For cavity quantum electrodynamics systems (cavity-QED) to play a role in quantum information processing applications and in quantum networks, they must be robust and scalable in addition to having a suitable method for the generation, processing and storage of quantum bits. One solution is to develop a composite system that couples a nitrogen vacancy (NV) center in diamond to a whispering gallery mode supported by a fused silica microsphere. Such a system is motivated by the optical and electron-spin properties of the NV center. The NV center is the leading spin-qubit and exhibits atomic like linewidths at cryogenic temperatures and has spin coherence times greater than milliseconds at room temperature. These long coherence times, coupled with nanosecond scale spin readout and manipulation times, allow for millions of quantum operations to be processed. Silica whispering gallery resonators are the only class of microresonators with quality factor high enough to reach the strong coupling regime, which is necessary for some quantum information processing applications. Integrating these two components into a system that could position a diamond nanopillar near the surface of a deformed-double stemmed microsphere system, with nanometer precision, at 10 K was a major achievement of this research. Cavity resonances in deformed microspheres can be excited with a free-space coupling technique which simplifies their integration into cryogenic environments. In these intentionally deformed resonators, an enhanced evanescent field decay length was observed at specific locations along the ray orbit. The double-stem arrangement enables the cavity resonance to be tuned over 450 GHz, with sub-10 MHz resolution, at 10 K. These two features, the enhanced decay length and broad range tuning with high resolution, are indispensible tools for cavity-QED studies with silica microspheres. Diamond nanopillars were fabricated from single crystal diamond with diameters as small as 140 nm in order to maintain a high quality factor. Studies were conducted on NV centers in nanopillars and bulk diamond to determine their suitability for cavity-QED applications. In an attempt to increase the light-matter interaction between NV centers and whispering gallery modes, diamond substrates were optically characterized that were irradiated with nitrogen ions.

Os micro-ressonadores que suportam whispering gallery modes têm atraído a atenção da comunidade científica devido a sua grande capacidade de confinar a luz, propriedade que faz dessas estruturas plataformas ideais para o desenvolvimento de pesquisa fundamental como interação da radiação com a matéria e óptica não linear. Além disso, suas características como operação em frequências do visível e de telecomunicações, facilidade de integração e alta sensitividade os tornam extremamente flexíveis para aplicações que vão desde filtros ópticos até sensores. Neste trabalho, demonstramos a fabricação de tais micro-ressonadores via fotopolimerização por absorção de dois fótons (FA2F). Esta técnica apresenta uma série de vantagens para a confecção de micro-dispositivos, sendo elas a capacidade de resolução inferior ao limite de difração, a flexibilidade de formas e ainda, a possibilidade de incorporar compostos de interesse à matriz polimérica a fim de introduzir novas funcionalidades ao material que compõe a estrutura final. Ademais, diferentes polímeros podem ser utilizados para a fabricação das microestruturas, tornando a técnica viável para uma vasta gama de aplicações. As microestruturas poliméricas que fabricamos são micro-cilindros ocos de boa integridade estrutural com 45 μm de diâmetro externo e 100 nm de rugosidade de superfície, o que as torna potencialmente aplicáveis como micro-ressonadores para frequências de operação típicas de telecomunicações. A fim de acoplar luz nessas estruturas, em colaboração com a Universidade de Valência, na Espanha, montamos um aparato de acoplamento. Neste aparato, a luz proveniente de uma fonte de luz centrada em 1540 nm é acoplada nos micro-ressonadores via campo evanescente por meio do uso de uma fibra óptica estirada de 1.5 μm de diâmetro. A potência transmitida é guiada para um analisador de espectro óptico, onde é possível identificar os modos ressonantes, representados como picos de atenuação com free spectral range em torno de 9.8 nm. Ao término desse projeto, um aparato similar foi montado no Grupo de Fotônica do IFSC/USP, a partir do qual pudemos medir os modos ressonantes tanto de fibras ópticas estiradas quanto dos micro-cilindros poliméricos. A finesse dos micro-ressonadores poliméricos caracterizados varia de 2.51 a 4.35, sendo da mesma ordem de grandeza do valor reportado na literatura para ressonadores de alta performance fabricados por FA2F a partir da mesma formulação de resina polimérica que utilizamos. / Whispering gallery modes microresonators have been attracting increasing interest due to their ability to strongly confine light within small dielectric volumes. This property is quite useful for basic research involving light-matter interaction and nonlinear optics, but their applications go beyond that. The ease of fabrication, on-chip integration and operation at telecommunication frequencies make them suitable for a variety of practical applications, including photonic filters and sensing. In the current work, we demonstrate the fabrication of such resonators via two-photon polymerization. Using this technique, complex 3D structures with submicrometer feature size can be produced. Besides, the flexibility of geometry and the possibility of incorporating a variety of additional materials, such as organic compounds make it a powerful tool for the fabrication of microresonators. The microstructures we have fabricated are 45 μm outer diameter hollow microcylinders, with good structural integrity and sidewall roughness estimated in 100 nm, which make their application as microresonators feasible in the near infrared wavelength regime. In order to couple light within these microresonators, an experimental setup was built at University of Valencia to implement the coupling. In this setup, light from a 1540 nm-centered broadband source was coupled into the fabricated microresonators via evanescent field using a 1.5 μm waist tapered fiber. The transmitted light was then guided to an optical spectral analyzer, where it was possible to measure resonances, represented as attenuation peaks, with free spectral range of about 9.8 nm. Afterwards, a similar experimental setup was assembled in the Photonics group at IFSC/USP, where we could observe resonances of both tapered optical fibers and the polymeric microresonators fabricated by means of two-photon polymerization. The finesse of the polymeric microresonators was estimated in 4.35, being in the same order of the finesse reported in the literature for high performance microring resonators fabricated using the same polymeric resin.

Os micro-ressonadores que suportam whispering gallery modes têm atraído a atenção da comunidade científica devido a sua grande capacidade de confinar a luz, propriedade que faz dessas estruturas plataformas ideais para o desenvolvimento de pesquisa fundamental como interação da radiação com a matéria e óptica não linear. Além disso, suas características como operação em frequências do visível e de telecomunicações, facilidade de integração e alta sensitividade os tornam extremamente flexíveis para aplicações que vão desde filtros ópticos até sensores. Neste trabalho, demonstramos a fabricação de tais micro-ressonadores via fotopolimerização por absorção de dois fótons (FA2F). Esta técnica apresenta uma série de vantagens para a confecção de micro-dispositivos, sendo elas a capacidade de resolução inferior ao limite de difração, a flexibilidade de formas e ainda, a possibilidade de incorporar compostos de interesse à matriz polimérica a fim de introduzir novas funcionalidades ao material que compõe a estrutura final. Ademais, diferentes polímeros podem ser utilizados para a fabricação das microestruturas, tornando a técnica viável para uma vasta gama de aplicações. As microestruturas poliméricas que fabricamos são micro-cilindros ocos de boa integridade estrutural com 45 μm de diâmetro externo e 100 nm de rugosidade de superfície, o que as torna potencialmente aplicáveis como micro-ressonadores para frequências de operação típicas de telecomunicações. A fim de acoplar luz nessas estruturas, em colaboração com a Universidade de Valência, na Espanha, montamos um aparato de acoplamento. Neste aparato, a luz proveniente de uma fonte de luz centrada em 1540 nm é acoplada nos micro-ressonadores via campo evanescente por meio do uso de uma fibra óptica estirada de 1.5 μm de diâmetro. A potência transmitida é guiada para um analisador de espectro óptico, onde é possível identificar os modos ressonantes, representados como picos de atenuação com free spectral range em torno de 9.8 nm. Ao término desse projeto, um aparato similar foi montado no Grupo de Fotônica do IFSC/USP, a partir do qual pudemos medir os modos ressonantes tanto de fibras ópticas estiradas quanto dos micro-cilindros poliméricos. A finesse dos micro-ressonadores poliméricos caracterizados varia de 2.51 a 4.35, sendo da mesma ordem de grandeza do valor reportado na literatura para ressonadores de alta performance fabricados por FA2F a partir da mesma formulação de resina polimérica que utilizamos. / Whispering gallery modes microresonators have been attracting increasing interest due to their ability to strongly confine light within small dielectric volumes. This property is quite useful for basic research involving light-matter interaction and nonlinear optics, but their applications go beyond that. The ease of fabrication, on-chip integration and operation at telecommunication frequencies make them suitable for a variety of practical applications, including photonic filters and sensing. In the current work, we demonstrate the fabrication of such resonators via two-photon polymerization. Using this technique, complex 3D structures with submicrometer feature size can be produced. Besides, the flexibility of geometry and the possibility of incorporating a variety of additional materials, such as organic compounds make it a powerful tool for the fabrication of microresonators. The microstructures we have fabricated are 45 μm outer diameter hollow microcylinders, with good structural integrity and sidewall roughness estimated in 100 nm, which make their application as microresonators feasible in the near infrared wavelength regime. In order to couple light within these microresonators, an experimental setup was built at University of Valencia to implement the coupling. In this setup, light from a 1540 nm-centered broadband source was coupled into the fabricated microresonators via evanescent field using a 1.5 μm waist tapered fiber. The transmitted light was then guided to an optical spectral analyzer, where it was possible to measure resonances, represented as attenuation peaks, with free spectral range of about 9.8 nm. Afterwards, a similar experimental setup was assembled in the Photonics group at IFSC/USP, where we could observe resonances of both tapered optical fibers and the polymeric microresonators fabricated by means of two-photon polymerization. The finesse of the polymeric microresonators was estimated in 4.35, being in the same order of the finesse reported in the literature for high performance microring resonators fabricated using the same polymeric resin.

The technique of single particle Total Internal Reflection Microscopy (TIRM) has been used to study the scattering intensity from levitated microspheres. TIRM can be used to monitor the separation between microscopic spheres immersed in liquid (water in our case) and a surface with nm resolution. In the technique, microspheres scatter light when the evanescent waves are incident upon them. The intensity of the scattered light is directly related to the height above the surface and allows determination of the height. From the separation distance histograms, the interaction between the microsphere and interface may be characterized with a force resolution in the range of 0.01 picoNewtons. Such a system can be applied to the measurement of biomolecular interactions biomolecules attached to the microsphere and the surface. The intensity and scattering pattern of this light has been modeled using a modified Mie theory which accounts for the evanescent nature of the incident light. Diffusing Colloidal Probe Microscopy (DCPM) is an extension of the TIRM technique that simultaneously monitors multiple microsphere probes. The use of multiple probes introduces the issue of probe polydispersity. When measured at the surface, a variation in scattered light intensity of nearly one order of magnitude has been observed from a purchased microsphere sample. Thus the polydisperse collection of microspheres adds significant complexity to the scattered light signal. It is hypothesized that the dependence of the total scattered light intensity on microsphere size accounts for the scattered intensity distribution in a polydisperse microsphere sample. Understanding this variation in the scattered light with microsphere size will allow improved characterization of the microsphere/surface separation. Additionally, larger microspheres have the ability to resonantly confine light and produce spectrally narrow Whispering Gallery Modes (WGMs). It is hypothesized that WGMs may be excited in microspheres with the DCPM system. These modes may be used as a refractometric biosensor with high sensitivity to local refractive index changes on the surface of the microsphere. This research involves modeling scattered intensity distributions for polydispersed collections of microspheres based on modified Mie theory. The theoretical results are compared to experimentally obtained results and found to qualitatively explain the scattered light intensity distribution in a multiple probe DCPM system. This is an important result suggesting that microsphere size variation plays a major role in determining the distribution of scattered intensity in multiple microsphere probe systems. This work also suggests that it may be possible to excite such WGMs in a DCPM system. The introduction of WGMs would enable refractometric biosensing in such evanescent mode systems.

The technique of single particle Total Internal Reflection Microscopy (TIRM) has been used to study the scattering intensity from levitated microspheres. TIRM can be used to monitor the separation between microscopic spheres immersed in liquid (water in our case) and a surface with nm resolution. In the technique, microspheres scatter light when the evanescent waves are incident upon them. The intensity of the scattered light is directly related to the height above the surface and allows determination of the height. From the separation distance histograms, the interaction between the microsphere and interface may be characterized with a force resolution in the range of 0.01 picoNewtons. Such a system can be applied to the measurement of biomolecular interactions biomolecules attached to the microsphere and the surface. The intensity and scattering pattern of this light has been modeled using a modified Mie theory which accounts for the evanescent nature of the incident light. Diffusing Colloidal Probe Microscopy (DCPM) is an extension of the TIRM technique that simultaneously monitors multiple microsphere probes. The use of multiple probes introduces the issue of probe polydispersity. When measured at the surface, a variation in scattered light intensity of nearly one order of magnitude has been observed from a purchased microsphere sample. Thus the polydisperse collection of microspheres adds significant complexity to the scattered light signal. It is hypothesized that the dependence of the total scattered light intensity on microsphere size accounts for the scattered intensity distribution in a polydisperse microsphere sample. Understanding this variation in the scattered light with microsphere size will allow improved characterization of the microsphere/surface separation. Additionally, larger microspheres have the ability to resonantly confine light and produce spectrally narrow Whispering Gallery Modes (WGMs). It is hypothesized that WGMs may be excited in microspheres with the DCPM system. These modes may be used as a refractometric biosensor with high sensitivity to local refractive index changes on the surface of the microsphere. This research involves modeling scattered intensity distributions for polydispersed collections of microspheres based on modified Mie theory. The theoretical results are compared to experimentally obtained results and found to qualitatively explain the scattered light intensity distribution in a multiple probe DCPM system. This is an important result suggesting that microsphere size variation plays a major role in determining the distribution of scattered intensity in multiple microsphere probe systems. This work also suggests that it may be possible to excite such WGMs in a DCPM system. The introduction of WGMs would enable refractometric biosensing in such evanescent mode systems.

The technique of single particle Total Internal Reflection Microscopy (TIRM) has been used to study the scattering intensity from levitated microspheres. TIRM can be used to monitor the separation between microscopic spheres immersed in liquid (water in our case) and a surface with nm resolution. In the technique, microspheres scatter light when the evanescent waves are incident upon them. The intensity of the scattered light is directly related to the height above the surface and allows determination of the height. From the separation distance histograms, the interaction between the microsphere and interface may be characterized with a force resolution in the range of 0.01 picoNewtons. Such a system can be applied to the measurement of biomolecular interactions biomolecules attached to the microsphere and the surface. The intensity and scattering pattern of this light has been modeled using a modified Mie theory which accounts for the evanescent nature of the incident light. Diffusing Colloidal Probe Microscopy (DCPM) is an extension of the TIRM technique that simultaneously monitors multiple microsphere probes. The use of multiple probes introduces the issue of probe polydispersity. When measured at the surface, a variation in scattered light intensity of nearly one order of magnitude has been observed from a purchased microsphere sample. Thus the polydisperse collection of microspheres adds significant complexity to the scattered light signal. It is hypothesized that the dependence of the total scattered light intensity on microsphere size accounts for the scattered intensity distribution in a polydisperse microsphere sample. Understanding this variation in the scattered light with microsphere size will allow improved characterization of the microsphere/surface separation. Additionally, larger microspheres have the ability to resonantly confine light and produce spectrally narrow Whispering Gallery Modes (WGMs). It is hypothesized that WGMs may be excited in microspheres with the DCPM system. These modes may be used as a refractometric biosensor with high sensitivity to local refractive index changes on the surface of the microsphere. This research involves modeling scattered intensity distributions for polydispersed collections of microspheres based on modified Mie theory. The theoretical results are compared to experimentally obtained results and found to qualitatively explain the scattered light intensity distribution in a multiple probe DCPM system. This is an important result suggesting that microsphere size variation plays a major role in determining the distribution of scattered intensity in multiple microsphere probe systems. This work also suggests that it may be possible to excite such WGMs in a DCPM system. The introduction of WGMs would enable refractometric biosensing in such evanescent mode systems.

New methods of biological analyte sensing are needed for development of miniature biosensors that are highly sensitive and require minimal sample preparation. One novel technique employs optical resonances known as Whispering Gallery Modes (WGMs). These modes arise from total internal reflection of light at the internal surface of a high index microsphere within a low index medium and produce an evanescent field that extends into the surrounding medium. The WGMs produce multiple narrow spectral peaks that shift position with variations in the local index of refraction sampled by the evanescent tail of the WGMs. To excite these WGMs, we embed quantum dots (QDs) in the periphery of polystyrene microspheres to serve as local light sources. By coupling emission from the QDs to the WGMs, the sensors can be excited and interrogated remotely and, by monitoring the shift of multiple resonance modes, may provide higher sensitivity and accuracy compared with similar techniques. The high refractometric sensitivity of the WGMs offers potential for trace detection of molecules adsorbed onto or bound to the microsphere sensor elements. The sensitivity of these sensors is demonstrated by monitoring the wavelength shift of multiple resonant modes as bulk index of refraction is changed. The potential for targeted biosensing is explored through addition of a protein that adsorbs to the microsphere surface, thrombin. Microsensor response in all cases demonstrated increased sensitivity over theoretical predictions. Models based on Mie theory and continuity of the radial functions across the sphere-media interface were used to model the location, Q-factor, and sensitivity of the WGMs in microspheres by considering the embedded QDs as a high index outer layer. This model was used, along with estimates of the QD-layer index and penetration depth, to relate the locations and sensitivities of the modes to our experimental results with strong agreement between the two. In all, these microspheres demonstrate feasibility for use as remote microsensors with sensitivities rivaling current techniques.

The technique of single particle Total Internal Reflection Microscopy (TIRM) has been used to study the scattering intensity from levitated microspheres. TIRM can be used to monitor the separation between microscopic spheres immersed in liquid (water in our case) and a surface with nm resolution. In the technique, microspheres scatter light when the evanescent waves are incident upon them. The intensity of the scattered light is directly related to the height above the surface and allows determination of the height. From the separation distance histograms, the interaction between the microsphere and interface may be characterized with a force resolution in the range of 0.01 picoNewtons. Such a system can be applied to the measurement of biomolecular interactions biomolecules attached to the microsphere and the surface. The intensity and scattering pattern of this light has been modeled using a modified Mie theory which accounts for the evanescent nature of the incident light. Diffusing Colloidal Probe Microscopy (DCPM) is an extension of the TIRM technique that simultaneously monitors multiple microsphere probes. The use of multiple probes introduces the issue of probe polydispersity. When measured at the surface, a variation in scattered light intensity of nearly one order of magnitude has been observed from a purchased microsphere sample. Thus the polydisperse collection of microspheres adds significant complexity to the scattered light signal. It is hypothesized that the dependence of the total scattered light intensity on microsphere size accounts for the scattered intensity distribution in a polydisperse microsphere sample. Understanding this variation in the scattered light with microsphere size will allow improved characterization of the microsphere/surface separation. Additionally, larger microspheres have the ability to resonantly confine light and produce spectrally narrow Whispering Gallery Modes (WGMs). It is hypothesized that WGMs may be excited in microspheres with the DCPM system. These modes may be used as a refractometric biosensor with high sensitivity to local refractive index changes on the surface of the microsphere. This research involves modeling scattered intensity distributions for polydispersed collections of microspheres based on modified Mie theory. The theoretical results are compared to experimentally obtained results and found to qualitatively explain the scattered light intensity distribution in a multiple probe DCPM system. This is an important result suggesting that microsphere size variation plays a major role in determining the distribution of scattered intensity in multiple microsphere probe systems. This work also suggests that it may be possible to excite such WGMs in a DCPM system. The introduction of WGMs would enable refractometric biosensing in such evanescent mode systems.

Optical whispering-gallery mode (WGM) cavities, which exhibit extraordinary spatial and temporal confinement of light, are one of the leading transducers for examining molecular recognition at low particle counts. With the advent of hybrid photonic-plasmonic and increasingly sophisticated forms of these resonators, the importance of supporting numerical methods has correspondingly become evident. In response, we adopt a full-vector finite difference approximation in order to solve for WGM's in terms of their field distributions, resonant wavelengths, and quality factors in the context of naturally discontinuous permittivity structure. A segmented Taylor series and alignment/rotation operator are utilized at such singularities in conjunction with arbitrarily spaced grid points. Simulations for microtoroids, with and without dielectric nanobeads, and plasmonic microdisks are demonstrated for short computation times and shown to be in agreement with data in the literature. Constricted surface plasmon polariton (SPP) WGM's are also featured within this document. The module of this thesis is devised as a keystone for composite WGM models that may guide experiments in the field. / Graduate

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