A general finite difference discretization of the time-dependent radiation transport equation is developed around the framework of an existing steady-state three dimensional radiation transport solver based on the slice-balance approach. Three related algorithms are outlined within the general finite difference scheme: an explicit, an implicit, and a semi-implicit approach. The three algorithms are analyzed with respect to the discretizations of each element of the phase space in the transport solver. The explicit method, despite its small computational cost per time step, is found to be unsuitable for many purposes due to its inability to accurately handle rapidly varying solutions. The semi-implicit method is shown to produce results nearly as reliable as the fully implicit solver, while requiring significantly less computational effort.

Herein we present the development of a fluorescence-enhanced, frequency-domain radiative transport reconstruction system designed for small animal optical tomography. The system includes a time-dependent data acquisition instrument, a radiative transport based forward model for prediction of time-dependent propagation of photons in small, non-diffuse volumes, and an algorithm which utilizes the forward model to reconstruct fluorescent yields from air/tissue boundary measurements. The major components of the instrumentation include a charge coupled device camera, an image intensifier, signal generators, and an optical switch. Time-dependent data were obtained in the frequency-domain using homodyne techniques on phantoms with 0.2% to 3% intralipid solutions. Through collaboration with Transpire, Inc., a fluorescence-enhanced, frequency-domain, radiative transport equation (RTE) solver was developed. This solver incorporates the discrete ordinates, source iteration with diffusion synthetic acceleration, and linear discontinuous finite element differencing schemes, to predict accurately the fluence of excitation and emission photons in diffuse and transport limited systems. Additional techniques such as the first scattered distributed source method and integral transport theory are used to model the numerical apertures of fiber optic sources and detectors. The accuracy of the RTE solver was validated against diffusion and Monte Carlo predictions and experimental data. The comparisons were favorable in both the diffusion and transport limits, with average errors of the RTE predictions, as compared to experimental data, typically being less than 8% in amplitude and 7% in phase. These average errors are similar to those of the Monte Carlo and diffusion predictions. Synthetic data from a virtual mouse were used to demonstrate the feasibility of using the RTE solver for reconstructing fluorescent heterogeneities in small, non-diffuse volumes. The current version of the RTE solver limits the reconstruction to one iteration and the reconstruction of marginally diffuse, frequency-domain experimental data using RTE was not successful. Multiple iterations using a diffusion solver successfully reconstructed the fluorescent heterogeneities, indicating that, when available, multiple iterations of the RTE based solver should also reconstruct the heterogeneities.

The first part of this study is focused on numerical studies of light scattering from a single microscopic particle using the Discrete Dipole Approximation (DDA) method. The conventional DDA formalism is generalized to two cases: (a) inelastic light scattering from a dielectric particle and (b) light scattering from a particle with magnetic permeability u /= 1. The first generalization is applied to simulations of Raman scattering from bioaerosol particles, and the second generalization is applied to confi rmation of irregular invisibility cloaks made from metamaterials. In the second part, radiative transfer in a coupled atmosphere-ocean system is solved to study the asymptotic nature of the polarized light in deep oceans. The rate at which the radiance and the polarization approach their asymptotic forms in an ideal homogeneous water body are studied. Effects of the single scattering albedo and the volume scattering function are studied. A more realistic water body with vertical pro files for oceanic optical properties determined by a Case 1 water model is then assumed to study the e ffects of wavelength, Raman scattering, and surface waves. Simulated Raman scattering patterns computed from the generalized DDA formalism are found to be sensitive to the distribution of Raman active molecules in the host particle. Therefore one can infer how the Raman active molecules are distributed from a measured Raman scattering pattern. Material properties of invisibility cloaks with a few irregular geometries are given, and field distributions in the vicinity of the cloaked particles computed from the generalized DDA formalism con rm that the designated material properties lead to invisibility. The radiative transfer model calculation in deep oceans suggest that the underwater radiance approaches its asymptotic form more quickly than the polarization does. Therefore, a vector radiative transfer solution is necessary for asymptotic light field studies. For a typical homogeneous water body whose scattering property is characterized by the Petzold phase function, a single scattering albedo of w0 > 0:8 is required in order that the asymptotic regime can be reached before there are too few photons to be detected.

Radiative Decays of the phi-meson to the scalar mesons f0(980) and a0(980) are investigated within the framework of charged kaon loop model for both point-like scalar mesons and for scalar mesons with extended structure. Then, the radiative phi-meson decay into neutral K-meson is studied via a two step mechanism in which the scalar mesons couple the final state to the phi-meson through the charged kaon loop. The branching ratio of this decay is calculated and it is shown that this reaction will not provide a significant background to the measurements of phi-meson into neutral K-meson states decay for testing CP violation.

A novel nonintrusive soot diagnostics methodology was developed, validated and applied for in-situ determination of temperature, volume fraction and refractive index of soot aggregates formed inside flames by using near-infrared emission spectrometry. Research was conducted in three main parts, first one addressing development and validation of a comprehensive &quot / direct&quot / model for simulation of line-of-sight radiative emission from axisymmetric sooty flames by coupling sub-models for radiative transfer, radiative properties and optical constants. Radiative property estimation for soot agglomerates was investigated by experimentally validating discrete dipole approximation against microwave measurements and using it as reference to assess applicability of simpler Rayleigh-Debye-Gans approximation for fractal aggregates (RDG-FA). Comparisons between predictions of two methods for soot-like model aggregates demonstrated that radiative property predictions of RDG-FA are acceptably accurate for relatively small soot aggregates encountered in small-scale flames. Part two concerns experimental investigation of an axisymmetric ethylene/air diffusion flame by Fourier Transform Near-Infrared spectroscopy. Measurement of line-of-sight emission intensity spectra was performed along with analyses on calibration, noise, uncertainty and reproducibility. A noise characterization approach was introduced to account for spatial fluctuations which were found to dominate over spectral noise. Final part focuses on development, evaluation and application of an inversion methodology that inputs spectral emission intensity measurements from optically thin flames, removes noise, identifies soot refractive index from spectral gradients and retrieves soot temperature and volume fraction fields by tomographic reconstruction. Validation with simulated data and favorable application to measurements indicate that proposed methodology is a promising option for nonintrusive soot diagnostics in flames.

Recent emphasis on the prediction of temperature and concentration fields in the atmosphere has led to the investigation of accurate solution methods of the time-dependent conservation equations for mass, momentum, energy and species. Atmospheric radiation is the key component of this system. Therefore, atmospheric radiation models were developed in isolation from the climate models. The time-dependent multi-dimensional governing equations of atmospheric models must be solved in conjunction with the radiative transfer equation for accurate modeling of the atmosphere. In order to achieve this objective, a 1-D Radiative-Convective Model for Earth-Atmosphere System (RCM4EAS) was developed for clear and cloudy sky atmospheres. The radiative component of the code is Santa Barbara DISORT (Discrete Ordinate Radiative Transfer) Atmospheric Radiative Transfer (SBDART) integrated with exponential sum-fitting method as the radiative property estimation technique. The accuracy of SBDART was tested by comparing its predictions of radiative fluxes with those of Line-by-Line Radiative Transfer Model (LBLRTM) for 1-D longwave (3.33-100 &micro / m) clear sky atmosphere and a good agreement was obtained. A parametric study aiming at finding the optimum parameters to be used as input in SBDART regarding the wavelength increment and order of approximation was also carried out. Variable wavelength and eight streams were selected as optimum parameters for the accuracy and computational efficiency. The code was then coupled with a 1-D Radiative-Convective Model (RCM) to obtain the time dependent code, (RCM4EAS), which was applied to the investigation of the sensitivity of climate to changes in the CO2 concentration for clear and cloudy sky conditions. CO2 sensitivity analyses revealed that doubling the CO2 concentration in the earth&rsquo / s atmosphere from its present value (387 ppm) results in an increase in equilibrium surface temperature of 4.2 K in the clear sky atmosphere as opposed to 2.1 K in cloudy sky atmosphere with typical cloud physical parameters. It is worth noting that times required to reach equilibrium surface temperatures are approximately 2000 and 6000 days for clear and cloudy sky atmospheres, respectively and these temperature increases are calculated assuming that all the other parameters except CO2 concentration remain unchanged within these time periods. Therefore, it should be noted that these temperature increases reflect only the effect of CO2 doubling and excludes the effect of other forcings which might positively or negatively affect these temperature increases. Overall evaluation of the performance of the code developed in this thesis study indicates that it can be used with confidence in 1-D radiative-convective modeling of the earth-atmosphere systems.

The objective of this thesis is to evaluate the sources of the differences between the NO2 satellite retrieval products provided by the Royal Dutch Meteorological Institute (KNMI) and the National Aeronautics and Space Administration (NASA). Ground studies have shown that although both products use the same satellite, these products yield different observations for NO2 tropospheric columns concentrations. This study does not validate either retrieval product, but rather indentifies the main sources for the discrepancy. There are several parameters which allow successful retrieval of NO2 vertical columns. For this study, only the difference between the radiative models and the a priori NO2 chemical transport models were considered relevant. All other parameters, such as cloud properties, slant columns, stratospheric serration and their assumptions, were held constant. Here, the models are referred to by their proprietor's acronym: "TOMRAD" refers to the radiative model used by NASA, "DAK" refers to the radiative model used by KNMI, "TM4" refers to the a priori chemical transport model used by KNMI, and "REAM" refers to the a priori chemical transport model maintained by the School of Earth and Atmospheric Sciences at the Georgia Institute of Technology. Mixing these parameters creates four retrievals for comparison. Many significant differences were identified after comparing these four retrievals. First, there are viewing geometry biases between the port side and the starboard side of the satellite retrieval for each swath. These viewing geometry biases lead to artificial periodicities in the retrievals of NO2 tropospheric vertical columns over a specific coordinate or site, such as a city. Furthermore, there were significant differences found after using different a priori NO2 chemical transport models. The low horizontal resolution of TM4 and the satellite retrieval/TM4 coupling effect compared to REAM leads to considerable questioning of the near real time application of the KNMI NO2 retrieval product. Though the TM4 model performs poorly, TM4 retrievals do perform nearly as well as REAM retrievals at capturing day-to-day variability and the spatial variability of the cities used as examples here. The retrievals using TOMRAD outperformed the retrievals using DAK when compared to the high resolution, hourly REAM a priori chemical transport model. In sum, these findings should lead to better optimizations of both the KNMI and NASA retrievals, and thus make their publicly available data products more reliable and accurate for general use.

Near-field thermal radiation which can exceed blackbody radiation by several orders of magnitude has potential applications in energy conversion devices, nanofabrication, and near-field imaging. The present dissertation provides a comprehensive and thorough investigation of near-field heat transfer between parallel plates at nanometer distances. The first part of this dissertation focuses on the fundamentals of nanoscale thermal radiation through a systematic study on the near-field heat transfer between doped Si plates. In order to calculate the near-field heat transfer, it is important to accurately predict the dielectric function of doped Si. The dielectric function of doped Si which is described by the Drude model is a function of carrier concentration and mobility. Hence, accurate ionization and carrier mobility models for both p- and n-type Si are identified after a careful review of the available literature. The radiative properties calculated using the improved dielectric function agrees to a good extent with measurements performed using a FTIR. The near-field heat transfer between doped Si plates at varying doping levels is then calculated using the improved dielectric functions. Several important and characteristic features of near-field radiation are revealed in the analysis. An interesting issue regarding the maximum achievable nanoscale thermal radiation arises out of the study on near-field heat transfer in doped Si. The second part of this dissertation investigates the maximum achievable near-field thermal radiation between two plates at finite vacuum gaps. Initially, both the emitter and the receiver are assumed to have identical frequency-independent dielectric functions and a cut off in the order of the lattice spacing is set on the upper limit of the wavevector. The energy transfer is maximum when the real part of dielectric function is around -1 due to surface waves. On the other hand, there is a strong relationship between the imaginary part of the dielectric function and the vacuum gap. While the study using frequency independent dielectric function is not realistic, it lays down the guidelines for the parametric optimization of dielectric functions of real materials for achieving maximum near-field heat transfer. A parametric study of the different adjustable parameters in the Drude and Loretz model is performed in order to analyze their effect on the near-field heat transfer. It is seen that the optimized Drude model always results in greater near-field heat transfer compared to the Lorentz model and the maximum achievable near-field heat transfer is nearly 1 order greater than that between real materials. In the third part of this dissertation, the unusual penetration depth and the energy streamlines in near-field thermal radiation are studied. It is seen that unlike far-field radiation, the penetration depth in near-field heat transfer is dependent on the vacuum gap. This unusual feature results in a 10 nm thick SiC film behaving as completely opaque when the vacuum gap is around 10 nm. The energy streamlines inside the emitter, receiver, and the vacuum gap are calculated using fluctuation electrodynamics and errors generated due to thin film optics are pointed out. It is seen that the lateral shift of the streamlines inside the emitter can be greater than that in the vacuum gap for SiC. However, for doped Si, the lateral shift is comparable in the different media. While the study on the penetration depth determines the thickness of the emitter, the streamlines determine the lateral dimension.

The objective of this study was to assess if new cloud datasets, namely horizontal fields of integrated cloud parameters and transects of cloud profiles becoming available from current and future satellites like MODIS and CloudSAT as well as EarthCARE will allow for the reconstruction of three-dimensional cloud fields. Because three-dimensional measured cloud fields do not exist, surrogate cloud fields were used to develop and test reconstruction techniques. In order to answer the question if surrogate cloud fields may represent real cloud fields and to evaluate potential constraints for cloud field reconstruction, statistics of surrogate cloud fields have been compared to statistics of various remote sensing retrievals. It has turned out that except for cloud droplet effective radius, which is too low, other cloud parameters are in line with parameters derived from measurements. The reconstruction approach is divided into two parts. The first one deals with the reconstruction of the cloud fields. Three techniques with varying complexity are presented constraining the reconstruction by measurements to various degrees. Whereas the first one applies only information of a satellite radiometer, the other two constrain the retrieval also by profile information measured within the domain. Comparing the reconstruction quality of the approaches, there is no superior algorithm performing better for all cloud fields. This might be ascribed to liquid water content profiles of the surrogate cloud fields close to their adiabatic reference. Consequently, the assumption of adiabatic liquid water content profiles of the first scheme yields adequate estimates and additional information from profiles does not improve the reconstruction. The second part of the reconstruction approach addresses the reconstruction quality by comparing parameters of radiative transfer describing photon path statistics as well as reflectances. Therefore three-dimensional radiative transfer simulations with a Monte Carlo code were carried out for the surrogate cloud fields as well as for the reconstructed cloud fields. It was assumed that deviations of the parameter simulated for the reconstructed cloud and the surrogate cloud field are smaller when reconstruction is more accurate. For parameter describing photon pathes it has been found that only deviations of geometrical pathlength statistics reflect the reconstruction quality to a certain degree. Deviations of other parameters like photon penetration depth do not allow for either assessing local differences in reconstruction quality by an individual reconstruction scheme or to infer the most appropriate reconstruction scheme. The differences in reflectances do also not enable to evaluate reconstruction quality. They prevent from gaining insight in local accuracy of reconstruction due to effects like horizontal photon transport weakening the relations between microphysical as well as optical properties and reflectances of the column. In order to address these effects, grids of various complexity, derived by applying photon path properties, were used to weight deviations of cloud properties when analyzing the relationships. Unfortunately, there is no increase of explained variance due to the application of the weighting grids. Additionally, the sensitivity of the results to the model set-up, namely the spatial resolution of the cloud fields as well as the simplification and neglection of ancillary parameters, were analyzed. Though one would assume a strengthening of relationships between deviations of cloud parameters and deviations of reflectances due to more reliable sampling and reduced inter-column transport of photons when column size increases, there is no indication for resolutions where an assessment of the reconstruction quality by means of reflectance deviations becomes feasible. It also has been shown that inappropriate treatment of aerosols in the radiative transfer simulation impose an error comparable in magnitude to differences in reflectances due to inaccurate cloud field reconstruction. This is especially the case when clouds are located in the boundary layer of the aerosol model. Consequently, appropriate aerosol models should be applied in the analysis. May be due to the low surface reflection and the high cloud optical depths, the representation of the surface reflection function seems to be of minor importance. Summarizing the results, differences in radiative transfer do not allow for the assessment of cloud field reconstruction quality. In order to accomplish the task of cloud field reconstruction, the reconstruction part could be constrained employing information from additional measurements. Observational geometries enabling to use tomographic methods and the application of additional wavelengths for validation might help, too. / Ziel der Arbeit war die Evaluierung inwieweit Datensätze von Wolkenparametern, horizontale Felder integraler Wolkenparameter und Schnitte vertikal aufgelöster Parameter, zur Rekonstruktion dreidimensionaler Wolkenfelder genutzt werden können. Entsprechende Datensätze sind durch MODIS und CloudSAT erstmals vorhanden und werden zusätzlich mit dem Start von EarthCARE zur Verfügung stehen. Da dreidimensionale Wolkenfelder aus Messungen nicht existieren, wurden zur Entwicklung der Rekonstruktionsmethoden surrogate Wolkenfelder genutzt. Um die Qualität der surrogaten Wolkenfelder abzuschätzen und um mögliche Randbedingungen zur Rekonstruktion aufzuzeigen, wurden Statistiken der surrogaten Wolkenfelder mit denen unterschiedlicher Fernerkundungsprodukte verglichen. Dabei zeigte sich, dass, abgesehen von den gegenüber Messungen zu geringen Effektivradien der Wolkentropfen in den surrogaten Wolkenfeldern, die übrigen Wolkenparameter gut übereinstimmen. Der Rekonstruktionsansatz gliedert sich in zwei Teile. Der erste Teil beinhaltet die Rekonstruktion der Wolkenfelder. Dazu werden drei Techniken unterschiedlicher Komplexität genutzt, wobei die Komplexität durch den Grad der eingebundenen Messungen bestimmt wird. Während die einfachste Technik lediglich Informationen, wie sie aus Messungen mit einem Satellitenradiometer gewonnen werden können, nutzt, binden die anderen Techniken zusätzlich Profilinformationen aus dem beobachteten Gebiet ein. Analysen zeigten, dass keine der Methoden für alle untersuchten Wolkenfelder den anderen Methoden überlegen ist. Dies mag daran liegen, dass die Flüssigwasserprofile der surrogaten Wolkenfelder nur geringfügig von den in der ersten Rekonstruktionsmethode angenommenen adiabatischen Flüssigwasserprofilen abweichen, so dass die Nutzung der Profile kaum zusätzliche Information für die Rekonstruktion liefert. Im zweiten Teil des Rekonstruktionsansatzes wird die Qualität der rekonstruierten Wolkenfelder durch den Vergleich von Parametern des Strahlungstransfers, wie Photonenpfad-Statistiken und Strahlungsgrößen, evaluiert. Dazu wurden sowohl für die surrogaten Wolkenfelder als auch für die rekonstruierten Wolkenfelder dreidimensionale Strahlungstransfersimulationen mit einem Monte-Carlo-Modell durchgeführt. Angenommen wurde hierbei, dass eine bessere Rekonstruktionsqualität durch geringere Abweichungen der betrachteten Strahlungsparameter aus Simulationen mit rekonstruierten und surrogaten Wolkenfeldern gekennzeichnet ist. Bei den Parametern, die die Photonenwege beschreiben, unterstützen lediglich die Abweichungen der geometrischen Photonenweglängen diese These. Weder erlauben die Abweichungen der übrigen Parameter, zum Beispiel der Eindringtiefen, Rückschlüsse auf die lokale Rekonstruktionsqualität der einzelnen Methoden zu ziehen, noch ermöglichen sie die beste Rekonstruktionsmethode zu identifizieren. Auch die Unterschiede der simulierten Reflektanzen können nicht zur Bestimmung der Rekonstruktionsqualität herangezogen werden. Durch Effekte wie horizontale Photonentransporte werden die Zusammenhänge zwischen mikrophysikalischen und optischen Eigenschaften und Reflektanzen der jeweiligen Gittersäule aufgeweicht, und folglich sind keine Rückschlüsse auf die lokale Rekonstruktionsqualität möglich. Um auf entsprechende Effekte einzugehen, wurden für die Analyse Wichtungsfelder unterschiedlicher Komplexität aus Photonenwegeigenschaften generiert, um diese zur Wichtung der Abweichungen der Wolkeneigenschaften zu nutzen. Der Anteil der erklärten Varianz konnte jedoch durch die Nutzung der entsprechenden Wichtungsfelder nicht erhöht werden. Zusätzlich wurden Sensitivitätsstudien hinsichtlich einzelner Vorgaben der Untersuchung durchgeführt. Dazu wurden sowohl der Einfluss der räumlichen Auflösung der Wolkenfelder als auch die Vereinfachung oder Nichtbetrachtung einzelner Modellparameter analysiert. Eine Reduzierung der Auflösung einhergehend mit einem zuverlässigeren Sampling und reduzierten Photonentransport zwischen den Gittersäulen führte zu keinem direkteren Zusammenhang zwischen den Abweichungen der Reflektanzen und den Abweichungen der mikrophysikalischen Eigenschaften. Folglich existiert keine Auflösung, die die Anwendung des Verfahrens ermöglichen würde. Ebenso wurde gezeigt, dass die unzureichende Einbeziehung von Aerosolen bei den Strahlungstransfersimulationen einen Fehler verursachen kann, der in der Größe dem Unterschied der Reflektanzen unzureichender Wolkenfeldrekonstruktionen gleichkommt. Dies ist insbesondere der Fall, wenn die Wolken sich innerhalb der Grenzschicht des Aerosolmodells befinden. Entspechend sollte in solchen Situationen dem verwendeten Aerosolmodell besondere Beachtung geschenkt werden. Hingegen ist der Einfluss des Ansatzes, wie die Bodenreflektion beschrieben wird, eher gering. Dies mag an dem verwendeten Modell mit einer geringen Albedo in Kombination mit optisch dicken Wolken liegen. Zusammenfassend kann festgestellt werden, dass die Unterschiede im Strahlungstransfer nicht zur Abschätzung der Rekonstruktionsqualität der Wolkenfelder herangezogen werden können. Um dem Ziel einer dreidimensionalen Wolkenfeldrekonstruktion näher zu kommen, könnten beim Rekonstruktionsteil Informationen aus zusätzlichen Messungen als Vorgaben genutzt werden. Ebenso könnten Beobachtungsgeometrien, welche die Anwendung tomographischer Methoden erlauben, sowie zusätzliche Wellenlängen zur Validierung der Rekonstruktionsergebnisse verwendet werden.

The character of the first galaxies at redshifts z [greater-than or equal to] 10 strongly depends on the star formation which takes place during their assembly. Conducting cosmological hydrodynamics simulations, we study how the radiative output and chemical enrichment from the first stars impacts the properties of the first galaxies. We find that the radiative feedback from the first stars suppresses the star formation rate at redshifts z [greater-than or equal to] 15 by a factor of only a few. In turn, this suggests that a large fraction of the first galaxies may form from gas which has already been enriched with the first heavy elements ejected by primordial supernovae. In order to characterize the properties of primordial dwarf galaxies, we carry out radiation hydrodynamics simulations which allow to determine how the luminosities in hydrogen and helium emission lines depend on the initial mass function of the stars in the galaxy. As well, we show that the chemical abundance patterns observed in metal-poor Galactic halo stars contain the signature of the first supernovae, and we use this data to indirectly probe the properties of the first stars. / text