A cinza obtida da queima controlada da casca de arroz é um material que apresenta propriedades pozzolânicas: reage na presença de água e dióxido de cálcio produzindo silicato de cálcio hidratado (C-S-H), o material que confere a resistência mecânica aos cimentos. Portanto, a cinza de casca de arroz é um material de potencial interesse para o desenvolvimento de cimentos não convencionais, baseados em subprodutos industriais ou agrícolas. Neste trabalho, os compostos presentes em cinzas de alta reatividade pozzolânica e os produtos obtidos de sua reação pozzolânica foram estudados através da Ressonância Magnética Nuclear (RMN) de alta resolução de 13C e 29Si. Na cinza não hidratada foram detectados domínios de sílica amorfa, o componente principal, e quantidades menores de sílica cristalina (cristobalita e quartzo), carbono amorfo e cadeias de siloxanos. Foi estudada a evolução da reação em pastas obtidas da hidratação da cinza na proporção água: cal: cinza O,47H20+O,53(O,1CCA+O,9Cal)=1 (entre 8 e 134 dias de idade). Mediante a RMN de 29Si foi possível caracterizar a formação de C-S-H e disposição dos grupos silicatos na estrutura. A estrutura do C-S-H obtido é comparável à observada em cimentos convencionais e cimentos de escoria de alto forno, e é compatível com os modelos propostos. A quantidade de C-S-H produzido e a velocidade da reação são menores quando comparadas com os outros cimentos. Efeitos da carbonatação de C-S-H foram observáveis em atmosfera ambiente. Foi detectado também o efeito da hidratação sobre os componentes minoritários da cinza. / The ashes obtained from burning rice husks have pozzolanic properties: in the presence of water and calcium dioxide the ashes react to produce calcium silicate hydrate (C-SH), the main binding agent in cementitiuos materials. Therefore, rice husk ashes are interesting materials in order to produce non-conventional cement, based in industrial or agricultural byproducts. The compounds present in a sample of rice husk ashes of high pozzolanic activity, and the products of hydration, were characterized using high resolution solid-state Nuclear Magnetic Resonance (NMR) of 13C and 29Si. Several compounds were detected in anhydrous ashes: amorphous silica (the main component), and minor quantities of crystalline silica (cristobalite and quartz), amorphous carbon and siloxane polymeric chains. Hardened pastes were prepared with a ratio water:calcium dioxide:ash O,47H20+O,53(O,1dioxide ash+O,9calcio)=1. The evolution of the hydration reaction was monitored at several ages between 8 to 134 days. The formation of C-S-H was detected by 29Si-NMR and the arrangement of the silicate groups was characterized. The structure of the C-S-H formed in these pastes agrees with the one observed in conventional cements and also b1ast furnace slag cements. Also, it is in agreement with the accepted structural models of C-S-H. The amount of C-S-H produced and the velocity of the reaction are minor than those observed in blast furnace slag cements. Carbonation effects were detected in ambient atmospheric conditions. Also, the effect of the hydration on the minority compounds was also detected.

A cinza obtida da queima controlada da casca de arroz é um material que apresenta propriedades pozzolânicas: reage na presença de água e dióxido de cálcio produzindo silicato de cálcio hidratado (C-S-H), o material que confere a resistência mecânica aos cimentos. Portanto, a cinza de casca de arroz é um material de potencial interesse para o desenvolvimento de cimentos não convencionais, baseados em subprodutos industriais ou agrícolas. Neste trabalho, os compostos presentes em cinzas de alta reatividade pozzolânica e os produtos obtidos de sua reação pozzolânica foram estudados através da Ressonância Magnética Nuclear (RMN) de alta resolução de 13C e 29Si. Na cinza não hidratada foram detectados domínios de sílica amorfa, o componente principal, e quantidades menores de sílica cristalina (cristobalita e quartzo), carbono amorfo e cadeias de siloxanos. Foi estudada a evolução da reação em pastas obtidas da hidratação da cinza na proporção água: cal: cinza O,47H20+O,53(O,1CCA+O,9Cal)=1 (entre 8 e 134 dias de idade). Mediante a RMN de 29Si foi possível caracterizar a formação de C-S-H e disposição dos grupos silicatos na estrutura. A estrutura do C-S-H obtido é comparável à observada em cimentos convencionais e cimentos de escoria de alto forno, e é compatível com os modelos propostos. A quantidade de C-S-H produzido e a velocidade da reação são menores quando comparadas com os outros cimentos. Efeitos da carbonatação de C-S-H foram observáveis em atmosfera ambiente. Foi detectado também o efeito da hidratação sobre os componentes minoritários da cinza. / The ashes obtained from burning rice husks have pozzolanic properties: in the presence of water and calcium dioxide the ashes react to produce calcium silicate hydrate (C-SH), the main binding agent in cementitiuos materials. Therefore, rice husk ashes are interesting materials in order to produce non-conventional cement, based in industrial or agricultural byproducts. The compounds present in a sample of rice husk ashes of high pozzolanic activity, and the products of hydration, were characterized using high resolution solid-state Nuclear Magnetic Resonance (NMR) of 13C and 29Si. Several compounds were detected in anhydrous ashes: amorphous silica (the main component), and minor quantities of crystalline silica (cristobalite and quartz), amorphous carbon and siloxane polymeric chains. Hardened pastes were prepared with a ratio water:calcium dioxide:ash O,47H20+O,53(O,1dioxide ash+O,9calcio)=1. The evolution of the hydration reaction was monitored at several ages between 8 to 134 days. The formation of C-S-H was detected by 29Si-NMR and the arrangement of the silicate groups was characterized. The structure of the C-S-H formed in these pastes agrees with the one observed in conventional cements and also b1ast furnace slag cements. Also, it is in agreement with the accepted structural models of C-S-H. The amount of C-S-H produced and the velocity of the reaction are minor than those observed in blast furnace slag cements. Carbonation effects were detected in ambient atmospheric conditions. Also, the effect of the hydration on the minority compounds was also detected.

Nous analysons les caractéristiques d'intrication de quelques matériaux à l'état solide ainsi que des systèmes particuliers d'atomes et de champs en interaction. Une étude détaillée de la riche structure de phase des modèles de spins de basse dimension, décrivant le minéral naturel d'azurite et les composés de coordination à base de cuivre, a révélé des régimes à comportement d'intrication des plus robustes. En utilisant l'approche des systèmes dynamiques, la structure de phase de certains modèles classiques en réseaux hiérarchiques (récursifs) a aussi été étudiée et, pour la première fois, la transition entre régime chaotique et régime périodique au moyen de la bifurcation tangente a été détectée.Nous présentons une description détaillée des propriétés d'intrication de trois atomes piégés dans la limite dispersive. Une relativement simple accordabilité de la force atomique d'interaction de ce système et son étroite relation aux problèmes de frustration magnétique est démontrée. Les effets de propagation de pulses laser intenses dans un système atomique de type [lambda] avec des forces d'oscillateurs différentes sont analysés. Les résultats obtenus sont d'extrême importance dans des problèmes d'information quantique, comme par exemple, dans l'analyse du mécanisme de transfert de population dans des milieux ayant les propriétés définies ci-avant. Enfin, nous avons analysé les effets dissipatifs dans un protocole de distillation de l'intrication à variable continue récemment proposé. Malgré des contraintes additionnelles sur les paramètres du protocole, il est encore possible d'implémenter ce schéma de distillation évoqué ci-avant dans les technologies émergentes. / The entanglement features of some solid state materials, as well as of particular systems of interacting atoms and fields are analyzed. A detailed investigation of the rich phase structure of low dimensional spin models, describing the natural mineral azurite and copper based coordination compounds, has revealed regimes with the most robust entanglement behavior. Using the dynamical system approach, the phase structure of some classical models on hierarchical (recursive) lattices has been also studied and, for the first time, the transition between chaotic and periodic regimes by means of tangent bifurcation has been detected.A detailed description of entanglement properties of three atoms trapped in a cavity within the dispersive limit is presented. A relatively simple tunability of the atomic interaction strength of the above system and its close relation to the problems of frustrated magnetism is shown. Furthermore, the propagation effects of two intense laser pulses in a medium of [lambda] atoms with unequal oscillator strengths are investigated. Obtained results are crucial in some problems of quantum information theory, as, e.g., in the analysis of population transfer mechanism in media possessing the above properties. Finally, the dissipation effects in a recently proposed compact continuous-variable entanglement distillation protocol have been analyzed. Despite additional constraints on the parameters of the protocol, the discussed entanglement distillation scheme in quantum memories is still possible to implement within emerging technologies.

Magnetic resonance imaging is a routine and powerful diagnostic technique capable of providing detailed information about the structure and composition of the tissues. This diploma thesis is concerned with the mechanisms of contrast origin and contrast modifications by molecular and nanoparticle contrast agents. First sections of the thesis summarize basic knowledge about pulse sequences and it aims to provide an overview on MRI contrast agent with a special emphasis on paramagnetic gadolinium contrast agents and superparamagnetic nanoparticles. The main purpose of this study is to develop the software called MRICalc, which is able to optimize contrast in MRI images. Based on analysis of signal formula of typical pulse sequences, MRICalc is able to propose the parameters of the pulse sequence for compartment-specific enhancement of the contrast. User chooses from the list of the samples and after calculation he obtains the values of echo time, repetition time and flip angle, all of which simultaneously seem to create the appropriate setting to enhance the contrast. MRICalc also allows to plot contrast function with respect to the chosen parameter. Software, including its graphical user interface, is designed in Python. The sample consists from solution of CuSO4 and distilled water was designed to verify the correct function of MRICalc. Sulphate represents a contrast agent. Preclinical MR system Bruker BioSpec 94/30 USR located at Institute of Scientific Instruments of the ASCR, v.v.i was used to measure contrast curve of FLASH pulse sequence, which is a typical representative of gradient echo. Results of the measurement were compared to the theoretical model provided by MRICalc.

In this work we studied magnetic properties of molecular magnets of the new heteropolyanion {Cu20}, dodecanuclear cluster {Ni12}, and the heterometallic {Cr7M} wheels, in which one of the CrIII ions of Cr8 has been replaced by a Fe, Cu, Zn, Ni, ion with this extra-spin acts as local probe for the spin dynamics.Such systems have been synthesized recently and they are well described using the Heisenberg spin Hamiltonian with a Zeeman term of an applied magnetic field along the z-axis. Using the numerical exact diagonalization method, we have calculated the energy spectrum and the eigenstates for different compounds,and we have used them for reexamining the available experimental susceptibility data to determine the values of exchange parameters.We have studied the thermodynamic properties such magnetization, susceptibility, heat-capacity. At low temperature regions molecular magnets act as individual quantum nanomagnets and can display super-paramagnetic phenomena like macroscopic quantum tunneling, ground state degeneracy, level-crossing. A crucial issue for understanding these phenomena is the coupling between magnetic molecular levels and the environment such as nuclear spins. We have modeled the behavior of the proton spin lattice relaxation rate as a function of applied magnetic field for low temperatures as it is measured in Nuclear Magnetic Resonance (NMR) experiments.

Conducting and semiconducting polymers, consisting of delocalized π-electrons, have been studied for the past three decades. These materials have shown novel physical properties with interesting applications in batteries, detectors, light emitting diodes, field effect transistors, solar cells, biosensors etc. Nevertheless the charge transport properties are yet to be understood in detail due to the complexity of the system, especially due to the interplay of quasi-one dimensionality (q-1D), disorder, localization and electron-electron interactions(EEI). A combined investigation of both conductivity and spin lattice relaxation time, especially at very low temperatures and high magnetic fields, is really lacking in conducting polymers. In this thesis a set of experiments – dc conductivity, magnetoresistance (MR), Nuclear Magnetic Resonance (NMR) spin lattice relaxation time (T1) measurements, magnetic susceptibility amd ac conductivity have been carried out in conducting polymers. NMR being a local probe it is possible to get the nanoscopic scale charge transport mechanism. Further, this helps to develop a consistent understanding among a wide range of the physical properties in conducting polymers. In this thesis author has reported the results of experiments at ultra low temperature (mk) and ultra high magnetic field which give more insight about the roles of electron-electron interaction(EEI) and disorderin charge transport properties. This thesis describes a detailed study of charge transport and NMR relaxation in three representative conducting polymers namely polypyrrole(PPy)., poly-3-methylthiophene(P3MT) and poly3-hexylthiophene(P3HT). The emphasis is to understand the charge transport phenomena and NMR relaxation, especially at ultra low temperatures (down to 20 mk) and high magnetic field (up to 23.4 T). The NMR T1 relaxation mechanisms are discussed in terms of (i) Korringa relaxation, (ii) relaxation due to spin diffusion to paramagnetic centers (SDPC) amd (iii) reorientation of symmetric groups, depending upon the temperature range.

In our pursuit of ever smaller transistors, with greater computational throughput, many questions arise about how material properties change with size, and how these properties may be modelled more accurately. Metallic nanocontacts, especially those for which magnetic properties are important, are of great interest due to their potential spintronic applications. Yet, serious challenges remain from the standpoint of theoretical and computational modelling, particularly with respect to the coupling of the spin and lattice degrees of freedom in ferromagnetic nanocontacts in emerging spintronic technologies. In this thesis, an extended method is developed, and applied for the first time, to model the interplay between magnetism and atomic structure in transition metal nanocontacts. The dynamic evolution of the model contacts emulates the experimental approaches used in scanning tunnelling microscopy and mechanically controllable break junctions, and is realised in this work by classical molecular dynamics and, for the first time, spin-lattice dynamics. The electronic structure of the model contacts is calculated via plane-wave and local-atomic orbital density functional theory, at the scalar- and vector-relativistic level of sophistication. The effects of scalar-relativistic and/or spin-orbit coupling on a number of emergent properties exhibited by transition metal nanocontacts, in experimental measurements of conductance, are elucidated by non-equilibrium Green’s Function quantum transport calculations. The impact of relativistic effects during contact formation in non-magnetic gold is quantified, and it is found that scalar-relativistic effects enhance the force of attraction between gold atoms much more than between between atoms which do not have significant relativistic effects, such as silver atoms. The role of non-collinear magnetism in the electronic transport of iron and nickel nanocontacts is clarified, and it is found that the most-likely conductance values reported for these metals, at first- and lastcontact, are determined by geometrical factors, such as the degree of covalent bonding in iron, and the preference of a certain crystallographic orientation in nickel. / Physics / Ph. D. (Physics)