Thesis (Ph.D.)--Hong Kong University of Science and Technology, 2005. / Includes bibliographical references. Also available in electronic version.

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This thesis concerns a study of the application, and performance optimization, of standard lead-lag compensation techniques to improve the closed loop performance of a focus servo system for an optical data storage device. Only with proper application of these compensation techniques will it be possible to meet the sub-micrometer focus error tolerances while maintaining the stability of the closed loop system. The performance indices used in this optimization study are the Integral of the Squared Error (ISE), the Integral of the Absolute Error (IAE), and the Integral of the Time multiplied by the Absolute Error (ITAE) as defined below, with the error function e(t) being the focus error of the closed loop servo system in response to a step input. ISE= ∫OT e²(t) dt IAE= ∫OT / e(t) / dt ITAE= ∫OT t / e(t) / dt

M.Com. (Informatics) / Please refer to full text to view abstract

Neste trabalho estudamos o processo de absorção de dois fótons em compostos azoaromáticos, abordando tanto aspectos fundamentais quanto aplicados. Moléculas azo-aromáticos têm recebido especial atenção nos últimos anos devido as suas potencias aplicações em dispositivos para armazenamento óptico de informação, modulação da luz e geração de relevos em superfície, processes estes associados ao mecanismo de foto isomerização. Os trabalhos apresentados nessa tese tiveram como principal foco explorar o fenômeno de absorção de dois fótons, utilizando a propriedade de foto-isomerização das moléculas azo-aromáticas. Nosso objetivo foi estudar as vantagens que podem ser obtidas pela utilização de pulsos intensos de luz, que interagem de maneira não linear com a matéria, para desenvolver aplicações utilizando compostos azo-aromáticos. Inicialmente, estudamos o processo de absorção de dois fótons em uma nova família de compostos azo-aromáticos, denominados Salen Dyes. Investigamos a influencia da presença de íons metálicos no processo de absorção de dois fótons dessas moléculas. Nossos resultados mostraram que, devido a ausência de conjugação entre as estruturas azo-aromáticas conectadas pelo metal, este tem pouca influência no processo não linear estudado. Pelo uso de um modelo de soma de estado para a seção de choque de absorção de dois fótons, fomos capazes de determinar os momentos de dipolo de transição destas moléculas. Em seguida, implementamos uma técnica para estudar o processo de armazenamento óptico, induzido através da orientação molecular dos compostos azo-aromáticos, via absorção de dois fótons. Observamos que de fato é possível se observar birrefringência induzida por dois fótons nestas moléculas, a qual esta confinada ao volume focal, conforme demonstrado pela obtenção de armazenamento tri-dimensional. Finalmente, exploramos o processo de controle coerente via formatação de pulsos ultra-curtos para manipular o processo de birrefringência induzida por dois fótons em compostos azo-aromáticos. Foi demonstrado que apenas a através da manipulação da fase do pulso ultra-curto, é possível modular a birrefringência induzida em filmes de compostos azo-aromáticos. / Here we investigated fundamental and applied aspects of the two-photon absorption process in azoaromatic compounds. Azoaromatic molecules have been studied in the last few years due to their applications in optical storage devices, light modulators and surface relief gratings, processes related to the photo-isomerization mechanism. The main focus of the results presented in this thesis was to explore the two-photon absorption process, taking advantage of the intrinsic photo-isomerization of the azo-aromatic chromophores. Our main goal was to study the advantages of utilizing intense pulses, which promote nonlinear excitation, to develop application with azo-aromatic compounds. Initially, we studied the two-photon absorption process in a new class of azo-aromatic compounds, named Salen Dyes. We investigated the influence of metal ions, presented in the Salen Dyes structure, on the two-photon absorption spectrum. Our results revealed that the metals have practically no influence in the nonlinear optical properties due to the lack of conjugation between the azo-moieties in the Salen Dyes. Through a theoretical model based on a sum-over-states calculation, we were able to determine the transition dipole moment of these molecules. Subsquently, we implememnted a technique to study the two-photon induced birefringence, resulting from the molecular re-orientation, in azo-aromatic compounds. We observed that the two-photon induced birefringence is confined to the focal volume, s demonstrated in a three dimensional optical storage experiment. Finally, we used coherent control processes to manipulate the two-photon induced birefringence in azo-compounds. It was demonstrated that it is possible to modulate the optically induced birefringence by manipulating the phase of the ultra-short pulses, via pulse shaping techniques.

Materiais poliméricos com propriedades de fotoisomerização, como os azopolímeros, apresentam grande potencial para aplicações em óptica não linear e dispositivos opto-eletrônicos. Entretanto há limitações para a aplicação dos azopolímeros devido à tendência à agregação dos cromóforos e dificuldade de formação de filmes. A mistura do azopolímero com polímeros metacrílicos e poli(3-alquiltiofenos) pode melhorar estas características sem acarretar prejuízos para a propriedade de isomerização fotoinduzida. Neste estudo o azopolímero foi sintetizado por ATRP usando o monômero DR1-MA, 4-[N-etil-N-(2-metacriloxietil)]-4- nitroazobenzeno, obtido a partir do corante Disperse Red 1 (DR1), os polímeros poli(metacrilato de hexila) (HPHex-MA) e poli(metacrilato de dodecila) (HPDod-MA) foram sintetizados por polimerização radicalar convencional a partir dos monômeros obtidos comercialmente e o poli(3-dodeciltiofeno) (HP3-DodT) obtido por polimerização oxidativa. As polimerizações foram bem sucedidas apresentando massas molares acima de 10.000 g/mol com polidispersividade relativamente baixa. As estruturas químicas foram confirmadas por espectroscopias UV-Vis, FTIR e RMN-H1. Misturas do azopolímero com os polímeros metacrílicos e o poli(3-alquiltiofeno) foram preparadas em diversas proporções e usadas na formação de filmes de Langmuir. Nestes filmes, isotermas de pressão de superfície apontaram interações para as três misturas em algumas proporções, entre elas a de 50%. Imagens de microscopia no ângulo de Brewster revelaram a contribuição do polímero metacrílico no espalhamento do filme do azopolímero sem a separação de fase. Os resultados de Espectroscopia de Infravermelho por Reflexão e Absorção com Polarização Modulada (PM-IRRAS) comprovaram que o comprimento da cadeia lateral do polímero afeta a organização molecular na interface. Filmes de Langmuir das misturas na proporção de 50% foram transferidos em substratos sólidos, obtendo os filmes Langmuir-Blodgett (LB). Comparações entre os filmes spin-coated e Langmuir-Blodgett mostraram que a organização molecular nos filmes nanoestruturados causa a redução na agregação de cromóforos e na hidrofobicidade da superfície. Filmes LB da mistura 50% HPDR1-MA/HPDod-MA com 101 camadas foram caracterizados quanto à capacidade de armazenamento óptico. Estes filmes apresentaram valores de birrefringência residual que permitem ser aplicados em armazenamento óptico com a vantagem de curtos tempos de escrita em comparação a outros filmes poliméricos. / Polymeric materials with photoisomerization properties, such as the azopolymers, offer great potential for applications in non-linear optics and opto electronic devices. However, there are important limitations for the application of azopolymers, since azopolymers with high content of azobenzene moieties tend to aggregate and show poor film-formation properties. The combination of azopolymers with methacrylic polymers and poly (3-alkylthiophenes) can improve their properties without reducing the optical storage capability. In this study, the azopolymer poly[4-[[2-(methacryloyloxy)-ethyl]ethylamino]-4-nitroazobenzene], HPDR1-MA, was synthesized by Atom Transfer Radical Polymerization (ATRP), the poly (hexylmethacrylate) (HPHex-MA) and poly(dodecylmethacrylate)(HPDod-MA) were synthesized by conventional radical polymerization, the poly(3-dodecylthiophene) (HP3-DodT) via oxidative polymerization. The polymerizations were successful with molecular weights above 10.000 g/mol and relatively low polydispersities. The chemical structures were confirmed with UV-Vis, infrared and nuclear magnetic resonance spectroscopies. Mixtures of azopolymer with the methacrylic polymer and poly(3-alkylthiophenes) were prepared in various proportions and used in the formation of Langmuir films. In the latter, surface pressure isotherms indicated interactions between the film components, mainly for a proportion of 50% in weight of HPDR1-MA. Phase segregation was not apparent in the BAM images, which revealed that the methacrylic polymer improves the formation of the film Langmuir. Through PM-IRRAS, we noted that the length of the side chain of the polymer affects the molecular organization at the interface. Langmuir films of the mixtures in the proportion of 50% were transferred onto solid supports as Langmuir-Blodgett (LB ) films. Comparison of LB and spin-coated films demonstrated that the molecular organization of nanostructured films prevents the aggregation of chromophores and reduces the surface hydrophobicity. Optical Storage measurements were performed in 101-layer LB films of the mixture 50% HPDR1-MA/HPDod-MA. The photoinduced birefringence shows features that make these films useful for optical storage, with the advantage of short writing times in comparison to other azopolymer films.

by Lui Bong Chun, Richard. / Thesis (M.Phil.)--Chinese University of Hong Kong, 1995. / Includes bibliographical references. / Abstract / Acknowledgment / Chapter Chapter 1 --- Introduction --- p.1 / Chapter 1.1 --- Background for the Project --- p.1 / Chapter 1.1.1 --- Interests in Blue-Green Laser --- p.1 / Chapter 1.1.2 --- Progress of Blue-Green Laser --- p.2 / Chapter 1.2 --- The Aim of the Project --- p.3 / Chapter 1.3 --- Overview the Remaining Parts of this Thesis --- p.4 / Chapter 1.4 --- References --- p.6 / Chapter Chapter 2 --- Sum Frequency Generation --- p.8 / Chapter 2.1 --- Introduction --- p.8 / Chapter 2.2 --- Sum Frequency Generation --- p.8 / Chapter 2.2.1 --- Theoretical Background for Sum Frequency Generation --- p.9 / Chapter 2.2.2 --- The Coupled Wave Equations for SFG --- p.13 / Chapter 2.2.3 --- Phase Matching Considerations --- p.16 / Chapter 2.3 --- References --- p.18 / Chapter Chapter 3 --- Cerenkov Radiation --- p.19 / Chapter 3.1 --- Introduction --- p.19 / Chapter 3.2 --- The Properties of Cerenkov Radiation by Using TM Mode --- p.21 / Chapter 3.2.1 --- Refractive Index Notation --- p.23 / Chapter 3.2.2 --- Fundamental Wave TM Guides Mode --- p.23 / Chapter 3.2.3 --- Second Harmonic TM Radiation Mode --- p.24 / Chapter 3.2.4 --- Efficiency of SHG --- p.25 / Chapter 3.3 --- Simplified Model Analysis of Cerenkov Radiation in TE Mode --- p.29 / Chapter 3.4 --- Simulation --- p.33 / Chapter 3.4.1 --- Modeling the LiNb03 --- p.33 / Chapter 3.4.2 --- Modeling an Asymmetric Slab Waveguide ´ؤPMMA doped with MNA on Fused Quartz --- p.37 / Chapter 3.4.3 --- Modeling a Symmetric Slab Waveguide ´ؤPMMA doped with MNA on Fused Quartz --- p.42 / Chapter 3.5 --- References --- p.47 / Chapter Chapter 4 --- Ellipsometry --- p.49 / Chapter 4.1 --- Introduction --- p.49 / Chapter 4.2 --- General Principles --- p.49 / Chapter 4.3 --- Basic Operation --- p.50 / Chapter 4.4 --- The Optical Constants of the Bulk Materials --- p.51 / Chapter 4.5 --- Calculation the Refractive Index of the Substrates --- p.53 / Chapter 4.6 --- Ellipsometric Theory for the Thin Film --- p.57 / Chapter 4.7 --- Measurement the Refractive Index and the Thickness of the Thin Film --- p.59 / Chapter 4.7.1 --- Data --- p.62 / Chapter 4.7.2 --- Discussions --- p.73 / Chapter 4.8 --- Calculation the Refractive Index of the thin Film by Considering as a Bulk Material --- p.78 / Chapter 4.9 --- References --- p.80 / Chapter Chapter 5 --- Prism Coupling --- p.81 / Chapter 5.1 --- Introduction --- p.81 / Chapter 5.2 --- Coupling of a Plane Wave --- p.82 / Chapter 5.3 --- Numerical Approach for the Calculation of the Coupling Efficiency --- p.85 / Chapter 5.4 --- Experiment --- p.88 / Chapter 5.4.1 --- Experimental Setup --- p.88 / Chapter 5.4.2 --- Experimental Result and Discussions --- p.90 / Chapter 5.5 --- References --- p.92 / Chapter Chapter 6 --- Conclusion --- p.93 / Chapter Chapter 7 --- Future Plans --- p.96 / Chapter 7.1 --- Simplified Model of Corona Poling --- p.96 / Chapter 7.2 --- Advanced Models of Poling --- p.98 / Chapter 7.2.1 --- Slab Waveguide --- p.98 / Chapter 7.2.2 --- Channel Waveguide --- p.99 / Chapter 7.3 --- References --- p.100 / Chapter Appendix 1 --- Materials' Descriptions --- p.A-l / Chapter A.1.1 --- 2-Methyl-4-Nitoaniline --- p.A-1 / Chapter A.1.2 --- Poly ( Methyl Methacrylate ) --- p.A-3 / Chapter A.1.3 --- References --- p.A-4 / Chapter Appendix 2 --- Fabrication Procedures --- p.A-5 / Chapter A.2.1 --- Cleaning the Apparatus --- p.A-5 / Chapter A.2.2 --- Cleaning the Substrate --- p.A-5 / Chapter A.2.3 --- Thin film Fabrication --- p.A-5 / Chapter A.2.4 --- Thin Film Removal --- p.A-6 / Chapter A.2.5 --- References --- p.A-6 / Chapter Appendix 3 --- Alpha Step --- p.A-7 / Chapter A.3.1 --- Introduction --- p.A-7 / Chapter A.3.2 --- Experimental Setup --- p.A-8 / Chapter A.3.3 --- Experimental Results --- p.A-9 / Chapter A.3.3.1 --- Thin Film of PMMA without Dopant --- p.A-9 / Chapter A.3.3.2 --- Thin Film of PMMA doped with MNA --- p.A-19 / Chapter A.3.4 --- Discussions --- p.A-27 / Chapter A.3.5 --- References --- p.A-28 / Chapter Appendix 4 --- Scanning Electron Microscope --- p.A-29 / Chapter A.4.1 --- Scanning Electron Microscope --- p.A-29 / Chapter A.4.2 --- Reference --- p.A-30 / Chapter Appendix 5 --- Gaussian Beam & Coordinate System Transformation --- p.A-31 / Chapter A.5.1 --- Gaussian Beam in a Homogeneous Medium --- p.A-31 / Chapter A.5.2 --- Transformation of the Coordinate Systems --- p.A-32 / Chapter A.5.3 --- Reference --- p.A-32 / Chapter Appendix 6 --- Waist Size Measurement of Gaussian Beam --- p.A-33 / Chapter A.6.1 --- Waist Size Measurement of Gaussian Beam --- p.A-33 / Chapter A.6.2 --- References --- p.A-34 / Chapter Appendix 7 --- Quasi Phase Matching --- p.A-35 / Chapter A. 7.1 --- Introduction --- p.A-35 / Chapter A.7.2 --- Basic Concept of QPM --- p.A-36 / Chapter A.7.3 --- References --- p.A-38 / Chapter Appendix 8 --- Program Listing --- p.A-41 / Chapter A.8.1 --- Program Listing ( Chapter 3 ) --- p.A-41 / Chapter A.8.1.1 --- Program 3.1 (transcendental.m ) --- p.A-41 / Chapter A.8.1.2 --- Program 3.2 (linbo3.m) --- p.A-42 / Chapter A.8.2 --- Program Listing ( Chapter 4 ) --- p.A-45 / Chapter A.8.2.1 --- Program 4.1 ( ellipsometry.m ) --- p.A-45 / Chapter A.8.3 --- Program Listing ( Chapter 5 ) --- p.A-47 / Chapter A.8.3.1 --- Program 5.1 ( parameter.m ) --- p.A-47 / Chapter A.8.3.2 --- Program 5.2 ( coupling.m ) --- p.A-49 / Chapter A.8.3.3 --- Program 5.3 ( v_3_amp.m ) --- p.A-50 / Chapter A.8.3.4 --- Program 5.4 ( input_profile.m ) --- p.A-51

Materiais poliméricos com propriedades de fotoisomerização, como os azopolímeros, apresentam grande potencial para aplicações em óptica não linear e dispositivos opto-eletrônicos. Entretanto há limitações para a aplicação dos azopolímeros devido à tendência à agregação dos cromóforos e dificuldade de formação de filmes. A mistura do azopolímero com polímeros metacrílicos e poli(3-alquiltiofenos) pode melhorar estas características sem acarretar prejuízos para a propriedade de isomerização fotoinduzida. Neste estudo o azopolímero foi sintetizado por ATRP usando o monômero DR1-MA, 4-[N-etil-N-(2-metacriloxietil)]-4- nitroazobenzeno, obtido a partir do corante Disperse Red 1 (DR1), os polímeros poli(metacrilato de hexila) (HPHex-MA) e poli(metacrilato de dodecila) (HPDod-MA) foram sintetizados por polimerização radicalar convencional a partir dos monômeros obtidos comercialmente e o poli(3-dodeciltiofeno) (HP3-DodT) obtido por polimerização oxidativa. As polimerizações foram bem sucedidas apresentando massas molares acima de 10.000 g/mol com polidispersividade relativamente baixa. As estruturas químicas foram confirmadas por espectroscopias UV-Vis, FTIR e RMN-H1. Misturas do azopolímero com os polímeros metacrílicos e o poli(3-alquiltiofeno) foram preparadas em diversas proporções e usadas na formação de filmes de Langmuir. Nestes filmes, isotermas de pressão de superfície apontaram interações para as três misturas em algumas proporções, entre elas a de 50%. Imagens de microscopia no ângulo de Brewster revelaram a contribuição do polímero metacrílico no espalhamento do filme do azopolímero sem a separação de fase. Os resultados de Espectroscopia de Infravermelho por Reflexão e Absorção com Polarização Modulada (PM-IRRAS) comprovaram que o comprimento da cadeia lateral do polímero afeta a organização molecular na interface. Filmes de Langmuir das misturas na proporção de 50% foram transferidos em substratos sólidos, obtendo os filmes Langmuir-Blodgett (LB). Comparações entre os filmes spin-coated e Langmuir-Blodgett mostraram que a organização molecular nos filmes nanoestruturados causa a redução na agregação de cromóforos e na hidrofobicidade da superfície. Filmes LB da mistura 50% HPDR1-MA/HPDod-MA com 101 camadas foram caracterizados quanto à capacidade de armazenamento óptico. Estes filmes apresentaram valores de birrefringência residual que permitem ser aplicados em armazenamento óptico com a vantagem de curtos tempos de escrita em comparação a outros filmes poliméricos. / Polymeric materials with photoisomerization properties, such as the azopolymers, offer great potential for applications in non-linear optics and opto electronic devices. However, there are important limitations for the application of azopolymers, since azopolymers with high content of azobenzene moieties tend to aggregate and show poor film-formation properties. The combination of azopolymers with methacrylic polymers and poly (3-alkylthiophenes) can improve their properties without reducing the optical storage capability. In this study, the azopolymer poly[4-[[2-(methacryloyloxy)-ethyl]ethylamino]-4-nitroazobenzene], HPDR1-MA, was synthesized by Atom Transfer Radical Polymerization (ATRP), the poly (hexylmethacrylate) (HPHex-MA) and poly(dodecylmethacrylate)(HPDod-MA) were synthesized by conventional radical polymerization, the poly(3-dodecylthiophene) (HP3-DodT) via oxidative polymerization. The polymerizations were successful with molecular weights above 10.000 g/mol and relatively low polydispersities. The chemical structures were confirmed with UV-Vis, infrared and nuclear magnetic resonance spectroscopies. Mixtures of azopolymer with the methacrylic polymer and poly(3-alkylthiophenes) were prepared in various proportions and used in the formation of Langmuir films. In the latter, surface pressure isotherms indicated interactions between the film components, mainly for a proportion of 50% in weight of HPDR1-MA. Phase segregation was not apparent in the BAM images, which revealed that the methacrylic polymer improves the formation of the film Langmuir. Through PM-IRRAS, we noted that the length of the side chain of the polymer affects the molecular organization at the interface. Langmuir films of the mixtures in the proportion of 50% were transferred onto solid supports as Langmuir-Blodgett (LB ) films. Comparison of LB and spin-coated films demonstrated that the molecular organization of nanostructured films prevents the aggregation of chromophores and reduces the surface hydrophobicity. Optical Storage measurements were performed in 101-layer LB films of the mixture 50% HPDR1-MA/HPDod-MA. The photoinduced birefringence shows features that make these films useful for optical storage, with the advantage of short writing times in comparison to other azopolymer films.

Neste trabalho apresentamos resultados de birrefringência opticamente induzida via absorção de um e dois fótons em filmes casting de poli (metil metacrilato) (PMMA), contendo uma nova série de compostos azoaromáticos chamados de corantes Salen, os quais podem ser usados em aplicações de memória óptica. Para a birrefringência opticamente induzida por um fóton, foi necessário um tempo de escrita maior para os compostos com metal na estrutura em comparação com o composto Salen que não contém metal, provavelmente devido a agregações do grupo azoaromático na estrutura do polímero diminuindo a mobilidade molecular. Além disso, como uma novidade em memórias ópticas deste tipo, birrefringência opticamente induzida por dois fótons pôde ser realizada nos filmes de Salen, o que pode permitir sua aplicação em memória óptica tridimensional. / In this work we present the one- and two-photon optically induced birefringence in cast films of amorphous poly(methyl methacrylate) (PMMA), containing a new series of organometallic azoaromatic compounds, referred to as Salen dyes, which may be used in optical storage applications. For the one-photon optically induced birefringence, longer writing times were required for the organometallic compounds in comparison with the nonmetal one, probably due to the higher degree of aggregation in the azoaromatic moieties that precludes molecular orientation. Furthermore, as a novelty concerning optical storage, two-photon optically induced birefringence could be achieved in the Salen dyes guest-host films, which allows their application in three-dimensional optical memories.