DISSERTAÇÃO DE MESTRADO - PROGRAMA DE PÓS-GRADUAÇÃO EM FISICA

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    PROPRIEDADES DIELÉTRICAS DO Bi2Sn2O7 PURO E DOPADO COM MANGANÊS
    (Universidade Federal do Maranhão, 2010-11-26) Almeida, Rafael Mendonça; PASCHOAL, Carlos William de Araújo; CPF:46161286372; Feio, Waldeci Paraguassu; CPF:57387540268; http://lattes.cnpq.br/3512689932467320
    In this work we have investigated the dielectric and ionic properties of the pure Bi2Sn2O7 (BSO) and manganese doped ceramics in the temperature range from 23°C to 326°C. Amongst the main results of the BSO it is worthwhile to point out the PTCR ef-fect when it was analysed the temperature dependence of the electrical resistance. Furthermore, in both samples, the imaginary electrical modulus relaxational peaks are related to conductive processes, but only the BSO shows an anomaly in the tempera-ture range investigated. This anomaly is expressed with a displacement of the peaks to the region of low frequencies, as the temperature rises from the ambient value until 100°C, and after to the region of high frequencies, when the temperature changes from 100°C to 326°C. This dynamic of the data allowed to estimate the phase transition value as being equal to 121.5°C. It was also observed that this transition is possibly ferroic because the capacitance dependence with temperature shows a Curie like behaviour. By other side, the analysis of the real part of the electrical permittivity with temperature highlighted that the BSO phase transition point is located some-where around 125°C, while the one from BSO:Mn is around 120°C. The conductivity dependence with the reciprocal temperature showed an Arrhenius like behaviour and, from the mathematical adjustment at high temperatures, it was possible to estimate an activation energy of 1.26 eV. It was also found that the manganese doping inhibited the effect observed in the graphs of versus frequency, favored the conduction me-chanism of the system and preclude the PTCR effect. Analyzing the temperature de-pendence of the dielectric loss it was realized that this quantity also presents an ano-maly at around 120°C that can be assigned to the structural phase transition. Studying the real part of the admittance as function of the frequency, one could segregate the contributions from the bulk and grain boundary of the system and observe that the response of the last one exhibits a peak at 120°C, probably due to the transi-tion. Regarding the manganese ion substitution in the BSO structure, two hypotheses are proposed. It is believed that in both, the tin ion occurs with an oxidation state equal to 2+ and, but substituting either in the tin ion site or in the bismuth ion site, and releasing oxygen vacancies.
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    PROPRIEDADES VIBRACIONAIS E DIELÉTRICAS DA MULITA Bi2Mn4O10
    (Universidade Federal do Maranhão, 2010-11-30) Silva Júnior, Flávio Moura e; PASCHOAL, Carlos William de Araújo; CPF:46161286372
    In this work we investigated the vibrational properties of ceramics Bi2Mn4O10 (BMO) at room temperature by the Raman and Infrared spectroscopies, the phonons were classified by FG matrix method of Wilson. The dielectric properties of the material, in turn, were studied using the impedance spectroscopy in a range of 22 ° C to 275 ° C. Furthermore, static atomistic simulations were performed at BMO in the range 0.0 to 10 GPa with a step of 0.5 GPa. Concerning the Raman modes, ten out forty eight modes predicted by the group theory, were observed in our experimental spectrum while the spectrum of the imaginary part of inverse dielectric constant, we observe 19 LO modes active in infrared. By using the method of FG Wilson saw that the modes in the range of 600-760 cm-1 are stretching into the ab plane to the octahedral chains MnO6. Libration and bending modes were predicted to 400-570 cm-1 and 300-400 cm-1, respectively. It was further observed that the low-frequency modes are mainly due to translations of the Bi ions. The analysis of the impedance spectroscopy measurements led to the conclusion that the relaxing process of BMO are associated with conductive mechanisms, these being due to movement of polarons. The frequencies, for which the imaginary parts of the module (M '' ) and impedance ( Z '' ) exhibit a maximum, obeyed the Arrhenius law in its dependence on the reciprocal temperature, and the calculated activation energies were 0.57 eV and 0.63 eV for each case, respectively. The frequency dependent peaks that appeared in the Bode plot of the real part of dielectric constant were attributed to thermal relaxation processes associated with activated jumps of polarons. The simulations showed that the compound is quite stable, showing no structural phase transition in the pressure range investigated
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    PROPRIEDADES VIBRACIONAIS E TRANSIÇÃO DE FASE DO PIROCLORO Bi₂Sn₂O₇
    (Universidade Federal do Maranhão, 2012-03-28) Silva, Rosivaldo Xavier da; PASCHOAL, Carlos William de Araújo; CPF:46161286372; Batista, Jerias Alves; CPF:30447984549; http://lattes.cnpq.br/1319645549100341
    In this work we investigated the vibrational, structural and dielectric properties of pyrochlore Bi2Sn2O7 (BSO) by Raman spectroscopy, differential scanning calorimetry (DSC) and infrared specular reflectance. The Raman spectrum of BSO was obtained as a function of temperature in the range from 23°C to 427°C. It was observed 18 broad Raman bands at room temperature (α phase) which have been classified according to the literature. The investigation of the evolution of the position, width, integrated area and intensity on the Raman modes depending on the temperature allowed estimating the temperature of the structural transition BSO α ( ) → β ( ) by approximately 127°C. The thermogram obtained by DSC under heating rates of 10K/min and 20K/min showed a peak with onset enthalpy at 98°C. Such peak was associated with the loss of structural domains discussed in the literature. Furthermore, theoretical calculations indicate that the observed peak is related to a displacive phase transition. The infrared reflectance spectrum was obtained at room temperature in the range 60 4000 cm-1, whose setting allowed us to identify the frequencies of transverse and longitudinal optical phonons which were also classified based on the literature. It was estimated the static dielectric constant, the dielectric losses tanδј and quality factor Q for the BSO in the microwave region. The dispersion parameters numerically obtained by Kramers - Kronig show to be in agreement with results obtained from the reflectance fitting.