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.

Dans le contexte du réchauffement et du changement climatique, il est important d’étudier les distributions, les cycles saisonniers et les tendances des gaz à l’état de trace dans l’atmosphère tels que la vapeur d’eau. L'Observatoire de Physique du Globe de Clermont-Ferrand a en charge plusieurs dispositifs d’observation dont le site instrumenté Cézeaux, Opme et Puy de Dôme (CO-PDD) situés dans le centre de la France (45◦ N, 3◦ E). Le site des Cézeaux dispose d’un LIDAR Rayleigh – Mie - Raman fournissant en routine des profils verticaux de vapeur d’eau et de paramètres optiques caractérisant les cirrus. Le site du puy de Dôme est équipé d’un spectroscope à cavité optique (CRDS-Picarro). Des mesures de colonnes totales de vapeur d’eau sont disponibles sur tous ces sites par GPS. Le site d’Opme est équipé d’un pluviomètre. Enfin Météo-France effectue le travail de contrôle qualité des données météorologiques sur les stations de mesure en France et ces données ont été utilisées dans cette thèse. La validation des données sur le site du puy de Dôme a été la première la première exploitation dans cette thèse. Des comparaisons des données sur le puy de Dôme ont montré un très bon accord entre les données de vapeur d’eau extraites de la station météorologique du puy de Dôme, de Météo France et les donnes CRDS du puy de Dôme, avec une corrélation de 0.94 et 0.98 respectivement. Les profils verticaux obtenus par LIDAR ont permis de sélectionner une anomalie de vapeur d’eau et d’identifier une intrusion stratosphère-troposphère en analysant les processus dynamique associés à cette anomalie. Les données OLR ont montré que cette intrusion est accompagnée de convection profonde et enfin LACYTRAJ confirme l'origine stratosphérique d’une partie de la masse d'air présente au-dessus de Clermont-Ferrand au cours de l’anomalie. Les longues séries d’observations (ex : Puy de Dôme 1995-2015) et des ré-analyse ECMWF ERA-Interim (1979-2017) et la diversité des sources de données (ex : satellites AIRS et COSMIC), nous permettent de documenter, analyser et comparer la variabilité, les cycles et la tendance de la vapeur d'eau à la surface et dans la troposphère, à différentes échelles de temps et déterminer les processus géophysiques responsables des distributions de vapeur d'eau sur le site CO-PDD. Le cycle annuel de la vapeur d'eau est clairement établi pour les deux sites de différentes altitudes et pour tous les types de mesure. Les sites de Cézeaux et du puy de Dôme ne présentent presque aucun cycle diurne, suggérant que la variabilité de la vapeur d'eau à la surface sur ces deux sites est plus influencée par les systèmes météorologique sporadiques que par les variations diurnes régulières. Les données LIDAR montrent une plus grande variabilité mensuelle de la distribution verticale que les produits satellites COSMIC et AIRS. La colonne totale de vapeur d'eau GPS sur le site des Cézeaux présente une tendance positive (0,42 ± 0,45 g/kg*décade entre 2006-2017). L'analyse par régressions multi-linéaires montre que les forçages continentaux (East Atlantic, East Atlantic-West Russia) ont une plus grande influence que le forçage océanique (Nord Atlantic Oscillation) sur les variations de vapeur d'eau. / In the context of global warming and climate change, it is important to study the distributions, seasonal cycles and trends of trace gases in the atmosphere such as water vapor. of the Observatoire de Physique du Globe de Clermont-Ferrand is in charge of several observation devices including the instrumented site Cézeaux, Opme and Puy de Dôme (CO-PDD) located near the center of France (45◦ N, 3◦ E). The site of Cézeaux is instrumented by a Rayleigh - Mie–LIDAR Raman providing routine vertical profiles of water vapor mixing ratio and optical parameters characterizing cirrus clouds. The puy de Dôme site is equipped with an optical cavity spectroscope (CRDS-Picarro). Measurements of total water vapor columns are available on all these sites by GPS. The Opme site is equipped with rain gauges. Finally, Météo-France performs the quality control work and of data on meteorological stations in France and these data were used in this thesis. The validation of the puy de Dôme data was the first the first task in this thesis. Comparisons between the puy de Dôme data sets showed a very good agreement between the water vapor datafrom the OPGC meteorological station of Puy de Dôme, Météo France and CRDS data with a correlation of 0.94 and 0.98 respectively. The vertical profiles deduced from the LIDAR allowed to identify a water vapor anomaly and a stratosphere-troposphere intrusion associated with this anomaly. OLR data showed that this intrusion could be linked with deep convection and LACYTRAJ confirms the stratospheric origin of a part of the air mass present above Clermont-Ferrand. Long series of observations (eg Puy de Dôme 1995-2015) and ECMWF ERA-Interim re-analysis (1979-2017) and the diversity of data sources (eg AIRS and COSMIC satellites), allowed us to document, analyze and compare the variability, cycles and trend of surface and tropospheric water vapor at different time scales and determine the geophysical processes responsible for water vapor distributions at the site of CO-PDD. The annual cycle of water vapor is clearly established for the two sites of different altitudes and for all types of measurement. Cézeaux and puy de Dôme present almost no diurnal cycle, suggesting that the variability of surface water vapor at this site is more influenced by a sporadic meteorological system than by regular diurnal variations. The LIDAR dataset shows a greater monthly variability of the vertical distribution than the COSMIC and AIRS satellite products. The Cézeaux site presents a positive trend for the GPS water vapor total column (0.42 ± 0.45 g/kg*decade during 2006–2017) and a significant negative trend for the surface water vapor mixing ratio (−0.16 ± 0.09 mm/decade during 2002–2017). The multi-linear regression analysis shows that continental forcings (East Atlantic Pattern and East Atlantic-West Russia Pattern) have a larger influence than oceanic forcing (North Atlantic Oscillation) on the water vapor variations.

Fundação de Amparo a Pesquisa no Estado do Rio Grande do Sul / It was identified Stratosphere-Troposphere Exchange (STE) events on Southern South America and their effects in the Ozone Total Column (OTC) above Central Region of Rio Grande do Sul (CRRS), Brazil, in the period between 2005 and 2014. To this end, it was developed a methodology able to verify the tropopause height and the descend mass flux in this region, using reanalysis 2 data provided by NCEP/DOE. Furthermore, these cases must have wind cores above 40m/s (Upper-level Jet Stream - ULJS) acting between 30 and 80°W and 20 and 50°S. The arrival confirmation of air parcels from the STE at the CRRS was made through HYSPLIT trajectory analysis model from NOAA. For cases that acted at the CRRS, it was computed the OTC variation in relation to five days prior to the STE effects, through daily OTC data obtained from the OMI instrument for Santa Maria city (29.72°S; 53.72°W). This methodology proved to be effective in identifying 755 STE events on Southern South America, from which 103 came to act on CRRS, with 65% of cases increasing and 35% reducing the OTC in this region. Seasonal analysis showed that most cases happens in winter, followed by spring and in less quantity in summer and fall. Averaged fields of the vertical wind profile, mass flux, temperature and potential vorticity, showed that STE events occur more often in post-frontal situations at the Bacia do Prata region. Moreover, it was analyzed the convergence role in relation to jet streak s vertical transversal circulations, demonstrating that, in STE cases, these circulations increase even more the stratospheric air intake into the troposphere by strong convergence in the ULJS level. In short, it was verified that STE events on Southern South America act as a stratospheric ozone-rich air source to the CRRS, having as an allied the ULJS, which increase the phenomena. / Foram identificados eventos de Troca Estratosfera-Troposfera (TET) sobre o Sul da América do Sul e seus efeitos na variação da Coluna Total de Ozônio (CTO) Região Central do Rio Grande do Sul (RCRS), Brasil, no período entre 2005 e 2014. Para este fim, desenvolveu-se uma metodologia capaz de verificar a altura da tropopausa e o fluxo de massa descendente nesta região, utilizando dados de reanálise 2 fornecidos pelo NCEP/DOE. Além disso, os casos deveriam possuir núcleos de vento acima de 40 m/s (Corrente de Jato em Altos Níveis - CJAN) atuando entre 30 e 80°O e 20 e 50°S. A confirmação da chegada das parcelas de ar provenientes da TET na RCRS deu-se através da análise das trajetórias do modelo Hysplit da NOAA. Para os casos que atuaram na RCRS, calculou-se a variação da CTO em relação aos cinco dias anteriores aos efeitos da TET, através de dados diários da CTO obtidos do instrumento OMI para a cidade de Santa Maria (29.72°S; 53.72°O). Esta metodologia mostrou-se eficaz na identificação de 755 eventos de TET sobre o Sul da América do Sul, dos quais 103 vieram a atuar na RCRS, com 65% dos casos aumentando e com 35% reduzindo a CTO nesta região. A análise sazonal mostrou que a maioria dos casos acontece no inverno, seguido da primavera e em menor quantidade no verão e outono. Campos médios do perfil vertical de vento, fluxo de massa, temperatura e vorticidade potencial, mostraram que os eventos de TET ocorrem com mais frequência em uma situação pós-frontal na região da Bacia do Prata. Além disso, analisou-se o papel da convergência relacionada às circulações verticais transversais do núcleo da CJAN, mostrando que, em casos de TET, estas circulações intensificam ainda mais a entrada de ar estratosférico para dentro da troposfera por intermédio da forte convergência no nível da CJAN. Em suma, verificou-se que os eventos de TET sobre o Sul da América do Sul atuam como uma fonte de ar estratosférico rico em Ozônio para a RCRS, tendo como um de seus aliados a CJAN, a qual intensifica o fenômeno.

This master's thesis deals with the issue of volcanic ash as a complex and its impact on aviation, including the volcanic activity itself (conditions for its existence, for existence of eruptions and their basic products). In addition, the thesis also deals with effect of volcanic ash on aircraft and airports, possibilities of its detection or monitoring as well as mechanism of its spreading in airspace. The emphasis is laid mainly on air incidents related to volcanic ash and on danger it poses to the airspace of the Czech Republic.

L’étude de la pollution troposphérique inclut l’étude des gaz traces provenant de sources anthropiquesdiverses, dont l’impact varie de l’échelle locale à globale. Pour caractériser cette pollution, il est nécessairede mesurer avec précision les concentrations en polluants. Dans le cadre de projets européens, troiscampagnes aéroportées ont été conduites, dans le bassin méditerranéen, en Afrique de l’ouest et enMalaisie, pour mesurer différents types de polluants grâce, entre autres, à un spectromètre à lasersinfrarouges, SPIRIT, capable de mesurer rapidement en ligne de faibles variations de NO2 et CO. Les jeuxde données de ces gaz traces (et d’autres) ont été combinés avec un modèle lagrangien de dispersion departicules, FLEXPART, pour identifier différentes sources de pollution locales et régionales de l’air. Cettethèse présente ainsi les mesures et le travail de modélisation entrepris afin de définir les sources depollution de chaque région. Il a été montré que le bassin méditerranéen a été impacté, de la moyenne à lahaute troposphère pendant l’été, par des émissions de feux de biomasse venant de Sibérie et du continentnord-américain. Les régions ouest-africaine et malaisienne sont aussi impactées par des émissions de feuxde biomasse transportées depuis l’Afrique centrale dans le premier cas, et de feux locaux dans le second.En outre, ces régions sont influencées par des émissions provenant de l’exploitation du pétrole et du traficmaritime. FLEXPART a été utilisé afin d’identifier l’origine des pics de pollution mesurés au cours descampagnes. Nous avons ainsi montré que les conditions atmosphériques, qui définissent la hauteurd’injection du panache de la plateforme pétrolière, ainsi que le flux d’émission sont des paramètres clésdans la caractérisation des mesures par le modèle. / The study of tropospheric pollution includes the study of trace gases coming from various anthropogenicsources that can impact scales ranging from local to global. To characterise this pollution, it is necessary tobe able to measure with precision pollutant concentrations. Within the frame of European projects, threeairborne campaigns in the Mediterranean Basin, in West Africa and in Malaysia were conducted to measuredifferent types of pollutants thanks to, among others, an infrared laser spectrometer, SPIRIT, able to rapidlymeasure on-line small variations in NO2 and CO. The data sets of these trace gases (and others) have beencombined with a Lagrangian model of particle dispersion, FLEXPART, to fingerprint different sources of localand regional air pollution. Thus, this thesis presents the measurements and the modelling work undertakenin order to define the sources of pollution of each region. It has been shown that the Mediterranean Basinwas impacted, in the mid to upper troposphere during summer, by biomass burning emissions coming fromSiberia and the Northern American continent. West African and Malaysian regions are also impacted bybiomass burning emissions transported from central Africa in the first case, and from local fires in thesecond. In addition, those regions are influenced by emissions coming from oil exploitation and maritimetraffic. FLEXPART was used in order to identify the origin of the pollution peaks measured during thecampaigns. It has been shown that atmospheric conditions, which define the injection height of the oilplatform plume, and also the emission flux are key parameters in the characterisation of the measurementsby the model.

The parabolic equation methods are advantageous in simulating under small time frames because of their low computational complexity. Because of this they are also feasible to implement on low end hardware. Due to the parabolic approximation they are based on, much work exists on improving the error introduced from the approximation. In this publication, further effort is put into developing these methods and the result from a master thesis at Tietoevry are presented. An in-house algorithm for evaporation duct propagation has been altered to improve the terrain modeling and to include range varying refractivity in a split step Fourier method called the discrete mixed Fourier transform. Previously only the piecewise linear shift map was utilized for terrain modeling which is known to become unstable at propagation angles exceeding around 15 degrees from the horizontal. By utilizing a hybrid method between piecewise linear shift map and knife edge method the stability issues are partially avoided, hence the solutions generated with the hybrid method are stable for a larger range of slope angles than with only using piecewise linear shift map. The range varying refractivity was included in the discrete mixed fourier transform by indexing making it possible to simulate dynamic evaporation duct heights. The report starts with a review of the theoretical foundation that the algorithm is built upon. Secondly, a logical list of steps outlines the altered algorithm. To conclude, the changes to the code are presented and discussed with the new results together with remarks on possible future improvements and current problems with the algorithm.