a basis for investigating PWTO applying space-time analysis methods to separate stationary and traveling wave components from the data. Compared to analyses of PW obtained by regular stratospheric reanalyses the seasonal behavior and possible coexisting wave activities during the considered period of time (2002-2008) are presented. Such a climatological consideration has revealed that recurring events in the course of the solar cycle are rare, but it seems that the westward propagating quasi 16-day wave with zonal wavenumber 1, analysed from stratospheric MetO reanalyses, and the ionosphere are indirectly coupled. Generally, the correspondence of other components are restricted around the solar maximum 2002-2005. There are some suggestions, how the middle and upper atmosphere are connected by PW. Sounding of the middle atmosphere by remote sensing techniques from satellites (e.g. SABER on TIMED) deliver a suitable basis to investigate the coupling by the modulation of gravity waves (GW). By calculating the potential energy for a certain wave spectrum, characterized by vertical wavelength shorter than 6 km, and determining proxies of traveling waves permits to investigate a possible mechanism. The results reveal that GW partly penetrate the lower thermosphere carrying a modulation by PW. In some cases, especially during the first three winter, near solar maximum, stratospheric PW show a good correlation to indirect signals in the lower thermosphere and to PWTO in the ionospheric F-region near 300 km.

Es wird angenommen, dass die Zirkulation der Nordhemisphäre durch den Rückgang von Meereis in der Arktis und der Zunahme der Oberflächenalbedo in Sibirien beeinflusst wird. Letzteres wurde mit dem aktuellen atmosphärischen Zirkulationsmodell ICON getestet. Die Albedo über Sibirien wurde innerhalb eines Experimentes erhöht, und zwar auf Werte welche vergleichbar mit denen über dem grönländischen Eisschild sind. Es wurde festgestellt, dass in den Wintermonaten Dezember und Januar die vertikale Wellenausbreitung stärker in die Stratosphäre reicht; dem folgt auch die in der Theorie erwartete Erwärmung in der Stratosphäre. / The Northern hemisphere circulation is supposed to change due to changed sea-ice cover in the Arctic and the increase of Siberian surface albedo. The latter is tested using the state of the art atmospheric circulation model ICON. We artificially increased the albedo of Siberia to values comparable to the Greenland ice sheet to investigate the change of vertical wave propagation and the general change of the background circulation. It was found for the winter season that the increased albedo results in increased vertical wave propagation for December and January. This is accompanied by a warming of the stratosphere that was found for the whole winter.

This thesis examines the utility of mathematical complexity measures for the analysis of stratospheric dynamics. Through theoretical considerations and tests with artificial data sets, e.g., the iteration of the logistic map, suitable parameters are determined for the application of the statistical entropy measures sample entropy (SE) and Rényi entropy (RE) to methane (a long-lived stratospheric tracer) data from simulations of the SOCOL chemistry-climate model. The SE is shown to be useful for quantifying the variability of recurring patterns in a time series and is able to identify tropical patterns similar to those reported by previous studies of the ``tropical pipe'' region. However, the SE is found to be unsuitable for use in polar regions, due to the non-stationarity of the methane data at extra-tropical latitudes. It is concluded that the SE cannot be used to analyse climate complexity on a global scale. The focus is turned to the RE, which is a complexity measure of probability distribution functions (PDFs). Using the second order RE and a normalisation factor, zonal PDFs of ten consecutive days of methane data are created with a Bayesian optimal binning technique. From these, the RE is calculated for every day (moving 10-day window). The results indicate that the RE is a promising tool for identifying stratospheric mixing barriers. In Southern Hemisphere winter and early spring, RE produces patterns similar to those found in other studies of stratospheric mixing. High values of RE are found to be indicative of the strong fluctuations in tracer distributions associated with relatively unmixed air in general, and with gradients in the vicinity of mixing barriers, in particular. Lower values suggest more thoroughly mixed air masses. The analysis is extended to eleven years of model data. Realistic inter-annual variability of some of the RE structures is observed, particularly in the Southern Hemisphere. By calculating a climatological mean of the RE for this period, additional mixing patterns are identified in the Northern Hemisphere. The validity of the RE analysis and its interpretation is underlined by showing that qualitatively similar patterns can be seen when using observational satellite data of a different tracer. Compared to previous techniques, the RE has the advantage that it requires significantly less computational effort, as it can be used to derive dynamical information from model or measurement tracer data without relying on any additional input such as wind fields. The results presented in this thesis strongly suggest that the RE is a useful new metric for analysing stratospheric mixing and its variability from climate model data. Furthermore, it is shown that the RE measure is very robust with respect to data gaps, which makes it ideal for application to observations. Hence, using the RE for comparing observations of tracer distributions with those from model simulations potentially presents a novel approach for analysing mixing in the stratosphere.

Cette thèse présente des reconstructions de l'irradiance totale et spectrale durant les 400 dernières années à l'aide des modèles pour l'irradiance totale et l'irradiance spectrale dans l'ultraviolet développés à l'Université de Montréal. Tous deux sont basés sur la simulation de l'émergence, de la fragmentation et de l'érosion des taches solaires, qui permet d'obtenir une distribution de l'aire des taches sombres et des facules brillantes en fonction du temps. Ces deux composantes sont principalement responsables de la variation de l'irradiance sur l'échelle de temps de la décennie, qui peut être calculée en sommant leur émissivité à celle de la photosphère inactive. La version améliorée du modèle d'irradiance solaire spectrale MOCASSIM inclut une extension de son domaine spectral entre 150 et 400 nm ainsi que de son domaine temporel, débutant originalement en 1874 et couvrant maintenant la période débutant en 1610 jusqu'au présent. Cela permet de reconstruire le spectre ultraviolet durant le minimum de Maunder et de le comparer à celui du minimum de 2009. Les conclusions tirées de cette étude spécifient que l'émissivité dans l'ultraviolet était plus élevée en 2009 que durant le minimum de Maunder, que le niveau de base de la photosphère non magnétisée contribuait pour environ les deux tiers de cette différence et que les structures magnétiques restantes étaient responsables pour le tiers restant. Le modèle d'irradiance totale a vu son domaine temporel étendu sur la même période et une composante représentant le réseau magnétique de façon réaliste y a été ajoutée. Il a été démontré que les observations des 30 dernières années ne sont bien reproduites qu'en incluant la composante du Soleil non magnétisé variable à long terme. Le processus d'optimisation des paramètres libres du modèle a été effectué en minimisant le carré de la somme de l'écart journalier entre les résultats des calculs et les données observées. Les trois composites disponibles, soit celui du PMOD (Physikalisch Meteorologisches Observatorium Davos), d'ACRIM (ACtive Radiometer Irradiance Monitor) et du IRMB (Institut Royal Météorologique de Belgique), ne sont pas en accord entre eux, en particulier au niveau des minima du cycle d'activité, et le modèle permet seulement de reproduire celui du PMOD avec exactitude lorsque la composante variable à long terme est proportionnelle au flux radio à 10.7 cm. Toutefois, en utilisant des polynômes de Lagrange pour représenter la variation du Soleil inactif, l'accord est amélioré pour les trois composites durant les minima, bien que les relations entre le niveau minimal de l'irradiance et la longueur du cycle précédent varient d'un cas à l'autre. Les résultats obtenus avec le modèle d'irradiance spectrale ont été utilisés dans une étude d'intercomparaison de la réponse de la photochimie stratosphérique à différentes représentations du spectre solaire. Les simulations en mode transitoire d'une durée de 10 jours ont été effectuées avec un spectre solaire constant correspondant soit à une période d'activité minimale ou à une période d'activité maximale. Ceci a permis d'évaluer la réponse de la concentration d'ozone à la variabilité solaire au cours d'un cycle et la différence entre deux minima. En plus de ceux de MOCASSIM, les spectres produits par deux modèles ont été utilisés (NRLSSI et MGNM) ainsi que les données de SIM et SOLSTICE/SORCE. La variabilité spectrale de chacun a été extraite et multipliée à un spectre de base représentant le minimum d'activité afin de simuler le spectre au maximum d'activité. Cela a été effectué dans le but d'isoler l'effet de la variabilité seule et d'exclure celui de la valeur absolue du spectre. La variabilité spectrale d'amplitude relativement élevée des observations de SORCE n'a pas provoqué l'inversion de la réponse de l'ozone à hautes altitudes obtenues par d'autres études, ce qui peut être expliqué par la nature même du modèle utilisé ainsi que par sa limite supérieure en altitude. Finalement, la réponse de l'ozone semble être à peu près proportionnelle à la variabilité de l'intégrale du flux pour lambda<241 nm. La comparaison des concentrations d'ozone obtenues avec les spectres originaux au minimum d'activité démontre que leur différence est du même ordre de grandeur que la variabilité entre le minimum et le maximum d'un cycle typique. Le problème du choix de la reconstruction de l'irradiance à utiliser pour les simulations climatiques dans le passé demeure non résolu. / This thesis presents reconstructions of the total and spectral solar irradiance for the last 400 years produced with the improved versions of the models for total and spectral solar irradiance in the ultraviolet developed at Université de Montréal. Both are based on the simulation of sunspot emergence, fragmentation and erosion, which produces a time-evolving area distribution of dark spots and bright faculae. These two components are the main drivers of irradiance decadal variations and this quantity can be calculated by summing their emissivity to that of the quiet photosphere. The improved version of the model for spectral irradiance, MOCASSIM, includes an extension of its spectral domain between 150 and 400 nm and of its temporal domain, with reconstructions now starting in 1610 instead of 1874. This allows to reconstruct the UV spectrum during the Maunder minimum and to compare it to the spectrum during the minimum of 2009. The conclusions of this study state that the Sun was slightly brighter during the recent minimum and that the slowly-varying quiet Sun contribution accounts for about two thirds of this difference, whereas remnant magnetic structure decay products account for the other third. The model for total irradiance was also extended further in the past, with reconstructions now starting in 1610. Also, a realistic network component was added. This was expected to help reproduce the observations spanning the last 30 years, especially the varying level of the irradiance during minimum activity. It was shown that the inclusion of a slowly-varying quiet Sun component was necessary to account for the observations. The free parameters of the model were adjusted by minimizing the sum of the daily squared difference between the model's output and the observations. The three available composites, from the PMOD (Physikalisch Meteorologisches Observatorium Davos), ACRIM (ACtive Radiometer Irradiance Monitor) and IRMB (Institut Royal Météorologique de Belgique) teams, do not agree between them, especially considering the minima of the activity cycle. The only composite reproduced in a satisfactory manner by the model when the variable quiet Sun component is proportionnal to the radio flux at 10.7 cm is the PMOD composite. However, using Lagrange polynomials to represent this component helps improve the agreement at minimum activity for all composites, even though the relation between the irradiance during the minima and the length of the preceding cycle varies from one to another. The results obtained with MOCASSIM were used during an intercomparison study of the photochemical response in the stratosphere to different representations of the solar spectrum. Transient simulations of duration 10-days were performed with a constant solar spectrum corresponding to either a maximum or minimum activity period. This allowed to estimate the response in stratospheric ozone to the solar variability over a cycle or between two minima. The spectra obtained with MOCASSIM were used along with those from two other models, NRLSSI and MGNM, and the SIM and SOLSTICE/SORCE data. The spectral variability from each data set was multiplied to a common baseline spectrum to produce the high activity spectrum in order to isolate the effet of the variability only, and to exclude the effect of the absolute spectral calibration. The high spectral variability of the SORCE data in the UV did not induce a negative response in ozone at high altitude, as obtained by various other studies. This is explained by the nature of the model and by its limited vertical extent. Finally, the ozone response is approximately proportional to the integrated UV flux below 241 nm. The comparison of the ozone concentration at minimum activity obtained with the original spectra shows that the difference is of the same magnitude as the response over a solar cycle. The problem of choosing a solar spectral irradiance reconstruction for climatic simulations in the past remains unsolved.

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. .

O clima na Antártica tem um papel fundamental no balanço de energia global. Estudos sugerem que a atividade convectiva tropical e a circulação estratosférica exercem um papel importante sobre a circulação atmosférica nos extratrópicos. A temperatura do ar é uma variável sensível às mudanças na circulação, no entanto, ainda não foi investigada a importância da escala intra-sazonal na sua variabilidade sobre a Antártica. Neste trabalho estudou-se a variabilidade intra-sazonal da temperatura do ar a superfície na região da Península Antártica enfocando as interações trópicos-extratrópicos e troposfera-estratosfera na modulação de eventos extremos de temperatura naquela região. Foram utilizados dados diários de estações localizadas nos setores leste e oeste da Península Antártica no período de 1986-2002. A análise espectral dos dados ressaltou a importância da escala intra-sazonal na variabilidade da temperatura na Península Antártica, principalmente no período de inverno, primavera e verão. Baseado nestes resultados, os dados foram filtrados na escala intra-sazonal (banda de 20-100 dias) e posteriormente, obteve-se os extremos intra-sazonais frios e quentes para as três estações do ano, através dos quartis da distribuição dos dados. Os eventos extremos intra-sazonais de temperatura (EIT) foram mais intensos no inverno e mais fracos no verão. As características da circulação atmosférica intra-sazonal associada aos EIT foram obtidas através de composições defasadas das anomalias intra-sazonais da altura geopotencial em 200 hPa, vento zonal em 200 hPa e vento meridional em 850 hPa. Nas três estações do ano, observou-se nos eventos extremos intra-sazonais frios (EIF) a persistência de anomalias ciclônicas em altos níveis, a diminuição da intensidade do jato polar e uma advecção de ar frio em baixos níveis sobre a região de estudo. Uma situação oposta foi verificada nos eventos extremos intra-sazonais quentes (EIQ). De forma geral, observou-se um trem de ondas entre latitudes médias e altas no Hemisfério Sul (HS) durante os EIT, particularmente no inverno e primavera. Esta configuração mostrou-se semelhante a tele-conexão conhecida como Pacífico-Sul Americano (PSA). O papel do modo anular do HS sobre os EIT foi analisado através do cálculo de Funções Ortogonais Empíricas das anomalias intra-sazonais da altura geopotencial em 700 hPa ao sul de 20ºS. Sua estrutura foi mais intensa (mais fraca) nos EIF (EIQ) de inverno sobre a região de estudo. A interação troposfera-estratosfera no controle dos EIT foi investigada através do Fluxo Eliassen-Palm. Nas composições das anomalias intra-sazonais deste fluxo (EPIS), observou-se durante os EIF (EIQ) de inverno, um aumento da atividade de onda da baixa estratosfera (alta troposfera) para a alta troposfera (baixa estratosfera) sobre a região de estudo, associado à diminuição (aumento) da intensidade do jato polar. Na primavera, a atividade de onda foi mais intensa e verificou-se uma mudança na direção do fluxo EPIS quando comparado com os EIT de inverno. O fluxo EPIS e as anomalias intra-sazonais do vento zonal foram mais fracos no verão. As anomalias intra-sazonais da circulação atmosférica e da atividade de onda na troposfera e estratosfera foram observadas por cerca de 10 dias antes da observação dos EIT de inverno. Portanto, a atividade intra-sazonal nos extratrópicos e as interações troposfera-estratosfera são fatores relevantes para um melhor entendimento da variabilidade da temperatura sobre a Península Antártica. / The Antarctic climate plays a significant role for the global energy budget. Previous studies suggest that interactions tropics-extratropics and the dynamics of the stratosphere are important factors to understand climate variations in the extratropics. The air temperature near surface responds to changes in circulation in low and upper levels. However, no previous studies have objectively investigated the importance of intraseasonal variations in modulating temperature around the Antarctica Peninsula. The present study examines intraseasonal extreme anomalies of near surface air temperature in the Antarctica Peninsula, and investigates interactions tropics-extratropics and troposphere-stratosphere. Daily temperature data from stations located east and west of the Antarctica Peninsula during 1986-2002 are investigated. Spectral analyses indicate that intraseasonal anomalies in temperature records are statistically significant during summer, winter and spring in all stations. Based on these results, temperatures are band-filtered on intraseasonal timescales (20-100 days) and extreme anomalies are investigated in each season (spring, summer and winter) based on the quartiles of the distributions. Intraseasonal extreme temperature (IET) anomalies are more intense during winter than during summer. Variations in the atmospheric circulation during IET are investigated by performing composites of intraseasonal anomalies of the geopotential height in 200hPa, zonal wind in 200hPa and meridional wind in 850hPa. During the three seasons, cold IET are associated with persistent upper level cyclonic anomalies, easterly anomalies of the polar jet and cold advection in low levels over the Peninsula. Opposite features are observed during warm IET. An extratropical wave-train is observed during all IET with stronger intensity during winter and spring. This feature resembles the Pacific South American (PSA) teleconnection pattern. The Southern Hemisphere Annular mode during the IET, identified as the first Empirical Orthogonal Function (EOF) of the intraseasonal 700hPa geopotential height anomalies poleward of 20oS, is more intense (weak) during cold (warm) IET events during winter. The stratosphere-troposphere interaction during IET events was examined with composites of the Eliassen-Palm Flux intraseasonal anomalies (EPIS). During spring, the wave activity is more intense and the EPIS direction is opposite to winter. During summer, EPIS are weak. Intraseasonal anomalies in the circulation and the wave activity in the troposphere and stratosphere lead the IET during winter in about 10 days. Therefore, the intraseasonal activity in the extratropics and the interactions stratosphere-troposphere are important factors for a complete understanding of the temperature variability over the Antarctica Peninsula.

To understand the contribution of aerosol particles to radiative forcing and heterogeneous chemical processes in the upper troposphere and lowermost stratosphere (UT/LMS), the knowledge of the particle size distribution is mandatory. Unfortunately, measurements in the UT/LMS are costly. Research aircrafts are expensive and thus their application is limited in time and space. Satellite remote sensing measurements provide a good temporal and spatial (horizontal) coverage, but only a limited vertical resolution and currently cannot resolve the particle size distribution. Therefore, within this thesis an optical particle counter (OPC) unit was modified for the application onboard a passenger long-haul aircraft within the CARIBIC project (www.caribic-atmospheric.com). The CARIBIC OPC unit provides regular and cost-efficient particle size distribution measurements of accumulation mode particles in the UT/LMS. In April 2010, the new OPC unit was installed for the first time onboard the Lufthansa Airbus A340 600 (D-AIHE) for the measurement of the volcanic ash cloud from the Eyjafjallajökull eruption (April to May 2010). Since June 2010 the OPC unit measures on usually four intercontinental flights per month the UT/LMS particle size distribution in the particle size range 125 to 1300 nm particle diameter. As the data acquisition stores the scattering raw signal and all housekeeping data as well, during the post flight data analysis the temporal- and size channel resolution can be flexible set. Within this work the data were analyzed with 32 size channels and 300 seconds. As aircraft-borne measurements are always time-consuming, the development of the OPC unit and the analysis routine, as well as its characterization and certification took more than two thirds of the total working time of this thesis. Therefore, the analysis of the data is limited to the first year of regular measurements until May 2011. Nevertheless, this dataset is sufficient to demonstrate the scientific relevance of these measurements. To validate the OPC data, a comparison to particle size distributions measured from board research aircraft was carried out. The analysis of the volcanic ash flights in April and May 2010 showed strongly enhanced particle mass concentrations inside the plumes and agreed in some regions very well to the particle mass concentration predicted by a dispersion model. A further case study shows the occurrence of a surprising large (1000 km) and high concentrated pollution plume over eastern Asia close to Osaka (Japan). Inside the plume the highest particle number- and mass concentrations measured with the OPC unit in the analysis period were observed (except volcanic ash flights). A detailed analysis of the in parallel measured trace gasses as well as meteorological- and LIDAR data showed, the observed plume originate from biomass burning and industrial emissions in eastern China. A third case study gives a first attempt of a mass closure/validation between the particle masses derived by the CARIBIC OPC unit and the CARIBIC impactor particle samples. First statistical analyses to the vertical, meridional, and seasonal variation of the accumulation mode particle size distribution and therefrom derived parameter indicate a stratospheric vertical increasing gradient for the particle number- and mass concentration. In general in the mid-latitude LMS the concentration of accumulation mode particles was found to be on average 120% higher than in the mid-latitude UT. The mid-latitude LMS particle size distribution shows a seasonal variation with on average 120% higher concentrations during spring compared to fall. This results can be explained with general dynamics in the stratosphere (Brewer-Dobson Circulation) and in the tropopause region (stratosphere-troposphere-exchange, STE). An anti-correlation of gaseous mercury to the stratospheric particle surface area concentration (R²=0.97) indicates that most likely stratospheric aerosol particles do act as a sink for gaseous mercury. Finally, two comparisons of the OPC data to data from satellite remote sensing and a global aerosol model underline the OPC potential and the benefits of creating an in situ measured reference dataset. / Um die Rolle von Aerosolpartikeln beim Strahlungsantrieb und der heterogenen chemischen Prozessen in der oberen Troposphäre und untersten Stratosphäre (OT/US) verstehen zu können, ist es unabdingbar die Partikelgrößenverteilung zu kennen. Messungen der Partikelgrößenverteilung in dieser Region sind allerdings aufwendig. Der Einsatz von Forschungsflugzeugen ist teuer und deshalb zeitlich und räumlich nur begrenzt. Satellitenmessungen bieten zwar eine gute zeitliche und räumliche (horizontal) Abdeckung, aber nur eine begrenzte vertikale Auflösung. Weiterhin können bisherige Satellitenmessungen die Partikelgrößenverteilung nicht auflösen. Im Rahmen dieser Arbeit wurde deshalb ein optischer Partikelzähler (OPC) Messeinschub für den Einsatz an Bord eines Langstrecken-Passagierflugzeugs aufgebaut (CARIBIC Projekt, www.caribic-atmospheric.com). Mit diesem Messeinschub kann regelmäßig und kosteneffizient die Partikelgrößenverteilung des Akkumulationsmodes in der OT/US gemessen werden. Im April 2010 wurde der neue OPC Einschub erstmals an Bord des Lufthansa Airbus A340-600 (D-AIHE) installiert um die Vulkanasche der Eyjafjallajökull Eruption (April bis Mai 2010) zu messen. Seit Juni 2010 misst der OPC Einschub auf durchschnittlich vier Interkontinentalflügen pro Monat die Partikelgrößenverteilung der OT/US im Größenbereich zwischen 125 und 1300 nm Partikeldurchmesser. Während des Fluges speichert die Datenerfassung alle Rohsignale ab und ermöglicht dadurch eine nutzerspezifische Datenauswertung nach dem Flug (z. B. Anzahl der Größenkanäle oder Zeitauflösung). Im Rahmen dieser Arbeit wurden die Daten mit 32 Größenkanälen und 300 Sekunden analysiert. Da fluggetragene Messungen immer sehr aufwendig sind, beanspruchte die Entwicklung des OPC Einschubs und des Analysealgorithmus, sowie die Charakterisierung und Zertifizierung mehr als zwei Drittel der Gesamtarbeitszeit dieser Arbeit. Daher ist die Analyse der Messdaten auf das erste Jahr der regulären Messungen bis Mai 2011 beschränkt. Dennoch ist dieser Datensatz geeignet um die wissenschaftliche Relevanz dieser Messungen zu demonstrieren. Um die OPC-Daten zu validieren, wurde ein Vergleich mit bisherigen OPC Messungen von Bord Forschungsflugzeugen durchgeführt. Die Analyse der Vulkanascheflüge im April und Mai 2010 zeigte in der Abluftfahne stark erhöhte Partikelmassekonzentrationen, welche in einigen Vergleichsregionen sehr gut mit der Vorhersage eines Disperionsmodells übereinstimmten. Eine weitere Fallstudie zeigt das Auftreten einer überraschend großen (1000 km) und hoch konzentrierten Abluftfahne über Ostasien nahe Osaka (Japan). In der Abluftfahne wurde die im Analysezeitraum höchste mit dem CARIBIC OPC gemessene Partikelanzahl- und Massenkonzentration beobachtet (ausgenommen Vulkanascheflüge). Eine detaillierte Analyse der parallel gemessenen Spurengase, sowie meteorologischer Daten und LIDAR Profile zeigte, dass die beobachtete Abluftfahne eine Mischung aus Biomasseverbrennungs- und Industrieabgasen aus Ost-China war. Eine dritte Fallstudie stellt einen ersten Versuch einer Massenschließung/Validierung zwischen der aus den CARIBIC OPC-Daten abgeleiteten Partikelmasse und der Partikelmasse aus CARIBIC Impaktorproben dar. Erste statistische Analysen zur vertikalen, meridionalen und saisonalen Variabilität der Partikelgrößenverteilung im Akkumulationsmode und daraus abgeleiteten Parametern zeigen einen vertikal ansteigenden Gradienten für die Partikelanzahl- und Massenkonzentration. Generell war in der US der mittleren Breiten die Konzentration von Akkumulationsmode Partikeln im Mittel um 120% höher als in der OT der mittleren Breiten. Weiterhin wurde in der US der mittleren Breiten eine jahreszeitliche Schwankung gefunden. Im Frühling war die mit dem OPC gemessene Partikelkonzentrationen im Mittel um 120% höher als im Herbst. Diese Befunde lassen sich mit der atmosphärischen Dynamik in der Stratosphäre (Brewer-Dobson Zirkulation) und in der Tropopausenregion (Stratosphäre-Troposphäre-Austauschprozesse) erklären. Eine gefundene negative Korrelation von gasförmigen Quecksilber mit der stratosphärischen Partikeloberflächenkonzentration (R²=0.97) ist ein starker Indikator dafür, dass in der US Aerosolpartikel eine Senke für gasförmiges Quecksilber darstellen. Zum Abschluss unterstreichen zwei Vergleiche der OPC-Daten mit Satellitenmessungen und Ergebnissen eines globalen Aerosolmodels das Potential und den Nutzen der CARIBIC OPC Daten als in-situ gemessenen Referenzdatensatz.

A lack of quality data on high clouds has led to inadequate representations within global weather and climate models. Recent advances in spaceborne measurements of the Earth’s atmosphere have provided complementary information on the interior of these clouds. This study demonstrate how an array of space-borne measurements can be used and combined, by close co-located comparisons in space and time, to form a more complete representation of high cloud processes and properties. High clouds are found in the upper atmosphere, where sub-zero temperatures frequently result in the formation of cloud particles that are composed of ice. Weather and climate models characterise the bulk properties of these ice particles to describe the current state of the cloud-sky atmosphere. By directly comparing measurements with simulations undertaken at the same place and time, this study demonstrates how improvements can be made to the representation of cloud properties. The results from this study will assist in the design of future cloud missions to provide a better quality input. These improvements will also help improve weather predictions and lower the uncertainty in cloud feedback response to increasing atmospheric temperature. Most clouds are difficult to monitor by more than one instrument due to continuous changes in: large-scale and sub-cloud scale circulation features, microphysical properties and processes and characteristic chemical signatures. This study undertakes co-located comparisons of high cloud data with a cloud ice dataset reported from the Microwave Limb Sounder (MLS) instrument onboard the Aura satellite that forms part of the A-train constellation. Data from the MLS science team include vertical profiles of temperature, ice water content (IWC) and the mixing ratios of several trace gases. Their vertical resolutions are 3 to 6 km. Initial investigations explore the link between cloud-top properties and the longwave radiation budget, developing methods for estimating cloud top heights using; longwave radiative fluxes, and IWC profiles. Synergistic trios of direct and indirect high cloud measurements were used to validate detections from the MLS by direct comparisons with two different A-train instruments; the NASA Moderate-resolution Imaging Spectroradiometer (MODIS) and the Clouds and the Earth’s Radiant Energy System (CERES) onboard on the Aqua satellite. This finding focuses later studies on two high cloud scene types that are well detected by the MLS; deep convective plumes that form from moist ascent, and their adjacent outflows that emanate outwards several hundred kilometres. The second part of the thesis identifies and characterises two different high cloud scenes in the tropics. Direct observational data is used to refine calculations of the climate sensitivity to upper tropospheric humidity and high cloud in different conditions. The data reveals several discernible features of convective outflows are identified using a large sample of MLS data. The key finding, facilitated by the use of co-location, reveals that deep convective plumes exert a large longwave warming effect on the local climate of 52 ± 28Wm−2, with their adjacent outflows presenting a more modest warming of 33 ± 20Wm−2.