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Study of phase-matching geometries in bulk and periodically-poled lithium niobate and their use in intracavity terahertz optical parametric oscillatorsThomson, Caroline L. January 2012 (has links)
This thesis describes the experimental implementation of novel intersecting cavity terahertz optical parametric oscillators based on bulk and periodically-poled magnesium oxide-doped lithium niobate. Both collinear and non-collinear phase-matching geometries have been demonstrated and injection-seeding has been implemented in devices using periodically-poled material to reduce threshold and increase the down-conversion efficiency. A comprehensive characterisation of the original intracavity terahertz OPO was undertaken, which revealed the parameters having the greatest impact on OPO efficiency (idler mirror reflectivity and cavity length) and led to a better understanding of the losses in the system. During the characterisation process, generation of further terahertz radiation at the same frequency as that generated by the parametric process was observed and identified as being a result of difference frequency generation (DFG) between the parametrically-generated idler and terahertz waves. This phenomenon had previously only been observed when periodically-poled materials were employed in the system. The effect of this additional DFG process has been analysed in terms of the enhancement of the terahertz field on the basis of the coupled wave equations and physically measured quantities. The use of periodically-poled lithium niobate has been a major part of the research presented in this thesis. A comprehensive study of the modified phase-matching conditions was carried out and both collinear and novel hybrid non-collinear phase-matching geometries were identified. Several computer models were developed to assess the performance of any given grating design in these different geometries and the effects of temperature tuning and pump wavelength variation were also investigated using the models. Experimental studies confirmed the viability of the modelling approach but material limitations (particularly the early onset of crystal damage) limited the outcomes of the experiments. A detailed comparison of the poled and bulk materials was made to highlight the present drawbacks of the poled material. Finally, injection seeding was used to improve the efficiency of the collinear phase-matched PPLN OPOs. When seeding was used the depletion of the pump pulse was increased to the point of being measurable, reaching an upper level of 10%. Coupling constraints placed on the seed laser limited the amount of depletion attained. The potential for injection seeding to be used in the hybrid non-collinear phase-matching scheme was also identified but not realised during the course of this work. Were this technique successful, the tuning range of the intersecting cavity terahertz OPO could be extended to encompass the sub-1THz region, something that has previously been limited by the available idler cavity angles.
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Efficient Resonantly Enhanced Mach-Zehnder Optical Modulator on Lithium NiobateNguyen, Giang Thach, thach.nguyen@rmit.edu.au January 2006 (has links)
Photonic links have been proposed to transport radio frequency (RF) signals over optical fiber. External optical modulation is commonly used in high performance RF-photonic links. The practical use of optical fiber to transport RF signals is still limited due to high RF signal loss. In order to reduce the RF signal loss, highly efficient modulators are needed. For many applications, modulators with broad bandwidths are required. However, there are applications that require only a narrow bandwidth. For these narrow-band applications, the modulation efficiency can be improved through the resonant enhancement technique at the expense of reduced bandwidth. The aim of this thesis is to investigate highly efficient Mach-Zehnder optical modulators (MZMs) on Lithium Niobate (LiNbO3) with resonant enhancement techniques for narrow-band RF-photonic applications. This work focuses in particular on analyzing the factors that affect the modulation efficiency through resonant enhancement so that the modulator electrode structure can be optimized for maximum modulation efficiency. A parameter study of the effects of the electrode characteristics on the modulation efficiency of resonantly enhanced modulators (RE-MZM) is provided. From this study, optimum design objectives are identified. Numerical optimization is employed to explore the design trade-offs so that optimal configurations can be found. A sensitivity analysis is carried out to assess the performance of optimal RE-MZMs with respect to the variations of fabrication conditions. The results of these investigations indicate that the RE-MZM with a large electrode gap is the optimal design since it provides high modulation efficiency although the inherent switching voltage is high, and is the most tolerant to the fabrication fluctuations. A highly efficient RE-MZM on X-cut LiNbO3 is practically demonstrated with the resonant enhancement factor of 5 dB when comparing to the unenhanced modulator with the same electrode structure and effective switching voltage of 2 V at 1.8 GHz. The performance of the RF-photonic link using the fabr icated RE-MZM is evaluated. Optimization of RE-MZMs for operating at millimeter-wave frequencies is also reported. Factors that limit the modulation efficiency of an RE-MZM at millimeter-wave frequencies are identified. Novel resonant structures that can overcome these limitations are proposed. Preliminary designs indicate that greatly improved modulation efficiency could be expected.
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Growth and Applications of Periodically Poled Lithium Niobate Crystal FibersLee, Li-Min 07 September 2010 (has links)
¡@¡@We integrated the laser-heated pedestal growth (LHPG) system with accurately controlled electrodes to build up our in situ poling system. The ZnO and MgO doped periodically poled lithium niobate crystal fiber were fabricated with the poling system. This poling system has the advantage of convenience and fast growth, but the ¡§screen effect¡¨ caused by free charges which exist near the molten zone must be eliminated. The micro swing resulted from the electric force is a feasible solution, because it can disarrange the free charges and reduce the ¡§screen effect¡¨. However, without excellently controlled micro swing, the uniformity of the poled domain pitch will loose and the conversion efficiency can not be improved. After analysis of the measured current data, the approximate system current model was presented and the proportional dependence between system current and micro swing was verified. Thus the system current was applied as the micro swing feedback signal, with that the variation of the micro swing was reduced from 25% to 15%. The stability of CO2 laser power is also a dominant factor to determine the quality of poled crystal fiber. The variation of the CO2 laser power was controlled within 1%. All the complicated works and precise control during the crystal fiber growth were accomplished with the LabVIEW program.
¡@¡@A novel and simple self-cascaded SHG + SFG scheme is presented for the generation of tunable blue/green light using ZnO doped periodically poled lithium niobate crystal fiber (PPLNCF) with a single designed pitch. A PPLNCF with a uniform period of 15.45£gm, the maximum conversion efficiency for the second harmonic generation and the cascaded SHG + SFG blue light can reach up to -9.2 dB and -31.9 dB, respectively. The 3 dB bandwidth of the tunable blue light is 3 nm (475-478 nm). In order to expand the tuning bandwidth range, a QPM gradient periodical structure was designed and can provide a 3 dB bandwidth of 65 nm for the tunable blue/green light output by simulation. We have successfully grown a crystal fiber with the domain pitch of 18.9 £gm for the C-band wavelength converter. The crystal length is 1.8 mm, the effective nonlinear coefficient of the lithium niobate crystal fiber is 18.2 pm/V that equals 0.53¡Ñdideal (34.4 pm/V). The conversion efficiency for converting the CW laser in C-band is about -59.3 dB.
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Une étape vers la réalisation par l'échange protonique de fils quantiques et de circuits intégrés à fort confinement sur LiNbO3Stepanenko, Oleksandr 18 December 2013 (has links) (PDF)
Le présent travail visait à développer et à étudier une nouvelle méthode de fabrication des guides d'onde, " High Index Soft Proton Exchange " (HISoPE) , qui permet de réaliser des guides d'onde très confinés (dne = 0,1). Des caractérisations en génération d'harmonique localisée ont montré que les propriétés non linéaires de ces guides ne sont pas détruites mais les guides HISoPE réalisés sur coupe Z peuvent présenter des modes ayant des pertes élevées. Ces pertes peuvent être éliminés en utilisant des bains plus acides pour l'échange, mais cela implique des déformations plus importante dans les guides d'onde canal et la nature hybride des modes propageant. Dans le cadre du projet PhoXcry, nous avons essayé de réaliser un modulateur électro-optique très efficace en combinant des cristaux photoniques et des guides HISoPE sur coupe X. Dans les meilleurs guides d'onde fabriqués sur coupe X, les pertes à la propagation, expliquées par la nature hybride des modes sont de 1.75dB/cm, mais dans les guides d'ondes nanostructurés il n'a pas été possible d'identifier clairement une bande interdite photonique. HISoPE en combinaison avec l'échange inverse (Reverse Proton Exchange, RPE) a montré un grand potentiel pour la fabrication de guides d'onde enterrés. Dans une expérience de SHG et malgré des pertes élevées de 2dB/cm, nous avons pu estimer une efficacité de conversion de 160%/W*cm2. Un comportement du coupleur directionnel a été observé dans les guides d'onde enterrés fabriqué en raison d'une cinétique RPE différente dans les différentes parties du guide d'onde. Un développement ultérieur de la méthode HISoPE + RPE devrait permettre d'améliorer la qualité des guides enterrés.
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Síntese, caracterização e avaliação da atividade fotocatalítica de BiTa(Nb)O4 dopados com cromo e molibdênio na geração de hidrogênioAlmeida, Cristiane Gomes 05 1900 (has links)
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Dissertação Cristiane.pdf: 9154051 bytes, checksum: aa1fa030f760c514e3fc02dbacb83066 (MD5) / Hidrogênio obtido a partir de água é uma atrativa fonte de energia, visto que
pode ser produzido por fontes renováveis e inesgotáveis, e é não poluente.
Atualmente, a principal forma de produção de hidrogênio é através da reforma
catalítica de gás natural; porém, um novo processo baseado na fotólise da
água com auxílio de semicondutores fotocatalíticos é considerado uma
alternativa promissora. Diversos materiais já foram testados e outros
desenvolvidos com o intuito de aumentar a atividade fotocatalítica na
decomposição da água, dentre estes estão o niobato e o tantalato de bismuto
(BiNbO4 e BiTaO4), fotocatalíticamente ativos quando irradiados com luz
ultravioleta. No entanto, é possível que modificações químicas e nas
dimensões de partículas resultem em melhor atividade. O método citrato de
precursores poliméricos foi empregado para preparar BiTaO4 e BiNbO4 com a
determinação da temperatura ideal de polimerização empregando técnicas
termoanalitícas, e um estudo exploratório da temperatura mínima de calcinação
foi realizado para obtenção da fase pura desejada, confirmada por difratometria
de raios X. A fim de ativar os semicondutores com radiação visível foi realizada
a dopagem desses semicondutores com íons de metais de transição, Cr(III) e
Mo(V), com concentrações que variaram de 1 – 4% (mol/mol), e um estudo de
como as energias de band gap sofreram modificações. Foi observado que a
atividade fotocatalítica dos óxidos dopados com molibdênio ou cromo, nas
condições avaliadas, é fortemente influenciada pelos teores dos metais e a
amostra que apresentou melhor atividade fotocatalítica na geração de
hidrogênio foi BiTaO4 dopado com Cr(III) a 2%. Os resultados desse trabalho
podem contribuir para o desenvolvimento de sistemas fotoquímicos eficientes
empregados na produção fotocatalítica de hidrogênio, utilizando matérias-
primas abundantes, renováveis e ambientalmente amigáveis, como água e luz
solar. / Hydrogen obtained from water is an attractive energy source, since it can be
produced by renewable and inexhaustible primary source, besides it is not
pollutant. Nowadays, the principal form of hydrogen production is through
catalytic reform of natural gas; although, a new process based on water
splitting, with the support of photocatalytic semiconductors, is considered a
promising alternative. Many materials have already been tested and developed
with the intention of increasing the photocatalytic activity for water splitting, in
which are present bismuth niobates and tantalates (BiNbO4 e BiTaO4),
photocatalyticly active under UV light irradiation. However, it is possible that
chemical modifications and modifications in particle dimensions result in better
activity. The citrate method of polymeric precursors was used to prepare
BiTaO4 e BiNbO4 with the determination of the ideal temperature of
polymerization using thermoanalytical techniques, and an exploratory study of
the minimal temperature of calcination was used to obtain a pure desired
phase, confirmed by X rays diffractometry. In order to activate the
semiconductors with visible radiation, a doping of these semiconductors with
ions of transition metals, Cr(III) and Mo(V), with concentrations that ranged from
1 – 4% (mol/mol), and a study of how the band gap energies suffered
modifications. The results suggest that the type and the concentration of metal
doping exercise great influence on the crystalline structure and morphology of
the oxides. While Cr(III) favors a beta phase (triclinic), Mo(V) favors an alpha
phase (orthorhombic). Also, the presence of Cr(III) induces the formation of
materials with more homogeneous morphologies and size of particles smaller
than the obtained in presence of Mo(V). It was observed that a photocatalytic
activity of the doped oxides with Molybdenum or Chromium, in the evaluated
conditions, is strongly influenced by the metal concentrations and the sample
that presented the best photocatalytic activity in hydrogen generation was
BiTaO4 doped with Cr(III) at 2%. The experimental ratio H2/CO2, in this case, is
much higher than the theoretical, suggesting that the isopropyl alcohol is not
completely mineralized. The results of this work can contribute for the
development of efficient photochemical systems applied in the photocatalytic
production of hydrogen, using raw material in abundance, renewable and
environmentally friendly like water and solar light.
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Preparação e avaliação fotocatalítica de hexaniobatos lamelares e seus filmes finos obtidos por Layer-by-LayerNunes, Barbara Nascimento 19 September 2017 (has links)
CAPES - Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Devido o contínuo desenvolvimento tecnológico e o crescimento populacional, o consumo de energia vem sendo cada vez maior ao longo dos anos. Neste aspecto, a fotocatálise atrai grande interesse devido seu potencial no aproveitamento da energia solar. No cenário nacional, os niobatos lamelares são materiais interessantes para atuarem como fotocatalisadores, uma vez que o Brasil detém 98% das reservas de nióbio no mundo. Dentro deste contexto, o presente trabalho apresenta as possibilidades do K4Nb6O17 como fotocatalisador tanto na forma em pó como imobilizado em filmes finos. O K4Nb6O17 foi preparado a partir da reação em estado sólido do Nb2O5 com K3CO2 e esfoliado em solução de hidróxido de tetrabutilamônio. O niobato esfoliado foi então modificado com platina, comparando-se dois diferentes precursores H2PtCl6 e [Pt(NH3)4]Cl2, e também combinado à nanopartículas de ouro. As amostras foram caracterizadas por diferentes técnicas e o desempenho fotocatalítico avaliado tanto para fotodegradação de azul de metileno e metanol como para a produção de H2. Na fotodegradação do corante, o niobato esfoliado sem qualquer co-catalisador apresentou a maior eficiência fotônica (ξ = 2,1%). Em contraste, para a fotodegradação de metanol e para a produção fotocatalítica de H2, as amostras modificadas apresentaram maior desempenho fotocatalítico em relação ao niobato esfoliado. Na produção de H2, foram obtidas eficiências fotônicas próximas a 0,2% para as amostras contendo tanto Pt como Au. Já na fotodegradação de metanol, as amostras de niobato e Pt resultaram em eficiências próximas a 4,0% e a modificada com ouro, 7,0%. A fabricação de filmes pode melhorar a aplicação dos fotocatalisadores por facilitar sua recuperação, prevenir perdas e diminuir a aglomeração de material. Os filmes de niobato e niobato com Pt foram montados utilizando a técnica Layer-by-Layer (LbL) devido sua facilidade e versatilidade. Os filmes foram caracterizados quanto às suas propriedades morfológicas, fotocatalíticas e fotoeletroquímicas. Na fotodegradação de azul de metileno, ambos os filmes resultaram em eficiências fotônicas semelhantes (ξ = 0,1%). Em contrapartida, para a produção fotocatalítica de H2, a presença da Pt nos filmes resultou em uma eficiência duas vezes maior (ξ = 1,2%) em relação ao filme de niobato (ξ = 0,6%). O aumento do número de bicamadas ocasionou o aumentou linear da velocidade de produção de H2, indicando que a imobilização do material não ocasionou a perda de sítios ativos. / As the technological development and population growth continuously increases, energy consumption is becoming higher over the years. In this aspect, photocatalysis attracts great interest due to its potential to harvest and convert solar energy. In a national scenario, layered niobates are interesting materials to act as photocatalysts, since Brazil accounts for 98% of the world’s niobium reserves. In this work application of K4Nb6O17 as a photocatalyst both, in powder form and immobilized as thin films, was investigated. K4Nb6O17 was prepared by the solid state reaction between Nb2O5 and K2CO3 and then it was exfoliated in tetrabutylammonium hydroxide solution. The exfoliated niobate was modified with platinum using two different precursors, H2PtCl6 and [Pt(NH3)4]Cl2, and it was also combined with gold nanoparticles. The samples were characterized by different techniques and the photocatalytic performance was evaluated for methylene blue and methanol oxidation and for H2 production. In the dye photodegradation, the unmodified exfoliated niobate exhibited the highest photonic efficieny (ξ = 2.1%). In contrast, for the methanol photodegradation and H2 evolution, the modified samples presented higher photocatalytic performance than the exfoliated niobate. For H2 evolution, photonic efficiencies close to 0.2% were obtained for samples modified by Pt and Au. For methanol photodegradation, the Pt-niobate composites exhibited photonic efficiencies close to 4.0% and the Au-niobate 7.0%. The assembly of thin films can favor the application as photocatalysts due to ease of recovering, smaller losses and reduced material agglomeration. The bare niobate and the Pt-niobate films were assembled by the Layer-by-Layer (LbL) technique because of its easiness and versatility. The films were characterized towards their morphology, photocatalytic and photoelectrochemical properties. For methylene blue photodegradation, both films resulted in similar photonic efficiencies (ξ = 0.1%). In contrast, for the H2 photocatalytic production, the presence of Pt in the films resulted in a photonic efficiency twice higher (ξ = 1.2%) than the bare niobate film (ξ = 0.6%). The increase in the bilayers number caused a linear increase of the H2 evolution rate, indicating that the material immobilization did not lead to the active sites losses. / Dissertação (Mestrado)
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Síntese e caracterização de KNbO3 aplicado na fotodegradação remazol amarelo ouro em solução fotodegradação de remazol amarelo ouro em solução aquosa aquosa / Ynthesis and characterization of KNbO3 applied to the photodegradation of remazol yellow goldSilva, Arnayra Sonayra de Brito 27 February 2014 (has links)
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Previous issue date: 2014-02-27 / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPES / The potassium niobate, KNbO3, of orthorhombic perovskite presenting ferroelectric, optical property, in addition to their use in heterogeneous photocatalysis. This work consists of two stages - the synthesis of potassium niobate and its evaluation in the photodegradation of the dye Remazol Yellow Gold (RNL). The synthesis of KNbO3 was performed by polymeric precursors and catalysts were characterized by X- ray diffraction ( XRD ), infrared spectroscopy (IR) spectroscopy, ultraviolet visible (UV-Vis) region and area analysis surface . XRD results showed that the perovskite had a far-reaching organization, and there was a decrease in the secondary phase (K4Nb6O17). IR spectra confirmed these data by presenting a reduction of the bands related to vibrations with short double bond character of the Nb = O. The surface area values were lower with increasing temperature. The photocatalyst was applied to the dye Remazol yellow discoloration of gold (RNL) and the parameters used were: radiation time (2 and 4 h), the amount of catalyst (5 or 20 mg) and the change in pH (3 and 6). It was observed that a higher radiation time, a smaller quantity of catalyst and lower pH favoring a better photocatalytic efficiency, obtaining a result of discoloration of 55 %. A comparative study was done with a temperature of 700 º C, as the best result obtained in the previous tests, and observed a photocatalytic efficiency of 67% discoloration. / O niobato de potássio, KNbO3, é uma perovskita ortorrômbica que apresenta propriedade ferroelétrica, óptica, além da sua utilização em fotocatálise heterogênea. O presente trabalho consiste em duas etapas a síntese de niobato de potássio e a sua avaliação na fotodegradação do corante Amarelo Remazol Ouro (RNL). A síntese do KNbO3 foi realizada pelo método dos precursores poliméricos e os catalisadores foram caracterizados por difratometria de raios-X (DRX), espectroscopia na região do infravermelho (IV), espectroscopia na região do ultravioleta visível (UV-Vis) e análise de área superficial. Os resultados de DRX mostraram que as perovskitas apresentaram uma organização a longo alcance, e houve uma diminuição da fase secundária (K4Nb6O17). Os espectros de IV confirmaram esses dados ao apresentarem uma redução das bandas referentes às vibrações curtas com caráter de dupla ligação do Nb=O. Os valores de área superficial foram menores com o aumento da temperatura. O fotocatalisador foi aplicado na descoloração do corante remazol amarelo ouro (RNL) e os parâmetros utilizados foram: o tempo de radiação (2 e 4 h), a quantidade de catalisador (5 ou 20 mg) e a variação do pH (3 e 6). Observou que um maior tempo de radiação, uma quantidade menor de catalisador e menor pH favoreceram uma melhor eficiência fotocatalítica, obtendo um resultado de 55% de descoloração. Um estudo comparativo foi feito com a temperatura de 700 ºC, como o melhor resultado obtido nos testes anteriores, e observou uma eficiência fotocatalítica de 67 % de descoloração.
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Fixação de hologramas em Niobato de Lítio / Fixing of holograms in Lithium NiobateOliveira, Ivan de, 1972- 28 February 2005 (has links)
Orientador: Jaime Frejlich / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin / Made available in DSpace on 2018-08-05T13:36:24Z (GMT). No. of bitstreams: 1
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Previous issue date: 2005 / Resumo: Neste trabalho foram realizadas contribuições importantes na área de registro holográfico auto-estabilizado em niobato de lítio (LiNbO3:Fe) e do estudo da dinâmica da formação e evolução dos hologramas durante as diferentes etapas da fixação. Outras contribuições importantes neste trabalho referem-se ao desenvolvimento de técnicas mais eficientes e/ou mais simples para a fixação de hologramas. Em termos de registro auto-estabilizado, nosso trabalho permitiu o uso dessas técnicas para obtermos hologramas com alta eficiência de difração e de forma reprodutível. O registro holográfico auto-estabilizado em niobato de lítio já tinha sido utilizado anteriormente. A novidade aqui reside no estudo detalhado da dinâmica do processo, que permitiu uma melhor compreensão das possibilidades e limitações da técnica, incluindo o estudo detalhado do efeito do grau de oxidação (isto é, da relação [Fe3+]/[Fe2+]) do material sobre o comportamento do sistema de estabilização. Em função dos estudos acima referidos que permitiram uma melhor compreensão dos processos, foi possível desenvolver uma técnica de fixação para cristais oxidados que permitiu obter redes fixas com alta eficiência de difração, com valores previzíveis em função das propriedades do cristal e de forma reprodutível. O registro auto-estabilizado foi aplicado com sucesso, pela primeira vez, à técnica de fixação (registro e compensação) a alta temperatura, de forma muito mais simples do que a técnica clássica, e que permitiu obter excelentes resultados mesmo com amostras reduzidas, para as quais o processo clássico não funciona satisfatoriamente. Paralelamente mostramos teórica e experimentalmente os problemas associados à medida da eficiência de difração em hologramas espessos. Mostramos que o uso de um feixe auxiliar (frequentemente utilizado) para este tipo de medida leva a erros consideráveis e para este caso propomos uma forma muito simples de realizar essa medida / Abstract: In this work important contributions to the field and to the self stabilized holographic record in litium niobate were achieved and to the dynamic formation and hologram evolution study during different fixing stages. Other important contributions in this work refer to more efficient technique development and/or simpler ones to hologram fixing. On terms of self stabilized record our work allowed the use of these techniques to obtain some holograms with high efficiency diffractions and in a reproducible form. The self stabilized holographic record in litium niobate had already been used before. The new point here is the detailed study about the process dynamic which allowed a better understanding of the technique possibilities and limitations including the detailed study of the effect of the oxidation degree (thus the relation [Fe3+]/[Fe2+]) of the material about the stabilization system behaviour. According to the referred studies above which permitted a better understanding of the process, it was possible to develop the oxidated crystals fixing technique which permitted to get fixed nets with high diffractions efficience with predictable values according to the crystals properties and in a reproducible form. The self stabilized record was applied sucessfully to the fixing technique (recording and compensation) for the first time to high temperature in a so much simpler form than the classical one which permitted to obtain excellent results even using reduced samples to which the classical process has not worked satisfactionally. Parallel to this, we showed (theoric and experimentally) the associated problems to the diffraction efficience in thick holograms. We showed the use of an auxiliar bin (frequently used) for this kind of measure results in considerable errors and to this case we propose a so much simpler form of achieving this measure / Doutorado / Física da Matéria Condensada / Doutor em Ciências
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Photorefractive Crystals : Optical Phase Conjugation And Phase Conjugate InterferometryJayanth, P 10 1900 (has links) (PDF)
No description available.
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Setup and application of a combined Brillouin-Raman systemRix, Jan 18 January 2023 (has links)
Die Schwingungsspektroskopie ist ein etabliertes Verfahren in der Materialwissenschaft sowie in der biomedizinischen Forschung zur Untersuchung von probenspezifischen Eigenschaften. Sie nutzt die Wechselwirkung von Licht (Photonen) mit Schwingungsquanten (Phononen) aus, um materialspezifische Informationen zu erlangen. Die Ramanspektroskopie ist sensitiv gegenüber optischen Phononen und findet seit der Erfindung des Lasers rege Verwendung. Im Gegensatz dazu untersucht die Brillouinspektroskopie die akustischen Phononen. Sie kam lange Zeit jedoch nur vereinzelt in der Materialwissenschaft zum Einsatz, da sie auf Grund der sequentiellen Spektrenaufnahme sehr zeitaufwendig war. Erst kürzlich konnte durch die Verwendung von einem virtually imaged phased array (VIPA) als dispersives Element im Brillouinspektrometer die Messzeit drastisch verkürzt werden, wodurch auch ein Einsatz in der biomedizinischen Forschung möglich ist. Im Rahmen dieser Dissertation wurde ein kombiniertes Brillouin-Raman-System aufgebaut, welches eine zeitgleiche und ko-lokalisierte Aufnahme von Brillouin und Ramanspektren ermöglicht. Im Vergleich zu anderen Systemen, profitiert dieser Aufbau von der Verwendung zweier VIPAs mit unterschiedlichen freien Spektralbereichen was zu einer Entkopplung der spektralen Achsen und damit zu sensitiveren Messungen führt. Außerdem ermöglicht dies eine eineindeutige Bestimmung von Brillouin-Verschiebungen. Darüber hinaus zeichnen die nahinfrarote Anregung bei 780 nm und die kontinuierliche Kalibrierung des Brillouinspektrums dieses System aus.
In einer ersten Anwendung wurden mit diesem kombinierten System ferroelektrische Domänenwände in periodisch gepoltem Lithiumniobat untersucht. Dabei stellte sich heraus, dass neben dem aus der Literatur bekannten Raman-Kontrast (Intensitätsvariation bei 635 cm−1) auch das Brillouinspektrum einen Unterschied zwischen der Domänenwand und einer flächigen Domäne aufweist (Verringerung der Brillouin-Verschiebung). Es konnte gezeigt werden, dass bestehende Theorien für den Raman-Kontrast auch verwendet werden können, um den Brillouin-Kontrast zu erklären. Kombinierte Brillouin-Raman Messungen verdeutlichten, dass beide Kontraste zu Bildgebungszwecken genutzt werden können.
In einer zweiten Anwendung, wurde das System dazu genutzt, die Tumorbiologie von Glioblastomzellen zu charakterisieren. Die Kombination der beiden spektroskopischen Methoden erlaubte es, die biochemischen mit den biomechanischen Eigenschaften zu korrelieren. So konnte ermittelt werden, dass der Zellkern die höchste Steifigkeit innerhalb einer adhärenten Zelle aufweist. Ein Vergleich zwischen adhärent und als Sphäroid gewachsenen Zellen offenbarte, dass letztere eine signifikant höhere Steifigkeit aufweisen, was bei der Wahl eines geeigneten Tumormodells berücksichtigt werden sollte. Darüber hinaus konnte anhand der klinisch bedeutsamen IDH1-mutation gezeigt werden, dass sich auch der Genotyp einer Zelle auf die Biomechanik auswirkt. Kombinierte Messungen an Sphäroiden wiesen darauf hin, dass sowohl Proteine sowie indirekt auch Lipide maßgeblich die biomechanischen Eigenschaften beeinflussen.
Die beiden Anwendungen verdeutlichen, welche Vorteile eine Kombination dieser beiden spektroskopischen Verfahren mit sich bringt. Ihre nicht-invasive, zerstörungs- und präparationsfreie Arbeitsweise bietet dabei die Grundlage für weitere Untersuchungen auch in anderen Anwendungsfelder. / Vibrational spectroscopy is an established technique in materials science as well as in biomedical research for the investigation of sample-specific properties. It exploits the interaction of light (photons) with vibrational quanta (phonons) to obtain material-characteristic information. Raman spectroscopy is sensitive to optical phonons and has been used extensively since the invention of lasers. In contrast, Brillouin spectroscopy investigates acoustic phonons. However, for a long time it was only used sporadically in materials science as it was very time-consuming due to the sequential spectrum acquisition. Only recently, the use of a virtually imaged phased array (VIPA) as dispersive element in the Brillouin spectrometer has drastically reduced the measurement time, thus facilitating its application in biomedical research.
In this dissertation, a combined Brillouin-Raman system was built, which allows simultaneous and co-localized acquisition of Brillouin and Raman spectra. Compared to other systems, this setup benefits from the use of two VIPAs with different free spectral ranges, which leads to a decoupling of the spectral axes and thus to more sensitive measurements. It further allows for an unambiguous determination of Brillouin shifts. Moreover, the near-infrared excitation at 780 nm and the continuous calibration of the Brillouin spectrum characterize this system.
In a first application, ferroelectric domain walls in periodically poled lithium niobate were studied with this combined system. It was found that, in addition to the Raman contrast known from literature (intensity variation at 635 cm−1), the Brillouin spectrum also shows a difference between the domain wall and a bulk domain (decrease of the Brillouin shift). It could be shown that existing theories for the Raman contrast can also be applied to explain the Brillouin contrast. Combined Brillouin-Raman measurements demonstrated that both contrasts can be used for imaging purposes.
In a second application, the system was used to characterize the tumor biology of glioblastoma cells. The combination of the two spectroscopic methods allowed the biochemical properties to be correlated with the biomechanical properties. Thus, it could be determined that the nucleus has the highest stiffness within an adherent cell. A comparison between adherent cells and cells grown as spheroid revealed that the latter exhibit significantly higher stiffness, which should be taken into account when choosing a suitable tumor model. In addition, clinically relevant IDH1 mutation was used to show that the genotype of a cell also affects biomechanics. Combined measurements indicated that proteins as well as in an indirect way also lipids significantly influence biomechanical properties. These two applications illustrate the advantages of combining the two spectroscopic techniques. Their non-invasive, non-destructive and preparation-free operation provides the basis for further investigations also in other fields of application.
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