In this thesis a new three–dimensional (3D) vector radiative transfer model, the Solver for Polarized Atmospheric Radiative Transfer Applications (SPARTA) is introduced, validated against benchmark results, and applied to scientific problems. SPARTA employs the statistical forward Monte Carlo technique for efficient column–response pixel–based radiance calculations comprising polarization for 3D inhomogeneous cloudless and cloudy atmospheres. By means of SPARTA, two scientific issues in the field of radiative transfer are investigated. A sensitivity study has been conducted to illustrate the errors introduced by neglecting the effects of polarization in radiation simulations. Two atmospheric scenarios have been considered: a pure one–dimensional (1D) Rayleigh atmosphere and two–dimensional (2D) realistic inhomogeneous dust fields. In case of a purely molecular atmosphere, these errors strongly depend on molecular anisotropy, isotropic reflection, and more importantly, on single scattering albedo and optical thickness (saturation occurs for τ close to 1). Overall errors in the reflected field range up to about 10.5%. On the other hand, for rather high optical thickness, the bias induced by ignoring polarization for realistic inhomogeneous atmospheres is negligible (less than 1%). In addition, solar radiative transfer simulations for LIDAR–measured fields of optical properties of Saharan dust have been performed in order to quantify the effects induced by neglecting the horizontal photon transport and internal inhomogeneities (3D radiative effects) in radiance simulations including polarization. Results are presented for two exemplary mineral dust fields constructed from LIDAR observations. For each case, three radiative calculations are investigated: a 1D calculation according to the plane–parallel (1D mode); an Independent Pixel Approximation (IPA mode); and the 2D mode. The differences in domain–averaged normalized radiances of reflection and transmission are insignificant between the 1D or IPA and 2D calculation modes. However, local differences were observed since extinction is hinge on horizontal spatial variability. In the areas with large spatial variability in optical thickness, the radiance fields of the 2D mode differ about ±20% for the first and second Stokes elements (I, Q) from the fields of the 1D mode. This work points to a brand–new field: the quantification of the sensitivity of polarization to 3D radiative effects.

(English)Ozone is one of the most important greenhouse gases in terms of radiative forcing, as aresult of increasing in its precursor emissions since pre-industrial times. Until recently,the ozone radiative forcing calculations were entirely model based, exhibiting high uncertaintiesand a large spread in model values, as shown in the Intergovernmental Panelon Climate Change, Assessment Report 5. Satellite sounders operating in the infrarednow offer the possibility to infer directly the longwave radiative effect (LWRE) of ozone.The hyperspectral measurements allow to retrieve a vertical profile of ozone, and also thevertical distribution of the LWRE, apart from its column integrated value. The separationbetween troposphere and stratosphere allows to better constrain model estimates ofozone radiative forcing, but also support the predictions for its future evolution.In this thesis, a new method for calculating the ozone LWRE is presented, by exploitingthe measurements of the Infrared Atmospheric Sounding Interferometer on board theMetop satellites. The method is based on the calculation of the Instantaneous RadiativeKernel (IRK), which implies the angular integration of the radiance (inthe 9.6 μm band) at the top of the atmosphere using a Gaussian Quadrature. This quantityis transformed into a radiative flux density (the LWRE) by multiplicationwith the ozone profile retrieved by FORLI, for each atmospheric scene. The LWRE calculationmethod is applied to IASI non-cloudy scenes, for day and night, for the periodof 01/10/2007 to 31/12/2016. The results are analyzed separately for the total column ofozone, and for its tropospheric and stratospheric components; they are compared to estimationsdetermined independently from the TES (Tropospheric Emission Spectrometer)measurements on-board Aura, and from three state-of the-art chemistry-climate models.The discussion of the results is focused then on the spatial and temporal variability ofthe LWRE in the troposphere and stratosphere, as well as the on the trends over 9 yearsof measurements.(French)L’ozone est actuellement l’un des gaz à effet de serre les plus importants en terme de forçage radiatif ;sa contribution est liée à l’augmentation des émissions de ses précurseurs depuis l’époque préindustrielle. Jusqu’à récemment, le calcul du forçage radiatif de l’ozone était entièrement basé sur des modèles et était sujet à de grandes incertitudes, qui se révèlent notamment par la large gamme des valeurs calculées et intégrées dans le Cinquième Rapport d’Évaluation du Groupe d’experts intergouvernemental sur l’évolution du climat (GIEC). Les sondeurs embarqués sur des satellites et travaillant dans le domaine de l’infrarouge thermique donnent aujourd’hui la possibilité de directement mesurer l’effet radiatif de l’ozone au niveau de la radiation infrarouge sortante. La possibilité qu’offrent les mesures hyperspectrales pour restituer un profil vertical d’ozone permet par ailleurs de fournir la distribution verticale du forçage radiatif, au-delà se valeur intégrée sur la colonne atmosphérique. La séparation entre la troposphère et la stratosphère est importante en particulier pour contraindre les estimations des modèles mais aussi pour prédire l’évolution future du forçage radiatif. Dans cette thèse, nous présentons une méthode de calcul de l’effet radiatif de l’ozone qui exploite les mesures de l’Interféromètre Atmosphérique de Sondage dans l’Infrarouge (IASI) à bord des satellites Metop en orbite polaire. La méthode se base sur le calcul, pour chaque mesure de IASI, d’une grandeur appelée Instantaneous Radiative Kernel (IRK), impliquant l’intégration angulaire de la radiance (dans la bande d’absorption d’ozone centrée à 9.6µm) au sommet de l’atmosphère via une quadrature de Gauss. Cette quantité est transformée en une densité de flux radiatif (appelée Longwave Radiative Effect, LWRE) par multiplication par le profil d’ozone restitué par le logiciel FORLI, pour la scène atmosphérique en question. La méthode du calcul du LWRE est appliquée aux scènes non nuageuses de IASI, de jour comme de nuit, pour la période du 01/10/2007 au 31/12/2016. Les résultats sont analysés séparément pour la colonne totale d’ozone mais également pour ses composantes troposphériques et stratosphériques ;ils sont comparés aux estimations déterminées de façon indépendantes des mesures de l’instrument TES (Tropospheric Emission Spectrometer) sur AURA. La discussion de nos résultats se focalise ensuite sur la variabilité spatiale et temporelle du LWRE dans la troposphère et la stratosphère ;des résultats préliminaires concernant les tendances sur les 9 années de mesures sont fournis. Le manuscrit est structuré en différentes parties. Après une série de chapitres introductifs décrivant les bases nécessaires à ce travail, nous présentons l’instrument IASI et l’algorithme FORLI dédié à la restitution des concentrations d’ozone. La méthode de calcul du LWRE, au centre de notre travail de recherche, est décrite avec ses fondements mathématiques dans un chapitre dédié. Les distributions spatiales et verticales du LWRE, ainsi que son évolution temporelle sur 9 ans, d’une part pour l’effet radiatif de l’ozone total et d’autre part pour sa contribution troposphérique/stratosphérique sont discutées dans les derniers chapitres, qui incluent également une brève comparaison des estimations du LWRE par trois modèles de chimie-climat différents. / Doctorat en Sciences / info:eu-repo/semantics/nonPublished

Atmosphärisches Aerosol kann den Strahlungstransport signifikant beeinflussen. Mineralstaub, der über der Sahara und anderen Wüsten in die Atmosphäre gelangt, ist das hinsichtlich der in letzterer dauerhaft verbleibenden Masse bedeutendste Aerosol. Darüber hinaus sind Saharamineralstaubpartikel nichtkugelförmig, und die Wirkungen dieser Partikeleigenschaft auf den Strahlungstransport in der Erdatmosphäre sind bislang nur ungenügend untersucht worden. Es werden die optischen Eigenschaften, Strahlungs- und Erwärmungseffekte von Saharamineralstaub unter Berücksichtigung der Nichtkugelförmigkeit seiner Partikel quantitativ untersucht, wobei der gesamte, im Hinblick auf den Strahlungshaushalt energetisch relevante Spektralbereich zugrunde gelegt wird. Zunächst werden auf Basis in-situ-gemessener Experimentaldaten die atmosphärischen Umgebungsbedingungen, Größenverteilungen, Brechungsindizes, Bodenalbedo und Partikelgestalt festgelegt, die in einem zweiten Schritt in ein Strahlungstransportmodell einfließen. Mit dessen Hilfe wird in umfangreichen numerischen Simulationen des Strahlungstransports in einer realistischen mineralstaubhaltigen Modellatmosphäre im Vergleich zu Messdaten beispielsweise geklärt, welche Partikelform und Größenäquivalenz angenommener sphäroidaler Modellpartikel am meisten realistisch sind. Des Weiteren werden im Zusammenhang mit der Partikelnichtkugelförmigkeit Sensitivitätsstudien zur Beantwortung der Fragen durchgeführt, inwieweit diese das Strahlungsfeld beeinflusst und zu veränderten Strahlungserwärmungswirkungen führt.

The atmospheres of exoplanets are being characterised in increasing detail by observational facilities and will be examined with even greater clarity with upcoming space based missions such as the James Webb Space Telescope (JWST) and the Wide Field InfraRed Survey Telescope (WFIRST). A major component of exoplanet atmospheres is the presence of cloud particles which produce characteristic observational signatures in transit spectra and influence the geometric albedo of exoplanets. Despite a decade of observational evidence, the formation, dynamics and radiative-transport of exoplanet atmospheric cloud particles remains an open question in the exoplanet community. In this thesis, we investigate the kinetic chemistry of cloud formation in hot Jupiter exoplanets, their effect on the atmospheric dynamics and observable properties. We use a static 1D cloud formation code to investigate the cloud formation properties of the hot Jupiter HD 189733b. We couple a time-dependent kinetic cloud formation to a 3D radiative-hydrodynamic simulation of the atmosphere of HD 189733b and investigate the dynamical properties of cloud particles in the atmosphere. We develop a 3D multiple-scattering Monte Carlo radiative-transfer code to post-process the results of the cloudy HD 189733b RHD simulation and compare the results to observational results. We find that the cloud structures of the hot Jupiter HD 189733b are likely to be highly inhomogeneous, with differences in cloud particle sizes, number density and composition with longitude, latitude and depth. Cloud structures are most divergent between the dayside and nightside faces of the planet due to the instability of silicate materials on the hotter dayside. We find that the HD 189733b simulation in post-processing is consistent with geometric albedo observations of the planet. Due to the scattering properties of the cloud particles we predict that HD 189733b will be brighter in the upcoming space missions CHaracterising ExOPlanet Satellite (CHEOPS) bandpass compared to the Transiting Exoplanet Space Survey (TESS) bandpass.

Aerosol properties are highly variable in space and time which makes the aerosol study more complex. The sources and production mechanism of aerosols decide the properties of the aerosols. Aerosol radiative forcing is defined as the perturbation to the radiative fluxes of the earth atmosphere system caused by the aerosols. High uncertainty in the aerosol radiative forcing values exists today due to the lack of the exact chemical composition data of the aerosols everywhere. There are previous studies which have introduced methods to estimate ‘optical equivalent’ composition of aerosols using spectral aerosol optical depth measurements at the surface. The impact of aerosols on the solar radiative flux depends on its size distribution and composition. Hence, measurements of downward solar spectral fluxes at the surface can be used to infer ‘optically equivalent’ composition of aerosols. Measurements of downward solar spectral flux at Bangalore were made on clear days using a spectroradiometer. This data has been used to infer the aerosol composition following an iterative method with the help of the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART). Aerosols have been classified as water soluble, black carbon and three types of dust. Influence of the different aerosol types on spectral down welling irradiance at the surface have been simulated using Optical Properties of Aerosols and Clouds (OPAC) and SBDART models. The strong spectral dependence influence of water soluble aerosols and the dust aerosols on the spectral irradiance is shown. Aerosol composition was inferred following least square error minimization principle. This method can be used to estimate near-surface aerosol concentration if the vertical profile of aerosols is known a priori. This method also enables derivation of spectral single scattering albedo. The aerosol spectral radiative forcing has been estimated using downward spectral flux at the surface and compared with modeled fluxes. The contribution to the total forcing by the wavelength band 360 – 528 nm is around 60% of the total forcing. The wavelength band of 453-518 nm contributes maximum to the total forcing and it is seen that the shape of the spectral forcing is a major function of shape of the incoming solar spectrum. Aerosol spectral radiative forcing from observations of radiative fluxes agreed with modeled values when derived aerosol chemical composition was used as input. This study demonstrates that spectral flux measurements at the surface are useful to infer aerosol composition (which is optically equivalent) when and where the conventional chemical analysis is unavailable.

This thesis details the development of the radiation transport code torus for radiation hydrodynamic applications and its subsequent use in investigating problems regarding radiative feedback. The code couples Monte Carlo photoionization with grid-based hydrodynamics and has the advantage that all of the features available to a dedicated radiation transport code are at its disposal in RHD applications. I discuss the development of the code, including the hydrodynamics scheme, the adaptive mesh refinement (AMR) framework and the coupling of radiation transport with hydrodynamics. Extensive testing of the resulting code is also presented. The main application involves the study of radiatively driven implosion (RDI), a mechanism where the expanding ionized region about a massive star impacts nearby clumps, potentially triggering star formation. Firstly I investigate the way in which the radiation field is treated, isolating the relative impacts of polychromatic and diffuse field radiation on the evolution of radiation hydrodynamic RDI models. I also produce synthetic SEDs, radio, Hα and forbidden line images of the bright rimmed clouds (BRCs) resulting from the RDI models, on which I perform standard diagnostics that are used by observers to obtain the cloud conditions. I test the accuracy of the diagnostics and show that considering the pressure difference between the neutral cloud and surrounding ionized layer can be used to infer whether or not RDI is occurring. Finally I use more synthetic observations to investigate the accuracy of molecular line diagnostics and the nature of line profiles of BRCs. I show that the previously unexplained lack of dominant blue-asymmetry (a blue-asymmetry is the expected signature of a collapsing cloud) in the line profiles of BRCs can be explained by the shell of material, swept up by the expanding ionized region, that drives into the cloud. The work in this thesis combines to help resolve the difficulties in understanding radiative feedback, which is a non–linear process that happens on small astrophysical timescales, by improving numerical models and the way in which they are compared with observations.

Les conditions pour la fusion DT peuvent-être obtenues dans les tokamaks. Dans ces machines, l'interaction plasma-paroi et l'extraction de puissance sont gérées dans une cavité appelée divertor. Toutefois, les hautes puissances impliquées et les limitations des composants face au plasma (CFP) sont problématiques. Ce domaine fait l'objet de nombreuses recherches dans le contexte de ITER qui doit démontrer 500 MW de puissance fusion durant 400 s. Ces opérations nécessitent sur la réduction des flux de chaleur sur les CFP à un niveau gérable et repose sur le détachement du plasma dans le divertor qui implique la décroissance des flux de particules et de chaleur. Malheureusement, ce processus demeure difficile à modéliser. Le but the ce doctorat est d'utiliser la modélisation d'expériences de JET avec EDGE2D-EIRENE pour faire des progrès dans la compréhension du détachement. Les simulations reproduisent le détachement observé en environnement C comme Be/W. La distribution du rayonnement est reproduite par le code en C mais des écarts subsistent en Be/W. La comparaison entre différents processus de physique atomique montre que les collisions élastiques ion-molécule sont responsables du détachement. Ce processus permet le confinement des neutres dans le divertor ainsi que des pertes de moments significatives à basse température lorsque le plasma est recombinant. La comparaison entre EDGE2D-EIRENE et SOLPS4.3 montre des tendances similaires pour le détachement. Les deux codes suggèrent que tout processus capable d'améliorer le confinement des neutres dans le divertor devrait faciliter la modélisation du détachement. / The conditions required for fusion can be obtained in tokamaks. In most of these machines, the plasma wall-interaction and the exhaust of heating power are handled in a cavity called divertor. However, the high heat flux involved and the limitations of the materials of the plasma facing components (PFC) are problematic. Many researches are done this field in the context of ITER which should demonstrate 500 MW of DT fusion power during ~ 400 s. Such operations could bring the heat flux on the PFC too high to be handled. Its reduction to manageable levels relies on the divertor detachment involving the reduction of the particle and heat fluxes on the PFC. Unfortunately, this phenomenon is still difficult to model. The aim of this PhD is to use the modelling of JET experiments with EDGE2D-EIRENE to make some progress in the understanding of the detachment. The simulations reproduce the observed detachment in C and Be/W environments. The distribution of the radiation is well reproduced by the code for C but with some discrepancies in Be/W. The comparison between different sets of atomic physics processes shows that ion-molecule elastic collisions are responsible for the detachment seen in EDGE2D-EIRENE. This process provides good neutral confinement in the divertor and significant momentum losses at low temperature, when the plasma is recombining. Comparison between EDGE2D-EIRENE and SOLPS4.3 shows similar detachment trends but the importance of the ion-molecule elastic collisions is reduced in SOLPS4.3. Both codes suggest that any process capable of improving the neutral confinement in the divertor should help to improve the modelling of the detachment.

Ionising radiation is present in a variety of astrophysical problems, and it is particularly important for shaping the process of star formation in molecular clouds, containing hot, high-mass stars. In order to account for the effects of ionising radiation within numerical models of star formation, we need to combine a hydrodynamics method with a radiative transfer method and obtain a radiation hydrodynamics scheme (RHD). In this thesis I achieve live radiation hydrodynamics by coupling the Smoothed Particle Hydrodynamics (SPH) code Phantom with the Monte Carlo Radiative Transfer (MCRT) code CMacIonize. Since SPH is particle-based and MCRT is grid-based, I construct an unstructured, Voronoi grid in order to establish a link between the two codes. In areas with large density gradients, a Voronoi grid based purely on the SPH particle positions achieves insufficient resolution, and therefore I propose a novel algorithm for inserting a small number of additional grid cells to improve the local resolution. Furthermore, the MCRT calculations require the knowledge of an average density for each Voronoi cell. To address this, I develop an analytic density mapping from SPH to a Voronoi grid, by deriving an expression for the integrals of a series of kernel functions over the volume of a random polyhedron. Finally, I demonstrate the validity of the live RHD through the benchmark test of D-type expansion of an H II region, where good agreement is shown with the existing literature. The RHD implementation is then used to perform a proof-of-concept simulation of a collapsing cloud, which produces high-mass stars and is subsequently partially ionised by them. The presented code is a valuable tool for future star formation studies, and it can be used for modelling a broad range of additional astronomical problems involving ionising radiation and hydrodynamics.

An investigation of the high spectral resolution signatures and radiative forcing of tropospheric aerosol in the thermal infrared was conducted. To do so and to support advanced modeling of optical properties, a high spectral resolution library of atmospheric aerosol optical constants was developed. This library includes new optical constants of sulfate-nitrate-ammonium aqueous solutions and the collection of a broad range of existing optical constants for aerosol components, particularly mineral optical constants. The mineral optical constants were used to model and study infrared dust optical signatures as a function of composition, size, shape and mixing state. In particular, spherical and non-spherical optical models of dust particles were examined and compared to high spectral resolution laboratory extinction measurements. Then the performance of some of the most common effective medium approximations for internal mixtures was examined by modeling the optical constants of the newly determined sulfate-nitrate-ammonium mixtures. The optical signature analysis was applied to airborne and satellite high spectral resolution thermal infrared radiance data impacted by Saharan dust events. A new technique to retrieve dust microphysical properties from the dust spectral signature was developed and compared to a standard technique. The microphysics retrieved from this new technique and from a standard technique were then used to investigate the effects of dust on radiative forcing and cooling rates in the thermal IR.

This thesis treats the optical properties of mixed mineral dust and biomass burning aerosol in the thermal infrared (TIR) based on Fourier Transform infrared spectrometer (FTIR) measurements and radiative transfer simulations. The measurements were part of the Saharan Mineral Dust Experiment 2 (SAMUM-2) conducted from January to February 2008 at Praia, Cape Verde. The large amount of different instruments co-located at the main field site during the campaign resulted in a unique dataset comprising in-situ information and remote sensing data perfectly suited for column closure studies. The ultimate goal of this work is to investigate the consistency of microphysical and TIR remote sensing data. This is achieved by reproducing the measured radiances at top and bottom of the atmosphere (TOA, BOA) with a radiative transfer model, which assimilates the microphysical aerosol information gathered during SAMUM-2. The first part of the thesis describes several experimental efforts, including a novel calibration method and a drift correction algorithm for the ground-based FTIR instrument operated within the scope of SAMUM-2 by the author. The second part introduces the concurrent radiative transfer library PIRATES, which has been developed in the framework of this thesis for the analysis of TIR aerosol optical properties. The third and final part of the treatise compares measured and simulated spectra for various typical scenarios encountered during SAMUM-2. It is demonstrated in three case studies, that measured radiances in the TIR atmospheric window region (8-12 µm) can be reproduced at BOA and TOA by radiative transfer simulations assuming spheroidal model particles. Moreover, spherical particles are shown to be an inadequate model for mineral dust aerosol in this spectral region unless the aerosol optical depth is small.