The effect of recent climate change in Central Asia poses a significant and potentially serious challenge to the region’s agricultural sector. An investigation of the aerosol-climate- crop yield correlation in this region is essential for a better understanding of the effect of aerosols and climate on Central Asian agriculture. Our goal is to investigate the linkages between aerosol, climate and major crop production (cotton, maize, wheat, and rice) in specified agricultural regions in the five Central Asian countries. Our approach is to perform the Pearson’s Correlation Coefficient analysis in order to observe the statistical correlation between crop yield, temperature, precipitation, and aerosol optical depth (AOD), for each indicated agricultural region in the selected countries. Besides, using NASA GIOVANNI website tools, we retrieve distribution maps and time series of temperature, precipitation and AOD to facilitate the analyses. The research shows that in some aspects, the relation between AOD, climate, and crop yield is different in Central Asia than in previous global or large scale research hypotheses. The statistical correlations vary not only across countries but also across agricultural regions. For example, in Kazakhstan, opposite correlations exist between precipitation and AOD in two different agricultural regions even though both regions are rain-fed. In the more arid countries (with lower rain rates) such as Turkmenistan and Uzbekistan, no correlation exists between crop production and temperature, precipitation, and AOD, while the less arid (with higher rain rate) countries (Kazakhstan, Kyrgyzstan, and Tajikistan) indicate a positive correlation.

An accurate and generalized global retrieval algorithm from satellite observations is a prerequisite to understand the radiative effect of atmospheric aerosols on the climate system. Current operational aerosol retrieval algorithms are limited by the inversion schemes and suffering from the non-uniqueness problem. In order to solve these issues, a new algorithm is developed for the retrieval of non-spherical dust aerosol over land using multi-angular radiance and polarized measurements of the POLDER (POLarization and Directionality of the Earth’s Reflectances) and wide spectral high-resolution measurements of the MODIS (MODerate resolution Imaging Spectro-radiometer). As the first step to account for the non-sphericity of irregularly shaped dust aerosols in the light scattering problem, the spheroidal model is introduced. To solve the basic electromagnetic wave scattering problem by a single spheroid, we developed an algorithm, by transforming the transcendental infinite-continued-fraction-formeigen equation into a symmetric tri-diagonal linear system, for the calculation of the spheroidal angle function, radial functions of the first and second kind, as well as the corresponding first order derivatives. A database is developed subsequently to calculate the bulk scattering properties of dust aerosols for each channel of the satellite instruments. For the purpose of simulation of satellite observations, a code is developed to solve the VRTE (Vector Radiative Transfer Equation) for the coupled atmosphere-surface system using the adding-doubling technique. An alternative fast algorithm, where all the solid angle integrals are converted to summations on an icosahedral grid, is also proposed to speed-up the code. To make the model applicable to various land and ocean surfaces, a surface BRDF (Bidirectional Reflectance Distribution Function) library is embedded into the code. Considering the complimentary features of the MODIS and the POLDER, the collocated measurements of these two satellites are used in the retrieval process. To reduce the time spent on the simulation of dust aerosol scattering properties, a single-scattering property database of tri-axial ellipsoid is incorporated. In addition, atmospheric molecule correction is considered using the LBLRTM (Line-By-Line Ra- diative Transfer Model). The Levenberg-Marquardt method was employed to retrieve all the interested dust aerosol parameters and surface parameters simultaneously. As an example, dust aerosol properties retrieved over the Sahara Desert are presented.

A theoretical model describing the motion of a small, fast rare gas atom as it passes over a liquid surface is developed and discussed in detail. A key feature of the model is its reliance on coarse-grained capillary wave and local mode descriptions of the liquid surface. Mathematically, the model is constructed with several concepts from probability and stochastic analysis. The model makes predictions that are quantitative agreement with neon-liquid surface scattering data collected by other research groups. These predictions include the dominance of single, rather than multiple, neon-liquid surface collision dynamics, an average of 60 % energy transfer from a neon atom upon colliding with a non-metallic surface, and an average of 25 % energy transfer upon colliding with a metallic surface. In addition to this work, two other investigations into the gas-liquid interface are discussed. The results of an experimental investigation into the thermodynamics of a gas flux through an aqueous surface are presented, and it is shown that a nitrous oxide flux is mostly due to the presence of a temperature gradient in the gas-liquid interface. Evidence for a reaction between a carbon dioxide flux and an ammonia monolayer on an aqueous surface to produce ammonium carbamate is also found. The second of these is an investigation into the mechanism of bromine production from deliquesced sodium bromide aerosol in the presence of ozone, and involves a sensitivity and uncertainty analysis of the computer aerosol kinetics model MAGIC. It is shown that under dark, non-photolytic conditions, bromine production can be accounted for almost exclusively by a reaction between gas-phase ozone and surface-bound bromide ions. Under photolytic conditions, bromine production instead involves a complicated interplay between various gas-phase and aqueous-phase reactions.

Im Rahmen dieser Dissertation werden eine Serie von Grundlagenexperimenten zur Ablagerung (Deposition) und Remobilisierung (Resuspension) von Aerosolpartikeln in turbulenten Strömungen beschrieben. Die Kernmotivation stellt die Quelltermanalyse von Druckentlastungsstörfällen von Hochtemperaturreaktoren (HTR) dar. Im Primärkreislauf früherer HTR-Forschungsanlagen wurden größere Mengen an radiologisch belastetem Graphitstaub gefunden. Dieser Staub scheint größtenteils durch Abrieb zwischen den graphitischen Kernstrukturen entstanden zu sein und verteilte sich während des fortlaufenden Reaktorbetriebs über sämtliche Oberflächen des Primärkreislaufs. Während eines Druckentlastungsstörfalls kann dieser Staub durch die Gasströmung remobilisiert und aus dem Primärkreislauf ausgetragen werden. Eine Quelltermanalyse solch eines Störfallszenarios erfordert die Kenntnis über die Menge und die räumliche Verteilung des Staubs, die radiologische Belastung sowie das Remobilisierungsverhalten in Bezug auf die zu erwartenden Strömungstransienten. Nach dem heutigen Stand von Wissenschaft und Technik kann die räumlich-zeitliche Verteilung des Staubs im Primärkreislauf für stationären Reaktorbetrieb unter Verwendung eindimensionaler Systemcodes abgeschätzt werden. Jedoch ist unbekannt, welcher Anteil des Staubinventars durch die Gasströmung remobilisiert und aus dem Primärkreislauf ausgetragen werden würde. Zur systematischen Untersuchung des Staubtransportverhaltens in turbulenten Strömungen wurden zwei kleinskalige Versuchsanlagen entwickelt und eine Serie von Depositions- und Resuspensionsexperimenten durchgeführt. Die partikelbeladene Strömung in der Heißgasumgebung des HTR-Primärkreislaufs wurde über die Verwendung von Ähnlichkeitskennzahlen auf eine Luftströmung bei Umgebungsbedingungen herunterskaliert. Die Strömung und die Partikel wurden mittels hochauflösender, bildgebender und nichtinvasiver Messverfahren räumlich und zeitlich vermessen, um eine umfangreiche Datenbasis für die Analyse der Partikeltransportprozesse zu erstellen. Inhaltlich lassen sich die durchgeführten Untersuchungen in drei Teile gliedern. Der erste Teil besteht aus zwei Studien über die Deposition und Resuspension monodisperser, sphärischer Einzelpartikel in einer ungestörten, horizontalen Kanalströmung. Die systematische Variation experimenteller Randbedingungen wie der Partikelgröße, der Oberflächenrauheit und der Strömungsgeschwindigkeit ermöglichte die Quantifizierung der einzelnen Einflussgrößen. Im zweiten und dritten Teil der Dissertation wurden die Deposition und Resuspension einer mehrschichtigen Ablagerung (Partikel-Multilayer) zwischen periodischen Stufen und in einer Kugelschüttung untersucht, um die komplexe Interaktion zwischen der turbulenten Strömung und der Multilayer-Ablagerung weiter zu erforschen. Die gewonnenen Erkenntnisse leisten einen Beitrag für die Quelltermanalyse des Staubtransports im HTR-Primärkreislauf und können für die Weiterentwicklung numerischer Strömungssimulationen des Partikeltransports in turbulenten Strömungen verwendet werden. / Aerosol particle deposition and resuspension experiments in turbulent flows were performed to investigate the complex particle transport phenomena and to provide a database for the development and validation of computational fluid dynamics (CFD) codes. The background motivation is related to the source term analysis of an accidental depressurization scenario of a High Temperature Reactor (HTR). During the operation of former HTR pilot plants, larger amounts of radio-contaminated graphite dust were found in the primary circuit. This dust most likely arose due to abrasion between the graphitic core components and was deposited on the inner wall surfaces of the primary circuit. In case of an accident scenario, such as a depressurization of the primary circuit, the dust may be remobilized and may escape the system boundaries. The estimation of the source term being discharged during such a scenario requires fundamental knowledge of the particle deposition, the amount of contaminants per unit mass as well as the resuspension phenomena. Nowadays, the graphite dust distribution in the primary circuit of an HTR can be calculated for stationary conditions using one-dimensional reactor system codes. However, it is rather unknown which fraction of the graphite dust inventory may be remobilized during a depressurization of the HTR primary circuit. Two small-scale experimental facilities were designed and a set of experiments was performed to investigate particle transport, deposition and resuspension in turbulent flows. The facility design concept is based on the fluid dynamic downscaling of the helium pressure boundary in the HTR primary circuit to an airflow at ambient conditions in the laboratory. The turbulent flow and the particles were recorded by high-resolution, non-invasive imaging techniques to provide a spatio-temporal insight into the particle transport processes. The different investigations of this thesis can be grouped into three categories. Firstly, the deposition and resuspension of monodisperse single particles in a horizontal turbulent channel flow was studied. The systematic variation of the experimental boundary conditions allows for the quantification of the influences of particle size, surface roughness, and fluid velocity. In the second and third part of this thesis, the deposition and resuspension of a particle multilayer between periodic steps and in a pebble bed was studied to explore the complex interaction between the turbulent flow and the particles, respectively. The findings of this thesis are a contribution to the source term analysis of HTR related accidental depressurizations. Furthermore, the database can be applied to CFD code developments for the numerical simulation of particle transport processes in turbulent flows.

This thesis addresses a series of questions related to the problem of achieving reliable and physically consistent representations of aerosol-cloud interaction in global circulation models (GCM). In-situ data and modeling tools are used to develop and evaluate novel parameterization schemes for the process of aerosol activation for applications in GCM simulations. Atmospheric models of different complexity were utilized, ranging from detailed Lagrangian parcel model simulations of the condensational growth of droplets, to one-dimensional single column model with aerosol and cloud microphysics, and finally GCM simulations performed with the Community Atmosphere Model (CAM). A scheme for mapping the sub-grid scale variability of cloud droplet number concentrations (CDNC) to a number of microphysical process rates in a GCM was tested, finding that neglecting this impact can have substantial influences in the integrated cloud properties. A comprehensive comparison and evaluation of two widely used, physically-based activation parameterizations was performed in the framework of CAM5.1. This was achieved by utilizing a numerical adjoint sensitivity approach to comprehensively investigate their response under the wide range of aerosol and dynamical conditions encountered in GCM simulations. As a result of this, the specific variables responsible for the observed differences in the physical response across parameterizations are encountered, leading to further parameterization improvement.

Chemical composition of particles and rain water at three sites in Turkey were extensively compared to determine if there is a relationship between aerosol and rain composition. If such relationship exists, it can allow one to construct rain water composition using aerosol data. This is important because, rain composition data is scarce as sampling and analysis of very low concentrations of elements and ions in rain water is more difficult compared to sampling and analysis of atmospheric aerosol. Results showed that aerosol composition can be closely reflected in composition of rain water if below cloud processes dominate over the incloud processes. This is clearly observed for crustal elements in all stations and for most of the elements in urban Ankara station. However, in rural stations there were differences in rain and aerosol that is attributed to significant contribution from in cloud processes. Seasonal patterns and enrichment factors observed in aerosol composition showed general agreement with corresponding temporal variations observed in rain water concentrations of elements, but short term variations became visible only if data is averaged over a long period of time. These observations suggest that certain features of rain water composition can be constructed from if concentration data is available for aerosols. However it should be noted that there are also significant differences between stations and between elements or element groups, indicating that composition of rain water constructed from aerosol data can only be a crude one. Similarities between rain and aerosol compositions is more pronounced in urban Ankara station compared to rural stations used in this study. Factor analysis performed to aerosol and rain water data sets showed that source types affecting chemical composition of rain and particles are generally the same, bur contribution of each source type to rain and aerosol composition shows differences. Similarly, the source regions, defined by potential source contribution function, affecting aerosol and rain compositions are not identical. In Antalya station Source regions affecting chemical composition of rain water are more local compared to source regions affecting composition of aerosol. Same difference is not observed in Amasra station. Scavenging ratios is found to be a suitable tool to construct rain water composition using aerosol data. Scavenging ratios calculated using paired daily data are more variable both between stations and within a station. Long-term averaged data was found to be more reliable for calculating SRs of elements and ions at all stations.

Aerodynamically rough surfaces of forests provide for efficient air/ canopy exchange of mass, heat and momentum. In that context, the effects of forest edges come into focus, and therefore, coastal-zone forests constitute aparticular concern. Aerosol-sink modelling is of importance to the global-scalecontext, because sink strengths influence the concentration of aerosol particles in the atmosphere, and that concentration, in turn, influences climate. Dry deposition models are insufficient due to a lack of semi-empirical data and because of difficulties in parameterization of the efficiency (E) with which leaves capture aerosols. Quantifications of such parameters promote possibilities for modelling aerosol-sink processes within various canopy layers. This thesis focuses on studies of sea-salt aerosol dry deposition within models of oak canopies exposed to artificially generated aerosols in a wind tunnel. The overall goal is to advance the understanding of deposition processes in forest ecosystems. Aims are to determine capture efficiencies and deposition velocities (Vd) for oak (Quercus robur L.), to investigate E and Vd dependence on aerosol particle size, wind velocity and vegetation structural elements such as Leaf Area Index (LAI), to explore edge effects on deposition, to relate my results to natural situations in the field, and to address modelling applications. This thesis is a result of five studies. The first study is based on developing awind tunnel approach with a main focus on establishing reference conditions.The next step is to quantify E and provide estimates of how E, with respect toa well defined mass-vs-particle-size distribution, varies with wind speed. To that end, a special wash-off technique is developed. Finally, edge effects ondeposition processes are investigated. Results demonstrate that forest ecosystems would experience substantially increased deposition at edges. The findings suggest that field measurements of deposition in the interior of a forest “island” in an otherwise open landscape would underestimate the deposition to the entire forest. Results clearly indicate needs for further research on the effects of LAI on capture efficiency and deposition velocity. The obtained capture efficiencies can be translated into deposition velocities for trees with a specific leaf area. An increase of Vd with increasing wind speed is found, and is consistent with other studies. Results confirm advantages of the wind tunnel approach, including its ability to enable experiments under controlled conditions. However, several problems require that explicit sub-models be developed of wind-speed dependent effects on leaf posture in the aerosol flow field and that gradients in relative humidity close to leaf surfaces need further attention. The results also propose needs for a range of further experimental investigations regarding aerosol deposition across the complete sea-to-land aerodynamic transition.

The role of aerosols and clouds is one of the largest sources of uncertainty in understanding climate change. The primary scientific goal of this thesis is to improve the understanding of cloud-aerosol interactions by applying inverse modeling using Markov Chain Monte Carlo (MCMC) simulation. Through a set of synthetic tests using a pseudo-adiabatic cloud parcel model, it is shown that a self adaptive MCMC algorithm can efficiently find the correct optimal values of meteorological and aerosol physiochemical parameters for a specified droplet size distribution and determine the global sensitivity of these parameters. For an updraft velocity of 0.3 m s-1, a shift towards an increase in the relative importance of chemistry compared to the accumulation mode number concentration is shown to exist somewhere between marine (~75 cm-3) and rural continental (~450 cm-3) aerosol regimes. Examination of in-situ measurements from the Marine Stratus/Stratocumulus Experiment (MASE II) shows that for air masses with higher number concentrations of accumulation mode (Dp = 60-120 nm) particles (~450 cm-3), an accurate simulation of the measured droplet size distribution requires an accurate representation of the particle chemistry. The chemistry is relatively more important than the accumulation mode particle number concentration, and similar in importance to the particle mean radius. This result is somewhat at odds with current theory that suggests chemistry can be ignored in all except for the most polluted environments. Under anthropogenic influence, we must consider particle chemistry also in marine environments that may be deemed relatively clean. The MCMC algorithm can successfully reproduce the observed marine stratocumulus droplet size distributions. However, optimising towards the broadness of the measured droplet size distribution resulted in a discrepancy between the updraft velocity, and mean radius/geometric standard deviation of the accumulation mode. This suggests that we are missing a dynamical process in the pseudo-adiabatic cloud parcel model. / At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Submitted. Paper 4: Manuscript.

Dans ce travail de thèse, des méthodes de simulation numérique ont été utilisées afin de modéliser, à l’échelle moléculaire,l’interaction entre des aérosols carbonés et diverses molécules de l’atmosphère.L’objectif était de caractériser les propriétés physico-chimiques de ces aérosols, qui jouent un rôle majeur dans le climat, en particulier via leur capacité à former des noyaux de condensation pour les molécules d’eau. En premier lieu, les techniques de la dynamique moléculaire ont été appliquées à la détermination de l’organisation d’agrégats d’acide carboxylique sur lesquels sont adsorbées des molécules d’eau. Les résultats montrent une influence à la fois de la température, du taux d’humidité et du type d’acide considéré sur le comportement global des agrégats. Par contre, il a été montré qu’un mélange binaire d’acides n’a que peu d’influence sur ce comportement. En second lieu, des techniques de simulation moléculaires quantiques, à la fois statiques et dynamiques, ont été appliquées à l’étude de la chloration de surfaces de suie, modélisées par de grands HAP, ainsi qu’à la caractérisation de leur affinité pour les molécules d’eau. Les résultats ont montré une forte propension de Cl, Cl2 et HCl à former des HAP chlorés à la faveur de la présence de défauts structurels. Ces structures chlorées présentent une forte hydrophilicité, ce qui pourrait expliquer la nature fortement hygroscopique de suies émises lors d’incendies industriels. / In this PhD work, molecular simulation methods have been used in order to model, at the molecular scale, the interaction between carbonaceous aerosols andvarious atmospheric species. The aim wasto characterize the physico-chemical properties of these aerosols, which play a major role in climate forcing, in particular through their ability to act as cloud condensation nuclei.First, molecular dynamics techniques have been applied to determine the structure of carboxylic acid aggregates on which water molecules are adsorbed. The results of our simulations show an influence of the temperature, of the humidity and of the type of carboxylic acid considered on the global behavior of the aggregates. By contrast,a mixture of different types of acid molecules has no influence on this behavior. Secondly, quantum molecular simulation techniques have been applied to study the chlorination of soot surfaces, modeled by large PAHs, and their behavior with respect to water molecules adsorption. The results show a strong propensity of Cl, Cl2and HCl species to form chlorinated PAHsthanks to the presence of structural defects.These chlorinated structures show as trong hydrophilicity, which may explain the strong hygroscopic nature of soots emitted by industrial fires.

La mucoviscidose est une maladie héréditaire monogénique grave en rapport avec une mutation du gène codant pour la protéine CFTR et dont la morbidité est due principalement aux atteintes pulmonaires. La greffe pulmonaire développée depuis quelques années semble être la seule thérapie curative efficace. Toutefois, la rareté des greffons disponibles, justifie de développer d’autres thérapies comme la thérapie génique. Les pseudovirions de papillomavirus sont capables de transférer des gènes dans de nombreuses lignées cellulaires. Cependant, le tropisme naturel des papillomavirus est l’épithélium malpighien et ces pseudovirions sont peu efficaces pour les cellules de l’épithélium pulmonaire. Afin de modifier le tropisme de nos pseudocapsides de papillomavirus, la première étape de mon travail a été d’identifier de nouveaux motifs de ciblage pulmonaire. La technique de phage display a permis l’identification des motifs PHPNRAQ et VDRLQQK par sélection sur les cellules épithéliales bronchique IB3-1 et S9. / Cystic fibrosis is an autosomal recessive genetic disorder caused by mutations in the gene encoding the cystic fibrosis transmembrane conductance regulator (CFTR) protein. Lung transplantation developed in recent years is the only effective curative treatment. However, due to the limitation in organ donors, it is necessary to develop other therapies such as gene therapy. Papillomavirus pseudovirions have the potential to deliver genes into different cells. However, the natural tropism of HPV is directed to the cervical epithelial cells and these pseudovirions have low transduction efficacy in pulmonary epithelial cells. The purpose of this thesis was to retarget and optimize the HPV-16 pseudovirions tropism to airway cells by insertion of short amino acid sequences within the major capsid protein L1.