<p> </p><p>The interaction between light and organometallic chromophores has been investigated theoretically in a strive for fast optical filters. The main emphasis is on two-photon absorption and excited state absorption as illustrated in the Jablonski diagram. We stress the need for relativistic calculations and have developed methods to address this issue. Furthermore, we present how quantum chemical calculations can be combined with Maxwell's equations in order to simulate propagation of laser pulses through a materials doped with chromophores with high two-photon absorption cross sections. Finally, we also discuss how fast agile filters using spin-transition materials can be modeled in order to accomplish theoretical material design.</p> / Report code: LIU-TEK-LIC-2006:55. On the day of the defence date the status on article III was Manuscript, article IV was Accepted and article V was Submitted.

<p>The solid oxide fuel cell (SOFC) technology has been under research since thelate 1950s, and most of the research has been on designs utilizing yttria stabilized zirconia (YSZ) as the electrolyte of choice. However, the SOFC technology has the major drawback of requiring high operation temperatures (up to 1000 degrees Celcius), so research of alternative materials have come into interest that would possibly require a lower working temperature without any significant loss of conductivity.One such material of interest for the electrolyte is compounds of ceriumdioxide (ceria). Ceria is well known for its ability to release oxygen by formingoxygen vacancies under oxygen-poor conditions, which increases its oxygen ionconductivity, and works at a lower temperature than the YSZ compounds whenproperly doped. Conversely, ceria is also able to absorb oxygen under oxygen-rich conditions, and those two abilities make it a very good material to use in catalytic converters for reduction of carbon monoxide and nitrogen oxide emission. The ability for the oxygen ions to easily relocate inbetween the different lattice sites is likely the key property of oxygen ion transportation in ceria. Also, in oxygen-rich conditions, the absorbed oxygen atom is assumed to join the structure at either the roomy octrahedral sites, or the vacant tetrahedral sites. Following that, the oxygen atom may relocate to other vacant locations, given it can overcome a possible potential barrier.</p><p>This thesis studies how those interstitial oxygen vacancies (defects) affect theenergy profile of ceria-based supercells by first principles calculations. The system is modeled within the density functional theory (DFT) with aid of (extended) local density approximation (LDA+U) using the software VASP. Furthermore, it is studied how those vacancies affect neighbouring oxygen atoms, and wether or not it is energetically benificial for the neighbouring atoms to readjust their positions closer or further away from the vacancy. The purpose of this thesis is to analyze wether or not it is theoretically possible that interstitial oxygen vacancies may cause neighbouring oxygen atoms to naturally relocate to the octahedral site in ceria, and how this affects the overall energy profile of the material.</p>

<p>The absorption spectra of a recently designed low-bandgap conjugated polymer has been studied using the semi-empirical method ZINDO and TDDFT/B3LYP/6-31G. The vertical excitation energies have been calculated for monomer up to hexamer. Two main absorption peaks can be seen, the one largest in wavelength corresponding to a HOMO to LUMO transition, and one involving higher order excitations. TDDFT results are red-shifted compared to the ZINDO results. Comparison with experiment yields that short conjugation lengths are dominating. This is possibly due to steric interactions between polymer chains, breaking the conjugation length. Such effects are also studied.</p>

<p>In this thesis we explore in particular the dynamics of a special type of quasi-particle in pi-conjugated materials termed polaron, the origin of which is intimately related to the strong interactions between the electronic and the vibrational degrees of freedom within these systems. In order to conduct such studies with the particular focus of each appended paper, we simultaneously solve the time-dependent Schrödinger equation and the lattice equation of motion with a three-dimensional extension of the famous Su-Schrieffer-Heeger (SSH) model Hamiltonian. In particular, we demonstrate in Paper I the applicability of the method to model transport dynamics in molecular crystals in a region were neither band theory nor perturbative treatments such as the Holstein model and extended Marcus theory apply. In Paper II we expand the model Hamiltonian to treat the revolution of phenylene rings around the sigma-bonds and demonstrate the great impact of stochastic ring torsion on the intra-chain mobility in conjugated polymers using poly[phenylene vinylene] (PPV) as a model system. Finally, in Paper III we go beyond the original purpose of the methodology and utilize its great flexibility to study radiationless relaxations of hot excitons.</p> / Report code: LiU-TEK-LIC-2007:4.

The solid oxide fuel cell (SOFC) technology has been under research since thelate 1950s, and most of the research has been on designs utilizing yttria stabilized zirconia (YSZ) as the electrolyte of choice. However, the SOFC technology has the major drawback of requiring high operation temperatures (up to 1000 degrees Celcius), so research of alternative materials have come into interest that would possibly require a lower working temperature without any significant loss of conductivity.One such material of interest for the electrolyte is compounds of ceriumdioxide (ceria). Ceria is well known for its ability to release oxygen by formingoxygen vacancies under oxygen-poor conditions, which increases its oxygen ionconductivity, and works at a lower temperature than the YSZ compounds whenproperly doped. Conversely, ceria is also able to absorb oxygen under oxygen-rich conditions, and those two abilities make it a very good material to use in catalytic converters for reduction of carbon monoxide and nitrogen oxide emission. The ability for the oxygen ions to easily relocate inbetween the different lattice sites is likely the key property of oxygen ion transportation in ceria. Also, in oxygen-rich conditions, the absorbed oxygen atom is assumed to join the structure at either the roomy octrahedral sites, or the vacant tetrahedral sites. Following that, the oxygen atom may relocate to other vacant locations, given it can overcome a possible potential barrier. This thesis studies how those interstitial oxygen vacancies (defects) affect theenergy profile of ceria-based supercells by first principles calculations. The system is modeled within the density functional theory (DFT) with aid of (extended) local density approximation (LDA+U) using the software VASP. Furthermore, it is studied how those vacancies affect neighbouring oxygen atoms, and wether or not it is energetically benificial for the neighbouring atoms to readjust their positions closer or further away from the vacancy. The purpose of this thesis is to analyze wether or not it is theoretically possible that interstitial oxygen vacancies may cause neighbouring oxygen atoms to naturally relocate to the octahedral site in ceria, and how this affects the overall energy profile of the material.

The absorption spectra of a recently designed low-bandgap conjugated polymer has been studied using the semi-empirical method ZINDO and TDDFT/B3LYP/6-31G. The vertical excitation energies have been calculated for monomer up to hexamer. Two main absorption peaks can be seen, the one largest in wavelength corresponding to a HOMO to LUMO transition, and one involving higher order excitations. TDDFT results are red-shifted compared to the ZINDO results. Comparison with experiment yields that short conjugation lengths are dominating. This is possibly due to steric interactions between polymer chains, breaking the conjugation length. Such effects are also studied.

This thesis describes the development of electronic modules for fusion neutron spectroscopy as well as several implementations of artificial neural networks (NN) for neutron diagnostics for the Joint European Torus (JET) experimental reactor in England. The electronics projects include the development of two fast light pulser modules based on Light Emitting Diodes (LEDs) for the calibration and stability monitoring of two neutron spectrometers (MPRu and TOFOR) at JET. The particular electronic implementation of the pulsers allowed for operation of the LEDs in the nanosecond time scale, which is typically not well accessible with simpler circuits. Another electronic project consisted of the the development and implementation at JET of 32 high frequency analog signal amplifiers for MPRu. The circuit board layout adopted and the choice of components permitted to achieve bandwidth above 0.5 GHz and low distortion for a wide range of input signals. The successful and continued use of all electronic modules since 2005 until the present day is an indication of their good performance and reliability. The NN applications include pulse shape discrimination (PSD), deconvolution of experimental data and tomographic reconstruction of neutron emissivity profiles for JET. The first study showed that NN can perform neutron/gamma PSD in liquid scintillators significantly better than other conventional techniques, especially for low deposited energy in the detector. The second study demonstrated that NN can be used for statistically efficient deconvolution of neutron energy spectra, with and without parametric neutron spectroscopic models, especially in the region of low counts in the data. The work on tomography provided a simple but effective parametric model for describing neutron emissivity at JET. This was then successfully implemented with NN for fast and automatic tomographic reconstruction of the JET camera data. The fast execution time of NN, i.e. usually in the microsecond time scale, makes the NN applications presented here suitable for real-time data analysis and typically orders of magnitudes faster than other commonly used codes. The results and numerical methods described in this thesis can be applied to other diagnostic instruments and are of relevance for future fusion reactors such as ITER, currently under construction in Cadarache, France.

Electric breakdown in power transformers is preceded by pre-breakdown events such as streamers. The understanding of these phenomena is important in order to optimize liquid insulation systems. Earlier works have derived a model that describes streamers in transformer oil and utilized a finite element method to produce numerical solutions. This research investigates the consequences of changing the numerical method to a finite volume-based solver implemented in OpenFOAM. Using a standardized needle-sphere geometry, a number of oil and voltage combinations were simulated, and the results are for the most part similar to those produced by the previous method. In cases with differing results the change is attributed to the more stable numerical performance of the OpenFOAM solver. A proof of concept for the extension of the simulation from a two-dimensional axial symmetry to three dimensions is also presented. / Elektriska genomslag i högspänningstransformatorer föregås av bildandet av elektriskt ledande kanaler som kallas streamers. En god förståelse av detta fenomen är viktigt vid konstruktionen av oljebaserad elektrisk isolation. Tidigare forskning i ämnet har tagit fram en modell för fortplantningen av streamers. Denna modell har sedan lösts numeriskt av ett beräkningsverktyg baserat på finita elementmetoden. I denna uppsats undersöks konsekvenserna av att byta metod till finita volymsmetoden genom att implementera en lösare i OpenFOAM. En standardiserad nål-sfär-geometri har ställts upp och ett flertal kombinationer av oljor och spänningar har simulerats. De flesta resultaten visar god överensstämmande med tidigare forskning medan resultat som avviker har tillskrivits de goda numeriska egenskaperna hos OpenFOAM-lösaren. En ny typ av simulering har även genomförts där simulationen utökas från en tvådimensionell axisymmetrisk geometri til tre dimensioner.

The acoustic environment generated during launch is the most demanding structural load case for large, lightweight satellite reflector antennas. The reflector is exposed to extremely high sound pressure levels originating from the structural excitation of the rocket engines and exterior air flow turbulence. This thesis aims to predict the structural responses in the reflector due to the acoustic pressure load with a model based on Finite Element Modelling (FEM). The FE-model is validated against a previously performed Boundary Element Method (BEM) analysis. An approach called Split Loading together with a combination of BEM and FEM will be utilized to handle the surrounding air mass and the applied sound pressures. The idea of Split Loading is to divide the structure into several patches and apply a unit pressure load to each patch separately. In the last step the unit pressure is scaled and correlated by a power spectral density calculated from the acoustic pressures. Split Loading will be implemented in software packages MSC.NASTRAN/PATRAN. The model developed in this thesis handles both the added mass of the surrounding air and the sound pressure applied to the reflector. The model can qualitatively well reproduce the results of the BEM-analysis and the test data. However, the model tends to overestimate responses at low frequencies and underestimate them at high frequencies. The end results is that the model becomes too conservative at low frequencies to be used without further development.

The interaction between light and organometallic chromophores has been investigated theoretically in a strive for fast optical filters. The main emphasis is on two-photon absorption and excited state absorption as illustrated in the Jablonski diagram. We stress the need for relativistic calculations and have developed methods to address this issue. Furthermore, we present how quantum chemical calculations can be combined with Maxwell's equations in order to simulate propagation of laser pulses through a materials doped with chromophores with high two-photon absorption cross sections. Finally, we also discuss how fast agile filters using spin-transition materials can be modeled in order to accomplish theoretical material design. / <p>Report code: LIU-TEK-LIC-2006:55. On the day of the defence date the status on article III was Manuscript, article IV was Accepted and article V was Submitted.</p>