We developed a model to investigate the dielectric properties of the BaTiO₃ − Bi(Zn₁/₂Ti₁/₂)O₃ (BT-BZT) solid solution, which is a relaxor ferroelectric and exhibits long range disorder. The model uses ab initio methods to determine all polarization states for every atomic configuration of 2 x 2 x 2 supercells of BT-BZT. Each supercell is placed on a lattice with an Ising-like interaction between neighboring cell polarizations. This method allows us to consider long range disorder, which is not possible with ab initio methods alone, and is required to properly understand relaxor ferroelectric materials. We analyze the Monte Carlo data for a single lattice configuration using the multiple histogram method, and develop a modified histogram technique to combine data from multiple lattice configurations. Our calculated values of dielectric constant, specific heat, and polarization agree reasonably well with experiment. / Graduation date: 2012

Made available in DSpace on 2014-12-17T14:55:13Z (GMT). No. of bitstreams: 1 JoemiaLGMM_TESE.pdf: 3140610 bytes, checksum: 8bdf88d29c888d95e74fd24e403e60fc (MD5) Previous issue date: 2013-06-07 / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior / Ceramic substrates have been investigated by researchers around the world and has achieved a high interest in the scientific community, because they had high dielectric constants and excellent performance in the structures employed. Such ceramics result in miniaturized structures with dimensions well reduced and high radiation efficiency. In this work, we have used a new ceramic material called lead zinc titanate in the form of Zn0,8Pb0,2TiO3, capable of being used as a dielectric substrate in the construction of various structures of antennas. The method used in constructing the ceramic combustion synthesis was Self- Sustained High Temperature (SHS - "Self-Propagating High-Temperature Synthesis") which is defined as a process that uses highly exothermic reactions to produce various materials. Once initiated the reaction area in the reaction mixture, the heat generated is sufficient to become self-sustaining combustion in the form of a wave that propagates converting the reaction mixture into the product of interest. Were analyzed aspects of the formation of the composite Zn0,8Pb0,2TiO3 by SHS powders and characterized. The analysis consisted of determining the parameters of the reaction for the formation of the composite, as the ignition temperature and reaction mechanisms. The production of composite Zn0,8Pb0,2TiO3 by SHS performed in the laboratory, was the result of a total control of combustion temperature and after obtaining the powder began the development of ceramics. The product was obtained in the form of regular, alternating layers of porous ceramics and was obtained by uniaxial pressing. 10 The product was characterized by analysis of dilatometry, X-ray diffraction analysis and scanning electron microscopy. One of the contributions typically defined in this work is the development of a new dielectric material, nevertheless presented previously in the literature. Therefore, the structures of the antennas presented in this work consisted of new dielectric ceramics based Zn0,8Pb0,2TiO3 usually used as dielectric substrate. The materials produced were characterized in the microwave range. These are dielectrics with high relative permittivity and low loss tangent. The Ansoft HFSS, commercial program employee, using the finite element method, and was used for analysis of antennas studied in this work / Substratos cer?micos t?m sido investigados por pesquisadores de todo o mundo e tem despertado um grande interesse na comunidade cient?fica, pelo fato de apresentarem altas constantes diel?tricas e um excelente desempenho nas estruturas empregadas. Tais cer?micas resultam em estruturas miniaturizadas, com dimens?es bem reduzidas e de alta efici?ncia de radia??o. Neste trabalho, utilizou-se um novo material cer?mico, chamado de titanato de zinco chumbo, na forma de Zn0,8Pb0,2TiO3, capaz de ser utilizado como substrato diel?trico na constru??o de diversas estruturas de antenas. O m?todo utilizado na constru??o da cer?mica foi a S?ntese por Combust?o Auto-Sustentada a Alta Temperatura (SHS Self-Propagating High-Temperature Synthesis ) que ? definido como um processo que utiliza rea??es altamente exot?rmicas para produzir os mais diversos materiais. Uma vez iniciada a rea??o numa ?rea da mistura reagente, o calor gerado ? suficiente para tornar a combust?o auto-sustent?vel, na forma de uma onda que se propaga convertendo a mistura reagente no produto de interesse. Foram analisados os aspectos da forma??o do comp?sito Zn0,8Pb0,2TiO3 por SHS e os p?s obtidos, foram caracterizados. A an?lise consistiu na determina??o dos par?metros da rea??o para a forma??o do comp?sito, como a temperatura de igni??o e os mecanismos de rea??o. A produ??o do comp?sito Zn0,8Pb0,2TiO3 por SHS, realizada em laborat?rio, foi resultado de um controle total da temperatura de combust?o e ap?s a obten??o do p? 8 iniciou-se o desenvolvimento das cer?micas. O produto foi obtido na forma de camadas regulares e altern?ncia de porosidades e as cer?micas foram obtidas por prensagem uniaxial. O produto foi caracterizado atrav?s de an?lises de dilatometria, difra??o de raios-X e an?lise de microscopia de varredura eletr?nica. Uma das contribui??es principais deste trabalho foi o desenvolvimento de um novo material diel?trico, n?o obstante apresentado anteriormente na literatura. Portanto, as estruturas das antenas apresentadas neste trabalho foram constitu?das por novas cer?micas diel?tricas ? base de Zn0,8Pb0,2TiO3, geralmente utilizado como substrato diel?trico. Os materiais desenvolvidos foram caracterizados na faixa de micro-ondas. S?o substratos diel?tricos de alta permissividade relativa e baixa tangente de perda. O software comercial empregado, Ansoft HFSS, baseado no m?todo dos elementos finitos, foi utilizado na an?lise das antenas estudadas neste trabalho

Submitted by Luciana Ferreira (lucgeral@gmail.com) on 2015-03-30T13:38:33Z No. of bitstreams: 3 1_pdfsam_Tese - Michelly Patrícia Santana de Almeida Fógia - 2014 - (1).pdf: 19290836 bytes, checksum: 2968ddb5cb0f3df6082b9b4716172cff (MD5) 109_pdfsam_Tese - Michelly Patrícia Santana de Almeida Fógia - 2014 - (2).pdf: 5395221 bytes, checksum: 4db4ad13c96adee2667748bc5321c48f (MD5) license_rdf: 23148 bytes, checksum: 9da0b6dfac957114c6a7714714b86306 (MD5) / Approved for entry into archive by Luciana Ferreira (lucgeral@gmail.com) on 2015-03-30T15:36:48Z (GMT) No. of bitstreams: 3 1_pdfsam_Tese - Michelly Patrícia Santana de Almeida Fógia - 2014 - (1).pdf: 19290836 bytes, checksum: 2968ddb5cb0f3df6082b9b4716172cff (MD5) 109_pdfsam_Tese - Michelly Patrícia Santana de Almeida Fógia - 2014 - (2).pdf: 5395221 bytes, checksum: 4db4ad13c96adee2667748bc5321c48f (MD5) license_rdf: 23148 bytes, checksum: 9da0b6dfac957114c6a7714714b86306 (MD5) / Made available in DSpace on 2015-03-30T15:36:48Z (GMT). No. of bitstreams: 3 1_pdfsam_Tese - Michelly Patrícia Santana de Almeida Fógia - 2014 - (1).pdf: 19290836 bytes, checksum: 2968ddb5cb0f3df6082b9b4716172cff (MD5) 109_pdfsam_Tese - Michelly Patrícia Santana de Almeida Fógia - 2014 - (2).pdf: 5395221 bytes, checksum: 4db4ad13c96adee2667748bc5321c48f (MD5) license_rdf: 23148 bytes, checksum: 9da0b6dfac957114c6a7714714b86306 (MD5) Previous issue date: 2014-09-24 / In this work the structural and optical properties of SiO2-ZnO-TiO2 system doped with of Eu3+ (1% in mol) or Er3+ ions (0,2% to 2,0% in mol) were investigated. The compositions xSiO2-([100-x]/2)ZnO-([100-x]/2)TiO2 with x ranging from 40 to 80 were synthesized and studied. A mixed methodology using the traditional sol-gel process and Pechini method was employed to prepare stable and transparent sols, homogeneous gels, powders and transparent thin films without cracks. The prepared powders were heat treated from 100°C to 1100°C. The optical “band gap” values, the lifetime of Eu3+ 5D0 level, the R/O ratio of Eu3+ emissions and refractive index are dependent on the composition and thermal treatment of the powders. Multilayered thin films were deposited onto silica substrates using the “spin coating” technique. Afterwards, the as-prepared thin films were calcined at 500°C followed by annealings from 700°C to 1000°C. The X-ray diffraction of powders showed that the crystallization starts at 800°C with a mixture of zinc titanate phases (ZnTiO3, Zn2TiO4) and titanium rutile (TiO2). In compositions with low silica content (x = 40 or 50) the formation of zinc silicate (Zn2SiO4) occurs at high temperatures. The optical properties were evaluated for both powders and thin films. Particularly, thin films exhibit transmittance above 80% in the visible region. The refractive index at 632.8 nm and thickness of thin films were estimated using the envelope method and m-Line spectrocopy. Furthermore, morphological analysis of the thin films surface was performed by scanning electron microscopy. The characteristic emission peaks of Er3+ or Eu3+ doped powders and thin films were measured. The photoluminescent emission of Eu3+ ions, obtained the highest intensities for the powders treated at 800°C, for films treated at 700°C, under excitation at 394 nm, where the system remains primarily amorphous. The photoluminescent emission of the Er3+ ions was more intense for the powders treated at 1100°C under excitation at 980 nm, mainly due to reduction of hydroxyl groups which act as photoluminescence quenchers. In the film the highest intensity occurred at a temperature of 700°C under excitation at 378 nm and showing only one guided mode. Thus, the obtained thin films can be suitable for application as waveguides in integrated optical systems. Moreover, the Eu and Er doped powders can be used as phosphors in displays. / Este trabalho avalia as propriedades estruturais e ópticas do sistema ternário SiO2-ZnO-TiO2 dopado com íons Eu3+ (1% em mol) ou Er3+ (0,2% a 2,0% em mol). As composições xSiO2-([100-x]/2)ZnO-([100-x]/2)TiO2, com x = 40, 50, 60, 70 e 80 foram estudadas. Através de metodologia mista do processo sol-gel com o método Pechini foi possível obter sóis estáveis e transparentes, géis homogêneos, pós tratados termicamente de 100ºC a 1100°C e filmes finos transparentes e sem trincas. Filmes finos multicamadas foram depositados sobre substratos de sílica usando “spin coating” e calcinados a 500°C, seguido de um tratamento térmico entre 700°C e 1000°C. Por fotoluminescência foram observadas as transições de emissão características de íons Er3+ e Eu3+. A caracterização por difração de raios X dos pós mostrou que a cristalização tem início a partir de 800°C, com uma mistura de fases de titanatos de zinco (ZnTiO3, Zn2TiO4) e segregação de titânio rutilo (TiO2). Em composições com menores proporções de sílica (x= 40 ou 50) também ocorreu a formação de silicato de zinco (Zn2SiO4) em temperaturas mais elevadas. Os espectros de transmissão dos filmes apresentaram transmitância superior a 80%. Os valores de “band gap” óptico, o tempo de vida, as razões R/O e o índice de refração são dependentes do tratamento térmico e da composição dos pós. Usando o método da envoltória, pôde-se calcular o índice de refração a 632,8 nm e a espessura dos filmes finos, sendo que esta também foi estimada por microscopia eletrônica de varredura (MEV) e espectroscopia m-Line. A emissão fotoluminescente dos íons Eu3+ tem maior intensidade nos pós tratados à 800°C e nos filmes tratados à 700°C, sob excitação a 394 nm. Nestas temperaturas o sistema permanece predominantemente amorfo. A emissão fotoluminescente dos íons Er3+ foi mais intensa para os pós tratados a 1100°C, sob excitação a 980 nm, devido à eliminação de grupos OH supressores das emissões de Er3+. Nos filmes a maior intensidade se deu à temperatura de 700°C, sob excitação a 378 nm. Os filmes apresentaram apenas um modo guiado, sendo o mais apropriado para uso como guia de onda e os pós são indicados como fósforos podendo ser aplicados em “displays".