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Ferroelectrics are dielectric materials possessing a switchable spontaneous polarization, which have attracted a growing interest for a broad variety of applications such as ferroelectric lithography, artificial photosynthesis, random and dynamic access memories (FeRAMs and DRAM), but also for the fabrication of devices for nonlinear optics, etc. All the aforementioned applications rely on the control of the ferroelectric domains arrangement, or the charge distribution and transport. In this regard, the main prerequisite is the engineering of the spontaneous polarization, obtained by reversing its orientation or locally inhibiting it. In the latter case, the interface created by the spatial discontinuity of the spontaneous polarization generates local charge accumulation, which can be used to extend the capabilities of ferroelectric materials. This thesis shows how engineering the spontaneous polarization in lithium niobate (LN) by means of proton exchange (PE), a temperature-activated ion exchange process, can be used to develop novel approaches for ferroelectric domain structuring, as well as fabrication of self-assembled nanostructures and control of ionic/electronic transport in this crystal. In particular, it is shown how the electrostatic charge at PE:LN junctions lying below the crystal surface can effectively counteract lateral domain broadening, which in standard electric field poling hampers the fabrication of ferroelectric gratings for Quasi-Phase Matching with periods shorter than 10 μm. By using such an approach, ferroelectric gratings with periods as small as ~ 8 μm are fabricated and characterized for efficient nonlinear optical applications. The viability of the approach for the fabrication of denser gratings is also investigated.  The charge distribution at PE:LN junctions lying on the crystal surface is modelled and used to drive the deposition of self-assembled nanowires by means of silver photoreduction. Such a novel approach for PE lithography is characterized for different experimental conditions. The results highlight a marked influence of the orientation of the spontaneous polarization, the deposition times, as well as the reactants concentrations and the doping of the substrate with MgO. Based on the fact that proton exchange locally reduces the spontaneous polarization, a quick and non-destructive method for imaging PE regions in lithium niobate with nanoscale resolution is also developed by using Piezoresponse Force Microscopy. Moreover the relative reduction of the piezoelectric d33 coefficient associated to PE is estimated in lithium niobate substrates with and without MgO-doping. Finally, by using advanced Scanning Probe Microscopy techniques, the features of charge transport in PE regions are further investigated with nanoscale resolution. A strong unipolar response is found and interpreted in light of ionic-electronic motion coupling due to the interplay of interstitial protons in the PE regions, nanoscale electrochemical reactions at the tip-surface interface, and rectifying metal-PE junctions. / <p>QC 20150325</p>

Multiferroics (MF) have attracted much research attention due to the coexistence of ferroelectric and magnetic ordering as well as magnetoelectric (ME) coupling. At present there are very few room temperature single phase MF except BiFeO3. Multiferroic properties of Aurivillius compound Bi5FeTi3O15 were reported at 80 K. The at 80 K. The at 80 K. The at 80 K. The at 80 K. The magnetization of Bi5FeTi3O15 was significantly improved by substituting parts of Fe cations by Co cations. Bi5FeTi3O15 showed ferromagnetic order above room temperature. The magnetic cations Fe/Co in B-site contribute to the both ferroelectric and ferromagnetic properties, which could possibly induce strong magnetoelectric effect. Aurivillius materials are layered structured materials with formula (Bi (Bi2O2)2+ (A m-1BmO3m+1 )2-. The polarization of Aurivillius materials is mainly in a-b plane . High dense and textured ceramics were fabricated by a two-step spark plasma sintering (SPS) method to improve the polarization of ceramics. The multiferroic properties of of Aurivillius materials with different octahedral layers (m=2, 3, 4 and 5) were investigated. All these materials showed ferroelectric and ferromagnetic order at room temperature except Bi 3Nb 1.1251.1251.1251.1251.125Fe 0.1250.1250.1250.1250.125Co 0.1250.1250.1250.1250.125Ti 0.750.750.750.75O9 (m = 2). (m = 2). (m = 2). (m = 2). (m = 2). Bi 3.253.253.253.25La 0.750.750.750.75Nb 0.250.250.250.25Fe 0.1250.1250.1250.1250.125Co 0.1250.1250.1250.1250.125Ti 2.52.52.5O12 (m = 3) was identified to be single phase. (m = 3) was identified to be single phase. Although a small amount of secondary phase (CoFe (CoFe2O4/Co /Co2FeOFeOFeO4) were found in Bi 4.254.254.254.25La 0.750.750.750.75Fe 0.50.50.5Co 0.50.50.5Ti 3O15 (m = 4) and Bi 5.25.25.25La 0.750.750.750.75FeCoTiFeCoTiFeCoTiFeCoTi FeCoTi3O18 (m = 5), ), the intrinsic multiferroicity of the main Aurivillius phase was confirmed by the magnetic controlled ferroelectric domain switching. Clear ME couplings were observed in these materials.

In this work, I start by introducing a relatively recently innovated thin film architecture which offers a new direction in strain control, the vertically aligned nanocomposite (VAN). I first present the literature in the field, explaining the advantages and unique novel properties stemming from VAN structures. Next, I introduce the work I did to examine the unique strain states of Ba0.6Sr0.4TiO3–Sm2O3 VAN structures. It was found that the strain states in the functional Ba0.6Sr0.4TiO3 phase are unconventional compared to those in planar thin films. 3-dimensional strain was found to be acting on the Ba0.6Sr0.4TiO3 phase in the VAN structure. The origin of the strain was explained using a simple model which takes into account thermal expansion mismatch as well as lattice mismatch and elastic coefficients. The ferroelectric properties of the films were presented in relation to the observed strain states. I next present the work I did on the influence of strain on the magnetic properties in VAN film of Sm0.34Sr0.66MnO3–Sm2O3. Ferromagnetism was achieved in an otherwise antiferromagnetic Sm0.34Sr0.66MnO3. The effect was explained by a strain induced transition from super-exchange to double exchange coupling in the material. Last but not least, the potential of scalability of VAN films was explored by using sputtering to grow VAN structures instead of the commonly-used PLD growth. BaTiO3–Sm2O3 was used as a primary study material due to its well reported VAN properties. Preliminary results showing indications of a VAN structure. Some basic physical property characterization is also presented and compared to the properties of PLD-grown films in the literature. Limitations and challenges that arise due to the fundamental differences between sputtering and PLD are also described.

High quality epitaxial thin films oflead magnesium niobate -lead titanate (PMN0.35PT) were deposited on MgAh04 substrates in the (001) direction with a lattice mismatch of less than 2%. Characterization by transmission electron microscopy and xray diffraction, has revealed high quality single crystal epitaxial thin films oriented in the (001) direction with a tetragonal unit cell. Capacitance measurements were completed by interdigital dielectrometry and using Finite Element Modeling the dielectric constant for the thin film yielded values ranging from 561 -799 at lk:Hz and 518-746 at 100kHz when the temperature was varied from 273-473K. Additionally, the dielectric maximum has been shifted to higher temperature and the frequency dispersion of the dielectric constant appears to be minimized. Piezoresponse microscopy and transmission electron microscopy was completed on both single and multilayer heterostructures. Transmission electron microscopy shows that the single layer samples show excellent morphology with single crystal epitaxial growth in the (001) direction. In addition piezoresponse microscopy and TEM have elucidated the difficulty in producing high quality films of PMN-0.35PT with a BaNb0.5Ti0.503 bottom electrode. The tendency for columnar growth of BaNb0.5Ti0.503 establishes an environment for polycrystalline growth drastically reducing the probability of single crystal growth in subsequent layers. Finally, piezoresponse microscopy allowed the observation of self polarization in PMN-0.35PT within the polycrystalline films which is in agreement with observations of previous researchers. / Thesis / Master of Applied Science (MASc)

Made available in DSpace on 2014-06-11T19:31:03Z (GMT). No. of bitstreams: 0 Previous issue date: 2011-12-05Bitstream added on 2014-06-13T20:41:14Z : No. of bitstreams: 1 lima_ec_dr_ilha.pdf: 2673140 bytes, checksum: 4fe5d64f1442666680854f09eb619017 (MD5) / Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) / O sistema ferroelétrico PbZr1-xTixO3 (PZT) vem sendo amplamente estudado devido às interessantes propriedades físicas para composições próximas ao Contorno de Fases Morfotrópico (CFM). A compreensão da fenomenologia de filmes ferroelétricos está atualmente sob intensa investigação, pois o fenômeno da ferroeletricidade exibe uma dependência intrínseca com relação à dimensão das amostras. O processamento de filmes é muito importante para o desenvolvimento da miniaturização de dispositivos eletrônicos com baixo consumo de energia e baixa tensão de operação. Desta forma, os métodos químicos tem tido grande evolução com respeito à obtenção de filmes com boa homogeneidade e cristalinidade. As temperaturas de pirólise e de cristalização desempenham um papel fundamental na cristalinidade dos filmes. Devido às altas temperaturas de obtenção dos filmes produzidos com os métodos químicos, a volatilidade do óxido de chumbo no sistema PZT torna-se um problema fundamental para discussão. Esta observação evidenciou a presença de uma fase indesejada intitulada pirocloro. A resposta dielétrica e ferroelétrica dos filmes obtidos com a fase pirocloro revela uma degradação destas propriedades. Para contornar o problema várias hipóteses foram testadas a fim de encontrar um meio para supressão da fase pirocloro. Desta forma, a síntese dos filmes foi empregada de forma a estudar o desempenho do excesso de óxido de chumbo em função da temperatura de pirólise para diferentes substratos. A transformação da fase pirocloro para perovskita foi reportada em função da temperatura de pirólise. Diferentes técnicas experimentais foram utilizadas neste estudo visando mapear a estrutura cristalina de longo e curto alcance ao longo da espessura dos filmes, o stress/strain residual em torno da interface... / The system ferroelectric PbZr1-xTixO3 (PZT) has been widely studied due to interesting physical properties for compositions near the Morphotropic Phase Boundary (MPB). The understanding of the phenomenology of ferroelectric films is currently under intense investigation, because the phenomenon of ferroelectricity shows an intrinsic dependence with respect to sample size. The film processing is very important for the development of miniaturization of electronic devices with low power consumption and low voltage operation. Therefore, chemical methods have had great progress with respect to obtaining films with good homogeneity and crystallinity. The pyrolysis temperature and crystallization play a key role in the crystallinity of the films. Due to high temperatures for obtaining films with chemical methods, the volatility of lead oxide in the PZT system becomes a fundamental problem for discussion. This observation revealed the presence of an unwanted entitled pyrochlore phase. The ferroelectric and dielectric response of the films obtained with the pyrochlore phase shows a degradation of these properties. To overcome this problem several hypotheses were tested in order to find a way to suppress the pyrochlore phase. Thus, the synthesis of the films was employed in order to study the performance of the excess lead oxide as a function of pyrolysis temperature for different substrates. The transformation of pyrochlore to perovskite phase was reported as a function of pyrolysis temperature. Different experimental techniques were used in this study to map the crystal structure of long and short range along the different thicknesses of the films, the stress/strain residual around the interface film/substrate, morphology, electrical properties, piezoelectric and ferroelectric films. The integrated analysis of the results aims to understand the phenomenology associated with the origins of self-polarization in ferroelectric thin films

Orientador: Eudes Borges de Araújo / Banca: José de los Santos Guerra / Banca: Keizo Yukimitu / Banca: Antonio Sergio Bezerra Sombra / Banca: José Antonio Eiras / Resumo: O sistema ferroelétrico PbZr1-xTixO3 (PZT) vem sendo amplamente estudado devido às interessantes propriedades físicas para composições próximas ao Contorno de Fases Morfotrópico (CFM). A compreensão da fenomenologia de filmes ferroelétricos está atualmente sob intensa investigação, pois o fenômeno da ferroeletricidade exibe uma dependência intrínseca com relação à dimensão das amostras. O processamento de filmes é muito importante para o desenvolvimento da miniaturização de dispositivos eletrônicos com baixo consumo de energia e baixa tensão de operação. Desta forma, os métodos químicos tem tido grande evolução com respeito à obtenção de filmes com boa homogeneidade e cristalinidade. As temperaturas de pirólise e de cristalização desempenham um papel fundamental na cristalinidade dos filmes. Devido às altas temperaturas de obtenção dos filmes produzidos com os métodos químicos, a volatilidade do óxido de chumbo no sistema PZT torna-se um problema fundamental para discussão. Esta observação evidenciou a presença de uma fase indesejada intitulada pirocloro. A resposta dielétrica e ferroelétrica dos filmes obtidos com a fase pirocloro revela uma degradação destas propriedades. Para contornar o problema várias hipóteses foram testadas a fim de encontrar um meio para supressão da fase pirocloro. Desta forma, a síntese dos filmes foi empregada de forma a estudar o desempenho do excesso de óxido de chumbo em função da temperatura de pirólise para diferentes substratos. A transformação da fase pirocloro para perovskita foi reportada em função da temperatura de pirólise. Diferentes técnicas experimentais foram utilizadas neste estudo visando mapear a estrutura cristalina de longo e curto alcance ao longo da espessura dos filmes, o stress/strain residual em torno da interface... (Resumo completo, clicar acesso eletrônico abaixo) / Abstract: The system ferroelectric PbZr1-xTixO3 (PZT) has been widely studied due to interesting physical properties for compositions near the Morphotropic Phase Boundary (MPB). The understanding of the phenomenology of ferroelectric films is currently under intense investigation, because the phenomenon of ferroelectricity shows an intrinsic dependence with respect to sample size. The film processing is very important for the development of miniaturization of electronic devices with low power consumption and low voltage operation. Therefore, chemical methods have had great progress with respect to obtaining films with good homogeneity and crystallinity. The pyrolysis temperature and crystallization play a key role in the crystallinity of the films. Due to high temperatures for obtaining films with chemical methods, the volatility of lead oxide in the PZT system becomes a fundamental problem for discussion. This observation revealed the presence of an unwanted entitled pyrochlore phase. The ferroelectric and dielectric response of the films obtained with the pyrochlore phase shows a degradation of these properties. To overcome this problem several hypotheses were tested in order to find a way to suppress the pyrochlore phase. Thus, the synthesis of the films was employed in order to study the performance of the excess lead oxide as a function of pyrolysis temperature for different substrates. The transformation of pyrochlore to perovskite phase was reported as a function of pyrolysis temperature. Different experimental techniques were used in this study to map the crystal structure of long and short range along the different thicknesses of the films, the stress/strain residual around the interface film/substrate, morphology, electrical properties, piezoelectric and ferroelectric films. The integrated analysis of the results aims to understand the phenomenology associated with the origins of self-polarization in ferroelectric thin films / Doutor

This thesis discusses the investigation and development of design methodologies for the creation of multifunctional band-pass filters capable of tuning to different frequency bands as well as varying their fractional bandwidth. This research also studies polynomial synthesis procedures as a tool for the derivation of reconfigurable planar filters with advanced asymmetrical responses. The work presented here relates to the evolving multifunction philosophy of RF systems. This analysis presents a comprehensive study of microwave resonators, which generate reliable and scalable filter topologies with tunable properties. The study includes the analysis of single, dual and triple-mode filters together with an investigation of the coupling behavior of synchronously and asynchronously tuned resonators. This study identified the main properties responsible for frequency and bandwidth control in a filter, and consequently systematically created innovative design techniques. The research also deals with the development of synthesis procedures for filters with advanced asymmetrical responses. The main goal of this effort is the creation of planar reconfigurable filters with arbitrary assigned transmission zeros. These advanced realizations requite meeting complex design specifications of advanced systems in both commercial and military applications. This work involves an in-depth investigation of polynomial synthesis methods for filters with crossed-coupled resonators and fully canonical form realizations using topologies with source and load coupling.