The high-frequency properties of coupled magnetic systems have been investigated using vector network analyzer ferromagnetic resonance (VNA-FMR) spectroscopy. SAF structures consist of two ferromagnetic layers separated by a non-magnetic spacer, coupled through the indirect exchange interaction. The ferromagnetic layers of our samples were composed of FeCoB separated by a layer of Ru. The thickness of Ru was varied in the range of 8 to 18 Å among the samples studied. Antiferromagnetic coupling can be quickly identified by the major hysteresis loop (MHL). A new way of displaying FMR data for these trilayer samples is presented which completely preserves the anisotropy effects while fully characterizing the angular dependence of FMR. The advantage of our representation is that the high-frequency data can be easily compared to the static switching behavior at any angle obtained through susceptibility measurements. Ferromagnetic resonance; Coupled; Synthetic antiferromagnet; Magnetization switching

Neste trabalho apresentamos estudos sobre a estrutura eletronica de impurezas isoladas e complexas em germanio as quais sao responsaveis pela introducao de niveis de energia profundos na banda proibida do semicondutor. O modelo utilizado e o do aglomerado molecular, dentro do formalismo autoconsistente do metodo do espalhamento multiplo-\'X IND.ALFA\' com o tratamento dos orbitais de superficie atraves da esfera de watson. Efeitos de polarizacao de spin e de relaxacao eletronica sao incluidos. Aplicamos o metodo para analisar impurezas isoladas de cobre substitucional (\'GE:\'cu ind.S\'); COBRE INTERSTICIAL (\'ge\':\'cu ind.I\') E DE LITIO INTERSTICIAL (\'ge\':\'li ind.I\') E AS IMPUREZAS COMPLEXAS DE COBRE SUBSTITUCIONAL - COBRE INTERSTICIAL (\'ge\':\'cu ind.I\'\'cu ind.S\') E COBRE SUBSTITUCIONAL - LITIO (\'ge\':\'li ind.I\'\'cu ind.S\'). Nossos resultados sao comparados com dados experimentais existentes na literatura / In this work we report results for the electronic structure of Isolated and complex impurities in Germanium which introduces deep leveis In the crystal band gap. The calculations are carried out by using the The theory-Scattering-X theory within the Watson-sphere-terminated molecular-cluster method. The self-constructive calculations are carried out by taking into account the spin-polarization and electronic relaxation effects. The following isolated and complex impurities are studied: substitutional Copper Interstitial Lithium Copper (Ge: Cu Cu); 1 s (Ge: Cu); S Interstitial Copper (Ge: Li); L Substitutional Copper Substitutional Copper Interstitial (Ge: Cu); 1 Interstitial Lithium (Ge: Li Cu). 1 s Our results are compared with experimental data in the literature.

Soft x-ray spectroscopy can provide a wealth of information on the electronic structure of solids. In this work, a suite of soft x-ray spectroscopies is applied to organic and inorganic materials with potential applications in electronic and energy generation devices. Using the techniques of x-ray absorption (XAS), x-ray emission spectroscopy (XES), and x-ray photoemission spectroscopy (XPS), the fundamental properties of these different materials are explored. Cycloparaphenylenes (CPPs) are a recently synthesized family of cyclic hydrocarbons with very interesting properties and many potential applications. Unusual UV/Visible fluorescence trends have spurred a number of theoretical investigations into the electronic properties of the CPP family, but thus far no comprehensive electronic structure measurements have been conducted. XPS, XAS, and XES data for two varieties, [8]- and [10]-CPP, are presented here, and compared with the results of relevant DFT calculations. Turning towards more application-centered investigations, similar measurements are applied to two materials commonly used in solid oxide fuel cell (SOFC) cathodes: La_(1−x)Sr_(x)MnO_(3) (LSMO) and La_(1−x)Sr_(x)Co_(1−y)Fe_(y)O_(3) (LSCF). Both materials are structurally perovskites, but they exhibit strikingly different electronic properties. SOFC systems very efficiently produce electricity by catalyzing reactions between oxygen and petroleum-based hydrocarbons at high temperatures (> 800 C). Such systems are already utilized to great effect in many industries, but more widespread adoption could be had if the cells could operate at lower temperatures. Understanding the electronic structure and operational evolution of the cathode materials is essential for the development of better low-temperature fuel cells. LSCF is a mixed ion-electron conductor which holds promise for low-temperature SOFC applications. XPS spectra of LSCF thin films are collected as the films are heated and gas-dosed in a controlled environment. The surface evolution of these films is discussed, and the effects of different gas environments on oxygen vacancy concentration are elucidated. LSMO is commonly used in commercial fuel cell devices. Here the resonant soft x-ray emission (RIXS) spectrum of LSMO is examined, and it is shown that the inelastic x-ray emission structure of LSMO arises from local atomic multiplet effects.

Estudamos o efeito do campo aleatório sobre um modelo de vidro de spin com interações de p spins de alcance infinito e distribuição de probabilidade gaussiana. O caso p = 2 corresponde ao modelo de Sherrington-Kirkpatrick na presença de um campo aleatório. O caso p \'SETA\' \'INFINITO\' corresponde ao REM (Random Energy Model) de Derrida na presença de um campo aleatório. Além da interação de p spins, consideramos a presença de interações uniformes ferro ou antiferromagnéticas de alcance infinito. Tanto no caso ferro quanto antiferromagnético, empregamos dois procedimentos para tratar o problema: o método de réplicas no ensemble canônico e o método da contagem de estados no ensemble microcanônico. No método de réplicas resolvemos o problema para qualquer valor de p tanto sem quebra da simetria de permutação entre réplicas, quanto com um passo de quebra de simetria de Parisi. Deste modo, recuperamos resultados conhecidos para alguns modelos já estudados na literatura. Em seguida, tomamos o limite p \'SETA\' \'INFINITO\' que fornece uma solução completa para o problema do REM na presença de um campo aleatório. No método da contagem de estados, aplicável apenas no limite p \'SETA\' \'INFINITO\', mostramos que podemos estender a solução de Derrida mesmo na presença de um campo aleatório. Isso nos permitiu fazer a contagem de estados evitando assim o problema da \"catástrofe da entropia negativa\" presenta na solução réplica simétrica. Além disso, mostramos que qualquer sistema que seja solúvel sem a interação aleatória de p spins continua solúvel na presença dessa interação no limite p \'SETA\' \'INFINITO\'. Portanto, concluímos que a interação aleatória de p spins é somente adicionar um carácter vidro de spin ao sistema. Obtivemos expressões gerais válidas para qualquer distribuição do campo aleatório, embora a análise numérica tenha sido restrita às distribuições duplo-delta e gaussiana. Estudamos a influência do campo aleatório sobre os diagramas de fases e, em particular, mostramos que podem surgir pontos tricríticos no caso de uma distribuição duplo-delta. / We studied the effect of a random field on spin-glass models with infinite-ranged p spin interactions with a Gaussian probability distribution. The case p = 2 corresponds to the Sherrington-Kirkpatrick model in the presence of a random field. The case p \'SETA\' \'INFINITO\' corresponds to the REM (Random Energy Model) introduced by Derrida in the presence of a random field. Besides the p-spin interactions we also included uniform infinite-ranged ferromagnetic and antiferromagnetic interactions. Both in the case of ferromagnetic and antiferromagnetic interactions we employed two different approaches: The replica method in the canonical ensemble and the method of counting of the states in the microcanonical ensemble. In the replica method we solved the problem for arbitrary p both in the case of replica symmetry and in the first step of Parisi\'s replica-symmetry breaking scheme. This allowed us to rederive results for some models already known in the Literature. Next we took the limit p \'SETA\' \'INFINITO\' which yielded a complete solution to the REM in a random field. In the method of counting of the states, which is effective only in the limit p \'SETA\' \'INFINITO\', we showed that we can extend the Derrida\'s solution even in the presence of a random field. This allowed us to do the counting of the states avoiding the so called negative-entropy catastrophe present in the replica-symmetric solution. We also showed that any solvable model without random p-spin interactions is also solvable in the presence of such interactions in the limit p \'SETA\' \'INFINITO\'. Therefore, we conclude that the p-spin random interactions only add a spin-glass character to the system. We have obtained general expressions valid for any random-field distributions, although we limited the numerical analysis to double-delta and Gaussian distributions. We studied the effects of the random field on the phase diagrams, and in particular, we showed the possibility of tricritical point in the case of double-delta distributions.

This thesis explores a range of photoactive metal halide perovskite materials for use in photovoltaic applications. These materials are of huge interest due to their outstanding optoelectronic properties which result in high photovoltaic power conversion efficiencies. In particular, this thesis discusses perovskites with stoichiometry ABX₃ where A is a singly charged cation, for example methylammonium (MA), B is predominantly lead (Pb²⁺), and X is iodide (I-) and/or bromide (Br^-). At present the commercial applications of these materials are limited by the chemical instability of the A-site cation. In this thesis, the effect of chemical substitution of the A-site is investigated as a way to increase the stability of the perovskite material. Full replacement with the inorganic cation caesium (Cs⁺) is shown to significantly improve the chemical stability. However, the inorganic lead halide perovskites with ideal bandgaps for photovoltaic applications exhibit structural instability. Routes to achieve both chemical and structural stability for these perovskites are discussed. Consequently, this thesis represents pioneering work in the field of inorganic halide perovskites and will greatly assist the development of stable inorganic perovskite materials for optoelectronic applications such as tandem photovoltaics and LEDs. Chapters 1 and 2 of this thesis present the motivation for perovskite materials to be used in solar cells, along with relevant background information about these materials and solar cell operation in general. Chapter 3 details the methods utilised in the experimental results chapters which follow. The first experimental results chapter, Chapter 4, shows how incorporation of Br^- in place of I^- in CsPbI₃ leads to increased ambient stability of the perovskite structure, and the first solar cells with CsPbI₂Br as the absorbing photovoltaic material are reported. Chapter 5 remedies the deficit of information about the optoelectronic properties of the CsPbI_3-xBr_x (0 ≤ x ≤ 3) perovskites through magneto-optical measurements on thin-films. These measurements raise questions about the room temperature perovskite structure of the CsPbI_3-xBrx compositions with small x, previously thought to be cubic perovskite, which is shown in Chapter 6 to be an orthorhombic perovskite polymorph. This finding motivates preliminary work presented in Chapter 7 aimed at chemical stabilisation of this orthorhombic perovskite polymorph. Finally, Chapter 8 summarises the work presented in this thesis, and recommends further research for the development of stable perovskite materials for photovoltaics.

We consider a series of problems regarding quantum Hall edges, focusing on both dynamics and the mathematical structure of edge states. We begin in Chapter 3 with a limiting case of the Laughlin state placed in a very steep confining potential, but which is weak compared to the interactions. We find that the eigenstates have a Jack polynomial structure and an energy spectrum which is extremely different from the well-known Luttinger liquid edge. In Chapter 5 we analyse the inner products of edge state wavefunctions, using an effective description given by a large-N expansion ansatz proposed by J. Dubail, N. Read and E. Rezayi, PRB 86, 245310 (2012). As noted by these authors, the terms in this ansatz can be constrained using symmetry, a procedure we perform to high orders. We then check the conjecture by calculating overlaps exactly for small system sizes and comparing the numerics with our high-order expansion to find excellent agreement. Finally, Chapter 6 considers the behaviour of quantum Hall edges close to the Luttinger liquid fixed point that occurs in the low energy, large system limit. We construct effective Hamiltonians using a local field theory description and then consider the effect of bulk symmetries on this edge. The symmetry analysis produces remarkable simplifications which allow for very accurate descriptions of the low-energy edge physics even relatively far away from the Luttinger liquid fixed point.

Neste trabalho apresentamos estudos sobre a estrutura eletronica de impurezas isoladas e complexas em germanio as quais sao responsaveis pela introducao de niveis de energia profundos na banda proibida do semicondutor. O modelo utilizado e o do aglomerado molecular, dentro do formalismo autoconsistente do metodo do espalhamento multiplo-\'X IND.ALFA\' com o tratamento dos orbitais de superficie atraves da esfera de watson. Efeitos de polarizacao de spin e de relaxacao eletronica sao incluidos. Aplicamos o metodo para analisar impurezas isoladas de cobre substitucional (\'GE:\'cu ind.S\'); COBRE INTERSTICIAL (\'ge\':\'cu ind.I\') E DE LITIO INTERSTICIAL (\'ge\':\'li ind.I\') E AS IMPUREZAS COMPLEXAS DE COBRE SUBSTITUCIONAL - COBRE INTERSTICIAL (\'ge\':\'cu ind.I\'\'cu ind.S\') E COBRE SUBSTITUCIONAL - LITIO (\'ge\':\'li ind.I\'\'cu ind.S\'). Nossos resultados sao comparados com dados experimentais existentes na literatura / In this work we report results for the electronic structure of Isolated and complex impurities in Germanium which introduces deep leveis In the crystal band gap. The calculations are carried out by using the The theory-Scattering-X theory within the Watson-sphere-terminated molecular-cluster method. The self-constructive calculations are carried out by taking into account the spin-polarization and electronic relaxation effects. The following isolated and complex impurities are studied: substitutional Copper Interstitial Lithium Copper (Ge: Cu Cu); 1 s (Ge: Cu); S Interstitial Copper (Ge: Li); L Substitutional Copper Substitutional Copper Interstitial (Ge: Cu); 1 Interstitial Lithium (Ge: Li Cu). 1 s Our results are compared with experimental data in the literature.

Este trabalho tem como objetivo o estudo das propriedades termoluminescentes de policristais de Aragonita, com o auxílio da técnica da Ressôncia do Spin Eletrônico (RSE); estudo este efetuado, visando a viabilidade da aragonita em ser utilizada na datação por Termoluminescência (TL) e RSE. A amostra estudada é uma deposição secundária de aragonita, na forma de um espeleotema, que foi retirado da Caverna do Diabo, Estado de São Paulo. Foram analisadas a estabilidade térmica dos picos TL e dos sinais de RSE, o comportamento dos mesmos mediante a irradiação com raios gamae cinética que envolve a emissão TL da amostra correlacionando-os com os centros RSE. A curva de emissão termoluminescente da amostra natural consiste de dois picos a 530 e 590 K, quando a amostra natural é irradiada com raios gama, observamos mais dois picos a temperaturas menores 405 e 485 K. Um tratamento térmico a temperatura de 653 K por 10 min e posterior irradiação com raios - gama, induz o crescimento do pico de 485 K. Todos os picos seguiram o modelo monoenergético da cinética de segunda ordem. Os sinais de RSE da aragonita foram identificados e os valores de g obtidos foram: g = 1,998, 2002, 2,003, 2,005, 2,007 e 2,016 esses sinais foram identificados com os centros \'C\'\'O POT. -, IND. 3\',\'C\'\'O POT. -3, IND. 3\',\'C\'\'O POT. -, IND. 2\',\'PB POT. 3+\'. Através de medidas de decaimento térmico dos sinais de RSE, relacionamos os mesmos com os picos TL da amostra e concluímos que os picos de menor temperatura (380, 405, 415, 480 K) provavelmente têm como centro de recombinação TL o \'PB POT. 3+\' e o \'C\'\'O POT. -, IND. 3\', como centro TL o \'C\'\'O POT. -, IND. 2\'. Os picos de alta temperatura o centro de recombinação TL seria o \'C\'\'O POT. -, IND. 3\' e o centro TL \'C\'\'O POT. -3, IND. 3\', estes resultados são baseados em um modelo qualitativo elaborado por Calderon et al, 1984, para amostras de calcita. Este modelo está de acordo com a hipótese da cinética de segunda ordem. Um valor preliminar da idade da amostra foi encontrada I = 4 x \'10 POT. 6\' anos, pelo método da datação por TL, considerando os resultados concluímos que a aragonita poderá ser uma amostra viável para a datação por TL. / Thermoluminescence and ESR properties of aragonite cristals were studied for dating purpose. The sample was a speleothem and it was collected from \"Devil Cave\", State of São Paulo. Natural sample has a TL emission curve with two peaks at 530 and 590 K. The irradiated sample ( gama- rays) has four peaks at 405, 485, 530, 590 K; and the pre-anneal and subsequent irradiation induced the increase of 485 K peak, and two news peaks at 380 and 415 K. Ali the peaks were fitted reasonably well with second - order kinetics model. The g-values of ESR signals was determined (g = 1.998, 2.002, 2.003, 2.005, 2.007, 2.016) and they were related to \'C\'\'O POT. -, IND. 3\',\'C\'\'O POT. -3, IND. 3\',\'C\'\'O POT. -, IND. 2\' and \'PB POT. 3+\' An isochronal thermal anneal sequence experiment indicates that \'PB POT. 3+\' and \'C\'\'O POT. -, IND. 3\' centres are related to low temperature peaks (380, 405, 415 and 480 K). The \'C\'\'O POT. -, IND. 2\' and \'C\'\'O POT. -, IND. 3\'- centres are correlated to high temperature peaks (590, 595K). Calderon et al, 1984 proposed a model that explains the mechanism of TL processes in calcite. This model applied to aragonite shows that \'PB POT. 3+\'and \'C\'\'O POT. -, IND. 3\' holes centres are the TL recombination centres and why one assumes electrons come from \'C\'\'O POT. -, IND. 2\' and \'C\'\'O POT. -3, IND. 3\' - centres. This model can explain second order kinetics for TL peaks. An age I = 4 x \'10 POT. 6\' years was obtained using TL dating method. We conclude that the aragonite can be used by TL dating method.

abstract: The rigidity of a material is the property that enables it to preserve its structure when deformed. In a rigid body, no internal motion is possible since the degrees of freedom of the system are limited to translations and rotations only. In the macroscopic scale, the rigidity and response of a material to external load can be studied using continuum elasticity theory. But when it comes to the microscopic scale, a simple yet powerful approach is to model the structure of the material and its interparticle interactions as a ball$-$and$-$spring network. This model allows a full description of rigidity in terms of the vibrational modes and the balance between degrees of freedom and constraints in the system. In the present work, we aim to establish a microscopic description of rigidity in \emph{disordered} networks. The studied networks can be designed to have a specific number of degrees of freedom and/or elastic properties. We first look into the rigidity transition in three types of networks including randomly diluted triangular networks, stress diluted triangular networks and jammed networks. It appears that the rigidity and linear response of these three types of systems are significantly different. In particular, jammed networks display higher levels of self-organization and a non-zero bulk modulus near the transition point. This is a unique set of properties that have not been observed in any other types of disordered networks. We incorporate these properties into a new definition of jamming that requires a network to hold one extra constraint in excess of isostaticity and have a finite non-zero bulk modulus. We then follow this definition by using a tuning by pruning algorithm to build spring networks that have both these properties and show that they behave exactly like jammed networks. We finally step into designing new disordered materials with desired elastic properties and show how disordered auxetic materials with a fully convex geometry can be produced. / Dissertation/Thesis / Doctoral Dissertation Physics 2018

Este trabalho tem como objetivo o estudo das propriedades termoluminescentes de policristais de Aragonita, com o auxílio da técnica da Ressôncia do Spin Eletrônico (RSE); estudo este efetuado, visando a viabilidade da aragonita em ser utilizada na datação por Termoluminescência (TL) e RSE. A amostra estudada é uma deposição secundária de aragonita, na forma de um espeleotema, que foi retirado da Caverna do Diabo, Estado de São Paulo. Foram analisadas a estabilidade térmica dos picos TL e dos sinais de RSE, o comportamento dos mesmos mediante a irradiação com raios gamae cinética que envolve a emissão TL da amostra correlacionando-os com os centros RSE. A curva de emissão termoluminescente da amostra natural consiste de dois picos a 530 e 590 K, quando a amostra natural é irradiada com raios gama, observamos mais dois picos a temperaturas menores 405 e 485 K. Um tratamento térmico a temperatura de 653 K por 10 min e posterior irradiação com raios - gama, induz o crescimento do pico de 485 K. Todos os picos seguiram o modelo monoenergético da cinética de segunda ordem. Os sinais de RSE da aragonita foram identificados e os valores de g obtidos foram: g = 1,998, 2002, 2,003, 2,005, 2,007 e 2,016 esses sinais foram identificados com os centros \'C\'\'O POT. -, IND. 3\',\'C\'\'O POT. -3, IND. 3\',\'C\'\'O POT. -, IND. 2\',\'PB POT. 3+\'. Através de medidas de decaimento térmico dos sinais de RSE, relacionamos os mesmos com os picos TL da amostra e concluímos que os picos de menor temperatura (380, 405, 415, 480 K) provavelmente têm como centro de recombinação TL o \'PB POT. 3+\' e o \'C\'\'O POT. -, IND. 3\', como centro TL o \'C\'\'O POT. -, IND. 2\'. Os picos de alta temperatura o centro de recombinação TL seria o \'C\'\'O POT. -, IND. 3\' e o centro TL \'C\'\'O POT. -3, IND. 3\', estes resultados são baseados em um modelo qualitativo elaborado por Calderon et al, 1984, para amostras de calcita. Este modelo está de acordo com a hipótese da cinética de segunda ordem. Um valor preliminar da idade da amostra foi encontrada I = 4 x \'10 POT. 6\' anos, pelo método da datação por TL, considerando os resultados concluímos que a aragonita poderá ser uma amostra viável para a datação por TL. / Thermoluminescence and ESR properties of aragonite cristals were studied for dating purpose. The sample was a speleothem and it was collected from \"Devil Cave\", State of São Paulo. Natural sample has a TL emission curve with two peaks at 530 and 590 K. The irradiated sample ( gama- rays) has four peaks at 405, 485, 530, 590 K; and the pre-anneal and subsequent irradiation induced the increase of 485 K peak, and two news peaks at 380 and 415 K. Ali the peaks were fitted reasonably well with second - order kinetics model. The g-values of ESR signals was determined (g = 1.998, 2.002, 2.003, 2.005, 2.007, 2.016) and they were related to \'C\'\'O POT. -, IND. 3\',\'C\'\'O POT. -3, IND. 3\',\'C\'\'O POT. -, IND. 2\' and \'PB POT. 3+\' An isochronal thermal anneal sequence experiment indicates that \'PB POT. 3+\' and \'C\'\'O POT. -, IND. 3\' centres are related to low temperature peaks (380, 405, 415 and 480 K). The \'C\'\'O POT. -, IND. 2\' and \'C\'\'O POT. -, IND. 3\'- centres are correlated to high temperature peaks (590, 595K). Calderon et al, 1984 proposed a model that explains the mechanism of TL processes in calcite. This model applied to aragonite shows that \'PB POT. 3+\'and \'C\'\'O POT. -, IND. 3\' holes centres are the TL recombination centres and why one assumes electrons come from \'C\'\'O POT. -, IND. 2\' and \'C\'\'O POT. -3, IND. 3\' - centres. This model can explain second order kinetics for TL peaks. An age I = 4 x \'10 POT. 6\' years was obtained using TL dating method. We conclude that the aragonite can be used by TL dating method.