The development and application of new cloud retrieval methods from ground–based and airborne measurements of spectral radiance fields above heteorogeneous surfaces is introduced. The potential of imaging spectrometers in remote–sensing applications is evaluated. The analyzed spectral radiance fields were measured during two international field campaigns in the visible wavelength range (400–970 nm) with high spatial (<10m) resolution. From ground–based measurements, high ice clouds were observed and from airborne measurements Arctic stratus. From the measurements, cloud optical thickness is retrieved with high spatial resolution and the horizontal cloud inhomogeneities are investigated. Depending on the measurement configuration, different uncertainties arise for the retrieval of the cloud optical thickness. A reduction of those uncertainties is derived by a specification of the ice crystal shape to improve the retrieval of the optical thickness of high ice clouds. The ice crystal shape is obtained independently from the angular information of the scattering phase function features, imprinted in the radiance fields. A performed sensitivity study reveals uncertainties of up to 90%, when neglecting this information and applying a wrong crystal shape to the retrieval. For remote-sensing of Arctic stratus, the highly variable surface albedo influences the accuracy of the cloud optical thickness retrieval. In cloudy cases the transition of reflected radiance from open water to sea ice is not instantaneous but horizontally smoothed. In general, clouds reduce the reflected radiance above bright surfaces in the vicinity of open water, while it is enhanced above open sea. This results in an overestimation of to up to 90% in retrievals of the optical thickness. This effect is investigated. Using observations and three-dimensional radiative transfer simulations, this effect is quantified to range to up to 2200 m distance to the sea-ice edge (for dark-ocean albedo of αwater = 0.042 and sea-ice albedo of αice = 0.91 at 645 nm wavelength) and to depend on macrophysical cloud and sea-ice properties. The retrieved fields of cloud optical thickness are statistically investigated. Auto–correlation functions and power spectral density analysis reveal that in case of clouds with prevailing directional cloud structures, cloud inhomogeneities cannot be described by a universally valid parameter. They have to be defined along and across the prevailing cloud structures to avoid uncertainties up to 85%. / Im folgenden wird die Entwicklung und Anwendung neuer Ableitungsverfahren von Wolkenparametern, basierend auf bodengebundener und flugzeuggetragener spektraler Strahldichtemessungen über heterogenen Untergründen, vorgestellt und das Fernerkundungspotential abbildender Spektrometer evaluiert. Die spektralen Strahldichtefelder wurden während zweier internationaler Feldkampagnen im sichtbaren Wellenlängenbereich (400–970 nm) mit hoher räumlich Auflösung (<10m) gemessen. Bodengebundene Messungen wurden genutzt, um hohe Eiswolken zu beobachten und flugzeuggetragenen um arktischen Stratus zu beobachten. Aus den Messungen werden räumlich hochaufgelöste wolkenoptische Dicken abgeleitet und anschließend horizontale Wolkeninhomogenitäten untersucht. Die Ableitung der wolkenoptischen Dicke birgt je nach Messkonfiguration verschiedene Unsicherheiten. Eine Reduzierung der Unsicherheiten wird durch die Vorgabe einer Eiskristallform zur Verbesserung der Ableitung der optischen Dicke hoher Eiswolken erreicht. Diese werden unabhängig aus den winkelabhängigen, in das gemessene Strahldichtefeld eingeprägten Eigenschaften der Streuphasenfunktion, abgeleitet. Bei Vernachlässigung dieser Information und Wahl der falschen Eiskristallform, treten Fehler in der abgeleiteten optischen Dicke von bis zu 90% auf. Bei der Fernerkundung von arktischem Stratus beeinflusst die sehr variable Bodenalbedo die Genauigkeit der Ableitung der optischen Dicke. Beim Übergang von Meereis zu Wasser, findet die Abnahme der reflektierten Strahldichte im bewölktem Fall nicht direkt über der Eiskante, sondern horizontal geglättet statt. Allgemein reduzieren Wolken die reflektierte Strahldichte über Eisflächen nahe Wasser, während sie über dem Wasser erhöht wird. Dies führt zur Überschätzung der wolkenoptischen Dicke über Wasserflächen nahe Eiskanten von bis zu 90 %. Dieser Effekt wird mit Hilfe von Beobachtungen und dreidimensionalen Strahlungstransferrechnungen untersucht und es wird gezeigt, dass sein Einfluss noch bis zu 2200 m Entfernung zur Eiskante wirkt (für Meeresalbedo 0.042 und Meereisalbedo 0.91 bei 645 nm Wellenlänge) und von den makrophysikalischen Wolken- und Meereiseigenschaften abhängt. Die abgeleiteten Felder der optischen Dicke werden statistisch ausgewertet, um die Inhomogeneität der Wolken zu charakterisieren. Autokorrelationsfunktionen und Leistungsdichtespektren zeigen, dass Inhomogenitäten von Wolken mit vorranging richtungsabhängiger Struktur nicht mit einem allgemeingültigen Parameter beschrieben werden können. Es sind Inhomogenitätsmaße entlang und entgegen der jeweiligen Wolkenstrukturen nötig, um Fehler von bis zu 85% zu vermeiden.

Das Afterglow tritt am Übergang vom Plasma zur Gasphase auf. Die dominierende aktive Spezies im Afterglow sind metastabil angeregte Neutralteilchen. Der Abbau der Metastabilen erfolgt in drei verschiedenen Prozessen: dem radiativen Zerfall, den Quenching-Stößen sowie der Relaxation in Stößen mit Oberflächen. Potentielle Anwendungsmöglichkeiten des Afterglows für Schichtabscheidung und Oberflächenmodifizierung werden diskutiert. Zur theoretischen Beschreibung des strömenden Afterglows wurde ein Collisional Radiative Modell entwickelt, welches die Reflexion angeregter Spezies an Oberflächen berücksichtigt. Als Diagnostikmethoden wurden die optische Emissionsspektroskopie (OES), die Chemolumineszenz sowie die Langmuir-Sondenmessungen eingesetzt, um die Konzentration metastabil angeregter Spezies zu bestimmen. Es wurde der Einfluß von konstruktiven und äußeren Paramentern auf die Konzentration metastabil angeregter Spezies im Afterglow untersucht. Es zeigt sich, daß unter den gegebenen Bedingungen die Quenching-Stöße der dominierende Verlustprozeß im Afterglow sind. Die Parameter Druck, Strömungsgeschwindigkeit und Länge des Afterglows können zu einem Skalierungsparameter zusammengefaßt werden, der zur online-Prozeßregulierung verwendet werden kann. Es werden

Using ion-trapping techniques, selected laboratory experiments on ion-molecule reactions of astrophysical interest have been performed. For the first time a carbon beam source has been integrated into an ion trapping machine for studying collisions between ions and neutral carbon atoms and molecules. Results are presented for the interaction of D3+ ions stored in a ring-electrode trap (RET), with a beam of hot neutral carbon molecules, Cn (n = 1, 2, 3). The measured reaction rate coefficients are up to a factor two smaller than values presently used in astrophysical models. In order to complete our knowledge about the ion chemistry involving three carbon atoms, detailed investigations of reactions of C3+, C3H+ and C3H3+ with H2 and HD have been performed between 15 K and room temperature. These studies have been performed in a second apparatus, a variable-temperature 22-pole trap machine (VT-22PT). Results include reactive collisions, deuteration and radiative association. It is discussed in connection with the increase in lifetime of the C3+ + H2 collision complexes with falling temperature, what could be responsible for producing more C3H+ at 15 K. Tunneling is excluded. In C3+ + HD collisions an isotope effect has been detected, the C3D+ product ions being slightly more abundant than C3H+. Comparison of the reaction of C3H+ primary ions with HD and H2 gas revealed that the deuterated molecules are significantly more reactive. The process of radiative association of C3H+ and for the first time of C3+ with hydrogen molecules has been observed. An analysis of the data shows that radiative association becomes slower, if the neutral reactant is deuterated. Finally, the theoretical prediction from ab initio calculations that C3H3+ does not exchange an H for a D in collisions with HD, has been proven in an ion trap experiment. Careful analysis of all competing processes allows the conclusion that the rate coefficient is smaller than 4x10-16 cm3s-1 at 15 K. / Unter Verwendung von zwei Speicherapparaturen wurden ausgewählte, astrophysikalische wichtige Ionen-Molekülreaktionen untersucht. Durch die Kombination einer Kohlenstoffquelle mit einem Ionenspeicher, in dem so Reaktionen zwischen Ionen und Kohlenstoffmolekülen oder -atomen untersucht werden können, wurde Neuland betreten. Es werden Ergebnisse vorgestellt für die Reaktion von D3+ Ionen, die in einem Ringelektrodenspeicher gefangen sind, mit einem Strahl von heißen Cn (n = 1, 2, 3). Die gemessenen Ratenkoeffizienten sind nur halb so groß wie die Werte, die in astrophysikalischen Modellen verwendet werden. Um die Kenntnis über alle möglichen Reaktionen, bei denen drei C-Atome beteiligt sind, abzurunden, wurden zwischen 15 K und Zimmertemperatur die Reaktionen zwischen C3+, C3H+ und C3H3+ Ionen mit H2 und HD in vielen Details untersucht. Diese Experimente wurden in einer zweiten Apparatur durchgeführt, in der ein temperaturvariabler 22-Polspeicher das zentrale Element ist (VT-22PT). Berichtet werden Ergebnisse zu reaktiven Stößen, zur Deuterierung von Kohlenwasserstoffen und zur Strahlungsassoziation. In der Diskussion bleibt offen, was - in Verbindung mit der von 300 K zu 15 K zunehmenden Lebensdauer - der Grund dafür sein kann, daß die Bildung des exothermen Produkts C3H+ anwächst. Der Tunneleffekt scheidet aus. Bei der Reaktion C3+ + HD wurde ein Isotopeneffekt beobachtet, das C3D+ Produkt wird etwas häufiger gebildet als C3H+. Ein Vergleich der Reaktion zwischen C3H+ Ionen mit HD bzw. H2 zeigt, daß das deuterierte Molekül wesentlich reaktiver ist. Es wurden Ratenkoeffizienten für die Strahlungsassoziation von H2 Molekülen mit C3H+ und erstmals mit C3+ Ionen gemessen. Die Auswertung der Daten zeigt, dass der Prozeß langsamer abläuft, wenn der neutrale Stoßpartner deuteriert ist. Schließlich wurde experimentell die theoretische Vorhersage überprüft, dass C3H3+ keinen H-D Austausch mit HD eingeht. Eine sorgfältige Analyse aller konkurrierenden Prozesse ergab, dass bei 15 K der Raten koeffizient kleiner als 4x10-16 cm3s-1 ist.

Title: Some aspects of low-energy QCD at the precision frontier Author: Tomáš Husek Department/Institute: Institute of Particle and Nuclear Physics Supervisor of the doctoral thesis: doc. RNDr. Karol Kampf, Ph.D. Abstract: This thesis concentrates on some low-energy aspects of QCD, namely on those which are connected to the electromagnetic decays of lightest neutral pseudoscalar mesons. Calculations of radiative corrections to neutral pion decays (the Dalitz decay and the rare decay) and a novel model for the pion electro- magnetic transition form factor are subjects discussed in the attached papers, which this work is based on. The associated theoretical aspects including Chiral Perturbation Theory or the large-Nc limit are introduced. We also discuss the complications which arise when the calculations of radiative corrections for η(′) Dalitz decays are performed. Some details about the collaboration with experi- ments which incorporate the calculation of the published corrections are provided. Last but not least, some techniques related to loop integrals are shown. Keywords: Chiral Perturbation Theory, large-Nc limit, radiative corrections, pion electromagnetic transition form factor 1

Persistent condensation trails are clouds, induced by the exhaust of an aircraft engine in a cold and ice-supersaturated environment. These artificial ice clouds can both cool and heat the atmosphere by scattering solar radiation and absorbing terrestrial radiation, respectively. The influence of condensation trails on the Earth-atmosphere energy balance and therewith the answer to the question of the dominating process had been mostly approximated on a global scale by treating the condensation trail as plane parallel layer with constant optical properties. Individual condensation trails and the influence of the solar angle had been analyzed, always using a course spatial grid and never under consideration of the aircraft performance, generating the condensation trail. For a trajectory optimization, highly precise results of the impact of condensation trails on the radiation budget and the influence of the aircraft performance on this impact is needed, so that future air traffic may consider the main factors of flight performance on the environmental impact of condensation trails. That’s why, a model is developed in this thesis to continuously estimate the scattering and absorption properties and their dependence on the aircraft performance.:1 Introduction 3 1.1 Motivation 3 1.2 State of the art 5 1.3 Approach 6 2 Theoretical background 9 2.1 The Earth’s atmosphere 9 2.1.1 The mean vertical structure of the atmosphere 12 2.1.2 Standard atmospheres 14 2.2 Radiation 15 2.2.1 Nature of radiation 15 2.2.2 Important metrics describing radiation 17 2.2.3 Relevant spectra and principles of radiation 19 2.2.4 Solar radiation 20 2.2.5 Terrestrial radiation 21 2.2.6 Radiative transfer and extinction 22 2.2.7 Radiative transfer equation 30 2.2.8 Energy budget of the Earth-atmosphere system 32 2.3 Thermodynamics 33 2.3.1 Atmospheric stability 33 2.3.2 Turbulence 36 2.3.3 Conditions of contrail formation 41 3 Development of a radiative forcing model 45 3.1 Model atmosphere 45 3.2 Flight performance model 46 3.3 Atmospheric radiative transfer model 49 3.3.1 Two Stream Approximation 51 3.3.2 Discrete ordinate radiative transfer solver 52 3.3.3 Methods to calculate broadband radiances and irradiances 53 3.4 Contrail life cycle model 57 3.4.1 Dissipation regime 58 3.4.2 Diffusion regime 63 3.5 Contrail radiative forcing model 74 3.5.1 Consideration of multiple scattering using a Monte Carlo simulation 74 3.5.2 Geometry of the Monte Carlo simulation 75 3.5.3 Interpretation of Beer’s law 76 3.5.4 Procedure of the Monte Carlo simulation 79 3.5.5 The extinguished power per unit length contrail 87 3.5.6 Scattering and absorption efficiencies Qs, Qa and asymmetry parameters gHG 89 3.5.7 Calibration of the Monte Carlo simulation 94 4 Calculations 99 4.1 Contrail properties 99 4.1.1 Conditions of contrail formation 100 4.1.2 Initial dimensions at the end of the dissipation regime 101 4.1.3 Microphysical properties during the diffusion regime 103 4.2 Radiative transport up to the contrail 105 4.2.1 Solar direct and diffuse radiance 106 4.2.2 Terrestrial irradiance 107 4.3 Scattering and absorption properties of radiation within the contrail 109 4.3.1 Monte Carlo simulation for solar radiation 109 4.3.2 Monte Carlo simulation for terrestrial irradiances 112 4.3.3 Relevance of multiple scattering 116 4.4 Radiative extinction 116 4.4.1 Solar zenith and azimuthal angle 118 4.4.2 Flightpath 120 4.4.3 Contrail evolution 122 4.4.4 Turbulence 126 4.4.5 Wavelength specific extinction 129 4.5 Terrestrial energy forcing of a contrail 133 4.6 Verification 135 5 Conclusion and outlook 141 5.1 Conclusion 141 5.2 Outlook 144 List of Figures 147 List of Tables 151 Abbreviations and Symbols 153 Glossary 161 Bibliography 169 Acknowledgements 183 / Langlebige Kondensstreifen sind Eiswolken, welche durch Kondensation von Wasserdampf an Rußpartikeln in einer eisübersättigten Atmosphäre entstehen. Der Wasserdampf entstammt einerseits aus dem Triebwerkabgas und andererseits aus der Atmosphäre. Kondensstreifen können die Atmosphäre durch Rückstreuung solarer Strahlung kühlen und durch Rückstreuung und Absorption terrestrischer Strahlung erwärmen. Der Einfluss von Kondensstreifen auf den Wärmehaushalt der Atmosphäre und damit die Antwort auf die Frage nach dem dominierenden Effekt wurde bisher zumeist auf globaler Ebene ermittelt, wobei der Kondensstreifen als planparallele Schicht mit konstanten optischen Eigenschaften angenähert wurde. Individuelle Kondensstreifen und der Einfluss des Sonnenstandes wurden bisher nur mithilfe eines groben Rasters betrachtet und niemals unter Berücksichtigung der Flugleistung des Luftfahrzeuges, welches den Kondensstreifen generiert hat. Für eine Trajektorienoptimierung sind jedoch präzise Berechnungen des Strahlungseinflusses und eine gewissenhafte Berücksichtigung der Flugleistung notwendig. Nur so kann der zukünftige Luftverkehr die Haupteinflussfaktoren der Flugeigenschaften auf den Strahlungseinfluss der Kondensstreifen berücksichtigen. Aus diesem Grund wurde in dieser Arbeit ein Modell entwickelt, welches die Eigenschaften des Strahlungstransfers durch den Kondensstreifen kontinuierlich bestimmt und die aus der Flugleistung resultierenden Parameter berücksichtigt.:1 Introduction 3 1.1 Motivation 3 1.2 State of the art 5 1.3 Approach 6 2 Theoretical background 9 2.1 The Earth’s atmosphere 9 2.1.1 The mean vertical structure of the atmosphere 12 2.1.2 Standard atmospheres 14 2.2 Radiation 15 2.2.1 Nature of radiation 15 2.2.2 Important metrics describing radiation 17 2.2.3 Relevant spectra and principles of radiation 19 2.2.4 Solar radiation 20 2.2.5 Terrestrial radiation 21 2.2.6 Radiative transfer and extinction 22 2.2.7 Radiative transfer equation 30 2.2.8 Energy budget of the Earth-atmosphere system 32 2.3 Thermodynamics 33 2.3.1 Atmospheric stability 33 2.3.2 Turbulence 36 2.3.3 Conditions of contrail formation 41 3 Development of a radiative forcing model 45 3.1 Model atmosphere 45 3.2 Flight performance model 46 3.3 Atmospheric radiative transfer model 49 3.3.1 Two Stream Approximation 51 3.3.2 Discrete ordinate radiative transfer solver 52 3.3.3 Methods to calculate broadband radiances and irradiances 53 3.4 Contrail life cycle model 57 3.4.1 Dissipation regime 58 3.4.2 Diffusion regime 63 3.5 Contrail radiative forcing model 74 3.5.1 Consideration of multiple scattering using a Monte Carlo simulation 74 3.5.2 Geometry of the Monte Carlo simulation 75 3.5.3 Interpretation of Beer’s law 76 3.5.4 Procedure of the Monte Carlo simulation 79 3.5.5 The extinguished power per unit length contrail 87 3.5.6 Scattering and absorption efficiencies Qs, Qa and asymmetry parameters gHG 89 3.5.7 Calibration of the Monte Carlo simulation 94 4 Calculations 99 4.1 Contrail properties 99 4.1.1 Conditions of contrail formation 100 4.1.2 Initial dimensions at the end of the dissipation regime 101 4.1.3 Microphysical properties during the diffusion regime 103 4.2 Radiative transport up to the contrail 105 4.2.1 Solar direct and diffuse radiance 106 4.2.2 Terrestrial irradiance 107 4.3 Scattering and absorption properties of radiation within the contrail 109 4.3.1 Monte Carlo simulation for solar radiation 109 4.3.2 Monte Carlo simulation for terrestrial irradiances 112 4.3.3 Relevance of multiple scattering 116 4.4 Radiative extinction 116 4.4.1 Solar zenith and azimuthal angle 118 4.4.2 Flightpath 120 4.4.3 Contrail evolution 122 4.4.4 Turbulence 126 4.4.5 Wavelength specific extinction 129 4.5 Terrestrial energy forcing of a contrail 133 4.6 Verification 135 5 Conclusion and outlook 141 5.1 Conclusion 141 5.2 Outlook 144 List of Figures 147 List of Tables 151 Abbreviations and Symbols 153 Glossary 161 Bibliography 169 Acknowledgements 183

Tropical forests, which provide important ecosystem functions and services, are increasingly threatened by anthropogenic pressures. This has resulted in an urgent need to understand tree species diversity of those forests. Where knowledge of that diversity is largely from the botanical surveys and local ecological studies, data must inevitably be up-scaled from point observations to the landscape and regional level if a holistic perspective is required. This thesis explores aspects of the spatio-temporal heterogeneity of canopy reflectance patterns over the forests of French Guiana, in order to assess whether this information could help defining an ecologically consistent forest typology. To gain insight into both the spatial and temporal heterogeneity of French Guiana’s forests, instrumental artefacts affecting the satellite data first had to be addressed. Data used in this study represent the spectral response of forest canopies, and the way in which such data are captured makes them susceptible to the ‘bi-directional reflectance distribution function’ (BRDF). BRDF indicates that objects do not reflect light in equal proportions in all directions (isotropically). Thus, forest canopies will reflect light anisotropically depending on factors including canopy roughness, leaf optical properties and inclination, and the position of the sun relative to the sensor. The second chapter of this thesis examines how BRDF affects the canopy reflectance of forests in French Guiana, and how not correcting for BRDF affects spectral classifications of those forests. When monthly reflectance data corrected for the artefact are examined, these suggest seasonally-occurring changes in forest structure or spectral properties of French Guiana’s forests. The third chapter of this thesis thus examines temporal effects of BRDF, and used cross-regional comparisons and plot-level radiative transfer modelling to seek to understand the drivers of the monthly variation of the forests’ canopy reflectance. For the latter, the Discrete Anisotropic Radiative Transfer (DART) model was used along with aerial laser scanning (ALS) observations over different forest structures, indicating that the observed variation in reflectance (and derivatives known as vegetation indices) could not be explained by monthly variations in solar direction. At the regional scale, it was also demonstrated that forests in the Guiana Shield possess temporal variation distinct from forests in central Africa or northern Borneo, forests also lying just above the Equator. Had the observed temporal variation in vegetation indices been the result of BRDF, it would have been expected that the forests in the three zones would have similar patterns of variation, which they did not. Central African forests appear to have their greening synchronized with rainfall, whereas forests in the Guianas appear synchronized with the availability of solar radiation. Further analysis of the vegetation index time-series of observations also indicated that different types of forests in French Guiana possess distinct patterns of temporal variation, suggesting that tropical forest types can be discriminated on the basis of their respective “temporal signatures.” That was exploited in the fourth chapter of the thesis, which maps forests in French Guiana based on their combined spatio-temporal canopy reflectance patterns and by so doing presents a novel way of addressing forest typology, based on ecologically meaningful information. The thesis presented demonstrates that it is possible to adequately address remote sensing data artefacts to examine patterns of spatial and temporal variation in tropical forests. It has shown that phenological patterns of tropical rainforests can be deduced from remote sensing data, and that forest types can be mapped based on spatio-temporal canopy reflectance patterns. It is thus an important contribution to understand the ecology of tropical forests in French Guiana and to improve the toolbox of scientists dealing with the identification of spatio-temporal patterns observable in forests at the landscape level.

L’étude du problème de la diffusion d’une onde électromagnétique par une suspension de particules non sphériques est une difficulté récurrente dans de nombreux domaines de la recherche et de l’ingénierie. Cela implique d’utiliser des dispositifs expérimentaux hautement spécialisés ou de résoudre les équations de Maxwell, ce qui représente un véritable défi lorsque les particules sont de géométries complexes et avec des distributions statistiques de taille, d’orientation et de forme. L’objectif de la présente thèse est d’explorer l’utilisation de la méthode de Monte Carlo pour résoudre des formulations intégrales du champ électromagnétique diffusé déduites des équations de Maxwell. En particulier, nous résolvons celles de l’approximation de Schiff, de l’approximation de Born ainsi que celle du développement en série de Born. Notre approche est basée sur un travail de reformulation intégrale permettant de concevoir des algorithmes incluant les avancées les plus récentes de la méthode. Cette approche originale, utilisant les outils de la synthèse d’image pour gérer n’importe quelle géométrie, permet de traiter des statistiques de particules ainsi que d’évaluer les sensibilités à des paramètres d’intérêts, sans augmentation significative du temps de calcul. Les outils développés répondent d’ores et déjà aux besoins d’optimisation des photobioréacteurs qui mettent en œuvre des particules à faible contraste d’indice (micro-algues). À l’issue de ce travail, des pistes de recherches ont émergé pour explorer le verrou bien identifié des grandes particules et des forts contrastes d’indice à partir du principe de zéro-variance. / The resolution of the problem of an electromagnetic wave scattered by non-spherical particles suspensions is a significant difficulty encountered in many fields of research and engineering. This implies to use highly specialized experiments or to solve Maxwell’s equations, which is a real challenge when weconsider particles with complex shapes and with statistical distributions of size, orientation and shape.The aim of this thesis is to investigate the use of the Monte Carlo method in order to solve the integral formulations of electromagnetic scattering deduced from Maxwell’s equations. In particular, we solvethose of Schiff’s approximation, Born’s approximation as well as the Born series expansion. Our approachis based on integral reformulation in order to design algorithms including the most recent advances of the method. This original approach, using computer graphics algorithms in order to manage arbitraryshape, permits treating any distributions of parameters as well as evaluating sensitivities to parameters ofinterest, without additionnal CPU time. The developed tools already meet the needs for the optimisation of photobioreactors which bring into play soft particles (micro-algae). From this work, some researchideas have emerged to explore the well-identified issue of large particles and large refractive indices from zero-variance principle.

En physique du transport, en particulier en physique du transfert radiatif, la méthode de Monte-Carlo a été développée à l'origine comme la simulation de l'histoire d'un grand nombre de particules, dont on déduit des observables moyennes. Cette méthode numérique doit son succès à plusieurs qualités : une gestion naturelle des espaces des phases aux nombreuses dimensions, une erreur systématique nulle par rapport au modèle physico-mathématique, les intervalles de confiance donnés avec les résultats, une capacité à prendre en compte simultanément de nombreux phénomènes physiques, la possibilité de calcul de sensibilités simultané, et une parallélisation aisée. En cinétique des gaz, les particules collisionnent entre elles et non pas avec un milieu extérieur ; on dit que leur transport est non-linéaire. Ces collisions mutuelles mettent en défaut l'approche évoquée ci-dessus de la méthode de Monte-Carlo ; car pour simuler des trajectoires indépendantes de multiples particules et ainsi estimer leur distribution, il faut connaître au préalable exactement cette même distribution...Cette thèse fait suite à celles de Jérémi DAUCHET (2012) et de Mathieu GALTIER (2014), consacrées au transfert radiatif. Entre autres travaux, ces auteurs montraient comment la méthode de Monte-Carlo peut s'accommoder de non-linéarités, en gardant son formalisme et ses spécificités habituelles. Les non-linéarités alors franchies étaient respectivement une loi de couplage chimie/luminance, et la dépendance de la luminance envers le coefficient d'absorption. On essaie dans ce manuscrit d'outrepasser la non-linéarité du transport. Pour cela, nos principaux outils sont un suivi des particules en remontant le temps, basé sur des formulations intégrales des équations de transport, formulations largement inspirées des algorithmes dits à collisions nulles. Nous montrons, sur plusieurs exemples académiques, que nous avons en effet étendu la méthode de Monte-Carlo à la résolution de l'équation de Boltzmann. Ces exemples sont aussi l'occasion de tester les limites de ce que nous avons mis en place. Les résultats les plus marquants sont certainement l'absence totale de maillage dans la méthode numérique, ainsi que sa capacité à calculer correctement les quantités de particules de haute énergie cinétique (toujours peu nombreuses par rapport au total, en cinétique des gaz). Au-delà des exemples fournis, ce manuscrit est voulu comme un essai de formalisme et une exploration des bases de la méthode développée. L'accent est mis sur les raisonnements menant à la mise au point de la méthode, plutôt que sur les implémentations particulières qui ont été abouties. La méthode est encore, aux yeux de l'auteur, largement susceptible d'être retravaillée. En particulier, les temps maximaux sur lesquels l'évolution des particules est calculable, qui constituent la faiblesse principale de la méthode numérique développée, peuvent sûrement être augmentés. / In transport physics, especially in radiative transfer physics, the Monte-Carlo method has been originally developed as the simulation of the history of numerous particles, from which are deduced mean observables. This numerical method owes its success to several qualities : a natural management of many-dimensional phase space, a null systematic error away from the mathematical and physical model, the confidence intervals given with the results, an ability to take into account simultaneously numerous physical phenomenons, the simultaneous sensitivities calculating possibility, and an easy parallelization. In gas kinetics, particles collide each other, not with an external fixed medium ; it is said that their transport is non-linear. These mutual collisions put out of action the aforesaid approach of the Monte-Carlo method ; because in order to simulate the independent trajectories of multiple particles and thus estimate their distribution, this distribution must beforehand be exactly known...This thesis follows on from those of Jérémy DAUCHET (2012) and of Mathieu GALTIER (2014), dedicated to radiative transfer physics. Between other works, these authors have shown how the Monte-Carlo method can bear non-linearities, while keeping its customary formalism and specificities. The then overcome non-linearities were respectively a chemistry/irradiance coupling law, and the dependence of the irradiance toward the absorption coefficient. We try in this manuscript to overcome the non-linearity of the transport. In this aim, our main tools are a reverse following of particles, based on integral formulations of the transport equations, formulations largely inspired from the so-called null collisions algorithms. We show, on several academic examples, that we have indeed extended the Monte Carlo method to the resolution of the Boltzmann equation. These examples are also occasions to test the limits of what we have built. The most noteworthy results are certainly the absence of any mesh in the numerical method, and its capacity to calculate correctly the high-speed particles quantities (always rare compared to the total, in gas kinetics). Beyond the given examples, this manuscript is wanted as a formalism attempt and an exploration of the developed method basics. The focus is made on the reasoning leading to the method, rather than on particular implementations which have been realized. In the eyes of the author, the method is still largely reworkable. In particular, the maximal times on which the evolution of particles is computable, which constitute the main weakness of the developed numerical method, can surely be increased.

The K-distribution method is a fast approximative method used for calculating thermal infrared radiative transfer in the atmosphere, as opposed to the traditional Line-by-line method, which is precise, but very time-costly. Here we consider the atmosphere to consist of homogeneous and plane-parallel layers in local thermal equilibrium. This lets us use efficient upwards recursion for calculating the thermal infrared radiative transfer and ultimately the outgoing irradiance at the top of the atmosphere. Our specific implementation of the K-distribution method revolves around changing the integration space from the wavenumber domain to the g domain by employing Gauss-Legendre quadrature in two steps. The method is implemented in MATLAB and is shown to be several thousand times faster than the traditional Line-by-line method, with the relative error being only 3 % for the outgoing irradiance at the top of the atmosphere.

Soot particles are a major absorber of shortwave radiation in the atmosphere. They exert a rather uncertain direct and semi-direct radiative effect, which causes a heating or in some cases a cooling of the atmosphere. The mass absorption coefficient is an essential quantity to describe this light absorption process. This work presents new experimental data on the mass absorption coefficient of soot particles in the troposphere over Central Europe. Mass absorption coefficients were derived as the ratio between the light absorption coefficient determined by multi angle absorption photometry (MAAP), and the soot mass concentration determined by Raman spectroscopy. The Raman method is sensitive to graphitic structures present in the particle samples, and was calibrated in the laboratory using Printex90 model particles. The mass absorption coefficients were determined for a number of seven observation sites, ranging between 3.9 and 7.4 m²/g depending on measurement site and observational period. The highest values were found in an continentally aged air mass in winter, where we presumed soot particles to be present mainly in internal mixture. The regional model WRF-Chem was used in conjunction with a high resolution soot emission inventory to simulate soot mass concentrations and absorption coefficients for the Central European Troposphere. The model was validated using soot mass concentrations from Raman measurements and absorption coefficients. Simulated soot mass concentrations were found to be too low by around 50 %, which could be improved by scaling the emissions by a factor of two. In contrast, the absorption coefficient was positively biased by around 20%. Adjusting the modeled mass absorption coefficient to measurements, the simulation of soot light absorption was improved. Finally, the positive direct radiative forcing at top of the atmosphere was found to be lowered by up to 70% for the model run with adjusted soot absorption behaviour, , indicating a decreased heating effect on the atmosphere.