Thèse (Ph. D.)--Université Laval, 2008. / Bibliogr. Publié aussi en version électronique dans la Collection Mémoires et thèses électroniques.

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Thèse doctorat : Chimie Physique : Strasbourg 1 : 2006. / Titre provenant de l'écran-titre. Bibliogr. 12 p.

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Potsdam, University, Diss., 2003.

Marburg, Universiẗat, Diss., 2001.

Twenty different materials have been successfully deposited as Langmuir- Blodgett monolayer films. All exhibit second harmonic generation (SHG) when irradiated with laser light at 1064 nm. E-1-docosyl-4-{2-(4-dimethylami nophenyl)ethenyl}quinolinium bromide (C22H45QHBr) and E-1-docosyl-4-{2-(4-dimethy laminonaphthyl)ethenyl}quinolinium bromide (C22H45QNBr) have been deposited separately as multilayer films. They form Y-type structures when deposition is alternated with the material N-docosyl-4- methylquinolinium bromide. The nonlinear responses are quadratic up to 20 and 10 bilayers respectively and the response from the thick films is only 2 orders less than that produced by a Y-cut quartz plate. Similar results were obtained with C22H45QHBr when interleaved with 4,4'-dioctadecyl-3,5,3', 5'- tetra me thyldipyrrylmethenehydrobromide. Ellipsometry studies of the 10 bilayer film of C H45QNBr indicate that the structure is interdigitated. This explains the stability of the film which gave the same SH response up to 6 months after deposition. A 10 bilayer films has also been fabricated using E-1- docosyl-4-{2-(4-{2-(4-dimethylaminophenyl)ethenyl}benzyl)ethenyl}pyridinium bromide (C22H45PBHBr) alternated with E-1-docosy1-4-{2-(4-methylphenyl)ethenyl}pyridinium bromide (C22H45PT). E-1-octadecyl-4-{2-(4-methyloxyphenyl)ethenyl}pyridinium iodide and E-1- methyl-4-{2-(4-octadecyloxyphenyl)ethenyl}pyridinium iodide have been fabricated into monolayer films that are transparent at 1064 and 532 nm, therefore resonant enhancement does not contribute to their nonlinear response which is attributed solely to charge transfer in the molecule. Mixed solutions of E-1-octadecyl-4-{2-(4-methyloxyphenyl)ethenyl}pyridinium iodide and sodium octadecylsulphate (C1SH37OSO3 Na+) have been deposited as very stable monolayers. The nonlinear response from the mixed film offers a significant improvement upon the performance of the film containing pure hemicyanine. Novel zwitterionic materials have been fabricated as LB monolayers that also exhibit SHG.

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O intuito do desenvolvimento de biomateriais potencialmente aplicáveis como implantes de substituição óssea é sintetizar superfícies que induzam respostas biológicas positivas quando em contato com o tecido hospedeiro. Para isso, faz-se necessário não somente estudos de composição química, mas também é importante buscar compreender propriedades físicas e estruturais dos sistemas que estes materiais irão substituir. O osso natural é constituído por compostos orgânicos, especialmente proteínas como o colágeno, reforçado com minerais, tais como hidroxiapatita. O processo pelo qual ocorre a formação do componente inorgânico é chamado biomineralização. Uma maneira de introduzir macromoléculas em sistemas modelo para estudos de biomineralização é a formação de monocamadas Langmuir, que são camadas monomoleculares altamente organizadas de moléculas anfifílicas na interface líquido-ar. Essas monocamadas podem ser transferidas para suportes sólidos formando filmes de Langmuir-Blodgett. Neste estudo, foi investigado a incorporação de colágeno tipo-I em monocamadas insolúveis contendo os fosfolipídeos 1,2-dipalmitoil-sn-glicero-3-fosfatidilcolina (DPPC) ou ácido octadecilfosfônico (OPA), bem como a transferência dessas monocamadas para suportes de titânio por meio da técnica de Langmuir-Blodgett. Estes filmes foram utilizados como matrizes para o crescimento de hidroxiapatita biomimética após a exposição dos discos de titânio modificados a uma solução que simula a concentração de íons e pH do plasma sanguíneo humano. As amostras foram caracterizadas por microscopia eletrônica de varredura (MEV), microscopia de força atômica (AFM), espectroscopia vibracional na região do infravermelho (FTIR) e difração de raios-X (DRX). A razão molar Ca/P foi determinada por espectroscopia de dispersão de energia de raios-X (EDX). Propriedades dos biomateriais como molhabilidade, rugosidade e energia livre de superfície também foram estudadas. A biocompatibilidade das amostras foi investigada in vitro utilizando-se ensaios de viabilidade de osteoblastos. O colágeno interage com os fosfolipídios na interface água/ar, como evidenciado pelas isotermas de pressão de superfície, obtidas na presença da proteína. Além disso, a estabilidade das monocamadas de Langmuir foi aumentada devido à presença de colágeno na subfase. A incorporação de colágeno e fosfolipídios em filmes Langmuir-Blodgett sobre as superfícies de titânio são fatores determinantes para a formação de filmes inorgânicos altamente organizado, contínuos e uniformes, compostos por nanopartículas de hidroxiapatita biomimética, semelhante à encontrada no osso natural. As modificações nas superfícies aumentaram a proliferação de osteoblasto no titânio indicando que este material não é tóxico a este tipo de célula. / The development potential of biomaterials for bone replacement is guided by the necessity to provide a surface that induces positive biological responses when the material is in contact with the host tissue. For this, it is necessary the study of the chemistry and surface composition and also to understand the physical properties and the structural organization of the natural system which is in contact with the biomaterial. Natural bone is composed by organic compounds, especially protein like collagen, reinforced with minerals, such as hydroxyapatite. The process by which the formation of the inorganic component takes place is named biomineralization. One way to introduce macromolecules in model systems for biomineralization studies is the formation of Langmuir monolayers, which are highly organized monomolecular layers of amphiphilic molecules adsorved at the liquid-air interface. These monolayers can be transferred to solid substrate to form the Langmuir-Blodgett films. In this study, it was investigated the incorporation of type-I collagen in insoluble Langmuir monolayers containing either 1,2-dipalmitoyl-sn-glycero-3-phosphatidylcholine (DPPC) or octadecylphosphonic acid (OPA) and their transference to titanium supports using the Langmuir-Blodgett technique. These films were used as matrices to the growth of biomimetic hydroxyapatite by the exposure of the modified titanium discs to a solution that mimics the ions concentration and pH of the human blood plasma. The samples were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), vibrational spectroscopy in the infrared region (FTIR), and X-ray diffraction (XRD). The Ca/P molar ratio was determined by energy dispersive X-ray spectroscopy (EDS). The properties of the biomaterials as wettability, roughness, and surface free energy were also studied. The biocompatibility of the samples was studied in vitro using osteoblasts viability assays. The collagen interacts with the phospholipids at air/water interface as evidenced by the pressure surface-surface area isotherms obtained in the presence of the protein. Moreover, the stability of the Langmuir monolayers was increased when collagen is present at the subphase. The incorporation of collagen and phospholipids on the titanium surfaces is important to the formation of organized, continuous and uniform inorganic films composed by biomimetic hydroxyapatite nanoparticles, similar to that found in the natural bone. These films are not toxic to osteoblasts as evidenced by the stimulation of their proliferation on the titanium-modified samples.