Considering noninstantaneous Kerr nonlinearity, the propagation of a partially coherent optical beam are theoretically investigated by using extensions of the nonlinear Schrödinger equation (NLSE). In order to account for the partial coherence of the beam, a phase-diffusion model is used for the laser beam. To introduce the finite response time of the medium, a time dependent nonlinear response is incorporated in the system of NLSE using the Debye relaxation model. We analytically deduce the dispersion relation and numerically compute the gain spectra along with relevant second-order statistical quantities. A detailed study of how these statistical properties are influenced by the group velocity dispersion regime as well as by the delayed nonlinear response of the material is presented. The distinct features for slow and fast delayed nonlinear response are also emphasized. In another aspect of this work, we also conducted theoretical studies on such statistical characteristics near zero-dispersion regime. / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Considerando a não-linearidade não-instantânea do tipo Kerr, a propagacão de um pulso parcialmente coerente é estudado teoricamente através do uso de extensões na equação não linear de Schrödinger. Para isso, levamos em conta um modelo de difusão de fase no pulso parcialmente coerente. Para incorporar o tempo de resposta finito no meio Kerr, utilizamos uma dependência temporal na resposta não linear do meio introduzida na equação não linear de Schrödinger através do modelo de relaxação de Debye. Deduzimos analiticamente também a relação de dispersão e computamos numericamente o espectro de ganho e algumas quantidades estatísticas de segunda ordem relevantes. Neste trabalho realizamos também um estudo detalhado de como estas propriedades estatísticas são influenciadas pelos regimes de dispersão da velocidade de grupo, tanto quanto pelo atraso na resposta não linear do meio em questão. Por fim, enfatizamos as diferentes características para as respostas não lineares rápidas e lentas. Em outra vertente deste trabalho, realizamos estudos teóoricos acerca de tais características estatísticas para o regime de dispersão zero.

xiv, 138 p. : ill. (some col.) / In this dissertation, we demonstrate the generation of optical Raman frequency combs by a single laser pump pulse traveling in hydrogen-filled hollow-core optical fibers. This comb generation process is a cascaded stimulated Raman scattering effect, where higher-order sidebands are produced by lower orders scattered from hydrogen molecules. We observe more than 4 vibrational and 20 rotational Raman sidebands in the comb. They span more than three octaves in optical wavelength, largely thanks to the broadband transmission property of the fiber. We found that there are phase correlations between the generated Raman comb sidebands (spectral lines), although their phases are fluctuating from one pump pulse to another due to the inherit spontaneous initiation of Raman scattering. In the experiment, we generated two Raman combs independently from two fibers and simultaneously observed the single-shot interferences between Stokes and anti-Stokes components from the two fibers. The experimental results clearly showed the strong phase anti-correlation between first-order side bands. We also developed a quantum theory to describe this Raman comb generation process, and it predicts and explains the phase correlations we observe. The phase correlation that we found in optical Raman combs may allow us to synthesize single-cycle optical pulse trains, creating attosecond pulses. However, the vacuum fluctuation in stimulated Raman scattering will result in the fluctuation of carrier envelope phase of the pulse trains. We propose that we can stabilize the comb by simultaneously injecting an auxiliary optical beam, mutually coherent with the main Raman pump laser pulse, which is resonant with the third anti-Stokes field. / Committee in Charge: Dr. Steven van Enk, Chair; Dr. Michael G. Raymer; Dr. Daniel A. Steck; Dr. David M. Strom; Dr. Andrew H. Marcus

No description available.

Submitted by Marco Antonio Oliveira da Silva (maosilva@ipen.br) on 2017-11-09T11:26:50Z No. of bitstreams: 0 / Made available in DSpace on 2017-11-09T11:26:50Z (GMT). No. of bitstreams: 0 / Os lasers Raman permitem a exploração de novos comprimentos de onda, não comumente acessíveis, graças ao Espalhamento Raman Estimulado. Unidos a processos de conversão não linear, abrem-se campos para emissão de comprimentos de onda na região do visível no espectro eletromagnético. Com uma mesma configuração, diversas combinações de cristais possibilitam a geração de múltiplas frequências, transformando esse tipo de laser em um dispositivo compacto e barato quando comparado com outras tecnologias existentes. Este trabalho apresenta a busca da conversão intracavidade em frequências de lasers Raman, em uma configuração linear. Com dois comprimentos de onda de bombeamento de energia (797 nm e 872 nm), diodos semicondutores foram utilizados para acessar dois picos de absorção do cristal Nd:YLF. O bombeamento em 797 nm levou a emissão fundamental em 908 nm. E através do cristal KGW, com linhas de emissão Stokes, um novo comprimento de onda foi alcançado, em 990 nm. Com o cristal dobrador, BiBO, soma de frequência e segundo harmônico foram gerados, permitindo as emissões em uma região espectral azul bastante larga (450 500 nm). Com o bombeamento em 872 nm, uma emissão de três níveis no cristal Nd:YLF não foi possível, conseguindo apenas a emissão em 1064 nm, linha comum para cristais de neodímio. Uma outra cavidade foi estudada, porém com bombeamento em 880 nm e cristal de Nd:YVO4, conhecido por ser self-Raman. Com uma configuração linear semelhante à anteriormente citada, somente sua linha de emissão fundamental em 914 nm foi obtida, não sendo possível com as condições trabalhadas a emissão Stokes, que permitisse dar continuidade ao estudo. / Dissertação (Mestrado em Tecnologia Nuclear) / IPEN/D / Instituto de Pesquisas Energéticas e Nucleares - IPEN-CNEN/SP

Les plasmons polaritons de surface (SPP) et les plasmons localisés de surface (LSP) font l’objet de nombreuses investigations du fait de leur fort potentiel technologique. Récemment, une attention particulière a été portée à des systèmes supportant ces deux types de résonances en déposant des nanoparticules (NPs) métalliques sur des films minces métalliques. Plusieurs études ont mis en évidence le couplage et l’hybridation entre modes localisés et délocalisés. Cependant, une compréhension en profondeur des propriétés optiques et du potentiel de ces interfaces est toujours manquante. Nous avons mené ici une étude de systèmes NPs/film couplés. Nous avons étudié à la fois expérimentalement et théoriquement l’influence d’une couche séparatrice ultra-mince en SiO2 ainsi que l’évolution des différents modes plasmoniques pour différentes épaisseurs. Nous avons ainsi mis en lumière que de tels systèmes couplés offrent des propriétés optiques exaltées et une large accordabilité spectrale. Nous avons aussi cherché à diminuer l’épaisseur de la couche séparatrice vers le cas ultime monoatomique en utilisant le graphène. Du fait du caractère non-diélectrique de celui-ci, nous avons mis en évidence un comportement optique inattendu de la résonance plasmonique. Nous avons expliqué celui-ci par la mise en évidence du dopage du graphène par les NPs, ce qui est un premier pas en direction de dispositifs optoélectroniques à base de graphène. Enfin, après avoir amélioré notre compréhension théorique de ces systèmes, nous avons évalué leur potentiel comme capteurs SERS ou LSP / Surface plasmon polariton (SPP) and Localized surface plasmon (LSP) have attracted numerous researchers due to their high technological potential. Recently, strong attention was paid to the potential of SPP and LSP combinations by investigating metallic nanoparticles (NPs) on top of metallic thin films. Several studies on such systems have shown the coupling and hybridization between localized and delocalized modes. In this work, we propose a full systematic study on coupled NP/film systems with Au NPs and Au films. We investigate both experimentally and theoretically the influence of an ultra-thin SiO2 dielectric spacer layer, as well as the evolution of the plasmonic modes as the spacer thickness increases. We show that coupled systems exhibit enhanced optical properties and larger tunability compared to uncoupled systems. We also compare these results with those measured for coupled interfaces using graphene as a non-dielectric sub-nanometer spacer. Introducing graphene adds complexity to the system. We show that such coupled systems also exhibit enhanced optical properties and larger tunability of their spectral properties compared to uncoupled systems as well as unexpected optical behavior. We explain this behavior by evidencing graphene doping by metallic NPs, which can be a first step towards graphene based optoelectronic devices. After establishing a deep understanding of coupled systems we perform both SERS and RI sensing measurements to validate the high potential of these plasmonic interfaces

La spectroscopie Raman exaltée de surface (SERS) est largement utilisée comme un outil non-intrusif et sans marquage pour identifier les empreintes spectrales moléculaires dans des applications comme la pharmacologie, la salubrité des aliments, etc. Cette thèse présente un micro-capteur SERS basé sur un guide d'ondes hybride constitué de fentes métalliques (Au/Al) et de rubans diélectriques (Si3N4) et sur une méthode pour promouvoir la capacité de détection SERS en plaçant des nanoparticules métalliques dans la fente du capteur. L'étude théorique du capteur est principalement menée par la méthode des différences finies dans le domaine temps en trois dimensions (3D-FDTD) qui fournit la réponse électromagnétique à large bande des nanostructures métalliques. Les facteurs d'exaltation du capteur sont estimés par l’approximation |E|4. Les expériences sont basées principalement sur la fabrication de fentes métalliques, qui est réalisée par la lithographie à faisceau d'électrons (EBL), et sur la caractérisation de la capacité de détection SERS des capteurs. Les résultats montrent que les signaux Raman donnés par les capteurs SERS sont détectables. Les nanoparticules métalliques, qui sont situées dans le capteur, peuvent améliorer considérablement la capacité de détection SERS. En combinant le capteur SERS avec les éléments photoniques et électroniques, un système de détection SERS entièrement intégré sur une puce peut être développé dans un proche avenir pour des détections SERS portables et stables / Surface-enhanced Raman spectroscopy (SERS) is widely used as a non-intrusive and label-free tool to identify the molecular spectral fingerprints in pharmacology, biology, etc. This thesis presents a SERS sensor based on the hybrid waveguide made of metallic (Au/Al) slots and dielectric (Si3N4) strips and a method to improve the SERS-detection capacity by placing metallic nanoparticles into the sensor’s slot. The theoretical investigation of the sensor is mainly conducted by the 3D finite-difference time-domain method (3D-FDTD) which provides the broadband electromagnetic response of metallic nanostructures. The enhancement factors in the sensor’s slot are estimated based on the |E|4-approximation. The experiments are mainly the fabrication of metallic slots, which is conducted by the electron beam lithography (EBL), and the characterization of the SERS-detection capacity of the sensors. The results show that the Raman signals given out by the SERS sensors are detectable. Metallic nanoparticles, which are located in the sensor’s slot, can improve dramatically the SERS-detection capacity. By combining the SERS sensor with the extended photonic and electronic elements, a fully integrated-on-chip SERS detection system on a chip can be developed in the near future for portable and stable SERS detections

In this work, new small deflection magnetic actuators have been proposed, designed, and tested for applications in Surface Enhanced Raman Scattering optical sensors. Despite the fact that SERS sensors have been shown to increase Raman over ten orders of magnitude for molecular detection, several technological challenges have prevented the design of practical sensors, such as making SERS sensors that can efficiently detect a wide variety of molecules. Since the optimum signal-to-noise in SERS occurs at different excitation wavelengths for different molecules, individual metal nanostructures need to be designed and fabricated for each independent chemical species. One possible solution to this problem is to tune the plasmon resonance frequency of the metal nanoparticles to eliminate the need for individually optimized particles. In order to achieve a tunable local dielectric environment, and thus allow for control over the resonance frequency of metal nanoparticles, a new SERS sensor geometry is proposed and a large deflection magnetic actuator is fabricated and tested as a starting point for the design of a small deflection magnetic actuator. Using the newly developed SERS geometry and the optimized fabrication processing techniques, two small deflection magnetic actuator beam structures were designed, fabricated, and tested. These devices utilizes an off-chip electromagnet source able to produce a magnetic force of approximately 14 μN on the on-chip nickel film generating deflections up to 139 nm for the straight beam device and 164 nm for the curved beam device. iii In the process of characterizing the newly developed small deflection magnetic actuator, an integrated magnetic actuator with electrostatic restoration geometry was conceived. This device was designed to meet the specifications of the small deflection magnetic actuator as well as eliminate the need of an off-chip magnetic source and fully integrate the process atop the metal nanoparticle arrays. Using adhesive iron based magnetic strips as the magnetic drive source, circular NiFe beams with 1, 2, 3, and 4 mm diameters were designed and simulated. Calculations predicted maximum achievable actuation of up to 2.5 μm. Processing steps were laid out for a set of integrated devices as a possible predecessor to the newly designed small deflection magnetic actuator.

The objectives of the work presented were to 1) fabricate reproducible nanorod array SERS substrates, 2) detection of bacteria using nanorod substrates, 3) detection of DNA hybridization using nanorod substrates and 4) critically evaluate the sensing method. Important findings from this work are as follows. A novel method for batch fabrication of substrates for surface enhanced Raman scattering (SERS) has been developed using a modified platen machined to fit in a commercial electron beam evaporator. The use of this holder enables simultaneous deposition of silver nanorod (AgNR) arrays onto six microscope slide substrates utilizing glancing angle deposition. In addition to multiple substrate fabrication, patterning of the AgNR substrates with 36 wells allows for physical isolation of low volume samples. The well-to-well, slide-to-slide, and batch-to-batch variability in both physical characteristics and SERS response of substrates prepared via this method was nominal. A critical issue in the continued development of AgNR substrates is their stability over time, and the potential impact on the SERS response. The thermal stability of the arrays was investigated and changes in surface morphology were evaluated using scanning electron microscopy and x-ray diffraction and correlated with changes in SERS enhancement. The findings suggest that the shelf-life of AgNR arrays is limited by migration of silver on the surface. Continued characterization of the AgNR arrays was carried out using fluorescent polystyrene microspheres of two different sizes. Theory suggests that enhancement between nanorods would be significantly greater than at the tops due to contributing electromagnetic fields from each nanostructure. In contrast to the theory, SERS response of microspheres confined to the tops of the AgNR array was significantly greater than that for beads located within the array. The location of the microspheres was established using optical fluorescence and scanning electron microscopy. The application of SERS to characterizing pathogens such as bacteria and viruses is an active area of investigation. AgNR array-based SERS substrates have enabled detection of pathogens present in biofluids. Specifically, several publications have focused on determining the spectral bands characteristic of bacteria from different species and cell lines. Studies were carried out on three strains of bacteria as well as the medium in which the bacteria were grown. The spectra of the bacteria and medium were surprisingly similar, so additional spectra were acquired for commonly used bacterial growth media. In many instances, these spectra were similar to published spectra purportedly characteristic of specific bacterial species. In addition to bacterial samples, nucleic acid hybridization assays were investigated. Oligonucleotide pairs specifically designed to detect respiratory syncytial virus (RSV) in nasal fluids were prepared and evaluated. SERS spectra acquired on oligos, alone or in combination, contain the known spectral signatures of the nucleosides that comprise the oligo. However, spectra acquired on an oligo with a 5'- or 3' thiol were distinctly different from that acquired on the identical oligo without a thiol pendant group suggesting some control over the orientation of the oligo on the nanorod surface. The signal enhancement in SERS depends markedly upon the location of the probe relative to the substrate surface. By systematic placement of nucleotide markers along the oligo chain, the point at which the nucleotide disappears from the spectrum was identified. The overall findings for AgNR SERS substrates suggest that the applicability of SERS for detecting nucleic acid hybridization is limited. The strong distance dependence coupled with the lack of substrate stability at temperatures required for annealing oligos during hybridization suggest that AgNRs are not the platform to use for hybridization assays.

Orientadores: Daniela Zanchet, Jose Antonio Brum / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin / Made available in DSpace on 2018-08-10T04:28:03Z (GMT). No. of bitstreams: 1 Rocha_TulioCostaRizutida_D.pdf: 8952935 bytes, checksum: 2283ed573c4cf94d5cba5aa42d7b2113 (MD5) Previous issue date: 2008 / Resumo: Nanopartículas de metais nobres têm atraído uma renovada atenção nos últimos anos devido às novas aplicações científicas e tecnológicas explorando suas propriedades ópticas únicas. No regime nanométrico, é bem conhecido que a resposta óptica de metais, associada aos plásmons de superfície, depende fortemente do tamanho e também da forma. De fato, grande parte das aplicações ópticas de nanopartículas de ouro e prata baseia-se na exploração dos efeitos de forma. Porém, apesar dos esforços realizados, os processos que levam à formação de morfologias anisotrópicas ainda não são bem compreendidos e a formulação de um mecanismo geral ainda é um desafio. Nesse trabalho, foram abordados os mecanismos de formação e crescimento de nanoprismas triangulares de prata produzidos por métodos de síntese coloidal. Uma combinação de diferentes técnicas experimentais foi utilizada para estudar diversos aspectos da síntese fotoquímica, dentre eles, a evolução morfológica, a cinética da reação e a estrutura cristalina das nanopartículas. As sólidas evidências experimentais obtidas associadas a outras observações da literatura foram utilizadas na formulação de um modelo fenomenológico para explicar a formação e crescimento dos nanoprismas de prata em métodos fotoquímicos. Esse modelo baseia-se na influência dos defeitos cristalográficos, que induzem a formação dos nanoprismas nos momentos iniciais da síntese, e na excitação de plásmons de superfície, que ocorre em estágios avançados, sendo responsável pela definição do tamanho final dos nanoprismas. Adicionalmente, cálculos teóricos indicaram que aspectos energéticos podem ter um papel ativo nesse sistema, favorecendo o crescimento dos nanoprismas em relação às nanopartículas esféricas durante os estágios iniciais da síntese. Finalmente, os nanoprismas triangulares de prata produzidos foram aplicados ao estudo de efeitos de intensificação do espalhamento Raman de moléculas. Medidas espectroscópicas de moléculas depositadas na superfície de nanoprismas com diferentes tamanhos foram realizadas e a comparação quantitativa dos resultados indicou a presença de um tamanho ótimo, que é determinado por processos de perda de energia dos plásmons de superfície / Abstract: Noble metal nanoparticles have attracted a recent renewed interest due to the new scientific and technological applications exploiting their unique optical properties. At nanometric scale, it is well known that the optical response of metals, related to the excitation of surface plasmons, strongly depends not only on the size of the particles but also on their shape. Several methodologies to produce silver and gold nanoparticles with different shapes are available in the literature. However, notwithstanding the efforts that have been made, the process that lead to the formation of anisotropic morphologies has not been fully understood yet and a general mechanism is still a challenge. In this work, we address the formation and growth mechanisms of silver triangular nanoprisms produced by photochemical methods. A set of characterization tools was used to study different aspects of the photochemical synthesis, namely, the morphological evolution, the reaction kinetics and the crystalline structure of the nanoprisms. The solid experimental evidences obtained here were used to build a phenomenological model that explains the formation and growth of silver triangular nanoplates in photochemical methods. This model was based on the influence of crystallographic defects, which induce the formation of the nanoprismas in the initial stages of the synthesis, and on the excitation of surface plasmons, which occurs in advanced stages and it is responsible for the definition of the final size of the nanoprismas. Additionally, theoretical calculations indicate that energetics might play an important role in this system, favoring the growth of nanoprismas relative to spheres. Finally, the silver triangular nanoprisms were used to study enhancement effects in the Raman scattering of molecules. We performed spectroscopic measurements for nanoplates with different sizes and the quantitative comparison of the curves indicated the existence of an optimum size that is dictated by surface plasmon energy losses / Doutorado / Física da Matéria Condensada / Doutor em Ciências

Orientadores: Aurea Rosas Vasconcellos, Roberto Luzzi / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin / Made available in DSpace on 2018-08-06T02:30:23Z (GMT). No. of bitstreams: 1 AndradeNeto_AntonioVieirade_D.pdf: 580703 bytes, checksum: 8cd331112c8a9047f3815f8b9238e984 (MD5) Previous issue date: 2005 / Resumo: Neste trabalho realizamos um estudo pormenorizado das propriedades ópticas de semicondutores polares de gap direto dopado tipo n.Em particular nos concentramos nos efeitos de muitos corpos (interação coulombiana)e na in .uência da interação elétron fônon LO (potencial de Fröhlich)sobre as propriedades ópticas do sistema. Para tanto,inicialmente,calculamos a função dielétrica longitudinal do sistema recorrendo ao elegante,prático e poderoso método das Funções de Green Termodinâmicas de Tempo Duplo. Obtivemos expressões analíticas para as partes real e imaginária da função dielétrica onde estão incorporados efeitos dinâmicos. Foi evidenciado o inter-relacionamento entre os efeitos coletivos ¿gerados pela interação coulombiana ¿e a interação polar.Isto se manifesta claramente nas expressões obtidas para a renormalização das energias de excitação bem como nas funções de relaxação dinâmicas associadas com os efeitos dissipativos no sistema.Tais características se mostram fundamentais para que os resultados numéricos,obtidos a partir da teoria,quando comparados com as curvas experimentais forneçam um muito bom acordo em posição e forma das bandas de espalhamento Raman por modos híbridos de plasmons-fônons LO e o espectros de re .etividade do GaN, inclusive é evidenciada e interpretada,uma banda anômala observada experimentalmente / Abstract: A detailed analysis of the in fluence of the polar and Coulomb interactions, and brief comments on impurities,on the optical properties of III-Nitrides is presented.Raman scattering by coupled plasmon-LO phonon modes is considered in particular.Numerical calculations are done in the case of n-doped GaN obtaining excellent agreement with the experimental data and,in the process,the explanation of certain observed so-called anomalies is done.A brief study of re .ectivity spectra is also included / Doutorado / Física da Matéria Condensada / Doutor em Ciências