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Plasmonic metasurfaces enable functionalities that extend beyond the possibilities of classical optical materials and as a result, have gained significant research interest over the years. This thesis aims towards introducing plasmonic metamaterials and metasurfaces, a two-dimensional subset of metamaterials. The thesis also provides insights into the nonlinear optical responses from subwavelength metallic nanostructures manifesting as extraordinary physical phenomena like the second harmonic generation (SHG). The hydrodynamic Drude model is a theory that characterizes electron conduction in a hydrodynamic way to predict optical responses of metals. The thesis discusses the various contributions to the second-order optical nonlinearities from the terms in the hydrodynamic model: Coulomb, convection, and the Lorentz magnetic force. The significance of these terms, specifically the Lorentz magnetic term, is validated in contrast with existing research. The details of the work carried out to achieve a significant contribution to SHG from the Lorentz magnetic term are provided. A dominant Lorentz magnetic force for SHG was achieved through engineering T-shaped aperture arrays milled into a thin gold film. The dimensions of these structures were tuned for fundamental wavelength resonance. The structures exhibit both magnetic and electric field enhancements at the plasmonic resonance. Furthermore, a revised theoretical model is developed to accurately predict both linear and nonlinear optical responses of metamaterials. The model is based on the hydrodynamic Drude model and nonlinear scattering theory. Results from the finite difference time domain simulations performed on the metasurface are presented. It is observed that the T-shaped structure provides 65% greater nonlinear generation from the Lorentz magnetic term than the sum of the other two hydrodynamic terms. The influence of incident beam polarization on SHG conversion efficiency was also investigated. It was discovered that even though the contributions of hydrodynamic (Coulomb and convection) terms are maximum at 0◦ and 90◦, the metasurface shows maximum SHG intensity at 45◦ which indicates a dominant Lorentz magnetic term. Experimental validation was performed using the fabricated metasurface and a good agreement between the experiment and theoretical calculations was observed. Another aspect of the magnetic Lorentz force contribution, Bethe’s aperture theory was evaluated for a circular aperture at off-normal incident light. It is shown that the Lorentz force dominates the SHG by an order of magnitude at angled incidence where the generation is maximized. The angular dependence was observed to match the magnetic and electric dipole interaction effects as predicted from Bethe’s theory. The revised theory developed in this thesis predicts the linear and nonlinear optical responses of metamaterials including their angular dependency. The analysis and numerical calculations for a circular aperture agree well with past experiments. To conclude, the thesis provides an outlook on future developments in the field of nonlinear plasmonic research with regards to the development of highly efficient nonlinear metasurfaces through optimization of the Lorentz contributions. An insight into the recent developments in nanofabrication capabilities, design methodologies, nano-characterization techniques, modern electromagnetic simulations is discussed as avenues for future research in nanophotonic and nanoplasmonic device design and development. / Graduate

O objetivo deste estudo foi o de avaliar os efeitos da irradiação laser de Er,Cr:YSGG em superfícies dentinárias no tratamento da hipersensibilidade dentinária cervical, em busca de um protocolo para ser aplicado clinicamente. Para o teste de permeabilidade, foram preparados 144 pré-molares, as coroas seccionadas e as raízes impermeabilizadas. Duas áreas de irradiação antagônicas foram delimitadas e livres da impermeabilização (controle e experimental). A seguir, os dentes foram subdivididos em dois sub-grupos, diferindo o condicionamento da superfície irradiada (EDTA 24% e ácido fosfórico 35%) e em grupos diferindo o protocolo:G1)Er:YAG, 60mJ/2Hz; G2)0,25W; G3)0,5W; G4)0,75W; G5)1W, G6)1,25W; G7)1,50W; G8)1,75W G9)2W. Após as irradiações, os espécimes foram imersos em azul de metileno 2% por 4 horas, e incluídos em resina epóxica para a realização dos cortes longitudinais. Estes tiveram suas imagens trabalhadas em computador para mensuração do nível de infiltração. Os dados foram submetidos à análise estatística. O Sub-grupo 1, condicionado com EDTA, apresentou diferenças entre os grupos sendo que as amostras irradiadas com Er:YAG demonstraram menor infiltração, diferindo estatisticamente dos grupos 3, 6 e 9. Os resultados do sub-grupo 2 mostraram que as médias das amostras irradiadas com Er:YAG tenderam a zero entretanto, não houve diferença entre os grupos. Na Fase B, fragmentos de dentina foram obtidos da região cervical de dentes humanos, preparados para análise em microscopia eletrônica de varredura. Morfologicamente, observou-se oclusão parcial dos túbulos dentinários após irradiação com Er:YAG e Er,Cr:YSGG nas condições de 0,25W e 0,50W. A partir de 0.75W, foi observado abertura dos túbulos e à medida que as energias aumentaram, foram observadas carbonização e fendas. De posse dos resultados dos trabalhos in vitro, foram selecionados os parâmetros para a aplicação e o acompanhamento clínico de 1 mês: G1)controle (placebo); G2)Er:YAG; G3)Er,Cr:YSGG 0,25W e G4)Er,Cr:YSGG 0,75W. Após a triagem, foram selecionados voluntários de acordo com critérios de exclusão e inclusão. O nível de sensibilidade de cada voluntário foi avaliado através da escala visual analógica de dor (VAS) com auxílio do ar da seringa tríplice 1 semana antes (Pré-1), 5 minutos anterior ao tratamento (Pré-2), após 5 minutos (Pós-1), 1 semana (Pós-2) e 1 mês após o tratamento (Pós-3). Os dados foram coletados e submetidos à análise estatística separadamente para os dois estímulos realizados: spray de ar e sonda exploradora. Tanto para o estímulo ar quanto para o estímulo sonda, não foram observadas diferenças estatisticamente significantes nas escalas Pré-1 e Pré-2, concluindo que os pacientes estavam padronizados e não houve efeito da profilaxia nos níveis de dor. Ao estímulo do spray de ar, nota-se uma redução nos níveis de dor na escala Pós-1, porém há uma estabilidade dos valores das escalas seguintes. O grupo 2 (Er:YAG) apresentou o menor nível de dor quando comparado aos outros grupos. Ao estímulo mecânico foi observado que o grupo 4 (Er,Cr:YSGG 0,50W) demonstrou o decréscimo de dor mais acentuado imediatamente após o tratamento, porém ao final do estudo, apresentou os maiores níveis de dor. Os grupos 1, 2 e 3 apresentam redução de dor, porém estatisticamente diferentes do grupo 4. Com base nos resultados apresentados e dentro dos limites e parâmetros estudados, pode-se concluir que nenhuma condição foi capaz de eliminar completamente a microinfiltração e diminuir a permeabilidade dentinária; porém o laser de Er:YAG e o laser de Er,Cr:YSGG 0,25W apresentaram resultados satisfatórios nos três estudos realizados. / The aim of the present study was to determine the correct parameters of the Er,Cr:YSGG laser in the treatment of cervical dentin hypersensitivity. This work was presented in 3 different stages. In the first one, it was evaluated the decrease in dentin permeability of dentinal tubules after Er,Cr:YSGG laser irradiation in radicular surfaces. Ninety premolars were prepared with its crows sectioned, and the roots completely impermeabilized. Two antagonist areas of irradiation were determined as control and experimental. Each surface was conditioned with EDTA 24% (sub-group1) and phosphoric acid 35% (sub-group2) and the selected parameters were: 1)Er:YAG, 60mJ, 2Hz, 4 irradiations of 20sec each, defocused mode; and groups 2 to 9 received irradiation with Er,Cr:YSGG laser, 20Hz, Z6 tip, 600µm diameter, defocus mode, 0% of air and water: 2)Er,Cr:YSGG 0,25W; 3) 0,5W; 4) 0,75W; 5) 1,0W; 6) 1,25W, 7) 1,50W, 8) 2W; 9) 2 W. After irradiation, samples were immersed in a solution of methylene blue for 4 hours, washed for 5 min and included in epoxy resin to allow longitudinal cuts. The images were digitalized and computed worked. Data was statistically analyzed. Although the samples irradiated with Er:YAG showed less microleakage, the sub-group 1 showed differences between the groups, statistically different from groups 3, 6 e 9. The results of the sub-group 2 showed that the mean values of the Er:YAG samples had a tendency to be negative, however, no differences were detected between the groups. In the second stage, cuts from the cervical area were obtained and prepared for scanning electron microscopy to evaluate the superficial morphology. It was observed the partial closure of dentinal tubules after the irradiation with Er:YAG and Er,Cr:YSGG laser in the 0.25 and 0.50W protocols. From the 0.75W until 2W, it was observed the dentinal tubules opened as the energy densities raised. With the results of the in vitro studies, the parameters were selected: G1)control; G2)Er:YAG; G3)Er,Cr:YSGG 0,25W e G4)Er,Cr:YSGG 0,75W. Thirty subjects, who met the entry criteria, were admitted into the study. The assessment method used to quantify sensitivity was the cold air syringe, recorded by the visual analogue scale (VAS), prior to treatment as baseline (Pre-1), immediately before (Pre-2) and immediately after (Post-1) the topical treatment, after 1 week (Post-2) and after 1 month (Post-3). Teeth were assigned to the 4 groups. After the follow-up, data was collected and submitted to statistical analysis for both kinds of stimulus: evaporative (air) and mechanical (probe). For both air and probe it was not observed differences among the Pre-1 and Pre-2 moments, for what it can be concluded that patients were standardized. Analyzing the evaporative stimulus, it can be observed the reduction in the pain level immediately after the treatment; however there was stability in the next values. Group 2 (Er:YAG) showed the least level of pain. Throughout the mechanical stimulus, it was observed that group 4 (Er,Cr:YSGG 0,50W) showed the most pronounced decrease of pain immediately after treatment, however, at the end of the study, the levels of pain increased. Groups 1, 2 e 3 showed reduction of pain, statistically different from the group 4. Based on the results and within the limits of this study, it can be concluded that none of the parameters and lasers studied were capable of eliminate the microleakage and decrease the dentin permeability, however, the Er:YAG and Er,Cr:YSGG 0,25W lasers showed satisfactory results in the three studies performed.

O objetivo deste estudo foi o de avaliar os efeitos da irradiação laser de Er,Cr:YSGG em superfícies dentinárias no tratamento da hipersensibilidade dentinária cervical, em busca de um protocolo para ser aplicado clinicamente. Para o teste de permeabilidade, foram preparados 144 pré-molares, as coroas seccionadas e as raízes impermeabilizadas. Duas áreas de irradiação antagônicas foram delimitadas e livres da impermeabilização (controle e experimental). A seguir, os dentes foram subdivididos em dois sub-grupos, diferindo o condicionamento da superfície irradiada (EDTA 24% e ácido fosfórico 35%) e em grupos diferindo o protocolo:G1)Er:YAG, 60mJ/2Hz; G2)0,25W; G3)0,5W; G4)0,75W; G5)1W, G6)1,25W; G7)1,50W; G8)1,75W G9)2W. Após as irradiações, os espécimes foram imersos em azul de metileno 2% por 4 horas, e incluídos em resina epóxica para a realização dos cortes longitudinais. Estes tiveram suas imagens trabalhadas em computador para mensuração do nível de infiltração. Os dados foram submetidos à análise estatística. O Sub-grupo 1, condicionado com EDTA, apresentou diferenças entre os grupos sendo que as amostras irradiadas com Er:YAG demonstraram menor infiltração, diferindo estatisticamente dos grupos 3, 6 e 9. Os resultados do sub-grupo 2 mostraram que as médias das amostras irradiadas com Er:YAG tenderam a zero entretanto, não houve diferença entre os grupos. Na Fase B, fragmentos de dentina foram obtidos da região cervical de dentes humanos, preparados para análise em microscopia eletrônica de varredura. Morfologicamente, observou-se oclusão parcial dos túbulos dentinários após irradiação com Er:YAG e Er,Cr:YSGG nas condições de 0,25W e 0,50W. A partir de 0.75W, foi observado abertura dos túbulos e à medida que as energias aumentaram, foram observadas carbonização e fendas. De posse dos resultados dos trabalhos in vitro, foram selecionados os parâmetros para a aplicação e o acompanhamento clínico de 1 mês: G1)controle (placebo); G2)Er:YAG; G3)Er,Cr:YSGG 0,25W e G4)Er,Cr:YSGG 0,75W. Após a triagem, foram selecionados voluntários de acordo com critérios de exclusão e inclusão. O nível de sensibilidade de cada voluntário foi avaliado através da escala visual analógica de dor (VAS) com auxílio do ar da seringa tríplice 1 semana antes (Pré-1), 5 minutos anterior ao tratamento (Pré-2), após 5 minutos (Pós-1), 1 semana (Pós-2) e 1 mês após o tratamento (Pós-3). Os dados foram coletados e submetidos à análise estatística separadamente para os dois estímulos realizados: spray de ar e sonda exploradora. Tanto para o estímulo ar quanto para o estímulo sonda, não foram observadas diferenças estatisticamente significantes nas escalas Pré-1 e Pré-2, concluindo que os pacientes estavam padronizados e não houve efeito da profilaxia nos níveis de dor. Ao estímulo do spray de ar, nota-se uma redução nos níveis de dor na escala Pós-1, porém há uma estabilidade dos valores das escalas seguintes. O grupo 2 (Er:YAG) apresentou o menor nível de dor quando comparado aos outros grupos. Ao estímulo mecânico foi observado que o grupo 4 (Er,Cr:YSGG 0,50W) demonstrou o decréscimo de dor mais acentuado imediatamente após o tratamento, porém ao final do estudo, apresentou os maiores níveis de dor. Os grupos 1, 2 e 3 apresentam redução de dor, porém estatisticamente diferentes do grupo 4. Com base nos resultados apresentados e dentro dos limites e parâmetros estudados, pode-se concluir que nenhuma condição foi capaz de eliminar completamente a microinfiltração e diminuir a permeabilidade dentinária; porém o laser de Er:YAG e o laser de Er,Cr:YSGG 0,25W apresentaram resultados satisfatórios nos três estudos realizados. / The aim of the present study was to determine the correct parameters of the Er,Cr:YSGG laser in the treatment of cervical dentin hypersensitivity. This work was presented in 3 different stages. In the first one, it was evaluated the decrease in dentin permeability of dentinal tubules after Er,Cr:YSGG laser irradiation in radicular surfaces. Ninety premolars were prepared with its crows sectioned, and the roots completely impermeabilized. Two antagonist areas of irradiation were determined as control and experimental. Each surface was conditioned with EDTA 24% (sub-group1) and phosphoric acid 35% (sub-group2) and the selected parameters were: 1)Er:YAG, 60mJ, 2Hz, 4 irradiations of 20sec each, defocused mode; and groups 2 to 9 received irradiation with Er,Cr:YSGG laser, 20Hz, Z6 tip, 600µm diameter, defocus mode, 0% of air and water: 2)Er,Cr:YSGG 0,25W; 3) 0,5W; 4) 0,75W; 5) 1,0W; 6) 1,25W, 7) 1,50W, 8) 2W; 9) 2 W. After irradiation, samples were immersed in a solution of methylene blue for 4 hours, washed for 5 min and included in epoxy resin to allow longitudinal cuts. The images were digitalized and computed worked. Data was statistically analyzed. Although the samples irradiated with Er:YAG showed less microleakage, the sub-group 1 showed differences between the groups, statistically different from groups 3, 6 e 9. The results of the sub-group 2 showed that the mean values of the Er:YAG samples had a tendency to be negative, however, no differences were detected between the groups. In the second stage, cuts from the cervical area were obtained and prepared for scanning electron microscopy to evaluate the superficial morphology. It was observed the partial closure of dentinal tubules after the irradiation with Er:YAG and Er,Cr:YSGG laser in the 0.25 and 0.50W protocols. From the 0.75W until 2W, it was observed the dentinal tubules opened as the energy densities raised. With the results of the in vitro studies, the parameters were selected: G1)control; G2)Er:YAG; G3)Er,Cr:YSGG 0,25W e G4)Er,Cr:YSGG 0,75W. Thirty subjects, who met the entry criteria, were admitted into the study. The assessment method used to quantify sensitivity was the cold air syringe, recorded by the visual analogue scale (VAS), prior to treatment as baseline (Pre-1), immediately before (Pre-2) and immediately after (Post-1) the topical treatment, after 1 week (Post-2) and after 1 month (Post-3). Teeth were assigned to the 4 groups. After the follow-up, data was collected and submitted to statistical analysis for both kinds of stimulus: evaporative (air) and mechanical (probe). For both air and probe it was not observed differences among the Pre-1 and Pre-2 moments, for what it can be concluded that patients were standardized. Analyzing the evaporative stimulus, it can be observed the reduction in the pain level immediately after the treatment; however there was stability in the next values. Group 2 (Er:YAG) showed the least level of pain. Throughout the mechanical stimulus, it was observed that group 4 (Er,Cr:YSGG 0,50W) showed the most pronounced decrease of pain immediately after treatment, however, at the end of the study, the levels of pain increased. Groups 1, 2 e 3 showed reduction of pain, statistically different from the group 4. Based on the results and within the limits of this study, it can be concluded that none of the parameters and lasers studied were capable of eliminate the microleakage and decrease the dentin permeability, however, the Er:YAG and Er,Cr:YSGG 0,25W lasers showed satisfactory results in the three studies performed.

Este estudo clínico randomizado duplo-cego avaliou a efetividade da irradiação com o laser de Nd:YAG e de uma pasta de fosfosilicato de cálcio e sódio (NovaMin®) no tratamento da hipersensibilidade dentinária cervical (HDC). Após seleção dos pacientes, estes foram aleatoriamente designados para os grupos experimentais: 1. controle-placebo, 2. Pasta de fosfosilicato de cálcio e sódio - NovaMin® e 3. Laser de Nd:YAG (1W, 10Hz, 85J/cm2). A dor foi avaliada através de uma escala visual analógica de dor após estímulo evaporativo com jato de ar e estímulo tátil com sonda exploradora antes do tratamento (baseline) e após 5 minutos, 1 e 4 semanas. Quando o paciente apresentava mais de um dente com HDC, a média dos valores obtidos era considerada. A irradiação com laser de Nd:YAG foi realizada duas vezes no sentido mésio-distal e duas no sentido ocluso-gengival. A pasta contendo NovaMin® foi aplicada com taça de borracha em baixa rotação após 60 segundos em contato com os dentes. Pacientes do grupo placebo receberam simulações de cada tratamento. Os avaliadores e os pacientes desconheciam o tratamento aplicado, enquanto que o pesquisador que realizou os tratamentos desconhecia os resultados das avaliações de dor. Como os dados apresentaram distribuição normal, foram comparados pelo teste ANOVA de medidas repetidas 2 fatores. Todos os tempos experimentais demonstraram diminuição na dor em relação ao baseline (p<0,05) e não houve diferença entre os grupos experimentais em nenhum dos tempos avaliados (p>0,05). Todos os tratamentos foram igualmente efetivos na diminuição da dor da HDC. / This double-blind randomized clinical trial assessed the Nd:YAG laser and calcium sodium phosphosilicate (NovaMin®) prophy paste effect in the treatment of cervical dentin hypersensitivity (CDH). The study consisted on three experimental groups: 1. Control-placebo, 2. calcium sodium phosphosilicate prophy paste - NovaMin® and 3. Nd:YAG Laser (1W, 10Hz, 85J/cm²). Pain was evaluated through a visual analogue scale (VAS) after evaporative stimuli with air blast and tactile stimuli with exploratory probe at baseline and after 5 minutes, 1 and 4 weeks. A simple mean was calculated for each patient, using individual results. Nd:YAG laser was irradiated twice at mesio-distal direction and twice at occluso-gingival direction. Prophylaxis using NovaMin® was performed 60 seconds after paste was applied. Patients from control group received each treatment simulation. Both patients and evaluators did not know the administered treatment, as the principal researcher were blinded to the pain results. The data presented normal distribution and ANOVA for repeated measures with 2 factors was used. There was no significant differences between groups (p>0,05) and all groups presented decreased pain levels after treatments. All the treatments were equally efficient in decrease pain related to CDH.

Un nouveau mod`ele r´eduit pour le transport de faisceaux d’´electrons relativistes dans des solide ou des plasma denses est propos´e. Il est bas´e sur la r´esolution des deux premiers moments angulaires de l’´equation cin´etique relativiste, compl´et´es par une relation de fermeture d´eduite du principe de maximisation de l’entropie angulaire de Minerbo. Le mod`ele prend en compte aussi bien les effets collectifs du transport avec les champs ´electromagn´etiques auto g´en´er´es que les effets collisionnels li´es au ralentissement des ´electrons par collision sur les plasmons, les ´electrons li´es et les ´electrons libres du milieu ainsi que leur diffusion angulaire par collisions sur les ´electrons et les ions. Le mod`ele permet une r´esolution num´erique rapide des ´equations du transport de faisceau d’´electrons rapides tout en d´ecrivant l’´evolution cin´etique de leur fonction de distribution. Malgr´e le fait de travailler avec les grandeurs angulaires moyennes, le mod`ele a ´et´e valid´e par comparaison avec des solutions analytiques d´eriv´ees dans un cas acad´emique de transport de faisceau mono ´energ´etique et collimat´e dans un plasma dense et chaud d’Hydrog`ene ainsi qu’avec une simulation PIC hybride dans un cas r´ealiste de transport d’´electrons acc´el´er´es par laser dans une cible solide. Le mod`ele est appliqu´e `a l’´etude de l’´emission de photons Kα lors d’exp´eriences laser-plasma ainsi qu’a` la g´en´eration d’ondes de choc. / A new hybrid reduced model for relativistic electron beam transport in solids and dense plasmas is presented. It is based on the two first angular moments of the relativistic kinetic equation completed with the Minerbo maximum angular entropy closure. It takes into account collective effects with the self-generated electromagnetic fields as well as collisional effects with the slowing down of the elec- trons in collisions with plasmons, bound and free electrons and their angular scattering on both ions and electrons. This model allows for fast computations of relativistic electron beam transport while describing the kinetic distribution function evolution. Despite the loss of information concerning the angular distribution of the electron beam, the model reproduces analytical estimates in the academic case of a collimated and monoenergetic electron beam propagating through a warm and dense Hydro- gen plasma and hybrid PIC simulation results in a realistic laser-generated electron beam transport in a solid target. The model is applied to the study of the emission of Kα photons in laser-solid experiments and to the generation of shock waves.