Diss. (sammanfattning) Stockholm : Karol. inst., 2005. / Härtill 4 uppsatser.

Diss. (sammanfattning) Stockholm : Karol. inst., 2005. / Härtill 4 uppsatser.

Diss. (sammanfattning) Stockholm : Karolinska institutet, 2007. / Härtill 6 uppsatser.

Diss. (sammanfattning) Umeå : Umeå universitet, 2006. / Härtill 4 uppsatser.

Thesis--University of Oklahoma. / Includes bibliographical references.

<strong>Chapter 1</strong> introduces the concept of spin, how spins interact, and how the spin state in a radical pair can affect the outcome of a chemical reaction between the unpaired electrons. The computational methodology for simulating such radical pairs is also discussed. <strong>Chapter 2</strong> discusses anisotropy in the singlet recombination yield of a radical pair in a carotenoid-porphyrin-fullerene triad, containing many hyperfine couplings. The singlet yield was calculated as a function of the direction of an applied magnetic field, using symmetry in the molecule to reduce the size of the problem. The symmetry reduction was partially successful, however it was not possible to include all the hyperfine couplings in the molecule. <strong>Chapter 3</strong> introduces a radical pair located on a flavin ligand and a tryptophan residue in the protein cryptochrome, and discusses the spin-relaxation mechanism of singlet-triplet dephasing. Magnetic field effect curves, describing the formation of a secondary radical pair as a function of applied magnetic field, were found to be broader in longer-lived radical pairs, due to dephasing caused by spin-selective recombination to the singlet ground state. Additional singlet-triplet dephasing may occur due to hopping of one of the unpaired electrons, between a zone of strong exchange interaction and a zone of negligible exchange interaction, although this is an incomplete description of the spin-relaxation. <strong>Chapter 4</strong> discusses the effect of rotational tumbling on spin-relaxation in the flavin-tryptophan radical pair in cryptochrome. Simulations indicated that the resulting modulation of anisotropic hyperfine couplings contributed modestly to spinrelaxation during transient absorption measurements, but was insufficient to explain the lack of an experimental low-field effect, or to explain the width of the experimental magnetic field effect curves as a function of magnetic field strength. <strong>Chapter 5</strong> discusses magnetic field effects on the mutual annihilation of a pair of triplet excitons in tetracene and anthracene crystals. The experimental singlet recombination yield was found, for the first time, to be modulated as a function of the direction of a applied magnetic field as weak as 2 mT. Simulations indicated that this anisotropy arose due to the zero field splitting of the electronic state in each triplet exciton. The direction of the external magnetic field altered the singlet component of the eigenstates of the Hamiltonian, and therefore altered the timeaverage of the singlet probability of a triplet exciton pair. This is different to the already established mechanism under a strong magnetic field, where the anisotropy arises from level crossings of eigenstates.

Title: Photoluminescence of CdTe crystals Author: Jan Procházka Department: Institute of Physics of Charles University in Prague Supervisor: Doc. RNDr. Pavel Hlídek, CSc. Abstract: Energy levels connected with defects in nominally undoped crystals CdTe, indium- doped crystals and chlorine-doped crystals were studied using low-temperature photoluminescence. The crystals are intended for X- and gamma- ray detectors operated at room temperature. An effect of annealing in cadmium or tellurium vapor on luminescence spectra was investigated. Some changes were interpreted by filling of vacancies not only by atoms coming from gaseous phase but also by impurities from defects like interstitials, precipitates, inclusions, grain boundaries etc. The luminescence bands assigned to defects important for compensation mechanism were examined, namely A-centers (complexes of vacancy in cadmium sublattice and impurity shallow donor) and complexes of two donors bound to a vacancy. It was shown, that temperature dependence of the luminescence bands results from more complicated processes than a simple thermal escape of bound excitons or thermal excitation of electrons (holes) from defects to bands. We observed expressive "selective pair luminescence" bands (SPL) on partially compensated In-doped samples during sub-gap...

Over the years `short-range order' (SRO), whereby the local atomic arrangement differs from that of a random distribution, has been used to explain physical phenomena such as thermodynamic discontinuities, increased strength, anomalous electrical resistivity and magnetic variations in a host of alloys. However, due mainly to experimental difficulties and the complexity of the calculations required for the analysis of diffuse scattering, such work has been largely abandoned and hence quantification and assessment of SRO is notably sparse in the literature. The recent development of reverse Monte-Carlo (RMC) methods for the analysis of total scattering data has opened a promising route for the assessment of a material's local environment and has already provided important insights into a host of complex chemical systems, including liquids, network glasses, nano-materials, functional oxides and metal organic frameworks. The work presented in this thesis focuses on the development of a new methodology for the analysis of local structural effects in metallic systems using total scattering, and the first systematic application to the study of alloys. The simulation of total scattering data from a range of model structures is used to show that the information content of total scattering functions, in particular the pair distribution function (PDF), is sufficiently high to allow the assessment of different types and degrees of short-range order. This is supported by a demonstration of how such orders can be quantified from large box models, produced by fitting total scattering data using the RMC algorithm, with the mathematical analyses outlined. This culminates in a proposed methodology for the analysis of SRO in alloys. Having developed this analytical methodology it is subsequently applied to a number of interesting alloy systems. To demonstrate the efficacy of this methodology it was first applied to the study of a sample of Cu$_{3}$Au - the classically cited case example of a system demonstrating SRO prior to an ordering transition. This experiment provides new insight into this well characterised transition, and also demonstrates the significance of data processing errors on the generation of artefacts in large box modelling. The technique is also applied to the study of the industrially important family of nickel superalloys, assessing ordering in the gamma-phase alloy Ni-Cr and the sublattice orderings occurring in L1$_{2}$ alloys. Next, the use of the technique for the analysis of local strains exhibited in a lattice is presented. A series of models is used to demonstrate how the PDF is expected to change under variations in local strain caused by increased concentration of atomic substitution and variation in atomic radii. This is subsequently used to study the characteristic high-entropy alloy (HEA) CrMnFeCoNi. Through analysis of the PDF, it is demonstrated that the level of local strain exhibited in this alloy is not significantly different from those of other related compositionally simpler alloys. This result is highly significant as it challenges one of the core principles of the field - that the lattices of HEAs are necessarily highly strained. Finally, the energetics of ordering reactions are briefly considered and used to justify some of the observed transformations presented in the earlier work. Together, the body of work in this thesis shows how the total scattering technique can be used to provide valuable insight into a host of interesting local phenomena occurring in alloy systems. It is hoped that this will open up a new field of study into these effects, and ultimately guide the creation of new alloys based on these structure-property relationships.

La génération d'objets quantiques intriqués est inévitable pour l'exploration de l'information quantique dans les systèmes de la matière condensée. Alors que des expériences de non-localité on été menées, avec succès, à partir de photons intriqués, il n'a pas encore été possible de réaliser leurs analogues électroniques dans les matériaux solides, où les fermions sont les objets quantiques à intriqués. Les paires de Cooper dans les supraconducteurs sont des candidats prometteurs pour réaliser une source d'électrons intriqués. L'intrication non-local est la clé de voûte et elle peut être induite par le processus de réflexion d'Andreev croisée. Ce phénomène sépare une paire de Cooper en deux électrons, dont les spins sont intriqués, dans deux conducteurs séparés spatialement.J'ai étudié un système composé de trois électrodes supraconductrices (Al) connectées par un métal normal (Cu) formant ainsi une tri-jonction Josephson. De nouvelles structures, dans cette nano-structure hybride, apparaissent dans la conductance différentielle lorsque deux terminaux sont polarisées par des potentiels opposés l'un par rapport à l'autre. Ces anomalies correspondent à des phénomène de transport de paires de Cooper corrélées et sont consistantes avec la prédictiondes Quartets formés par la séparation simultanée de deux paires de Cooper d'un réservoir supraconducteur vers les deux autres électrodes.Dans le but d'expérimenter la cohérence quantique de ces structures, j'ai irradié la tri-jonction à l'aide d'une micro-onde de 14 GHz à très basse température. Des résonances Shapiro apparaissent lorsque la fréquence de la micro-onde est équivalente à la fréquence des courants AC Josephson générés en appliquant des tensions à travers la tri-jonction.Mon étude révèle que les anomalies de type Quartet présentent aussi des résonances Shapiro. Ce résultat démontre que le phénomène de Quartet est un mécanisme quantique cohérent confirmant la séparation cohérente de deux pairs de Cooper à longue portée. / A fundamental route for the exploration of solid state based quantum information is the generation of EPR pairs of quantum-entangled objects. Although experimental tests of nonlocality have been successfully conducted with pair of entangled photons, it has not yet been possible to realize an electronic analogue of it in the solid state, where fermions are the natural quantum objects. However, Cooper pairs in superconductors are known as suitable sources of entanglement. Non-local entanglement is the key and Crossed Andreev reflection process can provide it by converting a Cooper pair into two spin-entangled electrons located in separate conductors.I investigated a device where three superconducting (Al) electrodes are connected by a sub-micron normal metal (Cu) composing a Josephson three-junction. In this hybrid nanostructure, new sub-gap features appear in the differential conductance when two terminals are biased at opposite voltage with respect to the third one. These features correspond to correlated motion of Cooper pairs and are consistent with the prediction of Quartets formed by the simultaneous splitting of two Cooper pairs from one of the superconducting reservoirs and the emission of two phase correlated Cooper pairs in the two other electrodes. In order to probe the quantum coherence of such features, I irradiated the device with a microwave at 14 GHz down to very low temperature (100 mK). Well known Shapiros resonances (both integer and half-integer) are observed when the microwave frequency matches the frequency of the AC Josephson currents generated by applying differents voltages across the three-junction.My study reveals that the quartet feature also shows Shapiro-like resonances. This result demonstrates that the quartet feature is a true quantum mechanism and confirms the quartet scenario that implies the coherent splitting of two Cooper pairs.

Not all combinations of nouns and adjectives are possible and some are clearly more fre- quent than other. With this in mind this study aims to construct semantic representations of the two types of parts-of-speech, based on how they occur with each other. By inves- tigating these ideas via automatic natural language processing paradigms the study aims to find evidence for a semantic mutuality between nouns and adjectives, this notion sug- gests that the semantics of a noun can be captured by its corresponding adjectives, and vice versa. Furthermore, a set of proposed categories of adjectives and nouns, based on the ideas of Gärdenfors (2014), is presented that hypothetically are to fall in line with the produced representations. Four evaluation methods were used to analyze the result rang- ing from subjective discussion of nearest neighbours in vector space to accuracy generated from manual annotation. The result provided some evidence for the hypothesis which suggests that further research is of value.