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With a population both increasing in number and age, comes a need for new diagnostic tools in the healthcare system, capable of diagnosing and monitoring multiple disorders in a cheap and effective way to provide personalised healthcare. Multiplex label-free biosensors have the potential to rejuvenate the current system. This thesis details the assessment of an ‘in house’ built labelfree array screening technology that has potential to be a point-of-care diagnostic for personalised medicine – the Array Reader. The performance of the Array Reader platform is considered in detail and optimised for both antibody and protein screening arrays. A Global Fit protocol is developed to extract kinetic constants for all protein-protein interactions, assuming a Langmuir adsorption binding model. Standard operating procedures are developed to provide optimised dynamic range, sensitivity, reproducibility and limit of detection of immuno-kinetic assay. A new antibody bio-stack signal amplification strategy is formed, improving the detection limit 60-fold. As a consequence, the bio-stack resulted in a novel method for determining the plasmon field penetration depth, defining the assay sensing volume at the nanoparticle surface. Antibody screening arrays were investigated with an IgG quantification assay to determine total IgG content from serum samples. It relied on the ability of protein A/G to bind antibodies via the Fc region. Specific antigens were used to measure the binding properties of the antibody Fab region. By characterising both regions, we have gained insight into the overall ability of an antibody to trigger an immune response. Protein screening assay were investigated targeting C-reactive protein (CRP), a marker of inflammation. The assays performance characteristics compared favourably with clinically used CRP assays. Finally, an antibody screening array was developed to assess the efficacy of a vaccine against Yersinia pestis in a non-human primate model. The vaccine screening array is an excellent example of the versatility of the platform and just one of many possible applications for the future.

The terahertz regime has until recently been some what neglected due to the difficulty of generating and measuring terahertz radiation. Terahertz time domain spectroscopy has allowed for affordable and broadband probing of this frequency regime with phase sensitive measurements (chapter 3). This thesis aims to use this tool to add to the knowledge of the interactions between electromagnetic radiation and matter specifically in regard to plasmonics. This thesis covers several distinct phenomena related to plasmonics at terahertz frequencies. The generation of terahertz radiation from metal nanoparticles is first described in chapter 4. It is shown that the field strength of the plasmon appears to relate to the strength of the generated field. It is also shown that the power dependence of the generated terahertz radiation is not consistent with the optical rectification description of this phenomenon. An alternative explanation is developed which appears more consistent with the observations. A simple model for the power dependence is derived and compared to the experimental results. In chapter 5 the parameters that make good plasmonic materials are discussed. These parameters are used to assess the suitability of semiconductors for terahertz surface plasmon experiments. The Drude permittivity of InSb is measured here, leading to a discussion of terahertz particle plasmons in chapter 6. Finite element method modelling is used to show some merits of these over optical particle plasmons. This also includes a discussion of fabrication methods for arrays of these particles. Finally, chapter 7 is a discussion of so called spoof surface plasmons. This includes some experimental work at microwave frequencies and an in depth analysis of open ended square hole arrays supported by model matching method modelling. Perfect endoscope effects are discussed and compared to superlensing. The thesis ends with a brief conclusions chapter where some of the ideas presented are brought together.

Neste trabalho apresentamos um estudo sistemático da transmissão da radiação eletromagnética em um conjunto de fendas metálicas individuais depositadas em substratos de vidro BK7 com larguras abaixo do comprimento de onda da luz incidente. As fendas foram obtidas através da evaporação térmica de prata e ouro sobre um substrato dielétrico (vidro BK7). A fabricação das fendas foi feita de forma direta através de um equipamento de feixe de íons de Gálio (FEI Quanta 3D). A transmissão óptica das fendas foi estudada com radiação laser para os comprimentos de onda de 488 nm e 632.8 nm. Observouse uma oscilação de intensidade na transmissão devido ao efeito de interferência dos surface plasmon polariton (SPP) gerados na superfície metálica como função da espessura do filme metálico. Os resultados experimentais obtidos foram confrontados com simulações computacionais, via método de elementos finitos, a partir das quais pode se compreender os mecanismos de propagação da radiação na estrutura em questão, e compará-los com detalhes da fabricação de fendas. Procedimento similar foi realizado ao variar a largura das mesmas. Também foi feita a análise da transmissão óptica em fendas fabricadas em filmes constituídos por camadas alternadas de prata e ouro, a fim de comparar como tal mudança na configuração da estrutura afeta os resultados anteriores. O trabalho serviu para mostrar que as dimensões dos filmes metálicos, assim como das fendas, apresentavam grande influência nas propriedades de transmissão e, além do que foi possível conferir diversos conceitos básicos da teoria eletromagnética num sistema relativamente simples. A compreensão dessas propriedades é fundamental para o desenvolvimento de futuros dispositivos que utilizam efeitos plasmônicos. / This work presents a systematic study of the transmission of electromagnetic radiation on a set of single metallic slits metallic with widths below the wavelength of incident light, deposited on BK7 glass substrates. The slits were obtained by thermal evaporation of silver and gold on a dielectric (BK7 glass). The fabrication of the slits was performed directly through a gallium ion beam equipment (FEI Quanta 3D). The optical transmission of the slits was studied by laser radiation for the wavelengths of 488 nm and 632.8 nm. An oscillation in the transmission intensity was observed due to the interference effect of the surface plasmon polariton (SPP) generated on the metallic surface as a function of the metal film thickness. The experimental results were compared with computational simulations, via finite element method, in order to comprehend the mechanisms of radiation propagation in the structure and compare them with details of slits fabrication. A similar procedure was performed by varying the width of the slits. An analagous analysis of the optical transmission in slits fabricated in films consisting of alternating layers of silver and gold was performed in order to compare how this change in structure configuration affects the previous results. The work served to show that the dimensions of the metal films, as well as of the slits, have a significant influence on the properties of transmission, and, moreover it was possible to confer different basic concepts of electromagnetic theory in a relatively simple system. Understanding these properties is fundamental for the development of future devices that make use of plasmonics effects.

Single particle microscopy and spectroscopy strategies reveal hidden relationships between the surface plasmon resonances (SPRs) and the sizes, shapes, and arrangements of gold nanoparticles (Au NPs). The SPR, the coherent oscillation of the conduction electrons, leads to intense absorption and scattering of light at frequencies satisfying the resonance condition determined by the size, shape, and spacings between NPs. Growing and assembling NPs through wet chemistry yields a diversity of geometries. Together, optical spectroscopy, scanning electron microscopy (SEM), and computational modeling of individual NPs and NP assemblies elucidate the resulting variety of SPRs. Strong coupling of the SPRs in linear assemblies provokes particular interest for tunable structures that will benefit surface enhanced spectroscopies and optical computing. The influence of the constituents and imperfections in such assemblies, which deviate from idealized model systems, must be established one assembly at a time. This thesis demonstrates previously unknown and sensitive relationships between the SPRs and these geometric parameters through systematic single particle experiments of self-assembled ring superstructures, nanorod dimers, individual nanorods populating different size regimes, and short linear chains of Au NPs through single particle spectroscopy. Dark-field scattering of self-assembled ring superstructures of 40 nm Au NPs reveals new plasmon modes that are redshifted from the single NP SPR by hundreds of nanometers, highly polarized along the axis of alignment, and indifferent to irregularities in the NP arrangement. SPRs of Au nanorod dimers, however, are dramatically altered by NP size heterogeneity, reduced symmetry, and metallic contact, consistent with previous studies of small assemblies. Broad band single particle extinction measurements of individual Au nanorods and short chains of 200-1000 nm long demonstrate the importance of the overall dimensions of an NP or an assembly of NPs. Finally, extinction measurements of these chains provide a compelling comparison to chemical polymers via the redshifting of the lowest energy SPR, tolerance to disorder, and the influence of the repeat unit. This result extends already well-defined analogies between plasmonic assemblies and chemical molecules to the ‘plasmonic polymer’. The findings presented in this thesis bring deeper and more detailed understanding to the tunable optical properties of real NP assemblies.

The high speed transfer of information in materials with dimensions below the sub-diffraction limit is essential for future technological developments. Metallic nanoparticle (NP) waveguides serve a unique role in efficient energy transfer in this size regime. Light may be confined to metallic structures and propagate along the surface of the waveguide via propagating plasmon waves known as surface plasmon polaritons (SPPs). Plasmon propagation of energy in metallic structures is not perfect however and damping losses from the waveguide material lead to a characteristic exponential decay in the plasmon near field intensity. This decay length is known as the propagation length and serves as an excellent metric to compare various waveguide materials and structures to one another at particular excitation wavelengths. This thesis presents recent work in the development of a novel measurement technique termed bleach imaged plasmon propagation (BlIPP). BlIPP uses the photobleaching property of fluorophores and far field fluorescence microscopy to probe the near-field intensity of propagating plasmons and determine the propagation length. The experimental setup, image analysis, conditions, and application of BlIPP are developed within this thesis and an in depth review of the 1-photon photobleaching mechanism is also investigated. The BlIPP method is used to investigate long plasmon propagation lengths along straight chains of tightly packed Au NPs through the coupling of light to sub-radiant propagating modes, where radiative energy losses are suppressed. The findings of this work reveal, experimentally, the importance of small gap distances for the propagation of energy. Complex chain architectures are then explored using BlIPP measurements of tightly packed straight and bent chains of spherical silver NPs. We observe the highly efficient propagation of energy around sharp corners with no additional bending losses. The findings of this thesis demonstrate the advantages and capabilities of using BlIPP propagation length measurement. Further, BlIPP is used to reveal the advantage of coupling light to sub-radiant modes of NP chains, which demonstrate the ability to guide light efficiently across long distances and around complex structures, bringing us a step closer to the goal of applying plasmonic devices and circuitry in ultra compact opto-electronic devices.

The Microelectronics Group has been researching sensors useful for detecting and quantifying events in biological molecular chemistry, for example, binding events. Our previous research has been based primarily on quartz resonators. This thesis describes the results of our initial research of Surface Plasmon Resonance (SPR) based technology. This study contains the design and implementation of a fully functional SPR biosensor with detailed disclosure of monolayer construction, digital hardware interfaces and software algorithms for process the SPR sensors output. An antibody monolayer was constructed on the biosensor surface with the goal of setting the strengths, weaknesses and limitation of measuring molecular events with SPR technology. We documented several characteristics of molecular chemistry that directly effect any measurements made using Surface Plasmon Resonance technology including pH, free ions, viscosity and temperature. Furthermore, the component used in our study introduced additional limitations due to wide variations amongst parts, the constraint of a liquid medium and the large surface area used for molecular interrogation. We have identified viable applications for this sensor by either eliminating or compensating for the factors that affect the measured results. This research has been published at the inaugural IEEE sensors conference and to our knowledge is the first time a biosensor has been constructed by attaching a sensor to a PDA and performing all signal processing, waveform analysis and display in the PDAs core processor.

Neste trabalho apresentamos um estudo sistemático da transmissão da radiação eletromagnética em um conjunto de fendas metálicas individuais depositadas em substratos de vidro BK7 com larguras abaixo do comprimento de onda da luz incidente. As fendas foram obtidas através da evaporação térmica de prata e ouro sobre um substrato dielétrico (vidro BK7). A fabricação das fendas foi feita de forma direta através de um equipamento de feixe de íons de Gálio (FEI Quanta 3D). A transmissão óptica das fendas foi estudada com radiação laser para os comprimentos de onda de 488 nm e 632.8 nm. Observouse uma oscilação de intensidade na transmissão devido ao efeito de interferência dos surface plasmon polariton (SPP) gerados na superfície metálica como função da espessura do filme metálico. Os resultados experimentais obtidos foram confrontados com simulações computacionais, via método de elementos finitos, a partir das quais pode se compreender os mecanismos de propagação da radiação na estrutura em questão, e compará-los com detalhes da fabricação de fendas. Procedimento similar foi realizado ao variar a largura das mesmas. Também foi feita a análise da transmissão óptica em fendas fabricadas em filmes constituídos por camadas alternadas de prata e ouro, a fim de comparar como tal mudança na configuração da estrutura afeta os resultados anteriores. O trabalho serviu para mostrar que as dimensões dos filmes metálicos, assim como das fendas, apresentavam grande influência nas propriedades de transmissão e, além do que foi possível conferir diversos conceitos básicos da teoria eletromagnética num sistema relativamente simples. A compreensão dessas propriedades é fundamental para o desenvolvimento de futuros dispositivos que utilizam efeitos plasmônicos. / This work presents a systematic study of the transmission of electromagnetic radiation on a set of single metallic slits metallic with widths below the wavelength of incident light, deposited on BK7 glass substrates. The slits were obtained by thermal evaporation of silver and gold on a dielectric (BK7 glass). The fabrication of the slits was performed directly through a gallium ion beam equipment (FEI Quanta 3D). The optical transmission of the slits was studied by laser radiation for the wavelengths of 488 nm and 632.8 nm. An oscillation in the transmission intensity was observed due to the interference effect of the surface plasmon polariton (SPP) generated on the metallic surface as a function of the metal film thickness. The experimental results were compared with computational simulations, via finite element method, in order to comprehend the mechanisms of radiation propagation in the structure and compare them with details of slits fabrication. A similar procedure was performed by varying the width of the slits. An analagous analysis of the optical transmission in slits fabricated in films consisting of alternating layers of silver and gold was performed in order to compare how this change in structure configuration affects the previous results. The work served to show that the dimensions of the metal films, as well as of the slits, have a significant influence on the properties of transmission, and, moreover it was possible to confer different basic concepts of electromagnetic theory in a relatively simple system. Understanding these properties is fundamental for the development of future devices that make use of plasmonics effects.